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Physical review. B, Condensed matter

Optical spectroscopy of atoms trapped in solid helium

S. I. Kanorsky, Markus Arndt, R. Dziewior, Antoine Weis, Theodor W. Hänsch

Published Feb 1, 1994• 91 citations
Publisher

Abstract

We report a study of implantation and optical spectroscopy of foreign atoms in a solid-helium matrix. With a sample of more than ${10}^{9}$ Ba atoms in 1 ${\mathrm{cm}}^{3}$, a storage time in excess of 5 hours has been demonstrated. Laser-induced fluorescence studies favor the assumption that the isotropy of the trapping site for the implanted atoms is preserved during the liquid-to-solid phase transition.

DOI
10.1103/physrevb.49.3645

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We report a study of implantation and optical spectroscopy of foreign atoms in a solid-helium matrix. With a sample of more than 109{10}^{9}109 Ba atoms in 1 cm3{\mathrm{cm}}^{3}cm3, a storage time in excess of 5 hours has been demonstrated. Laser-induced fluorescence studies favor the assumption that the isotropy of the trapping site for the implanted atoms is preserved during the liquid-to-solid phase transition.
We present an exhaustive overview of optical absorption and laser-induced fluorescence lines of Ba atoms in liquid and solid helium matrices in visible and near-infrared spectral ranges. Due to the increased density of isolated atoms, we have found a large number of spectral lines that were not observed in condensed helium matrices before. We have also measured the lifetimes of metastable states. The lowest 3D1{}^{3}{D}_{1}3D1​ metastable state has lifetime of 2.6 s and can be used as an intermediate state in two-step excitations of high-lying states. Various matrix-induced radiationless population transfer channels have been identified.
The excitation, emission spectra, and decay curves of the emission intensity of thulium atoms implanted in liquid and solid helium were observed in the presence and absence of an external magnetic field. The observed narrow line (width $\ensuremath{\sim}0.1$ nm) of the excitation spectrum at 590.60 nm is assigned as a zero-phonon transition from the electronic ground state 4f13(2F7/2o)6s2{4f}^{13}{(}^{2}{F}_{7/2}^{o}{)6s}^{2}4f13(2F7/2o​)6s2, which indicates that the transition between the inner shells is weakly perturbed by surrounding helium atoms. The pressure dependence of the emission wavelength suggests that the symmetry of helium atoms distributed around a thulium atom in the solid phase is similar to that in the liquid phase. The emission intensity was stable and large in the solid phase since thulium atoms were trapped at a density of 1010{}^{10}10--1011{}^{11}11 atoms/cm3{}^{3}3. The lifetime of the excited state was measured to be $7.09\ifmmode\pm\else\textpm\fi{}0.04$ $\ensuremath{\mu}$s, which was longer than that of the 4f12(3H6)5d5/26s2{4f}^{12}{(}^{3}{H}_{6}{)5d}_{5/2}{6s}^{2}4f12(3H6​)5d5/2​6s2 (6,5/2)7/2{(6,5/2)}_{7/2}(6,5/2)7/2​ state of free thulium atoms. The excited state is expected to be a mixed state of the 4f125d6s2{4f}^{12}{5d6s}^{2}4f125d6s2 and 4f136s6p{4f}^{13}6s6p4f136s6p configurations. The metastable state 4f13(2F5/2o)6s2{4f}^{13}{(}^{2}{F}_{5/2}^{o}{)6s}^{2}4f13(2F5/2o​)6s2 is populated by a radiative transition from this excited state and relaxes to the ground state through a magnetic dipole transition. The lifetime of the metastable state of a neutral thulium atom was measured to be $75\ifmmode\pm\else\textpm\fi{}3$ ms.
We have detected by optical means nonfluorescing 85Rb{}^{85}\mathrm{Rb}85Rb and 87Rb{}^{87}\mathrm{Rb}87Rb atoms implanted in a body centered cubic 4He{}^{4}\mathrm{He}4He crystal. In contrast to cesium the resonance fluorescence of rubidium is strongly quenched by the helium matrix, and the weak resonance absorption of the two Rb isotopes was detected using a double resonance technique. From a comparative study of the (optically detected) magnetic resonance spectra of 85Rb{}^{85}\mathrm{Rb}85Rb, 87Rb{}^{87}\mathrm{Rb}87Rb, and 133Cs{}^{133}\mathrm{Cs}133Cs we infer their effective gF{g}_{F}gF​ factors and conclude that they are not perturbed by the He matrix at a level of $2\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}4}$. We show further that optical pumping of Rb proceeds via depopulation, whereas for Cs it proceeds via repopulation.
We present new results on the properties of Celsium and Rubidium atoms trapped in crystalline helium matrices. We have extended the measurements of optical excitation spectra and excited state lifetimes, previously performed in superfluid helium, to solid helium. Cs atoms in the hcp phase of 4He exhibit several distinctive features, such as dipole-forbidden transitions and zero-field magnetic resonance lines. We interpret these features as being due to static quadrupolar deformations of the local trapping sites (atomic bubbles). The degree of deformation of the bubbles can be obtained by comparing hyperfine coupling constants in the cubic and hexagonal phases. We have investigated in detail optical pumping of Cs in solid helium, and have gained new insights into the pumping mechanism. We have also succeeded, for the first time, in detecting Rb and Rb in solid helium, by applying an absorption technique, based on driven spin precession.
We have measured the pressure broadening and shift of the excitation and emission lines of the 6s2{\mathit{s}}^{2}s2 1^{1}1S0{\mathit{S}}_{0}S0​\ensuremath{\rightarrow}6s6p 1^{1}1P1{\mathit{P}}_{1}P1​ transition of Ba atoms implanted in liquid and solid helium at 1.5 K. The observed spectra are quantitatively explained within the adiabatic line-broadening theory by assuming a bubble structure of the trapping sites for the Ba atoms. The evolution of the bubble shape and size in the optical excitation-deexcitation cycle is modeled theoretically.
We show that for atoms trapped in a liquid He matrix the excitation and emission spectra can be quantit- atively described by the bubble model which treats the matrix as an incompressible continuous medium. Com- parison with experimental results shows that the model also holds for a solid matrix. The model is only valid in the case where the attractive He-He interaction dominates the attractive part of the foreign atom-helium interaction. Its failure in the case of implanted Na atoms is discussed.