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• W2017019547 abstract "The photoluminescence of uranium(VI) is observed typically in the wavelength range 400-650 nm with the lifetime of several hundreds mus and is known to be quenched in the presence of various halide ions (case A) or alcohols (case B). Here, we show by density functional theory (DFT) calculations that the quenching involves an intermediate triplet excited state that exhibits uranium(V) character. The DFT results are consistent with previous experimental findings suggesting the presence of photoexcited uranium(V) radical pair during the quenching process. In the ground state of uranyl(VI) halides, the ligand contributions to the highest occupied molecular orbitals increase with the atomic number (Z) of halide ion allowing larger ligand-to-metal charge transfer (LMCT) between uranium and the halide ion. Consequently, a larger quenching effect is expected as Z increases. The quenching mechanism is essentially the same in cases A and B, and is driven by an electron transfer from the quencher to the UO(2)(2+) entity. The relative energetic stabilities of the triplet excited state define the fate of uranium, so that in case A uranium(V) is oxidized back to uranium(VI), while in case B uranium remains as pentavalent." @default.
• W2017019547 created "2016-06-24" @default.
• W2017019547 creator A5046012288 @default.
• W2017019547 creator A5051546849 @default.
• W2017019547 creator A5064302325 @default.
• W2017019547 date "2010-06-08" @default.
• W2017019547 modified "2023-09-25" @default.
• W2017019547 title "Photoluminescence of Uranium(VI): Quenching Mechanism and Role of Uranium(V)" @default.
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• W2017019547 doi "https://doi.org/10.1002/chem.201000408" @default.
• W2017019547 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/20533460" @default.
• W2017019547 hasPublicationYear "2010" @default.
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