# Theoretical and Computational Nanoscience

## Publications

### 2021

• Advanced Data Encryption ​using 2D Materials

Wen C., Li X., Zanotti T., Puglisi F.M., Shi Y., Saiz F., Antidormi A., Roche S., Zheng W., Liang X., Hu J., Duhm S., Roldan J.B., Wu T., Chen V., Pop E., Garrido B., Zhu K., Hui F., Lanza M. Advanced Materials; 33 (27, 2100185) 2021. 10.1002/adma.202100185. IF: 30.849

Advanced data encryption requires the use of true random number generators (TRNGs) to produce unpredictable sequences of bits. TRNG circuits with high degree of randomness and low power consumption may be fabricated by using the random telegraph noise (RTN) current signals produced by polarized metal/insulator/metal (MIM) devices as entropy source. However, the RTN signals produced by MIM devices made of traditional insulators, i.e., transition metal oxides like HfO2 and Al2O3, are not stable enough due to the formation and lateral expansion of defect clusters, resulting in undesired current fluctuations and the disappearance of the RTN effect. Here, the fabrication of highly stable TRNG circuits with low power consumption, high degree of randomness (even for a long string of 224 − 1 bits), and high throughput of 1 Mbit s−1 by using MIM devices made of multilayer hexagonal boron nitride (h-BN) is shown. Their application is also demonstrated to produce one-time passwords, which is ideal for the internet-of-everything. The superior stability of the h-BN-based TRNG is related to the presence of few-atoms-wide defects embedded within the layered and crystalline structure of the h-BN stack, which produces a confinement effect that avoids their lateral expansion and results in stable operation. © 2021 Wiley-VCH GmbH.

• Chiral anomaly trapped in Weyl metals: Nonequilibrium valley polarization at zero magnetic field

Perez-Piskunow P.M., Bovenzi N., Akhmerov A.R., Breitkreiz M. SciPost Physics; 11 (2, 046) 2021. 10.21468/SCIPOSTPHYS.11.2.046. IF: 6.050

In Weyl semimetals, the application of parallel electric and magnetic fields leads to valley polarization-an occupation disbalance of valleys of opposite chirality-a direct consequence of the chiral anomaly. In this work, we present numerical tools to explore such nonequilibrium effects in spatially confined three-dimensional systems with a variable disorder potential, giving exact solutions to leading order in the disorder potential and the applied electric field. Application to a Weyl-metal slab shows that valley polarization also occurs without an external magnetic field as an effect of chiral anomaly “trapping”: Spatial confinement produces chiral bulk states, which enable the valley polarization in a similar way as the chiral states induced by a magnetic field. Despite its finite-size origin, the valley polarization can persist up to macroscopic length scales if the disorder potential is sufficiently long ranged, so that direct inter-valley scattering is suppressed and the relaxation then goes via the Fermi-arc surface states. Copyright © Perez Piskunow et al.

• Disentangling Orbital and Valley Hall Effects in Bilayers of Transition Metal Dichalcogenides

Cysne T.P., Costa M., Canonico L.M., Nardelli M.B., Muniz R.B., Rappoport T.G. Physical Review Letters; 126 (5, 056601) 2021. 10.1103/PhysRevLett.126.056601. IF: 9.161

It has been recently shown that monolayers of transition metal dichalcogenides (TMDs) in the 2H structural phase exhibit relatively large orbital Hall conductivity plateaus within their energy band gaps, where their spin Hall conductivities vanish [Canonico et al., Phys. Rev. B 101, 161409 (2020)PRBMDO2469-995010.1103/PhysRevB.101.161409; Bhowal and Satpathy, Phys. Rev. B 102, 035409 (2020)PRBMDO2469-995010.1103/PhysRevB.102.035409]. However, since the valley Hall effect (VHE) in these systems also generates a transverse flow of orbital angular momentum, it becomes experimentally challenging to distinguish between the two effects in these materials. The VHE requires inversion symmetry breaking to occur, which takes place in the TMD monolayers but not in the bilayers. We show that a bilayer of 2H-MoS2 is an orbital Hall insulator that exhibits a sizeable orbital Hall effect in the absence of both spin and valley Hall effects. This phase can be characterized by an orbital Chern number that assumes the value CL=2 for the 2H-MoS2 bilayer and CL=1 for the monolayer, confirming the topological nature of these orbital-Hall insulator systems. Our results are based on density functional theory and low-energy effective model calculations and strongly suggest that bilayers of TMDs are highly suitable platforms for direct observation of the orbital Hall insulating phase in two-dimensional materials. Implications of our findings for attempts to observe the VHE in TMD bilayers are also discussed. © 2021 American Physical Society.

• Emerging properties of non-crystalline phases of graphene and boron nitride based materials

Antidormi A., Colombo L., Roche S. Nano Materials Science; 2021. 10.1016/j.nanoms.2021.03.003. IF: 0.000

We review recent developments on the synthesis and properties of two-dimensional materials which, although being mainly of an sp2 bonding character, exhibit highly disordered, non-uniform and structurally random morphologies. The emergence of such class of amorphous materials, including amorphous graphene and boron nitride, have shown superior properties compared to their crystalline counterparts when used as interfacial films. In this paper we discuss their structural, vibrational and electronic properties and present a perspective of their use for electronic applications. © 2021 Chongqing University

• Exploring billion-atom-scale quantum materials using linear scaling quantum transport

Garcia J.H. Nature Reviews Physics; 3 (6): 388. 2021. 10.1038/s42254-021-00318-1. IF: 31.068

[No abstract available]

• Graphene on two-dimensional hexagonal BN, AlN, and GaN: Electronic, spin-orbit, and spin relaxation properties

Zollner K., Cummings A.W., Roche S., Fabian J. Physical Review B; 103 (7, 075129) 2021. 10.1103/PhysRevB.103.075129. IF: 4.036

We investigate the electronic band structure of graphene on a series of two-dimensional hexagonal nitride insulators hXN, X=B, Al, and Ga, with first-principles calculations. A symmetry-based model Hamiltonian is employed to extract orbital parameters and spin-orbit coupling (SOC) from the low-energy Dirac bands of the proximitized graphene. While commensurate hBN induces a staggered potential of about 10 meV into the Dirac band structure, less lattice-matched hAlN and hGaN disrupt the Dirac point much less, giving a staggered gap below 100 μeV. Proximitized intrinsic SOC surprisingly does not increase much above the pristine graphene value of 12 μeV; it stays in the window of 1-16 μeV, depending strongly on stacking. However, Rashba SOC increases sharply when increasing the atomic number of the boron group, with calculated maximal values of 8, 15, and 65 μeV for B-, Al-, and Ga-based nitrides, respectively. The individual Rashba couplings also depend strongly on stacking, vanishing in symmetrically sandwiched structures, and can be tuned by a transverse electric field. The extracted spin-orbit parameters were used as input for spin transport simulations based on Chebyshev expansion of the time-evolution of the spin expectation values, yielding interesting predictions for the electron spin relaxation. Spin lifetime magnitudes and anisotropies depend strongly on the specific (hXN)/graphene/hXN system, and they can be efficiently tuned by an applied external electric field as well as the carrier density in the graphene layer. A particularly interesting case for experiments is graphene/hGaN, in which the giant Rashba coupling is predicted to induce spin lifetimes of 1-10 ns, short enough to dominate over other mechanisms, and lead to the same spin relaxation anisotropy as that observed in conventional semiconductor heterostructures: 50%, meaning that out-of-plane spins relax twice as fast as in-plane spins. © 2021 American Physical Society.

• Hinge Spin Polarization in Magnetic Topological Insulators Revealed by Resistance Switch

Perez-Piskunow P.M., Roche S. Physical Review Letters; 126 (16, 167701) 2021. 10.1103/PhysRevLett.126.167701. IF: 9.161

We report on the possibility of detecting hinge spin polarization in magnetic topological insulators by resistance measurements. By implementing a three-dimensional model of magnetic topological insulators into a multiterminal device with ferromagnetic contacts near the top surface, local spin features of the chiral edge modes are unveiled. We find local spin polarization at the hinges that inverts the sign between the top and bottom surfaces. At the opposite edge, the topological state with inverted spin polarization propagates in the reverse direction. A large resistance switch between forward and backward propagating states is obtained, driven by the matching between the spin polarized hinges and the ferromagnetic contacts. This feature is general to the ferromagnetic, antiferromagnetic, and canted antiferromagnetic phases, and enables the design of spin-sensitive devices, with the possibility of reversing the hinge spin polarization of the currents. © 2021 American Physical Society.

• Linear scaling quantum transport methodologies

Fan Z., Garcia J.H., Cummings A.W., Barrios-Vargas J.E., Panhans M., Harju A., Ortmann F., Roche S. Physics Reports; 903: 1 - 69. 2021. 10.1016/j.physrep.2020.12.001. IF: 25.600

In recent years, predictive computational modeling has become a cornerstone for the study of fundamental electronic, optical, and thermal properties in complex forms of condensed matter, including Dirac and topological materials. The simulation of quantum transport in realistic models calls for the development of linear scaling, or order-N, numerical methods, which then become enabling tools for guiding experimental research and for supporting the interpretation of measurements. In this review, we describe and compare different order-N computational methods that have been developed during the past twenty years, and which have been used extensively to explore quantum transport phenomena in disordered media. We place particular focus on the zero-frequency electrical conductivities derived within the Kubo–Greenwood​ and Kubo–Streda formalisms, and illustrate the capabilities of these methods to tackle the quasi-ballistic, diffusive, and localization regimes of quantum transport in the noninteracting limit. The fundamental issue of computational cost versus accuracy of various proposed numerical schemes is addressed in depth. We then illustrate the usefulness of these methods with various examples of transport in disordered materials, such as polycrystalline and defected graphene models, 3D metals and Dirac semimetals, carbon nanotubes, and organic semiconductors. Finally, we extend the review to the study of spin dynamics and topological transport, for which efficient approaches for calculating charge, spin, and valley Hall conductivities are described. © 2020 The Author(s)

• Observation of giant and tunable thermal diffusivity of a Dirac fluid at room temperature

Block A., Principi A., Hesp N.C.H., Cummings A.W., Liebel M., Watanabe K., Taniguchi T., Roche S., Koppens F.H.L., van Hulst N.F., Tielrooij K.-J. Nature Nanotechnology; 2021. 10.1038/s41565-021-00957-6. IF: 39.213

Conducting materials typically exhibit either diffusive or ballistic charge transport. When electron–electron interactions dominate, a hydrodynamic regime with viscous charge flow emerges1–13. More stringent conditions eventually yield a quantum-critical Dirac-fluid regime, where electronic heat can flow more efficiently than charge14–22. However, observing and controlling the flow of electronic heat in the hydrodynamic regime at room temperature has so far remained elusive. Here we observe heat transport in graphene in the diffusive and hydrodynamic regimes, and report a controllable transition to the Dirac-fluid regime at room temperature, using carrier temperature and carrier density as control knobs. We introduce the technique of spatiotemporal thermoelectric microscopy with femtosecond temporal and nanometre spatial resolution, which allows for tracking electronic heat spreading. In the diffusive regime, we find a thermal diffusivity of roughly 2,000 cm2 s−1, consistent with charge transport. Moreover, within the hydrodynamic time window before momentum relaxation, we observe heat spreading corresponding to a giant diffusivity up to 70,000 cm2 s−1, indicative of a Dirac fluid. Our results offer the possibility of further exploration of these interesting physical phenomena and their potential applications in nanoscale thermal management. © 2021, The Author(s).

• Optimizing the Photothermoelectric Effect in Graphene

Antidormi A., Cummings A.W. Physical Review Applied; 15 (5, 054049) 2021. 10.1103/PhysRevApplied.15.054049. IF: 4.985

Among its many uses, graphene shows significant promise for optical and optoelectronic applications. In particular, devices based on the photothermoelectric effect (PTE) in graphene can offer a strong and fast photoresponse with a high signal-to-noise ratio while consuming minimal power. In this work, we discuss how to optimize the performance of graphene PTE photodetectors by tuning the light confinement, device geometry, and material quality. This study should prove useful for the design of devices using the PTE in graphene, with applications including optical sensing, data communications, multigas sensing, and others. © 2021 American Physical Society.

• Room-temperature tunnel magnetoresistance across biomolecular tunnel junctions based on ferritin

Karuppannan S.K., Pasula R.R., Herng T.S., Ding J., Chi X., Barco E.D., Roche S., Yu X., Yakovlev N., Lim S., Nijhuis C.A. JPhys Materials; 4 (3, 035003) 2021. 10.1088/2515-7639/abfa79. IF: 0.000

We report exceptionally large tunnel magnetoresistance (TMR) for biomolecular tunnel junctions based on ferritins immobilized between Ni and EGaIn electrodes. Ferritin stores iron in the form of ferrihydrite nanoparticles (NPs) and fulfills the following roles: (a) it dictates the tunnel barrier, (b) it magnetically decouples the NPs from the ferromagnetic (FM) electrode, (c) it stabilizes the NPs, and (d) it acts as a spin filter reducing the complexity of the tunnel junctions since only one FM electrode is required. The mechanism of charge transport is long-range tunneling which results in TMR of 60 ± 10% at 200 K and 25 ± 5% at room temperature. We propose a magnon-assisted transmission to explain the substantially larger TMR switching fields (up to 1 Tesla) than the characteristic coercive fields (a few Gauss) of ferritin ferrihydrite particles at T < 20 K. These results highlight the genuine potential of biomolecular tunnel junctions in designing functional nanoscale spintronic devices. © 2021 The Author(s). Published by IOP Publishing Ltd.

• Strong Suppression of Thermal Conductivity in the Presence of Long Terminal Alkyl Chains in Low-Disorder Molecular Semiconductors

Selezneva E., Vercouter A., Schweicher G., Lemaur V., Broch K., Antidormi A., Takimiya K., Coropceanu V., Brédas J.-L., Melis C., Cornil J., Sirringhaus H. Advanced Materials; 33 (37, 2008708) 2021. 10.1002/adma.202008708. IF: 30.849

While the charge transport properties of organic semiconductors have been extensively studied over the recent years, the field of organics-based thermoelectrics is still limited by a lack of experimental data on thermal transport and of understanding of the associated structure–property relationships. To fill this gap, a comprehensive experimental and theoretical investigation of the lattice thermal conductivity in polycrystalline thin films of dinaphtho[2,3-b:2′,3′-f]thieno[3,2-b]thiophene (Cn-DNTT-Cn with n = 0, 8) semiconductors is reported. Strikingly, thermal conductivity appears to be much more isotropic than charge transport, which is confined to the 2D molecular layers. A direct comparison between experimental measurements (3ω–Völklein method) and theoretical estimations (approach-to-equilibrium molecular dynamics (AEMD) method) indicates that the in-plane thermal conductivity is strongly reduced in the presence of the long terminal alkyl chains. This evolution can be rationalized by the strong localization of the intermolecular vibrational modes in C8-DNTT-C8 in comparison to unsubstituted DNTT cores, as evidenced by a vibrational mode analysis. Combined with the enhanced charge transport properties of alkylated DNTT systems, this opens the possibility to decouple electron and phonon transport in these materials, which provides great potential for enhancing the thermoelectric figure of merit ZT. © 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH

• Thermal conductivity of benzothieno-benzothiophene derivatives at the nanoscale

Gueye M.N., Vercouter A., Jouclas R., Guérin D., Lemaur V., Schweicher G., Lenfant S., Antidormi A., Geerts Y., Melis C., Cornil J., Vuillaume D. Nanoscale; 13 (6): 3800 - 3807. 2021. 10.1039/d0nr08619c. IF: 7.790

We study by scanning thermal microscopy the nanoscale thermal conductance of films (40-400 nm thick) of [1]benzothieno[3,2-b][1]benzothiophene (BTBT) and 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene (C8-BTBT-C8). We demonstrate that the out-of-plane thermal conductivity is significant along the interlayer direction, larger for BTBT (0.63 ± 0.12 W m-1 K-1) compared to C8-BTBT-C8 (0.25 ± 0.13 W m-1 K-1). These results are supported by molecular dynamics calculations (approach to equilibrium molecular dynamics method) performed on the corresponding molecular crystals. The calculations point to significant thermal conductivity (3D-like) values along the 3 crystalline directions, with anisotropy factors between the crystalline directions below 1.8 for BTBT and below 2.8 for C8-BTBT-C8, in deep contrast with the charge transport properties featuring a two-dimensional character for these materials. In agreement with the experiments, the calculations yield larger values in BTBT compared to C8-BTBT-C8 (0.6-1.3 W m-1 K-1versus 0.3-0.7 W m-1 K-1, respectively). The weak thickness dependence of the nanoscale thermal resistance is in agreement with a simple analytical model. This journal is © The Royal Society of Chemistry.

