Abstract

Prior to the development of self-consistent approximations [1] to the solution of the master equation for electronic excitation transport, no analytic theory existed for dealing with the transport dynamics in both the short (non-diffusive) and long (diffusive) time regimes. The probability G^s(t) that the electronic excitation resides on the initially excited molecule at time t is related to the intensities of the polarized fluorescence components via where τ is the isotropic fluorescence lifetime. The current highest-order approximation (the 3-body approximation) to G^s(t) was tested by Gochanour and Fayer [2] using polarized fluorescence profiles from rhodamine 6G gated by sum frequency-mixing with 1.06 µm laser fundamental pulses; it yielded good visual agreement with the experimental profiles. In analyzing the self-consistent theory, Fedorenko and Burshtein [3] have recently noted that it exhibits incorrect long-time behavior and questioned the theory's validity.

© 1986 Optical Society of America