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Physical Review A

Modeling and efficient computation of nonlinear radiation trapping in three-level atomic vapors

A. F. Molisch, Walter Schupita, B. P. Oehry, Brigitte Sumetsberger, Gottfried Magerl

Published May 1, 1995• 13 citations
Publisher

Abstract

In three-level atoms where one level is the ground state and one is a metastable state, even low-intensity resonance radiation can lead to bleaching. This effect causes the radiation trapping to become nonlinear and thus greatly complicates the simulation of such a system. We set up equations to model an optically excited three-level atomic vapor in a two- or three-dimensional cylindrical cell; the model includes the effects of radiation trapping, particle diffusion, and quenching. We then develop a fast and efficient approximate method for the solution of these equations. Results are compared to Monte Carlo simulations; agreement within 15% is achieved.

DOI
10.1103/physreva.51.3576

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We investigate radiation trapping in an atomic vapor which has been excited by a strong short laser pulse. Since the saturation of the vapor by the pulse leads to a decrease in the effective absorption coefficient, the radiation trapping becomes nonlinear. We derive approximate analytical expressions for the excited-state density in the directly excited region, the fluorescence-excited region, and the density averaged over the whole cell. Starting out from fairly simple approximate expressions based on a prescribed distribution of excited atoms, we then develop physically motivated correction factors that drastically improve the accuracy. All these expressions are given for three important cell geometries: the plane-parallel slab, the infinite cylinder, and the sphere. We compare our results to accurate numerical solutions, and find agreement within 5--10%. We then derive the decay time of the emergent radiation, and find that it can be smaller than the natural lifetime of the excited atoms, in agreement with recent experimental results obtained for sodium vapors.
We present experiments of a laser with variable pulse energy and beam width saturating sodium vapor near the D1{D}_{1}D1​-line transition. At high optical depth and in a buffer gas atmosphere of argon, the effect of nonlinear radiation trapping is shown to drastically change the spatial distribution and temporal evolution of the excited-state population and of the fluorescence light trapped by the nonlinear medium. Besides observing the transient behavior of the fluorescence light, a pump-probe beam experiment enables us to gain a tomographic view inside the atomic vapor. Nitrogen as a buffer gas is used to compare with the situation where radiation trapping effects are negligible. Finally, numerical simulations based upon equations of radiative transfer for a two-level atomic system elucidate the role of nonlinear radiation trapping and support given interpretations of the experiments.
We solve the Holstein equation describing radiation trapping in an atomic vapor by the geometric quantization technique. The treatment is based on studying the integral trapping equation as a wave equation for an associated quasiparticle with a complicated form of its dispersion law. The latter is determined by the spectral properties of the vapor medium. Extending our previous work, which dealt with one-dimensional (1D) geometries, we consider here more realistic two- and three-dimensional (2D and 3D) vapor cell geometries. For this, an explicit representation of the phase factors is derived when the quasiparticle is reflected under arbitrary angles from the surface of the cell confining the vapor. We give closed-form equations to obtain analytically the complete 3D spectrum of escape factors in finite cylinder, sphere, parallelepiped, and finite prismlike geometries for all practically occurring line shapes and opacities. In addition, the relevant semiclassical variational method is applied to develop a perturbation theory for the evaluation of escape factors in more complicated geometries that are sometimes adopted in experiments, including infinite (or finite) elliptical cylinders, prolate and oblate ellipsoids. Comparisons with numerical calculations show that results are accurate within 55%5 for the ground modes and even better for higher-order modes.
We compute radiation trapping in a two-level atomic vapour excited by a laser beam, taking into account saturation effects and using a realistic vapour-cell geometry, the finite cylinder. By using an approximation for the angular distribution of the fluorescence radiation, CPU-time requirements are kept low. We then analyse various practical cases and present useful practical rules of thumb when certain simplifications are valid. When we consider the decay of an initial excitation, the decay at late times can be computed by using an equivalent one-dimensional geometry. For early times, it is usually important to include the three dimensionality of the problem. Finally, we present calculations how the `burn-through' effect of a strong laser affects the approximation of the geometry.
Effects of radiation transport in the interaction of a laser beam with sodium vapor in an argon atmosphere are reported. Investigations of the temporal and spatial evolution of ground-state orientation, which is produced by optical pumping with a circularly polarized near-resonant laser beam, reveal a strong deviation from the expected pure diffusive behavior. Transverse profiles are narrowed considerably with increasing sodium density as well as with increasing pump intensity. The temporal decay of orientation is also drastically altered. A simplified nonlinear and nonlocal theoretical model of radiation trapping gives excellent qualitative agreement with the observations and allows an intuitive interpretation.
A time-dependent theory for conical emission during near-resonant propagation of laser light in an atomic vapor, which includes full propagation for the laser and frequency sidebands in a nonlinear two-level medium is presented. The density-matrix equations for the dipole moment and population are solved in the dressed atomic frame. The polarization source terms are accurate to order \ensuremath{\gamma}/R, where \ensuremath{\gamma} is a damping constant and R is the generalized Rabi frequency. Analytical plane-wave solutions and numerical, cylindrically symmetric propagation simulations including diffraction are presented. It is shown that the calculations with cylindrically symmetric fields and atomic excitation profiles are incapable of accounting for the high levels of optical gain that are responsible for the intense conical emission observed in experiments. This result is at first surprising, since the model accounts rigorously for all of the physical phenomena that have been previously proposed as being responsible for generating large gains, and the calculation matches the symmetry of the observations. The lack of large calculated gain seems to imply the existence of higher-order (m>0)(m>0)(m>0) radial modes in the field for the experimental conditions that give rise to cone emission. In the simulations, however, the cylindrically symmetric fields do produce weak red-detuned cones with angular-frequency distributions similar to those seen in experiments.