Staff directory Marianna Sledzinska

Publications

2018

  • Mechanisms behind the enhancement of thermal properties of graphene nanofluids

    Rodríguez-Laguna M.R., Castro-Alvarez A., Sledzinska M., Maire J., Costanzo F., Ensing B., Pruneda M., Ordejón P., Sotomayor Torres C.M., Gómez-Romero P., Chávez-Ángel E. Nanoscale; 10 (32): 15402 - 15409. 2018. 10.1039/c8nr02762e.

    While the dispersion of nanomaterials is known to be effective in enhancing the thermal conductivity and specific heat capacity of fluids, the mechanisms behind this enhancement remain to be elucidated. Herein, we report on highly stable, surfactant-free graphene nanofluids, based on N,N-dimethylacetamide (DMAc) and N,N-dimethylformamide (DMF), with enhanced thermal properties. An increase of up to 48% in thermal conductivity and 18% in specific heat capacity was measured. The blue shift of several Raman bands with increasing graphene concentration in DMF indicates that there is a modification in the vibrational energy of the bonds associated with these modes, affecting all the molecules in the liquid. This result indicates that graphene has the ability to affect solvent molecules at long-range, in terms of vibrational energy. Density functional theory and molecular dynamics simulations were used to gather data on the interaction between graphene and solvent, and to investigate a possible order induced by graphene on the solvent. The simulations showed a parallel orientation of DMF towards graphene, favoring π-π stacking. Furthermore, a local order of DMF molecules around graphene was observed suggesting that both this special kind of interaction and the induced local order may contribute to the enhancement of the fluid's thermal properties. © The Royal Society of Chemistry.


2017

  • Elastic Properties of Few Nanometers Thick Polycrystalline MoS2 Membranes: A Nondestructive Study

    Graczykowski B., Sledzinska M., Placidi M., Saleta Reig D., Kasprzak M., Alzina F., Sotomayor Torres C.M. Nano Letters; 17 (12): 7647 - 7651. 2017. 10.1021/acs.nanolett.7b03669. IF: 12.712

    The performance gain-oriented nanostructurization has opened a new pathway for tuning mechanical features of solid matter vital for application and maintained performance. Simultaneously, the mechanical evaluation has been pushed down to dimensions way below 1 μm. To date, the most standard technique to study the mechanical properties of suspended 2D materials is based on nanoindentation experiments. In this work, by means of micro-Brillouin light scattering we determine the mechanical properties, that is, Young modulus and residual stress, of polycrystalline few nanometers thick MoS2 membranes in a simple, contact-less, nondestructive manner. The results show huge elastic softening compared to bulk MoS2, which is correlated with the sample morphology and the residual stress. © 2017 American Chemical Society.


  • Mechanical oscillations in lasing microspheres

    Toncelli A., Capuj N.E., Garrido B., Sledzinska M., Sotomayor-Torres C.M., Tredicucci A., Navarro-Urrios D. Journal of Applied Physics; 122 (5, 053101) 2017. 10.1063/1.4997182. IF: 2.068

    We investigate the feasibility of activating coherent mechanical oscillations in lasing microspheres by modulating the laser emission at a mechanical eigenfrequency. To this aim, 1.5%Nd3+:Barium- Titanium-Silicate microspheres with diameters around 50 lm were used as high quality factor (Q>106) whispering gallery mode lasing cavities. We have implemented a pump-and-probe technique in which the pump laser used to excite the Nd3+ ions is focused on a single microsphere with a microscope objective and a probe laser excites a specific optical mode with the evanescent field of a tapered fibre. The studied microspheres show monomode and multi-mode lasing action, which can be modulated in the best case up to 10 MHz. We have optically transduced thermally activated mechanical eigenmodes appearing in the 50-70MHz range, the frequency of which decreases with increasing the size of the microspheres. In a pump-and-probe configuration, we observed modulation of the probe signal up to the maximum pump modulation frequency of our experimental setup, i.e., 20 MHz. This modulation decreases with frequency and is unrelated to lasing emission, pump scattering, or thermal effects. We associate this effect to free-carrier-dispersion induced by multiphoton pump light absorption. On the other hand, we conclude that, in our current experimental conditions, it was not possible to resonantly excite the mechanical modes. Finally, we discuss on how to overcome these limitations by increasing the modulation frequency of the lasing emission and decreasing the frequency of the mechanical eigenmodes displaying a strong degree of optomechanical coupling.


