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Physical Review Letters

Ultraslow optical dephasing in Eu 3 + : Y 2 SiO 5

Randy W. Equall, Yazhou Sun, R. L. Cone, R. M. Macfarlane

Published Apr 4, 1994• 257 citations
Publisher

Abstract

We report the measurement of what we believe to be the narrowest known optical resonance in a solid. This was made on the $^{7}$${\mathit{F}}_{0}$${\ensuremath{\rightarrow}}^{5}$${\mathit{D}}_{0}$ transition of ${\mathrm{Eu}}^{3+}$:${\mathrm{Y}}_{2}$${\mathrm{SiO}}_{5}$ at 1.4 K using photon echoes with sufficiently low laser power to almost eliminate contributions from instantaneous diffusion. The optical resonance widths measured for ${\mathrm{Eu}}^{3+}$ ions in the two crystallographic sites of ${\mathrm{Y}}_{2}$${\mathrm{SiO}}_{5}$ and in a magnetic field of 100 G are 122 Hz (site 1) and 167 Hz (site 2). These widths are dominated by population decay, but up to 20 Hz is attributed to $^{89}\mathrm{Y}$ spin fluctuations which have been reduced by the applied magnetic field.

DOI
10.1103/physrevlett.72.2179

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Contributions to the homogeneous linewidth of the $^{3}$${\mathit{H}}_{4}$(1)${\ensuremath{\rightarrow}}^{1}$${\mathit{D}}_{2}$(1) transition for the two crystallographic sites of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{2}$${\mathrm{SiO}}_{5}$ have been investigated using photon echoes. The effects of excitation-intensity-dependent dephasing or instantaneous diffusion were systematically studied to allow accurate determination of the optical resonance widths. Homogeneous linewidths of 2.8 kHz (site 1) and 1 kHz (site 2) were measured with no applied magnetic field and with sufficiently low laser intensity to minimize the effects of instantaneous diffusion. Using the same excitation intensity, widths of 2.1 kHz (site 1) and 0.85 kHz (site 2) were obtained with an applied magnetic field of 77 G, demonstrating a significant contribution of $^{89}\mathrm{Y}$ nuclear-spin fluctuations to the zero-field homogeneous linewidth. Extrapolation to zero excitation intensity yielded optical resonance widths that were only slightly narrower than the measured values. Optically detected nuclear magnetic resonance measurements determined the hyperfine structure of the $^{3}$${\mathit{H}}_{4}$ ground state for each site; the hyperfine levels of the lowest component of the $^{1}$${\mathit{D}}_{2}$ manifold for each site were determined using photon echo nuclear double resonance. The relatively large oscillator strength of 3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}7}$ for a rare-earth ion, in conjunction with long dephasing times makes this material a useful candidate for demonstration of time-domain signal processing and optical data storage.

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The optical spectroscopy and dynamics of three materials; Eu^3+:Y2SiO5, Pr^3+:Y2SiO5, and Tm^3+:Y2SiO5 that are of interest for application in persistent spectral holeburning optical memory and signal processing devices were investigated using linear and nonlinear spectroscopic techniques.Two-pulse photon echoes have been used to measure the homogeneous linewidths.The effects of instantaneous spectral diffusion were systematically studied to allow accurate determination of the optical resonance widths, and external magnetic fields were applied to characterize the effects of fluctuating nuclear spins of the host lattice on dephasing of the dopant ion.The 7F0 → 5D0 transition of 0.1% Eu^3+ in the two crystallographic sites of Y2SiO5 was studied using photon echoes.Using this material, we succeeded in measuring the narrowest optical resonance in a solid by shielding the crystal from stray electromagnetic fields and using sufficiently low laser power to minimize contributions from instantaneous diffusion.The homogeneous linewidths measured in a magnetic field of 100 G are 122 Hz (site 1) and 167 Hz (site 2).These widths are dominated by population decay, but up to 20 Hz is attributed to 89Y spin fluctuations which have been reduced by the applied magnetic field.Similar studies were performed to determine the contributions to the homogeneous linewidth of the 3H4(1) → 1D2(1) transition for both sites of 0.02% Pr^3+ in Y2SiO5.Linewidths of 2.1 kHz (site 1) and 0.85 kHz (site 2) were obtained with an applied magnetic field of 77 G.A significant contribution of 89Y nuclear spin fluctuations to the zero-field homogeneous linewidth was found.Optically detected nuclear magnetic resonance measurements determined the hyperfine structure of the 3H4 ground state for each site, and photon echo nuclear double resonance was used to determine the hyperfine levels of the lowest component of the 1D2 manifold. 3) 2.1? Ec,2S

