화학공학소재연구정보센터
Journal of Chemical Physics, Vol.110, No.9, 4382-4393, 1999
Energy-resolved collision-induced dissociation of Al-n(+) clusters (n=2-11) in the center of mass energy range from few hundred meV to 10 eV
Energy-resolved collision-induced dissociation (CID) of Al-n(+) (n = 2 - 11) in collision with argon is presented for the energy ranges from few hundred meV to 10 eV in the center of mass frame. The experiments were carried out with a recently constructed secondary ion tandem mass spectrometer, that is described in detail. The collision energy dependence is measured for the total and the partial dissociation cross sections, and the dissociation thresholds for the individual processes are estimated. The release of Al+ is found to be the dominating channel for n < 8. For n > 8, the cross section for the release of Al+ and Al are comparable. The release of more than one neutral atom from the larger clusters (n > 6) is found to be in good agreement with sequential atom loss. In the case of the smaller clusters, on the other hand, fission is the energetically favorable process. The closed shell cluster, Al-7(+) (20 valence electrons), is found to be exceptionally stable and the adiabatic ionization potential of Al-7 is found to be lower than that of the monomer. The stability of Al-7(+) is further reflected in the dissociation dynamics of the next neighbor, Al-8(+). The high stability of Al-7(+) as well as the dissociation dynamics of Al-8(+) are treated in the simple frame of the electronic shell model. Unlike Al-7(+), Al-3(+) (with 8 valence electrons) shows no sign of increased stability, and the dissociation dynamics seems to be controlled by the spin selection rules, rather than the energetics. In the present work, general trends and the dissociation dynamics of individual clusters are discussed. Qualitative information on the development of the geometric and electronic structure, with increasing cluster size, is deduced and discussed in terms of a transition from a covalent to a metallic character. Finally, this work is compared to earlier theoretical and experimental approaches to Al-n(+) clusters.