Rhombohedral to Cubic Conversion of GeTe via MnTe Alloying Leads to Ultralow Thermal Conductivity, Electronic Band Convergence, and High Thermoelectric Performance

Zheng, Zheng; Su, Xianli; Deng, Rigui; Stoumpos, Constantinos; Xie, Hongyao; Liu, Wei; Yan, Yonggao; Hao, Shiqiang; Uher, Ctirad; Wolverton, Chris; Kanatzidis, Mercouri G.; Tang, Xinfeng

doi:10.1021/jacs.7b13611

Rhombohedral to Cubic Conversion of GeTe via MnTe Alloying Leads to Ultralow Thermal Conductivity, Electronic Band Convergence, and High Thermoelectric Performance

Journal Article · Thu Jan 18 23:00:00 EST 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b13611· OSTI ID:1775445

Zheng, Zheng ^[1]; ^[2]; Deng, Rigui ^[3]; ^[4]; Xie, Hongyao ^[3]; Liu, Wei ^[3]; Yan, Yonggao ^[3]; Hao, Shiqiang ^[4]; Uher, Ctirad ^[5]; ^[4]; ^[4]; ^[3]

Wuhan Univ. of Technology (China); Northwestern University
Wuhan Univ. of Technology (China); Northwestern Univ., Evanston, IL (United States)
Wuhan Univ. of Technology (China)
Northwestern Univ., Evanston, IL (United States)
Univ. of Michigan, Ann Arbor, MI (United States)

In this study, a series of Ge_1–xMn_xTe (x = 0–0.21) compounds were prepared by a melting–quenching–annealing process combined with spark plasma sintering (SPS). The effect of alloying MnTe into GeTe on the structure and thermoelectric properties of Ge_1–xMn_xTe is profound. With increasing content of MnTe, the structure of the Ge_1–xMn_xTe compounds gradually changes from rhombohedral to cubic, and the known R3m to Fm-3m phase transition temperature of GeTe moves from 700 K closer to room temperature. First-principles density functional theory calculations show that alloying MnTe into GeTe decreases the energy difference between the light and heavy valence bands in both the R3m and Fm-3m structures, enhancing a multiband character of the valence band edge that increases the hole carrier effective mass. The effect of this band convergence is a significant enhancement in the carrier effective mass from 1.44 m₀ (GeTe) to 6.15 m₀ (Ge_0.85Mn_0.15Te). In addition, alloying with MnTe decreases the phonon relaxation time by enhancing alloy scattering, reduces the phonon velocity, and increases Ge vacancies all of which result in an ultralow lattice thermal conductivity of 0.13 W m^–1 K^–1 at 823 K. Subsequent doping of the Ge_0.9Mn_0.1Te compositions with Sb lowers the typical very high hole carrier concentration and brings it closer to its optimal value enhancing the power factor, which combined with the ultralow thermal conductivity yields a maximum ZT value of 1.61 at 823 K (for Ge_0.86Mn_0.10Sb_0.04Te). In conclusion, the average ZT value of the compound over the temperature range 400–800 K is 1.09, making it the best GeTe-based thermoelectric material.

View Accepted Manuscript (DOE)

Research Organization:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Natural Science Foundation of China

Grant/Contract Number:: SC0014520

OSTI ID:: 1775445

Alternate ID(s):: OSTI ID: 1539680

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 7 Vol. 140; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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