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Journal of Nanoscience and Nanotechnology

Optical Dephasing of Triply Ionized Rare Earths in Transparent Glass Ceramics Containing LaF 3 Nanocrystals

Hairong Zheng, Xiangyu Zhang, Dangli Gao, Richard S. Meltzer

Published Mar 1, 2008• 1 citation
Publisher

Abstract

Optical dephasing of Pr3+ and Tm3+ ions doped in transparent oxyfluoride glass ceramics was studied with the two-pulse photon echo technique. It was found that the dephasing time of rare earth ions is dramatically less in nanocrystals embedded in a glass matrix than in bulk crystals. A quasi-linear temperature dependence obtained at low temperatures proved that the long-range interaction of the ions inside the nanocrystals with the two level systems of the glass matrix dominates the optical dephasing. The local thermal effect in glass ceramics containing nanocrystals elevates the local temperature, which results in the reduction of optical dephasing time. For Tm(3+)-doped glass ceramics, the elevation of local temperature induced by the irradiation of excitation laser even quenched the photon echo signals in the experimental study.

DOI
10.1166/jnn.2008.18174

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Optical dephasing of Pr3+ and Tm3+ ions doped in transparent oxyfluoride glass ceramics was studied with the two-pulse photon echo technique. It was found that the dephasing time of rare earth ions is dramatically less in nanocrystals embedded in a glass matrix than in bulk crystals. A quasi-linear temperature dependence obtained at low temperatures proved that the long-range interaction of the ions inside the nanocrystals with the two level systems of the glass matrix dominates the optical dephasing. The local thermal effect in glass ceramics containing nanocrystals elevates the local temperature, which results in the reduction of optical dephasing time. For Tm(3+)-doped glass ceramics, the elevation of local temperature induced by the irradiation of excitation laser even quenched the photon echo signals in the experimental study.
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.
A detailed description is presented of photon echo experiments in Nd3+{\mathrm{Nd}}^{3+}Nd3+-doped silica optical fibers at temperatures below 1 K. Dephasing rates ${T}_{2}^{\mathrm{\ensuremath{-}}1}$ have been obtained from two-pulse echo sequences at 0.89 \ensuremath{\mu}m and are found to follow a T1.3{T}^{1.3}T1.3 temperature dependence. An interpretation of this result is presented which invokes the interaction of tunneling systems with the optical ions via a dipole-dipole elastic interaction. The dynamics of the interaction originates in a spectral diffusion process and three pulse stimulated echo experiments confirm this interpretation.
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.
We present a theoretical scheme for laser cooling in Tm3+-doped oxy-fluoride glass ceramic (GC). Tm3+-doped GC has a unique combination of high chemical and mechanical stability related to the oxide glass and low phonon energy of the fluoride nanocrystals, which trap a majority of Tm3+ ions. This unique property of GC makes it attractive for a number of applications. The effective embedding of rare-earth ions in the crystalline phase with low phonon energy provides high quantum efficiency for the F43→H63 transition in the Tm3+ ions participating in the cooling cycle.
A theoretical description of the temperature-dependent dephasing rate of rare-earth ions in glass is given for temperatures T<1T<1T<1 K. The model invokes elastic dipole-dipole interactions between the rare-earth ions and atomic tunneling systems. The calculation explains features of a recent photon-echo experiment on SiO2{\mathrm{O}}_{2}O2​:Nd3+{\mathrm{Nd}}^{3+}Nd3+, namely, the magnitude and T1.3{T}^{1.3}T1.3 dependence of the dephasing rate.