期刊
FARADAY DISCUSSIONS
卷 154, 期 -, 页码 409-424出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c1fd00058f
关键词
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资金
- Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-FG02-89ER14020]
- German Research Foundation (DFG) [SPP 1191]
- China Scholarship Council
- Alexander von Humboldt Foundation
The complete solvation response of coumarin 153 (C153) has been determined over the range 10(-13)-10(-8) s in a variety of ionic liquids by combining femtosecond broad-band fluorescence upconversion and picosecond time-correlated single photon counting measurements. These data are used together with recently reported dielectric data in eight ionic liquids to test the accuracy of a simple continuum model for predicting solvation dynamics. In most cases the features of the solvation response functions predicted by the dielectric continuum model are similar to the measured dynamics of C153. The predicted dynamics are, however, systematically faster than those observed, on average by a factor of 3-5. Computer simulations of a model solute/ionic liquid system also exhibit the same relationship between dielectric predictions and observed dynamics. The simulations point to spatial dispersion of the polarization response as an important contributor to the over-prediction of solvation rates in ionic liquids.
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