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Acta Physica Sinica

THEORETICAL STUDY OF NON-EXPONENTIAL PHOTON ECHO DECAYS

WANG HAI-YU, Huang Shi-Hua, 中国科学院长春物理研究所激发态物理开放实验室

Published Jan 1, 1997• 0 citations
Publisher

Abstract

Photon echo decays of several impurity paramagnetic ions are calculated,the historical average of each lattice nuclear spin flip is described by a bivalued random telegraph process,and the spatial average is obtained according to the crystal structure. The results are very close to those of Monte Carlo simulations. From the experimental observations,we obtained that all samples have a universal decay form.

DOI
10.7498/aps.46.1108

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Flip-flop processes due to magnetic dipole-dipole interaction between neighboring ions in crystals doped by rare-earth ions are one of the mechanisms of relaxation between hyperfine levels. Modeling of this mechanism has so far been macroscopic, characterized by an average rate describing the relaxation of all ions. Here, however, we present a microscopic model of flip-flop interactions between individual nuclear spins of dopant ions. Every ion is situated in a unique local environment in the crystal, where each ion has different distances and a unique orientation relative to its nearest neighbors, as determined by the lattice structure. Thus each ion has a unique flip-flop rate and the collective relaxation dynamics of all ions in a bulk crystal is a sum of many exponential decays, giving rise to a distribution of rates rather than a single average decay rate. We employ this model to calculate flip-flop rates in Pr3+{\mathrm{Pr}}^{3+}Pr3+:Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ and show experimental measurements of population decay of the ground state hyperfine levels at $\ensuremath{\sim}2$ K. We also present a method to measure rates of individual transitions from hole burning spectra that requires significantly fewer fitting parameters in theoretical rate equations compared to earlier work. Furthermore, we measure the effect of external magnetic field on the flip-flop rates and observe that the rates slow down by two orders of magnitude in a field of 5--10 mT.
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We investigate a mechanism responsible for the observed very short times of the photon-echo decay (of the order of a few femtoseconds) in semiconductors. It is associated with the loss of phase memory as a result of the interaction of the interband mixed state with an unscreened random Coulomb potential of the photocarriers and/or charged impurities. A time characteristic of a system of interacting electrons is found. This is the time of phase breaking ${\mathrm{\ensuremath{\tau}}}_{\mathit{c}\mathit{p}\mathit{h}\mathit{i}}$, which we calculate within the eikonal approximation using diagrammatic techniques. ${\mathrm{\ensuremath{\tau}}}_{\mathit{c}\mathit{p}\mathit{h}\mathit{i}}$ is shown to be typically much shorter than both the time of electron-electron collisions and the period of plasma oscillations. We demonstrate that the screening of Coulomb potential cannot be built up during this time. ${\mathrm{\ensuremath{\tau}}}_{\mathit{c}\mathit{p}\mathit{h}\mathit{i}}$ is proportional to ${\mathit{n}}^{\mathrm{\ensuremath{-}}1/\mathit{d}}$ (where n is the carrier concentration and d the dimensionality of a system), which is consistent with the experimental results. The derived law of echo decay of the form exp[-(\ensuremath{\tau}/${\mathrm{\ensuremath{\tau}}}_{\mathit{c}\mathit{p}\mathit{h}\mathit{i}}$)d{)}^{\mathit{d}})d] agrees with the results of numerical simulation, although it does not agree with the existing results of physical experiment. We believe that such a disagreement is of a fundamental nature and manifests a basic need for further experimental and theoretical work.
A detailed experimental study is reported of the decay of circularly polarized photon echoes as a function of Cr concentration in samples ranging from 0.006 to 1.2 wt.% Cr2{\mathrm{Cr}}_{2}Cr2​O3{\mathrm{O}}_{3}O3​ in Al2{\mathrm{Al}}_{2}Al2​O3{\mathrm{O}}_{3}O3​. The decay is found to be independent of temperature in the liquid-helium range and generally depends on the pulse separation $\ensuremath{\tau}$ as $\mathrm{exp}(\ensuremath{-}K{\ensuremath{\tau}}^{\frac{1}{2}})$ with the decay constant KKK proportional to the square root of the Cr concentration. The measured decay is independent of external magnetic field in the range 1.5-6 kG except at 1.06 kG, where modified decays are observed. A theoretical analysis is made of photon-echo decay in terms of spin flips of echo ions resulting from Cr-Cr magnetic interactions and yields good agreement with the observed decays. Spectral diffusion, modified for photon echoes, is shown not to be an important effect. However, anomalously slow decay is observed in some samples when the laser is tuned to the long-wavelength tail of the sample absorption line and the spectral-diffusion mechanism may apply here. The photon-echo-decay measurements are compared with spin-resonance and available spin-echo data in ruby. Also, it is inferred that resonant optical energy transfer is not an important photon-echo-decay mechanism even in the darkest sample studied.