• Thermal transport in amorphous graphene with varying structural quality

Antidormi A., Colombo L., Roche S. 2D Materials; 8 (1, 015028) 2021. 10.1088/2053-1583/abc7f8. IF: 7.103

The synthesis of wafer-scale two-dimensional amorphous carbon monolayers has been recently demonstrated. This material presents useful properties when integrated as coating of metals, semiconductors or magnetic materials, such as enabling efficient atomic layer deposition and hence fostering the development of ultracompact technologies. Here we propose a characterization of how the structural degree of amorphousness of such carbon membranes could be controlled by the crystal growth temperature. We also identify how energy is dissipated in this material by a systematic analysis of emerging vibrational modes whose localization increases with the loss of spatial symmetries, resulting in a tunable thermal conductivity varying by more than two orders of magnitude. Our simulations provide some recipe to design most suitable 'amorphous graphene' based on the target applications such as ultrathin heat spreaders, energy harvesters or insulating thermal barriers. © 2020 IOP Publishing Ltd.

• Valley Hall effect and nonlocal resistance in locally gapped graphene

Aktor T., Garcia J.H., Roche S., Jauho A.-P., Power S.R. Physical Review B; 103 (11, 115406) 2021. 10.1103/PhysRevB.103.115406. IF: 4.036

We report on the emergence of bulk, valley-polarized currents in graphene-based devices, driven by spatially varying regions of broken sublattice symmetry, and revealed by nonlocal resistance (RNL) fingerprints. By using a combination of quantum transport formalisms, giving access to bulk properties as well as multiterminal device responses, the presence of a nonuniform local band gap is shown to give rise to valley-dependent scattering and a finite Fermi-surface contribution to the valley Hall conductivity, related to characteristics of RNL. These features are robust against disorder and provide a plausible interpretation of controversial experiments in graphene/hexagonal boron nitride superlattices. Our findings suggest both an alternative mechanism for the generation of valley Hall effect in graphene and a route towards valley-dependent electron optics, by materials and device engineering. © 2021 American Physical Society.

• Van der Waals heterostructures for spintronics and opto-spintronics

Sierra J.F., Fabian J., Kawakami R.K., Roche S., Valenzuela S.O. Nature Nanotechnology; 16 (8): 856 - 868. 2021. 10.1038/s41565-021-00936-x. IF: 39.213

The large variety of 2D materials and their co-integration in van der Waals heterostructures enable innovative device engineering. In addition, their atomically thin nature promotes the design of artificial materials by proximity effects that originate from short-range interactions. Such a designer approach is particularly compelling for spintronics, which typically harnesses functionalities from thin layers of magnetic and non-magnetic materials and the interfaces between them. Here we provide an overview of recent progress in 2D spintronics and opto-spintronics using van der Waals heterostructures. After an introduction to the forefront of spin transport research, we highlight the unique spin-related phenomena arising from spin–orbit and magnetic proximity effects. We further describe the ability to create multifunctional hybrid heterostructures based on van der Waals materials, combining spin, valley and excitonic degrees of freedom. We end with an outlook on perspectives and challenges for the design and production of ultracompact all-2D spin devices and their potential applications in conventional and quantum technologies. © 2021, Springer Nature Limited.

### 2020

• Blue emission at atomically sharp 1D heterojunctions between graphene and h-BN

Kim G., Ma K.Y., Park M., Kim M., Jeon J., Song J., Barrios-Vargas J.E., Sato Y., Lin Y.-C., Suenaga K., Roche S., Yoo S., Sohn B.-H., Jeon S., Shin H.S. Nature Communications; 11 (1, 5359) 2020. 10.1038/s41467-020-19181-2. IF: 12.121

Atomically sharp heterojunctions in lateral two-dimensional heterostructures can provide the narrowest one-dimensional functionalities driven by unusual interfacial electronic states. For instance, the highly controlled growth of patchworks of graphene and hexagonal boron nitride (h-BN) would be a potential platform to explore unknown electronic, thermal, spin or optoelectronic property. However, to date, the possible emergence of physical properties and functionalities monitored by the interfaces between metallic graphene and insulating h-BN remains largely unexplored. Here, we demonstrate a blue emitting atomic-resolved heterojunction between graphene and h-BN. Such emission is tentatively attributed to localized energy states formed at the disordered boundaries of h-BN and graphene. The weak blue emission at the heterojunctions in simple in-plane heterostructures of h-BN and graphene can be enhanced by increasing the density of the interface in graphene quantum dots array embedded in the h-BN monolayer. This work suggests that the narrowest, atomically resolved heterojunctions of in-plane two-dimensional heterostructures provides a future playground for optoelectronics. © 2020, The Author(s).

• Canted Persistent Spin Texture and Quantum Spin Hall Effect in WTe2

Garcia J.H., Vila M., Hsu C.-H., Waintal X., Pereira V.M., Roche S. Physical Review Letters; 125 (25, 256603) 2020. 10.1103/PhysRevLett.125.256603. IF: 8.385

We report an unconventional quantum spin Hall phase in the monolayer WTe2, which exhibits hitherto unknown features in other topological materials. The low symmetry of the structure induces a canted spin texture in the yz plane, which dictates the spin polarization of topologically protected boundary states. Additionally, the spin Hall conductivity gets quantized (2e2/h) with a spin quantization axis parallel to the canting direction. These findings are based on large-scale quantum simulations of the spin Hall conductivity tensor and nonlocal resistances in multiprobe geometries using a realistic tight-binding model elaborated from first-principle methods. The observation of this canted quantum spin Hall effect, related to the formation of topological edge states with nontrivial spin polarization, demands for specific experimental design and suggests interesting alternatives for manipulating spin information in topological materials. © 2020 American Physical Society.

• Computation of topological phase diagram of disordered Pb1-xSnxTe using the kernel polynomial method

Dániel Varjas, Michel Fruchart, Anton R. Akhmerov, Pablo M. Perez-Piskunow Physical Review Research; 2 (13229) 2020. 10.1103/PhysRevResearch.2.013229 .

We present an algorithm to determine topological invariants of inhomogeneous systems, such as alloys, disordered crystals, or amorphous systems. Based on the kernel polynomial method, our algorithm allows us to study samples with more than 107 degrees of freedom. Our method enables the study of large complex compounds, where disorder is inherent to the system. We use it to analyze Pb1−xSnxTe and tighten the critical concentration for the phase transition. Moreover, we obtain the topological phase diagram for related alloys in the family of three-dimensional mirror Chern insulators.

• Efficient machine-learning based interatomic potentialsfor exploring thermal conductivity in two-dimensional materials

Bohayra Mortazavi, V Evgeny Podryabinkin, Ivan S Novikov, Stephan Roche, Timon Rabczuk,Xiaoying Zhuang; V Alexander Shapeev Journal of Physics-Materials; 3 (2, 02LT02) 2020. 10.1088/2515-7639/ab7cbb. IF: 0.000

• Emergence of intraparticle entanglement and time-varying violation of Bell's inequality in Dirac matter

De Moraes B.G., Cummings A.W., Roche S. Physical Review B; 102 (4, 041403) 2020. 10.1103/PhysRevB.102.041403. IF: 3.575

We demonstrate the emergence and dynamics of intraparticle entanglement in massless Dirac fermions. This entanglement, generated by spin-orbit coupling, arises between the spin and sublattice pseudospin of electrons in graphene. The entanglement is a complex dynamic quantity but is generally large, independent of the initial state. Its time dependence implies a dynamical violation of a Bell inequality, while its magnitude indicates that large intraparticle entanglement is a general feature of graphene on a substrate. These features are also expected to impact entanglement between pairs of particles, and may be detectable in experiments that combine Cooper pair splitting with nonlocal measurements of spin-spin correlation in mesoscopic devices based on Dirac materials. © 2020 American Physical Society.

• Exploring event horizons and Hawking radiation through deformed graphene membranes

Morresi T., Binosi D., Simonucci S., Piergallini R., Roche S., Pugno N.M., Simone T. 2D Materials; 7 (4, 041006) 2020. 10.1088/2053-1583/aba448. IF: 7.140

Analogue gravitational systems are becoming an increasing popular way of studying the behaviour of quantum systems in curved spacetime. Setups based on ultracold quantum gases in particular, have been recently harnessed to explore the thermal nature of Hawking's and Unruh's radiation that was theoretically predicted almost 50 years ago. For solid state implementations, a promising system is graphene, in which a link between the Dirac-like low-energy electronic excitations and relativistic quantum field theories has been unveiled soon after its discovery. This link could be extended to the case of curved quantum field theory when the graphene sheet is shaped in a surface of constant negative curvature, known as Beltrami's pseudosphere. Here we provide numerical evidence that energetically stable negative curvature graphene surfaces can be realized. Owing to large-scale simulations, our geometrical realizations are characterized by a ratio between the carbon-carbon bond length and the pseudosphere radius small enough to allow the formation of an analog of a black hole event horizon. Additionally, from the energy dependence of the spatially resolved density of states, we infer some thermal properties of the corresponding gravitational system, which could be investigated using low temperature scanning tunnelling microscopy or optical near field spectroscopy. These findings pave the way to the realization of a solid-state system in which the curved spacetime dynamics of quantum many body systems can be investigated. © 2020 IOP Publishing Ltd.

• Exploring phononic properties of two-dimensional materials using machine learning interatomic potentials

Mortazavi B., Novikov I.S., Podryabinkin E.V., Roche S., Rabczuk T., Shapeev A.V., Zhuang X. Applied Materials Today; 20 (100685) 2020. 10.1016/j.apmt.2020.100685. IF: 8.352

Phononic properties are commonly studied by calculating force constants using the density functional theory (DFT) simulations. Although DFT simulations offer accurate estimations of phonon dispersion relations or thermal properties, but for low-symmetry and nanoporous structures the computational cost quickly becomes very demanding. Moreover, the computational setups may yield nonphysical imaginary frequencies in the phonon dispersion curves, impeding the assessment of phononic properties and the dynamical stability of the considered system. Here, we compute phonon dispersion relations and examine the dynamical stability of a large ensemble of novel materials and compositions. We propose a fast and convenient alternative to DFT simulations which derived from machine-learning interatomic potentials passively trained over computationally efficient ab-initio molecular dynamics trajectories. Our results for diverse two-dimensional (2D) nanomaterials confirm that the proposed computational strategy can reproduce fundamental thermal properties in close agreement with those obtained via the DFT approach. The presented method offers a stable, efficient, and convenient solution for the examination of dynamical stability and exploring the phononic properties of low-symmetry and porous 2D materials. © 2020 Elsevier Ltd

• Impact of oxidation morphology on reduced graphene oxides upon thermal annealing

Aleandro Antidormi, Stephan Roche, Luciano Colombo Journal Of Physics-Materials; 3 (1, 15011) 2020. 10.1088/2515-7639/ab5ef2. IF: 0.000

• Impact of synthetic conditions on the anisotropic thermal conductivity of poly(3,4-ethylenedioxythiophene) (PEDOT): A molecular dynamics investigation

Cappai A., Antidormi A., Bosin A., Narducci D., Colombo L., Melis C. Physical Review Materials; 4 (3, 035401) 2020. 10.1103/PhysRevMaterials.4.035401. IF: 3.337

In this work we study the effect of different synthetic conditions on thermal transport properties of poly(3,4-ethylenedioxythiophene) (PEDOT) by focusing in particular on the role of proton scavengers. To this aim, different PEDOT samples were generated in silico using a novel computational algorithm based on a combination of first-principles density functional theory and classical molecular dynamics simulations. The corresponding thermal conductivities were then estimated using the approach to equilibrium molecular dynamics methodology. The results show that the initial synthetic conditions strongly affect the corresponding thermal conductivities, which display variations up to a factor of ∼2 depending on the proton scavenger. By decomposing the thermal conductivity tensor along the direction of maximum chain alignment and the corresponding perpendicular directions, we attribute the thermal conductivity differences to the variations in the average polymer chain length λave. A dependence of the thermal conductivity with the polydispersity index was finally observed, suggesting a possible role of intercrystallite chains in enhancing thermal transport properties. By means of the Green-Kubo modal analysis, we eventually characterize the vibrational modes involved in PEDOT thermal transport and investigate how they are related to the thermal conductivity values of the samples. © 2020 American Physical Society.

• Machine-learning interatomic potentials enable first-principles multiscale modeling of lattice thermal conductivity in graphene/borophene heterostructures

Mortazavi B., Podryabinkin E.V., Roche S., Rabczuk T., Zhuang X., Shapeev A.V. Materials Horizons; 7 (9): 2359 - 2367. 2020. 10.1039/d0mh00787k. IF: 12.319

One of the ultimate goals of computational modeling in condensed matter is to be able to accurately compute materials properties with minimal empirical information. First-principles approaches such as density functional theory (DFT) provide the best possible accuracy on electronic properties but they are limited to systems up to a few hundreds, or at most thousands of atoms. On the other hand, classical molecular dynamics (CMD) simulations and the finite element method (FEM) are extensively employed to study larger and more realistic systems, but conversely depend on empirical information. Here, we show that machine-learning interatomic potentials (MLIPs) trained over short ab initio molecular dynamics trajectories enable first-principles multiscale modeling, in which DFT simulations can be hierarchically bridged to efficiently simulate macroscopic structures. As a case study, we analyze the lattice thermal conductivity of coplanar graphene/borophene heterostructures, recently synthesized experimentally (Sci. Adv., 2019, 5, eaax6444), for which no viable classical modeling alternative is presently available. Our MLIP-based approach can efficiently predict the lattice thermal conductivity of graphene and borophene pristine phases, the thermal conductance of complex graphene/borophene interfaces and subsequently enable the study of effective thermal transport along the heterostructures at continuum level. This work highlights that MLIPs can be effectively and conveniently employed to enable first-principles multiscale modeling via hierarchical employment of DFT/CMD/FEM simulations, thus expanding the capability for computational design of novel nanostructures. © 2020 The Royal Society of Chemistry.

• Magnetic proximity in a van der Waals heterostructure of magnetic insulator and graphene

Karpiak B., Cummings A.W., Zollner K., Vila M., Khokhriakov D., Hoque A.M., Dankert A., Svedlindh P., Fabian J., Roche S., Dash S.P. 2D Materials; 7 (1, 015026) 2020. 10.1088/2053-1583/ab5915. IF: 7.140

Engineering 2D material heterostructures by combining the best of different materials in one ultimate unit can offer a plethora of opportunities in condensed matter physics. Here, in the van der Waals heterostructures of the ferromagnetic insulator Cr2Ge2Te6 and graphene, our observations indicate an out-of-plane proximity-induced ferromagnetic exchange interaction in graphene. The perpendicular magnetic anisotropy of Cr2Ge2Te6 results in significant modification of the spin transport and precession in graphene, which can be ascribed to the proximity-induced exchange interaction. Furthermore, the observation of a larger lifetime for perpendicular spins in comparison to the in-plane counterpart suggests the creation of a proximity-induced anisotropic spin texture in graphene. Our experimental results and density functional theory calculations open up opportunities for the realization of proximity-induced magnetic interactions and spin filters in 2D material heterostructures and can form the basic building blocks for future spintronic and topological quantum devices. © 2019 IOP Publishing Ltd.

• Magnetism, spin dynamics, and quantum transport in two-dimensional systems

Savero Torres W., Sierra J.F., Benítez L.A., Bonell F., García J.H., Roche S., Valenzuela S.O. MRS Bulletin; 45 (5): 357 - 365. 2020. 10.1557/mrs.2020.121. IF: 5.061

Two-dimensional (2D) quantum materials offer a unique platform to explore mesoscopic phenomena driven by interfacial and topological effects. Their tunable electric properties and bidimensional nature enable their integration into sophisticated heterostructures with engineered properties, resulting in the emergence of new exotic phenomena not accessible in other platforms. This has fostered many studies on 2D ferromagnetism, proximity-induced effects, and quantum transport, demonstrating their relevance for fundamental research and future device applications. Here, we review ongoing progress in this lively research field with special emphasis on spin-related phenomena. © Materials Research Society 2020.

• Nonlocal Spin Dynamics in the Crossover from Diffusive to Ballistic Transport

Vila M., Garcia J.H., Cummings A.W., Power S.R., Groth C.W., Waintal X., Roche S. Physical Review Letters; 124 (19, 196602) 2020. 10.1103/PhysRevLett.124.196602. IF: 8.385

Improved fabrication techniques have enabled the possibility of ballistic transport and unprecedented spin manipulation in ultraclean graphene devices. Spin transport in graphene is typically probed in a nonlocal spin valve and is analyzed using spin diffusion theory, but this theory is not necessarily applicable when charge transport becomes ballistic or when the spin diffusion length is exceptionally long. Here, we study these regimes by performing quantum simulations of graphene nonlocal spin valves. We find that conventional spin diffusion theory fails to capture the crossover to the ballistic regime as well as the limit of long spin diffusion length. We show that the latter can be described by an extension of the current theoretical framework. Finally, by covering the whole range of spin dynamics, our study opens a new perspective to predict and scrutinize spin transport in graphene and other two-dimensional material-based ultraclean devices. © 2020 American Physical Society.

