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Physical review. B, Condensed matter

Two-pulse photon echo electron-nuclear double resonance of YAl O3 : Pr3+

Robert M. Shelby, R. M. Macfarlane, R. L. Shoemaker

Published Jun 1, 1982• 23 citations
Publisher

Abstract

Two-pulse photon echo electron-nuclear double resonance (or PENDOR) has been used to measure the second-order hyperfine splittings in the ground state and the lowest component of the excited $^{1}D_{2}$ state of YAl${\mathrm{O}}_{3}$:${\mathrm{Pr}}^{3+}$. The excited-state splittings are 0.923 and 1.565 MHz and are significantly different from previous hole-burning results because of greatly increased resolution. The mechanism for two-pulse PENDOR involves a modulation of the photon echo decay at the rf Rabi frequency. This modulation has been observed directly. A brief theoretical analysis is given which shows that the echo modulation is a result of phase and amplitude changes in the oscillating opitical dipole moment which are indirectly produced by the rf field.

DOI
10.1103/physrevb.25.6578

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A photon-echo nuclear double resonance (PENDOR) experiment which detects nuclear magnetic resonances by monitoring the stimulated photon-echo intensity after the application of an rf pulse is described and used to determine the Cr-Al hyperfine and electric-quadrupole interaction parameters associated with the ${\mathrm{Cr}}^{3+}$ ion in the $^{2}E(\overline{E})$ optically excited state in ruby. Most of these parameters are found to be within a few percent of the values associated with ${\mathrm{Cr}}^{3+}$ in the $^{4}A_{2}$ ground state. Resonances are also observed associated with the latter, state, and they are in agreement with previous spin-echo ENDOR work. High resolution is obtained by using a gated cw ruby laser which generates a rapid train of three-pulse stimulated-photon echoes with a long time interval between the second and third excitation pulses. The theoretical behavior of the PENDOR effect is discussed with emphasis on the ability to disentangle complicated multiple overlapping resonances by causing whole sets of resonances to disappear in a controlled way.

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Hyperfine structure and homogeneous broadening in Pr3+:KY(WO4)2

H. L. Xu, M. Nilsson, S. Ohser +4 more

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 ${\mathrm{Pr}}^{3+}:\mathrm{KY}{({\mathrm{WO}}_{4})}_{2}$ (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 $({T}_{1})$ of the $^{1}D_{2}$ 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 $^{1}D_{2}$ ($3.77\ifmmode\pm\else\textpm\fi{}0.03$ and $4.58\ifmmode\pm\else\textpm\fi{}0.04\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$) and $^{3}H_{4}$ ($17.1\ifmmode\pm\else\textpm\fi{}0.1$ 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.

