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arXiv:1401.0731 · Physical Review Letters

Kennard-Stepanov Relation Connecting Absorption and Emission Spectra in an Atomic Gas

Peter Moroshkin, Lars Weller, Anne Saß, Jan Klaers, Martin Weitz

Published Aug 6, 2014• 27 citations
arXivHTMLPDF

Abstract

The Kennard-Stepanov relation describes a thermodynamic, Boltzmann-type scaling between the absorption and emission spectral profiles of an absorber, which applies in many liquid state dye solutions as well as in semiconductor systems. Here we examine absorption and emission spectra of rubidium atoms in a dense argon buffer gas environment. We demonstrate that the Kennard-Stepanov relation between absorption and emission spectra is well fulfilled in the collisionally broadened atomic gas system. Our experimental findings are supported by a simple theoretical model.

DOI
10.1103/physrevlett.113.063002

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The Kennard-Stepanov relation describes a thermodynamic, Boltzmann-type scaling between the absorption and emission spectral profiles of an absorber, which applies in many liquid state dye solutions as well as in semiconductor systems. Here we examine absorption and emission spectra of rubidium atoms in a dense argon buffer gas environment. We demonstrate that the Kennard-Stepanov relation between absorption and emission spectra is well fulfilled in the collisionally broadened atomic gas system. Our experimental findings are supported by a simple theoretical model.
We report on experiments investigating laser cooling of atomic gases by collisional redistribution of radiation, a technique applicable to dense mixtures of alkali metals with noble gases. Thermal deflection spectroscopy is one of the methods used to measure the temperature change of the laser-cooled gas. In this work we describe experiments focusing on a different technique for precise determination of the local temperature achieved by the cooling within the gas cell. We investigate the Kennard-Stepanov relation, a thermodynamic, Boltzmann-type scaling between the absorption and emission spectral profiles of an absorber, which applies in many liquid state dye solutions as well as in semiconductor systems. To this end, absorption and emission spectra of rubidium atoms and dimers in dense argon buffer gas environment have been recorded. We demonstrate experimentally that the Kennard-Stepanov relation between absorption and emission spectra is well fulfilled for the collisionally broadened atomic and molecular transitions of the system, which allows for the extraction of the thermodynamic temperature.
Abstract Optical spectroscopy of atoms and molecules is a field where one usually operates very far from thermal equilibrium conditions. A prominent example is spectroscopy of thin vapors, where the pump irradiation leads to a non-equilibrium distribution within the electronic structure that is well shielded from the environment. Here we describe experimental work investigating absorption and emission lines of rubidium vapor subject to a noble buffer gas environment with pressure 100–200 bar, a regime interpolating between usual gas phase and liquid/solid state conditions. Frequent elastic collisions in the dense buffer gas sample cause a large coupling to the environment. We give a detailed account of recent observations of the Kennard–Stepanov scaling, a Boltzmann-like thermodynamic frequency scaling between absorption and emission profiles, for both atomic and molecular rubidium species in the gaseous environment. Our observations are interpreted as due to the thermalization of alkali-noble gas submanifolds in both ground and electronically excited states respectively. Both pressure broadening and shift of the high pressure buffer gas D -lines system are determined. We also discuss some prospects, including possible advances in collisional laser cooling and optical thermometry.
Spectroscopy of alkali-metal--buffer-gas mixtures at high pressures from single-digit to several hundred bars in the regime of substantial collisional broadening is relevant in a wide range of fields, ranging from collisional redistribution cooling to laboratory astrophysics. Here we report on spectroscopic measurements of dense rubidium--noble-gas mixtures recorded in a pressure cell equipped with soldered sapphire optical viewports, which allows for the controlled realization of extreme conditions of high temperature and high pressure in a table top laboratory experiment. In the gas cell, we have recorded absorption and emission spectra of rubidium subject to 188 bars of helium buffer-gas pressure at 548-K temperature. The spectra to good accuracy follow a Boltzmann-type Kennard-Stepanov frequency scaling of the ratio of absorption and emission spectral profiles. Further, the long optical path length in the cell allowed us to both record spectra of rubidium-argon mixtures at moderate temperatures and high pressures and observe redistributional laser cooling in this system.
Between the absorption and the emission spectral lineshapes of dense atomic and molecular media, such as dye solutions and alkali-noble buffer gas mixtures at high pressure, in many cases there exists a universal scaling, the Kennard-Stepanov relation, which is a manifestation of detailed balance. This relation plays a crucial role in recent Bose-Einstein condensation experiments of visible-spectral-photons in e.g.~dye-solution-filled optical microcavities. It has recently been proposed to use high-pressure xenon-noble gas mixtures as a thermalization medium for vacuum-ultraviolet regime photons, so as to extend the achievable wavelength range of such Bose-Einstein-condensed optical sources from the visible to the vacuum-ultraviolet regime. In this work, we report two-photon excitation spectroscopy measurements of ground state (5p65p^65p6) xenon atoms subject to up to 80bar of helium or krypton buffer gas pressure, respectively, in the 220-260nm wavelength range. The study of such two-photon spectra is of interest e.g.~for the exploration of possible pumping schemes of a future vacuum-ultraviolet photon Bose-Einstein condensate. We have also recorded absorption and emission spectra of the 5p6↔5p56s5p^6 \leftrightarrow 5p^56s5p6↔5p56s single-photon transition near 147nm wavelength of xenon atoms subject to 80bar of krypton buffer gas pressure. We find that the ratio of absorption and emission shows a Kennard-Stepanov scaling, which suggests that such gas mixtures are promising candidates as a thermalization medium for a Bose-Einstein condensate of vacuum-ultraviolet photons.
Laser cooling via collisional redistribution of fluorescence utilizes dense mixtures of alkali metals with noble buffer gases. Typical pressure values of the buffer gas are of the order of a few hundred bar, ensuring a frequent number of collisions between the two atomic species. The energy levels of the alkali atoms are thus perturbed so that excitation using far red-detuned laser light becomes feasible. Energy is then extracted via spontaneous emission occuring close to the unperturbed atomic resonances. Optimization of the cooling effect strongly depends on excitation conditions, namely the choice of detuning of the cooling beam, which in turn is dependent on the used pressure. We here report on spectroscopy measurements of atomic rubidium under high pressure buffer gas conditions. While thermal deflection spectroscopy has been previously used to measure the temperature change of the laser-cooled gas, an alternative approach for temperature measurements utilizing the Kennard-Stepanov relation is also investigated. We here exhibit that the collisionally thermalized atomic resonances well follow this thermodynamic scaling, allowing for temperature extraction of the dense gas mixture.
To understand the optical properties of atoms in solid state matrices, the absorption, excitation, and emission spectra of rubidium doped thin-films of argon, krypton, and xenon were investigated in detail. A two-dimensional spectral analysis extends earlier reports on the excitation and emission properties of rubidium in rare-gas hosts. We found that the doped crystals of krypton and xenon exhibit a simple absorption-emission relation, whereas rubidium in argon showed more complicated spectral structures. Our sample preparation employed in the present work yielded different results for the Ar crystal, but our peak positions were consistent with the prediction based on the linear extrapolation of Xe and Kr data. We also observed a bleaching behavior in rubidium excitation spectra, which suggests a population transfer from one to another spectral feature due to hole-burning. The observed optical response implies that rubidium in rare-gas thin-films is detectable with extremely high sensitivity, possibly down to a single atom level, in low concentration samples.