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Optics and Spectroscopy

Polarization of Luminescence in a System of Particles with Three Energy Levels as a Function of the Exciting Light Intensity

Boris I Stepanov, Viktor P. Gribkovskii

Published Feb 1, 1960• 2 citations
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We examine the optical pumping effect in an ensemble of three-level atoms with a Λ configuration of the energy sublevels excited by parametric luminescence light in the squeezed state. We derive quantum kinetic equations that describe the evolution of the density matrix of atoms irradiated by low-intensity squeezed light with a finite-width spectrum. In particular, we show that because of the quantum statistical properties of the squeezed light there can be a redistribution of atoms among the lower energy sublevels, despite the equality of the intensities of the spectral components of the light that resonantly excites optical transitions in the Λ-system. The relation of the optical pumping effect to the correlation and spatial-temporal spectral properties of squeezed light is discussed in detail. Finally, we show that the effects are closely linked to the finiteness of the width of the squeezed-light spectrum.
Various characteristics of frequency-integrated intensities of secondary radiation components near the resonance excitation region have been calculated for a three-level system coupled with a reservoir using a stochastic model. It has been found that the spectral and temporal characteristics of the resonant second-order optical processes can be understood consistently by considering that Raman scattering results from the average value of the induced-dipole moment with respect to the energy fluctuation due to the system-reservoir interaction, while luminescence results from its deviation from the average value. A simple method to determine parameter values that characterize the excited-state dynamics in condensed phases from the secondary radiation data is also discussed.
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.