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arXiv:1812.05275 · Physical review. B./Physical review. B

Zero-phonon lines in the spectra of dysprosium atoms in superfluid helium

Peter Moroshkin, Kimitoshi Kōno

Published Mar 18, 2019• 10 citations
arXivHTMLPDF

Abstract

We present an experimental study of a zero-phonon line (ZPL) in the absorption spectrum of Dy atoms solvated in superfluid He. The dopants reside in nanometer-sized spherical cavities known as atomic bubbles. We observe a temperature-dependent broadening of ZPL in the absorption spectrum. The effect is attributed to the scattering of thermal phonons on the atomic bubble that leads to the dephasing of the Dy transition dipole. The extrapolated ZPL intrinsic spectral width at zero temperature is 2300 times larger than the natural linewidth in a free atom. This can be assigned to a fast radiationless quenching of the upper state of the studied transition.

DOI
10.1103/physrevb.99.104512

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We present an experimental study of a zero-phonon line (ZPL) in the absorption spectrum of Dy atoms solvated in superfluid He. The dopants reside in nanometer-sized spherical cavities known as atomic bubbles. We observe a temperature-dependent broadening of ZPL in the absorption spectrum. The effect is attributed to the scattering of thermal phonons on the atomic bubble that leads to the dephasing of the Dy transition dipole. The extrapolated ZPL intrinsic spectral width at zero temperature is 2300 times larger than the natural linewidth in a free atom. This can be assigned to a fast radiationless quenching of the upper state of the studied transition.
The optical dephasing, caused by a quadratic interaction with acoustic phonons, is studied on the basis of the nonperturbative theory. The effect of a strong weakening of the elastic springs on the electronic transition is studied. It is found that, if the weakening brings the system close to the dynamical instability, then the usual ∝ T7 dependence of the homogeneous width of a zero-phonon line (ZPL) is replaced by the ∝ T3 dependence in a broad temperature interval. An equation is derived which describes the additional broadening of a ZPL caused by the dynamical instability of the final state. The model explains the temperature broadening and shift of the zero-phonon lines of some nitrogen-containing centers in diamond crystals.
We investigated the zero-phonon line (ZPL) of the deep donor EL2 in GaAs by means of high-resolution absorption spectroscopy with a narrow-band laser. Frequency-selective bleaching (``spectral-hole burning'') experiments and the measurement of the temperature broadening of the ZPL prove an essentially homogeneous broadening of the transition. The observed asymmetry of the line shape is interpreted to be caused by a Fano resonance of the 1T2^{1}\mathrm{T}_{2}1T2​ excited state with the conduction band. A splitting of the 1T2^{1}\mathrm{T}_{2}1T2​ state as the reason for the asymmetry seems unrealistic. The homogeneous broadening of the ZPL prevents the use of spectral-hole burning spectroscopy to study the effect of external perturbations on the ZPL of the EL2.
\n\t\t\t\tA theoretical analysis of the line broadening of localized atomic transitions in liquid helium is presented. It is shown that accurate information can be derived on the long-range part of the He*-He interaction as well as on the local structure near the He* emitters. The analysis confirms that in corona discharges in liquid helium the emitting He* atoms reside in cavities and that for known He*-He interaction the size of the cavities can be deduced from the line profile. The He*-He interaction was calculated using the full configuration interaction (CI) method as implemented in the Molpro package. The widths of atomic lines due to fluorescent transitions between different excited states of helium atoms were calculated as a function of external pressure in the range from 0.1 and 3.5 MPa using the static approximation method, and the input from the results of the CI calculation and cavity diameters calculated using the bubble model. The calculated widths showed excellent agreement with experimental data of liquid helium excited by corona discharges. A second, analytical analysis using a power function to represent the He*-He interaction showed qualitative agreement with the experimental data.\n\t\t\t
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We continue the discussion of the nonperturbative theory of zero-phonon impurity lines in crystals formulated by Osad’ko and more recently by us. In that paper, a diagrammatic analysis was undertaken which led to analytic results for the thermal width and shift of the zero-phonon line. Here we evaluate these results for two model phonon densities of states: the Debye model for acoustic phonons, and a sharply peaked density of states appropriate for optical phonons. For Debye phonons we find that at low temperatures the standard (perturbative) theory of optical dephasing is qualitatively correct, but at high temperatures it becomes very inaccurate. Moreover, if one of the excited state phonon frequencies tends to zero (a soft mode), then perturbation theory breaks down completely. For optical phonons our results give an Arrhenius temperature dependence for the linewidth and place an upper bound on the value of the preexponential. In paper II of this series we will discuss dephasing by pseudo-local phonons, and in paper III we will compare our results to absorption, photon echo, and hole burning experiments.
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.