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Femtosecond X-ray Spectroscopy Directly Quantifies Transient Excited-State Mixed Valency.
- Source :
- The journal of physical chemistry letters; vol 13, iss 1, 378-386; 1948-7185
- Publication Year :
- 2022
-
Abstract
- Quantifying charge delocalization associated with short-lived photoexcited states of molecular complexes in solution remains experimentally challenging, requiring local element specific femtosecond experimental probes of time-evolving electron transfer. In this study, we quantify the evolving valence hole charge distribution in the photoexcited charge transfer state of a prototypical mixed valence bimetallic iron-ruthenium complex, [(CN)5FeIICNRuIII(NH3)5]-, in water by combining femtosecond X-ray spectroscopy measurements with time-dependent density functional theory calculations of the excited-state dynamics. We estimate the valence hole charge that accumulated at the Fe atom to be 0.6 ± 0.2, resulting from excited-state metal-to-metal charge transfer, on an ∼60 fs time scale. Our combined experimental and computational approach provides a spectroscopic ruler for quantifying excited-state valency in solvated complexes.
Details
- Database :
- OAIster
- Journal :
- The journal of physical chemistry letters; vol 13, iss 1, 378-386; 1948-7185
- Notes :
- application/pdf, The journal of physical chemistry letters vol 13, iss 1, 378-386 1948-7185
- Publication Type :
- Electronic Resource
- Accession number :
- edsoai.on1377982758
- Document Type :
- Electronic Resource