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Optics Express

Slow light and photon echoes in the 7 F 0 → 5 D 0 transition of Sm 2+ in single-crystal BaFCl

Hans Riesen, Aleksander K. Rebane

Published Aug 16, 2023• 1 citation
Publisher

Abstract

Slow light effects induced by transient spectral hole-burning in the 7 F 0 → 5 D 0 transition of Sm 2+ in BaFCl at 688 nm are reported and a probe pulse delay of 1.25 μ s was observed through a 5 mm thick crystal. This delay corresponds to a reduction of the group velocity v G of the transmitted light to ∼4000 m/s. An analysis of the dependence of the slow light effect on the probe pulse timing indicates some broadening of the spectral hole caused by relatively fast excitation energy transfer. We also demonstrate two-pulse (2PE) and (three-pulse) stimulated photon echoes (SPE) for the first time for Sm 2+ in the solid state and a homogenous linewidth of 16 kHz (∼2.5·10 −8 nm) was obtained at 1.8 K. The echoes in the optically dense medium were very efficient and revealed spectral diffusion on the 100- μ s time scale possibly due to flipping of the fluorine and chlorine nuclear spins in the environment of the Sm 2+ ions. Furthermore, the SPE also indicates relatively fast energy transfer, commensurate with the hole decay.

DOI
10.1364/oe.499613

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Slow light effects induced by transient spectral hole-burning in the 7 F 0 → 5 D 0 transition of Sm 2+ in BaFCl at 688 nm are reported and a probe pulse delay of 1.25 μ s was observed through a 5 mm thick crystal. This delay corresponds to a reduction of the group velocity v G of the transmitted light to ∼4000 m/s. An analysis of the dependence of the slow light effect on the probe pulse timing indicates some broadening of the spectral hole caused by relatively fast excitation energy transfer. We also demonstrate two-pulse (2PE) and (three-pulse) stimulated photon echoes (SPE) for the first time for Sm 2+ in the solid state and a homogenous linewidth of 16 kHz (∼2.5·10 −8 nm) was obtained at 1.8 K. The echoes in the optically dense medium were very efficient and revealed spectral diffusion on the 100- μ s time scale possibly due to flipping of the fluorine and chlorine nuclear spins in the environment of the Sm 2+ ions. Furthermore, the SPE also indicates relatively fast energy transfer, commensurate with the hole decay.
We report on the observation of slow light induced by transient spectral hole-burning in a solid, that is based on excited-state population storage. Experiments were conducted in the R1-line (2E←4A2 transition) of a 2.3 mm thick pink ruby (Al2O3:Cr(III) 130 ppm). Importantly, the pulse delay can be controlled by the application of a low external magnetic field B||c≤9 mT and delays of up to 11 ns with minimal pulse distortion are observed for ~55 ns Gaussian pulses. The delay corresponds to a group velocity value of ~c/1400. The experiment is very well modelled by linear spectral filter theory and the results indicate the possibility of using transient hole-burning based slow light experiments as a spectroscopic technique.
Systematic measurements of stimulated-photon-echo intensities as a function of the first-to-second (\ensuremath{\tau}) and second-to-third (T) pulse separations allow the investigation of the dynamical properties of the spectral diffusion for the 7^{7}7F0{\mathit{F}}_{0}F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathit{D}}_{0}D0​ transition of a cryogenic Eu3+{\mathrm{Eu}}^{3+}Eu3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ sample. The existence of spectral diffusion was verified by the significant broadening (from 1.2 to 7.2 kHz) of the homogeneous linewidth (\ensuremath{\Gamma}) as T increases from microseconds to milliseconds, the effect being attributed to the flip flop of nearby aluminum nuclear spins surrounding the Eu3+{\mathrm{Eu}}^{3+}Eu3+ ion. A similar broadening effect (from 0.61 kHz, to a few kHz) was also observed in the presence of a static magnetic field H0{\mathit{H}}_{0}H0​=137 G, but with a much slower diffusion rate. To explain these observations, we use three theoretical models: the Bai-Fayer model, the diffusion-equation model, and the Monte Carlo model. Each agrees reasonably well with the experimental data and indicates the flip rates of sub-kHz order at H0{\mathit{H}}_{0}H0​=0 and an order of magnitude lower at 137 G.
We report ultraslow group velocities of light in a solid. Light speeds as slow as 45 m/s were observed, corresponding to a group delay of 66 microsecond(s) in a 3-mm thick, optically dense crystal of Pr doped Y2SiO5. Reduction of the group velocity is accomplished by using a sharp spectral feature in absorption and dispersion that is produced by resonance Raman excitation of a ground-state spin coherence. Potential applications of slow and stopped light for the highly efficient storage and recall of optical data are discussed.
The $^{2}F_{7/2}\ensuremath{\leftrightarrow}^{2}F_{5/2}$ optical transitions of Yb3+\mathrm{Y}{\mathrm{b}}^{3+}Yb3+ doped into Y3Al5O12{\mathrm{Y}}_{3}\mathrm{A}{\mathrm{l}}_{5}{\mathrm{O}}_{12}Y3​Al5​O12​ (YAG) were studied for potential quantum information and photonic signal processing applications. Absorption and fluorescence spectroscopy located the energy levels of the ground 2F7/2^{2}F_{7/2}2F7/2​ and excited 2F5/2^{2}F_{5/2}2F5/2​ manifolds, allowing inconsistencies between previous assignments of crystal field splittings in the literature to be resolved. These measurements reveal an unusually large splitting between the first and second levels in both the ground and excited multiplets, potentially providing for reduced sensitivity to thermally induced decoherence and spin-lattice relaxation. Spectral hole burning through two-level saturation was observed, determining the excited state lifetime to be 860 \ensuremath{\mu}s and resolving ambiguities in previous fluorescence measurements that were caused by the large radiation trapping effects in this material. Optical decoherence measurements using two-pulse photon echoes gave a homogeneous linewidth of 18 kHz for an applied magnetic field of 1 T, narrowing to 5 kHz at 2.5 T. The observed decoherence was described by spectral diffusion attributed to $\mathrm{Y}{\mathrm{b}}^{3+}\mathrm{\ensuremath{-}}\mathrm{Y}{\mathrm{b}}^{3+}$ magnetic dipole interactions. Laser absorption determined an inhomogeneous linewidth of 3.6 GHz for this transition in this 0.05%-doped crystal, which is narrower than for any other rare-earth-ion transition previously studied in the YAG host. The temperature dependence of the transition energy and linewidth of the lowest 2F7/2^{2}F_{7/2}2F7/2​ to lowest 2F5/2^{2}F_{5/2}2F5/2​ transition centered at 968.571 nm measured from 4 K to 300 K was well described by phonon scattering at higher temperatures, with an additional anomalous linear temperature-dependent broadening at temperatures below 80 K. Two magnetically inequivalent subgroups of Yb3+\mathrm{Y}{\mathrm{b}}^{3+}Yb3+ ions were identified when a magnetic field was applied along the $\ensuremath{\langle}111\ensuremath{\rangle}$ axis, as expected for the D2{D}_{2}D2​ sites in the cubic symmetry crystal, with ground and excited state effective ggg-values of gg=3.40{g}_{\mathrm{g}}=3.40gg​=3.40 (3.34) and ge=1.04{g}_{\mathrm{e}}=1.04ge​=1.04 (2.01), respectively. Together with the convenient diode laser wavelength of this transition, our study suggests that Yb3+\mathrm{Y}{\mathrm{b}}^{3+}Yb3+:YAG is a promising material system for spectral hole burning and quantum information applications.
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.