Analysis of bistability in molecular J aggregates under their resonant optical excitation taking into account multiparticle effects

作者：Nesterov L A^*; Fedorov S V; Rosanov N N; Levinsky B N; Fainberg B D

来源：Optics and Spectroscopy, 2013, 115(4): 499-507.

DOI：10.1134/S0030400X13100135

Using a model of a homogeneous chain of molecules, we have analyzed bistability in resonantly excited J aggregates taking into account three-particle contributions to the exciton-exciton annihilation. These contributions, which have an interference nature, have previously been calculated in a work by B.N. Levinsky, L.A. Nesterov, B.D. Fainberg, and N.N. Rosanov (Opt. Spectrosc. 115 (3), 406 (2013)) in the course of derivation of equations of motion for J aggregates from first principles. Factorization of expectation values that correspond to these contributions leads to a closed system of equations in which not only pair, but also triple, interactions between molecules of the chain are taken into account. Numerical calculations have been performed, and their results have been compared with those obtained in calculations without taking into account three-particle contributions. We have shown that, on the whole, the inclusion of three-particle interference contributions in equations of motion leads to a restriction of the domain of existence of hysteresis. This, in turn, makes it possible to more reliably single out a real range of parameters in which nonlinear optical effects can considerably manifest themselves.

• 出版日期2013-10