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Uncovering the Origin of the Emitting States in Bi3+-Activated CaMO3 (M = Zr, Sn, Ti) Perovskites: Metal-To-Metal Charge Transfer Versus s–p Transitions

Cite this: J. Phys. Chem. C 2019, 123, 23, 14677–14688
Publication Date (Web):May 15, 2019
https://doi.org/10.1021/acs.jpcc.9b03940
Copyright © 2019 American Chemical Society

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    Abstract

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    After more than a century of studies on the optical properties of Bi3+ ions, the assignment of the nature of the emissions and the bands of the absorption spectra remain ambiguous. Here, we report an insight into the spectroscopy of Bi3+-activated CaMO3 perovskites (M = Zr, Sn, and Ti), discussing the factors driving the metal-to-metal charge transfer and sp → s2 transitions. With the aim to figure out the whole scenario, a combined experimental and theoretical approach is employed. The comparison between the temperature dependence of the photoluminescence emissions with the temperature dependence of the exciton energy of the systems has led to an unprecedented evidence of the charge-transfer character of the emitting states in Bi3+-activated phosphors. Low-temperature vacuum ultraviolet spectroscopy together with the design of the vacuum-referred binding energy diagram of the luminescent center is exploited to shed light on the origin of the absorption bands. In addition, the X-ray absorption near the edge structure unambiguously confirmed the stabilization of Bi3+ in the Ca2+ site in both CaSnO3 and CaZrO3 perovskites. This breakthrough into the understanding of the excited-state origin of Bi3+ could pave the way toward the design of a new generation of effective Bi3+-activated phosphors.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.9b03940.

    • Normalized temperature-dependent PL spectra, synchrotron-radiation VUV–vis PLE spectra deconvolution analysis (9 K) and experimental Bi L3-edge HERFD–XANES together with the results of FDMNES calculations, and partial DOS extracted for Bi in the Bi2O3 and NaBiO3 references (PDF)

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