Staff directory Sara Martí Sánchez

Sara Martí Sánchez

Postdoctoral Researcher
sara.marti(ELIMINAR)@icn2.cat
Advanced Electron Nanoscopy

Publications

2024

  • Control of Ge island coalescence for the formation of nanowires on silicon

    Ramanandan, Santhanu Panikar; Sapera, Joel Rene; Morelle, Alban; Marti-Sanchez, Sara; Rudra, Alok; Arbiol, Jordi; Dubrovskii, Vladimir G; Fontcuberta i Morral, Anna Nanoscale Horizons; 9 (4) 2024. 10.1039/d3nh00573a.


  • Nanoporous graphene-based thin-film microelectrodes for in vivo high-resolution neural recording and stimulation

    Viana, Damia; Walston, Steven T; Masvidal-Codina, Eduard; Illa, Xavi; Rodriguez-Meana, Bruno; del Valle, Jaume; Hayward, Andrew; Dodd, Abbie; Loret, Thomas; Prats-Alfonso, Elisabet; de la Oliva, Natalia; Palma, Marie; del Corro, Elena; Bernicola, Maria del Pilar; Rodriguez-Lucas, Elisa; Gener, Thomas; de la Cruz, Jose Manuel; Torres-Miranda, Miguel; Duvan, Fikret Taygun; Ria, Nicola; Sperling, Justin; Marti-Sanchez, Sara; Spadaro, Maria Chiara; Hebert, Clement; Savage, Sinead; Arbiol, Jordi; Guimera-Brunet, Anton; Puig, M Victoria; Yvert, Blaise; Navarro, Xavier; Kostarelos, Kostas; Garrido, Jose A Nature Nanotechnology; 2024. 10.1038/s41565-023-01570-5.


2023

  • Cryogenic multiplexing using selective area grown nanowires

    Olsteins, D; Nagda, G; Carrad, DJ; Beznasyuk, DV; Petersen, CEN; Martí-Sánchez, S; Arbiol, J; Jespersen, TS Nature Communications; 14 (1): 7738. 2023. 10.1038/s41467-023-43551-1. IF: 16.600


  • Electrochemical Stability of Rhodium-Platinum Core-Shell Nanoparticles: An Identical Location Scanning Transmission Electron Microscopy Study

    Vega-Paredes, M; Aymerich-Armengol, R; Esteban, DA; Marti-Sanchez, S; Bals, S; Scheu, C; Manjon, AG Acs Nano; 17 (17): 16943 - 16951. 2023. 10.1021/acsnano.3c04039. IF: 17.100


  • Epitaxially Driven Phase Selectivity of Sn in Hybrid Quantum Nanowires

    Khan, SA; Marti-Sanchez, S; Olsteins, D; Lampadaris, C; Carrad, DJ; Liu, Y; Quinones, J; Spadaro, MC; Jespersen, TS; Krogstrup, P; Arbiol, J Acs Nano; 17 (12): 11794 - 11804. 2023. 10.1021/acsnano.3c02733. IF: 17.100


  • Hard superconducting gap in germanium

    Tosato, A; Levajac, V; Wang, JY; Boor, CJ; Borsoi, F; Botifoll, M; Borja, CN; Marti-Sanchez, S; Arbiol, J; Sammak, A; Veldhorst, M; Scappucci, G Communications Materials; 4 (1): 23. 2023. 10.1038/s43246-023-00351-w. IF: 7.800


  • Tubular C3N4 Nanotubes as Metal-Free Sulfur Hosts toward Stable Lithium-Sulfur Batteries

    Zhang, CQ; Du, RF; Marti-Sanchez, S; Xiao, K; Yang, DW; Zhang, CY; Li, CH; Zeng, GF; Chang, XQ; He, R; Arbiol, J; Li, JS; Biendicho, JJ; Cabot, A Energies; 16 (12): 4545. 2023. 10.3390/en16124545. IF: 3.200


2022

  • Doubling the mobility of InAs/InGaAs selective area grown nanowires

    Beznasyuk D.V., Martí-Sánchez S., Kang J.-H., Tanta R., Rajpalke M., Stankevič T., Christensen A.W., Spadaro M.C., Bergamaschini R., Maka N.N., Petersen C.E.N., Carrad D.J., Jespersen T.S., Arbiol J., Krogstrup P. Physical Review Materials; 6 (3, 034602) 2022. 10.1103/PhysRevMaterials.6.034602. IF: 3.989

    Selective area growth (SAG) of nanowires and networks promise a route toward scalable electronics, photonics, and quantum devices based on III-V semiconductor materials. The potential of high-mobility SAG nanowires however is not yet fully realised, since interfacial roughness, misfit dislocations at the nanowire/substrate interface and nonuniform composition due to material intermixing all scatter electrons. Here, we explore SAG of highly lattice-mismatched InAs nanowires on insulating GaAs(001) substrates and address these key challenges. Atomically smooth nanowire/substrate interfaces are achieved with the use of atomic hydrogen (a-H) as an alternative to conventional thermal annealing for the native oxide removal. The problem of high lattice mismatch is addressed through an InxGa1-xAs buffer layer introduced between the InAs transport channel and the GaAs substrate. The Ga-In material intermixing observed in both the buffer layer and the channel is inhibited via careful tuning of the growth temperature. Performing scanning transmission electron microscopy and x-ray diffraction analysis along with low-temperature transport measurements we show that optimized In-rich buffer layers promote high-quality InAs transport channels with the field-effect electron mobility over 10 000 cm2 V-1 s-1. This is twice as high as for nonoptimized samples and among the highest reported for InAs selective area grown nanostructures. © 2022 American Physical Society.


  • Extended-SWIR Photodetection in All-Group IV Core/Shell Nanowires

    Luo L., Assali S., Atalla M.R.M., Koelling S., Attiaoui A., Daligou G., Martí S., Arbiol J., Moutanabbir O. ACS Photonics; 9 (3): 914 - 921. 2022. 10.1021/acsphotonics.1c01728. IF: 7.529

    Group IV Ge1-xSnx semiconductors hold the premise of enabling broadband silicon-integrated infrared optoelectronics due to their tunable band gap energy and directness. Herein, we exploit these attributes along with the enhanced lattice strain relaxation in Ge/Ge0.92Sn0.08 core/shell nanowire heterostructures to implement highly responsive room-temperature short-wave infrared nanoscale photodetectors. Atomic-level studies confirm the uniform shell composition and its higher crystallinity with respect to thin films counterparts. The demonstrated Ge/Ge0.92Sn0.08 p-type field-effect nanowire transistors exhibit superior optoelectronic properties achieving simultaneously relatively high mobility, high ON/OFF ratio, and high responsivity, in addition to a broadband absorption in the short-wave infrared range. Indeed, the reduced band gap of the Ge0.92Sn0.08 shell yields an extended cutoff wavelength of 2.1 μm, with a room-temperature responsivity reaching 2.7 A/W at 1550 nm. These results highlight the potential of Ge/Ge1-xSnx core/shell nanowires as silicon-compatible building blocks for nanoscale-integrated infrared photonics. © 2022 American Chemical Society.


