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Physical review. B, Condensed matter

Observation of a magnetic-field-induced resonance in the homogeneous dephasing time for the 1 D2 −3 H4 transition in Pr3+ : YAlO3

Baozhu Luo, Stefan Kröll

Published Oct 1, 1996• 2 citations
Publisher

Abstract

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}$${\mathit{H}}_{4}$${\mathrm{\ensuremath{-}}}^{1}$${\mathit{D}}_{2}$ transition of ${\mathrm{Pr}}^{3+}$:${\mathrm{YAlO}}_{3}$. 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:${\mathrm{YAlO}}_{3}$ system the observed resonance could not be unambiguously tied to such effects. \textcopyright{} 1996 The American Physical Society.

DOI
10.1103/physrevb.54.9834

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Physical review. B, Condensed matter•Jun 1, 1990•33 citations
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}$${\mathit{H}}_{4}$${\mathrm{\ensuremath{-}}}^{1}$${\mathit{D}}_{2} 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.
Photon-echo techniques were employed to measure the homogeneous dephasing rate of the 592.5-nm, 3^{3}3${\mathit{H}}_{4\mathrm{\ensuremath{-}}}^{1}$D2{\mathit{D}}_{2}D2​, 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.
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.
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.
As part of a search for suitable materials for coherent quantum operations, relaxation times and hyperfine structure of the $^{1}D_{2}(1)\text{\ensuremath{-}}^{3}H_{4}(1)$ transition in Pr3+:KY(WO4)2{\mathrm{Pr}}^{3+}:\mathrm{KY}{({\mathrm{WO}}_{4})}_{2}Pr3+:KY(WO4​)2​ (0.29 at. %) at 4 K have been obtained using photon-echo and spectral hole burning techniques. The homogeneous linewidth and the effect of excitation-induced dephasing were measured using two-pulse photon-echo techniques. Linewidths of $23.4\ifmmode\pm\else\textpm\fi{}1.0$ and $17.6\ifmmode\pm\else\textpm\fi{}0.9\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}$ were obtained in the absence and presence of an external magnetic field of about 9 mT. The radiative lifetime (T1)({T}_{1})(T1​) of the 1D2^{1}D_{2}1D2​ state was measured to be $43\ifmmode\pm\else\textpm\fi{}2\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ using time-resolved laser-induced fluorescence and three-pulse photon-echo measurements. The transmission hole spectra were measured and directly yielded the quadrupole level splitting in the 1D2^{1}D_{2}1D2​ ($3.77\ifmmode\pm\else\textpm\fi{}0.03$ and $4.58\ifmmode\pm\else\textpm\fi{}0.04\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$) and 3H4^{3}H_{4}3H4​ ($17.1\ifmmode\pm\else\textpm\fi{}0.1$ and $33.2\ifmmode\pm\else\textpm\fi{}0.3\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$) states. The spectral hole lifetime due to population redistribution between the ground-state nuclear levels was also determined to be $70\ifmmode\pm\else\textpm\fi{}10\phantom{\rule{0.3em}{0ex}}\mathrm{ms}$. A strong dipole-dipole interaction observed in this crystal opens for potential applications in quantum computing schemes for performing quantum logic operations, but the short dephasing time makes it less useful in data storage applications.
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​.
Photon-echo-relaxation measurements made on the 3H4^{3}\mathrm{H}_{4}3H4​${\mathrm{\ensuremath{-}}}^{3}$P0{\mathrm{P}}_{0}P0​ transition of 0.01 at. % Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAG (where YAG represents yttrium aluminum garnet), 3H4^{3}\mathrm{H}_{4}3H4​${\mathrm{\ensuremath{-}}}^{1}$D2{\mathrm{D}}_{2}D2​ transition in 0.1 at. % Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​, and 7F0^{7}\mathrm{F}_{0}7F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathrm{D}}_{0}D0​ transition in 0.25 at. % Eu3+{\mathrm{Eu}}^{3+}Eu3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ show that the photon-echo relaxation rate increases when the intensities of the excitation pulses are increased. Although a part of the relaxation-rate increase in Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAG may be attributed to an instantaneous spectral diffusion (ISD) in which the presence of excited neighboring Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions change the local field and the absorption frequency of the rare-earth ions, our data deviate significantly from the ISD-model predictions. An additional intensity-dependent relaxation mechanism is required to explain the results.