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The Journal of Chemical Physics

Photonic superdiffusive motion in resonance radiation trapping

Mário Nuno Berberan-Santos, Eduardo J. Nunes-Pereira, José M. G. Martinho

Published Nov 7, 2006• 7 citations
Publisher

Abstract

In this work we consider the relation between the jump length probability density function and the line shape function in resonance radiation trapping in atomic vapors. The two-sided jump length probability density function suitable for a unidimensional formulation of radiative transfer is also derived. As a side result, a procedure to obtain the Maxwell distribution of velocities from the Maxwell-Boltzmann distribution of speeds was obtained. General relations that give the asymptotic jump length behavior and the Levy flight parameter mu for any line shape are obtained. The results are applied to generalized Doppler, generalized Lorentz, and Voigt line shape functions. It is concluded that the lighter the tail of the line shape function, the less heavy the tail of the jump length probability density function, although this tail is always heavy, with mu < or =1.

DOI
10.1063/1.2364889

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In this work we consider the relation between the jump length probability density function and the line shape function in resonance radiation trapping in atomic vapors. The two-sided jump length probability density function suitable for a unidimensional formulation of radiative transfer is also derived. As a side result, a procedure to obtain the Maxwell distribution of velocities from the Maxwell-Boltzmann distribution of speeds was obtained. General relations that give the asymptotic jump length behavior and the Levy flight parameter mu for any line shape are obtained. The results are applied to generalized Doppler, generalized Lorentz, and Voigt line shape functions. It is concluded that the lighter the tail of the line shape function, the less heavy the tail of the jump length probability density function, although this tail is always heavy, with mu < or =1.
Lévy flight superdiffusion consists of random walks characterized by very long jumps that dominate the transport. However, the finite size of real samples introduces truncation of long jumps and modifies the transport properties. We measure typical Levy flight parameters for photon diffusion in atomic vapor characterized by a Voigt absorption profile. We observe the change of Lévy parameter as a function of truncation length. We associate this variation with size-dependent contributions from different spectral regions of the emission profile with the Doppler core dominating the transport for thin samples and Lorentz wings for thick samples. Monte Carlo simulations are implemented to support the interpretation of results.
The propagation of a photon in an atomic medium can be seen as a L\'evy-flight random walk where the probability distribution P(z)P(z)P(z) for the photon step length zzz scales with ${z}^{\ensuremath{-}(\ensuremath{\alpha}+1)}$, with $0<\ensuremath{\alpha}<2$. In atomic vapors, previous work reported the value of $\ensuremath{\alpha}$ obtained from direct measurement of P(z)P(z)P(z) and also from the dependence of transmission on sample opacity, both for Doppler and Lorentz profiles. In this work, we report the measurement of $\ensuremath{\alpha}$ in a Cs cell from the scaling of transmission with starting point, i.e., the average penetration depth of the photon in the medium before the first scattering event. We show that the parameter $\ensuremath{\alpha}$ depends on the size of the system and on the probability that an atom suffers a collision before spontaneous emission. The measured $\ensuremath{\alpha}$ parameter corresponds to the expectation value for P(z=L)P(z=L)P(z=L), with LLL the size of the system, which is consistent with the so-called single-big-jump principle that states that a single jump rules the transport.
Multiple scattering is a process in which a particle is repeatedly deflected by other particles. In an overwhelming majority of cases, the ensuing random walk can successfully be described through Gaussian, or normal, statistics. However, like a (growing) number of other apparently inoffensive systems, diffusion of light in dilute atomic vapours eludes this familiar interpretation, exhibiting a superdiffusive behaviour. As opposed to normal diffusion, whereby the particle executes steps in random directions but with lengths slightly varying around an average value (like a drunkard whose next move is unpredictable but certain to within a few tens of centimetres), superdiffusion is characterised by sudden abnormally long steps (Lévy flights) interrupting sequences of apparently regular jumps which, although very rare, determine the whole dynamics of the system. The formal statistics tools to describe superdiffusion already exist and rely on stable, well understood distributions. As scientists become aware of, and more familiar with, this non-orthodox possibility of interpretation of random phenomena, new systems are discovered or re-interpreted as following Lévy statistics. Propagation of light in resonant atomic vapours is one of these systems which have been studied for decades and have only recently been shown to be the scene of Lévy flights.
The propagation of light in a resonant atomic vapor can a priori be thought of as a multiple scattering process, in which each scattering event redistributes both the direction and the frequency of the photons. Particularly, the frequency redistribution may result in L\'evy flights of photons, directly affecting the transport properties of light in a resonant atomic vapor and turning this propagation into a superdiffusion process. Here, we report on a Monte Carlo simulation developed to study the evolution of the spectrum of the light in a resonant thermal vapor. We observe the gradual change of the spectrum and its convergence towards a regime of complete frequency redistribution as the number of scattering events increases. We also analyze the probability density function of the step length of photons between emissions and reabsorptions in the vapor, which governs the statistics of the light diffusion. We observe two different regimes in the light transport: superdiffusion when the vapor is excited near the line center and normal diffusion for excitation far from the line center. The regime of complete frequency redistribution is not reached for excitation far from resonance even after many absorption and reemission cycles due to correlations between emitted and absorbed frequencies.
The line-shape function is expressed in terms of three boundary functions related to the two-particle Green's function. The transverse as well as the longitudinal interaction among atoms is considered, using the photon propagator approach. The broadening of one of the radiative states through the resonance interaction with the ground state is considered in detail. The contributions of multiple transfer of excitation and of two-body scattering are calculated separately. Several validity conditions are also obtained which clarify the approximations in the existing results. The velocity dependence of the width parameter is investigated in some detail; our results differ considerably from the existing results because we have included higher-order contributions. The extreme low-density region [where (collision width) \ensuremath{\sim} (natural width)] is also considered; the linewidth is found to be nonlinear in the number density. The additional contribution of the coupling between the radiative states is also calculated in a special case.