Abstract
Using a newly developed dual beam laser plasma method, the C4- anion cluster has been formed and deposited in an argon matrix and studied via Fourier transform infrared spectroscopy. An infrared band at 1699.8 cm-1, previously assigned to a combination mode of the neutral C4 cluster, is shown to be due to the asymmetric stretching fundamental of the C4- anion. This attribution is based on the different behavior of the known 1543.4 cm-1 neutral C4 asymmetric stretching mode and the 1699.8 cm-1 band under action of annealing, photolysis, and addition of the electron trap, CCl4, to the plasma gas. Density functional theory and ab initio theory calculations predict a stable, linear C4 anionic cluster that should possess a moderately strong IR band close to this position. Previous isotopic (12C/13C) splitting patterns are reinterpreted and shown to match very well with the theoretically predicted splitting patterns for C4-. An electron photodetachment energy of 4.51 eV is found and compares well with the gas-phase value when account is taken of the matrix stabilization energy of 0.63 eV. It is proposed that anions are formed via electron capture by preformed neutral C4 clusters and that a steady state of neutral and anionic C4 clusters is established in the matrix.
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