  • Majorana-like Coulomb spectroscopy in the absence of zero-bias peaks

    Valentini M; Borovkov M; Prada E; Martí-Sánchez S; Botifoll M; Hofmann A; Arbiol J; Aguado R; San-Jose P; Katsaros G Nature; 612 (7940): 442 - +. 2022. 10.1038/s41586-022-05382-w. IF: 69.504


  • Sub-nanometer mapping of strain-induced band structure variations in planar nanowire core-shell heterostructures

    Martí-Sánchez S., Botifoll M., Oksenberg E., Koch C., Borja C., Spadaro M.C., Di Giulio V., Ramasse Q., García de Abajo F.J., Joselevich E., Arbiol J. Nature Communications; 13 (1, 4089) 2022. 10.1038/s41467-022-31778-3.

    Strain relaxation mechanisms during epitaxial growth of core-shell nanostructures play a key role in determining their morphologies, crystal structure and properties. To unveil those mechanisms, we perform atomic-scale aberration-corrected scanning transmission electron microscopy studies on planar core-shell ZnSe@ZnTe nanowires on α-Al2O3 substrates. The core morphology affects the shell structure involving plane bending and the formation of low-angle polar boundaries. The origin of this phenomenon and its consequences on the electronic band structure are discussed. We further use monochromated valence electron energy-loss spectroscopy to obtain spatially resolved band-gap maps of the heterostructure with sub-nanometer spatial resolution. A decrease in band-gap energy at highly strained core-shell interfacial regions is found, along with a switch from direct to indirect band-gap. These findings represent an advance in the sub-nanometer-scale understanding of the interplay between structure and electronic properties associated with highly mismatched semiconductor heterostructures, especially with those related to the planar growth of heterostructured nanowire networks. © 2022, The Author(s).


2021

  • Enhancement of proximity-induced superconductivity in a planar Ge hole gas

    Aggarwal K., Hofmann A., Jirovec D., Prieto I., Sammak A., Botifoll M., Martí-Sánchez S., Veldhorst M., Arbiol J., Scappucci G., Danon J., Katsaros G. Physical Review Research; 3 (2, L022005) 2021. 10.1103/PhysRevResearch.3.L022005. IF: 0.000

    Hole gases in planar germanium can have high mobilities in combination with strong spin-orbit interaction and electrically tunable g factors, and are therefore emerging as a promising platform for creating hybrid superconductor-semiconductor devices. A key challenge towards hybrid Ge-based quantum technologies is the design of high-quality interfaces and superconducting contacts that are robust against magnetic fields. In this work, by combining the assets of aluminum, which provides good contact to the Ge, and niobium, which has a significant superconducting gap, we demonstrate highly transparent low-disordered JoFETs with relatively large ICRN products that are capable of withstanding high magnetic fields. We furthermore demonstrate the ability of phase-biasing individual JoFETs, opening up an avenue to explore topological superconductivity in planar Ge. The persistence of superconductivity in the reported hybrid devices beyond 1.8 T paves the way towards integrating spin qubits and proximity-induced superconductivity on the same chip. © 2021 authors. Published by the American Physical Society.


  • Rotated domains in selective area epitaxy grown Zn3P2: Formation mechanism and functionality

    Spadaro M.C., Escobar Steinvall S., Dzade N.Y., Martí-Sánchez S., Torres-Vila P., Stutz E.Z., Zamani M., Paul R., Leran J.-B., Fontcuberta I Morral A., Arbiol J. Nanoscale; 13 (44): 18441 - 18450. 2021. 10.1039/d1nr06190a. IF: 7.790

    Zinc phosphide (Zn3P2) is an ideal absorber candidate for solar cells thanks to its direct bandgap, earth-abundance, and optoelectronic characteristics, albeit it has been insufficiently investigated due to limitations in the fabrication of high-quality material. It is possible to overcome these factors by obtaining the material as nanostructures, e.g. via the selective area epitaxy approach, enabling additional strain relaxation mechanisms and minimizing the interface area. We demonstrate that Zn3P2 nanowires grow mostly defect-free when growth is oriented along the [100] and [110] of the crystal, which is obtained in nanoscale openings along the [110] and [010] on InP(100). We detect the presence of two stable rotated crystal domains that coexist in the structure. They are due to a change in the growth facet, which originates either from the island formation and merging in the initial stages of growth or lateral overgrowth. These domains have been visualized through 3D atomic models and confirmed with image simulations of the atomic scale electron micrographs. Density functional theory simulations describe the rotated domains' formation mechanism and demonstrate their lattice-matched epitaxial relation. In addition, the energies of the shallow states predicted closely agree with transition energies observed by experimental studies and offer a potential origin for these defect transitions. Our study represents an important step forward in the understanding of Zn3P2 and thus for the realisation of solar cells to respond to the present call for sustainable photovoltaic technology. © 2021 The Royal Society of Chemistry.


2020

  • 3D Ordering at the Liquid–Solid Polar Interface of Nanowires

    Zamani M., Imbalzano G., Tappy N., Alexander D.T.L., Martí-Sánchez S., Ghisalberti L., Ramasse Q.M., Friedl M., Tütüncüoglu G., Francaviglia L., Bienvenue S., Hébert C., Arbiol J., Ceriotti M., Fontcuberta i Morral A. Advanced Materials; 32 (38, 2001030) 2020. 10.1002/adma.202001030. IF: 27.398

    The nature of the liquid–solid interface determines the characteristics of a variety of physical phenomena, including catalysis, electrochemistry, lubrication, and crystal growth. Most of the established models for crystal growth are based on macroscopic thermodynamics, neglecting the atomistic nature of the liquid–solid interface. Here, experimental observations and molecular dynamics simulations are employed to identify the 3D nature of an atomic-scale ordering of liquid Ga in contact with solid GaAs in a nanowire growth configuration. An interplay between the liquid ordering and the formation of a new bilayer is revealed, which, contrary to the established theories, suggests that the preference for a certain polarity and polytypism is influenced by the atomic structure of the interface. The conclusions of this work open new avenues for the understanding of crystal growth, as well as other processes and systems involving a liquid–solid interface. © 2020 The Authors. Published by Wiley-VCH GmbH


  • Coherent Epitaxial Semiconductor-Ferromagnetic Insulator InAs/EuS Interfaces: Band Alignment and Magnetic Structure

    Liu Y., Luchini A., Martí-Sánchez S., Koch C., Schuwalow S., Khan S.A., Stankevič T., Francoual S., Mardegan J.R.L., Krieger J.A., Strocov V.N., Stahn J., Vaz C.A.F., Ramakrishnan M., Staub U., Lefmann K., Aeppli G., Arbiol J., Krogstrup P. ACS Applied Materials and Interfaces; 12 (7): 8780 - 8787. 2020. 10.1021/acsami.9b15034. IF: 8.758

    Hybrid semiconductor-ferromagnetic insulator heterostructures are interesting due to their tunable electronic transport, self-sustained stray field, and local proximitized magnetic exchange. In this work, we present lattice-matched hybrid epitaxy of semiconductor-ferromagnetic insulator InAs/EuS heterostructures and analyze the atomic-scale structure and their electronic and magnetic characteristics. The Fermi level at the InAs/EuS interface is found to be close to the InAs conduction band and in the band gap of EuS, thus preserving the semiconducting properties. Both neutron and X-ray reflectivity measurements show that the overall ferromagnetic component is mainly localized in the EuS thin film with a suppression of the Eu moment in the EuS layer nearest the InAs and magnetic moments outside the detection limits on the pure InAs side. This work presents a step toward realizing defect-free semiconductor-ferromagnetic insulator epitaxial hybrids for spin-lifted quantum and spintronic applications without external magnetic fields. Copyright © 2019 American Chemical Society.


