Probing Solvation Dynamics around Aromatic and Biological Molecules at the Single-Molecular Level
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- Otto Dopfer
- Institut für Optik und Atomare Physik, Technische Universität Berlin, Hardenbergstrasse 36, 10623 Berlin, Germany
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- Masaaki Fujii
- Laboratory for Chemistry and Life Science, Tokyo Institute of Technology, Yokohama 226-8503, Japan
書誌事項
- 公開日
- 2016-04-07
- 資源種別
- journal article
- DOI
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- 10.1021/acs.chemrev.5b00610
- 公開者
- American Chemical Society (ACS)
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説明
Solvation processes play a crucial role in chemical reactions and biomolecular recognition phenomena. Although solvation dynamics of interfacial or biological water has been studied extensively in aqueous solution, the results are generally averaged over several solvation layers and the motion of individual solvent molecules is difficult to capture. This review describes the development and application of a new experimental approach, namely, picosecond time-resolved pump-probe infrared spectroscopy of size- and isomer-selected aromatic clusters, in which for the first time the dynamics of a single individual solvent molecule can be followed in real time. The intermolecular isomerization reaction is triggered by resonant photoionization (pump), and infrared photodissociation (probe) at variable delay generates the spectroscopic signature of salient properties of the reaction, including rates, yields, pathways, branching ratios of competing reactions, existence of reaction intermediates, occurrence of back reactions, and time scales of energy relaxation processes. It is shown that this relevant information can reliably be decoded from the experimental spectra by sophisticated molecular dynamics simulations. This review covers a description of the experimental strategies and spectroscopic methods along with all applications to date, which range from aromatic clusters with nonpolar solvent molecules to aromatic monohydrated biomolecules.
収録刊行物
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- Chemical Reviews
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Chemical Reviews 116 (9), 5432-5463, 2016-04-07
American Chemical Society (ACS)
