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The Journal of Chemical Physics

Mirrorless optical bistability of an ultrathin glassy film built up of oriented J-aggregates: Effects of two-exciton states and exciton–exciton annihilation

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

Published Feb 1, 2001• 16 citations
Publisher

Abstract

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.

DOI
10.1063/1.1344232

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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.
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.
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 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 theoretical study of transmittivity of an ultrathin film (of thickness smaller than an optical wavelength) consisting of oriented linear aggregates is carried out. We show that within a certain domain of the incident field amplitude, optical transitions of a single disordered aggregate, the eigenstates of which are represented by the Frenkel exciton states, can be treated in the framework of a two-level approximation. This allows us to claim that an ensemble of linear aggregates is analogous to that comprised of inhomogeneously broadened two-level systems. Based on this analogy, we show that the transmittivity of the film can manifest a bistable behavior originating from the coupling of the aggregates via the emission (far-zone) field. This mechanism of bistability differs from that occurring in a single perfect aggregate. In the latter case, bistability results from the population-dependent resonance frequency shift of an individual aggregate, originating from the coupling of the molecules via the dipole–dipole (near-zone) field. Estimates of the driving parameters show that real candidates, to realize the type of behavior we found, are such well-studied objects as J-aggregates of polymethine dyes or thin films of thiophene oligomers.
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.