  • Engineering grain boundaries at the 2D limit for the hydrogen evolution reaction

    He Y., Tang P., Hu Z., He Q., Zhu C., Wang L., Zeng Q., Golani P., Gao G., Fu W., Huang Z., Gao C., Xia J., Wang X., Wang X., Zhu C., Ramasse Q.M., Zhang A., An B., Zhang Y., Martí-Sánchez S., Morante J.R., Wang L., Tay B.K., Yakobson B.I., Trampert A., Zhang H., Wu M., Wang Q.J., Arbiol J., Liu Z. Nature Communications; 11 (1, 57) 2020. 10.1038/s41467-019-13631-2. IF: 12.121

    Atom-thin transition metal dichalcogenides (TMDs) have emerged as fascinating materials and key structures for electrocatalysis. So far, their edges, dopant heteroatoms and defects have been intensively explored as active sites for the hydrogen evolution reaction (HER) to split water. However, grain boundaries (GBs), a key type of defects in TMDs, have been overlooked due to their low density and large structural variations. Here, we demonstrate the synthesis of wafer-size atom-thin TMD films with an ultra-high-density of GBs, up to ~1012 cm−2. We propose a climb and drive 0D/2D interaction to explain the underlying growth mechanism. The electrocatalytic activity of the nanograin film is comprehensively examined by micro-electrochemical measurements, showing an excellent hydrogen-evolution performance (onset potential: −25 mV and Tafel slope: 54 mV dec−1), thus indicating an intrinsically high activation of the TMD GBs. © 2020, The Author(s).


  • GaAs nanoscale membranes: Prospects for seamless integration of III-Vs on silicon

    Raya A.M., Friedl M., Martí-Sánchez S., Dubrovskii V.G., Francaviglia L., Alén B., Morgan N., Tütüncüoglu G., Ramasse Q.M., Fuster D., Llorens J.M., Arbiol J., Fontcuberta I Morral A. Nanoscale; 12 (2): 815 - 824. 2020. 10.1039/c9nr08453c. IF: 6.895

    The growth of compound semiconductors on silicon has been widely sought after for decades, but reliable methods for defect-free combination of these materials have remained elusive. Recently, interconnected GaAs nanoscale membranes have been used as templates for the scalable integration of nanowire networks on III-V substrates. Here, we demonstrate how GaAs nanoscale membranes can be seamlessly integrated on silicon by controlling the density of nuclei in the initial stages of growth. We also correlate the absence or presence of defects with the existence of a single or multiple nucleation regime for the single membranes. Certain defects exhibit well-differentiated spectroscopic features that we identify with cathodoluminescence and micro-photoluminescence techniques. Overall, this work presents a new approach for the seamless integration of compound semiconductors on silicon. © 2019 The Royal Society of Chemistry.


  • Semiconductor-Ferromagnetic Insulator-Superconductor Nanowires: Stray Field and Exchange Field

    Liu Y., Vaitiekėnas S., Martí-Sánchez S., Koch C., Hart S., Cui Z., Kanne T., Khan S.A., Tanta R., Upadhyay S., Cachaza M.E., Marcus C.M., Arbiol J., Moler K.A., Krogstrup P. Nano Letters; 20 (1): 456 - 462. 2020. 10.1021/acs.nanolett.9b04187. IF: 11.238

    Nanowires can serve as flexible substrates for hybrid epitaxial growth on selected facets, allowing for the design of heterostructures with complex material combinations and geometries. In this work we report on hybrid epitaxy of freestanding vapor-liquid-solid grown and in-plane selective area grown semiconductor-ferromagnetic insulator-superconductor (InAs/EuS/Al) nanowire heterostructures. We study the crystal growth and complex epitaxial matching of wurtzite and zinc-blende InAs/rock-salt EuS interfaces as well as rock-salt EuS/face-centered cubic Al interfaces. Because of the magnetic anisotropy originating from the nanowire shape, the magnetic structure of the EuS phase is easily tuned into single magnetic domains. This effect efficiently ejects the stray field lines along the nanowires. With tunnel spectroscopy measurements of the density of states, we show that the material has a hard induced superconducting gap, and magnetic hysteretic evolution which indicates that the magnetic exchange fields are not negligible. These hybrid nanowires fulfill key material requirements for serving as a platform for spin-based quantum applications, such as scalable topological quantum computing. Copyright © 2019 American Chemical Society.


2019

  • Ballistic InSb Nanowires and Networks via Metal-Sown Selective Area Growth

    Aseev P., Wang G., Binci L., Singh A., Martí-Sánchez S., Botifoll M., Stek L.J., Bordin A., Watson J.D., Boekhout F., Abel D., Gamble J., Van Hoogdalem K., Arbiol J., Kouwenhoven L.P., De Lange G., Caroff P. Nano Letters; 19 (12): 9102 - 9111. 2019. 10.1021/acs.nanolett.9b04265. IF: 12.279

    Selective area growth is a promising technique to realize semiconductor-superconductor hybrid nanowire networks, potentially hosting topologically protected Majorana-based qubits. In some cases, however, such as the molecular beam epitaxy of InSb on InP or GaAs substrates, nucleation and selective growth conditions do not necessarily overlap. To overcome this challenge, we propose a metal-sown selective area growth (MS SAG) technique, which allows decoupling selective deposition and nucleation growth conditions by temporarily isolating these stages. It consists of three steps: (i) selective deposition of In droplets only inside the mask openings at relatively high temperatures favoring selectivity, (ii) nucleation of InSb under Sb flux from In droplets, which act as a reservoir of group III adatoms, done at relatively low temperatures, favoring nucleation of InSb, and (iii) homoepitaxy of InSb on top of the formed nucleation layer under a simultaneous supply of In and Sb fluxes at conditions favoring selectivity and high crystal quality. We demonstrate that complex InSb nanowire networks of high crystal and electrical quality can be achieved this way. We extract mobility values of 10※000-25※000 cm2 V-1 s-1 consistently from field-effect and Hall mobility measurements across single nanowire segments as well as wires with junctions. Moreover, we demonstrate ballistic transport in a 440 nm long channel in a single nanowire under a magnetic field below 1 T. We also extract a phase-coherent length of ∼8 μm at 50 mK in mesoscopic rings. © 2019 American Chemical Society.


