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Theory of resonantly enhanced multiphoton processes in molecules

Dixit, S. N. and McKoy, V. (1985) Theory of resonantly enhanced multiphoton processes in molecules. Journal of Chemical Physics, 82 (8). pp. 3546-3553. ISSN 0021-9606. http://resolver.caltech.edu/CaltechAUTHORS:20120628-111541172

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Abstract

In this paper we formulate a theory for the analysis of resonant enhanced multiphoton ionization processes in molecules. Our approach consists of viewing the (n+m) photon ionization process from an isotropic initial state as m‐photon ionization out of an oriented, excited state. The orientation in this resonant state, which is reached by n‐photon excitation from the initial state, is nonisotropic, and is characteristic of this absorption process. The ionization simply probes this anisotropic population. The calculation of the REMPI process thus consists of determining the anisotropy created in the resonant state and then coupling this anisotropic population to ionization out of it. While the former is accomplished by the solution of appropriate density matrix equations, the latter is done by coupling these density matrix elements to angle‐resolved ionization rates out of this state. An attractive feature of this approach is that the influence of saturation effects, and other interactions, such as collisions, on the photoelectron properties is easily understood and incorporated. General expressions are derived for photoelectron angular distributions. Based on these, several properties of the angular distributions that follow purely on symmetry considerations are discussed. One of the new features that emerge out of this work is the saturation induced anisotropy in REMPI. In this effect higher order contributions to the angular distributions appear since saturation influences different ionization channels differently thereby creating an additional anisotropy in the excited state.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1063/1.448934DOIUNSPECIFIED
http://jcp.aip.org/resource/1/jcpsa6/v82/i8/p3546_s1PublisherUNSPECIFIED
Additional Information:© 1985 American Institute of Physics. Received 16 August 1984; accepted 5 October 1984. One of us (S.N.D.) acknowledges useful discussions with Peter Lambropoulos. This material is based upon research supported by the National Science Foundation under Grant No. CHE-8218166.
Funders:
Funding AgencyGrant Number
NSFCHE-8218166
Subject Keywords:MULTI−PHOTON PROCESSES, PHOTOIONIZATION, ANGULAR DISTRIBUTION, POLYATOMIC MOLECULES, NONLINEAR OPTICS
Classification Code:PACS: 33.80.Rv
Record Number:CaltechAUTHORS:20120628-111541172
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20120628-111541172
Official Citation: Theory of resonantly enhanced multiphoton processes in molecules S. N. Dixit and V. McKoy J. Chem. Phys. 82, 3546 (1985); http://dx.doi.org/10.1063/1.448934
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:32171
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:28 Jun 2012 18:26
Last Modified:26 Dec 2012 15:25

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