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Disordered zinc in Zn_4Sb_3 with phonon-glass and electron-crystal thermoelectric properties

Snyder, G. Jeffrey and Christensen, Mogens and Nishibori, Eiji and Caillat, Thierry and Iversen, Bo Brummerstedt (2004) Disordered zinc in Zn_4Sb_3 with phonon-glass and electron-crystal thermoelectric properties. Nature Materials, 3 (7). pp. 458-463. ISSN 1476-1122. doi:10.1038/nmat1154. https://resolver.caltech.edu/CaltechAUTHORS:20150512-144224016

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Abstract

By converting waste heat into electricity, thermoelectric generators could be an important part of the solution to today's energy challenges. The compound Zn_4Sb_3 is one of the most efficient thermoelectric materials known. Its high efficiency results from an extraordinarily low thermal conductivity in conjunction with the electronic structure of a heavily doped semiconductor. Previous structural studies have been unable to explain this unusual combination of properties. Here, we show through a comprehensive structural analysis using single-crystal X-ray and powder-synchrotron-radiation diffraction methods, that both the electronic and thermal properties of Zn_4Sb_3 can be understood in terms of unique structural features that have been previously overlooked. The identification of Sb^(3-) ions and Sb_2^(4-) dimers reveals that Zn_4Sb_3 is a valence semiconductor with the ideal stoichiometry Zn_(13)Sb_(10). In addition, the structure contains significant disorder, with zinc atoms distributed over multiple positions. The discovery of glass-like interstitial sites uncovers a highly effective mechanism for reducing thermal conductivity. Thus Zn_4Sb_3 is in many ways an ideal 'phonon glass, electron crystal' thermoelectric material.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1038/nmat1154DOIArticle
http://www.nature.com/nmat/journal/v3/n7/full/nmat1154.htmlPublisherArticle
http://www.nature.com/nmat/journal/v3/n7/suppinfo/nmat1154_S1.htmlPublisherSupporting Information
ORCID:
AuthorORCID
Snyder, G. Jeffrey0000-0003-1414-8682
Additional Information:© 2004 Nature Publishing Group. Received 4 January 2004; Accepted 20 April 2004; Published 27 June 2004. We would like to thank Philippe Rabiller, Sossina Haile, Franck Gascoin and Peter Stephens for discussions and preliminary results, and Helena Kauppila for Ga-doping experiments. The Danish Research Councils are acknowledged for funding through the DANSYNC centre, and access to a 512 node PC cluster at the Danish Supercomputer Centre, Southern Denmark University. E. N. thanks M. Sakata and M. Takata for valuable discussions, and K.Kato for experimental help at SPring-8. The synchrotron radiation experiments were performed at beam line BL02B2 at SPring-8 with the approval of the Japan Synchrotron Radiation Research Institute (JASRI).We also thank the European Commission for financial support under the NANOTHERMEL contract. This work was supported in part by the National Science Foundation Center for the Science and Engineering of Materials at Caltech and the Defence Advanced Research Projects Agency at the Jet Propulsion Laboratory under contract with NASA.
Funders:
Funding AgencyGrant Number
Danish Natural Science Research CouncilUNSPECIFIED
European CommissionNANOTHERMEL
NSFUNSPECIFIED
Defence Advanced Research Projects Agency (DARPA)UNSPECIFIED
Issue or Number:7
DOI:10.1038/nmat1154
Record Number:CaltechAUTHORS:20150512-144224016
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20150512-144224016
Official Citation:Snyder, G. J., Christensen, M., Nishibori, E., Caillat, T., & Iversen, B. B. (2004). Disordered zinc in Zn4Sb3 with phonon-glass and electron-crystal thermoelectric properties. [10.1038/nmat1154]. Nat Mater, 3(7), 458-463.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:57465
Collection:CaltechAUTHORS
Deposited By: Joanne McCole
Deposited On:12 May 2015 23:15
Last Modified:10 Nov 2021 21:50

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