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Time-Resolved Study on Photo-Initiated Isomerization of Clusters

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Physical Chemistry of Cold Gas-Phase Functional Molecules and Clusters

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Abstract

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 detected in real time. The intermolecular isomerization reaction is triggered by resonant photoionization, and infrared absorption at variable delay is detected by decrease of parent ion signal due to photodissociation. The advantage of this time-resolved spectroscopy is demonstrated by the isomerization reactions in phenol with nonpolar ligands (rare gas and methane molecule). It gives salient properties of the reaction, including rates, yields, pathways, branching ratios of competing reactions, back reactions, and timescales of energy relaxation processes. Mechanism of the isomerization reaction and its relation to intracluster vibrational relaxation are also discussed.

This article is based on the review entitled “Probing Solvation Dynamics around Aromatic and Biological Molecules at the Single-Molecular Level” with permission from Chemical Review (Reference [12], Copyright 2016 American Chemical Society).

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Acknowledgements

The studies described in this review were generously supported over the years by Deutsche Forschungsgemeinschaft (DFG, DO/729-1,2,4), MEXT (innovative area 2503 and the Cooperative Research Program of the “Network Joint Research Center for Materials and Devices”), JSPS (Grant-in-Aid for Scientific Research (A) 15H02157, the Core-to-Core Program 22003 and Bilateral Open Partnership Joint Research Projects) and World Research Hub Initiative (WRHI) of Tokyo Institute of Technology. O.D. acknowledges two JSPS fellowships in 2001 (S-01234), during which this project was initiated, and in 2006 (S-06068). M. M. and M. F. are grateful for supports from the Alexander von Humboldt foundation. We are very grateful to the former and current undergraduate, graduate, and postgraduate students of our two groups, who substantially contributed to the results described in this review and whose names are mentioned in the corresponding references. We further deeply acknowledge fruitful discussions and contributions of our collaborators Mitsuhiko Miyazaki, Shun-ichi Ishuichi, Makoto Sakai (all Tokyo Institute of Technology), Hiroshi Sekiya (Kyushu University), Klaus Müller-Dethlefs (University of Manchester), Roland Mitric, and Volker Engel (both University of Würzburg).

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Authors and Affiliations

  1. Laboratory for Chemistry and Life Science, Institute of Innovative Research, Tokyo Institute of Technology, Yokohama, 226-8503, Japan

    Masaaki Fujii

  2. Institut für Optik und Atomare Physik, Technische Universität Berlin, Hardenbergstr. 36, 10623, Berlin, Germany

    Otto Dopfer

  3. School of Life Science and Technology, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa, 226-8501, Japan

    Masaaki Fujii

  4. Tokyo Tech World Research Hub Initiative (WRHI), Institute of Innovation Research, Tokyo Institute of Technology, 4259, Nagatsuta-cho, Midori-ku, Yokohama, Japan

    Masaaki Fujii & Otto Dopfer

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  1. Masaaki Fujii
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  2. Otto Dopfer
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Correspondence to Masaaki Fujii .

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Editors and Affiliations

  1. Hiroshima University, Higashi-hiroshima, Japan

    Takayuki Ebata

  2. Tokyo Institute of Technology, Yokohama, Japan

    Masaaki Fujii

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Fujii, M., Dopfer, O. (2019). Time-Resolved Study on Photo-Initiated Isomerization of Clusters. In: Ebata, T., Fujii, M. (eds) Physical Chemistry of Cold Gas-Phase Functional Molecules and Clusters. Springer, Singapore. https://doi.org/10.1007/978-981-13-9371-6_13

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