TY - JOUR
T1 - Optical phonon dominated heat transport
T2 - A first-principles thermal conductivity study of BaSnS2
AU - Li, Zhi
AU - Xie, Hongyao
AU - Hao, Shiqiang
AU - Xia, Yi
AU - Su, Xianli
AU - Kanatzidis, Mercouri G.
AU - Wolverton, Christopher
AU - Tang, Xinfeng
N1 - Funding Information:
This work at Northwestern University was supported by a grant from the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences under Award No. DE-SC0014520. The Northwestern Quest computational resources are acknowledged. X.T. wishes to acknowledge support from the National Key Research and Development Program of China (Grant No. 2019YFA0704902), Natural Science Foundation of China (Grants No. 51972256, No. 51872219, No. 51632006, and No. 51521001), and 111 Project of China (Grant No. B07040). Z.L. was supported by the China Scholarship Council (Grant No. 201906950054) for a two-year study at Northwestern University.
Publisher Copyright:
©2021 American Physical Society
PY - 2021/12/15
Y1 - 2021/12/15
N2 - Acoustic phonons with long mean free paths have long been believed to control the lattice thermal conductivity κL in solids dominantly. In this study, however, we demonstrate an optical phonon dominated κL in BaSnS2. By solving the Peierls-Boltzmann transport equation, we predict a low diagonal lattice thermal conductivity κL(D) of 0.34Wm−1K−1 at 850 K, which is less than half the κL(D) of SnS at the same temperature. Further calculations following the Allen-Feldman model suggest the additional off-diagonal lattice thermal conductivity κL(OD) contributed by wavelike tunneling phonons. The κL(OD) becomes pronounced at the high temperature (0.17Wm−1K−1 at 850 K) and leads to a deviation of the temperature dependence of κL from T–1 to T–0.76, suggesting the potential lattice anharmonicity in BaSnS2. Further analyses indicate BaSnS2 has over 68% of κL contributed by optical phonons. We show this uncommon optical phonon dominated κL is due to the relatively high group velocities of optical phonons in BaSnS2. The phonon mode visualization suggests these relatively high-velocity optical phonons correspond to the antiphase vibrations in BaSnS2 monolayers, which is originated from the unique permutation of SnS3 tetrahedra. Finally, by investigating the mode-resolved group velocity, relaxation time, and Grüneisen parameter, we attribute the intrinsic low κL of BaSnS2 to the soft lattice and the relatively high lattice anharmonicity induced by the Ba-S weak bonding and Sn(II) lone-pair electrons. Our study explicitly analyzes the microscopic mechanism of optical phonon dominated heat transport in BaSnS2 and suggests it worthy of further experimental studies as an intrinsic low-κL material.
AB - Acoustic phonons with long mean free paths have long been believed to control the lattice thermal conductivity κL in solids dominantly. In this study, however, we demonstrate an optical phonon dominated κL in BaSnS2. By solving the Peierls-Boltzmann transport equation, we predict a low diagonal lattice thermal conductivity κL(D) of 0.34Wm−1K−1 at 850 K, which is less than half the κL(D) of SnS at the same temperature. Further calculations following the Allen-Feldman model suggest the additional off-diagonal lattice thermal conductivity κL(OD) contributed by wavelike tunneling phonons. The κL(OD) becomes pronounced at the high temperature (0.17Wm−1K−1 at 850 K) and leads to a deviation of the temperature dependence of κL from T–1 to T–0.76, suggesting the potential lattice anharmonicity in BaSnS2. Further analyses indicate BaSnS2 has over 68% of κL contributed by optical phonons. We show this uncommon optical phonon dominated κL is due to the relatively high group velocities of optical phonons in BaSnS2. The phonon mode visualization suggests these relatively high-velocity optical phonons correspond to the antiphase vibrations in BaSnS2 monolayers, which is originated from the unique permutation of SnS3 tetrahedra. Finally, by investigating the mode-resolved group velocity, relaxation time, and Grüneisen parameter, we attribute the intrinsic low κL of BaSnS2 to the soft lattice and the relatively high lattice anharmonicity induced by the Ba-S weak bonding and Sn(II) lone-pair electrons. Our study explicitly analyzes the microscopic mechanism of optical phonon dominated heat transport in BaSnS2 and suggests it worthy of further experimental studies as an intrinsic low-κL material.
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U2 - 10.1103/PhysRevB.104.245209
DO - 10.1103/PhysRevB.104.245209
M3 - Article
AN - SCOPUS:85122039303
SN - 0163-1829
VL - 104
JO - Physical Review B-Condensed Matter
JF - Physical Review B-Condensed Matter
IS - 24
M1 - 245209
ER -