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Physical review. B, Condensed matter

Stimulated-photon-echo spectroscopy. I. Spectral diffusion in Eu3+ : YAlO3

Ryuzi Yano, Masaharu Mitsunaga, Naoshi Uesugi

Published Jun 1, 1992• 26 citations
Publisher

Abstract

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}$${\mathit{F}}_{0}$${\mathrm{\ensuremath{-}}}^{5}$${\mathit{D}}_{0}$ transition of a cryogenic ${\mathrm{Eu}}^{3+}$:${\mathrm{YAlO}}_{3}$ 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 ${\mathrm{Eu}}^{3+}$ ion. A similar broadening effect (from 0.61 kHz, to a few kHz) was also observed in the presence of a static magnetic field ${\mathit{H}}_{0}$=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 ${\mathit{H}}_{0}$=0 and an order of magnitude lower at 137 G.

DOI
10.1103/physrevb.45.12752

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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}$${\mathit{F}}_{0}$${\mathrm{\ensuremath{-}}}^{5}$${\mathit{D}}_{0} 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.
Photon-echo-relaxation measurements made on the 3H4^{3}\mathrm{H}_{4}3H4​${\mathrm{\ensuremath{-}}}^{3}$P0{\mathrm{P}}_{0}P0​ transition of 0.01 at. % Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAG (where YAG represents yttrium aluminum garnet), 3H4^{3}\mathrm{H}_{4}3H4​${\mathrm{\ensuremath{-}}}^{1}$D2{\mathrm{D}}_{2}D2​ transition in 0.1 at. % Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​, and 7F0^{7}\mathrm{F}_{0}7F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathrm{D}}_{0}D0​ transition in 0.25 at. % Eu3+{\mathrm{Eu}}^{3+}Eu3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ show that the photon-echo relaxation rate increases when the intensities of the excitation pulses are increased. Although a part of the relaxation-rate increase in Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAG may be attributed to an instantaneous spectral diffusion (ISD) in which the presence of excited neighboring Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions change the local field and the absorption frequency of the rare-earth ions, our data deviate significantly from the ISD-model predictions. An additional intensity-dependent relaxation mechanism is required to explain the results.
Stimulated-photon-echo measurements as a function of both the first-to-second (\ensuremath{\tau}) and the second-to-third (T) pulse separations were conducted to study the echo-modulation behavior for the 3^{3}3H4{\mathit{H}}_{4}H4​${\mathrm{\ensuremath{-}}}^{1}$D2{\mathit{D}}_{2}D2​ transition of a cryogenic Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ sample. When T is shorter than the excited-state lifetime T1{\mathit{T}}_{1}T1​, deep echo modulations along both the \ensuremath{\tau} and T axes are observed, the frequencies of which correspond to the excited-state sublevel splittings. When T exceeds T1{\mathit{T}}_{1}T1​, the modulation is still observed, although only along the \ensuremath{\tau} axis. A density-matrix theory is developed in a perturbative manner to explain these coherent dynamical properties. The numerically simulated three-dimensional plots of the echo intensity versus \ensuremath{\tau} and T are presented, predicting quite satisfactorily the seemingly complicated experimental modulation patterns.
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
We have observed a significant ``instantaneous spectral diffusion'' phenomenon in photon-echo experiments on Tb3+{\mathrm{Tb}}^{3+}Tb3+:LiYF4{\mathrm{LiYF}}_{4}LiYF4​. This laser-induced effect makes observed optical dephasing rates intensity dependent and can also contribute a frequency dependence to the measured rates. A change in the magnetic dipole-dipole interaction between Tb3+{\mathrm{Tb}}^{3+}Tb3+ echo ions and surrounding Tb3+{\mathrm{Tb}}^{3+}Tb3+ ions occurs when surrounding ions are excited. This causes an instantaneous shift in the optical frequency of the echo ion that lasts for T1{\mathit{T}}_{1}T1​\ensuremath{\sim}1 msec. Frequency shifts caused by the first excitation pulse have no effect on echo rephasing (T1{\mathit{T}}_{1}T1​\ensuremath{\gg}T2{\mathit{T}}_{2}T2​), but those caused by the second pulse prevent proper echo rephasing. A summary is given of other ion-lattice and ion-ion interactions that can cause similar laser-induced effects in a wide variety of insulating compounds. There is potential for probing the nature of inhomogeneous broadening.
The mechanisms and effects of spectral diffusion for optical transitions of paramagnetic ions have been explored using the inhomogeneously broadened 1536 nm $^{4}\mathrm{I}_{15∕2}\ensuremath{\rightarrow}^{4}\mathrm{I}_{13∕2}$ transition in Er3+:Y2SiO5{\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Er3+:Y2​SiO5​. Using photon echo spectroscopy, spectral diffusion was measured by observing the evolution of the effective coherence lifetimes over time scales from $1\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ to 20 ms for magnetic-field strengths from 0.3 to 6.0 T, temperatures from 1.6 to 6.5 K, and nominal Er3+{\mathrm{Er}}^{3+}Er3+ concentrations of 0.0015%, 0.005%, and 0.02%. To understand the effect of spectral diffusion on material decoherence for different environmental conditions and material compositions, data and models were compared to identify spectral diffusion mechanisms and microscopic spin dynamics. Observations were successfully modeled by ${\mathrm{Er}}^{3+}\ensuremath{-}{\mathrm{Er}}^{3+}$ magnetic dipole interactions and Er3+{\mathrm{Er}}^{3+}Er3+ electron spin flips driven by the one-phonon direct process. At temperatures of 4.2 K and higher, spectral diffusion due to 89Y^{89}\mathrm{Y}89Y nuclear spin flips was also observed. The success in describing our extensive experimental results using simple models provides an important capability for exploring larger parameter spaces, accelerating the design and optimization of materials for spatial-spectral holography, and spectral hole-burning devices. The broad insight into spectral diffusion mechanisms and dynamics is applicable to other paramagnetic materials, such as those containing Yb3+{\mathrm{Yb}}^{3+}Yb3+ or Nd3+{\mathrm{Nd}}^{3+}Nd3+.
Linear- and nonlinear-optical properties of Eu3+:Y2SiO5 have been investigated. All the energy levels of the7F0,1,2,… ground-state manifold and the 5D0,1,2 excited-state manifold were identified, and they were found to be doubly structured because of the two inequivalent optical sites. Two absorption lines of the 7F0–5D0 transition were studied in detail by using nonlinear spectroscopic techniques, photon-echo and stimulated-photon-echo methods. It was found by the photon-echo measurement that the optical dephasing time for one site is extremely long and is excitation-intensity dependent. With the smallest possible intensity we observed the longest ever dephasing time in a solid, 822 μs, or a 387-Hz homogeneous linewidth. From the stimulated-photon-echo measurement, the linewidth was found to be constant over a wide range of time scales, implying the absence of spectral diffusion in this crystal. These quite advantageous properties of this crystal were used for the demonstration of two novel types of time-domain optical data readout: time- and frequency-domain hybrid optical memory and spectrally programmed coherent transients.