• Optimization of the sensitivity of a double-dot magnetic detector

Macucci M., Marconcini P., Roche S. Electronics (Switzerland); 9 (7, 1134): 1 - 13. 2020. 10.3390/electronics9071134. IF: 2.412

We investigate, by means of numerical simulations, the lowest magnetic field level that can be detected with a given relative accuracy with a sensor based on a double-dot device fabricated in a high-mobility two-dimensional electron gas. The double dot consists of a cavity delimited by an input and an output constriction, with a potential barrier exactly in the middle. In conditions of perfect symmetry, a strong conductance enhancement effect appears as a consequence of the constructive interference between symmetric trajectories. When the symmetry is broken, for example by the presence of an applied magnetic field, this enhancement effect is suppressed. We explore the design parameter space and assess the minimum magnetic field value that can be measured with a given accuracy in the presence of flicker noise. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.

• Tunable room-temperature spin galvanic and spin Hall effects in van der Waals heterostructures

Benítez L.A., Savero Torres W., Sierra J.F., Timmermans M., Garcia J.H., Roche S., Costache M.V., Valenzuela S.O. Nature Materials; 19 (2): 170 - 175. 2020. 10.1038/s41563-019-0575-1. IF: 38.663

Spin–orbit coupling stands as a powerful tool to interconvert charge and spin currents and to manipulate the magnetization of magnetic materials through spin-torque phenomena. However, despite the diversity of existing bulk materials and the recent advent of interfacial and low-dimensional effects, control of this interconversion at room temperature remains elusive. Here, we demonstrate strongly enhanced room-temperature spin-to-charge interconversion in graphene driven by the proximity of WS2. By performing spin precession experiments in appropriately designed Hall bars, we separate the contributions of the spin Hall and the spin galvanic effects. Remarkably, their corresponding conversion efficiencies can be tailored by electrostatic gating in magnitude and sign, peaking near the charge neutrality point with an equivalent magnitude that is comparable to the largest efficiencies reported to date. Such electric-field tunability provides a building block for spin generation free from magnetic materials and for ultra-compact magnetic memory technologies. © 2020, The Author(s), under exclusive licence to Springer Nature Limited.

• Ultralow-dielectric-constant amorphous boron nitride

Hong S., Lee C.-S., Lee M.-H., Lee Y., Ma K.Y., Kim G., Yoon S.I., Ihm K., Kim K.-J., Shin T.J., Kim S.W., Jeon E.-C., Jeon H., Kim J.-Y., Lee H.-I., Lee Z., Antidormi A., Roche S., Chhowalla M., Shin H.-J., Shin H.S. Nature; 582 (7813): 511 - 514. 2020. 10.1038/s41586-020-2375-9. IF: 42.779

Decrease in processing speed due to increased resistance and capacitance delay is a major obstacle for the down-scaling of electronics1–3. Minimizing the dimensions of interconnects (metal wires that connect different electronic components on a chip) is crucial for the miniaturization of devices. Interconnects are isolated from each other by non-conducting (dielectric) layers. So far, research has mostly focused on decreasing the resistance of scaled interconnects because integration of dielectrics using low-temperature deposition processes compatible with complementary metal–oxide–semiconductors is technically challenging. Interconnect isolation materials must have low relative dielectric constants (κ values), serve as diffusion barriers against the migration of metal into semiconductors, and be thermally, chemically and mechanically stable. Specifically, the International Roadmap for Devices and Systems recommends4 the development of dielectrics with κ values of less than 2 by 2028. Existing low-κ materials (such as silicon oxide derivatives, organic compounds and aerogels) have κ values greater than 2 and poor thermo-mechanical properties5. Here we report three-nanometre-thick amorphous boron nitride films with ultralow κ values of 1.78 and 1.16 (close to that of air, κ = 1) at operation frequencies of 100 kilohertz and 1 megahertz, respectively. The films are mechanically and electrically robust, with a breakdown strength of 7.3 megavolts per centimetre, which exceeds requirements. Cross-sectional imaging reveals that amorphous boron nitride prevents the diffusion of cobalt atoms into silicon under very harsh conditions, in contrast to reference barriers. Our results demonstrate that amorphous boron nitride has excellent low-κ dielectric characteristics for high-performance electronics. © 2020, The Author(s), under exclusive licence to Springer Nature Limited.

### 2019

• Gate electrostatics and quantum capacitance in ballistic graphene devices

Caridad J.M., Power S.R., Shylau A.A., Gammelgaard L., Jauho A.-P., Bøggild P. Physical Review B; 99 (19, 195408) 2019. 10.1103/PhysRevB.99.195408. IF: 3.736

We experimentally investigate the charge induction mechanism across gated, narrow, ballistic graphene devices with different degrees of edge disorder. By using magnetoconductance measurements as the probing technique, we demonstrate that devices with large edge disorder exhibit a nearly homogeneous capacitance profile across the device channel, close to the case of an infinitely large graphene sheet. In contrast, devices with lower edge disorder (<1nm roughness) are strongly influenced by the fringing electrostatic field at graphene boundaries, in quantitative agreement with theoretical calculations for pristine systems. Specifically, devices with low edge disorder present a large effective capacitance variation across the device channel with a nontrivial, inhomogeneous profile due not only to classical electrostatics but also to quantum mechanical effects. We show that such quantum capacitance contribution, occurring due to the low density of states across the device in the presence of an external magnetic field, is considerably altered as a result of the gate electrostatics in the ballistic graphene device. Our conclusions can be extended to any two-dimensional (2D) electronic system confined by a hard-wall potential and are important for understanding the electronic structure and device applications of conducting 2D materials. © 2019 American Physical Society.

• Green function, quasi-classical Langevin and Kubo-Greenwood methods in quantum thermal transport

Sevinçli H., Roche S., Cuniberti G., Brandbyge M., Gutierrez R., Sandonas L.M. Journal of Physics Condensed Matter; 31 (27, 273003) 2019. 10.1088/1361-648X/ab119a. IF: 2.711

With the advances in fabrication of materials with feature sizes at the order of nanometers, it has been possible to alter their thermal transport properties dramatically. Miniaturization of device size increases the power density in general, hence faster electronics require better thermal transport, whereas better thermoelectric applications require the opposite. Such diverse needs bring new challenges for material design. Shrinkage of length scales has also changed the experimental and theoretical methods to study thermal transport. Unsurprisingly, novel approaches have emerged to control phonon flow. Besides, ever increasing computational power is another driving force for developing new computational methods. In this review, we discuss three methods developed for computing vibrational thermal transport properties of nano-structured systems, namely Green function, quasi-classical Langevin, and Kubo-Green methods. The Green function methods are explained using both nonequilibrium expressions and the Landauer-type formula. The partitioning scheme, decimation techniques and surface Green functions are reviewed, and a simple model for reservoir Green functions is shown. The expressions for the Kubo-Greenwood method are derived, and Lanczos tridiagonalization, continued fraction and Chebyshev polynomial expansion methods are discussed. Additionally, the quasi-classical Langevin approach, which is useful for incorporating phonon-phonon and other scatterings is summarized. © 2019 IOP Publishing Ltd.

• Nonvolatile Memories Based on Graphene and Related 2D Materials

Bertolazzi S., Bondavalli P., Roche S., San T., Choi S.-Y., Colombo L., Bonaccorso F., Samorì P. Advanced Materials; 31 (10, 1806663) 2019. 10.1002/adma.201806663. IF: 25.809

The pervasiveness of information technologies is generating an impressive amount of data, which need to be accessed very quickly. Nonvolatile memories (NVMs) are making inroads into high-capacity storage to replace hard disk drives, fuelling the expansion of the global storage memory market. As silicon-based flash memories are approaching their fundamental limit, vertical stacking of multiple memory cell layers, innovative device concepts, and novel materials are being investigated. In this context, emerging 2D materials, such as graphene, transition metal dichalcogenides, and black phosphorous, offer a host of physical and chemical properties, which could both improve existing memory technologies and enable the next generation of low-cost, flexible, and wearable storage devices. Herein, an overview of graphene and related 2D materials (GRMs) in different types of NVM cells is provided, including resistive random-access, flash, magnetic and phase-change memories. The physical and chemical mechanisms underlying the switching of GRM-based memory devices studied in the last decade are discussed. Although at this stage most of the proof-of-concept devices investigated do not compete with state-of-the-art devices, a number of promising technological advancements have emerged. Here, the most relevant material properties and device structures are analyzed, emphasizing opportunities and challenges toward the realization of practical NVM devices. © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

• Probing the nanoscale origin of strain and doping in graphene-hBN heterostructures

Vincent T., Panchal V., Booth T., Power S.R., Jauho A.-P., Antonov V., Kazakova O. 2D Materials; 6 (1, 015022) 2019. 10.1088/2053-1583/aaf1dc. IF: 7.343

We use confocal Raman microscopy and a recently proposed vector analysis scheme to investigate the nanoscale origin of strain and carrier concentration in exfoliated graphene-hexagonal boron nitride (hBN) heterostructures on silicon dioxide (SiO2). Two types of heterostructures are studied: graphene on SiO2 partially covered by hBN, and graphene fully encapsulated between two hBN flakes. We extend the vector analysis method to produce separated spatial maps of the strain and doping variation across the heterostructures. This allows us to visualise and directly quantify the much-speculated effect of the environment on carrier concentration in graphene. Moreover, we demonstrate that variations in strain and carrier concentration in graphene arise from nanoscale features of the heterostructures such as fractures, folds and bubbles trapped between layers. For bubbles in hBN-encapsulated graphene, hydrostatic strain is shown to be greatest at bubble centres, whereas the maximum carrier concentration is localised at bubble edges. Raman spectroscopy is shown to be a non-invasive tool for probing strain and doping in graphene, which could prove useful for engineering of two-dimensional devices. © 2018 IOP Publishing Ltd.

• Room-Temperature Spin Hall Effect in Graphene/MoS 2 van der Waals Heterostructures

Safeer C.K., Ingla-Aynés J., Herling F., Garcia J.H., Vila M., Ontoso N., Calvo M.R., Roche S., Hueso L.E., Casanova F. Nano Letters; 2019. 10.1021/acs.nanolett.8b04368. IF: 12.279

Graphene is an excellent material for long-distance spin transport but allows little spin manipulation. Transition-metal dichalcogenides imprint their strong spin-orbit coupling into graphene via the proximity effect, and it has been predicted that efficient spin-to-charge conversion due to spin Hall and Rashba-Edelstein effects could be achieved. Here, by combining Hall probes with ferromagnetic electrodes, we unambiguously demonstrate experimentally the spin Hall effect in graphene induced by MoS 2 proximity and for varying temperatures up to room temperature. The fact that spin transport and the spin Hall effect occur in different parts of the same material gives rise to a hitherto unreported efficiency for the spin-to-charge voltage output. Additionally, for a single graphene/MoS 2 heterostructure-based device, we evidence a superimposed spin-to-charge current conversion that can be indistinguishably associated with either the proximity-induced Rashba-Edelstein effect in graphene or the spin Hall effect in MoS 2 . By a comparison of our results to theoretical calculations, the latter scenario is found to be the most plausible one. Our findings pave the way toward the combination of spin information transport and spin-to-charge conversion in two-dimensional materials, opening exciting opportunities in a variety of future spintronic applications. © 2019 American Chemical Society.

• The phase diagram of 2D antiferromagnets

Valenzuela S.O., Roche S. Nature Nanotechnology; 14 (12): 1088 - 1089. 2019. 10.1038/s41565-019-0592-x. IF: 33.407

[No abstract available]

• Tunable circular dichroism and valley polarization in the modified Haldane model

Vila M., Hung N.T., Roche S., Saito R. Physical Review B; 99 (16, 161404) 2019. 10.1103/PhysRevB.99.161404. IF: 3.736

We study the polarization dependence of optical absorption for a modified Haldane model, which exhibits antichiral edge modes in the presence of sample boundaries and has been argued to be realizable in transition metal dichalcogenides or Weyl semimetals. A rich optical phase diagram is unveiled, in which the correlations between perfect circular dichroism, pseudospin andvalley polarization can be tuned independently upon varying the Fermi energy. In particular, perfect circular dichroism and valley polarization are achieved simultaneously. This combination of optical properties suggests some interesting photonic device functionality (e.g., light polarizer) which could be combined with valleytronics applications (e.g., generation of valley currents). © 2019 American Physical Society.

• Universal Spin Diffusion Length in Polycrystalline Graphene

Cummings A.W., Dubois S.M.-M., Charlier J.-C., Roche S. Nano Letters; 19 (10): 7418 - 7426. 2019. 10.1021/acs.nanolett.9b03112. IF: 12.279

Graphene grown by chemical vapor deposition (CVD) is the most promising material for industrial-scale applications based on graphene monolayers. It also holds promise for spintronics; despite being polycrystalline, spin transport in CVD graphene has been measured over lengths up to 30 μm, which is on par with the best measurements made in single-crystal graphene. These results suggest that grain boundaries (GBs) in CVD graphene, while impeding charge transport, may have little effect on spin transport. However, to date very little is known about the true impact of disordered networks of GBs on spin relaxation. Here, by using first-principles simulations, we derive an effective tight-binding model of graphene GBs in the presence of spin-orbit coupling (SOC), which we then use to evaluate spin transport in realistic morphologies of polycrystalline graphene. The spin diffusion length is found to be independent of the grain size, and it is determined only by the strength of the substrate-induced SOC. This result is consistent with the D'yakonov-Perel' mechanism of spin relaxation in the diffusive regime, but we find that it also holds in the presence of quantum interference. These results clarify the role played by GBs and demonstrate that the average grain size does not dictate the upper limit for spin transport in CVD-grown graphene, a result of fundamental importance for optimizing large-scale graphene-based spintronic devices. Copyright © 2019 American Chemical Society.

### 2018

• 1D ferromagnetic edge contacts to 2D graphene/h-BN heterostructures

Karpiak B., Dankert A., Cummings A.W., Power S.R., Roche S., Dash S.P. 2D Materials; 5 (1, 014001) 2018. 10.1088/2053-1583/aa8d2b. IF: 7.042

We report the fabrication of one-dimensional (1D) ferromagnetic edge contacts to two-dimensional (2D) graphene/h-BN heterostructures. While aiming to study spin injection/detection with 1D edge contacts, a spurious magnetoresistance signal was observed, which is found to originate from the local Hall effect in graphene due to fringe fields from ferromagnetic edge contacts and in the presence of charge current spreading in the nonlocal measurement configuration. Such behavior has been confirmed by the absence of a Hanle signal and gate-dependent magnetoresistance measurements that reveal a change in sign of the signal for the electron- and hole-doped regimes, which is in contrast to the expected behavior of the spin signal. Calculations show that the contact-induced fringe fields are typically on the order of hundreds of mT, but can be reduced below 100 mT with careful optimization of the contact geometry. There may be an additional contribution from magnetoresistance effects due to tunneling anisotropy in the contacts, which needs further investigation. These studies are useful for optimization of spin injection and detection in 2D material heterostructures through 1D edge contacts. © 2017 IOP Publishing Ltd.

• A barrier to spin filters

Valenzuela S.O., Roche S. Nature Electronics; 1 (6): 328 - 329. 2018. 10.1038/s41928-018-0089-x.

Electron tunnelling through a two-dimensional magnetic insulator is assisted by magnon inelastic processes that provide spin-filtering. © 2018 The Author(s).

• Ballistic tracks in graphene nanoribbons

Aprojanz J., Power S.R., Bampoulis P., Roche S., Jauho A.-P., Zandvliet H.J.W., Zakharov A.A., Tegenkamp C. Nature Communications; 9 (1, 4426) 2018. 10.1038/s41467-018-06940-5. IF: 12.353

High quality graphene nanoribbons epitaxially grown on the sidewalls of silicon carbide (SiC) mesa structures stand as key building blocks for graphene-based nanoelectronics. Such ribbons display 1D single-channel ballistic transport at room temperature with exceptionally long mean free paths. Here, using spatially-resolved two-point probe (2PP) measurements, we selectively access and directly image a range of individual transport modes in sidewall ribbons. The signature of the independently contacted channels is a sequence of quantised conductance plateaus for different probe positions. These result from an interplay between edge magnetism and asymmetric terminations at opposite ribbon edges due to the underlying SiC structure morphology. Our findings demonstrate a precise control of transport through multiple, independent, ballistic tracks in graphene-based devices, opening intriguing pathways for quantum information device concepts. © 2018, The Author(s).

• Charge and spin transport anisotropy in nanopatterned graphene

Søren Schou Gregersen, Jose H Garcia, Antti-Pekka Jauho, Stephan Roche and Stephen R Power Journal of Physics: Materials; 1 (1) 2018. 10.1088/2515-7639/aadca3..

