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Physical review. B, Condensed matter

Optically induced shifts in the frequency of the 3 H4 −1 D2 transition of Pr3+ in LaF3

Jiamin Zhang, THOMAS W. MOSSBERG

Published Sep 1, 1993• 8 citations
Publisher

Abstract

Photon-echo techniques were employed to measure the homogeneous dephasing rate of the 592.5-nm, $^{3}$${\mathit{H}}_{4\mathrm{\ensuremath{-}}}^{1}$${\mathit{D}}_{2}$, transition of ${\mathrm{Pr}}^{3+}$ as experimental parameters affecting the number of ${\mathrm{Pr}}^{3+}$ ions optically excited were varied. These parameters include the dopant concentration and the intensity, carrier frequency, and bandwidth of the excitation pulses. Dephasing rates are found to contain a background contribution whose magnitude is dependent upon the specific crystal sample studied and a second contribution whose magnitude increases with the number of ${\mathrm{Pr}}^{3+}$ ions changing state in the course of the echo excitation sequence. The second contribution to the dephasing rate is attributed to the presence of optical instantaneous diffusion, i.e., the redistribution of ionic transition frequencies consequent to optical excitation, in the samples.

DOI
10.1103/physrevb.48.7668

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Physical Review Letters•Jun 4, 1979•70 citations
Photon-echo techniques were employed to measure the homogeneous dephasing rate of the 592.5-nm, ^{3}$${\mathit{H}}_{4\mathrm{\ensuremath{-}}}^{1}$${\mathit{D}}_{2}, transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+ as experimental parameters affecting the number of Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions optically excited were varied. These parameters include the dopant concentration and the intensity, carrier frequency, and bandwidth of the excitation pulses. Dephasing rates are found to contain a background contribution whose magnitude is dependent upon the specific crystal sample studied and a second contribution whose magnitude increases with the number of Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions changing state in the course of the echo excitation sequence. The second contribution to the dephasing rate is attributed to the presence of optical instantaneous diffusion, i.e., the redistribution of ionic transition frequencies consequent to optical excitation, in the samples.
Using two-pulse photon echo excitation a strong resonance in the measured homogeneous dephasing time as a function of magnetic field is observed in the 3^{3}3H4{\mathit{H}}_{4}H4​${\mathrm{\ensuremath{-}}}^{1}$D2{\mathit{D}}_{2}D2​ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​. The resonance could only be observed at low excitation energies since it otherwise was masked by excitation intensity dependent extra dephasing processes in the crystal. Thus intensity dependent dephasing processes may not only affect the apparent dephasing time of a system but may also mask other more subtle interactions in the materials studied. It is reasonable to assume that the type of resonance observed could be caused by Zeeman induced level crossings in the active ion or in the host crystal ions or, possibly, that it could be due to coincidences between Zeeman level transition frequencies. However, based on current data of the Pr:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ system the observed resonance could not be unambiguously tied to such effects. \textcopyright{} 1996 The American Physical Society.
Contributions to the homogeneous linewidth of the 3^{3}3H4{\mathit{H}}_{4}H4​(1)${\ensuremath{\rightarrow}}^{1}$D2{\mathit{D}}_{2}D2​(1) transition for the two crystallographic sites of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in Y2{\mathrm{Y}}_{2}Y2​SiO5{\mathrm{SiO}}_{5}SiO5​ have been investigated using photon echoes. The effects of excitation-intensity-dependent dephasing or instantaneous diffusion were systematically studied to allow accurate determination of the optical resonance widths. Homogeneous linewidths of 2.8 kHz (site 1) and 1 kHz (site 2) were measured with no applied magnetic field and with sufficiently low laser intensity to minimize the effects of instantaneous diffusion. Using the same excitation intensity, widths of 2.1 kHz (site 1) and 0.85 kHz (site 2) were obtained with an applied magnetic field of 77 G, demonstrating a