Bulletin of the Chemical Society of Japan
Online ISSN : 1348-0634
Print ISSN : 0009-2673
ISSN-L : 0009-2673
The Chemical Society of Japan Award for Creative Work for 2012
Nonadiabatic Electronic Dynamics in Isolated Molecules and in Solution Studied by Ultrafast Time–Energy Mapping of Photoelectron Distributions
Toshinori Suzuki
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2014 Volume 87 Issue 3 Pages 341-354

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Abstract

Nonadiabatic electronic dynamics contribute to the diversity of chemical reactions. We investigate nonadiabatic dynamics in isolated molecules and aqueous solutions by time-resolved photoelectron spectroscopy. For isolated molecules in the gas phase, we combine two-dimensional imaging detection of electrons and a sub-20 fs deep UV and vacuum UV light source to measure time-evolution of the photoelectron kinetic energy and angular distributions. Time–energy mapping of photoelectron angular anisotropy reveals the S2 → S1 internal conversion dynamics through conical intersection in pyrazine, benzene, and toluene. The time–energy mapping is also employed to extract the photoelectron angular distribution in the molecular frame for nitric oxide. For electronic dynamics in aqueous solution, we employ time-resolved photoelectron spectroscopy using a liquid beam and an electrostatic or a time-of-flight electron energy analyzer. Successful observation of ultrafast electron-transfer reactions in aqueous solutions and measurement of electron binding energies of solvated species suggest promising future developments of this very young field.

Nonadiabatic transition between potential energy surfaces creates the diversity of chemical reactions. Ultrafast photoelectron spectroscopy has enabled real-time observation of electronic dynamics in isolated molecules, and its frontier is now extended to aqueous solution. Fullsize Image
 
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© 2014 The Chemical Society of Japan
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