Anisotropic electronic transport is a possible route towards nanoscale circuitry design, particularly in two-dimensional materials. Proposals to introduce such a feature in patterned graphene have to date relied on large-scale structural inhomogeneities. Here we theoretically explore how a random, yet homogeneous, distribution of zigzag-edged triangular perforations can generate spatial anisotropies in both charge and spin transport. Anisotropic electronic transport is found to persist under considerable disordering of the perforation edges, suggesting its viability under realistic experimental conditions. Furthermore, controlling the relative orientation of perforations enables spin filtering of the transmitted electrons, resulting in a half-metallic anisotropic transport regime. Our findings point towards a co-integration of charge and spin control in a two-dimensional platform of relevance for nanocircuit design. We further highlight how geometrical effects allow finite samples to display finite transverse resistances, reminiscent of Spin Hall effects, in the absence of any bulk fingerprints of such mechanisms, and explore the underlying symmetries behind this behaviour.

• Conductance quantization suppression in the quantum Hall regime

Caridad J.M., Power S.R., Lotz M.R., Shylau A.A., Thomsen J.D., Gammelgaard L., Booth T.J., Jauho A.-P., Bøggild P. Nature Communications; 9 (1, 659) 2018. 10.1038/s41467-018-03064-8. IF: 12.353

Conductance quantization is the quintessential feature of electronic transport in non-interacting mesoscopic systems. This phenomenon is observed in quasi one-dimensional conductors at zero magnetic field B, and the formation of edge states at finite magnetic fields results in wider conductance plateaus within the quantum Hall regime. Electrostatic interactions can change this picture qualitatively. At finite B, screening mechanisms in narrow, gated ballistic conductors are predicted to give rise to an increase in conductance and a suppression of quantization due to the appearance of additional conduction channels. Despite being a universal effect, this regime has proven experimentally elusive because of difficulties in realizing one-dimensional systems with sufficiently hard-walled, disorder-free confinement. Here, we experimentally demonstrate the suppression of conductance quantization within the quantum Hall regime for graphene nanoconstrictions with low edge roughness. Our findings may have profound impact on fundamental studies of quantum transport in finite-size, two-dimensional crystals with low disorder. © 2018 The Author(s).

• Deciphering the origin of nonlocal resistance in multiterminalgraphene on hexagonal-boron-nitride withab initioquantumtransport: Fermi surface edge currents rather than Fermi seatopological valley currents

J M Marmolejo-Tejada, J H García, M D Petrovic, P-H Chang, X-L Sheng, A Cresti, P Plechác, S Roche and B K Nikolic Journal of Physics: Materials; 1 (1) 2018. 10.1088/2515-7639/aad585.

The recent observation (Gorbachev et al 2014 Science 346 448) of nonlocal resistance R NL near the Dirac point (DP) of multiterminal graphene on aligned hexagonal-boron nitride (G/hBN) has been interpreted as the consequence of topological valley Hall currents carried by the Fermi sea states just beneath the bulk gap E g induced by inversion symmetry breaking. However, the corresponding valley Hall conductivity ${\sigma }_{{xy}}^{v}$, quantized inside E g , is not directly measurable. Conversely, the Landauer–Büttiker formula, as a numerically exact approach to observable nonlocal transport quantities, yields R NL ≡ 0 for the same simplistic Hamiltonian of gapped graphene that generates ${\sigma }_{{xy}}^{v}\ne 0$ via the Kubo formula. We combine ab initio with quantum transport calculations to demonstrate that G/hBN wires with zigzag edges host dispersive edge states near the DP that are absent in theories based on the simplistic Hamiltonian. Although such edge states exist also in isolated zigzag graphene wires, aligned hBN is required to modify their energy–momentum dispersion and generate ${R}_{\mathrm{NL}}\ne 0$ near the DP. The Fermi surface-determined edge currents carrying the nonlocal signal persist also in the presence of edge disorder and over long distances. Concurrently, they resolve the long-standing puzzle of why the highly insulating state of G/hBN is rarely observed. Thus, we conclude that the observed R NL is unrelated to Fermi sea topological valley currents conjectured for gapped Dirac spectra.

• Effect of the channel length on the transport characteristics of transistors based on boron-doped graphene ribbons

Marconcini P., Cresti A., Roche S. Materials; 11 (5, 667) 2018. 10.3390/ma11050667. IF: 2.467

Substitutional boron doping of devices based on graphene ribbons gives rise to a unipolar behavior, a mobility gap, and an increase of the ION/IOFF ratio of the transistor. Here we study how this effect depends on the length of the doped channel. By means of self-consistent simulations based on a tight-binding description and a non-equilibrium Green's function approach, we demonstrate a promising increase of the ION/IOFF ratio with the length of the channel, as a consequence of the different transport regimes in the ON and OFF states. Therefore, the adoption of doped ribbons with longer aspect ratios could represent a significant step toward graphene-based transistors with an improved switching behavior. © 2018 by the authors.

• Finite-size correction scheme for supercell calculations in Dirac-point two-dimensional materials

Rocha C.G., Rocha A.R., Venezuela P., Garcia J.H., Ferreira M.S. Scientific Reports; 8 (1, 9348) 2018. 10.1038/s41598-018-27632-6. IF: 4.122

Modern electronic structure calculations are predominantly implemented within the super cell representation in which unit cells are periodically arranged in space. Even in the case of non-crystalline materials, defect-embedded unit cells are commonly used to describe doped structures. However, this type of computation becomes prohibitively demanding when convergence rates are sufficiently slow and may require calculations with very large unit cells. Here we show that a hitherto unexplored feature displayed by several 2D materials may be used to achieve convergence in formation- A nd adsorption-energy calculations with relatively small unit-cell sizes. The generality of our method is illustrated with Density Functional Theory calculations for different 2D hosts doped with different impurities, all of which providing accuracy levels that would otherwise require enormously large unit cells. This approach provides an efficient route to calculating the physical properties of 2D systems in general but is particularly suitable for Dirac-point materials doped with impurities that break their sublattice symmetry. © 2018 The Author(s).

• Large spin relaxation anisotropy and valley-Zeeman spin-orbit coupling in WSe2 /graphene/ h -BN heterostructures

Zihlmann S., Cummings A.W., Garcia J.H., Kedves M., Watanabe K., Taniguchi T., Schönenberger C., Makk P. Physical Review B; 97 (7, 075434) 2018. 10.1103/PhysRevB.97.075434. IF: 3.813

Large spin-orbital proximity effects have been predicted in graphene interfaced with a transition-metal dichalcogenide layer. Whereas clear evidence for an enhanced spin-orbit coupling has been found at large carrier densities, the type of spin-orbit coupling and its relaxation mechanism remained unknown. We show an increased spin-orbit coupling close to the charge neutrality point in graphene, where topological states are expected to appear. Single-layer graphene encapsulated between the transition-metal dichalcogenide WSe2 and h-BN is found to exhibit exceptional quality with mobilities as high as 1×105 cm2 V-1 s-1. At the same time clear weak antilocalization indicates strong spin-orbit coupling, and a large spin relaxation anisotropy due to the presence of a dominating symmetric spin-orbit coupling is found. Doping-dependent measurements show that the spin relaxation of the in-plane spins is largely dominated by a valley-Zeeman spin-orbit coupling and that the intrinsic spin-orbit coupling plays a minor role in spin relaxation. The strong spin-valley coupling opens new possibilities in exploring spin and valley degree of freedom in graphene with the realization of new concepts in spin manipulation. © 2018 American Physical Society.

• Proximity-induced spin-orbit coupling in graphene/ Bi1.5Sb0.5Te1.7Se1.3 heterostructures

Jafarpisheh S., Cummings A.W., Watanabe K., Taniguchi T., Beschoten B., Stampfer C. Physical Review B; 98 (24) 2018. 10.1103/PhysRevB.98.241402. IF: 3.813

The weak intrinsic spin-orbit coupling in graphene can be greatly enhanced by proximity coupling. Here, we report on the proximity-induced spin-orbit coupling in graphene transferred by hexagonal boron nitride (hBN) onto the topological insulator Bi1.5Sb0.5Te1.7Se1.3 (BSTS) which was grown on a hBN substrate by vapor solid synthesis. Phase coherent transport measurements, revealing weak localization, allow us to extract the carrier density-dependent phase coherence length lφ. While lφ increases with increasing carrier density in the hBN/graphene/hBN reference sample, it decreases in graphene/BSTS due to the proximity coupling of BSTS to graphene. The latter behavior results from D'yakonov-Perel'-type spin scattering in graphene with a large proximity-induced spin-orbit coupling strength of at least 2.5 meV. © 2018 American Physical Society.

• Quantum Hall effect in graphene with interface-induced spin-orbit coupling

Cysne T.P., Garcia J.H., Rocha A.R., Rappoport T.G. Physical Review B; 97 (8, 085413) 2018. 10.1103/PhysRevB.97.085413. IF: 3.813

We consider an effective model for graphene with interface-induced spin-orbit coupling and calculate the quantum Hall effect in the low-energy limit. We perform a systematic analysis of the contribution of the different terms of the effective Hamiltonian to the quantum Hall effect (QHE). By analyzing the spin splitting of the quantum Hall states as a function of magnetic field and gate voltage, we obtain different scaling laws that can be used to characterize the spin-orbit coupling in experiments. Furthermore, we employ a real-space quantum transport approach to calculate the quantum Hall conductivity and investigate the robustness of the QHE to disorder introduced by hydrogen impurities. For that purpose, we combine first-principles calculations and a genetic algorithm strategy to obtain a graphene-only Hamiltonian that models the impurity. © 2018 American Physical Society.

• Sensing ion channel in neuron networks with graphene field effect transistors

Veliev F., Cresti A., Kalita D., Bourrier A., Belloir T., Briançon-Marjollet A., Albrieux M., Roche S., Bouchiat V., Delacour C. 2D Materials; 5 (4, 045020) 2018. 10.1088/2053-1583/aad78f. IF: 7.042

Graphene, the atomically-thin honeycomb carbon lattice, is a highly conducting 2D material whose exposed electronic structure offers an ideal platform for chemical and biological sensing. Its biocompatible, flexible and chemically inert nature associated with the lack of dangling bonds, offers novel perspectives for direct interfacing with biological molecules. Combined with its exceptional electronic and optical properties, this promotes graphene as a unique platform for bioelectronics. Among the successful bio-integrations of graphene, the detection of action potentials in numerous electrogenic cells including neurons has paved the road for the high spatio-temporal and wide-field mapping of neuronal activity. Ultimate resolution of sensing ion channel activity can be achieved with neural interfaces, and it was shown that macroscale electrodes can record extracellular current of individual ion channels in model systems, by charging the quantum capacitance of large graphene monolayer (mm2). Here, we show the field effect detection of ion channel activity within neuron networks, cultured during several weeks above graphene transistor arrays. Dependences upon drugs, reference potential gating and device geometry confirm the field effect detection of individual ion channel and suggest a significant contribution of grain boundaries, which provide highly sensitive nanoscale-sized sensing sites. Our theoretical analysis and simulations demonstrate that the ion gating of a single grain boundary in liquid affects the electronic transmission of the whole transistor channel, resulting in significant conductance variations. Monitoring the ion channels activity is of great interest as most of neurodegenerative diseases relied on channelopathies, which rely on ion channel abnormal activity. Thus, such highly sensitive and biocompatible neuro-electronics which open the way to FET detection at the sub-cell precision should be useful for a wide range of fundamental and applied research areas, including brain-on-chip, pharmacology, and in vivo monitoring or diagnosis. © 2018 IOP Publishing Ltd.

• Shubnikov-de Haas oscillations in the anomalous Hall conductivity of Chern insulators

Canonico L.M., García J.H., Rappoport T.G., Ferreira A., Muniz R.B. Physical Review B; 98 (8, 085409) 2018. 10.1103/PhysRevB.98.085409. IF: 3.813

The Haldane model on a honeycomb lattice is a paradigmatic example of a system featuring quantized Hall conductivity in the absence of an external magnetic field, that is, a quantum anomalous Hall effect. Recent theoretical work predicted that the anomalous Hall conductivity of massive Dirac fermions can display Shubnikov-de Haas (SdH) oscillations, which could be observed in topological insulators and honeycomb layers with strong spin-orbit coupling. Here, we investigate the electronic transport properties of Chern insulators subject to high magnetic fields by means of accurate spectral expansions of lattice Green's functions. We find that the anomalous component of the Hall conductivity displays visible SdH oscillations at low temperature. The effect is shown to result from the modulation of the next-nearest-neighbor flux accumulation due to the Haldane term, which removes the electron-hole symmetry from the Landau spectrum. To support our numerical findings, we derive a long-wavelength description beyond the linear ("Dirac cone") approximation. Finally, we discuss the dependence of the energy spectra shift for reversed magnetic fields with the topological gap and the lattice bandwidth. © 2018 American Physical Society.

• Spin Proximity Effects in Graphene/Topological Insulator Heterostructures

Song K., Soriano D., Cummings A.W., Robles R., Ordejón P., Roche S. Nano Letters; 18 (3): 2033 - 2039. 2018. 10.1021/acs.nanolett.7b05482. IF: 12.080

Enhancing the spin-orbit interaction in graphene, via proximity effects with topological insulators, could create a novel 2D system that combines nontrivial spin textures with high electron mobility. To engineer practical spintronics applications with such graphene/topological insulator (Gr/TI) heterostructures, an understanding of the hybrid spin-dependent properties is essential. However, to date, despite the large number of experimental studies on Gr/TI heterostructures reporting a great variety of remarkable (spin) transport phenomena, little is known about the true nature of the spin texture of the interface states as well as their role on the measured properties. Here, we use ab initio simulations and tight-binding models to determine the precise spin texture of electronic states in graphene interfaced with a Bi2Se3 topological insulator. Our calculations predict the emergence of a giant spin lifetime anisotropy in the graphene layer, which should be a measurable hallmark of spin transport in Gr/TI heterostructures and suggest novel types of spin devices. © 2018 American Chemical Society.

• Spin transport in graphene/transition metal dichalcogenide heterostructures

Garcia J.H., Vila M., Cummings A.W., Roche S. Chemical Society Reviews; 47 (9): 3359 - 3379. 2018. 10.1039/c7cs00864c. IF: 40.182

Since its discovery, graphene has been a promising material for spintronics: its low spin-orbit coupling, negligible hyperfine interaction, and high electron mobility are obvious advantages for transporting spin information over long distances. However, such outstanding transport properties also limit the capability to engineer active spintronics, where strong spin-orbit coupling is crucial for creating and manipulating spin currents. To this end, transition metal dichalcogenides, which have larger spin-orbit coupling and good interface matching, appear to be highly complementary materials for enhancing the spin-dependent features of graphene while maintaining its superior charge transport properties. In this review, we present the theoretical framework and the experiments performed to detect and characterize the spin-orbit coupling and spin currents in graphene/transition metal dichalcogenide heterostructures. Specifically, we will concentrate on recent measurements of Hanle precession, weak antilocalization and the spin Hall effect, and provide a comprehensive theoretical description of the interconnection between these phenomena. © 2018 The Royal Society of Chemistry.

• Tailoring emergent spin phenomena in Dirac material heterostructures

Khokhriakov D., Cummings A.W., Song K., Vila M., Karpiak B., Dankert A., Roche S., Dash S.P. Science Advances; 4 (9, aat9349) 2018. 10.1126/sciadv.aat9349. IF: 11.511

Dirac materials such as graphene and topological insulators (TIs) are known to have unique electronic and spintronic properties. We combine graphene with TIs in van der Waals heterostructures to demonstrate the emergence of a strong proximity-induced spin-orbit coupling in graphene. By performing spin transport and precession measurements supported by ab initio simulations, we discover a strong tunability and suppression of the spin signal and spin lifetime due to the hybridization of graphene and TI electronic bands. The enhanced spin-orbit coupling strength is estimated to be nearly an order of magnitude higher than in pristine graphene. These findings in graphene-TI heterostructures could open interesting opportunities for exploring exotic physical phenomena and new device functionalities governed by topological proximity effects. Copyright © 2018 The Authors.

• Unequivocal signatures of the crossover to Anderson localization in realistic models of disordered quasi-one-dimensional materials

Lopez-Bezanilla A., Froufe-Pérez L.S., Roche S., Sáenz J.J. Physical Review B; 98 (23, 235423) 2018. 10.1103/PhysRevB.98.235423.

The only unequivocal known criterion for single-parameter scaling Anderson localization relies on the knowledge of the full conductance statistics. To date, theoretical studies have been restricted to model systems with symmetric scatterers, hence lacking universality. We present an in-depth statistical study of conductance distributions P(g), in disordered 'micrometer-long' carbon nanotubes using first principles simulations. In perfect agreement with the Dorokov-Mello-Pereyra-Kumar scaling equation, the computed P(g) exhibits a nontrivial, non-Gaussian, crossover to Anderson localization which could be directly compared with experiments. © 2018 American Physical Society.

### 2017

• A DETERMINISTIC APPROACH TO THE SYNCHRONIZATION OF NONLINEAR CELLULAR AUTOMATA

De Abreu J., García P., García J. Advances in Complex Systems; 20 (4-5, 1750006) 2017. 10.1142/S0219525917500060.

