학술논문

Electronic excited states as a probe of surface adsorbate structure and dynamics in liquid xenon
Document Type
Technical Report
Author
Source
Other Information: Thesis (Ph.D.)
Subject
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY ADSORPTION
MATHEMATICAL MODELS
EXCITONS
RHODAMINES
SILICON OXIDES
SORPTIVE PROPERTIES
XENON
ABSORPTION SPECTRA
DIMERS
DIPOLES
ENERGY TRANSFER
HARMONIC GENERATION
AMINES
CARBOXYLIC ACIDS
CHALCOGENIDES
DYES
ELEMENTS
FLUIDS
FREQUENCY MIXING
GASES
HETEROCYCLIC ACIDS
HETEROCYCLIC COMPOUNDS
MULTIPOLES
NONMETALS
ORGANIC ACIDS
ORGANIC COMPOUNDS
ORGANIC OXYGEN COMPOUNDS
OXIDES
OXYGEN COMPOUNDS
QUASI PARTICLES
RARE GASES
REAGENTS
SILICON COMPOUNDS
SORPTION
SPECTRA
SURFACE PROPERTIES 400201* -- Chemical & Physicochemical Properties
Language
English
Abstract
A combination of second harmonic generation (SHG) and a simple dipole-dipole interaction model is presented as a new technique for determining adsorbate geometries on surfaces. The polarization dependence of SHG is used to define possible geometries of the adsorbate about the surface normal. Absorption band shifts using geometry constraints imposed by SHG data are derived for a dimer constructed from two arbitrarily placed monomers on the surface using the dipole-dipole interaction potential. These formulae can be used to determine the orientation of the two monomers relative to each other. A simplified version of this formalism is used to interpret absorption band shifts for rhodamine B adsorbed on fused silica. A brief history of the exciton is given with particular detail to Xe. Data are presented for transient absorption at RT in liquid xenon on the picosecond time scale. These are observations of both tunneling through the barrier that separates the free and trapped exciton states and the subsequent trapping of the exciton. In high densities both of these processes are found to occur within 2 to 6 picoseconds in agreement with theories of Kmiecik and Schreiber and of Martin. A threshold density is observed that separates relaxation via single binary collisions and relaxation that proceeds via Martin's resonant energy transfer hopping mechanism.