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Physica Scripta

Decay times of radiative and non-radiative transitions in rare-earth ions

E. F. Kustov, Victor B. Loschenov, Irina Basieva

Published Dec 1, 2014• 3 citations
Publisher

Abstract

We present a theoretical method for evaluation of decay times of both radiative and non-radiative transitions in rare-earth ions in crystals and glasses. Relying on one experimentally known lifetime and known parameters of electrostatic and spin–orbit interaction, the fluorescence spectra can be modelled for various pumping wavelengths providing new insights into dynamical processes of fluorescence.

DOI
10.1088/0031-8949/2014/t163/014032

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We present a theoretical method for evaluation of decay times of both radiative and non-radiative transitions in rare-earth ions in crystals and glasses. Relying on one experimentally known lifetime and known parameters of electrostatic and spin–orbit interaction, the fluorescence spectra can be modelled for various pumping wavelengths providing new insights into dynamical processes of fluorescence.
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Flip-flop processes due to magnetic dipole-dipole interaction between neighboring ions in crystals doped by rare-earth ions are one of the mechanisms of relaxation between hyperfine levels. Modeling of this mechanism has so far been macroscopic, characterized by an average rate describing the relaxation of all ions. Here, however, we present a microscopic model of flip-flop interactions between individual nuclear spins of dopant ions. Every ion is situated in a unique local environment in the crystal, where each ion has different distances and a unique orientation relative to its nearest neighbors, as determined by the lattice structure. Thus each ion has a unique flip-flop rate and the collective relaxation dynamics of all ions in a bulk crystal is a sum of many exponential decays, giving rise to a distribution of rates rather than a single average decay rate. We employ this model to calculate flip-flop rates in Pr3+{\mathrm{Pr}}^{3+}Pr3+:Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ and show experimental measurements of population decay of the ground state hyperfine levels at $\ensuremath{\sim}2$ K. We also present a method to measure rates of individual transitions from hole burning spectra that requires significantly fewer fitting parameters in theoretical rate equations compared to earlier work. Furthermore, we measure the effect of external magnetic field on the flip-flop rates and observe that the rates slow down by two orders of magnitude in a field of 5--10 mT.
The negative ion of lanthanum has one of the richest bound-state spectra observed for an atomic negative ion and it has been proposed as a promising candidate for laser cooling, which has not yet been achieved for any negatively charged system. In the present study, radiative decays of low-lying excited states of ${\mathrm{La}}^{\ensuremath{-}}$ were experimentally investigated at the DESIREE cryogenic electrostatic ion-beam storage ring facility using state-selective photodetachment over storage times of up to 800 s. Independently, the transition rates for the relevant states were calculated using a high-precision hybrid theoretical approach. The measured lifetime of the lowest excited state of ${\mathrm{La}}^{\ensuremath{-}}$ (3F3e)({}^{3}{F}_{3}^{e})(3F3e​) of 132(20) s agrees very well with the theoretical calculations and previous predictions. However, a puzzling discrepancy exists for the next-higher state 3F4e{}^{3}{F}_{4}^{e}3F4e​, with the experiments yielding a lifetime $\ensuremath{\sim}4$ times shorter than calculated, highlighting the challenges for this complex ion. The results provide valuable insights into the prospects for laser cooling ${\mathrm{La}}^{\ensuremath{-}}$.
A method has been proposed for the direct detection and study of long-lived excited states of singly and multiply charged ions of transition and rare earth metals. It allows both the measurement of the photon spectra from the decay of long-lived states of ions with a given charge, as well as the lifetimes of such states, and the investigation of the influence of an electric field on the characteristics of long-lived states. The fast electric-field-induced decay of long-lived states has been found for the first time.