Critical angle for interfacial phonon scattering: Results from ab initio lattice dynamics calculations

Thermal boundary resistance is a critical quantity that controls heat transfer at the nanoscale, which is primarily related to interfacial phonon scattering. Here, we combine lattice dynamics calculations and inputs from first principles ab initio simulations to predict phonon transmission at the Si/Ge interface as a function of both the phonon frequency and the phonon wavevector. This technique allows us to determine the overall thermal transmission coefficient as a function of the phonon scattering direction and frequency. Our results show that the thermal energy transmission is highly anisotropic, while thermal energy reflection is almost isotropic. In addition, we found the existence of a global critical angle of transmission beyond which almost no thermal energy is transmitted. This critical angle around 50 degrees is found to be almost independent of the interaction range between Si and Ge, the interfacial bonding strength, and the temperature above 30 K. We interpret these results by carrying out a spectral and angular analysis of the phonon transmission coefficient and differential thermal boundary conductance

Enhancing the superconducting transition temperature of BaSi2 by structural tuning

We present a joint experimental and theoretical study of the superconducting phase of the layered binary silicide BaSi2. Compared with the layered AlB2 structure of graphite or diboride-like superconductors, in the hexagonal structure of binary silicides the sp3 arrangement of silicon atoms leads to corrugated sheets. Through a high-pressure synthesis procedure we are able to modify the buckling of these sheets, obtaining the enhancement of the superconducting transition temperature from 4 K to 8.7 K when the silicon planes flatten out. By performing ab-initio calculations based on density functional theory we explain how the electronic and phononic properties of the system are strongly affected by changes in the buckling. This mechanism is likely present in other intercalated layered superconductors, opening the way to the tuning of superconductivity through the control of internal structural parameters.Comment: Submitte

Reduced phase space of heat-carrying acoustic phonons in single-crystalline InTe

Chalcogenide semiconductors and semimetals are a fertile class of efficient thermoelectric materials, which, in most cases, exhibit very low lattice thermal conductivity κph despite lacking a complex crystal structure such as the tetragonal binary compound InTe. Our measurements of κph(T) in single-crystalline InTe along the c axis show that κph exhibits a smooth temperature dependence upon cooling to about 50 K, the temperature below which a strong rise typical for dielectric compounds is observed. Using a combination of first-principles calculations, inelastic neutron scattering (INS), and low-temperature specific heat and transport properties measurements on single-crystalline InTe, we show that the phonon spectrum exhibits well-defined acoustic modes, the energy dispersions of which are constrained to low energies due to distributions of dispersionless, optical modes, which are responsible for a broad double peak structure in the low-temperature specific heat. The latter are assigned to the dynamics of In+ cations in tunnels formed by edge-sharing (In3+Te42−)− tetrahedra chains, the atomic thermal displacement parameters of which, probed as a function of temperature by means of single-crystal x-ray diffraction, suggest the existence of a complex energy potential. Indeed, the In+-weighted optical modes are not observed by INS, which is ascribed to the anharmonic broadening of their energy profiles. While the low κph value of 1.2Wm−1K−1 at 300 K originates from the limited energy range available for acoustic phonons, we show that the underlying mechanism is specific to InTe and argue that it is likely related to the presence of local disorder induced by the In+ sit

The crystal structure of cold compressed graphite

Through a systematic structural search we found an allotrope of carbon with Cmmm symmetry which we predict to be more stable than graphite for pressures above 10 GPa. This material, which we refer to as Z-carbon, is formed by pure sp3 bonds and is the only carbon allotrope which provides an excellent match to unexplained features in experimental X-ray diffraction and Raman spectra of graphite under pressure. The transition from graphite to Z-carbon can occur through simple sliding and buckling of graphene sheets. Our calculations predict that Z-carbon is a transparent wide band gap semiconductor with a hardness comparable to diamond.Comment: 4 pages, 5 figure

