TY - JOUR
T1 - Particlelike Phonon Propagation Dominates Ultralow Lattice Thermal Conductivity in Crystalline Tl3VSe4
AU - Xia, Yi
AU - Pal, Koushik
AU - He, Jiangang
AU - Ozoliņš, Vidvuds
AU - Wolverton, Chris
N1 - Funding Information:
The authors from Northwestern University acknowledge financial support received from (i) Toyota Research Institute (TRI) through the Accelerated Materials Design and Discovery program (thermal conductivity calculations), (ii) the Department of Energy, Office of Science, Basic Energy Sciences under Grant No.DE-SC0014520 (theory of anharmonic phonons), and (iii) the U.S. Department of Commerce and National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) under Grant No.70NANB14H012 (DFT calculations). V.O. (overall project guidance) acknowledges financial support from the National Science Foundation Grant No.DMR-1611507. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No.DE-AC02-05CH11231. Y.X. gratefully acknowledges discussions with Michele Simoncelli.
Publisher Copyright:
© 2020 American Physical Society.
PY - 2020/2/14
Y1 - 2020/2/14
N2 - We investigate the microscopic mechanisms of ultralow lattice thermal conductivity (κl) in Tl3VSe4 by combining a first principles density functional theory based framework of anharmonic lattice dynamics with the Peierls-Boltzmann transport equation for phonons. We include contributions of the three-and four-phonon scattering processes to the phonon lifetimes as well as the temperature dependent anharmonic renormalization of phonon energies arising from an unusually strong quartic anharmonicity in Tl3VSe4. In contrast to a recent report by Mukhopadhyay et al. [Science 360, 1455 (2018)SCIEAS0036-807510.1126/science.aar8072] which suggested that a significant contribution to κl arises from random walks among uncorrelated oscillators, we show that particlelike propagation of phonon excitations can successfully explain the experimentally observed ultralow κl. Our findings are further supported by explicit calculations of the off-diagonal terms of the heat current operator, which are found to be small and indicate that wavelike tunneling of heat carrying vibrations is of minor importance. Our results (i) resolve the discrepancy between the theoretical and experimental κl, (ii) offer new insights into the minimum κl achievable in Tl3VSe4, and (iii) highlight the importance of high order anharmonicity in low-κl systems. The methodology demonstrated here may be used to resolve the discrepancies between the experimentally measured and the theoretically calculated κl in skutterides and perovskites, as well as to understand the glasslike κl in complex crystals with strong anharmonicity, leading towards the goal of rational design of new materials.
AB - We investigate the microscopic mechanisms of ultralow lattice thermal conductivity (κl) in Tl3VSe4 by combining a first principles density functional theory based framework of anharmonic lattice dynamics with the Peierls-Boltzmann transport equation for phonons. We include contributions of the three-and four-phonon scattering processes to the phonon lifetimes as well as the temperature dependent anharmonic renormalization of phonon energies arising from an unusually strong quartic anharmonicity in Tl3VSe4. In contrast to a recent report by Mukhopadhyay et al. [Science 360, 1455 (2018)SCIEAS0036-807510.1126/science.aar8072] which suggested that a significant contribution to κl arises from random walks among uncorrelated oscillators, we show that particlelike propagation of phonon excitations can successfully explain the experimentally observed ultralow κl. Our findings are further supported by explicit calculations of the off-diagonal terms of the heat current operator, which are found to be small and indicate that wavelike tunneling of heat carrying vibrations is of minor importance. Our results (i) resolve the discrepancy between the theoretical and experimental κl, (ii) offer new insights into the minimum κl achievable in Tl3VSe4, and (iii) highlight the importance of high order anharmonicity in low-κl systems. The methodology demonstrated here may be used to resolve the discrepancies between the experimentally measured and the theoretically calculated κl in skutterides and perovskites, as well as to understand the glasslike κl in complex crystals with strong anharmonicity, leading towards the goal of rational design of new materials.
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U2 - 10.1103/PhysRevLett.124.065901
DO - 10.1103/PhysRevLett.124.065901
M3 - Article
C2 - 32109101
AN - SCOPUS:85080961029
VL - 124
JO - Physical Review Letters
JF - Physical Review Letters
SN - 0031-9007
IS - 6
M1 - 065901
ER -