2015/02/20 by Andreas Fischer, Ernst‐Wilhelm Scheidt, Fischer, Andreas +13
Engineering · Materials Science · Physics and Astronomy · #Advanced Semiconductor Detectors and Materials #Advanced Thermoelectric Materials and Devices #FOS: Physical sciences #Machine Learning in Materials Science #Materials Science (cond-mat.mtrl-sci) #cond-mat.mtrl-sci
paper · pdf · doi:10.48550/arxiv.1502.05901
25 pages, 10 figures, supporting information attached
arxiv created 2015/02/20 · openalex publication_date 2015/02/20 · arxiv updated 2015/02/23 · openalex created_date 2022/10/02 · openalex updated_date 2026/07/28
The intermetallic compound ZnSb is an interesting thermoelectric material, largely due to its low lattice thermal conductivity. The origin of the low thermal conductivity has so far been speculative. Using multi-temperature single crystal X-ray diffraction (9 - 400 K) and powder X-ray diffraction (300 - 725 K) measurements we characterized the volume expansion and the evolution of structural properties with temperature and identify an increasingly anharmonic behavior of the Zn atoms. From a combination of Raman spectroscopy and first principles calculations of phonons we consolidate the presence of low-energy optic modes with wavenumbers below 60 cm-1. Heat capacity measurements between 2 and 400 K can be well described by a Debye-Einstein model containing one Debye and two Einstein contributions with temperatures ΘD = 195K, ΘE1 = 78 K and ΘE2 = 277 K as well as a significant contribution due to anharmonicity above 150 K. The presence of a multitude of weakly dispersed low-energy optical modes (which couple with the acoustic, heat carrying phonons) combined with anharmonic thermal behavior provides an effective mechanism for low lattice thermal conductivity. The peculiar vibrational properties of ZnSb are attributed to its chemical bonding properties which are characterized by multicenter bonded structural entities. We argue that the proposed mechanism to explain the low lattice thermal conductivity of ZnSb might also control the thermoelectric properties of electron poor semiconductors, such as Zn4Sb3, CdSb, Cd4Sb3, Cd13-xInyZn10, and Zn5Sb4In2-x.