In this work, we introduce a deterministic scheme of synchronization of nonlinear cellular automata with chaotic behavior, connected through a master-slave coupling. By using a definition of Boolean derivative, we utilize the linear approximation of the cellular automata rules to design a deterministic and simple coupling function that ensures synchronization. Our results show that it is possible to synchronize nonlinear chaotic cellular automata using a deterministic coupling function that does not introduce into the slave all the information about the state of the master. © 2017 World Scientific Publishing Company.

• Electrical and Thermal Transport in Coplanar Polycrystalline Graphene-hBN Heterostructures

Barrios-Vargas J.E., Mortazavi B., Cummings A.W., Martinez-Gordillo R., Pruneda M., Colombo L., Rabczuk T., Roche S. Nano Letters; 17 (3): 1660 - 1664. 2017. 10.1021/acs.nanolett.6b04936. IF: 12.712

We present a theoretical study of electronic and thermal transport in polycrystalline heterostructures combining graphene (G) and hexagonal boron nitride (hBN) grains of varying size and distribution. By increasing the hBN grain density from a few percent to 100%, the system evolves from a good conductor to an insulator, with the mobility dropping by orders of magnitude and the sheet resistance reaching the MΩ regime. The Seebeck coefficient is suppressed above 40% mixing, while the thermal conductivity of polycrystalline hBN is found to be on the order of 30-120 Wm-1 K-1. These results, agreeing with available experimental data, provide guidelines for tuning G-hBN properties in the context of two-dimensional materials engineering. In particular, while we proved that both electrical and thermal properties are largely affected by morphological features (e.g., by the grain size and composition), we find in all cases that nanometer-sized polycrystalline G-hBN heterostructures are not good thermoelectric materials. © 2017 American Chemical Society.

• Electron trajectories and magnetotransport in nanopatterned graphene under commensurability conditions

Power S.R., Thomsen M.R., Jauho A.-P., Pedersen T.G. Physical Review B; 96 (7, 075425) 2017. 10.1103/PhysRevB.96.075425. IF: 3.836

Commensurability oscillations in the magnetotransport of periodically patterned systems, emerging from the interplay of cyclotron orbit and pattern periodicity, are a benchmark of mesoscopic physics in electron gas systems. Exploiting similar effects in two-dimensional materials would allow exceptional control of electron behavior, but it is hindered by the requirement to maintain ballistic transport over large length scales. Recent experiments have overcome this obstacle and observed distinct magnetoresistance commensurability peaks for perforated graphene sheets (antidot lattices). Interpreting the exact mechanisms behind these peaks is of key importance, particularly in graphene, where a range of regimes are accessible by varying the electron density. In this work, a fully atomistic, device-based simulation of magnetoresistance experiments allows us to analyze both the resistance peaks and the current flow at commensurability conditions. Magnetoresistance spectra are found in excellent agreement with experiment, but we show that a semiclassical analysis, in terms of simple skipping or pinned orbits, is insufficient to fully describe the corresponding electron trajectories. Instead, a generalized mechanism in terms of states bound to individual antidots, or to groups of antidots, is required. Commensurability features are shown to arise when scattering between such states is enhanced. The emergence and suppression of commensurability peaks is explored for different antidot sizes, magnetic field strengths, and electron densities. The insights gained from our study will guide the design and optimization of future experiments with nanostructured graphene. © 2017 American Physical Society.

• Giant Spin Lifetime Anisotropy in Graphene Induced by Proximity Effects

Cummings A.W., Garcia J.H., Fabian J., Roche S. Physical Review Letters; 119 (20, 206601) 2017. 10.1103/PhysRevLett.119.206601. IF: 8.462

We report on fundamental aspects of spin dynamics in heterostructures of graphene and transition metal dichalcogenides (TMDCs). By using realistic models derived from first principles we compute the spin lifetime anisotropy, defined as the ratio of lifetimes for spins pointing out of the graphene plane to those pointing in the plane. We find that the anisotropy can reach values of tens to hundreds, which is unprecedented for typical 2D systems with spin-orbit coupling and indicates a qualitatively new regime of spin relaxation. This behavior is mediated by spin-valley locking, which is strongly imprinted onto graphene by TMDCs. Our results indicate that this giant spin lifetime anisotropy can serve as an experimental signature of materials with strong spin-valley locking, including graphene-TMDC heterostructures and TMDCs themselves. Additionally, materials with giant spin lifetime anisotropy can provide an exciting platform for manipulating the valley and spin degrees of freedom, and for designing novel spintronic devices. © 2017 American Physical Society.

• Grain boundary-induced variability of charge transport in hydrogenated polycrystalline graphene

Vargas J.E.B., Falkenberg J.T., Soriano D., Cummings A.W., Brandbyge M., Roche S. 2D Materials; 4 (2, 025009) 2017. 10.1088/2053-1583/aa59de. IF: 6.937

Chemical functionalization has proven to be a promising means of tailoring the unique properties of graphene. For example, hydrogenation can yield a variety of interesting effects, including a metal-insulator transition or the formation of localized magnetic moments. Meanwhile, graphene grown by chemical vapor deposition is the most suitable for large-scale production, but the resulting material tends to be polycrystalline. Up to now there has been relatively little focus on how chemical functionalization, and hydrogenation in particular, impacts the properties of polycrystalline graphene. In this work, we use numerical simulations to study the electrical properties of hydrogenated polycrystalline graphene. We find a strong correlation between the spatial distribution of the hydrogen adsorbates and the charge transport properties. Charge transport is weakly sensitive to hydrogenation when adsorbates are confined to the grain boundaries, while a uniform distribution of hydrogen degrades the electronic mobility. This difference stems from the formation of the hydrogen-induced resonant impurity states, which are inhibited when the honeycomb symmetry is locally broken by the grain boundaries. These findings suggest a tunability of electrical transport of polycrystalline graphene through selective hydrogen functionalization, and also have implications for hydrogen-induced magnetization and spin lifetime of this material. © 2017 IOP Publishing Ltd.

• Growth of Twin-Free and Low-Doped Topological Insulators on BaF2(111)

Bonell F., Cuxart M.G., Song K., Robles R., Ordejón P., Roche S., Mugarza A., Valenzuela S.O. Crystal Growth and Design; 17 (9): 4655 - 4660. 2017. 10.1021/acs.cgd.7b00525. IF: 4.055

We demonstrate the growth of twin-free Bi2Te3 and Sb2Te3 topological insulators by molecular beam epitaxy and a sizable reduction of the twin density in Bi2Se3 on lattice-matched BaF2(111) substrates. Using X-ray diffraction, electron diffraction and atomic force microscopy, we systematically investigate the parameters influencing the formation of twin domains and the morphology of the films, and show that Se- and Te-based alloys differ by their growth mechanism. Optimum growth parameters are shown to result in intrinsically low-doped films, as probed by angle-resolved photoelectron spectroscopy. In contrast to previous approaches in which twin-free Bi2Se3 films are achieved by increasing the substrate roughness, the quality of our Bi2Te3 is superior on the flattest BaF2 substrates. This finding indicates that, during nucleation, the films not only interact with the topmost atomic substrate layer but also with buried layers that provide the necessary stacking information to promote a single twin, an observation that is supported by ab initio calculations. © 2017 American Chemical Society.

• Large edge magnetism in oxidized few-layer black phosphorus nanomeshes

Nakanishi Y., Ishi A., Ohata C., Soriano D., Iwaki R., Nomura K., Hasegawa M., Nakamura T., Katsumoto S., Roche S., Haruyama J. Nano Research; 10 (2): 718 - 728. 2017. 10.1007/s12274-016-1355-8. IF: 7.354

The formation and control of a room-temperature magnetic order in two-dimensional (2D) materials is a challenging quest for the advent of innovative magnetic- and spintronic-based technologies. To date, edge magnetism in 2D materials has been experimentally observed in hydrogen (H)-terminated graphene nanoribbons (GNRs) and graphene nanomeshes (GNMs), but the measured magnetization remains far too small to allow envisioning practical applications. Herein, we report experimental evidences of large room-temperature edge ferromagnetism (FM) obtained from oxygen (O)-terminated zigzag pore edges of few-layer black phosphorus (P) nanomeshes (BPNMs). The magnetization values per unit area are ~100 times larger than those reported for H-terminated GNMs, while the magnetism is absent for H-terminated BPNMs. The magnetization measurements and the first-principles simulations suggest that the origin of such a magnetic order could stem from ferromagnetic spin coupling between edge P with O atoms, resulting in a strong spin localization at the edge valence band, and from uniform oxidation of full pore edges over a large area and interlayer spin interaction. Our findings pave the way for realizing high-efficiency 2D flexible magnetic and spintronic devices without the use of rare magnetic elements. [Figure not available: see fulltext.] © 2017, Tsinghua University Press and Springer-Verlag Berlin Heidelberg.

• Nanostructured graphene for spintronics

Gregersen Sø.S., Power S.R., Jauho A.-P. Physical Review B; 95 (12, 121406) 2017. 10.1103/PhysRevB.95.121406. IF: 3.836

Zigzag edges of the honeycomb structure of graphene exhibit magnetic polarization, making them attractive as building blocks for spintronic devices. Here, we show that devices with zigzag-edged triangular antidots perform essential spintronic functionalities, such as spatial spin splitting or spin filtering of unpolarized incoming currents. Near-perfect performance can be obtained with optimized structures. The device performance is robust against substantial disorder. The gate-voltage dependence of transverse resistance is qualitatively different for spin-polarized and spin-unpolarized devices, and can be used as a diagnostic tool. Importantly, the suggested devices are feasible within current technologies. © 2017 American Physical Society.

• Record Low Thermal Conductivity of Polycrystalline MoS2 Films: Tuning the Thermal Conductivity by Grain Orientation

Sledzinska M., Quey R., Mortazavi B., Graczykowski B., Placidi M., Saleta Reig D., Navarro-Urrios D., Alzina F., Colombo L., Roche S., Sotomayor Torres C.M. ACS Applied Materials and Interfaces; 9 (43): 37905 - 37911. 2017. 10.1021/acsami.7b08811. IF: 7.504

We report a record low thermal conductivity in polycrystalline MoS2 obtained for ultrathin films with varying grain sizes and orientations. By optimizing the sulfurization parameters of nanometer-thick Mo layers, five MoS2 films containing a combination of horizontally and vertically oriented grains, with respect to the bulk (001) monocrystal, were grown. From transmission electron microscopy, the average grain size, typically below 10 nm, and proportion of differently oriented grains were extracted. The thermal conductivity of the suspended samples was extracted from a Raman laser-power-dependent study, and the lowest value of thermal conductivity of 0.27 W m-1 K-1, which reaches a similar value as that of Teflon, is obtained in a polycrystalline sample formed by a combination of horizontally and vertically oriented grains in similar proportion. Analysis by means of molecular dynamics and finite element method simulations confirm that such a grain arrangement leads to lower grain boundary conductance. We discuss the possible use of these thermal insulating films in the context of electronics and thermoelectricity. © 2017 American Chemical Society.

• Scale-invariant large nonlocality in polycrystalline graphene

Ribeiro M., Power S.R., Roche S., Hueso L.E., Casanova F. Nature Communications; 8 (1, 2198) 2017. 10.1038/s41467-017-02346-x. IF: 12.124

The observation of large nonlocal resistances near the Dirac point in graphene has been related to a variety of intrinsic Hall effects, where the spin or valley degrees of freedom are controlled by symmetry breaking mechanisms. Engineering strong spin or valley Hall signals on scalable graphene devices could stimulate further practical developments of spin- and valleytronics. Here we report on scale-invariant nonlocal transport in large-scale chemical vapor deposition graphene under an applied external magnetic field. Contrary to previously reported Zeeman spin Hall effect, our results are explained by field-induced spin-filtered edge states whose sensitivity to grain boundaries manifests in the nonlocal resistance. This phenomenon, related to the emergence of the quantum Hall regime, persists up to the millimeter scale, showing that polycrystalline morphology can be imprinted in nonlocal transport. This suggests that topological Hall effects in large-scale graphene materials are highly sensitive to the underlying structural morphology, limiting practical realizations. © 2017 The Author(s).

• Scaling properties of polycrystalline graphene: A review

Isacsson A., Cummings A.W., Colombo L., Colombo L., Kinaret J.M., Roche S. 2D Materials; 4 (1, 012002) 2017. 10.1088/2053-1583/aa5147. IF: 6.937

We present an overview of the electrical, mechanical, and thermal properties of polycrystalline graphene. Most global properties of this material, such as the charge mobility, thermal conductivity, or Young's modulus, are sensitive to its microstructure, for instance the grain size and the presence of line or point defects. Both the local and global features of polycrystalline graphene have been investigated by a variety of simulations and experimental measurements. In this review, we summarize the properties of polycrystalline graphene, and by establishing a perspective on how the microstructure impacts its large-scale physical properties, we aim to provide guidance for further optimization and improvement of applications based on this material, such as flexible and wearable electronics, and high-frequency or spintronic devices. © 2016 IOP Publishing Ltd.

• Spin hall effect and weak antilocalization in graphene/transition metal dichalcogenide heterostructures

Garcia J.H., Cummings A.W., Roche S. Nano Letters; 17 (8): 5078 - 5083. 2017. 10.1021/acs.nanolett.7b02364. IF: 12.712

We report on a theoretical study of the spin Hall Effect (SHE) and weak antilocalization (WAL) in graphene/transition metal dichalcogenide (TMDC) heterostructures, computed through efficient real-space quantum transport methods, and using realistic tight-binding models parametrized from ab initio calculations. The graphene/WS2 system is found to maximize spin proximity effects compared to graphene on MoS2, WSe2, or MoSe2 with a crucial role played by disorder, given the disappearance of SHE signals in the presence of strong intervalley scattering. Notably, we found that stronger WAL effects are concomitant with weaker charge-to-spin conversion efficiency. For further experimental studies of graphene/TMDC heterostructures, our findings provide guidelines for reaching the upper limit of spin current formation and for fully harvesting the potential of two-dimensional materials for spintronic applications. © 2017 American Chemical Society.

• Spin precession in anisotropic media

Raes B., Cummings A.W., Bonell F., Costache M.V., Sierra J.F., Roche S., Valenzuela S.O. Physical Review B; 95 (8, 085403) 2017. 10.1103/PhysRevB.95.085403. IF: 3.836

We generalize the diffusive model for spin injection and detection in nonlocal spin structures to account for spin precession under an applied magnetic field in an anisotropic medium, for which the spin lifetime is not unique and depends on the spin orientation. We demonstrate that the spin precession (Hanle) line shape is strongly dependent on the degree of anisotropy and on the orientation of the magnetic field. In particular, we show that the anisotropy of the spin lifetime can be extracted from the measured spin signal, after dephasing in an oblique magnetic field, by using an analytical formula with a single fitting parameter. Alternatively, after identifying the fingerprints associated with the anisotropy, we propose a simple scaling of the Hanle line shapes at specific magnetic field orientations that results in a universal curve only in the isotropic case. The deviation from the universal curve can be used as a complementary means of quantifying the anisotropy by direct comparison with the solution of our generalized model. Finally, we applied our model to graphene devices and find that the spin relaxation for graphene on silicon oxide is isotropic within our experimental resolution. © 2017 American Physical Society.

• Tailoring magnetic insulator proximity effects in graphene: First-principles calculations

Hallal A., Ibrahim F., Yang H., Roche S., Chshiev M. 2D Materials; 4 (2, 025074) 2017. 10.1088/2053-1583/aa6663. IF: 6.937

We report a systematic first-principles investigation of the influence of different magnetic insulators on the magnetic proximity effect induced in graphene. Four different magnetic insulators are considered: two ferromagnetic europium chalcogenides namely EuO and EuS and two ferrimagnetic insulators yttrium iron garnet (YIG) and cobalt ferrite (CFO). The obtained exchange-splitting in graphene varies from tens to hundreds of meV depending on substrates. We find an electron doping to graphene induced by YIG and europium chalcogenides substrates, that shift the Fermi level above the Dirac cone up to 0.78 eV and 1.3 eV respectively, whereas hole doping shifts the Fermi level down below the Dirac cone about 0.5 eV in graphene/CFO. Furthermore, we study the variation of the extracted exchange and tight-binding parameters as a function of the EuO and EuS thicknesses. We show that those parameters are robust to thickness variation such that a single monolayer of magnetic insulator can induce a strong magnetic proximity effect on graphene. Those findings pave the way towards possible engineering of graphene spin-gating by proximity effect especially in view of recent experimental advancements. © 2017 IOP Publishing Ltd.

• Valley-polarized quantum transport generated by gauge fields in graphene

Settnes M., Garcia J.H., Roche S. 2D Materials; 4 (3, 031006) 2017. 10.1088/2053-1583/aa7cbd. IF: 6.937

We report on the possibility to simultaneously generate in graphene a bulk valley-polarized dissipative transport and a quantum valley Hall effect by combining strain-induced gauge fields and real magnetic fields. Such unique phenomenon results from a ‘resonance/anti-resonance’ effect driven by the superposition/cancellation of superimposed gauge fields which differently affect time reversal symmetry. The onset of a valley-polarized Hall current concomitant to a dissipative valley-polarized current flow in the opposite valley is revealed by a e2 /h Hall conductivity plateau. We employ efficient linear scaling Kubo transport methods combined with a valley projection scheme to access valley-dependent conductivities and show that the results are robust against disorder.

