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 Young Chemists for 2005
Formation of Large Molecular Cluster Anions and Elucidation of Their Electronic Structures
Masaaki MitsuiAtsushi Nakajima
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2007 Volume 80 Issue 6 Pages 1058-1074

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Abstract

The present account describes our efforts to understand the microscopic aspects of condense phase phenomena, such as ion solvation in molecular liquids and charge carrier localization in molecular solids, by viewing finite-size molecular clusters as their embryonic forms. In this effort, we efficiently prepared supersonically cooled, isolated molecular cluster anions with up to more than 100 constituent molecules and size-selectively investigated their electronic structures using anion photoelectron spectroscopy. Large anionic clusters of two different types of organic molecule; acetonitrile and naphthalene reported as examples of the noteworthy results obtained in our studies. In these two systems, we found that energetically close anionic isomers coexist over a broad range in size, and their contribution in the photoelectron spectra could be separated using anion beam hole-burning technique. A detailed inspection into the electronic states and size-dependent energetics of each isomer has enabled us to establish a link from the large finite cluster to the infinite bulk system.

We efficiently prepared supersonically cooled, isolated molecular cluster anions with up to more than 100 constituent molecules and examined their electronic structures step-by-step using anion photoelectron spectroscopy, to reveal the coexistence of isomers in large finite clusters. Fullsize Image
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© 2007 The Chemical Society of Japan
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