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Copper-based chalcogenide semiconductors are particularly attractive materials for photovoltaic and nonlinear optical applications. Unfortunately, accurate theoretical understanding of the optical responses of these materials is hindered by the presence of strongly localized Cu 3d electrons. To assess the validity of calculation schemes for determining the optical properties of Cu-based chalcogenides, different density functional theory (DFT) approaches including the conventional Perdew-Burke-Ernzerhof (PBE) method and the modified Becke-Johnson (mBJ) potential with and without Hubbard U correction, and the hybrid HSE06 methods are employed to evaluate the linear and nonlinear optical performances of 16 typical Cu-based chalcogenides. We calculate band gaps, dielectric functions, refractive indices, absorption coefficients, and the second harmonic generation susceptibilities of these compounds and compare the results with available experimental measurements. It is clear that the mBJ + U approach yields band gaps close to those predicted using the HSE06 method, which is consistent with the experimental values. More importantly, the fundamental optical properties in the infrared-visible light region calculated within the mBJ + U method agree better with experiments compared with the HSE06 functional. In addition to the linear optical responses, the mBJ potential with on-site Coulomb U correction to the Cu-3d state is also capable of describing the optical nonlinearity of copper chalcogenides reasonably.
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JOURNAL OF PHYSICAL CHEMISTRY C
ISSN: 1932-7447
Year: 2022
Issue: 9
Volume: 126
Page: 4684-4697
3 . 7
JCR@2022
3 . 3 0 0
JCR@2023
ESI Discipline: CHEMISTRY;
ESI HC Threshold:74
JCR Journal Grade:2
CAS Journal Grade:3
Cited Count:
WoS CC Cited Count: 8
SCOPUS Cited Count:
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 0
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