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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Optical bistable response of a linear molecular aggregate

Viktor A. Malyshev, Pablo Moreno

Published Feb 5, 1996• 0 citations
Publisher

Abstract

Optical bistable response of a molecular aggregate modeled as a linear chain of two-level molecules is shown. We have found that bistability may exist but bistable response is strongly affected by spatial inhomogeneity of the aggregate population.
DOI
10.1117/12.231023

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The bistable response of linear molecular aggregates modeled as linear chains of two-level systems is shown. We carry out analytical and numerical calculations of the aggregate population by means of the system of coupled nonlinear equations for the density matrices of individual molecules. Our conclusion is that bistable behavior of the population results from the dependence of resonance frequency of the aggregate on the number of excited molecules. \textcopyright{} 1996 The American Physical Society.
A four-level model, involving the ground, one-exciton and two-exciton states as well as a high-lying molecular term through which the two-exciton state annihilates, is used for analyzing the bistable optical response of a thin film built up of oriented molecular aggregates. We focus on the effects of inhomogeneous broadening of the exciton optical transitions and exciton-exciton annihilation on bistability of the thin film response. It turns out that the inhomogeneous broadening, preventing generally the occurrence of bistability, may be suppressed considerably due to a fast exciton-exciton annihilation.
A numerical study of the optical bistable response of an open linear Frenkel chain of three-level molecules is carried out, making use of the one-molecule density-matrix approach. We analyze the joint effect of the presence of boundaries and of the exciton-exciton annihilation on the bistable behavior of a chain. The former is going to destroy such behavior due to the spatial inhomogeneity of the population growing with time. The latter resists a preferable creation of the population at a certain segment of the chain stabilizing the system and, thus, provides the conditions for bistability to be realized.
The problem is examined whether a bistable behavior of optical response of a dimer really exists. We carry out an exact treatment of this problem based on the two-molecule density matrix, without its representation in the form of a product of the one-molecule density matrices of each molecule composing the dimer. Our conclusion is that the bistability discussed is an artifact originating from the splitting procedure. A condition for getting the bistable optical response from a linear chain of a large number of monomers is also formulated.
We generalize our recent work on the optical bistability of thin films of molecular aggregates [J. A. Klugkist et al., J. Chem. Phys. 127, 164705 (2007)] by accounting for the optical transitions from the one-exciton manifold to the two-exciton manifold as well as the exciton-exciton annihilation of the two-exciton states via a high-lying molecular vibronic term. We also include the relaxation from the vibronic level back to both the one-exciton manifold and the ground state. By selecting the dominant optical transitions between the ground state, the one-exciton manifold, and the two-exciton manifold, we reduce the problem to four levels, enabling us to describe the nonlinear optical response of the film. The one- and two-exciton states are obtained by diagonalizing a Frenkel Hamiltonian with an uncorrelated on-site (diagonal) disorder. The optical dynamics is described by means of the density matrix equations coupled to the electromagnetic field in the film. We show that the one- to two-exciton transitions followed by a fast exciton-exciton annihilation promote the occurrence of bistability and reduce the switching intensity. We provide estimates of pertinent parameters for actual materials and conclude that the effect can be realized.