Cesium atoms in cryogenic argon matrix

Abstract

This paper presents both experimental and theoretical investigations into the spectroscopy of dilute cesium (Cs) atoms within a solid argon (Ar) matrix at cryogenic temperatures. This system is relevant for matrix isolation spectroscopy and in particular for recently proposed methods for investigating phenomena that extend beyond the standard model of particle physics. We record absorption spectra at various deposition temperatures and examine the evolution of these spectra post-deposition with respect to temperature changes. Taking advantage of Cs-Ar and Ar-Ar pairwise interaction potentials, we conduct a stability study of trapping sites, which indicates a preference for T$_{\rm d}$ (tetrahedral, 4 vacancies) and O$_{\rm h}$ (cubic, 6 vacancies) symmetries. By implementing a mean-field analysis of the long-range Cs(6s,6p)-Ar-Ar triple dipole interaction, combined with a temperature-dependent shift in zero point energy, we propose effective Cs(6s,6p)-Ar pairwise potentials. Upon integrating these pairwise potentials with spin-orbit coupling, we achieve a satisfactory agreement between the observed and simulated absorption line positions. The observed line broadening is reasonably well reproduced by a semi-classical thermal Monte Carlo approach based on Mulliken-type differences between excited and ground potential curves. Additionally, we develop a simple, first-order crystal field theory featuring only 6 interaction mode coordinates. It uses the reflection approximation and incorporates quantized (phonon) normal modes. This produces a narrow triplet structure but not the observed amount of splitting.