  • High Magnetic Coercivity in Nanostructured Mn3O4 Thin Films Obtained by Chemical Vapor Deposition

    Bigiani L., Hassan M., Peddis D., Maccato C., Varvaro G., Sada C., Bontempi E., Martí-Sánchez S., Arbiol J., Barreca D. ACS Applied Nano Materials; 2 (3): 1704 - 1712. 2019. 10.1021/acsanm.9b00141. IF: 0.000

    Nanostructured α-Mn3O4 (haussmannite) thin films consisting of evenly interconnected nanoaggregates were prepared on Si(100) substrates by chemical vapor deposition from a Mn(II) diketonate-diamine precursor under different reaction atmospheres (dry vs wet O2) and total operating pressures. The combination of chemico-physical results obtained by the joint use of complementary techniques enabled us to demonstrate the obtainment of high-purity Mn3O4 materials free from other manganese oxide phases, characterized by controllable structural and morphological characteristics as a function of the adopted processing conditions. Magnetic properties were investigated by analyzing temperature dependence (i.e., field-cooled and zero-field-cooled measurements) and field-dependence of the magnetization behavior. The obtained films show bulk-like magnetic properties, together with extraordinarily high low-temperature in-plane coercivities (up to ∼1 T). The possibility to tailor these values by varying the content of microstructural defects may foster the implementation of the obtained films in eventual technological applications. © Copyright © 2019 American Chemical Society.


  • III-V Integration on Si(100): Vertical Nanospades

    Güniat L., Martí-Sánchez S., Garcia O., Boscardin M., Vindice D., Tappy N., Friedl M., Kim W., Zamani M., Francaviglia L., Balgarkashi A., Leran J.-B., Arbiol J., Fontcuberta I Morral A. ACS Nano; 13 (5): 5833 - 5840. 2019. 10.1021/acsnano.9b01546. IF: 13.903

    III-V integration on Si(100) is a challenge: controlled vertical vapor liquid solid nanowire growth on this platform has not been reported so far. Here we demonstrate an atypical GaAs vertical nanostructure on Si(100), coined nanospade, obtained by a nonconventional droplet catalyst pinning. The Ga droplet is positioned at the tip of an ultrathin Si pillar with a radial oxide envelope. The pinning at the Si/oxide interface allows the engineering of the contact angle beyond the Young-Dupré equation and the growth of vertical nanospades. Nanospades exhibit a virtually defect-free bicrystalline nature. Our growth model explains how a pentagonal twinning event at the initial stages of growth provokes the formation of the nanospade. The optical properties of the nanospades are consistent with the high crystal purity, making these structures viable for use in integration of optoelectronics on the Si(100) platform. © 2019 American Chemical Society.


  • Role of Boron and Phosphorus in Enhanced Electrocatalytic Oxygen Evolution by Nickel Borides and Nickel Phosphides

    Masa J., Andronescu C., Antoni H., Sinev I., Seisel S., Elumeeva K., Barwe S., Marti-Sanchez S., Arbiol J., Roldan Cuenya B., Muhler M., Schuhmann W. ChemElectroChem; 6 (1): 235 - 240. 2019. 10.1002/celc.201800669. IF: 3.975

    The modification of nickel with boron or phosphorus leads to significant enhancement of its electrocatalytic activity for the oxygen evolution reaction (OER). However, the precise role of the guest elements, B and P, in enhancing the OER of the host element (Ni) remains unclear. Herein, we present insight into the role of B and P in enhancing electrocatalysis of oxygen evolution by nickel borides and nickel phosphides. The apparent activation energy, Ea*, of electrocatalytic oxygen evolution on Ni2P was 78.4 kJ/mol, on Ni2B 65.4 kJ/mol, and on Ni nanoparticles 94.0 kJ/mol, thus revealing that both B and P affect the intrinsic activity of nickel. XPS data revealed shifts of −0.30 and 0.40 eV in the binding energy of the Ni 2p3/2 peak of Ni2B and Ni2P, respectively, with respect to that of pure Ni at 852.60 eV, thus indicating that B and P induce opposite electronic effects on the surface electronic structure of Ni. The origin of enhanced activity for oxygen evolution cannot, therefore, be attributed to such electronic modification or ligand effect. Severe changes induced on the nickel lattice, specifically, the Ni-Ni atomic order and interatomic distances (strain effect), by the presence of the guest atoms seem to be the dominant factors responsible for enhanced activity of oxygen evolution in nickel borides and nickel phosphides. © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim


  • Segregation scheme of indium in AlGaInAs nanowire shells

    Francaviglia L., Tütüncüoglu G., Martí-Sánchez S., Di Russo E., Escobar Steinvall S., Segura Ruiz J., Potts H., Friedl M., Rigutti L., Arbiol J., Fontcuberta I Morral A. Physical Review Materials; 3 (2, 023001) 2019. 10.1103/PhysRevMaterials.3.023001. IF: 2.926

    Quaternary alloys enable the independent optimization of different semiconductor properties, such as the separate tuning of the band gap and the lattice constant. Nanowire core-shell structures should allow a larger range of compositional tuning as strain can be accommodated in a more effective manner than in thin films. Still, the faceted structure of the nanowire may lead to local segregation effects. Here, we explore the incorporation of indium in AlGaAs shells up to 25%. In particular, we show the effect of In incorporation on the energy shift of the AlGaInAs single-photon emitters present in the shell. We observe a redshift up to 300 meV as a function of the group-III site fraction of In. We correlate the shift with segregation at the nanoscale. We find evidence of the segregation of the group-III elements at different positions in the nanowire, not observed before. We propose a model that takes into account the strain distribution in the nanowire shell and the adatom diffusion on the nanowire facets to explain the observations. This work provides novel insights on the segregation phenomena necessary to engineer the composition of multidinary alloys. © 2019 American Physical Society.


  • Selectivity Map for Molecular Beam Epitaxy of Advanced III-V Quantum Nanowire Networks

    Aseev P., Fursina A., Boekhout F., Krizek F., Sestoft J.E., Borsoi F., Heedt S., Wang G., Binci L., Martí-Sánchez S., Swoboda T., Koops R., Uccelli E., Arbiol J., Krogstrup P., Kouwenhoven L.P., Caroff P. Nano Letters; 19 (1): 218 - 227. 2019. 10.1021/acs.nanolett.8b03733. IF: 12.279

    Selective-area growth is a promising technique for enabling of the fabrication of the scalable III-V nanowire networks required to test proposals for Majorana-based quantum computing devices. However, the contours of the growth parameter window resulting in selective growth remain undefined. Herein, we present a set of experimental techniques that unambiguously establish the parameter space window resulting in selective III-V nanowire networks growth by molecular beam epitaxy. Selectivity maps are constructed for both GaAs and InAs compounds based on in situ characterization of growth kinetics on GaAs(001) substrates, where the difference in group III adatom desorption rates between the III-V surface and the amorphous mask area is identified as the primary mechanism governing selectivity. The broad applicability of this method is demonstrated by the successful realization of high-quality InAs and GaAs nanowire networks on GaAs, InP, and InAs substrates of both (001) and (111)B orientations as well as homoepitaxial InSb nanowire networks. Finally, phase coherence in Aharonov-Bohm ring experiments validates the potential of these crystals for nanoelectronics and quantum transport applications. This work should enable faster and better nanoscale crystal engineering over a range of compound semiconductors for improved device performance. © 2018 American Chemical Society.