  • Nonlinear dynamics and chaos in an optomechanical beam

    Navarro-Urrios D., Capuj N.E., Colombano M.F., Garciá P.D., Sledzinska M., Alzina F., Griol A., Martínez A., Sotomayor-Torres C.M. Nature Communications; 8 ( 14965) 2017. 10.1038/ncomms14965. IF: 12.124

    Optical nonlinearities, such as thermo-optic mechanisms and free-carrier dispersion, are often considered unwelcome effects in silicon-based resonators and, more specifically, optomechanical cavities, since they affect, for instance, the relative detuning between an optical resonance and the excitation laser. Here, we exploit these nonlinearities and their intercoupling with the mechanical degrees of freedom of a silicon optomechanical nanobeam to unveil a rich set of fundamentally different complex dynamics. By smoothly changing the parameters of the excitation laser we demonstrate accurate control to activate two- A nd four-dimensional limit cycles, a period-doubling route and a six-dimensional chaos. In addition, by scanning the laser parameters in opposite senses we demonstrate bistability and hysteresis between two- A nd four-dimensional limit cycles, between different coherent mechanical states and between four-dimensional limit cycles and chaos. Our findings open new routes towards exploiting silicon-based optomechanical photonic crystals as a versatile building block to be used in neurocomputational networks and for chaos-based applications. © 2017 The Author(s).


  • 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.


  • Thermal conductivity and air-mediated losses in periodic porous silicon membranes at high temperatures

    Graczykowski B., El Sachat A., Reparaz J.S., Sledzinska M., Wagner M.R., Chavez-Angel E., Wu Y., Volz S., Wu Y., Alzina F., Sotomayor Torres C.M. Nature Communications; 8 (1, 415) 2017. 10.1038/s41467-017-00115-4. IF: 12.124

    Heat conduction in silicon can be effectively engineered by means of sub-micrometre porous thin free-standing membranes. Tunable thermal properties make these structures good candidates for integrated heat management units such as waste heat recovery, rectification or efficient heat dissipation. However, possible applications require detailed thermal characterisation at high temperatures which, up to now, has been an experimental challenge. In this work we use the contactless two-laser Raman thermometry to study heat dissipation in periodic porous membranes at high temperatures via lattice conduction and air-mediated losses. We find the reduction of the thermal conductivity and its temperature dependence closely correlated with the structure feature size. On the basis of two-phonon Raman spectra, we attribute this behaviour to diffuse (incoherent) phonon-boundary scattering. Furthermore, we investigate and quantify the heat dissipation via natural air-mediated cooling, which can be tuned by engineering the porosity. © 2017 The Author(s).


2016

  • Fabrication of phononic crystals on free-standing silicon membranes

    Sledzinska M., Graczykowski B., Alzina F., Santiso Lopez J., Sotomayor Torres C.M. Microelectronic Engineering; 149: 41 - 45. 2016. 10.1016/j.mee.2015.09.004. IF: 1.277

    Free-standing Si films have been and remain an excellent example to study experimentally the effect of the reduction of the characteristic size on the phonon dispersion relation. A step further in geometrical complexity and, therefore, in increasing the control and manipulation of phonons is achieved by introducing periodicity in the medium to form phononic crystals. Here we report on the development of the fabrication process of large-area, solid-air and solid-solid two-dimensional phononic crystals, directly on free-standing, single crystalline silicon membranes. The patterning of the membranes involved electron-beam lithography and reactive ion etching for holes or metal evaporation and lift-off for pillars. The fabrication was possible due to the external strain induced on the membrane in order to reduce the buckling, which is typically found in large area free-standing structures. As a result, we obtained 250 nm thick structured membranes with patterned areas up to 100 × 100 μm, feature size between 100 and 300 nm and periodicity between 300 and 500 nm. The changes in dispersion relations of hypersonic acoustic phonons due to nanopatterning in free-standing silicon membranes were measured by Brillouin light scattering and the results were compared with numerical calculations by finite elements method. Information on phonon dispersion relation combined with a reliable fabrication process for large-scale structures opens a way for phonon engineering in more complex devices. © 2015 Elsevier B.V. All rights reserved.


