Two-Dimensional CsAg5Te3–xSx Semiconductors: Multi-anion Chalcogenides with Dynamic Disorder and Ultralow Thermal Conductivity

Hodges, James M.; Xia, Yi; Malliakas, Christos D.; Alexander, Grant C. B.; Chan, Maria K. Y.; Kanatzidis, Mercouri G.

doi:10.1021/acs.chemmater.8b03306

Title: Two-Dimensional CsAg₅Te_3–xS_x Semiconductors: Multi-anion Chalcogenides with Dynamic Disorder and Ultralow Thermal Conductivity

Journal Article · Wed Sep 12 00:00:00 EDT 2018 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.8b03306· OSTI ID:1487454

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Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Metal chalcogenides underpin a wide variety of energyrelated applications and are ideal systems for probing lattice dynamics and fundamental transport phenomena. Here we describe the synthesis and transport properties of CsAg₅TeS₂ and its solid solution CsAg₅Te_3-xS_x (x = 1-2), new semiconductors with tunable band gaps ranging from 0.17 to 0.30 eV. CsAg₅TeS₂ has a fully ordered two-dimensional structure that includes a group of Ag atoms in a heteroleptic tetrahedral coordination geometry (AgTe₂S₂). Single-crystal X-ray diffraction indicates that the compounds crystallize in the tetragonal space group P4/mmm, while pair distribution function (PDF) analysis reveals off-centering at the heteroleptic Ag sites, signifying the lower-symmetry I4/mcm space group. The underlying disorder as a phonon-blocking mechanism that helps facilitate an ultralow lattice thermal conductivity below 0.40 Wm^-1 • K^-1 at , ~ 300 K , highlighting the importance of local disorder in thermal transport. In conclusion, density functional theory provides additional insight into the electronic and thermal properties of the materials, which are good candidates for p-type thermoelectrics.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1487454

Journal Information:: Chemistry of Materials, Vol. 30, Issue 20; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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Title: Two-Dimensional CsAg5Te3–xSx Semiconductors: Multi-anion Chalcogenides with Dynamic Disorder and Ultralow Thermal Conductivity

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