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Excimer Emission from Alkali Diatomic and Alkaline-Earth-Noble Gas Molecules

John Huennekens

Published Mar 1, 1994• 0 citations
OpenAlex

Abstract

We have carried out a series of experiments to study collisional and radiative processes in alkali metal and alkaline-earth vapors. Our principal interest has been to understand fundamental atom-atom, atom-molecule, and atom- light interactions in order to model alkali diatomic and alkaline-earth excimer systems for possible laser applications. During this funding period, we have concentrated on collisional excitation transfer, quenching and diffusion processes involving the metastable 6s5dD sub J levels of barium. We have also investigated alkali and alkaline-earth vapors as media for observing low threshold nonlinear optical processes

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We have carried out a series of experiments to study collisional and radiative processes in alkali metal and alkaline-earth vapors. Our principal interest has been to understand fundamental atom-atom, atom-molecule, and atom- light interactions in order to model alkali diatomic and alkaline-earth excimer systems for possible laser applications. During this funding period, we have concentrated on collisional excitation transfer, quenching and diffusion processes involving the metastable 6s5dD sub J levels of barium. We have also investigated alkali and alkaline-earth vapors as media for observing low threshold nonlinear optical processes
We describe a series of measurements of absorption and laser induced fluorescence on cells that contained cesium and rubidium and a rare gas: He, Ar, Kr, or Xe. These studies showed strong blue wing absorption to the short wavelength side of the alkali atom D2 lines due to collisionally formed Cs- or Rb-rare gas excimers. We also have observed an efficient two photon excitation of higher lying states in Cs and Rb that produces both intense blue emission and IR atomic emission in the 1.3 to 3.8 μm spectral region.
An investigation was made of the mechanisms of quenching of excited states and of excitation of atomic levels as a result of absorption of laser radiation by alkali metal (Na, K, Cs) vapors. It was found that several processes participated in the excitation of atomic levels: collisional mechanism of excitation energy transfer from molecules to atoms, photodissociation, predissociation, and nonresonant excitation of atomic levels (radiative collisions). The partial contribution of each of these processes (dependent on the vapor density, intensity of laser radiation, and its frequency) should be allowed for in the balance of the filling and deactivation of molecular and atomic states. Qualitative characteristics were obtained for these processes and an analysis was made of their likely role in the emission of radiation from diatomic molecules in alkali metal vapors.
Research on ultracold molecules has seen a growing interest recently in the context of high-resolution spectroscopy and quantum computation. After forming weakly bound molecules from atoms in cold collisions, the preparation of molecules in low vibrational levels of the ground state is experimentally challenging, and typically achieved by population transfer using excited electronic states. Accurate potential energy surfaces are needed for a correct description of processes such as the coherent de-excitation from the highest and therefore weakly bound vibrational levels in the electronic ground state via couplings to electronically excited states. This paper is dedicated to the vibrational analysis of potentially relevant electronically excited states in the alkali-metal (Li, Na, K, Rb)-- alkaline-earth metal (Ca,Sr) diatomic series. Graphical maps of Frank-Condon overlap integrals are presented for all molecules of the group. By comparison to overlap graphics produced for idealized potential surfaces, we judge the usability of the selected states for future experiments on laser-enhanced molecular formation from mixtures of quantum degenerate gases.