  • Measurement and modeling of the effective thermal conductivity of sintered silver pastes

    Ordonez-Miranda J., Hermens M., Nikitin I., Kouznetsova V.G., Van Der Sluis O., Ras M.A., Reparaz J.S., Wagner M.R., Sledzinska M., Gomis-Bresco J., Sotomayor Torres C.M., Wunderle B., Volz S. International Journal of Thermal Sciences; 108: 185 - 194. 2016. 10.1109/THERMINIC.2015.7389630. IF: 2.769

    The effective thermal conductivity of sintered porous pastes of silver is modeled through two theoretical methods and measured by means of three experimental techniques. The first model is based on the differential effective medium theory and provides a simple analytical description considering the air pores like ellipsoidal voids of different sizes, while the second one arises from the analysis of the scanning-electron-microscope images of the paste cross-sections through the finite element method. The predictions of both approaches are consistent with each other and show that the reduction of the thermal conductivity of porous pastes can be minimized with spherical pores and maximized with pancake-shaped ones, which are the most efficient to block the thermal conducting pathways. A thermal conductivity of 151.6 W/m K is numerically determined for a sintered silver sample with 22% of porosity. This thermal conductivity agrees quite well with the one measured by the Lateral Thermal Interface Material Analysis for a suspended sample and matches, within an experimental uncertainty smaller than 16%, with the values obtained by means of Raman thermometry and the 3u technique, for two samples buried in a silicon chip. The consistence between our theoretical and experimental results demonstrates the good predictive performance of our theoretical models to describe the thermal behavior of porous thermal interface materials and to guide their engineering with a desired thermal conductivity. © 2016 Elsevier Masson SAS.


  • 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.


  • Thermal transport in suspended silicon membranes measured by laser-induced transient gratings

    Vega-Flick A., Duncan R.A., Eliason J.K., Cuffe J., Johnson J.A., Peraud J.-P.M., Zeng L., Lu Z., Maznev A.A., Wang E.N., Alvarado-Gil J.J., Sledzinska M., Sotomayor Torres C.M., Chen G., Nelson K.A. AIP Advances; 6 (12, 121903) 2016. 10.1063/1.4968610. IF: 1.444

    Studying thermal transport at the nanoscale poses formidable experimental challenges due both to the physics of the measurement process and to the issues of accuracy and reproducibility. The laser-induced transient thermal grating (TTG) technique permits non-contact measurements on nanostructured samples without a need for metal heaters or any other extraneous structures, offering the advantage of inherently high absolute accuracy. We present a review of recent studies of thermal transport in nanoscale silicon membranes using the TTG technique. An overview of the methodology, including an analysis of measurements errors, is followed by a discussion of new findings obtained from measurements on both "solid" and nanopatterned membranes. The most important results have been a direct observation of non-diffusive phonon-mediated transport at room temperature and measurements of thickness-dependent thermal conductivity of suspended membranes across a wide thickness range, showing good agreement with first-principles-based theory assuming diffuse scattering at the boundaries. Measurements on a membrane with a periodic pattern of nanosized holes (135nm) indicated fully diffusive transport and yielded thermal diffusivity values in agreement with Monte Carlo simulations. Based on the results obtained to-date, we conclude that room-temperature thermal transport in membrane-based silicon nanostructures is now reasonably well understood. © 2016 Author(s).


  • Two-Dimensional Phononic Crystals: Disorder Matters

    Wagner M.R., Graczykowski B., Reparaz J.S., El Sachat A., Sledzinska M., Alzina F., Sotomayor Torres C.M. Nano Letters; 16 (9): 5661 - 5668. 2016. 10.1021/acs.nanolett.6b02305. IF: 13.779

    The design and fabrication of phononic crystals (PnCs) hold the key to control the propagation of heat and sound at the nanoscale. However, there is a lack of experimental studies addressing the impact of order/disorder on the phononic properties of PnCs. Here, we present a comparative investigation of the influence of disorder on the hypersonic and thermal properties of two-dimensional PnCs. PnCs of ordered and disordered lattices are fabricated of circular holes with equal filling fractions in free-standing Si membranes. Ultrafast pump and probe spectroscopy (asynchronous optical sampling) and Raman thermometry based on a novel two-laser approach are used to study the phononic properties in the gigahertz (GHz) and terahertz (THz) regime, respectively. Finite element method simulations of the phonon dispersion relation and three-dimensional displacement fields furthermore enable the unique identification of the different hypersonic vibrations. The increase of surface roughness and the introduction of short-range disorder are shown to modify the phonon dispersion and phonon coherence in the hypersonic (GHz) range without affecting the room-temperature thermal conductivity. On the basis of these findings, we suggest a criteria for predicting phonon coherence as a function of roughness and disorder. © 2016 American Chemical Society.


