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Journal of Experimental and Theoretical Physics

Self-localization of excitons and nonlinear optical properties of J-aggregates in a periodically modulated thin film

Alexander A. Zabolotskii

Published Feb 1, 2008• 8 citations
Publisher

Abstract

Nonlinear optical properties of dye J-aggregates embedded in a one-dimensional periodic medium are analyzed theoretically and numerically. The effect of strain-induced exciton self-localization in a chain of monomers on nonlinear optical properties of the system is investigated for weakly and highly ordered J-aggregates. It is found that exciton self-localization in a periodic medium enhances light absorption and effective optical susceptibility. Optical bistability thresholds are examined for weakly and strongly excited dye J-aggregate thin films. It is shown that the threshold intensity of incident electromagnetic field is lower by more than an order of magnitude as compared to that for a homogeneous medium.

DOI
10.1134/s1063776108020192

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Nonlinear optical properties of dye J-aggregates embedded in a one-dimensional periodic medium are analyzed theoretically and numerically. The effect of strain-induced exciton self-localization in a chain of monomers on nonlinear optical properties of the system is investigated for weakly and highly ordered J-aggregates. It is found that exciton self-localization in a periodic medium enhances light absorption and effective optical susceptibility. Optical bistability thresholds are examined for weakly and strongly excited dye J-aggregate thin films. It is shown that the threshold intensity of incident electromagnetic field is lower by more than an order of magnitude as compared to that for a homogeneous medium.
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.
The resonance interaction of a three-component electromagnetic field with a planar polymer film containing J aggregates of dyes is studied. The field consists of two counterpropagating waves traveling along the J aggregate film and a wave directed along a normal to the plane of the film. It is shown that, compared to the case of a one-component field, the polariton-phonon interaction in such a system leads to qualitatively different conditions of the occurrence of localized exciton states and bistability.
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.
A numerical study of reflectivity and transmittivity of an ensemble of short oriented linear Frenkel chains, which forms a thin film with a thickness of the order of an optical wavelength, is carried out. The eigenstates of a single chain are considered to be of a collective (excitonic) origin. A distribution of chains over lengths resulting in inhomogeneous broadening of the exciton optical transition is taken into account. We report a bistable behavior of both reflectivity and transmittivity of the film in a spectral domain close to the exciton resonance, caused by saturation of the nonlinear refraction index. Estimates of driving parameters show that thin films of oriented J-aggregates of polymethine dyes deposited on a dielectric substrate seem to be a suitable object for observation of the predicted behavior.
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.
Exciton self-trapping in a molecular medium is considered within a self-consistent model taking into account the change in the dipole moment as a result of a displacement of molecules and the resonance interaction with an electromagnetic field. New mechanisms and specific features of the formation of localized structures in quasi-one-dimensional molecular structures are investigated. It is shown that the dependence of the dipole moment on molecular vibrations leads to new conditions for exciton self-trapping and intrinsic optical bistability, as well as for the formation of electromagnetically induced transparency. The theory proposed is used to explain the specific features of exciton self-trapping in a conjugated polymer and J aggregates of dyes under the action of an external laser field.