### 2016

• Anomalous ballistic transport in disordered bilayer graphene: A Dirac semimetal induced by dimer vacancies

Van Tuan D., Roche S. Physical Review B; 93 (4, 041403) 2016. 10.1103/PhysRevB.93.041403.

We report anomalous quantum transport features in bilayer graphene in the presence of a random distribution of structural vacancies. By using an efficient real-space Kubo-Greenwood transport methodology, the impact of a varying density of dimer versus nondimer vacancies is investigated in very large scale disordered models. While nondimer vacancies are shown to induce localization regimes, dimer vacancies result in an unexpected ballistic regime whose energy window surprisingly enlarges with increasing impurity density. Such counterintuitive phenomenon is explained by the formation of an effective linear dispersion in the bilayer band structure, which roots in the symmetry breaking effects driven by dimer vacancies, and provides a realization of Dirac semimetals in high dimension. © 2016 American Physical Society.

• Charge, spin and valley Hall effects in disordered grapheme

Cresti A., Nikolíc B.K., Garćia J.H., Roche S. Rivista del Nuovo Cimento; 39 (12): 587 - 667. 2016. 10.1393/ncr/i2016-10130-6. IF: 1.250

The discovery of the integer quantum Hall effect in the early eighties of the last century, with highly precise quantization values for the Hall conductance in multiples of e2/h, has been the first fascinating manifestation of the topological state of matter driven by magnetic field and disorder, and related to the formation of non-dissipative current flow. Throughout the 2000's, several new phenomena such as the spin Hall effect and the quantum spin Hall effect were confirmed experimentally for systems with strong spin-orbit coupling effects and in the absence of external magnetic field. More recently, the Zeeman spin Hall effect and the formation of valley Hall topological currents have been introduced for graphene-based systems, under time-reversal or inversion symmetry-breaking conditions, respectively. This review presents a comprehensive coverage of all these Hall effects in disordered graphene from the perspective of numerical simulations of quantum transport in two-dimensional bulk systems (by means of the Kubo formalism) and multiterminal nanostructures (by means of the Landauer-Buttiker scattering and non-equilibrium Green's function approaches). In contrast to usual two-dimensional electron gases in semiconductor heterostructures, the presence of defects in graphene generates more complex electronic features such as electron-hole asymmetry, defect-induced resonances in the electron density of states or percolation effect between localized impurity states, which, together with extra degrees of freedom (sublattice pseudospin and valley isospin), bring a higher degree of complexity and enlarge the transport phase diagram.

• Effects of Dephasing on Spin Lifetime in Ballistic Spin-Orbit Materials

Cummings A.W., Roche S. Physical Review Letters; 116 (8, 086602) 2016. 10.1103/PhysRevLett.116.086602. IF: 7.645

We theoretically investigate spin dynamics in spin-orbit-coupled materials. In the ballistic limit, the spin lifetime is dictated by dephasing that arises from energy broadening plus a nonuniform spin precession. For the case of clean graphene, we find a strong anisotropy with spin lifetimes that can be short even for modest energy scales, on the order of a few ns. These results offer deeper insight into the nature of spin dynamics in graphene, and are also applicable to the investigation of other systems where spin-orbit coupling plays an important role. © 2016 American Physical Society.

• Gate-tunable atomically thin lateral MoS2 Schottky junction patterned by electron beam

Katagiri Y., Nakamura T., Ishii A., Ohata C., Hasegawa M., Katsumoto S., Cusati T., Fortunelli A., Iannaccone G., Fiori G., Roche S., Haruyama J. Nano Letters; 16 (6): 3788 - 3794. 2016. 10.1021/acs.nanolett.6b01186. IF: 13.779

Among atomically thin two-dimensional (2D) materials, molybdenum disulfide (MoS2) is attracting considerable attention because of its direct bandgap in the 2H-semiconducting phase. On the other hand, a 1T-metallic phase has been revealed, bringing complementary application. Recently, thanks to top-down fabrication using electron beam (EB) irradiation techniques, in-plane 1T-metal/2H-semiconductor lateral (Schottky) MoS2 junctions were demonstrated, opening a path toward the co-integration of active and passive two-dimensional devices. Here, we report the first transport measurements evidencing the formation of a MoS2 Schottky barrier (SB) junction with barrier height of 0.13-0.18 eV created at the interface between EB-irradiated (1T)/nonirradiated (2H) regions. Our experimental findings, supported by state-of-the-art simulation, reveal unique device fingerprint of SB-based field-effect transistors made from atom-thin 1T layers. © 2016 American Chemical Society.

• How disorder affects topological surface states in the limit of ultrathin Bi2Se3 films

Song K., Soriano D., Robles R., Ordejon P., Roche S. 2D Materials; 3 (4, 045007) 2016. 10.1088/2053-1583/3/4/045007. IF: 9.611

We present a first-principles study of electronic properties of ultrathin films of topological insulators (TIs) and scrutinize the role of disorder on the robustness of topological surface states, which can be analysed through their spin textures. The presence of twin grain boundaries is found to increase the band gap of the film, while preserving the spin texture of states in first conduction and valence bands. Differently, partial hydrogenation of one surface not only results in some self-doping effect, but also provokes some alteration of the spin texture symmetry of the electronic states. The formation of a new Dirac cone at M-point of the Brillouin zone of the hydrogenated surface, together with a modified spin texture characteristics are consistent with a dominant Dresselhaus spin-orbit interaction type, more usually observed in 3D materials. Our findings indicate that defects can either be detrimental or beneficial for exploring spin transport of surface states in the limit of ultrathin films of TIs, which maximizes surface over bulk phenomena. © 2016 IOP Publishing Ltd.

• Localized electronic states at grain boundaries on the surface of graphene and graphite

Luican-Mayer A., Barrios-Vargas J.E., Falkenberg J.T., Autès G., Cummings A.W., Soriano D., Li G., Brandbyge M., Yazyev O.V., Roche S., Yandrei E. 2D Materials; 3 (3, 031005) 2016. 10.1088/2053-1583/3/3/031005. IF: 9.611

Recent advances in large-scale synthesis of graphene and other 2D materials have underscored the importance of local defects such as dislocations and grain boundaries (GBs), and especially their tendency to alter the electronic properties of the material. Understanding how the polycrystalline morphology affects the electronic properties is crucial for the development of applications such as flexible electronics, energy harvesting devices or sensors.Wehere report on atomic scale characterization of several GBs and on the structural-dependence of the localized electronic states in their vicinity. Using low temperature scanning tunneling microscopy"Q and spectroscopy, together with tight binding and ab initio numerical simulations we explore GBs on the surface of graphite and elucidate the interconnection between the local density of states and their atomic structure.Weshow that the electronic fingerprints of these GBs consist of pronounced resonances which, depending on the relative orientation of the adjacent crystallites, appear either on the electron side of the spectrum or as an electron-hole symmetric doublet close to the charge neutrality point. These two types of spectral features will impact very differently the transport properties allowing, in the asymmetric case to introduce transport anisotropy which could be utilized to design novel growth and fabrication strategies to control device performance. © 2016 IOP Publishing Ltd.

• Near-field photocurrent nanoscopy on bare and encapsulated graphene

Woessner A., Alonso-González P., Lundeberg M.B., Gao Y., Barrios-Vargas J.E., Navickaite G., Ma Q., Janner D., Watanabe K., Cummings A.W., Taniguchi T., Pruneri V., Roche S., Jarillo-Herrero P., Hone J., Hillenbrand R., Koppens F.H.L. Nature Communications; 7 ( 10783) 2016. 10.1038/ncomms10783. IF: 11.329

Optoelectronic devices utilizing graphene have demonstrated unique capabilities and performances beyond state-of-the-art technologies. However, requirements in terms of device quality and uniformity are demanding. A major roadblock towards high-performance devices are nanoscale variations of the graphene device properties, impacting their macroscopic behaviour. Here we present and apply non-invasive optoelectronic nanoscopy to measure the optical and electronic properties of graphene devices locally. This is achieved by combining scanning near-field infrared nanoscopy with electrical read-out, allowing infrared photocurrent mapping at length scales of tens of nanometres. Using this technique, we study the impact of edges and grain boundaries on the spatial carrier density profiles and local thermoelectric properties. Moreover, we show that the technique can readily be applied to encapsulated graphene devices. We observe charge build-up near the edges and demonstrate a solution to this issue.

• Quantum transport in graphene in presence of strain-induced pseudo-Landau levels

Settnes M., Leconte N., Barrios-Vargas J.E., Jauho A.-P., Roche S. 2D Materials; 3 (3, 034005) 2016. 10.1088/2053-1583/3/3/034005. IF: 9.611

Wereport on mesoscopic transport fingerprints in disordered graphene caused by strain-field induced pseudomagnetic Landau levels (pLLs). Efficient numerical real space calculations of the Kubo formula are performed for an ordered network of nanobubbles in graphene, creating pseudomagnetic fields up to several hundreds of Tesla, values inaccessible by real magnetic fields. Strain-induced pLLs yield enhanced scattering effects across the energy spectrum resulting in lower mean free path and enhanced localization effects. In the vicinity of the zeroth order pLL, we demonstrate an anomalous transport regime, where the mean free paths increases with disorder.Weattribute this puzzling behavior to the low-energy sub-lattice polarization induced by the zeroth order pLL, which is unique to pseudomagnetic fields preserving time-reversal symmetry. These results, combined with the experimental feasibility of reversible deformation fields, open the way to tailor a metal-insulator transition driven by pseudomagnetic fields. © 2016 IOP Publishing Ltd.

• Spin dynamics and relaxation in graphene dictated by electron-hole puddles

Van Tuan D., Ortmann F., Cummings A.W., Soriano D., Roche S. Scientific Reports; 6 ( 21046) 2016. 10.1038/srep21046. IF: 5.228

The understanding of spin dynamics and relaxation mechanisms in clean graphene, and the upper time and length scales on which spin devices can operate, are prerequisites to realizing graphene-based spintronic technologies. Here we theoretically reveal the nature of fundamental spin relaxation mechanisms in clean graphene on different substrates with Rashba spin-orbit fields as low as a few tens of μeV. Spin lifetimes ranging from 50 picoseconds up to several nanoseconds are found to be dictated by substrate-induced electron-hole characteristics. A crossover in the spin relaxation mechanism from a Dyakonov-Perel type for SiO2 substrates to a broadening-induced dephasing for hBN substrates is described. The energy dependence of spin lifetimes, their ratio for spins pointing out-of-plane and in-plane, and the scaling with disorder provide a global picture about spin dynamics and relaxation in ultraclean graphene in the presence of electron-hole puddles. © 2016, Nature Publishing Group. All rights reserved.

• Spin dynamics in bilayer graphene: Role of electron-hole puddles and Dyakonov-Perel mechanism

Van Tuan D., Adam S., Roche S. Physical Review B; 94 (4, 041405) 2016. 10.1103/PhysRevB.94.041405.

We report on spin transport features which are unique to high quality bilayer graphene, in the absence of magnetic contaminants and strong intervalley mixing. The time-dependent spin polarization of a propagating wave packet is computed using an efficient quantum transport method. In the limit of vanishing effects of substrate and disorder, the energy dependence of the spin lifetime is similar to monolayer graphene with an M-shaped profile and minimum value at the charge neutrality point, but with an electron-hole asymmetry fingerprint. In sharp contrast, the incorporation of substrate-induced electron-hole puddles (characteristics of supported graphene either on SiO2 or hBN) surprisingly results in a large enhancement of the low-energy spin lifetime and a lowering of its high-energy values. Such a feature, unique to the bilayer, is explained in terms of a reinforced Dyakonov-Perel mechanism at the Dirac point, whereas spin relaxation at higher energies is driven by pure dephasing effects. This suggests further electrostatic control of the spin transport length scales in graphene devices. © 2016 American Physical Society.

• Spin Hall Effect and Origins of Nonlocal Resistance in Adatom-Decorated Graphene

Van Tuan D., Marmolejo-Tejada J.M., Waintal X., Nikolić B.K., Valenzuela S.O., Roche S. Physical Review Letters; 117 (17, 176602) 2016. 10.1103/PhysRevLett.117.176602. IF: 7.645

Recent experiments reporting an unexpectedly large spin Hall effect (SHE) in graphene decorated with adatoms have raised a fierce controversy. We apply numerically exact Kubo and Landauer-Büttiker formulas to realistic models of gold-decorated disordered graphene (including adatom clustering) to obtain the spin Hall conductivity and spin Hall angle, as well as the nonlocal resistance as a quantity accessible to experiments. Large spin Hall angles of ∼0.1 are obtained at zero temperature, but their dependence on adatom clustering differs from the predictions of semiclassical transport theories. Furthermore, we find multiple background contributions to the nonlocal resistance, some of which are unrelated to the SHE or any other spin-dependent origin, as well as a strong suppression of the SHE at room temperature. This motivates us to design a multiterminal graphene geometry which suppresses these background contributions and could, therefore, quantify the upper limit for spin-current generation in two-dimensional materials. © 2016 American Physical Society.

• Spin Manipulation in Graphene by Chemically Induced Pseudospin Polarization

Van Tuan D., Roche S. Physical Review Letters; 116 (10, 106601) 2016. 10.1103/PhysRevLett.116.106601. IF: 7.645

Spin manipulation is one of the most critical challenges to realize spin-based logic devices and spintronic circuits. Graphene has been heralded as an ideal material to achieve spin manipulation, but so far new paradigms and demonstrators are limited. Here we show that certain impurities such as fluorine adatoms, which locally break sublattice symmetry without the formation of strong magnetic moment, could result in a remarkable variability of spin transport characteristics. The impurity resonance level is found to be associated with a long-range sublattice pseudospin polarization, which by locally decoupling spin and pseudospin dynamics provokes a huge spin lifetime electron-hole asymmetry. In the dilute impurity limit, spin lifetimes could be tuned electrostatically from 100 ps to several nanoseconds, providing a protocol to chemically engineer an unprecedented spin device functionality. © 2016 American Physical Society.

• Thermal conductivity of MoS2 polycrystalline nanomembranes

Sledzinska M., Graczykowski B., Placidi M., Reig D.S., El Sachat A., Reparaz J.S., Alzina F., Mortazavi B., Quey R., Colombo L., Roche S., Torres C.M.S. 2D Materials; 3 (3, 035016) 2016. 10.1088/2053-1583/3/3/035016. IF: 9.611

Heat conduction in 2D materials can be effectively engineered by means of controlling nanoscale grain structure. Afavorable thermal performance makes these structures excellent candidates for integrated heat management units. Here we show combined experimental and theoretical studies for MoS2 nanosheets in a nanoscale grain-size limit.Wereport thermal conductivity measurements on 5 nm thick polycrystalline MoS2 by means of 2-laser Raman thermometry. The free-standing, drum-like MoS2 nanomembranes were fabricated using a novel polymer- and residue-free, wet transfer, in which we took advantage of the difference in the surface energies between MoS2 and the growth substrate to transfer the CVD-grown nanosheets. The measurements revealed a strong reduction in the in-plane thermal conductivity down to about 0.73 ± 0.25 W m-1 K-1. The results are discussed theoretically using finite elements method simulations for a polycrystalline film, and a scaling trend of the thermally conductivity with grain size is proposed. © 2016 IOP Publishing Ltd.

• Unconventional features in the quantum Hall regime of disordered graphene: Percolating impurity states and Hall conductance quantization

Leconte N., Ortmann F., Cresti A., Roche S. Physical Review B; 93 (11, 115404) 2016. 10.1103/PhysRevB.93.115404.

We report on the formation of critical states in disordered graphene, at the origin of variable and unconventional transport properties in the quantum Hall regime, such as a zero-energy Hall conductance plateau in the absence of an energy band gap and Landau-level degeneracy breaking. By using efficient real-space transport methodologies, we compute both the dissipative and Hall conductivities of large-size graphene sheets with random distribution of model single and double vacancies. By analyzing the scaling of transport coefficients with defect density, system size, and magnetic length, we elucidate the origin of anomalous quantum Hall features as magnetic-field-dependent impurity states, which percolate at some critical energies. These findings shed light on unidentified states and quantum-transport anomalies reported experimentally. © 2016 American Physical Society.