Giant tuning of electronic and thermoelectric properties by epitaxial strain in p-type Sr-doped LaCrO3 transparent thin films

The impact of epitaxial strain on the structural, electronic, and thermoelectric properties of p-type transparent Sr-doped LaCrO3 thin films has been investigated. For this purpose, high-quality fully-strained La0.75Sr0.25CrO3 (LSCO) epitaxial thin films were grown by molecular beam epitaxy on three different (pseudo)cubic (001)-oriented perovskite-oxide substrates: LaAlO3, (LaAlO3)0.3(Sr2AlTaO6)0.7, and DyScO3. The lattice mismatch between the LSCO films and the substrates induces in-plane strain ranging from -2.06% (compressive) to +1.75% (tensile). The electric conductivity can be controlled over two orders of magnitude, σ ranging from ~0.5 S cm-1 (tensile strain) to 35 S cm-1 (compressive strain). Consistently, the Seebeck coefficient S can be finely tuned by a factor of almost two from ~127 μV K-1 (compressive strain) to 208 μV K-1 (tensile strain). Interestingly, we show that the thermoelectric power factor (PF = S2 σ) can consequently be tuned by almost two orders of magnitude. The compressive strain yields a remarkable enhancement by a factor of three for 2% compressive strain with respect to almost relaxed films. These results demonstrate that epitaxial strain is a powerful lever to control the electric properties of LSCO and enhance its thermoelectric properties, which is of high interest for various devices and key applications such as thermal energy harvesters, coolers, transparent conductors, photo-catalyzers and spintronic memories.Financial support from the European Commission through the project TIPS (H2020-ICT-02-2014-1-644453), the French national research agency (ANR) through the projects MITO (ANR-17-CE05-0018), LILIT (ANR-16-CE24-0022), DIAMWAFEL (ANR-15-CE08-0034-02), the CNRS through the MITI interdisciplinary programs (project NOTE), IDEX Lyon-St-Etienne through the project IPPON, the Spanish Ministerio de Ciencia e Innovación, through the “Severo Ochoa” Programme for Centres of Excellence in R&D (SEV2015-0496) and the MAT2017-85232-R (AEI/FEDER, EU), PID2019-107727RB-I00 (AEI/FEDER, EU), and from Generalitat de Catalunya (2017 SGR 1377) is acknowledged. The China Scholarship Council (CSC) is acknowledged for the grant of Dong Han. Ignasi Fina acknowledges Ramón y Cajal contract RYC-2017-22531. Seebeck measurements at ILM were made within the ILMTech transport platform. The authors are also grateful to Jean-Baptiste Goure, Philippe Regreny, Aziz Benamrouche, and Bernat Bozzo for their technical support and the reviewers for their valuable and constructive comments that have improved the quality of the manuscript.Peer reviewe

Isostructural phase transition by point defect reorganization in the binary type-I clathrate Ba7.5Si45

International audienceCompetition between microscopic point defect (vacancy and interstitial) configurations is inherent to crystalline phases of increased structural complexity. Phase transitions that preserve symmetry between them belong to a specific class of isostructural transitions. Type-I silicon clathrates are representatives of such structurally complex crystalline phases showing an intriguing structural transition at high pressure associated with an abrupt reduction of volume with no indication for any breakage of symmetry. Using isothermal high-pressure X-ray diffraction performed on a single crystal of the simplest representative type-I silicon clathrates, binary Ba 8 Si 46 , we confirm the isostructural character of the transition and identify the associated mechanism. A detailed analysis of the atomic structural parameters across the transition in combination with ab initio studies allow us to pinpoint a microscopic mechanism driven by a rearrangement of point defects initially present in the structure. An analysis based on the Landau theory gives a coherent description of the experimental observations. A discussion on the analogy between this transformation and liquid-liquid transitions is proposed

Development of High-Pressure Device, based on Paris-Edinburgh Press, Applied on SPS Process

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Localization of Propagative Phonons in a Perfectly Crystalline Solid

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