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Physical review. B, Condensed matter

Photon-echo nuclear double resonance in La F3 : Pr3+

Kophu P. Chiang, Edward A. Whittaker, Sven R. Hartmann

Published Jun 1, 1981• 22 citations
Publisher

Abstract

Using the photon-echo-nuclear-double-resonance technique, we have measured the nuclear hyperfine splittings in the excited $^{1}D_{2}$ state of La${\mathrm{F}}_{3}$:${\mathrm{Pr}}^{3+}$. 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 La${\mathrm{F}}_{3}$:${\mathrm{Pr}}^{3+}$.

DOI
10.1103/physrevb.23.6142

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Physical review. B, Condensed matter•Aug 1, 1989•10 citations
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 3H4\ensuremath−1D2^{3}H_{4}\ensuremath{-}^{1}D_{2}3H4​\ensuremath−1D2​ transition in LaF3{\mathrm{F}}_{3}F3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+.
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.
The sizable ground-state nuclear polarization which accompanies the optical pumping of the $^{3}H_{4}\ensuremath{-}^{1}D_{2}$ (16 872-${\mathrm{cm}}^{\ensuremath{-}1}$) $\ensuremath{\sigma}$ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in LaF3{\mathrm{F}}_{3}F3​ was utilized to observe enhanced and saturated absorptions within the inhomogeneously broadened spectral line. The observed hyperfine splittings of the lowest 1D2^{1}D_{2}1D2​ state are 3.7 and 4.7 MHz at 2.0\ifmmode^\circ\else\textdegree\fi{}K. These splittings were fitted by a spin Hamiltonian $\mathcal{H}=D[{I}_{z}^{2}\ensuremath{-}\frac{I(I+1)}{3}]+(\frac{E}{2})({I}_{+}^{2}+{I}_{\ensuremath{-}}^{2})$, where $D=\ensuremath{-}1.10\ifmmode\pm\else\textpm\fi{}0.05$ and $E=\ensuremath{-}0.48\ifmmode\pm\else\textpm\fi{}0.05$ MHz. The observed linewidths (including the exciting laser linewidth) were 0.8 MHz. The deconvoluted optical transition linewidths (full widths at half-maximum) are 0.20\ifmmode\pm\else\textpm\fi{}0.05 MHz.
We have performed a photon echo modulation measurement of the $^{1}D_{2}\ensuremath{-}^{3}H_{4}$ levels of Pr3+{\mathrm{Pr}}^{3+}Pr3+: LaF3{\mathrm{F}}_{3}F3​. This time-domain method yields a precise determination of the 1D2^{1}D_{2}1D2​ excited-state hyperfine splittings and linewidths. New information on the relative orientation of the principal axes of the excited- and ground-state hyperfine Hamiltonians is presented.
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 direct two-photon absorption between crystal-field components of the 3H4^{3}H_{4}3H4​ ground-state configuration to the highest excited state 1S0^{1}S_{0}1S0​ in the 4f24{f}^{2}4f2 manifold of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in LaF3{\mathrm{F}}_{3}F3​ has been observed. The magnitude of the intensities and the polarization dependence require a third- and fourth-order theoretical analysis, similar to that developed for two-photon absorption of Gd3+{\mathrm{Gd}}^{3+}Gd3+ in LaF3{\mathrm{F}}_{3}F3​.
The hyperfine structure of the 1D2^{1}\mathrm{D}_{2}1D2​${\mathrm{\ensuremath{-}}}^{3}$H4{\mathrm{H}}_{4}H4​ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+: yttrium aluminum garnet (YAG) is studied using a photon echo modulation technique. The Fourier transform of modulation data gives hyperfine frequencies of the 1D2^{1}\mathrm{D}_{2}1D2​ state as 3.42 and 5.96 MHz. The photon echo modulation is a very sensitive function of the atomic environment, and we find that the site symmetry of Pr3+{\mathrm{Pr}}^{3+}Pr3+ impurity ions in YAG is lowered to C2{C}_{2}C2​ from the D2{D}_{2}D2​ symmetry of Y3+{\mathrm{Y}}^{3+}Y3+ ions.