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arXiv:1012.3139 · Optics and Spectroscopy

Simulation of interaction of oriented J aggregates with resonance laser radiation

N. V. Vysotina, Victor A Malyshev, Vladimir G. Maslov, Leonid A. Nesterov, Nikolay N. Rosanov, Sergey V. Fedorov, A. N. Shatsev

Published Jul 1, 2010• 8 citations
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Abstract

The interaction of laser radiation with single J aggregates of cyanine dyes is theoretically analyzed and numerically simulated. The quantum-mechanical calculations of the equilibrium geometry and the energies and intensities of the lowest singlet electronic transitions in pseudoisocyanine chloride and its linear (chain) oligomers are fulfilled. The data of these calculations can serve as parameters of the analyzed model of interaction of J aggregates with radiation in the one-particle density matrix approximation. This model takes into account relaxation processes, the annihilation of excitations at neighboring molecules, and inhomogeneous broadening. Assuming that the inhomogeneous broadening is absent, calculations demonstrate the existence of spatial bistability, molecular switching waves, and dissipative solitons. The effect of the inhomogeneous broadening and the radiation intensity on the effective coherence length in linear (chain) J aggregates is analyzed.

DOI
10.1134/s0030400x10070180

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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)•Nov 11, 2002•0 citations
The interaction of laser radiation with single J aggregates of cyanine dyes is theoretically analyzed and numerically simulated. The quantum-mechanical calculations of the equilibrium geometry and the energies and intensities of the lowest singlet electronic transitions in pseudoisocyanine chloride and its linear (chain) oligomers are fulfilled. The data of these calculations can serve as parameters of the analyzed model of interaction of J aggregates with radiation in the one-particle density matrix approximation. This model takes into account relaxation processes, the annihilation of excitations at neighboring molecules, and inhomogeneous broadening. Assuming that the inhomogeneous broadening is absent, calculations demonstrate the existence of spatial bistability, molecular switching waves, and dissipative solitons. The effect of the inhomogeneous broadening and the radiation intensity on the effective coherence length in linear (chain) J aggregates is analyzed.
Using a model of a homogeneous chain of molecules, we have analyzed bistability in resonantly excited J aggregates taking into account three-particle contributions to the exciton-exciton annihilation. These contributions, which have an interference nature, have previously been calculated in a work by B.N. Levinsky, L.A. Nesterov, B.D. Fainberg, and N.N. Rosanov (Opt. Spectrosc. 115 (3), 406 (2013)) in the course of derivation of equations of motion for J aggregates from first principles. Factorization of expectation values that correspond to these contributions leads to a closed system of equations in which not only pair, but also triple, interactions between molecules of the chain are taken into account. Numerical calculations have been performed, and their results have been compared with those obtained in calculations without taking into account three-particle contributions. We have shown that, on the whole, the inclusion of three-particle interference contributions in equations of motion leads to a restriction of the domain of existence of hysteresis. This, in turn, makes it possible to more reliably single out a real range of parameters in which nonlinear optical effects can considerably manifest themselves.
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.
We have performed a linear analysis of the stability of stationary states of homogeneous resonant excitation regimes of molecular J aggregates with coherent sustaining radiation. In the analysis, we have taken into account not only two-particle but also three-particle interactions of molecules, which are related to the exciton-exciton annihilation mechanism. Our detailed investigation of the stability of stationary states has allowed us to determine stability and instability regions and correlate them with the existence of bistability boundaries.
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.
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.
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.