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Optics Letters•Dec 1, 1991•125 citations
We report the measurement of what we believe to be the narrowest known optical resonance in a solid. This was made on the ^{7}$${\mathit{F}}_{0}$${\ensuremath{\rightarrow}}^{5}$${\mathit{D}}_{0} transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+:{\mathrm{Y}}_{2}$${\mathrm{SiO}}_{5} at 1.4 K using photon echoes with sufficiently low laser power to almost eliminate contributions from instantaneous diffusion. The optical resonance widths measured for Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions in the two crystallographic sites of {\mathrm{Y}}_{2}$${\mathrm{SiO}}_{5} and in a magnetic field of 100 G are 122 Hz (site 1) and 167 Hz (site 2). These widths are dominated by population decay, but up to 20 Hz is attributed to 89Y^{89}\mathrm{Y}89Y spin fluctuations which have been reduced by the applied magnetic field.
Contributions to the homogeneous linewidth of the 3^{3}3H4{\mathit{H}}_{4}H4​(1)${\ensuremath{\rightarrow}}^{1}$D2{\mathit{D}}_{2}D2​(1) transition for the two crystallographic sites of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in Y2{\mathrm{Y}}_{2}Y2​SiO5{\mathrm{SiO}}_{5}SiO5​ have been investigated using photon echoes. The effects of excitation-intensity-dependent dephasing or instantaneous diffusion were systematically studied to allow accurate determination of the optical resonance widths. Homogeneous linewidths of 2.8 kHz (site 1) and 1 kHz (site 2) were measured with no applied magnetic field and with sufficiently low laser intensity to minimize the effects of instantaneous diffusion. Using the same excitation intensity, widths of 2.1 kHz (site 1) and 0.85 kHz (site 2) were obtained with an applied magnetic field of 77 G, demonstrating a significant contribution of 89Y^{89}\mathrm{Y}89Y nuclear-spin fluctuations to the zero-field homogeneous linewidth. Extrapolation to zero excitation intensity yielded optical resonance widths that were only slightly narrower than the measured values. Optically detected nuclear magnetic resonance measurements determined the hyperfine structure of the 3^{3}3H4{\mathit{H}}_{4}H4​ ground state for each site; the hyperfine levels of the lowest component of the 1^{1}1D2{\mathit{D}}_{2}D2​ manifold for each site were determined using photon echo nuclear double resonance. The relatively large oscillator strength of 3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}7}$ for a rare-earth ion, in conjunction with long dephasing times makes this material a useful candidate for demonstration of time-domain signal processing and optical data storage.
The optical spectroscopy and dynamics of three materials; Eu^3+:Y2SiO5, Pr^3+:Y2SiO5, and Tm^3+:Y2SiO5 that are of interest for application in persistent spectral holeburning optical memory and signal processing devices were investigated using linear and nonlinear spectroscopic techniques.Two-pulse photon echoes have been used to measure the homogeneous linewidths.The effects of instantaneous spectral diffusion were systematically studied to allow accurate determination of the optical resonance widths, and external magnetic fields were applied to characterize the effects of fluctuating nuclear spins of the host lattice on dephasing of the dopant ion.The 7F0 → 5D0 transition of 0.1% Eu^3+ in the two crystallographic sites of Y2SiO5 was studied using photon echoes.Using this material, we succeeded in measuring the narrowest optical resonance in a solid by shielding the crystal from stray electromagnetic fields and using sufficiently low laser power to minimize contributions from instantaneous diffusion.The homogeneous linewidths measured in a magnetic field of 100 G are 122 Hz (site 1) and 167 Hz (site 2).These widths are dominated by population decay, but up to 20 Hz is