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DOE OSTI · 3364168

Stabilization of high-performance rock-salt LiMnSbTe3 thermoelectrics with embedded van der Waals-like gaps

Dong, Jinfeng [Nanyang Technological Univ. (Singapore)] (ORCID:0000000230268054)·Liu, Yukun [Northwestern Univ., Evanston, IL (United States)]·Sun, Yandong [China Academy of Engineering Physics, Beijing (China)] (ORCID:000000034491208X)·Yu, Yuan [RWTH Aachen Univ. (Germany)] (ORCID:0000000231486600)·Jiang, Yilin [Tsinghua Univ., Beijing (China)]·Zhang, Chenguang [Nanyang Technological Univ. (Singapore)] (ORCID:0000000346585633)·None, Sumayya [RWTH Aachen Univ. (Germany)]·Chen, Chen [Tsinghua Univ., Beijing (China)]·Tan, Xian Yi [Agency for Science, Technology and Research (A*STAR) (Singapore)]·Tan, Li Ping [Nanyang Technological Univ. (Singapore)] (ORCID:0000000252393745)·Acharyya, Paribesh [Northwestern Univ., Evanston, IL (United States)]·Repaka, D. V. Maheswar [Agency for Science, Technology and Research (A*STAR) (Singapore)] (ORCID:0000000339170229)·Yang, Dongwang [Nanyang Technological Univ. (Singapore)] (ORCID:0000000260964261)·Xu, Ben [China Academy of Engineering Physics, Beijing (China)] (ORCID:0000000215570052)·Hippalgaonkar, Kedar [Nanyang Technological Univ. (Singapore); Agency for Science, Technology and Research (A*STAR) (Singapore)] (ORCID:0000000212709047)·Ramanujan, R. V. [Nanyang Technological Univ. (Singapore)]·Li, Jing-Feng [Tsinghua Univ., Beijing (China)] (ORCID:0000000201850512)·Dravid, Vinayak P. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000260073063)·Yan, Qingyu [Nanyang Technological Univ. (Singapore); Agency for Science, Technology and Research (A*STAR) (Singapore)] (ORCID:0000000303173225)·Kanatzidis, Mercouri G. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000320374168)

Abstract

Rock-salt-structured compounds like lead chalcogenides are promising thermoelectrics, as their high symmetry, strong anharmonicity, and favorable phase behavior collectively lead to high performance by enabling large power factors and ultralow thermal conductivity. Here, we report LiMnSbTe 3 , a new rock-salt semiconductor stabilized through targeted chemical design by combining hexagonal MnTe with cubic LiSbTe 2 . Embedded in the highsymmetry matrix, van der Waals-like gaps form due to Sb 2 Te 3 nanoscale segregation, which acts as effective phonon-scattering centers, leading to a low lattice thermal conductivity of 0.37Wm- 1 K -1 at 873 K with alloy scattering from disordered cations. The ordered local structure of Sb2Te 3 -type vdW-like gaps and the cross-gap interaction facilitate the carrier transport. Aided by energyconverged valence bands and a paramagnon drag effect, high Seebeck coefficients and enhanced power factor can be achieved, leading to a high ZT of 1.2 at 873 K. Furthermore, introducing Mn deficiency increases ZT to 1.5, highlighting the potential for higher performance through optimized doping or alloying. A segmented single-leg thermoelectric module achieves an output power density of 0.52 Wcm -2 and an efficiency of 8.7% under ΔT of 478 K, further demonstrating its promising thermoelectric applications.

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Dong, Jinfeng [Nanyang Technological Univ. (Singapore)] (ORCID:0000000230268054), Liu, Yukun [Northwestern Univ., Evanston, IL (United States)], Sun, Yandong [China Academy of Engineering Physics, Beijing (China)] (ORCID:000000034491208X), Yu, Yuan [RWTH Aachen Univ. (Germany)] (ORCID:0000000231486600), Jiang, Yilin [Tsinghua Univ., Beijing (China)], Zhang, Chenguang [Nanyang Technological Univ. (Singapore)] (ORCID:0000000346585633), None, Sumayya [RWTH Aachen Univ. (Germany)], Chen, Chen [Tsinghua Univ., Beijing (China)], Tan, Xian Yi [Agency for Science, Technology and Research (A*STAR) (Singapore)], Tan, Li Ping [Nanyang Technological Univ. (Singapore)] (ORCID:0000000252393745), Acharyya, Paribesh [Northwestern Univ., Evanston, IL (United States)], Repaka, D. V. Maheswar [Agency for Science, Technology and Research (A*STAR) (Singapore)] (ORCID:0000000339170229), Yang, Dongwang [Nanyang Technological Univ. (Singapore)] (ORCID:0000000260964261), Xu, Ben [China Academy of Engineering Physics, Beijing (China)] (ORCID:0000000215570052), Hippalgaonkar, Kedar [Nanyang Technological Univ. (Singapore); Agency for Science, Technology and Research (A*STAR) (Singapore)] (ORCID:0000000212709047), Ramanujan, R. V. [Nanyang Technological Univ. (Singapore)], Li, Jing-Feng [Tsinghua Univ., Beijing (China)] (ORCID:0000000201850512), Dravid, Vinayak P. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000260073063), Yan, Qingyu [Nanyang Technological Univ. (Singapore); Agency for Science, Technology and Research (A*STAR) (Singapore)] (ORCID:0000000303173225), Kanatzidis, Mercouri G. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000320374168). 2025-11-20. Stabilization of high-performance rock-salt LiMnSbTe3 thermoelectrics with embedded van der Waals-like gaps. https://doi.org/10.1038/s41467-025-66518-w

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