2015

  • A diffractometer for quality control in nano fabrication processing based on subwavelength diffraction

    Kreuzer M., Gomis Bresco J., Sledzinska M., Sotomayor Torres C.M. Proceedings of SPIE - The International Society for Optical Engineering; 9424 (942426) 2015. 10.1117/12.2085924. IF: 0.000

    Mass production of nanostructured surfaces relies on the periodic repetition of micrometre scale patterns. A unit cell with nanometre features in the micrometre size range is repeated thousands of times. The ensemble can used as a diffraction grating for visible light. The relative intensity distribution of the diffraction orders is characteristic for the grating and sensitive to nanometre scale changes. A newly designed subwavelength diffraction setup allows the measurement in real time of the diffraction pattern of an illuminated polymer grating with only one detector image. The setup records diffraction patterns of, for example, polymer gratings with intentionally low scattering contrast and line features ranging from 610 to 80 nm. Thus, sub-100 nm features can be traced. The comparison of the measured diffraction patterns with simulated patterns allows to sense nanometre scale deviations from fabrication goals. © 2015 SPIE.


  • In-line metrology setup for periodic nanostructures based on sub-wavelength diffraction

    Kreuzer M., Gomis Bresco J., Sledzinska M., Sotomayor Torres C.M. Proceedings of SPIE - The International Society for Optical Engineering; 9628 ( 96281Q) 2015. 10.1117/12.2191346. IF: 0.000

    The analysis of diffracted light from periodic structures is shown to be a versatile metrology technique applicable to inline metrology for periodic nanostructures. We show that 10 nm changes in periodic structures can be traced optically by means of sub-wavelength diffraction. Polymer gratings were fabricated by electron beam lithography. The gratings have a common periodicity of 6 μm, but different line width, ranging from 370 to 550 nm in 10 nm steps. A comparison between the resulting diffraction patterns shows marked differences in intensity which are used to sense nanometre scale deviations in periodic structures. © 2015 SPIE.


  • Phonon dispersion in hypersonic two-dimensional phononic crystal membranes

    Graczykowski B., Sledzinska M., Alzina F., Gomis-Bresco J., Reparaz J.S., Wagner M.R., Sotomayor Torres C.M. Physical Review B - Condensed Matter and Materials Physics; 91 (7, 075414) 2015. 10.1103/PhysRevB.91.075414. IF: 3.736

    We investigate experimentally and theoretically the acoustic phonon propagation in two-dimensional phononic crystal membranes. Solid-air and solid-solid phononic crystals were made of square lattices of holes and Au pillars in and on 250 nm thick single crystalline Si membrane, respectively. The hypersonic phonon dispersion was investigated using Brillouin light scattering. Volume reduction (holes) or mass loading (pillars) accompanied with second-order periodicity and local resonances are shown to significantly modify the propagation of thermally activated GHz phonons. We use numerical modeling based on the finite element method to analyze the experimental results and determine polarization, symmetry, or three-dimensional localization of observed modes. © 2015 American Physical Society.


  • Tuning Thermal Transport in Ultrathin Silicon Membranes by Surface Nanoscale Engineering

    Neogi S., Reparaz J.S., Pereira L.F.C., Graczykowski B., Wagner M.R., Sledzinska M., Shchepetov A., Prunnila M., Ahopelto J., Sotomayor-Torres C.M., Donadio D. ACS Nano; 9 (4): 3820 - 3828. 2015. 10.1021/nn506792d. IF: 12.881

    A detailed understanding of the connections of fabrication and processing to structural and thermal properties of low-dimensional nanostructures is essential to design materials and devices for phononics, nanoscale thermal management, and thermoelectric applications. Silicon provides an ideal platform to study the relations between structure and heat transport since its thermal conductivity can be tuned over 2 orders of magnitude by nanostructuring. Combining realistic atomistic modeling and experiments, we unravel the origin of the thermal conductivity reduction in ultrathin suspended silicon membranes, down to a thickness of 4 nm. Heat transport is mostly controlled by surface scattering: rough layers of native oxide at surfaces limit the mean free path of thermal phonons below 100 nm. Removing the oxide layers by chemical processing allows us to tune the thermal conductivity over 1 order of magnitude. Our results guide materials design for future phononic applications, setting the length scale at which nanostructuring affects thermal phonons most effectively. © 2015 American Chemical Society.


2014

  • Hypersonic phonon propagation in one-dimensional surface phononic crystal

    Graczykowski, B.; Sledzinska, M.; Kehagias, N.; Alzina, F.; Reparaz, J.S.; Sotomayor Torres, C.M. Applied Physics Letters; 2014. 10.1063/1.4870045. IF: 3.515