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Physical review. B, Condensed matter

Systematic control of spectral hole burning and homogeneous linewidth by disorder in Y2O3:Pr3+ crystalline systems

Tsuyoshi Okuno, Tohru Suemoto

Published Apr 1, 1999• 14 citations
Publisher

Abstract

We investigated the hole-burning phenomena and homogeneous linewidth in ${\mathrm{Pr}}^{3+}$-doped ${\mathrm{Y}}_{2}{\mathrm{O}}_{3}$-based crystals under the systematic control of disorder in the crystal. When divalent ions are doped into an ${\mathrm{Y}}_{2}{\mathrm{O}}_{3}{:\mathrm{P}\mathrm{r}}^{3+}$ crystal, holes due to rearrangement of local structure around ${\mathrm{Pr}}^{3+}$ ions are burned. The burning curves are successfully analyzed in terms of a distributed tunneling rate model for hole formation. The burning efficiency from this analysis and the homogeneous linewidth become larger as the crystal includes a larger amount of divalent ions. The interaction of ${\mathrm{Pr}}^{3+}$ ions with oxygen vacancies is thought to be one of the origins of the hole production and the line broadening. The interaction length between ${\mathrm{Pr}}^{3+}$ ions and oxygen vacancies is discussed.

DOI
10.1103/physrevb.59.9078

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We investigated the hole-burning phenomena and homogeneous linewidth in Pr3+{\mathrm{Pr}}^{3+}Pr3+-doped Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Y2​O3​-based crystals under the systematic control of disorder in the crystal. When divalent ions are doped into an Y2O3:Pr3+{\mathrm{Y}}_{2}{\mathrm{O}}_{3}{:\mathrm{P}\mathrm{r}}^{3+}Y2​O3​:Pr3+ crystal, holes due to rearrangement of local structure around Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions are burned. The burning curves are successfully analyzed in terms of a distributed tunneling rate model for hole formation. The burning efficiency from this analysis and the homogeneous linewidth become larger as the crystal includes a larger amount of divalent ions. The interaction of Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions with oxygen vacancies is thought to be one of the origins of the hole production and the line broadening. The interaction length between Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions and oxygen vacancies is discussed.
Persistent spectral hole-burning is extensively studied in many materials. In inorganic materials doped with rare earth ions, we have mainly two mechanisms for hole-burning; one is optical pumping to hyperfine sublevels in rare earth ions, and the other is optically induced rearrangement of local structure around optical centers. In crystals we often observe the hole due to the former mechanism while the hole due to the latter is reported mainly in glasses. Up to now, there seems to be only little study about the correlation between the mechanism of hole-burning and sample-quality or defects. Recently we reported that the character of holes in Y2O3:Pr3+ depends on the quality of samples [1]. In this paper we study the origin of these holes in Y2O3 with a well-controlled manner. For this purpose, we applied hole-burning spectroscopy to various Y2O3:Pr3+(0.2mol%) samples doped with other metallic ions.
Due to their narrow homogeneous linewidths, rare-earth ions in inorganic crystals at low temperatures have recently been given considerable attention as test materials for experiments in coherent quantum optics. Because these narrow linewidth transitions have been buried in a wide inhomogeneous line, the scope of experiments that could be carried out in these materials has been limited. However, here we present spectroscopic techniques, based on spectral hole burning and optical pumping, which allow hyperfine transitions that are initially buried within an inhomogeneously broadened absorption line to be studied with no background absorption from other transitions. A sequence of hole-burning pulses is used to isolate selected transitions between hyperfine levels, which makes it possible to directly study properties of the transitions, e.g., transition strengths, and gives access to information that is difficult to obtain in standard hole-burning spectroscopy, such as the ordering of hyperfine levels. The techniques introduced are applicable to absorbers in a solid with long-lived sublevels in the ground state and where the homogeneous linewidth and sublevel separations are smaller than the inhomogeneous broadening of the optical transition. In particular, this includes rare-earth ions doped into inorganic crystals and in the present work the techniques are demonstrated in spectroscopy of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​. Information on the hyperfine structure and relative transition strengths of the $^{3}H_{4}\text{\ensuremath{-}}^{1}D_{2}$ hyperfine transitions in Pr3+:Y2SiO5{\mathrm{Pr}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Pr3+:Y2​SiO5​ has been obtained from frequency-resolved absorption measurements, in combination with coherent and incoherent driving of the transitions.
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.
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 persistent spectral hole-burning phenomenon was investigated for Sm2+ ions-doped Al2O3-SiO2 glasses prepared by the sol-gel method. The efficiency of hole-burning, burned at low temperature ~77K, was proportionally increased with the content of OH groups surrounding the rare-earth ions. The proposed mechanism for hole-burning was the optically activated rearrangement of the OH bonds surrounding the rare-earth ions. The burned-hole was thermally refilled and erased above ~200 K. On the other hand, the glasses obtained by heating in H2 gas or irradiating with x-rays showed PSHB up to room temperature. When heated in H2 gas, the H2 molecules react with oxygen ions to form H2O. Removal of the generated H2O causes the number of oxygen ions surrounding rare-earth ions to decrease, resulting into the reduction of the ions. The hole burning in the H2-treated glasses was performed by the electron transfer between the rare-earth ions and the trapping centers. In contrast, in the x-ray irradiated glass, it was concluded that the rear-earth ions are deuced into the divalent state by electron transfer from the oxygen defect center. The hole defect centers are trapped in oxygen ions bound with Al3+ ions. The spectral hole burning of the x-ray irradiated glasses could be burned by the reverse reaction of the reduction of the rare-earth ions. A short distance between the Sm2+ and oxygen defect centers brought a high-speed hole burning, that is, 30 times faster than in a similar H2 gas treated glass.
Photon gated spectral hole-burning was first observed in a samarium doped crystal, BaFCl:Sm2+ [1]. This material was of interest to the developement of optical memories as the holes were found to be stable to room temperature thermal cycling. Holes could be burnt at liquid helium temperatures but as the temperature was raised the line quickly became homogeneously broadened. The addition of bromine to the melt succeeded in broadening the inhomogeneous linewidths to about 2 nm through substitutional disorder [2] and persistent holes were observed at 77 K [3]. Subsequently, a study of the parameters for spectral hole-burning in a BaFCl0.5Br0.5:Sm2+ crystalline powder was performed [4] and the highest temperature for which persistent hole-burning had been observed was raised to 133 K. Here we report spectral hole-burning at room temperature (figure 1) in a related compound, Sr0.5Mg0.5FCl0.5Br0.5:Sm2+.