Raman studies of molecular dynamics in bulk and confined liquids
Yi, Jiarui
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https://hdl.handle.net/2142/23561
Description
Title
Raman studies of molecular dynamics in bulk and confined liquids
Author(s)
Yi, Jiarui
Issue Date
1996
Doctoral Committee Chair(s)
Jonas, Jiri
Department of Study
Chemistry, Physical
Physics, Molecular
Discipline
Chemistry, Physical
Physics, Molecular
Degree Granting Institution
University of Illinois at Urbana-Champaign
Degree Name
Ph.D.
Degree Level
Dissertation
Keyword(s)
Chemistry, Physical
Physics, Molecular
Language
eng
Abstract
Molecular dynamics studies is aimed at achieving a molecular level understanding of the macroscopic transport properties of fluids. Raman light scattering technique in combination with high pressure and temperature control equipment provides a powerful experimental tool for studying the molecular dynamic behavior in fluids. Studying the dynamic behavior of liquids confined to the space approaching molecular dimensions is important for understanding the fundamental mechanisms of the various technological applications of porous materials.
The first part of this thesis research focuses on the molecular dynamics and interactions in bulk liquids. The Raman spectra of liquid carbon disulfide were measured as a function of temperature and pressure. From the symmetric allowed Raman bands, the molecular vibrational and reorientational relaxation were studied. From the symmetric forbidden Raman bands, the intermolecular dynamics was studied. The experimental results were discussed and compared with various theoretical models concerning molecular vibrational and reorientational relaxation in liquids. In addition, two phenomena, namely the Fermi resonance and frequency noncoincidence, related to the intermolecular interactions in the liquid were studied as a function of the thermodynamic states.
The second part of this thesis research focuses on the molecular dynamics in confined geometry. The dynamic behavior of two liquids, the interacting liquid acetonitrile and the non-interacting liquid carbon disulfide, confined to the porous sol-gel silica glasses was studied from their Raman spectra with varying pore size, temperature and pressure. The mechanisms leading to the observed confinement effect were discussed in terms of the surface interaction effect, especially the interaction with the surface OH groups, and pure geometrical confinement effect. In addition to the molecular reorientational motion, the confinement effect on the molecular spinning motion in the confined geometry was also investigated using Raman spectroscopy in the last study.
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