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Journal of Luminescence

Hyperfine spectroscopy and spin dynamics by optical and sublevel coherence

Robert M. Shelby, R. M. Macfarlane

Published Dec 1, 1984• 39 citations
Publisher
DOI
10.1016/0022-2313(84)90141-8

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Due to their narrow homogeneous linewidths, rare-earth ions in inorganic crystals at low temperatures have recently been given considerable attention as test materials for experiments in coherent quantum optics. Because these narrow linewidth transitions have been buried in a wide inhomogeneous line, the scope of experiments that could be carried out in these materials has been limited. However, here we present spectroscopic techniques, based on spectral hole burning and optical pumping, which allow hyperfine transitions that are initially buried within an inhomogeneously broadened absorption line to be studied with no background absorption from other transitions. A sequence of hole-burning pulses is used to isolate selected transitions between hyperfine levels, which makes it possible to directly study properties of the transitions, e.g., transition strengths, and gives access to information that is difficult to obtain in standard hole-burning spectroscopy, such as the ordering of hyperfine levels. The techniques introduced are applicable to absorbers in a solid with long-lived sublevels in the ground state and where the homogeneous linewidth and sublevel separations are smaller than the inhomogeneous broadening of the optical transition. In particular, this includes rare-earth ions doped into inorganic crystals and in the present work the techniques are demonstrated in spectroscopy of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$. Information on the hyperfine structure and relative transition strengths of the $^{3}H_{4}\text{\ensuremath{-}}^{1}D_{2}$ hyperfine transitions in ${\mathrm{Pr}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ has been obtained from frequency-resolved absorption measurements, in combination with coherent and incoherent driving of the transitions.

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It has been well established that for many metastable electronic levels of impurity ions in insulators, optical coherence times at liquid helium temperatures are limited by magnetic interactions with host nuclear spins. 1 To understand coherence loss in detail, one needs measurements of optical and spin dephasing, magnetic properties and hyperfine structure of impurity ions, and spin dynamics of host nuclei. To this end techniques such as spectral hole burning, 2 coherent transients (e.g. photon echo), 1,3 and optical-rf double resonance 4 have been used. All of these are limited directly or indirectly by optical T2, and have not directly probed the dynamics of host nuclei.
A compact source which produces atomic alkali-metal beams in individual hyperfine sublevels has been developed. The methods are demonstrated with 23Na^{23}\mathrm{Na}23Na atoms. Initially nearly all atoms are transferred into one hyperfine sublevel (∣F,mF〉=∣2,2〉|F, {m}_{F}〉=|2, 2〉∣F,mF​〉=∣2,2〉) by a double-resonance technique using laser optical pumping and rf transitions. Subsequently the other hyperfine sublevels can be populated selectively by an adiabatic high-frequency transition. The hyperfine sublevel populations are determined by laser-induced fluorescence spectroscopy in a magnetic field.
Due to their narrow homogeneous linewidths, rare-earth ions in inorganic crystals at low temperatures have recently been given considerable attention as test materials for experiments in coherent quantum optics. Because these narrow linewidth transitions have been buried in a wide inhomogeneous line, the scope of experiments that could be carried out in these materials has been limited. However, here we present spectroscopic techniques, based on spectral hole burning and optical pumping, which allow hyperfine transitions that are initially buried within an inhomogeneously broadened absorption line to be studied with no background absorption from other transitions. A sequence of hole-burning pulses is used to isolate selected transitions between hyperfine levels, which makes it possible to directly study properties of the transitions, e.g., transition strengths, and gives access to information that is difficult to obtain in standard hole-burning spectroscopy, such as the ordering of hyperfine levels. The techniques introduced are applicable to absorbers in a solid with long-lived sublevels in the ground state and where the homogeneous linewidth and sublevel separations are smaller than the inhomogeneous broadening of the optical transition. In particular, this includes rare-earth ions doped into inorganic crystals and in the present work the techniques are demonstrated in spectroscopy of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​. Information on the hyperfine structure and relative transition strengths of the $^{3}H_{4}\text{\ensuremath{-}}^{1}D_{2}$ hyperfine transitions in Pr3+:Y2SiO5{\mathrm{Pr}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Pr3+:Y2​SiO5​ has been obtained from frequency-resolved absorption measurements, in combination with coherent and incoherent driving of the transitions.