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Europhysics Letters (EPL)

Resonance absorption and fluorescence of a bi-chromatic electromagnetic field by the molecule coupled to a quantum molecular aggregate

Andrei A. Zvyagin, Iryna Yu. Ropakova

Published Feb 1, 2017• 1 citation
Publisher

Abstract

The resonance absorption and fluorescence of a bi-chromatic electromagnetic field by a single molecule, coupled to a one-dimensional quantum molecular aggregate is studied. Depending on the values of the coupling of the single molecule and its own frequency, with respect to the own frequency of the aggregated molecules, and the strength of the aggregation, the absorption and the fluorescence of the molecule show the contribution from the exciton band, or/and the ones from the local level(s) caused by the single molecule. The linear polarized component of the electromagnetic field produces additional resonances, compared to the only circular polarized component, due to the coherent interference. The strength of the absorption and the fluorescence, caused by those additional resonances, depends on the ratio of the magnitude and the frequency of the linear polarized component. For additional resonances the magnitude of the absorption and the frequency is the decaying oscillating function of the mentioned ratio. Copyright (C) EPLA, 2017

DOI
10.1209/0295-5075/117/47005

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The resonance absorption and fluorescence of a bi-chromatic electromagnetic field by a single molecule, coupled to a one-dimensional quantum molecular aggregate is studied. Depending on the values of the coupling of the single molecule and its own frequency, with respect to the own frequency of the aggregated molecules, and the strength of the aggregation, the absorption and the fluorescence of the molecule show the contribution from the exciton band, or/and the ones from the local level(s) caused by the single molecule. The linear polarized component of the electromagnetic field produces additional resonances, compared to the only circular polarized component, due to the coherent interference. The strength of the absorption and the fluorescence, caused by those additional resonances, depends on the ratio of the magnitude and the frequency of the linear polarized component. For additional resonances the magnitude of the absorption and the frequency is the decaying oscillating function of the mentioned ratio. Copyright (C) EPLA, 2017
The linear response of the molecular aggregate chain with the random distribution of the strength of the neighboring intermolecular interactions to the bichromatic electromagnetic field has been calculated. The presence of the linearly polarized field produces additional resonance absorption at the combined frequencies of the circularly polarized and linear polarized field. The strength of the absorption oscillates with the amplitude and the frequency of the linearly polarized electromagnetic field. Additional resonance absorption is weaker than the main absorption at the frequency of the circularly polarized field. Similar behavior has been predicted for the interaction of the bichromatic magnetic field with the quantum spin-1/2 chain with the random distribution of the exchange constants for nearest neighbor spins.
Abstract Electromagnetically induced transparency (EIT) plays an essential role in quantum communication and photon storage. Investigating the EIT phenomenon in molecular aggregates is of significant importance for understanding the coherence properties and nonlinear behaviors of the systems. In this paper, we consider molecular aggregates composed of identical molecules, including single and double molecular chains, and investigate their dynamics under the combined excitation of probe and control light fields. Using the truncated sets of differential equations derived from the quantum Master equation, populations of the excited band and their properties are obtained. The results show that EIT occurs when the frequency of the control light field is near-resonant with the transition frequency between the first excited state and a higher excited state of the individual molecules. EIT is more likely to appear under weak coupling conditions, while a stronger field intensity leads to the appearance of the Autler–Townes phenomenon. The clear EIT window can take place for some specific orientations of the molecular dipole moments. A transition between electromagnetically induced absorption and EIT is found in a double chain configuration. Our study provides a platform for understanding the EIT mechanism in molecular systems and offers theoretical guidance for the design of molecular-based quantum devices.
