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Journal of Luminescence

Dynamical theory for two-photon correlators: spectral line jumps and spectral diffusion

Игорь Сергеевич Осадько, L. B. Yershova

Published Apr 1, 2000• 9 citations
Publisher
DOI
10.1016/s0022-2313(00)00186-1

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Physical Review E•Oct 28, 2009•1 citation
A dynamic theory of two-photon correlators for a single impurity center developed recently by the author [I. S. Osad’ko, Zh. Éksp. Teor. Fiz. 113 , 1606 (1998) [JETP 86 , 875 (1998)] has been generalized to the case in which the center interacts with nonequilibrium two-level systems (TLSs) in polymers and glasses. Quantum tunneling transitions in TLS manifest themselves as random jumps of a spectral line of an impurity center. These jumps can be either spontaneous or light-induced. Interaction between the impurity center and many nonequilibrium TLSs, which exist in polymers, results in a time dependence of the optical dephasing rate 1/ T 2 of an impurity molecule, i.e., in spectral diffusion. This paper describes how the jumps of the spectral line manifest themselves in the two-photon correlator, which can be measured in experiments.
We revisit the line-shape theory of a single molecule with anomalous stochastic spectral diffusion. Waiting time profiles for bath induced spectral jumps in the ground and excited states become different when a molecule, probed by continuous-wave laser field, reaches the steady state. This effect is studied for the stationary dichotomic continuous-time-random-walk spectral diffusion of a single two-level chromophore with power-law distributions of waiting times. Correlated waiting time distributions, line shapes, two-point fluorescence correlation function, and Mandel Q parameter are calculated for arbitrary magnitude of laser field. We extended previous weak field results and examined the breakdown of the central limit theorem in photon statistics, indicated by asymptotic power-law growth of Mandel Q parameter. Frequency profile of the Mandel Q parameter identifies the peaks of spectrum, which are related to anomalous spectral diffusion dynamics.