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Excitation and emission spectra of rubidium in rare-gas thin-films

Ilja Gerhardt, A Brian Sin, Takamasa Momose

Published Aug 16, 2016• 8 citations
OpenAlex

Abstract

To understand the optical properties of atoms in solid state matrices, the absorption, excitation and emis-sion 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 consis-tent 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. I.

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To understand the optical properties of atoms in solid state matrices, the absorption, excitation and emis-sion 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 consis-tent 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. I.
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.
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.
Relaxation experiments have been performed between 0–200 G on optically polarized Rb atoms in argon, krypton or xenon, at pressures ranging from 0.1 to 20 torr. They clearly show the existence of Rb–Ar, Rb–Kr and Rb–Xe molecules of low binding energy (smaller than kT). Molecular parameters such as lifetime, spin-orbit coupling constant, formation rate, constant of mass action, etc., are measured, or evaluated when they cannot be directly measured. Experimental values of the diffusion coefficient of Rb in the gas (except xenon) and of the disorientation cross sections by usual binary collisions are also obtained.
Rare-earth (RE) atoms, such as erbium (Er), have inner-shell optical transitions in the near-infrared, some of which are in the telecom bands. These transitions are largely insensitive to the host environment due to effective shielding by the filled outer shells. Cryogenic rare-gas (RG) solids, such as solid neon (Ne) and argon (Ar), combine high chemical purity with a nearly nuclear-spin-free environment, making them attractive solid hosts for preserving optical and spin coherence. In this work, we isolate neutral Er atoms in solid Ne and Ar at 6 K and characterize their emission by steady-state and time-resolved photoluminescence (PL) spectroscopy. In both hosts, we observe several near-infrared transitions between 1000--1500 nm, including inner-shell emission in the telecom O and E bands. The 4f→5d4f \rightarrow 5d4f→5d transition near 1299 nm forms a multiplet of narrow components, consistent with crystal-field splitting, and decays on a microsecond timescale. The 4f→4f4f \rightarrow 4f4f→4f transition near 1437 nm shows a matrix shift below 1 cm−1^{-1}−1 in both hosts. In solid Ne, its inhomogeneous linewidth is bounded by the spectrometer resolution to < 22 GHz, and its PL lifetime reaches up to 78.9 ms, close to the estimated radiative limit. Thermal annealing extends the 1437 nm lifetime in Ne and suppresses the phonon sidebands relative to the zero-phonon lines in Ar. These results identify RG solids as promising hosts for long-lived telecom-band Er emission and provide a foundation for future spin-photon interfaces and hybrid quantum architectures.
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.