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.
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.
The theory of the coherent pairing of excitons in the presence of a resonant electromagnetic field is generalized to describe the biexciton spectra of molecular crystals, which contain several molecules (atoms) in the unit cell. The excitation spectrum for crystals like anthracene having two molecules per unit cell is discussed in detail. It is found that, at high exciton densities and under resonance of near-resonance conditions and at temperatures below some value T c , the formation of four biexciton states is feasible provided that the dielectric gaps induced by the electromagnetic field are less than those of the corresponding biexciton states. Expressions for the absorption coefficient describing optical transitions to the biexciton states are derived.
We analyze the fluorescence and absorption spectra of a two-level atom driven by a bichromatic field with frequencies ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$, separated by ${\mathrm{\ensuremath{\omega}}}_{2}$-${\mathrm{\ensuremath{\omega}}}_{1}$=2\ensuremath{\delta}, and Rabi frequencies (at resonance) 2${\mathrm{\ensuremath{\Omega}}}_{1}$ and 2${\mathrm{\ensuremath{\Omega}}}_{2}$ such that their ratio \ensuremath{\alpha}=${\mathrm{\ensuremath{\Omega}}}_{2}$/${\mathrm{\ensuremath{\Omega}}}_{1}$1. We focus on the case of ${\mathrm{\ensuremath{\omega}}}_{1}$ close to the atomic frequency ${\mathrm{\ensuremath{\omega}}}_{0}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$ near the Rabi sideband frequency ${\mathrm{\ensuremath{\omega}}}_{1}$+2${\mathrm{\ensuremath{\Omega}}}_{1}$; the detunings are denoted by ${\mathrm{\ensuremath{\Delta}}}_{1}$=${\mathrm{\ensuremath{\omega}}}_{0}$-${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\Delta}}}_{2}$=${\mathrm{\ensuremath{\omega}}}_{1}$+2${\mathrm{\ensuremath{\Omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{2}$. We find that the spectra depend critically on the detuning ${\mathrm{\ensuremath{\Delta}}}_{2}$: For large ${\mathrm{\ensuremath{\Delta}}}_{2}$, the fluorescence spectrum consists of the well known Mollow triplet, centered at ${\mathrm{\ensuremath{\omega}}}_{1}$; for smaller (but nonzero) ${\mathrm{\ensuremath{\Delta}}}_{2}$, the spectrum is composed of a triplet at ${\mathrm{\ensuremath{\omega}}}_{1}$ together with doublets near the sideband frequencies ${\mathrm{\ensuremath{\omega}}}_{1}$\ifmmode\pm\else\textpm\fi{}2${\mathrm{\ensuremath{\Omega}}}_{1}$. However, when ${\mathrm{\ensuremath{\Delta}}}_{2}$=0 (and \ensuremath{\alpha}\ensuremath{\ll}1), the spectrum consists of a doublet centered at ${\mathrm{\ensuremath{\omega}}}_{1}$ and triplets at ${\mathrm{\ensuremath{\omega}}}_{1}$\ifmmode\pm\else\textpm\fi{}2${\mathrm{\ensuremath{\Omega}}}_{1}$: there is then no fluorescence at ${\mathrm{\ensuremath{\omega}}}_{1}$. As \ensuremath{\alpha} increases, additional triplet structures appear in the spectrum at frequencies ${\mathrm{\ensuremath{\omega}}}_{1}$\ifmmode\pm\else\textpm\fi{}2n${\mathrm{\ensuremath{\Omega}}}_{1}$ with intensities proportional to ${\mathrm{\ensuremath{\alpha}}}^{2(\mathit{n}\mathrm{\ensuremath{-}}1)}$, n\ensuremath{\gtrsim}1, and a line reappears at ${\mathrm{\ensuremath{\omega}}}_{1}$, with intensity proportional to ${\mathrm{\ensuremath{\alpha}}}^{4}$. The absorption by the system of a weak probe beam is also strongly dependent on the detuning, and the spectrum is composed of emission-dispersion-absorption features located near ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{1}$\ifmmode\pm\else\textpm\fi{}2n${\mathrm{\ensuremath{\Omega}}}_{1}$. An analysis in the dressed-atom picture is presented which explains the physical origin of all these features, in both fluorescence and absorption. \textcopyright{} 1996 The American Physical Society.