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Advanced Materials for Optics and Electronics

Mirrorless optical bistability in molecular aggregates with dipole–dipole interaction

V. V. Gusev

Published Oct 1, 1992• 15 citations
Publisher

Abstract

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.

DOI
10.1002/amo.860010505

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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.
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.
This paper considers a thin plane nanosystem consisting of molecular chains of dye J-aggregates forming bundles elongated in one direction and spherical gold nanoparticles located near them. Expressions are derived for the polarization of the exciton transition in the external field under the mutual influence of the dipole fields of the monomers constituting the dye J-aggregates and for the induced dipole of the nanoparticle. It is shown that in this system, mirrorless optical bistability of the fluorescence spectral density of the dye J-aggregates is possible, depending on the pump field intensity. The parameters of this dependence are critically determined by the distance between the molecular bundles and nanoparticles and by the angle between the field polarization direction and the axis of the bundle of J-aggregates. The use of the nanosystem as a sensor is discussed.
Electromagnetically induced transparency (EIT), which is known as an efficient control method of optical absorption property, is investigated using the polarizability spectra and population dynamics obtained by solving the quantum Liouville equation. In order to clarify the intermolecular interaction effect on EIT, we examine several molecular aggregate models composed of three-state monomers with the dipole-dipole coupling. On the basis of the present results, we discuss the applicability of EIT in molecular aggregate systems to a new type of optical switch.
Summary form only given. We provide a theoretical study of transmittivity of an ultrathin layer (of thickness smaller than an optical wavelength) consisting of oriented organic molecular aggregates (J-aggregates). In spite of the fact that those are complicated systems the excited states of which have the character of Frenkel excitons, an analysis of spectroscopic data of J-aggregates shows, that in a definite area of intensity of the incoming field such films can be modeled as an ensemble of inhomogeneously broadened two-level-systems. An appropriate renormalization of the spontaneous emission rate ensures, that mainly the fewest excitonic state couples to the radiation field. Because of a quite high concentration necessary for the aggregation process itself, in such systems a mechanism of optical bistability, that is due to coupling of the single aggregates via the far-zone field is shown to be possible.
A theory of resonant interaction with radiation of J aggregates based on chains of two-level molecules coupled by the retarded dipole‒dipole interaction has been developed. The effect of pair correlations between the chain molecules on the bistable response of this system under the influence of external resonant radiation has been investigated within the homogeneous chain model. Traditionally, these systems have been described using single-particle density matrices corresponding to each molecule. In this description, twoparticle interactions are represented in the factorized form and do not include correlations between the interacting molecules. In this study, the correlation corrections have been estimated taking into account the influence of only the nearest neighbors, while their values have found to be of the same order of magnitude as the factorized two-particle expectation values for which these corrections have been calculated. As a result, the dipole‒dipole interaction of a particular molecule with the nearest neighbors is so strong that the description of this interaction in the factorized form becomes inappropriate and can be used only for a qualitative analysis of the response of the chain. In order to obtain correct quantitative characteristics, it is necessary to abandon the factorization of the two-particle expectation values, at least for nearest neighbors.
Within the framework of a developed model of a medium consisting of molecular J aggregates and placed in an external resonant light field, it is shown how exciton self-localization and the dependence of the dipole moment components on molecule deformation affect optical bistability. Deformation of the molecules substantially facilitates the observation of a bistable dependence of the state of the medium and of the transmitted field amplitude on the incident field amplitude. The evolution of the system to a quasi-stationary, nonground state after the passage of an electromagnetic field pulse under the conditions of self-localization of excitons is studied.