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Physical Review A

Effects of higher exciton manifolds and exciton-exciton annihilation on optical bistable response of an ultrathin glassy film comprised of oriented linear Frenkel chains

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

Published Feb 26, 2002• 13 citations
Publisher

Abstract

We theoretically analyze the optical response from an ultrathin film built up of oriented molecular aggregates, the operating states of which are represented by Frenkel exciton states. A four-level model, involving transitions between the ground, one-exciton and two-exciton states, exciton-exciton annihilation from the two-exciton state as well as relaxation from the annihilation level back to the one-exciton and ground states, is used for describing the film optical response. It is proved that the exciton-exciton annihilation may act not as a destructive but, on the contrary, as a constructive factor tending towards the occurrence of bistability. In particular, the effect of inhomogeneous broadening of the exciton optical transition, preventing the bistable behavior, may be suppressed considerably due to a fast exciton-exciton annihilation.

DOI
10.1103/physreva.65.033821

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arXiv:physics/0104011•The Journal of Chemical Physics•Sep 1, 2001•6 citations
We theoretically analyze the optical response from an ultrathin film built up of oriented molecular aggregates, the operating states of which are represented by Frenkel exciton states. A four-level model, involving transitions between the ground, one-exciton and two-exciton states, exciton-exciton annihilation from the two-exciton state as well as relaxation from the annihilation level back to the one-exciton and ground states, is used for describing the film optical response. It is proved that the exciton-exciton annihilation may act not as a destructive but, on the contrary, as a constructive factor tending towards the occurrence of bistability. In particular, the effect of inhomogeneous broadening of the exciton optical transition, preventing the bistable behavior, may be suppressed considerably due to a fast exciton-exciton annihilation.
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 an ultrathin 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 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 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.
We theoretically analyze the optical response of an ultrathin film with accounting for the effects of creating two exciton states as well as their annihilation in an individual aggregate. We show that these two processes do not violate mirrorless optical bistability of the film found in the framework of the ground-to-one exciton state transitions but, contrary to that, act towards improving the conditions for bistability to occur. In particular, the killing action of inhomogeneous broadening of the one-exciton absorption spectrum may be considerably reduced due to the exciton–exciton annihilation process giving hope for creating a unit for an all-optical device based on such systems.
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.
We perform a theoretical study of the nonlinear optical response of an ultrathin film consisting of oriented linear aggregates. A single aggregate is described by a Frenkel exciton Hamiltonian with uncorrelated on-site disorder. The exciton wave functions and energies are found exactly by numerically diagonalizing the Hamiltonian. The principal restriction we impose is that only the optical transitions between the ground state and optically dominant states of the one-exciton manifold are considered, whereas transitions to other states, including those of higher exciton manifolds, are neglected. The optical dynamics of the system is treated within the framework of truncated optical Maxwell-Bloch equations, in which the electric polarization is calculated by using a joint distribution of the transition frequency and the transition dipole moment of the optically dominant states. This function contains all the statistical information about these two quantities that govern the optical response and is obtained numerically by sampling many disorder realizations. We derive a steady-state equation that establishes a relationship between the output and input intensities of the electric field and show that within a certain range of the parameter space this equation exhibits a three-valued solution for the output field. A time-domain analysis is employed to investigate the stability of different branches of the three-valued solutions and to get insight into switching times. We discuss the possibility to experimentally verify the bistable behavior.
A theoretical study of the resonance optical response of assemblies of oriented short (as compared to an optical wavelength) linear Frenkel chains is carried out. Despite the fact that the energy spectrum of a single chain is composed of the bands of Frenkel exciton states, a two-level model is used to describe the optical response of a single linear chain. We account for only the (on-resonance) optical transition between the ground state and the state of the one-exciton band bottom as having the dominating oscillator strength as compared to the other states of the one-exciton manifold. The (off-resonance) process of creation of two excitons per chain is neglected because it requires a higher excitation frequency due to the quasi-fermionic nature of one-dimensional Frenkel excitons. A distribution of linear chains over length resulting in fluctuations of all exciton optical parameters, such as the transition frequency and dipole moment as well as the radiative rate, are taken explicitly into account. We show that both transmittivity and reflectivity of the film may behave in a bistable fashion, originating from saturation of the nonlinear refraction index, and analyze how the effects found depend on the film thickness and on the inhomogeneous width of the exciton optical transition. Estimates of the driving parameters show that films of oriented J-aggregates of polymethine dyes at low temperatures seem to be suitable species for the experimental verification of the behavior found.