| Título: | Spectroscopic investigations of the X and A state dynamics of ¹³C₂H₂ |
| Autores: | Silva, Michelle Lee, 1974- |
| Fecha: |
2005-08-23 2005-08-23 2002 2002 |
| Publicador: | MIT |
| Fuente: |
 |
| Tipo: | Thesis |
| Tema: | Chemistry. |
| Descripción: |
The objective of the experiments described in this thesis is to perform a detailed spectroscopic study of the dynamics on the A and X state surfaces of 13C2H2 in order to further understand the acetylene - vinylidene isomerization process in the ground electronic state. Acetylene exemplifies one of the simplest bond-breaking isomerization systems and it has served as a prototype for studies of large amplitude vibrational motion in molecules. The short-time, large amplitude, vibrational dynamics of acetylene are well understood up to the acetylene - vinylidene isomerization barrier. However, direct observation of acetylene - vinylidene isomerization remains elusive. To this end, five experimental techniques, Laser Induced Fluorescence (LIF), Dispersed Fluorescence (DF), Cavity Ring-Down Spectroscopy (CRDS), Noise Immune Cavity Enhanced Optical Heterodyne Molecular Spectroscopy (NICE-OHMS) and Stimulated Emission Pumping (SEP) are employed to study the spectroscopy and dynamics of acetylene. All of these experiments focus on 13C2H2 instead of 12C2H2, except for the Cavity Ring-Down measurements. These experiments concentrate on 13C2H2 because of the possibility of observing nuclear permutation tunneling splittings which are indicative of acetylene - vinylidene isomerization. The experiments described here provide the necessary foundation for observing nuclear permutation tunneling splittings. Attempts were made to observe nuclear permutation tunneling splittings in 13C2H2 using NICE-OHMS and SEP. Although permutation splittings were not observed, these experiments enhanced our knowledge of the dynamics and spectroscopy of the A and X states of 13C2H2. (cont.) Moreover, these experiments have led to a better understanding of how to design and focus future studies in order to successfully observe nuclear permutation tunneling splittings in 13C2H2 as a means for directly observing acetylene - vinylidene isomerization. by Michelle Lee Silva. Thesis (Ph.D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2002. In title on t.p. and in abstract, "A" and "X" appear with a tilde above the letter. Vita. Includes bibliographical references (p. 170-175). |
| Idioma: | Inglés |
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