The Mg 3 Sb 2− x Bi x family has emerged as the potential candidates for thermoelectric applications due to their ultra-low lattice thermal conductivity ( κ L ) at room temperature (RT) and structural complexity. Here, using ab initio calculations of the electron-phonon averaged (EPA) approximation coupled with Boltzmann transport equation (BTE), we have studied electronic, phonon and thermoelectric properties of Mg 3 Sb 2− x Bi x (x = 0, 1, and 2) monolayers. In violation of common mass-trend expectations, increasing Bi element content with heavier Zintl phase compounds yields an abnormal change in κ L in two-dimensional Mg 3 Sb 2− x Bi x crystals at RT (∼0.51, 1.86, and 0.25 W/mK for Mg 3 Sb 2 , Mg 3 SbBi, and Mg 3 Bi 2 ). The κ L trend was detailedly analyzed via the phonon heat capacity, group velocity and lifetime parameters. Based on quantitative electronic band structures, the electronic bonding through the crystal orbital Hamilton population (COHP) and electron local function analysis we reveal the underlying mechanism for the semiconductor-semimetallic transition of Mg 3 Sb 2-− x Bi x compounds, and these electronic transport properties (Seebeck coefficient, electrical conductivity, and electronic thermal conductivity) were calculated. We demonstrate that the highest dimensionless figure of merit ZT of Mg 3 Sb 2− x Bi x compounds with increasing Bi content can reach ∼1.6, 0.2, and 0.6 at 700 K, respectively. Our results can indicate that replacing heavier anion element in Zintl phase Mg 3 Sb 2− x Bi x materials go beyond common expectations (a heavier atom always lead to a lower κ L from Slack’s theory), which provide a novel insight for regulating thermoelectric performance without restricting conventional heavy atomic mass approach.
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Topological phase and thermoelectric properties of bialkali bismuthide compounds (Na, K) 2 RbBi from first-principles
Abstract We report the topological phase and thermoelectric properties of bialkali bismuthide compounds (Na, K) 2 RbBi, as yet hypothetical. The topological phase transitions of these compounds under hydrostatic pressure are investigated. The calculated topological surface states and Z 2 topological index confirm the nontrivial topological phase. The electronic properties and transport coefficients are obtained using the density functional theory combined with the Boltzmann transport equation. The relaxation times are determined using the deformation potential theory to calculate the electronic thermal and electrical conductivity. The calculated mode Grüneisen parameters are substantial, indicating strong anharmonic acoustic phonons scattering, which results in an exceptionally low lattice thermal conductivity. These compounds also have a favorable power factor leading to a relatively flat p-type figure-of-merit over a broad temperature range. Furthermore, the mechanical properties and phonon band dispersions show that these structures are mechanically and dynamically stable. Therefore, they offer excellent candidates for practical applications over a wide range of temperatures.
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- Award ID(s):
- 2110603
- NSF-PAR ID:
- 10374293
- Date Published:
- Journal Name:
- Journal of Physics: Condensed Matter
- Volume:
- 34
- Issue:
- 10
- ISSN:
- 0953-8984
- Page Range / eLocation ID:
- 105702
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1088/1361-648X/ac431d