Physical Review B•Dec 30, 2004•8 citations
Two-pulse photon echo electron-nuclear double resonance (or PENDOR) has been used to measure the second-order hyperfine splittings in the ground state and the lowest component of the excited 1D2^{1}D_{2}1D2​ state of YAlO3{\mathrm{O}}_{3}O3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+. The excited-state splittings are 0.923 and 1.565 MHz and are significantly different from previous hole-burning results because of greatly increased resolution. The mechanism for two-pulse PENDOR involves a modulation of the photon echo decay at the rf Rabi frequency. This modulation has been observed directly. A brief theoretical analysis is given which shows that the echo modulation is a result of phase and amplitude changes in the oscillating opitical dipole moment which are indirectly produced by the rf field.
A photon-echo nuclear double resonance (PENDOR) experiment which detects nuclear magnetic resonances by monitoring the stimulated photon-echo intensity after the application of an rf pulse is described and used to determine the Cr-Al hyperfine and electric-quadrupole interaction parameters associated with the Cr3+{\mathrm{Cr}}^{3+}Cr3+ ion in the 2E(E‾)^{2}E(\overline{E})2E(E) optically excited state in ruby. Most of these parameters are found to be within a few percent of the values associated with Cr3+{\mathrm{Cr}}^{3+}Cr3+ in the 4A2^{4}A_{2}4A2​ ground state. Resonances are also observed associated with the latter, state, and they are in agreement with previous spin-echo ENDOR work. High resolution is obtained by using a gated cw ruby laser which generates a rapid train of three-pulse stimulated-photon echoes with a long time interval between the second and third excitation pulses. The theoretical behavior of the PENDOR effect is discussed with emphasis on the ability to disentangle complicated multiple overlapping resonances by causing whole sets of resonances to disappear in a controlled way.
By using a new, delayed-heterodyne photon-echo technique, we have obtained a spectral resolving power of 1.2\ifmmode\times\else\texttimes\fi{}1011{10}^{11}1011, measuring a 2.0-kHz linewidth (half width at half maximum) for the 6105-\AA{} $^{1}D_{2}\ensuremath{\leftrightarrow}^{3}H_{4}$ transition of YAlO3{\mathrm{O}}_{3}O3​: Pr3+{\mathrm{Pr}}^{3+}Pr3+ in an external magnetic field. This appears to be the highest resolution ever obtained in optical spectroscopy. Measurements were also made on the corresponding transition of LaF3{\mathrm{F}}_{3}F3​: Pr3+{\mathrm{Pr}}^{3+}Pr3+ giving a linewidth of 5 kHz. Optical free induction decay gave incorrect results (i.e., significantly broader linewidths).
The hyperfine structure and relaxation character of the terminal levels of the $^{3}P_{0}\ensuremath{-}^{3}H_{4}$ (4777 \AA{}) transition in LaF3{\mathrm{F}}_{3}F3​: Pr3+{\mathrm{Pr}}^{3+}Pr3+ (0.03 at.%) were studied using the photon-echo technique. Using two independent nitrogen-laser pumped dye lasers we have observed modulated photon echoes for pulse separations over a \ensuremath{\sim}10-\ensuremath{\mu}sec range. In this interval our modulated photon echoes decay in a simple exponential manner by a factor of 105{10}^{5}105 and yield a homogeneous linewidth of 70 kHz [full width at half maximum (FWHM)]. Fourier transformation of the echo-modulation data yields directly the nuclear level splittings and their associated linewidths in the 3P0^{3}P_{0}3P0​ and 3H4^{3}H_{4}3H4​ states. In the 3P0(3H4)^{3}P_{0}(^{3}H_{4})3P0​(3H4​) state the nuclear splittings are 0.73 and 1.12 MHz (8.48 and 16.68 MHz). The measurements for the nuclear level splittings and associated linewidths in the 3H4^{3}H_{4}3H4​ state are in excellent agreement with those obtained from the optical-rf double-resonance experiments of Erickson. We find that the calculated echo modulation is a sensitive function of the relative orientation of the principal axes associated with the ground-and excited-state Hamiltonians. By comparing our experimental and calculated echo-modulation patterns we are able to determine their relative orientations.
Using the photon-echo-nuclear-double-resonance technique, we have measured the nuclear hyperfine splittings in the excited 1D2^{1}D_{2}1D2​ state of LaF3{\mathrm{F}}_{3}F3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+. Our measurements are in agreement with the results obtained by Erickson from his saturated-and-enhanced-absorption study of the $^{3}H_{4}\ensuremath{-}^{1}D_{2}$ transition in LaF3{\mathrm{F}}_{3}F3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+.
The hyperfine splitting of the ground state and the lowest electronic component of the (1)D(2) excited state have been measured for Pr(3+) in YAG. We show that a particularly simple and powerful technique is the production of sublevel coherence by short-pulse (impact) excitation, which is detected by coherent forward scattering of a weak probe beam and Fourier transformation of the resulting quantum-beat signal. This yielded excited-state splittings of 6.49 and 8.29 MHz. The ground state shows large pseudoquadrupole splittings of 33.4 and 41.6 MHz, which were obtained by optically detected nuclear quadrupole resonance.
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.