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Electronic Modulation in Site-Selective Occupation of Quasi-2D Triangular-Lattice Cs 2 CuCl 4- x Br x Perovskite Probed by Surface-Sensitive Characterization
A controllable electronic manipulation in a frustrated magnetic system such as solution-based two-dimensional (2D) all-inorganic perovskites offers a possible route for their integrations with electronic and magnetic devices for their advanced applications. Here, we perform element-specific investig...
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Published in: | ACS applied materials & interfaces 2020-01, Vol.12 (3), p.4114-4122 |
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Main Authors: | , , , , , , , , , , , |
Format: | Article |
Language: | English |
Citations: | Items that this one cites Items that cite this one |
Online Access: | Get full text |
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Summary: | A controllable electronic manipulation in a frustrated magnetic system such as solution-based two-dimensional (2D) all-inorganic perovskites offers a possible route for their integrations with electronic and magnetic devices for their advanced applications. Here, we perform element-specific investigations of an emergent class of quasi-2D all-inorganic perovskites Cs
CuCl
Br
with (0 ≤
≤ 4) using a combination of synchrotron-radiation photoelectron techniques. Surface- and element-sensitive X-ray absorption spectroscopy spectra of Cu
edges indicate strong electronic transition that is largely influenced by their halogen content at room temperature. This implies that site-selective occupation largely dominates the electronic transition across the unoccupied states of these series since chlorine atoms possess a stronger electronegative character than bromine atoms. Moreover, the implication of halogen site is reflected in the valence band of Cl-rich copper perovskite in which the valence band edge is closer to Fermi energy (
) than that of the Br-rich compound. Furthermore, X-ray magnetic circular dichroism spectra of mixed ratio and Br-rich compounds exhibit antiferromagnetism at room temperature. These site-specific magnetic-spectroscopic results are corroborated by density functional theory calculations. The strong electronic modulation and the local magnetic spectroscopy results in these solution-based and low-temperature-growth materials will pave the way toward energy- and cost-efficient perovskite devices. |
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ISSN: | 1944-8244 1944-8252 |
DOI: | 10.1021/acsami.9b19517 |