Binding energy of solvated electrons and retrieval of true UV photoelectron spectra of liquids
Binding energy of solvated electrons and retrieval of true UV photoelectron spectra of liquids
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DOI：
10.1126/sciadv.aaw6896
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发表时间：
2019-08-01
期刊：
影响因子：
13.6
通讯作者：
Suzuki, Toshinori
中科院分区：
文献类型：
--
作者：
Nishitani, Junichi;Yamamoto, Yo-ichi;Suzuki, Toshinori
溶剂化电子的电子能量和动力学是最简单但难以捉摸的化学物质，引起了化学、物理学和生物学的兴趣。在这里，我们展示了使用单阶高次谐波液体的极紫外（EUV）光电子能谱精确测量了液态水、甲醇和乙醇中溶剂化电子的电子结合能分布。在所有情况下分布都是高斯分布。利用溶剂化电子的EUV和UV光电子能谱，我们成功地从液体中非弹性散射导致的光谱展宽和能量转移中恢复了尖锐的电子动能分布，克服了液体超快UV光电子能谱的障碍。该方法针对电荷转移到溶剂反应以及水合电子从第一激发态的超快内部转换的基准系统进行了演示。
The electronic energy and dynamics of solvated electrons, the simplest yet elusive chemical species, is of interest in chemistry, physics, and biology. Here, we present the electron binding energy distributions of solvated electrons in liquid water, methanol, and ethanol accurately measured using extreme ultraviolet (EUV) photoelectron spectroscopy of liquids with a single-order high harmonic. The distributions are Gaussian in all cases. Using the EUV and UV photoelectron spectra of solvated electrons, we succeeded in retrieving sharp electron kinetic energy distributions from the spectra broadened and energy shifted by inelastic scattering in liquids, overcoming an obstacle in ultrafast UV photoelectron spectroscopy of liquids. The method is demonstrated for the benchmark systems of charge transfer to solvent reaction and ultrafast internal conversion of hydrated electron from the first excited state.