  • The Role of Polarity in Nonplanar Semiconductor Nanostructures

    De La Mata M., Zamani R.R., Martí-Sánchez S., Eickhoff M., Xiong Q., Fontcuberta Morral A., Caroff P., Arbiol J. Nano Letters; 19 (6): 3396 - 3408. 2019. 10.1021/acs.nanolett.9b00459. IF: 12.279

    The lack of mirror symmetry in binary semiconductor compounds turns them into polar materials, where two opposite orientations of the same crystallographic direction are possible. Interestingly, their physical properties (e.g., electronic or photonic) and morphological features (e.g., shape, growth direction, and so forth) also strongly depend on the polarity. It has been observed that nanoscale materials tend to grow with a specific polarity, which can eventually be reversed for very specific growth conditions. In addition, polar-directed growth affects the defect density and topology and might induce eventually the formation of undesirable polarity inversion domains in the nanostructure, which in turn will affect the photonic and electronic final device performance. Here, we present a review on the polarity-driven growth mechanism at the nanoscale, combining our latest investigation with an overview of the available literature highlighting suitable future possibilities of polarity engineering of semiconductor nanostructures. The present study has been extended over a wide range of semiconductor compounds, covering the most commonly synthesized III-V (GaN, GaP, GaAs, GaSb, InN, InP, InAs, InSb) and II-VI (ZnO, ZnTe, CdS, CdSe, CdTe) nanowires and other free-standing nanostructures (tripods, tetrapods, belts, and membranes). This systematic study allowed us to explore the parameters that may induce polarity-dependent and polarity-driven growth mechanisms, as well as the polarity-related consequences on the physical properties of the nanostructures. © 2019 American Chemical Society.


2018

  • Colloidal synthesis of CsX nanocrystals (X = Cl, Br, I)

    Shaw P.J., Meyns M., Zuo Y., Grau-Carbonell A., Lagoudakis P.G., Charlton M.D.B., Martí-Sánchez S., Arbiol J., Cabot A., Kanaras A.G. Nanomaterials; 8 (7, 506) 2018. 10.3390/nano8070506. IF: 3.504

    A facile colloidal synthesis of highly ionic cesium halide nanocrystals is reported. Colloidal nanocrystals of CsI, CsCl and CsBr with unprecedentedly small dimensions are obtained using oleylammonium halides and cesium oleate as precursors. The ease and adaptability of our method enables its universalization for the formation of other highly ionic nanocrystals. © 2018 by the authors. Licensee MDPI, Basel, Switzerland.


  • Controllable vapor phase fabrication of F:Mn3O4 thin films functionalized with Ag and TiO2

    Bigiani L., Barreca D., Gasparotto A., Sada C., Martí-Sanchez S., Arbiol J., Maccato C. CrystEngComm; 20 (22): 3016 - 3024. 2018. 10.1039/c8ce00387d. IF: 3.304

    A facile two-step vapor phase synthetic approach is proposed for the fabrication of Mn3O4 thin films chemically modified with fluorine, and eventually functionalized with silver or titania. The adopted strategy exploits the initial chemical vapor deposition (CVD) of Mn3O4 on Si(100) substrates starting from a diamine diketonate Mn(ii) complex, followed by the controlled radio frequency (RF)-sputtering of silver or titania. Complementary analytical techniques were employed to investigate the crystallinity (X-ray diffraction), chemical composition (X-ray photoelectron spectroscopy, secondary ion mass spectrometry, energy dispersive X-ray spectroscopy), morphology and nano-organization (field emission-scanning electron microscopy, atomic force microscopy, transmission electron microscopy) of both pristine and functionalized manganese oxide thin films. Under the adopted operating conditions, the target Mn(ii) complex acted as a single-source precursor for both Mn and F, leading to the formation of phase-pure hausmannite Mn3O4 films characterized by a uniform in-depth fluorine content. In addition, the obtained results gave evidence of the formation of high purity Ag/F:Mn3O4 and TiO2/F:Mn3O4 composites with a close contact between the single constituents. This work outlines an amenable and efficient method for the vapor phase growth of composite Mn3O4-based thin films, which are favorable candidates for diverse technological applications, from photocatalysis to gas sensing. © 2018 The Royal Society of Chemistry.


  • Crystallographically Textured Nanomaterials Produced from the Liquid Phase Sintering of BixSb2-xTe3 Nanocrystal Building Blocks

    Liu Y., Zhang Y., Ortega S., Ibáñez M., Lim K.H., Grau-Carbonell A., Martí-Sánchez S., Ng K.M., Arbiol J., Kovalenko M.V., Cadavid D., Cabot A. Nano Letters; 18 (4): 2557 - 2563. 2018. 10.1021/acs.nanolett.8b00263. IF: 12.080

    Bottom-up approaches for producing bulk nanomaterials have traditionally lacked control over the crystallographic alignment of nanograins. This limitation has prevented nanocrystal-based nanomaterials from achieving optimized performances in numerous applications. Here we demonstrate the production of nanostructured BixSb2-xTe3 alloys with controlled stoichiometry and crystallographic texture through proper selection of the starting building blocks and the adjustment of the nanocrystal-to-nanomaterial consolidation process. In particular, we hot pressed disk-shaped BixSb2-xTe3 nanocrystals and tellurium nanowires using multiple pressure and release steps at a temperature above the tellurium melting point. We explain the formation of the textured nanomaterials though a solution-reprecipitation mechanism under a uniaxial pressure. Additionally, we further demonstrate these alloys to reach unprecedented thermoelectric figures of merit, up to ZT = 1.96 at 420 K, with an average value of ZTave = 1.77 for the record material in the temperature range 320-500 K, thus potentially allowing up to 60% higher energy conversion efficiencies than commercial materials. © 2018 American Chemical Society.


  • Field effect enhancement in buffered quantum nanowire networks

    Krizek F., Sestoft J.E., Aseev P., Marti-Sanchez S., Vaitiekenas S., Casparis L., Khan S.A., Liu Y., Stankevič T., Whiticar A.M., Fursina A., Boekhout F., Koops R., Uccelli E., Kouwenhoven L.P., Marcus C.M., Arbiol J., Krogstrup P. Physical Review Materials; 2 (9, 093401) 2018. 10.1103/PhysRevMaterials.2.093401.

