2021/03/17 by Gang Tang, Philippe Ghosez, Jiawang Hong
Chemistry · Engineering · Materials Science · Physics and Astronomy · #Antibonding molecular orbital #Atomic orbital #Band gap #Chalcogenide Semiconductor Thin Films #Chemistry #Computational chemistry #Computer science #Crystallography #Electron #Electronic structure #Enhanced Data Rates for GSM Evolution #Materials science #Molecular orbital #Optoelectronics #Perovskite (structure) #Perovskite Materials and Applications #Physics #Quantum Dots Synthesis And Properties #Quantum mechanics #Semiconductor #Telecommunications #cond-mat.mtrl-sci
paper · pdf · doi:10.1021/acs.jpclett.0c03816
published as Journal of Physical Chemistry Letters, 12, 4227-4239 (2021)
arxiv created 2021/03/17 · openalex publication_date 2021/04/26 · arxiv updated 2021/05/07 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/05
Lead (Pb) halide perovskites have achieved great success in recent years because of their excellent optoelectronic properties, which is largely attributed to the lone-pair s orbital-derived antibonding states at the valence band edge. Guided by the key band-edge orbital character, a series of ns 2 -containing (i.e., Sn 2+, Sb 3+, and Bi 3+ ) Pb-free perovskite alternatives have been explored as potential photovoltaic candidates. On the other hand, based on the band-edge orbital components (i.e., M 2+ s and p /X – p orbitals), a series of strategies have been proposed to optimize their optoelectronic properties by modifying the atomic orbitals and orbital interactions. Therefore, understanding the band-edge electronic features from the recently reported halide perovskites is essential for future material design and device optimization. This Perspective first attempts to establish the band-edge orbital–property relationship using a chemically intuitive approach and then rationalizes their superior properties and explains the trends in electronic properties. We hope that this Perspective will provide atomic-level guidance and insights toward the rational design of perovskite semiconductors with outstanding optoelectronic properties.