Intracluster Chemical Reactions in the Gas Phase and on the Liquid Surface -State-Selective Analysis of the Reactions-

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In this research project, we explored chemical reaction processes involving clusters and cluster ions. First, intracluster anionic polymerization of acrylonitrile clusters was investigated by use of mass spectroscopy, photoelectron spectoscopy, photodissociation spectroscopy and collision-induced dissociation. It was revealed that three acrylonitrile molecules present in a neutral acrylonitrile cluster are arranged in a ring geometry, and they are polymerized by electron attachment. Secondly, we investigated the collisional dissociation of Na^+_ by He impact, and found that the branching fraction of Na release from Na^+_ is reduced by collisional deformation of Na^+_. Thirdly, we have disovered that in the collision of I^-_ (CO_2)_n with a silicon surface a solvent CO_2 molecule located halfway between the two iodine stoms splits the I^-_ bond as a molecular 'wedge'.As a basis of the reactivity studies, we investigated the electronic and the geometric structures of several transition metal clusters such as Co^+_, Co^-_, V^+_, V^-_and Mn^-_ by means of optical absorption spectroscopy and photoelectron spectroscopy, together with the spin-polarized DV-Xalpha method.We explored a technique to introduce a continuous liquid flow into vacuum (liquid beam) and investigated photo-induced ion-molecule reactions ; the surface of the liquid beam was irradiated with a laser and ions ejected from the surface were mass-analyzed and detected. Proton-transfer reactions and acetal formation reactions were iscovered.