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Journal of the Physical Society of Japan

Optical Dephasing of Eu 3+ in Yttrium Oxide Crystals

Kiwan Jang, Il-Gon Kim, Sungtae Park

Published Nov 1, 1998• 1 citation
Publisher

Abstract

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.

DOI
10.1143/jpsj.67.3969

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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.
Two-pulse photon-echo measurements were made on the 7^{7}7F0{\mathit{F}}_{0}F0​${\mathrm{\ensuremath{\leftrightarrows}}}^{5}$D0{\mathit{D}}_{0}D0​ optical transition in a number of crystalline samples of Y2{\mathrm{Y}}_{2}Y2​O3{\mathrm{O}}_{3}O3​: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.
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.
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.
We study the optical properties of rare-earth-ion-doped inorganic crystals with an emphasis on the dependence of two-pulse photon echoes on the excitation density in the system. The experimental investigations concentrate on Pr3+{\mathrm{Pr}}^{3+}Pr3+:Nd3+{\mathrm{Nd}}^{3+}Nd3+:Eu3+{\mathrm{Eu}}^{3+}Eu3+ codoped Y2{\mathrm{Y}}_{2}Y2​SiO5{\mathrm{O}}_{5}O5​ and YAlO3{\mathrm{O}}_{3}O3​ crystals at low temperatures. With two pulses of one laser the echo is induced in one ion species and with a third, "scrambler" pulse of a second laser another species is excited. These scrambler excitations lead to a dephasing and thus to an echo attenuation which depends on the strength, frequency, and time of the scrambler pulse. The spectral sensitivity of the echo attenuation is used for a spectroscopic technique: "photon-echo attenuation spectroscopy." As a function of the delay time ts{t}_{s}ts​ between the scrambler pulse and the onset of the two-pulse echo sequence the attenuation shows a very specific behavior dictated by the excitation-induced frequency shifts (EFS's). For ts{t}_{s}ts​ between the two echo-inducing pulses the echo intensity is partially regained by the "dephasing-rephasing balancing" of the reversible EFS's. For the theoretical description a stochastic model is introduced and the dephasing by excitation-induced lattice vibrations and by EFS's are analyzed in detail. The present results are discussed in the light of previous experimental and theoretical investigations.
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.
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.