Violation of the T-1 Relationship in the Lattice Thermal Conductivity of Mg3Sb2 with Locally Asymmetric Vibrations

Zhu, Yifan1,2,3; Xia, Yi4; Wang, Yancheng1,2; Sheng, Ye3; Yang, Jiong1,3; Fu, Chenguang5; Li, Airan6; Zhu, Tiejun6; Luo, Jun3,7; Wolverton, Christopher4; Snyder, G. Jeffrey4; Liu, Jianjun1,2; Zhang, Wenqing1,8,9,10,11

2020-11-30

10.34133/2020/4589786

Research   影响因子和分区

2639-5274

Most crystalline materials follow the guidelines of T-1 temperature-dependent lattice thermal conductivity (kappa(L)) at elevated temperatures. Here, we observe a weak temperature dependence of kappa(L) in Mg3Sb2, T-0.48 from theory and T-0.57 from measurements, based on a comprehensive study combining ab initio molecular dynamics calculations and experimental measurements on single crystal Mg3Sb2. These results can be understood in terms of the so-called "phonon renormalization" effects due to the strong temperature dependence of the interatomic force constants (IFCs). The increasing temperature leads to the frequency upshifting for those low-frequency phonons dominating heat transport, and more importantly, the phonon-phonon interactions are weakened. In-depth analysis reveals that the phenomenon is closely related to the temperature-induced asymmetric movements of Mg atoms within MgSb4 tetrahedron. With increasing temperature, these Mg atoms tend to locate at the areas with relatively low force in the force profile, leading to reduced effective 3rd -order IFCs. The locally asymmetrical atomic movements at elevated temperatures can be further treated as an indicator of temperature-induced variations of IFCs and thus relatively strong phonon renormalization. The present work sheds light on the fundamental origins of anomalous temperature dependence of kappa(L), in thermoelectrics.

ESCI ; EI

英语

通讯

National Key Research and Development Program of China[2018YFB0703600][2017YFB0701600][2019YFA0704901] ; Natural Science Foundation of China[11674211][51632005][51761135127] ; 111 Project[D16002] ; Guangdong Innovation Research Team Project[2017ZT07C062] ; Guangdong Provincial Key Lab program[2019B030301001] ; Shenzhen Municipal Key Lab program[ZDSYS20190902092905285] ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)[392228380] ; National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD)[70NANB14H012] ; Office of Science of the U.S. Department of Energy (U.S. Department of Energy)[DEAC02-05CH11231]

Science & Technology - Other Topics

Multidisciplinary Sciences

WOS:000594154000001

AMER ASSOC ADVANCEMENT SCIENCE

20205209694868

Phonons ; Calculations ; Lattice vibrations ; Molecular dynamics ; Single crystals ; Temperature distribution ; Thermoelectricity ; Crystalline materials ; Thermal conductivity ; Magnesium ; Magnesium compounds

Magnesium and Alloys:542.2 ; Alkaline Earth Metals:549.2 ; Thermodynamics:641.1 ; Electricity: Basic Concepts and Phenomena:701.1 ; Physical Chemistry:801.4 ; Mathematics:921 ; Atomic and Molecular Physics:931.3 ; Crystalline Solids:933.1 ; Crystal Lattice:933.1.1

Web of Science

1.Chinese Acad Sci, Shanghai Inst Ceram, State Key Lab High Performance Ceram & Superfine, Shanghai 200050, Peoples R China
2.Univ Chinese Acad Sci, Ctr Mat Sci & Optoelect Engn, Beijing 100049, Peoples R China
3.Shanghai Univ, Mat Genome Inst, Shanghai 200444, Peoples R China
4.Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA
5.Max Planck Inst Chem Phys Solids, D-01187 Dresden, Germany
6.Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R China
7.Shanghai Univ, Sch Mat Sci & Engn, Shanghai 200444, Peoples R China
8.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
9.Southern Univ Sci & Technol, Shenzhen Inst Quantum Sci & Engn, Shenzhen 518055, Peoples R China
10.Southern Univ Sci & Technol, Guangdong Prov Key Lab Computat Sci & Mat Design, Shenzhen 518055, Peoples R China
11.Southern Univ Sci & Technol, Shenzhen Municipal Key Lab Adv Quantum Mat & Devi, Shenzhen 518055, Peoples R China

Zhu, Yifan,Xia, Yi,Wang, Yancheng,et al. Violation of the T-1 Relationship in the Lattice Thermal Conductivity of Mg3Sb2 with Locally Asymmetric Vibrations[J]. Research,2020,2020.

Zhu, Yifan.,Xia, Yi.,Wang, Yancheng.,Sheng, Ye.,Yang, Jiong.,...&Zhang, Wenqing.(2020).Violation of the T-1 Relationship in the Lattice Thermal Conductivity of Mg3Sb2 with Locally Asymmetric Vibrations.Research,2020.

Zhu, Yifan,et al."Violation of the T-1 Relationship in the Lattice Thermal Conductivity of Mg3Sb2 with Locally Asymmetric Vibrations".Research 2020(2020).