attributed to 89Y spin fluctuations which have been reduced by the applied magnetic field.Similar studies were performed to determine the contributions to the homogeneous linewidth of the 3H4(1) → 1D2(1) transition for both sites of 0.02% Pr^3+ in Y2SiO5.Linewidths of 2.1 kHz (site 1) and 0.85 kHz (site 2) were obtained with an applied magnetic field of 77 G.A significant contribution of 89Y nuclear spin fluctuations to the zero-field homogeneous linewidth was found.Optically detected nuclear magnetic resonance measurements determined the hyperfine structure of the 3H4 ground state for each site, and photon echo nuclear double resonance was used to determine the hyperfine levels of the lowest component of the 1D2 manifold. 3) 2.1? Ec,2S
Eu-doped yttrium orthosilicate (Eu(3+) : Y2SiO5) had been a subject being investigated for coherent time-domain optical memory and information processing applications since its ultraslow optical dephasing was discovered several years ago. In this crystal the weakly allowed (7)F0 - (5)D0 transition of europium ions exhibits a sufficient long dephasing time and no spectral difli.usion on a time scale of several hours at low temperature, thus an information pattern or data can be stored as a population grating in the ground state hyperfine levels. On the other hand, the study on photon-echo relaxation shows that the dephasing time T2 of Eu (3+) and other rare-earth ions doped YAG, YAlO3 strongly depends on the intensity of the excitation pulses. In Eu (3+) :YAlO3, an exponential decay of photon-echo with T2 = 53 microseconds if the excitation pulses are weak (5 vJ/pulse) was observed. However, when the excitation pulses are strong (80 pJ/pulse) they observed a much shortened T2 with a highly nonexponential decay pattern. The conclusion they derived is that the intensity-dependent dephasing rate effects are quite general, and it depends on how much the excitation intensity varies. In this paper we use transient grating formation technique showing that a temporal lattice distortion may only occur along crystal c axis, caused by EU (3+) excitation. At high excitation level the produced exciton in conduction band may also couple to the dynamical lattice relaxation process, giving rise to an apparently much shortened dephasing time.
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.
Working on the 7F0^{7}\mathrm{F}_{0}7F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathrm{D}}_{0}D0​ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ in Y2{\mathrm{Y}}_{2}Y2​O3{\mathrm{O}}_{3}O3​, we provide the first detailed characterization of excitation-induced shifts in optical transition frequencies and demonstrate their exaggeration of nominally homogeneous dephasing rates. The shifts (found to vary in rough proportion to the number of Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions excited and to be as small as one part in 1012{10}^{12}1012) were identified through their unique signature in specially designed photon-echo experiments. The effects reported may constitute a rather general complication in optical measurements of homogeneous relaxation rates in solids.
We report what is to our knowledge the first measurement of linear and nonlinear spectroscopic properties for the (7)F(0)-(5)D(0) transition of Eu(3+):Y(2)SiO(5). Two clearly resolved lines at 579.879 and 580.049 nm, stemming from different sites, show dissimilar photoluminescence and hole spectra. In addition, these two sites have different inhomogeneous and homogeneous linewidths, which suggests that the local-field effect is smaller for one site. Specifically, the less affected site exhibits the longest dephasing time (822 micros) of any solid, which corresponds to a homogeneous linewidth of 387 Hz, and this linewidth is found to persist for hours without apparent spectral diffusion.