Fluorescence interference noise in a two-site system: Excitation transfer dynamics from intensity fluctuations

Abstract

The optical response of a two-site system driven by a pair of optical pulses in an interferometric set up has been studied theoretically by applying the density operator formalism. The one-exciton approach is taken for modeling two coupled two-level systems (TLS), the external field is presented semiclassically and bath-induced dissipative processes are included. In the δ-pulse limit the population of the excited state has been formulated to the lowest order perturbation expansion in the external field. In the limit of slow luminescence the interferogram of time-integrated total fluorescence has been calculated for pulses with constant relative phase. For phase-randomized pulses the variance of the correlated fluorescence signal as a function of the pulse delay allows direct interrogation of coherent transients and dephasing processes. Our analysis follows the principle of coherence observation by interference noise, COIN [O. Kinrot, I. Sh. Averbukh, and Y. Prior, Phys. Rev. Lett. 75, 3822 (1995)], but is a generalization of this concept to expand on electronically interacting TLS. The theoretical results demonstrate that analysis of fluorescence interference fluctuations may provide a powerful diagnostic tool for probing the initial quantum coherence of energy transfer, i.e., excitation oscillations by employing fs-fluorescence correlation measurements in stable interferometric configurations.