    III-V semiconductor nanowires have shown great potential in various quantum transport experiments. However, realizing a scalable high-quality nanowire-based platform that could lead to quantum information applications has been challenging. Here, we study the potential of selective area growth by molecular beam epitaxy of InAs nanowire networks grown on GaAs-based buffer layers, where Sb is used as a surfactant. The buffered geometry allows for substantial elastic strain relaxation and a strong enhancement of field effect mobility. We show that the networks possess strong spin-orbit interaction and long phase-coherence lengths with a temperature dependence indicating ballistic transport. With these findings, and the compatibility of the growth method with hybrid epitaxy, we conclude that the material platform fulfills the requirements for a wide range of quantum experiments and applications. © 2018 American Physical Society.


  • Growth of Au-Pd2Sn Nanorods via Galvanic Replacement and Their Catalytic Performance on Hydrogenation and Sonogashira Coupling Reactions

    Nafria R., Luo Z., Ibáñez M., Martí-Sànchez S., Yu X., De La Mata M., Llorca J., Arbiol J., Kovalenko M.V., Grabulosa A., Muller G., Cabot A. Langmuir; 34 (36): 10634 - 10643. 2018. 10.1021/acs.langmuir.8b02023. IF: 3.789

    Colloidal Pd2Sn and Au-Pd2Sn nanorods (NRs) with tuned size were produced by the reduction of Pd and Sn salts in the presence of size- and shape-controlling agents and the posterior growth of Au tips through a galvanic replacement reaction. Pd2Sn and Au-Pd2Sn NRs exhibited high catalytic activity toward quasi-homogeneous hydrogenation of alkenes (styrene and 1-octene) and alkynes (phenylacetylene and 1-octyne) in dichloromethane. Au-Pd2Sn NRs showed higher activity than Pd2Sn for 1-octene, 1-octyne, and phenylacetylene. In Au-Pd2Sn heterostructures, X-ray photoelectron spectroscopy evidenced an electron donation from the Pd2Sn NR to the Au tips. Such heterostructures showed distinct catalytic behavior in the hydrogenation of compounds containing a triple bond such as tolan. This can be explained by the aurophilicity of triple bonds. To further study this effect, Pd2Sn and Au-Pd2Sn NRs were also tested in the Sonogashira coupling reaction between iodobenzene and phenylacetylene in N,N-dimethylformamide. At low concentration, this reaction provided the expected product, tolan. However, at high concentration, more reduced products such as stilbene and 1,2-diphenylethane were also obtained, even without the addition of H2. A mechanism for this unexpected reduction is proposed. Copyright © 2018 American Chemical Society.


  • High Thermoelectric Performance in Crystallographically Textured n-Type Bi2Te3- xSex Produced from Asymmetric Colloidal Nanocrystals

    Liu Y., Zhang Y., Lim K.H., Ibáñez M., Ortega S., Li M., David J., Martí-Sánchez S., Ng K.M., Arbiol J., Kovalenko M.V., Cadavid D., Cabot A. ACS Nano; 12 (7): 7174 - 7184. 2018. 10.1021/acsnano.8b03099. IF: 13.709

    In the present work, we demonstrate crystallographically textured n-type Bi2Te3-xSex nanomaterials with exceptional thermoelectric figures of merit produced by consolidating disk-shaped Bi2Te3-xSex colloidal nanocrystals (NCs). Crystallographic texture was achieved by hot pressing the asymmetric NCs in the presence of an excess of tellurium. During the hot press, tellurium acted both as lubricant to facilitate the rotation of NCs lying close to normal to the pressure axis and as solvent to dissolve the NCs approximately aligned with the pressing direction, which afterward recrystallize with a preferential orientation. NC-based Bi2Te3-xSex nanomaterials showed very high electrical conductivities associated with large charge carrier concentrations, n. We hypothesize that such large n resulted from the presence of an excess of tellurium during processing, which introduced a high density of donor TeBi antisites. Additionally, the presence in between grains of traces of elemental Te, a narrow band gap semiconductor with a work function well below Bi2Te3-xSex, might further contribute to increase n through spillover of electrons, while at the same time blocking phonon propagation and hole transport through the nanomaterial. NC-based Bi2Te3-xSex nanomaterials were characterized by very low thermal conductivities in the pressing direction, which resulted in ZT values up to 1.31 at 438 K in this direction. This corresponds to a ca. 40% ZT enhancement from commercial ingots. Additionally, high ZT values were extended over wider temperature ranges due to reduced bipolar contribution to the Seebeck coefficient and the thermal conductivity. Average ZT values up to 1.15 over a wide temperature range, 320 to 500 K, were measured, which corresponds to a ca. 50% increase over commercial materials in the same temperature range. Contrary to most previous works, highest ZT values were obtained in the pressing direction, corresponding to the c crystallographic axis, due to the predominance of the thermal conductivity reduction over the electrical conductivity difference when comparing the two crystal directions. © 2018 American Chemical Society.


  • Optical Analysis of Oxygen Self-Diffusion in Ultrathin CeO2 Layers at Low Temperatures

    Neuderth P., Hille P., Martí-Sánchez S., de la Mata M., Coll M., Arbiol J., Eickhoff M. Advanced Energy Materials; 8 (29, 1802120) 2018. 10.1002/aenm.201802120. IF: 21.875

    An optical in situ strategy for the analysis of oxygen diffusion in ultrathin ceria layers with a thickness of 2–10 nm at temperatures between 50 and 200 °C is presented, which allows for the determination of diffusion coefficients. This method is based on the sensitivity of the photoluminescence (PL) intensity of InGaN nanowires to adsorbed oxygen. The oxygen diffusion through an ultrathin CeO2 coating deposited on the InGaN nanowires is monitored by analyzing the transient PL behavior of the InGaN nanowires, which responds to changes of the oxygen concentration in the environment when the corresponding oxygen concentration is established at the CeO2/InGaN interface due to diffusion through the coating. Quantitative evaluation of the oxygen diffusion in CeO2 based on a model considering Langmuir Adsorption and recombination yields a diffusion coefficient D of (2.55 ± 0.05) × 10−16 cm2 s−1 at a temperature of 100 °C. Temperature-dependent measurements reveal an Arrhenius type behavior of D with an activation energy of (0.28 ± 0.04) eV. In contrast, no oxygen diffusion is detected for an ultrathin layer (≥5 nm) of Al2O3, which is known as a poor oxygen ion conductor within the analyzed temperature regime. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim


  • Optical emission of GaN/AlN quantum-wires-the role of charge transfer from a nanowire template

    Müßener J., Greif L.A.T., Kalinowski S., Callsen G., Hille P., Schörmann J., Wagner M.R., Schliwa A., Martí-Sánchez S., Arbiol J., Hoffmann A., Eickhoff M. Nanoscale; 10 (12): 5591 - 5598. 2018. 10.1039/c7nr08057c. IF: 7.233

    We show that one-dimensional (1d) GaN quantum-wires (QWRs) exhibit intense and spectrally sharp emission lines. These QWRs are realized in an entirely self-assembled growth process by molecular beam epitaxy (MBE) on the side facets of GaN/AlN nanowire (NW) heterostructures. Time-integrated and time-resolved photoluminescence (PL) data in combination with numerical calculations allow the identification and assignment of the manifold emission features to three different spatial recombination centers within the NWs. The recombination processes in the QWRs are driven by efficient charge carrier transfer effects between the different optically active regions, providing high intense QWR luminescence despite their small volume. This is deduced by a fast rise time of the QWR PL, which is similar to the fast decay-time of adjacent carrier reservoirs. Such processes, feeding the ultra-narrow QWRs with carriers from the relatively large NWs, can be the key feature towards the realization of future QWR-based devices. While processing of single quantum structures with diameters in the nm range presents a serious obstacle with respect to their integration into electronic or photonic devices, the QWRs presented here can be analyzed and processed using existing techniques developed for single NWs. © 2018 The Royal Society of Chemistry.


