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arXiv · 2103.09453

Band-Edge Orbital Engineering of Perovskite Semiconductors for Optoelectronic Applications

Gang Tang·Philippe Ghosez·Jiawang Hong
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Abstract

Lead (Pb) halide perovskites have achieved great success in recent years due to 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 ns2-containing (i.e., Sn2+, Sb3+, Bi3+) Pb-free perovskite alternatives have been explored as potential photovoltaic candidates. On the other hand, based on the band-edge orbital components (i.e., M2+ 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. Here, this Perspective first attempts to establish the band-edge orbital-property relationship using a chemically intuitive approach, and then rationalizes their superior properties and understands 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.

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Gang Tang, Philippe Ghosez, Jiawang Hong. 2021-03-17. Band-Edge Orbital Engineering of Perovskite Semiconductors for Optoelectronic Applications. https://doi.org/10.1021/acs.jpclett.0c03816

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