Fundamentals of Chemistry at Surfaces and Beyond
Abstract
Fundamental developments in this project include (1) an analytic theory of pooling of infrared quanta on surfaces, with a potential application to laser-selective chemistry, (2) diffusion-electron transfer reaction rate theory for intermittent fluorescence of semiconductor nanoparticles, explaining the power law distribution of bright and dark periods and the exponential tail for bright periods, (3) theory of intermittent fluorescence of dyes on semiconductor nanoparticles and plane surfaces, (4) approximate semiclassical instanton theory for H-tunneling in small and large systems, computationally less demanding than more accurate approaches and whose utility is being explored, and (5) marked improvement of the range of validity of the maximum likelihood method so as to treat power law data, converging when the common method diverges. The theory of infrared quanta pooling (accumulation of quanta in individual adsorbed molecules on surfaces) rapid equilibration of the quanta was assumed among the sites and the results were compared with a kinetic Monte Carlo computational solution of the coupled kinetic differential equations. When the assumption is valid (high light intensities), the theory has applications to infrared laser selective chemistry on surfaces. Research has also been initiated on a fundamental electron transfer theory for perovskite-like and other photovoltaic solar cells.
Document Details
- Document Type
- Technical Report
- Publication Date
- Sep 23, 2013
- Accession Number
- ADA597550
Entities
People
- Rudolph A. Marcus
Organizations
- California Institute of Technology