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Long-lived coherences for homogeneous line narrowing in spectroscopy.

Riddhiman Sarkar, Puneet Ahuja, Paul R. Vasos, Geoffrey Bodenhausen

Published Feb 2, 2010• 2 citations
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General features of coherence effects in spectroscopy

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Journal of Photochemistry•Jan 1, 1981•0 citations
A polarized laser beam can bleach narrow, long-lived, anisotropic holes in the 607-nm zero-phonon line of the NaF N1{N}_{1}N1​ center. The width of these holes is twice the homogeneous linewidth, and three orders of magnitude less than the inhomogeneous width of the line. We report a polarization-spectroscopy technique which detects the dichroism and birefringence of the hole with better sensitivity than absorption spectroscopy. A simple rateequation model is developed to account for hole burning, but the recovery of the initial isotropic absorption profile appears to be a complex, slow, and intractable process.
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.