Two-Dimensional CsAg5Te3–xSx Semiconductors: Multi-anion Chalcogenides with Dynamic Disorder and Ultralow Thermal Conductivity
Abstract
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 CsAg5Te3-xSx (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.
- Authors:
-
[1];
[2];
[1];
[1];
[2];
[3]
- 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)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1487454
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 30; Journal Issue: 20; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Hodges, James M., Xia, Yi, Malliakas, Christos D., Alexander, Grant C. B., Chan, Maria K. Y., and Kanatzidis, Mercouri G. Two-Dimensional CsAg5Te3–xSx Semiconductors: Multi-anion Chalcogenides with Dynamic Disorder and Ultralow Thermal Conductivity. United States: N. p., 2018.
Web. doi:10.1021/acs.chemmater.8b03306.
Hodges, James M., Xia, Yi, Malliakas, Christos D., Alexander, Grant C. B., Chan, Maria K. Y., & Kanatzidis, Mercouri G. Two-Dimensional CsAg5Te3–xSx Semiconductors: Multi-anion Chalcogenides with Dynamic Disorder and Ultralow Thermal Conductivity. United States. doi:10.1021/acs.chemmater.8b03306.
Hodges, James M., Xia, Yi, Malliakas, Christos D., Alexander, Grant C. B., Chan, Maria K. Y., and Kanatzidis, Mercouri G. Wed .
"Two-Dimensional CsAg5Te3–xSx Semiconductors: Multi-anion Chalcogenides with Dynamic Disorder and Ultralow Thermal Conductivity". United States. doi:10.1021/acs.chemmater.8b03306. https://www.osti.gov/servlets/purl/1487454.
@article{osti_1487454,
title = {Two-Dimensional CsAg5Te3–xSx Semiconductors: Multi-anion Chalcogenides with Dynamic Disorder and Ultralow Thermal Conductivity},
author = {Hodges, James M. and Xia, Yi and Malliakas, Christos D. and Alexander, Grant C. B. and Chan, Maria K. Y. and Kanatzidis, Mercouri G.},
abstractNote = {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 CsAg5Te3-xSx (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.},
doi = {10.1021/acs.chemmater.8b03306},
journal = {Chemistry of Materials},
number = 20,
volume = 30,
place = {United States},
year = {2018},
month = {9}
}
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Works referencing / citing this record:
CSD 1876895: Experimental Crystal Structure Determination: Non-CSD Structure
dataset, November 2018
- Hodges, James M.; Xia, Yi; Malliakas, Christos D.
- Cambridge Structural Database (CSD)
CSD 1876896: Experimental Crystal Structure Determination: Non-CSD Structure
dataset, November 2018
- Hodges, James M.; Xia, Yi; Malliakas, Christos D.
- Cambridge Structural Database (CSD)
CSD 1876897: Experimental Crystal Structure Determination: Non-CSD Structure
dataset, November 2018
- Hodges, James M.; Xia, Yi; Malliakas, Christos D.
- Cambridge Structural Database (CSD)
Compressive sensing lattice dynamics. I. General formalism
journal, November 2019
- Zhou, Fei; Nielson, Weston; Xia, Yi
- Physical Review B, Vol. 100, Issue 18