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International Conference on Spectral Line Shapes (ICSLS)

Optical spectra of atoms in liquid helium and cold helium gas

Michio Takami

Published Jan 1, 1999• 0 citations
Publisher

Abstract

Lineshapes associated with the absorption and emission spectra of neutral atoms in liquid helium and cold helium gas are discussed. A neutral atom in liquid helium forms a microcavity due to a strong short-range repulsive force between the helium and impurity atoms, producing very broad and largely blueshifted absorption bands and relatively narrow emission lines with much smaller shifts. A broad and weak emission band observed by exciting the D2 line of Ag atoms in liquid helium has confirmed the hypothesis that quenching of D2 emission lines for heavy group 1a and 1b atoms are due to the formation of exciplex. In cold helium gas, sudden decrease of the emission lifetimes below 5.2 K by the excitation of the D2 line of Ag atoms is attributed to the condensation of He atoms on the metastable 2D5/2 state. Very narrow absorption lines of Eu innershell electron transitions have revealed that superfluid helium behaves as a static and highly homogeneous low temperature matrix.

DOI
10.1063/1.58324

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Physical review. B, Condensed matter•Sep 1, 1994•74 citations
Lineshapes associated with the absorption and emission spectra of neutral atoms in liquid helium and cold helium gas are discussed. A neutral atom in liquid helium forms a microcavity due to a strong short-range repulsive force between the helium and impurity atoms, producing very broad and largely blueshifted absorption bands and relatively narrow emission lines with much smaller shifts. A broad and weak emission band observed by exciting the D2 line of Ag atoms in liquid helium has confirmed the hypothesis that quenching of D2 emission lines for heavy group 1a and 1b atoms are due to the formation of exciplex. In cold helium gas, sudden decrease of the emission lifetimes below 5.2 K by the excitation of the D2 line of Ag atoms is attributed to the condensation of He atoms on the metastable 2D5/2 state. Very narrow absorption lines of Eu innershell electron transitions have revealed that superfluid helium behaves as a static and highly homogeneous low temperature matrix.
The excitation and emission spectra of alkali-metal atoms (Cs and Rb) in liquid helium are studied. The helium pressure is changed from the saturated vapor pressure to about 25 atm at 1.6 K, under which conditions the liquid helium is in a superfluid state. The pressure shift and broadening of the observed spectra corresponding to the D lines are explained qualitatively by a theoretical calculation based on the spherical atomic bubble model. The Cs D2{\mathit{D}}_{2}D2​ excitation spectra are found to have double peaks, indicating the existence of anisotropic oscillations of the bubble surface. The disappearance of the D2{\mathit{D}}_{2}D2​ emission lines and the pressure-dependent quenching of the Rb D1{\mathit{D}}_{1}D1​ emission lines are also discussed.
Laser induced fluorescence spectra of Ag atoms and their time profiles have been studied in cold He gas at temperatures 4.3--25 K and pressure $\ensuremath{\lesssim}1\mathrm{atm}$. The emission spectra following the excitation of the atomic D2D2D2 line consist of three narrow lines and three broadbands, which are assigned to transitions of Ag atoms and AgHe and AgHe2{\mathrm{AgHe}}_{2}AgHe2​ exciplexes. Surprisingly long ( $\ensuremath{\gtrsim}300\mathrm{ns}$) effective emission lifetimes are observed at T>TcT>{T}_{c}T>Tc​ (5.2 K). The long lifetimes are the result of population trapping in the 2D5/2{}^{2}{D}_{5/2}2D5/2​ metastable state. At $T\ensuremath{\lesssim}{T}_{c}$, the effective lifetimes decrease to $\ensuremath{\lesssim}20\mathrm{ns}$ due to the condensation of He gas on the Ag atom in its 2D5/2{}^{2}{D}_{5/2}2D5/2​ state.
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 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.
We report on the systematic observation of emission spectra of Rb∗Hen{\mathrm{Rb}}^{*}{\mathrm{He}}_{n}Rb∗Hen​ exciplexes (n=1,2,…,6),(n=1,2,\dots{},6),(n=1,2,…,6), realized by exciting Rb atoms to the 52P{5}^{2}P52P states (Rb∗)({\mathrm{Rb}}^{*})(Rb∗) in a cold 4He{}^{4}\mathrm{He}4He gas. The observed broad spectral components are assigned to Rb∗Hen{\mathrm{Rb}}^{*}{\mathrm{He}}_{n}Rb∗Hen​ (n=1−−6)(n=1--6)(n=1−−6) using theoretical spectra obtained from ab initio potential curves. The dynamics of the exciplex formation is discussed, based on the observed temperature dependence of the spectra. The He gas density dependence of the spectra of Rb∗He{\mathrm{Rb}}^{*}\mathrm{He}Rb∗He is understood as a change in the population distribution over the vibrational levels. The present results are compared with our previous work with Cs [K. Enomoto et al., Phys. Rev. A 66, 042505 (2002)], and differences are explained in terms of the difference in the fine-structure splitting. Furthermore, we show the emission spectrum observed after the excitation of Rb in liquid He and conclude that it is the fluorescence from the exciplex Rb∗He6.{\mathrm{Rb}}^{*}{\mathrm{He}}_{6}.Rb∗He6​.
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.