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Journal of Optical Technology

How coherence affects the evolution of the interaction of laser radiation with optically dense molecular media under conditions close to resonance

Г. М. Ермолаева, В. А. Смирнов, В. Б. Шилов

Published Jun 1, 2006• 0 citations
Publisher

Abstract

This paper discusses how the degree of coherence of intense resonance radiation affects the evolution process of collective photoinduced luminescence, which determines the absorption-emission dynamics in concentrated molecular systems. It is shown that the partial breakdown of coherence reduces the radius of the volume in which effective collective interaction occurs in the field-matter system and in which the relative role of classical mechanisms in the absorption-emission cycle increases.

DOI
10.1364/jot.73.000403

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This paper discusses how the degree of coherence of intense resonance radiation affects the evolution process of collective photoinduced luminescence, which determines the absorption-emission dynamics in concentrated molecular systems. It is shown that the partial breakdown of coherence reduces the radius of the volume in which effective collective interaction occurs in the field-matter system and in which the relative role of classical mechanisms in the absorption-emission cycle increases.
A new theoretical model describing the emission and absorption dynamics in an ensemble of molecules under intense coherent pulsed pumping is developed on the basis of the concepts of cooperative light-induced luminescence (CLIL). The CLIL development is described within the framework of formalism of the system density matrix in the space of photon wave functions. It is shown that the fast growth of CLIL relates to the development of coherent states of the quantum field in the area of efficient cooperative interactions of molecules (coherence volume). A system of equations for the calculation of CLIL energy, population of excited states, and optical absorption of the system in dependence on the laser pump energy density is solved. The theoretical results obtained are in good agreement with the experimental data.
We model the response of a molecular medium to an intense pulse of light. We begin by reducing the Maxwell-Bloch equations for a multilevel molecular model system to a set of simplified propagation equations. We thereby obtain expressions for the frequency, temperature, and field intensity dependence of the ground and excited electronic state absorption cross sections, and the emission cross section, as well as the temperature dependence of the decay rate of the excited state. The phenomena of saturation, excited-state absorption, optically induced dichroism and birefringence, vibronic energy transfer, induced molecular alignment, decay of the matter-field interaction energy, and rotational diffusion are considered within the general formalism for describing the propagation of an intense pulse of light in the molecular medium. We find that the cross section for absorption (emission) of a photon is not identical to the cross section for molecular excitation (deexcitation) via the matter-field interaction. This is explained in terms of an energy balance between the matter, radiation, the matter-radiation interaction, and the bath responsible for the broadening of the molecular transitions. The inequality of these cross sections determines whether the system supplies or draws energy from the thermal bath. The rise in the vibrational temperature of molecules subjected to an intense short pulse is shown to significantly affect propagation of the pulse. The alignment of the molecular system resulting from saturation of the ground-state transition by a polarized laser pulse and the effects of the orientational dependence of the matter-field interaction including effects of rotational diffusion are determined. As an example of the formalism we consider pulse propagation in a Rhodamine 6G solution. We fit the parameters of the model to determine the frequency dependence of the ground- and excited-state absorption cross sections and the emission cross section and compare with experimentally determined cross sections. We describe the propagation of a pulse whose temporal width is comparable to the rotational diffusion time of the molecules in the dye solution and calculate polarization pulse probe signals.
The dynamical evolution of an excited-state population in a macroscopic volume of three-level molecules is considered where the population is driven optically between the initial ground state and the excited states by an externally applied (ccc-number) coherent pump. The intermediate and ground states are taken as nonradiatively coupled whereas the excited-to-intermediate-state transition is coupled to the radiation field which is treated quantum mechanically. It is found that stimulated Raman processes can significantly influence the dynamical evolution of population inversion and macroscopic polarization by producing coherence effects among the populations. We examine the evolution of collective relaxation between the excited and intermediate levels in the time regime of the pump pulse duration. It is shown, using the mean-field approximation, that for uniform pumping and conditions such that the pump Rabi rate ${\ensuremath{\omega}}_{R}$, the characteristic collective radiation time ${\ensuremath{\tau}}_{R}$, and the pump pulse duration ${\ensuremath{\tau}}_{P}$ satisfy the inequalities, ${\ensuremath{\omega}}_{R}>\frac{1}{{\ensuremath{\tau}}_{R}}>\ensuremath{\gamma}$ and ${\ensuremath{\tau}}_{P}\ensuremath{\gtrsim}{\ensuremath{\tau}}_{R}$ ($\ensuremath{\gamma}$ is a characteristic internal dephasing rate for the molecules), the system is left in a state with classical transverse polarization when the pump pulse terminates. The system can evolve collectively from such a state only as superradiant (classical) evolution. For superfluorescent evolution which requires a state of preparation of complete inversion (zero transverse polarization), it is shown that the pump pulse must be effectively of area $\ensuremath{\pi}$ and that ${\ensuremath{\tau}}_{P}<{\ensuremath{\tau}}_{R}$. Our results show that when the former conditions are satisfied the delay time ${\ensuremath{\tau}}_{D}$ for collective free pulse evolution is a function of both ${\ensuremath{\tau}}_{P}$ and ${\ensuremath{\tau}}_{R}$. It is shown further that the pump pulse shape as well as temporal duration significantly affect the final state of preparation. The results of this work are interpreted in connection with recent reported results of experiments in superfluorescence and superradiance.
This work is devoted to nonlinear effects in the atomic medium excited by multifrequency laser radiation. We have considered collective light scattering in the optically dense medium in conditions of coherent population trapping. Propagation of intermode correlation coefficient was calculated and it was found that correlation can increase in the medium. Light shifts of the coherent population trapping resonances and ways of their suppression were analyzed. Propagation of radiation in the medium with closed excitation scheme was investigated.
Experimental and theoretical investigation of the coherent propagation and amplification of polychromatic broadband laser pulses in optically dense resonant media without population inversion was carried out for the cases of plasma in a Ne glow discharge and a pulse discharge in Hg-Ar mixture. High density of Ne and Hg atoms in the metastable state (about 1012 cm-3), which was chosen to be the ground state of the two-level system under consideration, leads to the collective behavior of the atomic system in resonant electromagnetic field. The broadband probe field attenuation and the sideband amplification of the probe under the action of the coherent pump were observed. The amplification dependence on the pump intensity was obtained. The model of the parametrically enhanced collective interactions was developed and comparison the experimental data was made.