significant contribution of 89Y^{89}\mathrm{Y}89Y nuclear-spin fluctuations to the zero-field homogeneous linewidth. Extrapolation to zero excitation intensity yielded optical resonance widths that were only slightly narrower than the measured values. Optically detected nuclear magnetic resonance measurements determined the hyperfine structure of the 3^{3}3H4{\mathit{H}}_{4}H4​ ground state for each site; the hyperfine levels of the lowest component of the 1^{1}1D2{\mathit{D}}_{2}D2​ manifold for each site were determined using photon echo nuclear double resonance. The relatively large oscillator strength of 3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}7}$ for a rare-earth ion, in conjunction with long dephasing times makes this material a useful candidate for demonstration of time-domain signal processing and optical data storage.
Two-pulse photon-echo measurements on the 0.1 at. % Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ 3^{3}3H4{\mathit{H}}_{4}H4​${\mathrm{\ensuremath{-}}}^{1}$D2{\mathit{D}}_{2}D2​ transition suggest that the relaxation time depends on the density of excited states created by the excitation pulses. The dependence of the relaxation time on the intensity of each excitation pulse shows that our results are inconsistent with instantaneous spectral diffusion, a model often invoked in this type of experiment, where excited states created by the second pulse chiefly influence the relaxation time. A homogeneous linewidth contribution, noted in previous work as being of unknown origin, is eliminated at low excitation fluences.
Intensity-dependent optical dephasing is shown to arise from nonresonant excitation of 1% Pr3+{\mathrm{Pr}}^{3+}Pr3+-doped yttrium aluminum garnet (YAG) with UV radiation between 325--355 nm. UV irradiation of the sample with intensities greater than 30 MW/cm2{\mathrm{cm}}^{2}cm2 produces persistent changes in the optical dephasing. Two-pulse photon echo decays on the 3^{3}3H4{\mathit{H}}_{4}H4​${\ensuremath{\rightarrow}}^{1}$D2{\mathit{D}}_{2}D2​ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+ were measured at 1.5 K before and after exposure to UV radiation. Changes persisting for at least several hours are observed in the echo intensity, echo decay rate, and temporal form of the echo decay. Changes persist if the sample is kept below 10 K, but warming to 77 K results in the echo decays resuming their initial intensity and duration. No change is detected in the optical absorption spectrum of the Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions after UV exposure, indicating that most of the ions remain in that charge state. Although the mechanism giving rise to the increased optical dephasing is not completely understood, the additional dynamics may arise from the UV radiation freeing electrons that become trapped in lattice defects. The presence of the dephasing at low temperatures indicates the availability of low-energy excitations of the electronic system.
Working on the 7F0^{7}\mathrm{F}_{0}7F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathrm{D}}_{0}D0​ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ in Y2{\mathrm{Y}}_{2}Y2​O3{\mathrm{O}}_{3}O3​, we provide the first detailed characterization of excitation-induced shifts in optical transition frequencies and demonstrate their exaggeration of nominally homogeneous dephasing rates. The shifts (found to vary in rough proportion to the number of Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions excited and to be as small as one part in 1012{10}^{12}1012) were identified through their unique signature in specially designed photon-echo experiments. The effects reported may constitute a rather general complication in optical measurements of homogeneous relaxation rates in solids.
Optical free-induction dephasing times as long as 16 \ensuremath{\mu}sec, corresponding to an optical homogenous linewidth of 10 kHz, have been observed for the $^{3}H_{4}\ensuremath{\leftrightarrow}^{1}D_{2}$ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions in LaF3{\mathrm{F}}_{3}F3​ at 2\ifmmode^\circ\else\textdegree\fi{}K. Measurements are facilitated by a frequency-locked cw dye laser and a new form of laser frequency switching. Zeeman studies reveal a Pr-F dipole-dipole dephasing mechanism where the Pr nuclear moment is enhanced in both 1D2^{1}D_{2}1D2​ and 3H4^{3}H_{4}3H4​.