Generalized Stokes-Mueller formalism for two-photon absorption, frequency doubling, and hyper-Raman scattering

Yaoming Shi, W. M. McClain, and R. A. Harris
Phys. Rev. A 49, 1999 – Published 1 March 1994
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Abstract

We consider processes quadratic in incident intensity, in which two identical photons are annihilated simultaneously. We construct a formalism for these processes that is maximally analogous to the Stokes-Mueller formalism for linear processes. The two-photon properties of the incident beam require nine Stokes-like parameters for their description; the Mueller-like matrix which gives a complete description of frequency doubling or hyper-Raman scattering is of size 4×9. Of the 36 independent observable matrix elements, 12 are activated by pure real elastic dipole susceptibilities, four by an imaginary component in the electric dipole susceptibility (absorption), nine by handedness alone, two by extramultipole mechanisms alone, and nine require both handedness and extramultipole mechanisms.

  • Received 2 August 1993

DOI:https://doi.org/10.1103/PhysRevA.49.1999

©1994 American Physical Society

Authors & Affiliations

Yaoming Shi and W. M. McClain

  • Department of Chemistry, Wayne State University, Detroit, Michigan 48202

R. A. Harris

  • Department of Chemistry, University of California at Berkeley, Berkeley, California 94720

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Vol. 49, Iss. 3 — March 1994

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