### 2015

• Efficient linear scaling approach for computing the Kubo Hall conductivity

Ortmann F., Leconte N., Roche S. Physical Review B - Condensed Matter and Materials Physics; 91 (16, 165117) 2015. 10.1103/PhysRevB.91.165117. IF: 3.736

We report an order-N approach to compute the Kubo Hall conductivity for disorderd two-dimensional systems reaching tens of millions of orbitals, and realistic values of the applied external magnetic fields (as low as a few Tesla). A time-evolution scheme is employed to evaluate the Hall conductivity σxy using a wave-packet propagation method and a continued fraction expansion for the computation of diagonal and off-diagonal matrix elements of the Green functions. The validity of the method is demonstrated by comparison of results with brute-force diagonalization of the Kubo formula, using (disordered) graphene as the system of study. This approach to mesoscopic system sizes is opening an unprecedented perspective for so-called reverse engineering in which the available experimental transport data are used to get a deeper understanding of the microscopic structure of the samples. Besides, this will not only allow addressing subtle issues in terms of resistance standardization of large-scale materials (such as wafer scale polycrystalline graphene), but will also enable the discovery of new quantum transport phenomena in complex two-dimensional materials, out of reach with classical methods. © 2015 American Physical Society.

• Graphene spintronics: The European Flagship perspective

Roche S., Åkerman J., Beschoten B., Charlier J.-C., Chshiev M., Dash S.P., Dlubak B., Fabian J., Fert A., Guimarães M., Guinea F., Grigorieva I., Schönenberger C., Seneor P., Stampfer C., Valenzuela S.O., Waintal X., Van Wees B. 2D Materials; 2 (3, 030202) 2015. 10.1088/2053-1583/2/3/030202. IF: 0.000

Wereview current challenges and perspectives in graphene spintronics, which is one of themost promising directions of innovation, given its room-temperature long-spin lifetimes and the ability of graphene to be easily interfaced with other classes ofmaterials (ferromagnets, magnetic insulators, semiconductors, oxides, etc), allowing proximity effects to be harvested. The general context of spintronics is first discussed togetherwith open issues and recent advances achieved by theGraphene SpintronicsWork Package consortiumwithin theGraphene Flagship project. Based on such progress, which establishes the state of the art, several novel opportunities for spinmanipulation such as the generation of pure spin current (through spinHall effect) and the control of magnetization through the spin torque phenomena appear on the horizon. Practical applications arewithin reach, but will require the demonstration of wafer-scale graphene device integration, and the realization of functional prototypes employed for determined applications such as magnetic sensors or nano-oscillators. This is a specially commissioned editorial from the Graphene Flagship Work Package on Spintronics. This editorial is part of the 2DMaterials focus collection on 'Progress on the science and applications of twodimensionalmaterials,' published in association with theGraphene Flagship. It provides an overviewof key recent advances of the spintronicswork package aswell as the mid-term objectives of the consortium. © 2015 IOP Publishing Ltd.

• Role of grain boundaries in tailoring electronic properties of polycrystalline graphene by chemical functionalization

Seifert M., Vargas J.E.B., Bobinger M., Sachsenhauser M., Cummings A.W., Roche S., Garrido J.A. 2D Materials; 2 (2, 024008) 2015. 10.1088/2053-1583/2/2/024008. IF: 0.000

Grain boundaries, inevitably present in chemical vapor deposited graphene, are expected to have considerable impact on the development of graphene-based hybrid materials with tailored material properties.Wedemonstrate here the critical role of polycrystallinity on the chemical functionalization of graphene comparing ozone-induced oxidation with remote plasma hydrogenation.Weshow that graphene oxidation and hydrogenation occur in two consecutive stages upon increasing defect density: an initial step in which surface-bound functional groups are generated, followed by the creation of vacancies. Remarkably, we find that hydrogenation yields homogeneously distributed defects while ozone-induced defects are preferentially accumulated at the grain boundaries eventually provoking local cracking of the structure. Supported by quantum simulations, our experimental findings reveal distinct electronic transport regimes depending on the density and distribution of induced defects on the polycrystalline graphene films. Our findings highlight the key role played by grain boundaries during graphene functionalization, and at the same time provide a novel perspective to tailor the properties of polycrystalline graphene. © 2015 IOP Publishing Ltd.

• Science and technology roadmap for graphene, related two-dimensional crystals, and hybrid systems

Ferrari A.C., Bonaccorso F., Fal'ko V., Novoselov K.S., Roche S., Bøggild P., Borini S., Koppens F.H.L., Palermo V., Pugno N., Garrido J.A., Sordan R., Bianco A., Ballerini L., Prato M., Lidorikis E., Kivioja J., Marinelli C., Ryhänen T., Morpurgo A., Coleman J.N., Nicolosi V., Colombo L., Fert A., Garcia-Hernandez M., Bachtold A., Schneider G.F., Guinea F., Dekker C., Barbone M., Sun Z., Galiotis C., Grigorenko A.N., Konstantatos G., Kis A., Katsnelson M., Vandersypen L., Loiseau A., Morandi V., Neumaier D., Treossi E., Pellegrini V., Polini M., Tredicucci A., Williams G.M., Hee Hong B., Ahn J.-H., Min Kim J., Zirath H., Van Wees B.J., Van Der Zant H., Occhipinti L., Di Matteo A., Kinloch I.A., Seyller T., Quesnel E., Feng X., Teo K., Rupesinghe N., Hakonen P., Neil S.R.T., Tannock Q., Löfwander T., Kinaret J. Nanoscale; 7 (11): 4598 - 4810. 2015. 10.1039/c4nr01600a. IF: 7.394

We present the science and technology roadmap for graphene, related two-dimensional crystals, and hybrid systems, targeting an evolution in technology, that might lead to impacts and benefits reaching into most areas of society. This roadmap was developed within the framework of the European Graphene Flagship and outlines the main targets and research areas as best understood at the start of this ambitious project. We provide an overview of the key aspects of graphene and related materials (GRMs), ranging from fundamental research challenges to a variety of applications in a large number of sectors, highlighting the steps necessary to take GRMs from a state of raw potential to a point where they might revolutionize multiple industries. We also define an extensive list of acronyms in an effort to standardize the nomenclature in this emerging field. © The Royal Society of Chemistry 2015.

• Spin transport in hydrogenated graphene

Soriano D., Van Tuan D., Dubois S.M.-M., Gmitra M., Cummings A.W., Kochan D., Ortmann F., Charlier J.-C., Fabian J., Roche S. 2D Materials; 2 (2, 022002) 2015. 10.1088/2053-1583/2/2/022002. IF: 0.000

In this review we discuss the multifaceted problem of spin transport in hydrogenated graphene from a theoretical perspective. The current experimental findings suggest that hydrogenation can either increase or decrease spin lifetimes, which calls for clarification.We first discuss the spin-orbit coupling induced by local σ-π re-hybridization and sp3 C-Hdefect formation togetherwith the formation of a local magnetic moment. First-principles calculations of hydrogenated graphene unravel the strong interplay of spin-orbit and exchange couplings. The concept of magnetic scattering resonances, recently introduced by Kochan et al (2014 Phys. Rev. Lett. 112 116602) is revisited by describing the local magnetism through the self-consistent Hubbard model in the mean field approximation in the dilute limit, while spin relaxation lengths and transport times are computed using an efficient real space orderNwavepacket propagation method. Typical spin lifetimes on the order of 1 ns are obtained for 1 ppm of hydrogen impurities (corresponding to a transport time of about 50 ps), and the scaling of spin lifetimes with impurity density is described by the Elliott-Yafet mechanism. This reinforces the statement that local defect-induced magnetism can be at the origin of the substantial spin polarization loss in the clean graphene limit. © 2015 IOP Publishing Ltd.

• Velocity renormalization and Dirac cone multiplication in graphene superlattices with various barrier-edge geometries

De Jamblinne De Meux A., Leconte N., Charlier J.-C., Lherbier A. Physical Review B - Condensed Matter and Materials Physics; 91 (23, 235139) 2015. 10.1103/PhysRevB.91.235139. IF: 3.736

The electronic properties of one-dimensional graphene superlattices strongly depend on the atomic size and orientation of the 1D external periodic potential. Using a tight-binding approach, we show that the armchair and zigzag directions in these superlattices have a different impact on the renormalization of the anisotropic velocity of the charge carriers. For symmetric potential barriers, the velocity perpendicular to the barrier is modified for the armchair direction while remaining unchanged in the zigzag case. For asymmetric barriers, the initial symmetry between the forward and backward momentum with respect to the Dirac cone symmetry is broken for the velocity perpendicular (armchair case) or parallel (zigzag case) to the barriers. At last, Dirac cone multiplication at the charge neutrality point occurs only for the zigzag geometry. In contrast, band gaps appear in the electronic structure of the graphene superlattice with barrier in the armchair direction. © 2015 American Physical Society.

### 2014

• Anisotropic behavior of quantum transport in graphene superlattices: Coexistence of ballistic conduction with Anderson insulating regime

Pedersen, J.G.; Cummings, A.W.; Roche, S. Physical Review B - Condensed Matter and Materials Physics; 2014. 10.1103/PhysRevB.89.165401. IF: 3.664

• Anomalous dissipation mechanism and Hall quantization limit in polycrystalline graphene grown by chemical vapor deposition

Lafont, F.; Ribeiro-Palau, R.; Han, Z.; Cresti, A.; Delvallee, A.; Cummings, A.W.; Roche, S.; Bouchiat, V.; Ducourtieux, S.; Schopfer, F.; Poirier, W. Physical Review B - Condensed Matter and Materials Physics; 2014. 10.1103/PhysRevB.90.115422. IF: 3.664

• Anomalous exchange interaction between intrinsic spins in conducting graphene systems

Santos, H.; Soriano, D.; Palacios, J.J. Physical Review B - Condensed Matter and Materials Physics; 2014. 10.1103/PhysRevB.89.195416. IF: 3.664

• Charge transport in polycrystalline graphene: Challenges and opportunities

Cummings, A.W.; Duong, D.L.; Nguyen, V.L.; Van Tuan, D.; Kotakoski, J.; Barrios Vargas, J.E.; Lee, Y.H.; Roche, S. Advanced Materials; 26 (30): 5079 - 5094. 2014. 10.1002/adma.201401389. IF: 15.409

• Fingerprints of inelastic transport at the surface of the topological insulator Bi 2 Se 3: Role of electron-phonon coupling

Costache, M.V.; Neumann, I.; Sierra, J.F.; Marinova, V.; Gospodinov, M.M.; Roche, S.; Valenzuela, S.O. Physical Review Letters; 2014. 10.1103/PhysRevLett.112.086601. IF: 7.728

• Graphene spintronics: Puzzling controversies and challenges for spin manipulation

Roche, S.; Valenzuela, S.O. Journal of Physics D - Applied Physics; 2014. 10.1088/0022-3727/47/9/094011. IF: 2.521

• Impact of graphene polycrystallinity on the performance of graphene field-effect transistors

Jiménez, D.; Cummings, A.W.; Chaves, F.; Van Tuan, D.; Kotakoski, J.; Roche, S. Applied Physics Letters; 2014. 10.1063/1.4863842. IF: 3.515

• Multiple quantum phases in graphene with enhanced spin-orbit coupling: From the quantum spin hall regime to the spin hall effect and a robust metallic state

Cresti, A.; Van Tuan, D.; Soriano, D.; Cummings, A.W.; Roche, S. Physical Review Letters; 113 (24): NC. 2014. 10.1103/PhysRevLett.113.246603. IF: 7.728

• Physical model of the contact resistivity of metal-graphene junctions

Chaves F.A., Jiménez D., Cummings A.W., Roche S. Journal of Applied Physics; 115 (16, 164513) 2014. 10.1063/1.4874181. IF: 2.101

While graphene-based technology shows great promise for a variety of electronic applications, including radio-frequency devices, the resistance of the metal-graphene contact is a technological bottleneck for the realization of viable graphene electronics. One of the most important factors in determining the resistance of a metal-graphene junction is the contact resistivity. Despite the large number of experimental works that exist in the literature measuring the contact resistivity, a simple model of it is still lacking. In this paper, we present a comprehensive physical model for the contact resistivity of these junctions, based on the Bardeen Transfer Hamiltonian method. This model unveils the role played by different electrical and physical parameters in determining the specific contact resistivity, such as the chemical potential of interaction, the work metal-graphene function difference, and the insulator thickness between the metal and graphene. In addition, our model reveals that the contact resistivity is strongly dependent on the bias voltage across the metal-graphene junction. This model is applicable to a wide variety of graphene-based electronic devices and thus is useful for understanding how to optimize the contact resistance in these systems. © 2014 AIP Publishing LLC.

• Pseudospin-driven spin relaxation mechanism in graphene

Tuan, D.V.; Ortmann, F.; Soriano, D.; Valenzuela, S.O.; Roche, S. Nature Physics; 10 (11): 857 - 863. 2014. 10.1038/nphys3083. IF: 20.603

• Quantum Hall Effect in Polycrystalline Graphene: The Role of Grain Boundaries

Cummings, A.W.; Cresti, A.; Roche, S. Physical Review B - Condensed Matter and Materials Physics; 90: 161401 (R). 2014. 10.1103/PhysRevB.90.161401. IF: 3.664

• Quantum transport in chemically functionalized graphene at high magnetic field: defect-induced critical states and breakdown of electron-hole symmetry

Leconte, N; Ortmann, F.; Cresti, A.; Charlier, J.C.; Roche, S. 2D Materials; 2014. 10.1088/2053-1583/1/2/021001. IF: 0.000

• Transport fingerprints at graphene superlattice Dirac points induced by a boron nitride substrate

Martinez-Gordillo, R.; Roche, S.; Ortmann, F.; Pruneda, M. Physical Review B - Condensed Matter and Materials Physics; 2014. 10.1103/PhysRevB.89.161401. IF: 3.664

• Tunneling magnetoresistance phenomenon utilizing graphene magnet electrode

Hashimoto, T.; Kamikawa, S.; Soriano, D.; Pedersen, J. G.; Roche, S.; Haruyama, J. Applied Physics Letters; 105: 183111. 2014. 10.1063/1.4901279. IF: 3.515

### 2013

• Band gap engineering via edge-functionalization of graphene nanoribbons

Wagner, P.; Ewels, C.P.; Adjizian, J.-J.; Magaud, L.; Pochet, P.; Roche, S.; Lopez-Bezanilla, A.; Ivanovskaya, V.V.; Yaya, A.; Rayson, M.; Briddon, P.; Humbert, B. Journal of Physical Chemistry C; 117 (50): 26790 - 26796. 2013. 10.1021/jp408695c. IF: 4.814

• Broken symmetries, zero-energy modes, and quantum transport in disordered graphene: From supermetallic to insulating regimes

Cresti, A.; Ortmann, F.; Louvet, T.; Van Tuan, D.; Roche, S. Physical Review Letters; 110 2013. 10.1103/PhysRevLett.110.196601. IF: 7.943

• Highly defective graphene: A key prototype of two-dimensional Anderson insulators

Lherbier, A.; Roche, S.; Restrepo, O.A.; Niquet, Y.-M.; Delcorte, A.; Charlier, J.-C. Nano Research; 6: 326 - 334. 2013. 10.1007/s12274-013-0309-7. IF: 7.392

• Impact of vacancies on diffusive and pseudodiffusive electronic transport in graphene

Cresti, A.; Louvet, T.; Ortmann, F.; Van Tuan, D.; Lenarczyk, P.; Huhs, G.; Roche, S. Crystals; 3 (2): 289 - 305. 2013. 10.3390/cryst3020289. IF: 0.000

• Multiscale simulation of carbon nanotube transistors

Maneux, C.; Fregonese, S.; Zimmer, T.; Retailleau, S.; Nguyen, H.N.; Querlioz, D.; Bournel, A.; Dollfus, P.; Triozon, F.; Niquet, Y.M.; Roche, S. Solid-State Electronics; 89: 26 - 67. 2013. 10.1016/j.sse.2013.06.013. IF: 1.482

• Non-perturbative effects of laser illumination on the electrical properties of graphene nanoribbons

Calvo, H.L.; Perez-Piskunow, P.M.; Pastawski, H.M.; Roche, S.; Foa Torres, L.E.F. Journal of Physics Condensed Matter; 25 2013. 10.1088/0953-8984/25/14/144202. IF: 2.355

• Proximity effects induced in graphene by magnetic insulators: First-principles calculations on spin filtering and exchange-splitting gaps

Yang, H.X.; Hallal, A.; Terrade, D.; Waintal, X.; Roche, S.; Chshiev, M. Physical Review Letters; 110 2013. 10.1103/PhysRevLett.110.046603. IF: 7.943

• Scaling properties of charge transport in polycrystalline graphene

Van Tuan, D.; Kotakoski, J.; Louvet, T.; Ortmann, F.; Meyer, J.C.; Roche, S. Nano Letters; 13: 1730 - 1735. 2013. 10.1021/nl400321r. IF: 13.025

• Splitting of the zero-energy Landau level and universal dissipative conductivity at critical points in disordered graphene

Ortmann, F.; Roche, S. Physical Review Letters; 2013. 10.1103/PhysRevLett.110.086602. IF: 7.943

### 2012

• Atomistic boron-doped graphene field-effect transistors: A route toward unipolar characteristics

Marconcini, P.; Cresti, A.; Triozon, F.; Fiori, G.; Biel, B.; Niquet, Y.M.; Macucci, M.; Roche, S. ACS Nano; 6: 7942 - 7947. 2012. 10.1021/nn3024046.