  • Optimizing the yield of A-polar GaAs nanowires to achieve defect-free zinc blende structure and enhanced optical functionality

    Zamani M., Tütüncüoglu G., Martí-Sánchez S., Francaviglia L., Güniat L., Ghisalberti L., Potts H., Friedl M., Markov E., Kim W., Leran J.-B., Dubrovskii V.G., Arbiol J., Fontcuberta I Morral A. Nanoscale; 10 (36): 17080 - 17091. 2018. 10.1039/c8nr05787g. IF: 7.233

    Compound semiconductors exhibit an intrinsic polarity, as a consequence of the ionicity of their bonds. Nanowires grow mostly along the (111) direction for energetic reasons. Arsenide and phosphide nanowires grow along (111)B, implying a group V termination of the (111) bilayers. Polarity engineering provides an additional pathway to modulate the structural and optical properties of semiconductor nanowires. In this work, we demonstrate for the first time the growth of Ga-assisted GaAs nanowires with (111)A-polarity, with a yield of up to ∼50%. This goal is achieved by employing highly Ga-rich conditions which enable proper engineering of the energies of A and B-polar surfaces. We also show that A-polarity growth suppresses the stacking disorder along the growth axis. This results in improved optical properties, including the formation of AlGaAs quantum dots with two orders or magnitude higher brightness. Overall, this work provides new grounds for the engineering of nanowire growth directions, crystal quality and optical functionality. © The Royal Society of Chemistry.


  • Passivation layers for nanostructured photoanodes: Ultra-thin oxides on InGaN nanowires

    Neuderth P., Hille P., Schörmann J., Frank A., Reitz C., Martí-Sánchez S., De La Mata M., Coll M., Arbiol J., Marschall R., Eickhoff M. Journal of Materials Chemistry A; 6 (2): 565 - 573. 2018. 10.1039/c7ta08071a. IF: 9.931

    An experimental strategy for systematically assessing the influence of surface passivation layers on the photocatalytic properties of nanowire photoanodes by combining photocurrent analysis, photoluminescence spectroscopy and high resolution transmission electron microscopy with a systematic variation of sample structure and the surrounding electrolyte is demonstrated. Following this approach we can separate the impact on recombination and transport processes of photogenerated carriers. We apply this strategy to analyze the influence of ultra-thin TiO2, CeO2 and Al2O3 coatings deposited by atomic layer deposition on the photoelectrochemical performance of InxGa1-xN/GaN nanowire (NW) photoelectrodes. The passivation of surface states results in an increase of the anodic photocurrent (PC) by a factor of 2.5 for the deposition of 5 nm TiO2. In contrast, the PC is reduced for CeO2- and Al2O3-coated NWs due to enhanced defect recombination in the passivation layer or increased band discontinuities. Furthermore, photoelectrochemical oxidation of the InxGa1-xN/GaN NW photoelectrode is attenuated by the TiO2 layer and completely suppressed for a layer thickness of 7 nm or more. Due to efficient charge transfer from the InxGa1-xN NW core a stable TiO2-covered photoanode with visible light excitation is realized. © 2018 The Royal Society of Chemistry.


  • Selective-Area-Grown Semiconductor-Superconductor Hybrids: A Basis for Topological Networks

    Vaitiekenas S., Whiticar A.M., Deng M.-T., Krizek F., Sestoft J.E., Palmstrøm C.J., Marti-Sanchez S., Arbiol J., Krogstrup P., Casparis L., Marcus C.M. Physical Review Letters; 121 (14, 147701) 2018. 10.1103/PhysRevLett.121.147701. IF: 8.839

    We introduce selective area grown hybrid InAs/Al nanowires based on molecular beam epitaxy, allowing arbitrary semiconductor-superconductor networks containing loops and branches. Transport reveals a hard induced gap and unpoisoned 2e-periodic Coulomb blockade, with temperature dependent 1e features in agreement with theory. Coulomb peak spacing in parallel magnetic field displays overshoot, indicating an oscillating discrete near-zero subgap state consistent with device length. Finally, we investigate a loop network, finding strong spin-orbit coupling and a coherence length of several microns. These results demonstrate the potential of this platform for scalable topological networks among other applications. © 2018 American Physical Society.


  • Supported Mn3O4 Nanosystems for Hydrogen Production through Ethanol Photoreforming

    Barreca D., Bigiani L., Monai M., Carraro G., Gasparotto A., Sada C., Martí-Sanchez S., Grau-Carbonell A., Arbiol J., Maccato C., Fornasiero P. Langmuir; 34 (15): 4568 - 4574. 2018. 10.1021/acs.langmuir.8b00642. IF: 3.789

    Photoreforming promoted by metal oxide nanophotocatalysts is an attractive route for clean and sustainable hydrogen generation. In the present work, we propose for the first time the use of supported Mn3O4 nanosystems, both pure and functionalized with Au nanoparticles (NPs), for hydrogen generation by photoreforming. The target oxide systems, prepared by chemical vapor deposition (CVD) and decorated with gold NPs by radio frequency (RF) sputtering, were subjected to a thorough chemico-physical characterization and utilized for a proof-of-concept H2 generation in aqueous ethanolic solutions under simulated solar illumination. Pure Mn3O4 nanosystems yielded a constant hydrogen production rate of 10 mmol h-1 m-2 even for irradiation times up to 20 h. The introduction of Au NPs yielded a significant enhancement in photocatalytic activity, which decreased as a function of irradiation time. The main phenomena causing the Au-containing photocatalyst deactivation have been investigated by morphological and compositional analysis, providing important insights for the design of Mn3O4-based photocatalysts with improved performances. © 2018 American Chemical Society.


