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• W2973258243 startingPage "114503" @default.
• W2973258243 abstract "We report solvated electron (esolv-) formation dynamics from the conduction band of liquid methanol studied using femtosecond time-resolved photoelectron spectroscopy. Liquid methanol is excited with vacuum UV (9.3 eV) pump pulses, and the subsequent electron dynamics are probed with UV pulses. The photoelectron signal exhibits a short-lived component (τ = 85 fs) without spectral evolution followed by a long-lived component with continuous spectral evolution over tens of picoseconds. We ascribe the former to a superexcited state, most likely the Wannier exciton, and the latter to the ground electronic state of esolv-. In order to extract accurate energetics from the observed photoelectron spectra, we employ a spectral retrieval method to account for spectral broadening and shifting due to inelastic scattering of photoelectrons in the liquid. The electron binding energy (eBE) of the initial trap state of an electron is determined to be about 1.5 eV, and its biexponential increase up to 3.4 eV is observed with time constants of 2 and 31 ps, which are greater than 0.27 and 13 ps observed for esolv- created by the charge-transfer-to-solvent reaction from CH3O- to liquid methanol. The solvation dynamics of esolv- created by the electron trapping exhibit a pseudoisosbestic point at a pump-probe delay time of around 15 ps, and the peak energy of the eBE distribution rapidly changes around that time. These results indicate that there exist two trap states, both of which exhibit increasing eBE with time; however, the eBE of the shallow trap state increases only up to 2.1 eV, and transformation to a deep trap state at 25 ps occurs to reach an eBE of 3.4 eV." @default.
• W2973258243 created "2019-09-26" @default.
• W2973258243 creator A5004124288 @default.
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• W2973258243 date "2019-09-21" @default.
• W2973258243 modified "2023-09-24" @default.
• W2973258243 title "Solvated electron formation from the conduction band of liquid methanol: Transformation from a shallow to deep trap state" @default.
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• W2973258243 doi "https://doi.org/10.1063/1.5116818" @default.
• W2973258243 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/31542023" @default.
• W2973258243 hasPublicationYear "2019" @default.
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