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Discordant Distortion in Cubic GeMnTe<sub>2</sub> and High Thermoelectric Properties of GeMnTe<sub>2</sub>-<i>x</i>%SbTe

Jinfeng Dong, Yilin Jiang, Yandong Sun, Jue Liu, Jun Pei, Wei Li, Xian Yi Tan, Lei Hu, Ning Jia, Ben Xu, Qian Li, Jing‐Feng Li, Qingyu Yan, Mercouri G. Kanatzidis

2023Journal of the American Chemical Society53 citationsDOIOpen Access PDF

Abstract

GeMnTe 2 adopts a cubic rock salt structure and is a promising mid-temperature thermoelectric material. The pair distribution function analysis of neutron total scattering data, however, indicates that GeMnTe 2 is locally distorted from the ideal rock salt structure with Ge 2+ cations being discordant and displaced ∼0.3 Å off the octahedron center. By alloying GeMnTe 2 with SbTe, the carrier concentration can be tuned in GeMnTe 2 - x %SbTe ( x = 15.1), leading to converged multiple broad valence bands and a high Seebeck coefficient of >200 μV K –1 from 300 to 823 K. The system exhibits a large density-of-state effective mass of >10 m e and a high weighted mobility of 80 cm 2 V –1 s –1, leading to a power factor of 15 μWcm –1 K –2 at 823 K. The composition GeMnTe 2 -15.1%SbTe exhibits very low lattice thermal conductivity of ∼0.5 Wm –1 K –1 at 823 K, attributed to the combination of off-centering cations in the rock salt structure, Ge/Mn positional disorder, dislocations, and abundant Ge-rich and Mn-rich nanoparticles. A ZT value of ∼1.5 can be achieved for GeMnTe 2 -15.1%SbTe with a ZT ave of 0.96 in the temperature range of 400–823 K.

Topics & Concepts

Seebeck coefficientValence (chemistry)ChemistryOctahedronElectrical resistivity and conductivityThermoelectric effectAnalytical Chemistry (journal)Thermoelectric materialsPair distribution functionScatteringCrystallographyCondensed matter physicsCrystal structureThermodynamicsOpticsPhysicsChromatographyOrganic chemistryQuantum mechanicsAdvanced Thermoelectric Materials and DevicesChalcogenide Semiconductor Thin FilmsPhase-change materials and chalcogenides
Discordant Distortion in Cubic GeMnTe<sub>2</sub> and High Thermoelectric Properties of GeMnTe<sub>2</sub>-<i>x</i>%SbTe | Litcius