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Optics Letters

Coherent population oscillations and hole burning observed in Sm^+2:CaF_2 using polarization spectroscopy

J. H. Lee, J. J. Song, M. A. F. Scarparo, M. D. Levenson

Published May 1, 1980• 45 citations
Publisher

Abstract

Polarization spectroscopy was used for the first time known to the authors to measure the homogeneous linewidth and excited-state lifetime of an inhomogeneously broadened transition of an absorbing impurity ion in a crystalline host. The observed line shapes agree with those predicted by a density-matrix calculation.
DOI
10.1364/ol.5.000196

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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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Persistent spectral hole burning (PSHB) was discovered in organic molecular system in 1974[1]. Five years later, PSHB in inorganic materials was discovered in NaF by R. M. Macfarlane et al [2]. In 1985, A. Winnacker et al [3] first observed photon gated spectral hole burning in BaFCl: Sm2+ at 2K. Hole burning(HB) is useful in high resolution spectroscopy. It is also of crucial importance for the application to frequency domain optical storage. The storage density is proportional to the ratio of inhomogeneous linewidth(Γi) to the homogeneous linewidth(Γh), N(= Γi/Γh). The inhomogeneous linewidth of 5D0-TF0 transition of Sm2+ is 16GHz and the hole width is 25MHz in BaFCl at 2K[3]. For this material, the inhomogeneous linewidth changes only moderately with the temperature; On the other hand, the homogeneous linewidth increases rapidly as the temperature rises. Then, a small value of N(~2) can be estimated when HB temperature is raised to 77K. That means, it is difficult to burn a hloe in the inhomogeneous line in BaFCl:Sm2+ at 77K. To maintain a reasonable storage capacity or to study HB at a quite high temperature, a large inhomogeneous linewidth is in great request.

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Europhysics Letters (EPL)•Oct 7, 1991•173 citations
We use persistent spectral hole burning to simultaneously measure the homogeneous linewidth and the frequency shift of the lowest one-photon allowed transition of the CaF2:Sm2+{\mathrm{CaF}}_{2}{:\mathrm{S}\mathrm{m}}^{2+}CaF2​:Sm2+ system. A nonmonotonous temperature dependence is observed for the frequency shift. Our measurements for both width and shift indicate that the dominant dephasing process is a direct one-phonon absorption process, the (acoustic) phonon frequency being $\ensuremath{\sim}45 {\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}.$ This means that the Sm2+{\mathrm{Sm}}^{2+}Sm2+ ion possesses a level $\ensuremath{\sim}45 {\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ above the T1u{T}_{1u}T1u​ level. Our discussion suggests that this is the T2u{T}_{2u}T2u​ level. The inhomogeneous distribution is Lorentzian and its width and position depend on the Sm3+{\mathrm{Sm}}^{3+}Sm3+ concentration (the ${\mathrm{Sm}}^{3+}\ensuremath{-}{\mathrm{F}}^{\mathrm{\ensuremath{-}}}$ complexes acting as point defects) exactly as predicted by theory.
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.
The study of optical relaxation processes in solids at low temperature has progressed tremendously in the last 20 years due to the development of coherent optical techniques. The latter would not have been possible without the advent of narrow-band tunable lasers, on the one hand, and lasers with very short pulses (picoseconds, femtosecoods) on the other hand. Such coherent techniques are necessary because spectral line shapes of solids doped with guest molecules are seldom determined by dynamical interactions but principally by strain or structural disorder. This gives rise to inhomogeneous broadening, rlOh, which in crystalline hosts at low temperature varies between ' 0.1 and 10 cm -I, whereas in glasses it may amount to � 100-500 em-I. One of the techniques to achieve narrowing of spectral lines is site­ selection spectroscopy (1-3). A sub-ensemble of molecules within thc inhomogeneously broadened absorption band is selectively excited by mcans of a narrow-band laser, and the fluorescence or phosphoresccnce signal is detected with a high-resolution monochromator and/or a Fabry­ Perot interferometer. Fluorescence line-narrowing ( I) is a special case of this technique (for a review see 3). The intrinsic or homogeneous spectral linewidth, r hom, which yields information on the relaxation processes of the excited state, is given by the effective optical dephasing time, T2:
Persistent spectral hole burning (PSHB) was discovered in organic molecular system in 1974[1]. Five years later, PSHB in inorganic materials was discovered in NaF by R. M. Macfarlane et al [2]. In 1985, A. Winnacker et al [3] first observed photon gated spectral hole burning in BaFCl: Sm2+ at 2K. Hole burning(HB) is useful in high resolution spectroscopy. It is also of crucial importance for the application to frequency domain optical storage. The storage density is proportional to the ratio of inhomogeneous linewidth(Γi) to the homogeneous linewidth(Γh), N(= Γi/Γh). The inhomogeneous linewidth of 5D0-TF0 transition of Sm2+ is 16GHz and the hole width is 25MHz in BaFCl at 2K[3]. For this material, the inhomogeneous linewidth changes only moderately with the temperature; On the other hand, the homogeneous linewidth increases rapidly as the temperature rises. Then, a small value of N(~2) can be estimated when HB temperature is raised to 77K. That means, it is difficult to burn a hloe in the inhomogeneous line in BaFCl:Sm2+ at 77K. To maintain a reasonable storage capacity or to study HB at a quite high temperature, a large inhomogeneous linewidth is in great request.
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.
Two-photon persistent hole burning is observed at T = 296 K in 5 D 1 – 7 F 0 and 5 D 0 – 7 F 0 transitions of Sm 2+ ions in substitutionally disordered SrFCl 1/2 single crystals, showing the ratio of inhomogeneous to homogeneous linewidth of 20 ÷ 25. The minimum hole widths of 3.5 cm -1 and 2.6 cm -1 , respectively, were determined for these transitions. In fact, the applicability of persistent spectral hole burning, known as a low-temperature high-resolution spectroscopic method and a potential basis for the use of a new–spectral–dimension in optical data storage and processing, is demonstrated for the first time at room temperature in inorganic materials.