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Isotope effect on ultrafast charge-transfer-to-solvent reaction from I- to water in aqueous NaI solution
Suzuki, Yoshi-Ichi1,2,3; Shen, Huan1,2; Tang, Ying1,2,4; Kurahashi, Naoya1,2; Sekiguchi, Kentaro1,2; Mizuno, Tomoya3; Suzuki, Toshinori1,2,3
2011
Source PublicationCHEMICAL SCIENCE
Volume2Issue:6Pages:1094-1102
SubtypeArticle
AbstractA charge-transfer-to-solvent (CTTS) reaction from a photoexcited iodine atomic anion, I- (aq), in bulk water (H2O and D2O) was studied by time-resolved photoelectron spectroscopy using a liquid beam (microjet) of aqueous NaI solution. The P-2(3/2) CTTS state of I- (aq) was excited by a 226 nm femtosecond laser pulse and the evolution of the nonstationary electronic state was probed using another ultraviolet femtosecond laser pulse. Global fitting of the observed time-dependent photoelectron kinetic energy distributions provided the time constants of individual reaction steps and the photoelectron spectra from the CTTS state, a contact pair, the solvent-separated state, and a hydrated electron. Most of the elementary reaction steps revealed a strong deuterium isotope effect, indicating coupling of the electron dynamics and the hydrogen atomic motion of solvent water. However, nondiffusive geminate recombination processes from the CTTS state and a contact pair were almost insensitive to deuteration. Consequently, geminate recombination processes from the CTTS state and a contact pair occurs more efficiently in D2O, because the response of water is decelerated in D2O. In contrast, the recombination process from the solvent-separated state in the final step of the CTTS reaction is less efficient in D2O, presumably due to the smaller zero point energy.
WOS HeadingsScience & Technology ; Physical Sciences
DOI10.1039/c0sc00650e
WOS KeywordRESOLVED PHOTOELECTRON-SPECTROSCOPY ; ELECTRON-BINDING ENERGIES ; DENSITY-FUNCTIONAL THEORY ; RESONANCE RAMAN-SPECTRA ; LIQUID WATER ; HYDRATED ELECTRON ; SOLVATED ELECTRONS ; MOLECULAR-DYNAMICS ; RECOMBINATION DYNAMICS ; TEMPERATURE-DEPENDENCE
Indexed BySCI
Language英语
WOS Research AreaChemistry
WOS SubjectChemistry, Multidisciplinary
WOS IDWOS:000290629900015
Citation statistics
Cited Times:25[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.apm.ac.cn/handle/112942/8230
Collection2011年以前论文发表(包括2011年)
Affiliation1.Kyoto Univ, Grad Sch Sci, Dept Chem, Kyoto 6068502, Japan
2.Japan Sci & Technol Agcy, CREST, Chiyoda Ku, Tokyo 1020075, Japan
3.RIKEN, Adv Sci Inst, Chem Dynam Lab, Wako, Saitama 3510198, Japan
4.Chinese Acad Sci, Wuhan Inst Phys & Math, Wuhan, Peoples R China
Recommended Citation
GB/T 7714
Suzuki, Yoshi-Ichi,Shen, Huan,Tang, Ying,et al. Isotope effect on ultrafast charge-transfer-to-solvent reaction from I- to water in aqueous NaI solution[J]. CHEMICAL SCIENCE,2011,2(6):1094-1102.
APA Suzuki, Yoshi-Ichi.,Shen, Huan.,Tang, Ying.,Kurahashi, Naoya.,Sekiguchi, Kentaro.,...&Suzuki, Toshinori.(2011).Isotope effect on ultrafast charge-transfer-to-solvent reaction from I- to water in aqueous NaI solution.CHEMICAL SCIENCE,2(6),1094-1102.
MLA Suzuki, Yoshi-Ichi,et al."Isotope effect on ultrafast charge-transfer-to-solvent reaction from I- to water in aqueous NaI solution".CHEMICAL SCIENCE 2.6(2011):1094-1102.
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