Mortimer, Robert George (1963) I. Irreversible thermodynamics of systems containing radiation. Application to photochemical reactions. II. Mean values in ensembles of systems of particles with long-range potentials. III. Approximations to time-dependent ensemble averages. Dissertation (Ph.D.), California Institute of Technology. http://resolver.caltech.edu/CaltechTHESIS:04302012-143409544
I. The general theory of the irreversible thermodynamics of chemically reacting systems interacting with radiation is developed. From this, a limit to the efficiency of photochemical processes is derived, and this is compared with approximate experimental efficiencies of published researches, which are found to be considerably lower.
II. A general cluster method of obtaining approximations to ensemble averages of functions depending on coordinates and/or momenta at a single time is derived, starting with a method, due to Mazo and Zemach, valid only for short-range forces, and proceeding to a method capable of treating systems of particles with long and short-range potentials, such as ionic solutions.
III. Approaches to the time evolution of distribution functions and to time-correlation functions are discussed. A general perturbation series approach to time-correlation functions through the exponential Liouville operator is derived, and this is applied to the calculation of the first-order correction to a Fokker-Planck friction constant and to first and second-order corrections to a momentum autocorrelation function.
|Item Type:||Thesis (Dissertation (Ph.D.))|
|Degree Grantor:||California Institute of Technology|
|Division:||Chemistry and Chemical Engineering|
|Thesis Availability:||Public (worldwide access)|
|Defense Date:||1 January 1963|
|Default Usage Policy:||No commercial reproduction, distribution, display or performance rights in this work are provided.|
|Deposited By:||Benjamin Perez|
|Deposited On:||02 May 2012 14:37|
|Last Modified:||26 Dec 2012 04:42|
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