Cooperative effects in photon statistics of molecular dimers with spectral diffusion.
The two-point fluorescence intensity correlation function g(2)t and the Mandel parameter Mt are calculated for a strongly pumped dimer of two-level molecules undergoing Gaussian-Markovian frequency fluctuations. The effects of detuning and saturation are examined. All fluctuation time scale regimes are explored using a continued fraction solution of the stochastic Liouville equation for the generating function. Bunching and antibunching are observed for slow and fast fluctuations, respectively. The short-time antibunching dip in g(2) and its variation with intermolecular coupling, the exciton annihilation rate, and laser detuning are studied.
Sanda
Frantisek
F
Department of Chemistry, University of California, Irvine, California 92697-2025, USA.
Mukamel
Shaul
S