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Physical review. B, Condensed matter

Persistent spectral hole burning spectroscopy of the T1u←A1g (690 nm) line in the CaF2:Sm2+ system

W. Beck, D. Ricard, Christos Flytzanis

Published Nov 1, 1998• 5 citations
Publisher

Abstract

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 ${\mathrm{CaF}}_{2}{:\mathrm{S}\mathrm{m}}^{2+}$ 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 ${\mathrm{Sm}}^{2+}$ ion possesses a level $\ensuremath{\sim}45 {\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ above the ${T}_{1u}$ level. Our discussion suggests that this is the ${T}_{2u}$ level. The inhomogeneous distribution is Lorentzian and its width and position depend on the ${\mathrm{Sm}}^{3+}$ concentration (the ${\mathrm{Sm}}^{3+}\ensuremath{-}{\mathrm{F}}^{\mathrm{\ensuremath{-}}}$ complexes acting as point defects) exactly as predicted by theory.

DOI
10.1103/physrevb.58.11996

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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∼45cm\ensuremath−1.\ensuremath{\sim}45 {\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}.\ensuremath∼45cm\ensuremath−1. This means that the Sm2+{\mathrm{Sm}}^{2+}Sm2+ ion possesses a level \ensuremath∼45cm\ensuremath−1\ensuremath{\sim}45 {\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}\ensuremath∼45cm\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 Sm3+\ensuremath−F\ensuremath−{\mathrm{Sm}}^{3+}\ensuremath{-}{\mathrm{F}}^{\mathrm{\ensuremath{-}}}Sm3+\ensuremath−F\ensuremath− complexes acting as point defects) exactly as predicted by theory.
With a ring dye laser persistent spectral hole-burning was measured by fluorescence excitation spectroscopy in the zero-phonon lines of the 2llg ↔ 2llu transition in KI:S2 − and of the 3H4 → 3P0 transition of a defect center with three D− ions in SrF2:Pr3+:D−and also in the zero-phonon line at 462.5 nm of a color center in neutron-irradiated and annealed α-Al2O3. In all three lines holes with a width in the order of 1 GHz could be obtained at 1.5 K with single frequency laser. With broad-band laser in KI:S2 − and SrF2:Pr3+:D− spectral redistribution within the full range of inhomogeneous broadening could be observed which are explained by a photophysical model based on barrier crossing in asymmetric double-well-potentials. In the case of sapphire a photobleaching process is dominant which is effective also for nonselective excitation, and the holes are thermoresistant up to 300 K.
Photon gated spectral hole-burning was first observed in a samarium doped crystal, BaFCl:Sm2+ [1]. This material was of interest to the developement of optical memories as the holes were found to be stable to room temperature thermal cycling. Holes could be burnt at liquid helium temperatures but as the temperature was raised the line quickly became homogeneously broadened. The addition of bromine to the melt succeeded in broadening the inhomogeneous linewidths to about 2 nm through substitutional disorder [2] and persistent holes were observed at 77 K [3]. Subsequently, a study of the parameters for spectral hole-burning in a BaFCl0.5Br0.5:Sm2+ crystalline powder was performed [4] and the highest temperature for which persistent hole-burning had been observed was raised to 133 K. Here we report spectral hole-burning at room temperature (figure 1) in a related compound, Sr0.5Mg0.5FCl0.5Br0.5:Sm2+.
We measured the temperature dependence of the fluorescence of Sm 2+ ions doped into a Mg 0.5 Sr 0.5 FCl 0.5 Br 0.5 mixed crystal and observed the persistent spectral hole burning at 90 K and 300 K. The electrons appearing at the 5 D 0 → 7 F 0 transition mostly come via the 4f5d→ 5 D 1 → 5 D 0 → 7 F 0 route but some of the electrons come directly from the 4f5d band. At 90 K, persistent spectral hole burning was achieved much more efficiently by the photon-gated spectral hole-burning process than by the one-photon hole-burning process, while the one-photon hole-burning process is much more efficient at 300 K.
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.
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.