  • Template-Assisted Scalable Nanowire Networks

    Friedl M., Cerveny K., Weigele P., Tütüncüoglu G., Martí-Sánchez S., Huang C., Patlatiuk T., Potts H., Sun Z., Hill M.O., Güniat L., Kim W., Zamani M., Dubrovskii V.G., Arbiol J., Lauhon L.J., Zumbühl D.M., Fontcuberta Morral A.I. Nano Letters; 18 (4): 2666 - 2671. 2018. 10.1021/acs.nanolett.8b00554. IF: 12.080

    Topological qubits based on Majorana Fermions have the potential to revolutionize the emerging field of quantum computing by making information processing significantly more robust to decoherence. Nanowires are a promising medium for hosting these kinds of qubits, though branched nanowires are needed to perform qubit manipulations. Here we report a gold-free templated growth of III-V nanowires by molecular beam epitaxy using an approach that enables patternable and highly regular branched nanowire arrays on a far greater scale than what has been reported thus far. Our approach relies on the lattice-mismatched growth of InAs on top of defect-free GaAs nanomembranes yielding laterally oriented, low-defect InAs and InGaAs nanowires whose shapes are determined by surface and strain energy minimization. By controlling nanomembrane width and growth time, we demonstrate the formation of compositionally graded nanowires with cross-sections less than 50 nm. Scaling the nanowires below 20 nm leads to the formation of homogeneous InGaAs nanowires, which exhibit phase-coherent, quasi-1D quantum transport as shown by magnetoconductance measurements. These results are an important advance toward scalable topological quantum computing. © 2018 American Chemical Society.


2017

  • Solution-based synthesis and processing of Sn- and Bi-doped Cu3SbSe4 nanocrystals, nanomaterials and ring-shaped thermoelectric generators

    Liu Y., García G., Ortega S., Cadavid D., Palacios P., Lu J., Ibáñez M., Xi L., De Roo J., López A.M., Martí-Sánchez S., Cabezas I., Mata M.D.L., Luo Z., Dun C., Dobrozhan O., Carroll D.L., Zhang W., Martins J., Kovalenko M.V., Arbiol J., Noriega G., Song J., Wahnón P., Cabot A. Journal of Materials Chemistry A; 5 (6): 2592 - 2602. 2017. 10.1039/c6ta08467b. IF: 8.867

    Copper-based chalcogenides that comprise abundant, low-cost, and environmental friendly elements are excellent materials for a number of energy conversion applications, including photovoltaics, photocatalysis, and thermoelectrics (TE). In such applications, the use of solution-processed nanocrystals (NCs) to produce thin films or bulk nanomaterials has associated several potential advantages, such as high material yield and throughput, and composition control with unmatched spatial resolution and cost. Here we report on the production of Cu3SbSe4 (CASe) NCs with tuned amounts of Sn and Bi dopants. After proper ligand removal, as monitored by nuclear magnetic resonance and infrared spectroscopy, these NCs were used to produce dense CASe bulk nanomaterials for solid state TE energy conversion. By adjusting the amount of extrinsic dopants, dimensionless TE figures of merit (ZT) up to 1.26 at 673 K were reached. Such high ZT values are related to an optimized carrier concentration by Sn doping, a minimized lattice thermal conductivity due to efficient phonon scattering at point defects and grain boundaries, and to an increase of the Seebeck coefficient obtained by a modification of the electronic band structure with Bi doping. Nanomaterials were further employed to fabricate ring-shaped TE generators to be coupled to hot pipes, which provided 20 mV and 1 mW per TE element when exposed to a 160 °C temperature gradient. The simple design and good thermal contact associated with the ring geometry and the potential low cost of the material solution processing may allow the fabrication of TE generators with short payback times. © The Royal Society of Chemistry.


  • Surface-Guided Core-Shell ZnSe@ZnTe Nanowires as Radial p-n Heterojunctions with Photovoltaic Behavior

    Oksenberg E., Martí-Sánchez S., Popovitz-Biro R., Arbiol J., Joselevich E. ACS Nano; 11 (6): 6155 - 6166. 2017. 10.1021/acsnano.7b02199. IF: 13.942

    The organization of nanowires on surfaces remains a major obstacle toward their large-scale integration into functional devices. Surface-material interactions have been used, with different materials and substrates, to guide horizontal nanowires during their growth into well-organized assemblies, but the only guided nanowire heterostructures reported so far are axial and not radial. Here, we demonstrate the guided growth of horizontal core-shell nanowires, specifically of ZnSe@ZnTe, with control over their crystal phase and crystallographic orientations. We exploit the directional control of the guided growth for the parallel production of multiple radial p-n heterojunctions and probe their optoelectronic properties. The devices exhibit a rectifying behavior with photovoltaic characteristics upon illumination. Guided nanowire heterostructures enable the bottom-up assembly of complex semiconductor structures with controlled electronic and optoelectronic properties. © 2017 American Chemical Society.


2016

  • Fe3O4@NiFexOy Nanoparticles with Enhanced Electrocatalytic Properties for Oxygen Evolution in Carbonate Electrolyte

    Luo Z., Martí-Sànchez S., Nafria R., Joshua G., De La Mata M., Guardia P., Flox C., Martínez-Boubeta C., Simeonidis K., Llorca J., Morante J.R., Arbiol J., Ibáñez M., Cabot A. ACS Applied Materials and Interfaces; 8 (43): 29461 - 29469. 2016. 10.1021/acsami.6b09888. IF: 7.145

    The design and engineering of earth-abundant catalysts that are both cost-effective and highly active for water splitting are crucial challenges in a number of energy conversion and storage technologies. In this direction, herein we report the synthesis of Fe3O4@NiFexOy core-shell nanoheterostructures and the characterization of their electrocatalytic performance toward the oxygen evolution reaction (OER). Such nanoparticles (NPs) were produced by a two-step synthesis procedure involving the colloidal synthesis of Fe3O4 nanocubes with a defective shell and the posterior diffusion of nickel cations within this defective shell. Fe3O4@NiFexOy NPs were subsequently spin-coated over ITO-covered glass and their electrocatalytic activity toward water oxidation in carbonate electrolyte was characterized. Fe3O4@NiFexOy catalysts reached current densities above 1 mA/cm2 with a 410 mV overpotential and Tafel slopes of 48 mV/dec, which is among the best electrocatalytic performances reported in carbonate electrolyte. © 2016 American Chemical Society.


  • Thermoelectric properties of semiconductor-metal composites produced by particle blending

    Liu Y., Cadavid D., Ibáñez M., Ortega S., Martí-Sánchez S., Dobrozhan O., Kovalenko M.V., Arbiol J., Cabot A. APL Materials; 4 (10, 104813) 2016. 10.1063/1.4961679. IF: 4.323

    In the quest for more efficient thermoelectric material able to convert thermal to electrical energy and vice versa, composites that combine a semiconductor host having a large Seebeck coefficient with metal nanodomains that provide phonon scattering and free charge carriers are particularly appealing. Here, we present our experimental results on the thermal and electrical transport properties of PbS-metal composites produced by a versatile particle blending procedure, and where the metal work function allows injecting electrons to the intrinsic PbS host. We compare the thermoelectric performance of composites with microcrystalline or nanocrystalline structures. The electrical conductivity of the microcrystalline host can be increased several orders of magnitude with the metal inclusion, while relatively high Seebeck coefficient can be simultaneously conserved. On the other hand, in nanostructured materials, the host crystallites are not able to sustain a band bending at its interface with the metal, becoming flooded with electrons. This translates into even higher electrical conductivities than the microcrystalline material, but at the expense of lower Seebeck coefficient values. © 2016 Author(s).