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Physical Review A

Reexamination of the theory of light-induced atomic desorption

Krzysztof Rębilas, Marek Jan Kasprowicz

Published Apr 17, 2009• 16 citations

Abstract

The commonly accepted theory of light-induced atomic desorption (LIAD) [S. N. Atutov et al., Phys. Rev. A 60, 4693 (1999)] explains the dynamics of this effect by referring to a light-enhanced diffusion process proceeding in the absorbing medium. On the other hand, recently performed measurements show that in siloxane films which are used in LIAD experiments, the characteristic time of diffusion is extremely short (a fraction of 1 s) compared to the duration of the LIAD effect (hundreds of seconds). This is in contradiction to the conceptual basis of the theory of Atutov et al. that requires the characteristic diffusion time to be sufficiently long. What is more, the theory of Atutov et al. relies on an unjustified assumption about the dependence of the diffusion coefficient on the light intensity. In consequence, the theoretical results of Atutov et al. yield unsatisfactory predictions and do not fit well with experimental data. In this paper, we consider a partially illuminated siloxane-coated cell and propose an alternative theory of LIAD dynamics based on an assumption about lateral diffusion proceeding in the siloxane coating. Our theory provides a unique solution for the desorbed atoms' density regardless of the power of the laser light, explains the lengthy duration of LIAD, and accurately reproduces experimental results. A reasoning which explains how the boundary condition at the siloxane surface is established by the incident light gives us a proper relation between the desorbed atoms' density and the intensity of the desorbing light.

DOI: 10.1103/physreva.79.042903

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The commonly accepted theory of light-induced atomic desorption (LIAD) [S. N. Atutov et al., Phys. Rev. A 60, 4693 (1999)] explains the dynamics of this effect by referring to a light-enhanced diffusion process proceeding in the absorbing medium. On the other hand, recently performed measurements show that in siloxane films which are used in LIAD experiments, the characteristic time of diffusion is extremely short (a fraction of 1 s) compared to the duration of the LIAD effect (hundreds of seconds). This is in contradiction to the conceptual basis of the theory of Atutov et al. that requires the characteristic diffusion time to be sufficiently long. What is more, the theory of Atutov et al. relies on an unjustified assumption about the dependence of the diffusion coefficient on the light intensity. In consequence, the theoretical results of Atutov et al. yield unsatisfactory predictions and do not fit well with experimental data. In this paper, we consider a partially illuminated siloxane-coated cell and propose an alternative theory of LIAD dynamics based on an assumption about lateral diffusion proceeding in the siloxane coating. Our theory provides a unique solution for the desorbed atoms' density regardless of the power of the laser light, explains the lengthy duration of LIAD, and accurately reproduces experimental results. A reasoning which explains how the boundary condition at the siloxane surface is established by the incident light gives us a proper relation between the desorbed atoms' density and the intensity of the desorbing light.

The light-induced atomic desorption effect, known as LIAD, has been explained so far by a debatable Atutov's theory [S. N. Atutov et al., Phys. Rev. A 60, 4693 (1999)]. In this Brief Report, we propose an approach in which the difficulties of this theory are removed. The theory yields predictions for the atomic vapor density

n(t)

in a fully illuminated resonance cell, the time

{t}_{max}

that it takes the vapor density to arrive at a maximum value

{n}_{max}

and the dependence of

{n}_{max}

and

dn/d{t}_{t=+0}

on the desorbing light intensity. Some of our results are at variance with outcomes of Atutov's model (such as saturation effect for

{n}_{max}

and the dependence of

{t}_{max}

on the light intensity) but are in agreement with the experimental data. Additionally, the model presented in this Brief Report satisfactorily explains a reservoir effect recently investigated in experiments where cells equipped with a lockable stem were used.

The light-induced desorption and diffusion of alkali-metal atoms in organic films are interesting fields of investigation. An impressive demonstration is given by the recently observed light-induced atomic desorption (LIAD) effect, where a huge alkali-metal atom desorption from siloxane films, previously exposed to atomic vapors, is induced by weak and nonresonant light. In this paper, experimental data and a one-dimensional theoretical model of the effect are presented. The model gives a good description of the vapor density dynamics by taking into account both the atomic diffusion inside the coating and the surface desorption. General equations are reported and discussed within the limits of experimental interest. The potential barrier at the vapor-surface interface and the activation energy for Rb in (poly)dimethylsiloxane have been determined.

We observe Light-induced atomic desorption (LIAD) of Rb and Cs atoms from a PDMS-coated cell containing both atoms at the same time. The desorption rate and the relative vapor density variation have been simultaneously measured for both alkali atoms as a function of the desorbing light intensity and frequency. They show the same behaviour upon the different illumination conditions. This work demonstrates the possibility to provide light controlled atomic dispenser delivering different atomic species using the LIAD effect.

We review some recent studies on light-induced atomic desorption (LIAD) from dielectric surfaces. Alkali-metal atoms adsorbed either on organic films or on porous glass are released into the vapor phase under illumination. The measurements were performed in Pyrex resonance cells either coated with siloxane films or containing a porous glass sample. In both cases, the experimental results show that LIAD can be used to produce atomic densities suitable for most atomic physics experiments. Moreover, we find that photoinduced effects, correlated with LIAD, produce reversible formation and evaporation of alkali-metal clusters in porous glass. These processes depend on the light frequency, making the porous glass transmittance controllable by light.

This work is devoted to a systematic study of the effect of Light-Induced Atomic Desorption (LIAD). LIAD is a non-heating process in which atoms adsorbed on a surface are desorbed by illumination with non-resonant light. The aim of the dissertation is an experimental study of the LIAD process, its influence on the spectra of alkali atoms in optical cells without and with Anti-Relaxation Coating (ARC) and the possibilities of LIAD for optical characterization of ARC, as well as in high resolution spectroscopy. For the first time, the LIAD process under homogeneous illumination was investigated experimentally, whereby the efficiency of the LIAD was significantly increased even for a cell without ARC, the dynamic characteristics are obtained with a better signal to noise ratio and repeatability, and the desorption and adsorption processes are faster. LIAD effect in cells with different ARC coatings has shown that each coating has different desorption and adsorption rates and the results obtained show the possibility of applying the method for optical characterization of ARC. An experimental study of the number of collisions without atomic spin depolarization in cells with different ARCs and the impact of LIAD was performed, as well as various parameters such as laser intensity and cell temperature were investigated.

The study of the very complicated atom-surface interaction in presence of light had an increasing momentum during these last few years. A new field has been opened by a recent experiment made by Gozzini et al.,1 where a new and interesting effect, consisting in a huge sodium desorption when a silane coated cell is illuminated at room temperature, has been observed. Similar results, still in silane coated cells, have also been obtained by Meucci et al.2 with rubidium and cesium. The effect, shortly indicated hereafter as LIAD (light-induced atom desorption), is totally different from the other processes produced by very intense laser pulses, where the main effect produced by light is a thermal one.