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  Inorganic Halide Double Perovskites with Optoelectronic Properties Modulated by Sublattice Mixing

Bartel, C. J., Clary, J. M., Sutton, C. A., Vigil-Fowler, D., Goldsmith, B. R., Holder, A. M., et al. (2020). Inorganic Halide Double Perovskites with Optoelectronic Properties Modulated by Sublattice Mixing. Journal of the American Chemical Society, 142(11), 5135-5145. doi:10.1021/jacs.9b12440.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0006-1A30-7 Version Permalink: http://hdl.handle.net/21.11116/0000-0007-5438-C
Genre: Journal Article

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 Creators:
Bartel, Christopher J.1, Author
Clary, Jacob M.1, Author
Sutton, Christopher A.2, Author              
Vigil-Fowler, Derek3, Author
Goldsmith, Bryan R.4, Author
Holder, Aaron M.1, 3, Author
Musgrave, Charles B.1, 3, 5, 6, 7, Author
Affiliations:
1Department of Chemical and Biological Engineering, University of Colorado Boulder, Boulder, Colorado 80309, United States, ou_persistent22              
2Theory, Fritz Haber Institute, Max Planck Society, ou_634547              
3Materials and Chemical Science and Technology Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States, ou_persistent22              
4Department of Chemical Engineering, University of Michigan, Ann Arbor, Michigan 48109, United States, ou_persistent22              
5Department of Chemistry, University of Colorado Boulder, Boulder, Colorado 80309, United States, ou_persistent22              
6Renewable and Sustainable Energy Institute, University of Colorado Boulder, Boulder, Colorado 80309, United States, ou_persistent22              
7Materials Science and Engineering Program, University of Colorado Boulder, Boulder, Colorado 80309, United States, ou_persistent22              

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 Abstract: All-inorganic halide double perovskites have emerged as a promising class of materials that are potentially more stable and less toxic than lead-containing hybrid organic–inorganic perovskite optoelectronic materials. In this work, 311 cesium chloride double perovskites (Cs2BB′Cl6) were selected from a set of 903 compounds as likely being stable on the basis of a statistically learned tolerance factor (τ) for perovskite stability. First-principles calculations on these 311 double perovskites were then performed to assess their stability and identify candidates with band gaps appropriate for optoelectronic applications. We predict that 261 of the 311 Cs2BB′Cl6 compounds are likely synthesizable on the basis of a thermodynamic analysis of their decomposition to competing compounds (decomposition enthalpy <0.05 eV/atom). Of these 261 likely synthesizable compounds, 47 contain no toxic elements and have direct or nearly direct (within 100 meV) band gaps between 1 and 3 eV, as computed with hybrid density functional theory (HSE06). Within this set, we identify the triple-alkali perovskites Cs2[Alk]+[TM]3+Cl6, where Alk is a group 1 alkali cation and TM is a transition-metal cation, as a class of Cs2BB′Cl6 double perovskites with remarkable optical properties, including large and tunable exciton binding energies as computed by the GW-Bethe–Salpeter equation (GW-BSE) method. We attribute the unusual electronic structure of these compounds to the mixing of the Alk-Cl and TM-Cl sublattices, leading to materials with small band gaps, large exciton binding energies, and absorption spectra that are strongly influenced by the identity of the transition metal. The role of the double-perovskite structure in enabling these unique properties is probed through an analysis of the electronic structures and chemical bonding of these compounds in comparison with other transition-metal and alkali transition-metal halides.

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Language(s): eng - English
 Dates: 2019-11-182020-02-242020-03-18
 Publication Status: Published in print
 Pages: 11
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/jacs.9b12440
 Degree: -

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Title: Journal of the American Chemical Society
  Other : J. Am. Chem. Soc.
  Abbreviation : JACS
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: 11 Volume / Issue: 142 (11) Sequence Number: - Start / End Page: 5135 - 5145 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870