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Physical review. B, Condensed matter

Sample-dependent optical dephasing in bulk crystalline samples of Y2 O3 : Eu3+

G.P. Flinn, Kiwan Jang, Joseph Ganem, Michieal L. Jones, Richard S. Meltzer, R. M. Macfarlane

Published Mar 1, 1994• 55 citations
Publisher

Abstract

Two-pulse photon-echo measurements were made on the $^{7}$${\mathit{F}}_{0}$${\mathrm{\ensuremath{\leftrightarrows}}}^{5}$${\mathit{D}}_{0}$ optical transition in a number of crystalline samples of ${\mathrm{Y}}_{2}$${\mathrm{O}}_{3}$:${\mathrm{Eu}}^{3+}$ prepared by three different crystal-growth techniques. For crystals prepared by a laser-heated pedestal growth or arc-imaging furnace process, we report the observation of an additional sample-dependent contribution to the optical dephasing in comparison with a crystal grown by flame fusion. The dephasing rate 1/${\mathit{T}}_{\mathit{m}}$ at 1.4 K is up to two orders of magnitude faster than that previously reported for the flame-fusion-grown crystal, and is uncorrelated with concentration. Measurements up to 14 K show that 1/${\mathit{T}}_{\mathit{m}}$ increases linearly with temperature, in contrast to the expected ${\mathit{T}}^{7}$ behavior due to a two-phonon Raman process. The linear temperature dependence is similar to that seen in glasses and disordered crystalline systems, suggesting the presence of disorder in the samples with more rapid dephasing. The crystals were examined by x-ray diffraction, excitation spectroscopy, and near-field optical microscopy to provide information on the nature of the disorder. The effect of annealing on the crystal dynamics is also investigated.

DOI
10.1103/physrevb.49.5821

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We identify and analyze dephasing mechanisms that broaden the optical transitions of rare-earth ions in randomly oriented transparent ceramics. The study examines the narrow $^{7}F_{0}\phantom{\rule{4pt}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{4pt}{0ex}}^{5}D_{0}$ transition of ${\mathrm{Eu}}^{3+}$ dopants in a series of ${\mathrm{Y}}_{2}{\mathrm{O}}_{3}$ ceramic samples prepared under varying conditions. We characterize the temperature and magnetic field dependence of the homogeneous linewidth, as well as long-term spectral diffusion on time scales up to 1 s. The results highlight significant differences between samples with differing thermal treatments and ${\mathrm{Zr}}^{4+}$ additive concentrations. In particular, several distinct magnetic interactions from defect centers are observed, which are clearly distinguished from the broadening due to interactions with two-level systems and phonons. By minimizing the broadening due to the different defect centers, linewidths of the order of 4 kHz are achieved for all samples. The linewidths are limited by temperature-dependent interactions and by an interaction that is yet to be identified. Although the homogeneous linewidth can be narrowed further in these ceramic samples, the broadening is now comparable to the linewidths achieved in rare-earth-ion--doped single crystals. Thus, this work emphasizes the usefulness of studying ceramics to gain insights into dephasing mechanisms relevant to single crystals and suggests that ceramics may be an interesting alternative for applications in classical and quantum information processing.