• Chemically enriched graphene-based switching devices: A novel principle driven by impurity-induced quasibound states and quantum coherence

Roche, S.; Biel, B.; Cresti, A.; Triozon, F. Physica E: Low-Dimensional Systems and Nanostructures; 44: 960 - 962. 2012. 10.1016/j.physe.2011.06.008.

• Electron-hole transport asymmetry in boron-doped graphene field effect transistors

Marconcini, P. ; Cresti, A. ; Triozon, F.; Fiori, G. ; Biel, B. ; Niquet, Y.M.; Macucci, M.; Roche, S. Journal of Computational Electronics; 1: 1 - 4. 2012. 10.1109/IWCE.2012.6242844.

• Embedded boron nitride domains in graphene nanoribbons for transport gap engineering

Lopez-Bezanilla, A.; Roche, S. Physical Review B - Condensed Matter and Materials Physics; 86 2012. 10.1103/PhysRevB.86.165420.

• Insulating behavior of an amorphous graphene membrane

Van Tuan D., Kumar A., Roche S., Ortmann F., Thorpe M.F., Ordejon P. Physical Review B - Condensed Matter and Materials Physics; 86 (12, 121408) 2012. 10.1103/PhysRevB.86.121408.

We investigate the charge transport properties of planar amorphous graphene that is fully topologically disordered, in the form of sp2 threefold coordinated networks consisting of hexagonal rings but also including many pentagons and heptagons distributed in a random fashion. Using the Kubo transport methodology and the Lanczos method, the density of states, mean free paths, and semiclassical conductivities of such amorphous graphene membranes are computed. Despite a large increase in the density of states close to the charge neutrality point, all electronic properties are dramatically degraded, evidencing an Anderson insulating state caused by topological disorder alone. These results are supported by Landauer-Büttiker conductance calculations, which show a localization length as short as 5 nm. © 2012 American Physical Society.

• Interplay between sublattice and spin symmetry breaking in graphene

Soriano, D.; Fernández-Rossier, J. Physical Review B - Condensed Matter and Materials Physics; 85 2012. 10.1103/PhysRevB.85.195433.

• Large bandwidths in synthetic one-dimensional stacks of biological molecules

Oetzel, B.; Ortmann, F.; Matthes, L.; Tandetzky, F.; Bechstedt, F.; Hannewald, K. Physical Review B - Condensed Matter and Materials Physics; 86 2012. 10.1103/PhysRevB.86.195407.

• Laser-induced effects on the electronic features of graphene nanoribbons

Calvo, H.L.; Perez-Piskunow, P.M.; Roche, S.; Foa Torres, L.E.F. Applied Physics Letters; 101 2012. 10.1063/1.4772496.

• Quantum transport in disordered graphene: A theoretical perspective

Roche, S.; Leconte, N.; Ortmann, F.; Lherbier, A.; Soriano, D.; Charlier, J.-C. Solid State Communications; 152: 1404 - 1410. 2012. 10.1016/j.ssc.2012.04.030.

• Quenching of the quantum hall effect in graphene with scrolled edges

Cresti, A.; Fogler, M.M.; Guinea, F.; Castro Neto, A.H.; Roche, S. Physical Review Letters; 108 2012. 10.1103/PhysRevLett.108.166602.

• Spin-filtered edge states in graphene

Gosálbez-Martínez, D.; Soriano, D.; Palacios, J.J.; Fernández-Rossier, J. Solid State Communications; 152: 1469 - 1476. 2012. 10.1016/j.ssc.2012.04.046.

• Three-dimensional models of topological insulators: Engineering of Dirac cones and robustness of the spin texture

Soriano, D.; Ortmann, F.; Roche, S. Physical Review Letters; 109 2012. 10.1103/PhysRevLett.109.266805.

• Transport properties of graphene containing structural defects

Lherbier, A.; Dubois, S.M.-M.; Declerck, X.; Niquet, Y.-M.; Roche, S.; Charlier, J.-C. Physical Review B - Condensed Matter and Materials Physics; 86 2012. 10.1103/PhysRevB.86.075402.

### 2011

• Effects of domains in phonon conduction through hybrid boron nitride and graphene sheets

Sevinçli, H.; Li, W.; Mingo, N.; Cuniberti, G.; Roche, S. Physical Review B - Condensed Matter and Materials Physics; 84 2011. 10.1103/PhysRevB.84.205444.

• Efficient linear scaling method for computing the thermal conductivity of disordered materials

Li, W.; Sevinçli, H.; Roche, S.; Cuniberti, G. Physical Review B - Condensed Matter and Materials Physics; 83 2011. 10.1103/PhysRevB.83.155416.

• Engineering carbon chains from mechanically stretched graphene-based materials

Erdogan, E.; Popov, I.; Rocha, C.G.; Cuniberti, G.; Roche, S.; Seifert, G. Physical Review B - Condensed Matter and Materials Physics; 83 2011. 10.1103/PhysRevB.83.041401.

• Graphene: Piecing it together

Rümmeli, M.H.; Rocha, C.G.; Ortmann, F.; Ibrahim, I.; Sevincli, H.; Börrnert, F.; Kunstmann, J.; Bachmatiuk, A.; Pötschke, M.; Shiraishi, M.; Meyyappan, M.; Büchner, B.; Roche, S.; Cuniberti, G. Advanced Materials; 23: 4471 - 4490. 2011. 10.1002/adma.201101855.

• Inducing and optimizing magnetism in graphene nanomeshes

Yang, H.-X.; Chshiev, M.; Boukhvalov, D.W.; Waintal, X.; Roche, S. Physical Review B - Condensed Matter and Materials Physics; 84 2011. 10.1103/PhysRevB.84.214404.

• Integer quantum Hall effect in trilayer graphene

Kumar, A.; Escoffier, W.; Poumirol, J.M.; Faugeras, C.; Arovas, D.P.; Fogler, M.M.; Guinea, F.; Roche, S.; Goiran, M.; Raquet, B. Physical Review Letters; 107 2011. 10.1103/PhysRevLett.107.126806.

• Magnetism-dependent transport phenomena in hydrogenated graphene: From spin-splitting to localization effects

Leconte N., Soriano D., Roche S., Ordejon P., Charlier J.-C., Palacios J.J. ACS Nano; 5 (5): 3987 - 3992. 2011. 10.1021/nn200558d.

Spin-dependent transport in hydrogenated two-dimensional graphene is explored theoretically. Adsorbed atomic hydrogen impurities can either induce a local antiferromagnetic, ferromagnetic, or nonmagnetic state depending on their density and relative distribution. To describe the various magnetic possibilities of hydrogenated graphene, a self-consistent Hubbard Hamiltonian, optimized by ab initio calculations, is first solved in the mean field approximation for small graphene cells. Then, an efficient order N Kubo transport methodology is implemented, enabling large scale simulations of functionalized graphene. Depending on the underlying intrinsic magnetic ordering of hydrogen-induced spins, remarkably different transport features are predicted for the same impurity concentration. Indeed, while the disordered nonmagnetic graphene system exhibits a transition from diffusive to localization regimes, the intrinsic ferromagnetic state exhibits unprecedented robustness toward quantum interference, maintaining, for certain resonant energies, a quasiballistic regime up to the micrometer scale. Consequently, low temperature transport measurements could unveil the presence of a magnetic state in weakly hydrogenated graphene. © 2011 American Chemical Society.

• Magnetoresistance and magnetic ordering fingerprints in hydrogenated graphene

Soriano D., Leconte N., Ordejón P., Charlier J.-C., Palacios J.-J., Roche S. Physical Review Letters; 107 (1, 016602) 2011. 10.1103/PhysRevLett.107.016602.

Spin-dependent features in the conductivity of graphene, chemically modified by a random distribution of hydrogen adatoms, are explored theoretically. The spin effects are taken into account using a mean-field self-consistent Hubbard model derived from first-principles calculations. A Kubo transport methodology is used to compute the spin-dependent transport fingerprints of weakly hydrogenated graphene-based systems with realistic sizes. Conductivity responses are obtained for paramagnetic, antiferromagnetic, or ferromagnetic macroscopic states, constructed from the mean-field solutions obtained for small graphene supercells. Magnetoresistance signals up to ∼7% are calculated for hydrogen densities around 0.25%. These theoretical results could serve as guidance for experimental observation of induced magnetism in graphene. © 2011 American Physical Society.

• Magnetoresistance in disordered graphene: The role of pseudospin and dimensionality effects unraveled

Ortmann, F.; Cresti, A.; Montambaux, G.; Roche, S. Europhysics Letters; 94 2011. 10.1209/0295-5075/94/47006.

• Mechanically-induced transport switching effect in graphene-based nanojunctions

Kawai, T.; Poetschke, M.; Miyamoto, Y.; Rocha, C.G.; Roche, S.; Cuniberti, G. Physical Review B - Condensed Matter and Materials Physics; 83 2011. 10.1103/PhysRevB.83.241405.

• Nanoelectronics: Graphene gets a better gap

Roche, S. Nature Nanotechnology; 2011. 10.1038/nnano.2010.262 .

• Oxygen surface functionalization of graphene nanoribbons for transport gap engineering

Cresti A., Lopez-Bezanilla A., Ordejón P., Roche S. ACS Nano; 5 (11): 9271 - 9277. 2011. 10.1021/nn203573y.

We numerically investigate the impact of epoxide adsorbates on the transport properties of graphene nanoribbons with width varying from a few nanometers to 15 nm. For the wider ribbons, a scaling analysis of conductance properties is performed for adsorbate density ranging from 0.1% to 0.5%. Oxygen atoms introduce a large electron-hole transport asymmetry with mean free paths changing by up to 1 order of magnitude, depending on the hole or electron nature of charge carriers. The opening of a transport gap on the electron side for GNRs as wide as 15 nm could be further exploited to control current flow and achieve larger ON/OFF ratios, despite the initially small intrinsic energy gap. The effect of the adsorbates in narrow ribbons is also investigated by full ab initio calculations to explore the limit of ultimate downsized systems. In this case, the inhomogeneous distribution of adsorbates and their interplay with the ribbon edge are found to play an important role. © 2011 American Chemical Society.

• Polaron transport in organic crystals: Temperature tuning of disorder effects

Ortmann, F.; Roche, S. Physical Review B - Condensed Matter and Materials Physics; 84 2011. 10.1103/PhysRevB.84.180302.

• Quantum transport in chemically modified two-dimensional graphene: From minimal conductivity to Anderson localization

Leconte N., Lherbier A., Varchon F., Ordejon P., Roche S., Charlier J.-C. Physical Review B - Condensed Matter and Materials Physics; 84 (23, 235420) 2011. 10.1103/PhysRevB.84.235420.

An efficient computational methodology is used to explore charge transport properties in chemically modified (and randomly disordered) graphene-based materials. The Hamiltonians of various complex forms of graphene are constructed using tight-binding models enriched by first-principles calculations. These atomistic models are further implemented into a real-space order-N Kubo-Greenwood approach, giving access to the main transport length scales (mean free paths, localization lengths) as a function of defect density and charge carrier energy. An extensive investigation is performed for epoxide impurities with specific discussions on both the existence of a minimum semiclassical conductivity and a crossover between weak to strong localization regime. The 2D generalization of the Thouless relationship linking transport length scales is here illustrated based on a realistic disorder model. © 2011 American Physical Society.

• Tuning laser-induced band gaps in graphene

Calvo, H.L.; Pastawski, H.M.; Roche, S.; Torres, L.E.F.F. Applied Physics Letters; 98 2011. 10.1063/1.3597412.

• Two-dimensional graphene with structural defects: Elastic mean free path, minimum conductivity, and anderson transition

Lherbier, A.; Dubois, S.M.M.; Declerck, X.; Roche, S.; Niquet, Y.M.; Charlier, J.C. Physical Review Letters; 106 2011. 10.1103/PhysRevLett.106.046803.

• Unveiling the magnetic structure of graphene nanoribbons

Ribeiro, R.; Poumirol, J.-M.; Cresti, A.; Escoffier, W.; Goiran, M.; Broto, J.-M.; Roche, S.; Raquet, B. Physical Review Letters; 107 2011. 10.1103/PhysRevLett.107.086601.

### 2010

• Conductance of functionalized nanotubes, graphene and nanowires: from ab initio to mesoscopic physics

Blase, X. ; Adessi, C.; Biel, B.; Lopez-Bezanilla, A.; Fernández-Serra, M.V.; Margine, E. R.; Triozon, F.; Roche, S. Physica Status Solidi (B): Basic Research; 2010. .

• Damaging graphene with ozone treatment: A chemically tunable metal - Insulator transition

Leconte N., Moser J., Ordejón P., Tao H., Lherbier A., Bachtold A., Alsina F., Sotomayor Torres C.M., Charlier J.-C., Roche S. ACS Nano; 4 (7): 4033 - 4038. 2010. 10.1021/nn100537z.

We present a multiscale ab initio study of electronic and transport properties of two-dimensional graphene after epoxide functionalization via ozone treatment. The orbital rehybridization induced by the epoxide groups triggers a strong intervalley scattering and changes dramatically the conduction properties of graphene. By varying the coverage density of epoxide defects from 0.1 to 4%, charge conduction can be tuned from a diffusive to a strongly localized regime, with localization lengths down to a few nanometers long. Experimental results supporting the interpretation as a metal - insulator transition are also provided. © 2010 American Chemical Society.

• Edge magnetotransport fingerprints in disordered graphene nanoribbons

Poumirol, J.-M.; Cresti, A.; Roche, S.; Escoffier, W.; Goiran, M.; Wang, X.; Li, X.; Dai, H.; Raquet, B. Physical Review B - Condensed Matter and Materials Physics; 82 2010. 10.1103/PhysRevB.82.041413.

• Inelastic transport in vibrating disordered carbon nanotubes: Scattering times and temperature-dependent decoherence effects

Ishii, H.; Roche, S.; Kobayashi, N.; Hirose, K. Physical Review Letters; 104 2010. 10.1103/PhysRevLett.104.116801.

• Magnetotransport in disordered graphene exposed to ozone: From weak to strong localization

Moser, J.; Tao, H.; Roche, S.; Alzina, F.; Sotomayor Torres, C.M.; Bachtold, A. Physical Review B - Condensed Matter and Materials Physics; 81 2010. 10.1103/PhysRevB.81.205445.

• Mobility gaps in disordered graphene-based materials: An ab initio -based tight-binding approach to mesoscopic transport

Biel, B.; Cresti, A.; Avriller, R.; Dubois, S.; López-Bezanilla, A.; Triozon, F.; Blase, X.; Charlier, J.-C.; Roche, S. Physica Status Solidi (C) Current Topics in Solid State Physics; 7: 2628 - 2631. 2010. 10.1002/pssc.200983826.

• Modeling graphene-based nanoelectromechanical devices

Poetschke, M.; Rocha, C.G.; Foa Torres, L.E.F.; Roche, S.; Cuniberti, G. Physical Review B - Condensed Matter and Materials Physics; 81 2010. 10.1103/PhysRevB.81.193404.

• Phonon transport in large scale carbon-based disordered materials: Implementation of an efficient order-N and real-space Kubo methodology

Li, W.; Sevinçli, H.; Cuniberti, G.; Roche, S. Physical Review B - Condensed Matter and Materials Physics; 82 2010. 10.1103/PhysRevB.82.041410.

• Preface: Phys. stat. sol. (c) 7/11-12

Correia, A.; Sáenz, J.J.; Ordejon, P.; Roche, S. Physica Status Solidi (C) Current Topics in Solid State Physics; 7: 2593 - 2595. 2010. 10.1002/pssc.201060100.

• Quantum transport in graphene nanoribbons: Effects of edge reconstruction and chemical reactivity

Dubois, S.M.-M.; Lopez-Bezanilla, A.; Cresti, A.; Triozon, F.; Biel, B.; Charlier, J.-C.; Roche, S. ACS Nano; 4: 1971 - 1976. 2010. 10.1021/nn100028q.

• Simulation, modelling and characterisation of quasi-ballistic transport in nanometer sized field effect transistors: from TCAD to atomistic simulation

Roche, S.; Poiroux, T.; Lecarval, G.; Barraud, S.; Triozon, F.; Persson, M.; Niquet, Y.M. International Journal of Nanotechnology; 7 (04-ag.): 348 - 366. 2010. 10.1504/IJNT.2010.031724.

• Tuning the band gap of semiconducting carbon nanotube by an axial magnetic field

Fedorov, G.; Barbara, P.; Smirnov, D.; Jiménez, D.; Roche, S. Applied Physics Letters; 2010. .

### 2009

• Propagative Landau states and Fermi level pinning in carbon nanotubes

Nanot, S.; Avriller, R.; Escoffier, W.; Broto, J.-M.; Roche, S.; Raquet, B. Physical Review Letters; 103 2009. 10.1103/PhysRevLett.103.256801.