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Physical Review A

Absence of bistable behavior in the optical response of a dimer

Viktor A. Malyshev, H. Glaeske, K.‐H. Feller

Published Aug 1, 1998• 19 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.58.1496

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Advanced Materials for Optics and Electronics•Oct 1, 1992•15 citations
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.
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 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.
Optical bistability has been observed in highly concentrated fluorescein dye solutions and in thin (-1 pm) doped polymeric films. At concentrations larger than 10-5 mole/k dye dimers are formed. For fluorescein dye, the dimer-monomer equilibrium constant is 10 -5 mole/ℓ so that most of the dye species are in the dimer form. At 480 nm the dimer absorption cross section is 10-18 cm2/molecule, while that for the dye monomer molecule is 7.6 x 10-17 cm2/molecule. Upon laser excitation dimers dissociate to form monomers thus providing a highly nonlinear laser induced absorption. This high nonlinear absorption coefficient can be utilized for optically bistable response of the dye system. Optical bistability was observed by placing dye solutions or dye thin films inside a Fabry-Perot resonator and exciting it with 480 nm dye laser pulses of 10 ns duration. The effect is more pronounced in 10-4 mole/ℓ fluorescein than in 10-6 mole/k fluorescein in which dimer formation is not that efficient.
Abstract The possibility of mirrorless optical bistability in molecular aggregates with dipole–dipole interaction was studied theoretically. Dimers and ordered layers of the Langmuir–Blodgett type or J‐aggregates consisting of identical polyatomic fluorescent molecules were chosen as molecular aggregate models. The investigation was carried out on the basis of the Bogolubov equation chain for the density matrix of molecular aggregates and its components. It is shown that the fluorescence intensity and absorption ability are described by bistable and hysteresislike behaviour when the parameters of the molecular aggregate and pumping radiation are chosen suitably. An analysis of the bistability mechanism in such aggregates is given. Possibilities of controlling one light beam by another and switching polychromatic light flow by using a bistable device based on molecular aggregates are discussed.