Isotope effect on ultrafast charge-transfer-to-solvent reaction from I(-) to water in aqueous NaI solution | |
Suzuki,YI ; Shen,H ; Tang,Y ; Kurahashi,N ; Sekiguchi,K ; Mizuno,T ; Suzuki,T | |
刊名 | CHEMICAL SCIENCE
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2011 | |
卷号 | 2期号:6 |
产权排序 | 第四 |
英文摘要 | A 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. |
学科主题 | 化学 |
公开日期 | 2015-07-14 |
内容类型 | 期刊论文 |
源URL | [http://ir.wipm.ac.cn/handle/112942/1884] ![]() |
专题 | 武汉物理与数学研究所_2011年以前论文发表(包括2011年) |
推荐引用方式 GB/T 7714 | Suzuki,YI,Shen,H,Tang,Y,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). |
APA | Suzuki,YI.,Shen,H.,Tang,Y.,Kurahashi,N.,Sekiguchi,K.,...&Suzuki,T.(2011).Isotope effect on ultrafast charge-transfer-to-solvent reaction from I(-) to water in aqueous NaI solution.CHEMICAL SCIENCE,2(6). |
MLA | Suzuki,YI,et al."Isotope effect on ultrafast charge-transfer-to-solvent reaction from I(-) to water in aqueous NaI solution".CHEMICAL SCIENCE 2.6(2011). |
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