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Two-pulse photon-echo measurements were made on the ^{7}$${\mathit{F}}_{0}$${\mathrm{\ensuremath{\leftrightarrows}}}^{5}$${\mathit{D}}_{0} optical transition in a number of crystalline samples of {\mathrm{Y}}_{2}$${\mathrm{O}}_{3}:Eu3+{\mathrm{Eu}}^{3+}Eu3+ prepared by three different crystal-growth techniques. For crystals prepared by a laser-heated pedestal growth or arc-imaging furnace process, we report the observation of an additional sample-dependent contribution to the optical dephasing in comparison with a crystal grown by flame fusion. The dephasing rate 1/Tm{\mathit{T}}_{\mathit{m}}Tm​ at 1.4 K is up to two orders of magnitude faster than that previously reported for the flame-fusion-grown crystal, and is uncorrelated with concentration. Measurements up to 14 K show that 1/Tm{\mathit{T}}_{\mathit{m}}Tm​ increases linearly with temperature, in contrast to the expected T7{\mathit{T}}^{7}T7 behavior due to a two-phonon Raman process. The linear temperature dependence is similar to that seen in glasses and disordered crystalline systems, suggesting the presence of disorder in the samples with more rapid dephasing. The crystals were examined by x-ray diffraction, excitation spectroscopy, and near-field optical microscopy to provide information on the nature of the disorder. The effect of annealing on the crystal dynamics is also investigated.
Optical dephasing in a number of crystalline samples of Y 2 O 3 : Eu 3+ prepared by two different crystal-growth techniques were measured using two pulse photon echo method. For crystals prepared by a laser-heated pedestal growth, we report the dephasing rate, 1/ T m , at 1.4 K is up to two orders of magnitude faster than that previuosly reported for the flame fusion growth crystal. The spatial dependence of the optical dephasing rate, measured by TPPE (two-pulse photon echo), tells that the environments of echo producing ions at least highly depend on the spatial position which can not be detected by conventional laser spectroscopy techniques, suggesting two-pulse photon echo experiment can be served as a tool for probing the uniformity of the samples.
Optical hole burning is used to study optical dephasing of the 7F0 ⇒ 5D0 transition in samples of Y2O3:Eu3+ grown by both flame fusion and laser-heated pedestal growth. The samples exhibited a wide variation in their low-temperature hole widths, and the measured hole linewidths were in reasonable agreement with homogeneous linewidths obtained from values of T2 that were determined with two-pulse photon echoes. The sample that had the longest value of T2 (510 μs) from the echo measurements gave a hole width of 3.5 kHz. This is believed to be the narrowest spectral feature observed directly in the frequency domain for a solid. Other samples produced wider holes that were not correlated with the Eu3+ impurity concentrations. Time-resolved hole burning in one of the samples showed a slow and continuous broadening of the spectral hole from 130 kHz at 3 ms to 900 kHz at 10 s after hole burning. It is suggested that the additional broadening is associated with some form of disorder modes in this ordered crystalline solid.
The role of disorder on the inhomogeneous and homogeneous linewidths of Eu3+{\mathrm{Eu}}^{3+}Eu3+ in single crystals with various degrees of disorder is described for samples grown by LHPG (laser-heated pedestal growth). Emission spectra, hole-burning spectra, and results of the two-pulse photon echo are reported for ${\mathrm{Y}}_{2\mathrm{\ensuremath{-}}\mathit{x}}$Scx{\mathrm{Sc}}_{\mathit{x}}Scx​O3{\mathrm{O}}_{3}O3​ (x=0.04,0.3,1) and YSZ (yttria-stabilized zirconia). For the ${\mathrm{Y}}_{2\mathrm{\ensuremath{-}}\mathit{x}}$Scx{\mathrm{Sc}}_{\mathit{x}}Scx​O3{\mathrm{O}}_{3}O3​ system, the inhomogeneous linewidths increase with x while the homogeneous linewidths are nearly independent of x. Dynamics associated with low-frequency excitations observed previously in x=0 LHPG samples are nearly absent for x>0. However, both the static and dynamic properties of YSZ show behavior which is characteristic of amorphous systems like silicate glass.
We have employed spectral-hole-burning, coherent-transient, and optical-rf double-resonance techniques to measure various parameters associated with the 580.8-nm 7F0^{7}\mathrm{F}_{0}7F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathrm{D}}_{0}D0​ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ doped into Y2{\mathrm{Y}}_{2}Y2​O3{\mathrm{O}}_{3}O3​. In particular, we have measured the hyperfine splittings of the terminal levels (for both 151Eu^{151}\mathrm{Eu}151Eu and 153Eu^{153}\mathrm{Eu}153Eu), an effective thermalization rate of the ground-state (7{(}^{7}(7F0{\mathrm{F}}_{0}F0​) hyperfine manifold over the temperature range of \ensuremath{\simeq}4--15 K, and the homogeneous linewidth of the optical transition over the range of \ensuremath{\simeq}14--35 K. Large ratios of inhomogeneous to homogeneous linewidth at elevated temperatures (103{10}^{3}103 at 25 K) and long ground-state hyperfine thermalization times (>30 h at 4 K) make this an interesting crystal in the context of spectrally addressable optical memories.
Detailed site-selective spectroscopy has been performed as a function of temperature on the ${}^{7}{F}_{0}{\ensuremath{\leftrightarrow}}^{5}{D}_{0}$ transition of Eu3+:Y2SiO5{\mathrm{Eu}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Eu3+:Y2​SiO5​ for Eu3+{\mathrm{Eu}}^{3+}Eu3+ concentrations of 0.02%, 0.1%, 0.5%, and 1%. Time-domain optical dephasing, spectral hole lifetimes, anisotropic absorption coefficients, inhomogeneous linewidths, and fluorescence lifetimes for Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions at both crystallographic sites were measured. The temperature dependence of the optical dephasing, transition energy, and linewidth of the ${}^{7}{\stackrel{\ensuremath{\rightarrow}}{{F}_{0}}}^{5}{D}_{0}$ absorption was measured and interpreted in terms of Raman scattering of phonons. Photon echo measurements of optical dephasing gave T2{T}_{2}T2​ values as long as 2.6 ms, approaching the limit set by the fluorescence decay time. Spectral hole lifetimes were measured for temperatures from 2 K to 18 K, with observed lifetimes varying from 1 s at 18 K to an estimated value of greater than 20 days at 2 K. Anisotropic absorption coefficients were measured, and an increase in Eu3+{\mathrm{Eu}}^{3+}Eu3+ concentration from 0.02% to 7% produced an increase in the inhomogeneous linewidth ${\ensuremath{\Gamma}}_{\mathrm{inh}}$ from 0.5 GHz to \ensuremath{\sim}150 GHz, indicating that Eu3+{\mathrm{Eu}}^{3+}Eu3+ doping induces significant strain in the crystal. New determinations of many energy levels of 7FJ{}^{7}{F}_{J}7FJ​ multiplets have been made for J=0J=0J=0 to 6.
We identify and analyze dephasing mechanisms that broaden the optical transitions of rare-earth ions in randomly oriented transparent ceramics. The study examines the narrow $^{7}F_{0}\phantom{\rule{4pt}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{4pt}{0ex}}^{5}D_{0}$ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ dopants in a series of Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Y2​O3​ ceramic samples prepared under varying conditions. We characterize the temperature and magnetic field dependence of the homogeneous linewidth, as well as long-term spectral diffusion on time scales up to 1 s. The results highlight significant differences between samples with differing thermal treatments and Zr4+{\mathrm{Zr}}^{4+}Zr4+ additive concentrations. In particular, several distinct magnetic interactions from defect centers are observed, which are clearly distinguished from the broadening due to interactions with two-level systems and phonons. By minimizing the broadening due to the different defect centers, linewidths of the order of 4 kHz are achieved for all samples. The linewidths are limited by temperature-dependent interactions and by an interaction that is yet to be identified. Although the homogeneous linewidth can be narrowed further in these ceramic samples, the broadening is now comparable to the linewidths achieved in rare-earth-ion--doped single crystals. Thus, this work emphasizes the usefulness of studying ceramics to gain insights into dephasing mechanisms relevant to single crystals and suggests that ceramics may be an interesting alternative for applications in classical and quantum information processing.