Fifth-order nonlinear Raman processes using broadband, incoherent light are treated for a multiply resonant, multicomponent mixture. In particular, the theoretical development of the direct and the sequential fifth-order analogs of coherent Raman scattering is presented. Of the complete formalism, only the dominant doubly Raman resonant hyperpolarizability contributions to the signal intensity are discussed in this article. Furthermore, application is made to simulate fifth-order signals from a variety of hypothetical molecular liquids. It is seen how the direct and the sequential processes can distinguish themselves in a mixture, in a neat liquid with more than one Raman coherence, and also whenever the Raman active modes are taken to be anharmonic. This theoretical treatment anticipates experimental results presented in the following paper.
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1 July 1999
Research Article|
July 01 1999
Fifth-order nonlinear Raman processes in molecular liquids using quasi-cw noisy light. I. Theory
Jason C. Kirkwood;
Jason C. Kirkwood
Department of Chemistry, Baker Laboratory, Cornell University, Ithaca, New York 14853
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A. C. Albrecht;
A. C. Albrecht
Department of Chemistry, Baker Laboratory, Cornell University, Ithaca, New York 14853
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Darin J. Ulness
Darin J. Ulness
Department of Chemistry, Concordia College, Moorhead, Minnesota 56562
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J. Chem. Phys. 111, 253–271 (1999)
Article history
Received:
August 12 1998
Accepted:
April 06 1999
Connected Content
A companion article has been published:
Fifth-order nonlinear Raman processes in molecular liquids using quasi-cw noisy light. II. Experiment
Citation
Jason C. Kirkwood, A. C. Albrecht, Darin J. Ulness; Fifth-order nonlinear Raman processes in molecular liquids using quasi-cw noisy light. I. Theory. J. Chem. Phys. 1 July 1999; 111 (1): 253–271. https://doi.org/10.1063/1.479287
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Fifth-order nonlinear Raman processes in molecular liquids using quasi-cw noisy light. II. Experiment
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