Espectroscopia de multicoincidencia aplicada ao estudo de moleculas

AUTOR(ES)

Alexandra Mocellin

DATA DE PUBLICAÇÃO

2002

RESUMO

The main purpose of this thesis is to study selective photo-fragmentation processes of free molecules excited by synchrotron radiation using multi-coincidence spectros-copy. Below are summarized some original and important contributions of this work: 1) We show for the first time experimental evidences of ultrafast dissociation in water molecule after O1s ® 4a1 excitation. Before this work there was in the literature a controversy where many authors pointed to the non-bonding character of the 4a1 orbital. Our study present a clear evidence of the anti-bonding character of this orbital. Another important point was the presentation of a new method to study ultrafast dissociation using multi-coincidence spectroscopy. 2) We presented for the first time a study about the dissociation channels of the ozone molecule using the multi-coincidence technique between 12 and 21 eV photo excitation energy. 3) We show in a clear way how the nuclear movement in the intermediate state together with the localization of core states can lead to the selective dissociation of the ozone molecule. In the studies of selective dissociation of molecules it is desirable to observe changes in the pattern of dissociation as a function of the vibrational quantum number of the intermediate state. Although, in the case of ozone the vibrational levels of many normal modes inhibit the individual identification of each vibrational state it is possible to choose a group of this states. By selecting different groups we change the internal energy of the intermediate state. One of the main contributions of this thesis was the observation of changes in the dissociation patterns when different groups of vibrational states were populated in the intermediate state of ozone. These changes demonstrate that the nuclear movement in the intermediate state, which has lifetime of few femtoseconds, can influence the dissociation pattem after electron ionization from inner shell orbital. 4) A new experimental chamber developed at LNLS was used to demonstrate that (even for some polyatomic molecules) the excitation from inner shell orbital leads to the quasi-alignment of this excited molecules. Such alignment occurs with respect to the electric field polarization vector of the synchrotron light. One of the consequences of this study is a better knowledge of the kinetic energy released in the dissociation. The local symmetry of the unoccupied orbital of the molecules can also be obtained. 5) We presented also an instrumentation study in the electron analyzer used in the measurements of article 3. This work provided a substantial improvement of the electron analyzer resolution allowing the realization of the studies performed with ozone. The resolution achieved was due the development of a new electrostatic lens system

ASSUNTO(S)

oxigenio espectroscopia molecular ozonio espectroscopia de ultravioleta sincrotron dissociação

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