Effects of spectral cross relaxation and collisional dephasing on the absorption of light by organic-dye solutions

Creators: Vahey, David W.; Yariv, Amnon

Abstract

The nonlinear absorption of intense laser light is used to obtain information about the times required for spectral cross relaxation (T3) and collisional dephasing (T2) in organic-dye solutions. The steady-state transmission experiment of Huff and DeShazer indicates that T2 is in the range 0.1-1 psec for cryptocyanine-methanol, while T3 is in the range 1-10 psec. For DDI-glycerin (1, 1′-diethyl-2, 2′-dicarbocyanine-iodide-glycerin), measurements of ultrashort-pulse transmission as a function of incident energy and optical polarization suggest a value T2=0.4±0.2 psec for that system. These results are based on a new set of rate equations for absorption by inhomogeneously broadened organic-dye solutions. The equations display the effects of spectral cross relaxation and are not limited to light intensities less than those at which coherent interaction effects become important. For the case of ultrashort incident pulses, the equations are extended to account for excited-state absorption, the dependence of absorption on optical polarization, and the existence of a multiplicity of interacting excited states.

Additional Information

©1974 The American Physical Society Received 31 December 1973; revised 22 April 1974 This work, particularly in its experimental aspects, was supported by the U.S. Air Force Office of Scientific Research. Much of the theory and data analysis were made possible through fellowship support by Battelle Memorial, for which one of us (D.V.) is very grateful. That author also wishes to thank Dr. C. W. Kern for his encouragement and interest in this work throughout its final stages.

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