Computational study of halide perovskite-derived A2BX6 inorganic compounds : chemical trends in electronic structure and structural stability

The electronic structure and energetic stability of A2BX6 halide compounds with the cubic and tetragonal variants of the perovskite-derived K2PtCl6 prototype structure are investigated computationally within the frameworks of density-functional-theory (DFT) and hybrid (HSE06) functionals. The HSE06...

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Main Authors: Cai, Yao, Xie, Wei, Ding, Hong, Chen, Yan, Thirumal, Krishnamoorthy, Wong, Lydia Helena, Mathews, Nripan, Mhaisalkar, Subodh Gautam, Sherburne, Matthew, Asta, Mark
Other Authors: School of Materials Science & Engineering
Format: Article
Language:English
Published: 2020
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Online Access:https://hdl.handle.net/10356/140302
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Institution: Nanyang Technological University
Language: English
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spelling sg-ntu-dr.10356-1403022023-07-14T15:44:40Z Computational study of halide perovskite-derived A2BX6 inorganic compounds : chemical trends in electronic structure and structural stability Cai, Yao Xie, Wei Ding, Hong Chen, Yan Thirumal, Krishnamoorthy Wong, Lydia Helena Mathews, Nripan Mhaisalkar, Subodh Gautam Sherburne, Matthew Asta, Mark School of Materials Science & Engineering Interdisciplinary Graduate School (IGS) Energy Research Institute @ NTU (ERI@N) Engineering::Materials Band Structure Anions The electronic structure and energetic stability of A2BX6 halide compounds with the cubic and tetragonal variants of the perovskite-derived K2PtCl6 prototype structure are investigated computationally within the frameworks of density-functional-theory (DFT) and hybrid (HSE06) functionals. The HSE06 calculations are undertaken for seven known A2BX6 compounds with A = K, Rb, and Cs; and B = Sn, Pd, Pt, Te, and X = I. Trends in band gaps and energetic stability are identified, which are explored further employing DFT calculations over a larger range of chemistries, characterized by A = K, Rb, Cs, B = Si, Ge, Sn, Pb, Ni, Pd, Pt, Se, and Te; and X = Cl, Br, I. For the systems investigated in this work, the band gap increases from iodide to bromide to chloride. Further, variations in the A site cation influences the band gap as well as the preferred degree of tetragonal distortion. Smaller A site cations such as K and Rb favor tetragonal structural distortions, resulting in a slightly larger band gap. For variations in the B site in the (Ni, Pd, Pt) group and the (Se, Te) group, the band gap increases with increasing cation size. However, no observed chemical trend with respect to cation size for band gap was found for the (Si, Sn, Ge, Pb) group. The findings in this work provide guidelines for the design of halide A2BX6 compounds for potential photovoltaic applications. NRF (Natl Research Foundation, S’pore) Accepted version 2020-05-28T01:23:00Z 2020-05-28T01:23:00Z 2017 Journal Article Cai, Y., Xie, W., Ding, H., Chen, Y., Thirumal, K., Wong, L., . . ., Asta, M. (2017). Computational study of halide perovskite-derived A2BX6 inorganic compounds : chemical trends in electronic structure and structural stability. Chemistry of Materials, 29(18), 7740–7749. doi:10.1021/acs.chemmater.7b02013 0897-4756 https://hdl.handle.net/10356/140302 10.1021/acs.chemmater.7b02013 2-s2.0-85029931749 18 29 7740 7749 en Chemistry of Materials This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.chemmater.7b02013 application/pdf
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Materials
Band Structure
Anions
spellingShingle Engineering::Materials
Band Structure
Anions
Cai, Yao
Xie, Wei
Ding, Hong
Chen, Yan
Thirumal, Krishnamoorthy
Wong, Lydia Helena
Mathews, Nripan
Mhaisalkar, Subodh Gautam
Sherburne, Matthew
Asta, Mark
Computational study of halide perovskite-derived A2BX6 inorganic compounds : chemical trends in electronic structure and structural stability
description The electronic structure and energetic stability of A2BX6 halide compounds with the cubic and tetragonal variants of the perovskite-derived K2PtCl6 prototype structure are investigated computationally within the frameworks of density-functional-theory (DFT) and hybrid (HSE06) functionals. The HSE06 calculations are undertaken for seven known A2BX6 compounds with A = K, Rb, and Cs; and B = Sn, Pd, Pt, Te, and X = I. Trends in band gaps and energetic stability are identified, which are explored further employing DFT calculations over a larger range of chemistries, characterized by A = K, Rb, Cs, B = Si, Ge, Sn, Pb, Ni, Pd, Pt, Se, and Te; and X = Cl, Br, I. For the systems investigated in this work, the band gap increases from iodide to bromide to chloride. Further, variations in the A site cation influences the band gap as well as the preferred degree of tetragonal distortion. Smaller A site cations such as K and Rb favor tetragonal structural distortions, resulting in a slightly larger band gap. For variations in the B site in the (Ni, Pd, Pt) group and the (Se, Te) group, the band gap increases with increasing cation size. However, no observed chemical trend with respect to cation size for band gap was found for the (Si, Sn, Ge, Pb) group. The findings in this work provide guidelines for the design of halide A2BX6 compounds for potential photovoltaic applications.
author2 School of Materials Science & Engineering
author_facet School of Materials Science & Engineering
Cai, Yao
Xie, Wei
Ding, Hong
Chen, Yan
Thirumal, Krishnamoorthy
Wong, Lydia Helena
Mathews, Nripan
Mhaisalkar, Subodh Gautam
Sherburne, Matthew
Asta, Mark
format Article
author Cai, Yao
Xie, Wei
Ding, Hong
Chen, Yan
Thirumal, Krishnamoorthy
Wong, Lydia Helena
Mathews, Nripan
Mhaisalkar, Subodh Gautam
Sherburne, Matthew
Asta, Mark
author_sort Cai, Yao
title Computational study of halide perovskite-derived A2BX6 inorganic compounds : chemical trends in electronic structure and structural stability
title_short Computational study of halide perovskite-derived A2BX6 inorganic compounds : chemical trends in electronic structure and structural stability
title_full Computational study of halide perovskite-derived A2BX6 inorganic compounds : chemical trends in electronic structure and structural stability
title_fullStr Computational study of halide perovskite-derived A2BX6 inorganic compounds : chemical trends in electronic structure and structural stability
title_full_unstemmed Computational study of halide perovskite-derived A2BX6 inorganic compounds : chemical trends in electronic structure and structural stability
title_sort computational study of halide perovskite-derived a2bx6 inorganic compounds : chemical trends in electronic structure and structural stability
publishDate 2020
url https://hdl.handle.net/10356/140302
_version_ 1772828490520854528