1. Anharmonicity and Effect of the Nanostructuring on the Lattice Dynamics of CrSi 2
- Author
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Mickael Beaudhuin, Jérôme Rouquette, Jérôme Debray, S Laborde, Adrien Moll, Romain Viennois, Y Sidis, Michael Marek Koza, Bertrand Lenoir, J.-P Castellan, Christophe Candolfi, Bertrand Ménaert, Patrick Hermet, Martin Boehm, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Institut Laue-Langevin (ILL), ILL, Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, Cristaux Massifs (CrisMass), Institut Néel (NEEL), Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Institut Jean Lamour (IJL), Université de Lorraine (UL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2), LLB - Nouvelles frontières dans les matériaux quantiques (NFMQ), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Cristaux massifs (NEEL - CrisMass), and Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS)
- Subjects
Materials science ,Phonon ,02 engineering and technology ,01 natural sciences ,Inelastic neutron scattering ,symbols.namesake ,0103 physical sciences ,Thermoelectric effect ,[CHIM]Chemical Sciences ,Physical and Theoretical Chemistry ,[PHYS.COND]Physics [physics]/Condensed Matter [cond-mat] ,010306 general physics ,Debye model ,Strengthening mechanisms of materials ,ComputingMilieux_MISCELLANEOUS ,[PHYS]Physics [physics] ,Condensed matter physics ,Anharmonicity ,[CHIM.MATE]Chemical Sciences/Material chemistry ,021001 nanoscience & nanotechnology ,Nanocrystalline material ,Surfaces, Coatings and Films ,Electronic, Optical and Magnetic Materials ,General Energy ,symbols ,Density functional theory ,0210 nano-technology - Abstract
International audience; Chromium disilicide CrSi2 is an interesting compound for thermoelectric applications. In order to decrease its lattice thermal conductivity that mainly limits its performance, two main routes have been investigated thus far, either increasing the unit cell disorder or creating multiple interfaces through nanostructuring. Here, we explore the effect of the latter route by investigating in detail the effect of the grain size reduction and residual microstrains on the lattice dynamics and lattice thermal conductivity. The phonon dispersion curves were measured on single-crystalline CrSi2 using inelastic neutron scattering, while the generalized vibrational density of states (GVDOS) was determined on bulk and nanostructured CrSi2. All experimental results are consistent with our density functional theory calculations. The results show that the optical phonons contribute from 50 to 70% of the lattice thermal conductivity. The temperature variations in the GVDOS of CrSi2 follow a quasi-harmonic behavior, which explains its rather large lattice thermal conductivity measured on the single-crystalline specimen. In addition, the GVDOS of nanocrystalline CrSi2 evidences a spectral weight transfer at low energy, which is related to a decrease in both the Debye temperature and the sound velocities that may be ascribed to an increase in both the interface density and internal strain. These observations explain the strong decrease in the lattice thermal conductivity observed in our prior study on densified nanostructured CrSi2 pellets.
- Published
- 2021