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International Conference on Luminescence - 1984

Low Temperature Optical Dephasing of Rare Earth Ions by Tunneling Systems in Glass

Matthijs M. Broer

Published Jan 1, 1984• 1 citation
Publisher

Abstract

Optical dephasing of paramagnetic ions and molecules in organic and inorganic amorphous solids at low temperatures (≲100K) is characterized by unusual temperature dependences and enhanced relaxation rates compared to crystalline systems1. For a large variety of impurity-host combinations the dephasing rate has been found to follow a Tm temperature dependence with m approximately 2. Several theories have attempted to explain this behavior by assuming interactions between the optical center, phonons, and atomic tunneling systems. However, the role of the intrinsic disorder in optical dephasing in these systems is not clearly understood.

DOI
10.1364/icol.1984.wf1

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Optical dephasing of paramagnetic ions and molecules in organic and inorganic amorphous solids at low temperatures (≲100K) is characterized by unusual temperature dependences and enhanced relaxation rates compared to crystalline systems1. For a large variety of impurity-host combinations the dephasing rate has been found to follow a Tm temperature dependence with m approximately 2. Several theories have attempted to explain this behavior by assuming interactions between the optical center, phonons, and atomic tunneling systems. However, the role of the intrinsic disorder in optical dephasing in these systems is not clearly understood.
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.
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.
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.
Picosecond photon echo (PE) experiments are used to examine the optical dephasing and intermolecular interactions of organic chromophores in a variety of glassy organic and polymer hosts. The inherent disorder in these systems leads to dynamics which span times from picoseconds to hours and longer. The temperature dependent optical dephasing as measured by the PE follows a power law characteristic of tunnelling twolevel systems (TLS) at low temperatures (1 °K to 4 °K) and is exponentially activated at higher temperatures due to dephasing by additional modes. The nature of these modes will be addressed. These data and those from other line narrowing experiments such as hole burning allow the study both of fast dephasing processes and spectral diffusion due to slow fluctuations in the host. The observed lineshapes and holewidths require dipolar coupling between the chromophore and TLS and offer information on the distribution of relaxation rates. Furthermore, techniques sensitive to different timescales are used to examine host dynamics by removing the guest-host coupling from consideration. The data are discussed in conjunction with recently developed theoretical treatments of dephasing in disordered systems.
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.