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• W4281987046 endingPage "10911" @default.
• W4281987046 startingPage "10902" @default.
• W4281987046 abstract "Singlet oxygen, O2(a1Δg), the lowest excited electronic state of molecular oxygen, plays an important role in a range of chemical and biological processes. In liquid solvents, the reactions of singlet oxygen with a solute kinetically compete with solvent-mediated deactivation that yields the ground electronic state of oxygen, O2(X3Σg-). In this regard, the key parameter is the solvent-mediated lifetime of singlet oxygen, which embodies fundamental physical principles ranging from intermolecular interactions that perturb the forbidden O2(a1Δg) → O2(X3Σg-) transition to the transfer of oxygen's excitation energy into the vibrational modes of a solvent molecule M. Extensive research performed by the global community on this oxygen-related issue over the past ∼50 years reflects its significance. Unfortunately, a satisfactory quantitative understanding of this unique solvent effect has remained elusive thus far. In temperature-dependent studies, we have quantified the singlet oxygen lifetime in common aromatic and aliphatic organic solvents, including partially deuterated molecules that exploit the H/D solvent isotope effect on the lifetime. We now account for experimental data, including previously intractable data, using a model that exploits both weak and strong coupling in the M-O2 complex to accommodate the roles that M plays to (1) induce the forbidden O2(a1Δg) → O2(X3Σg-) transition and (2) accept the excitation energy of O2(a1Δg). As such, our approach brings us appreciably closer to an accurate and predictive ab initio solution for the long-standing oxygen-dependent problem that, in turn, should be relevant for a host of other molecular systems." @default.
• W4281987046 created "2022-06-13" @default.
• W4281987046 creator A5021237555 @default.
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• W4281987046 date "2022-06-10" @default.
• W4281987046 modified "2023-09-30" @default.
• W4281987046 title "Perturbed and Activated Decay: The Lifetime of Singlet Oxygen in Liquid Organic Solvents" @default.
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• W4281987046 doi "https://doi.org/10.1021/jacs.2c03444" @default.
• W4281987046 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/35686951" @default.
• W4281987046 hasPublicationYear "2022" @default.
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