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Physical review. B, Condensed matter

Spectroscopic and relaxation character of the P03−H43 transition in La F3 : Pr3+ measured by photon echoes

Y.C. Chen, Kophu P. Chiang, Sven R. Hartmann

Published Jan 1, 1980• 64 citations
Publisher

Abstract

The hyperfine structure and relaxation character of the terminal levels of the $^{3}P_{0}\ensuremath{-}^{3}H_{4}$ (4777 \AA{}) transition in La${\mathrm{F}}_{3}$: ${\mathrm{Pr}}^{3+}$ (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 ${10}^{5}$ 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 $^{3}P_{0}$ and $^{3}H_{4}$ states. In the $^{3}P_{0}(^{3}H_{4})$ 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 $^{3}H_{4}$ 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.

DOI
10.1103/physrevb.21.40

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Physical review. B, Condensed matter•Nov 1, 1991•13 citations
The hyperfine structure and relaxation character of the terminal levels of the 3P0\ensuremath−3H4^{3}P_{0}\ensuremath{-}^{3}H_{4}3P0​\ensuremath−3H4​ (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.
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.
Using optical detection, we have observed rf nutation, free-induction decay, and echoes, on the 16.70-MHz nuclear hyperfine transition of dilute Pr3+{\mathrm{Pr}}^{3+}Pr3+ in LaF3{\mathrm{F}}_{3}F3​ at 2 K. From a comparison of free-induction decay and echo decay we find that the previously observed linewidth of 200 kHz is inhomogeneous and that the homogeneous width is 19 kHz. On the basis of these measurements it is suggested that optical dephasing times for the $^{1}D_{2}\ensuremath{\leftrightarrow}^{3}H_{4}$ and $^{3}P_{0}\ensuremath{\leftrightarrow}^{3}H_{4}$ transitions are as long as \ensuremath{\sim}20 \ensuremath{\mu} sec.
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 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.
Photon-echo and stimulated-photon-echo experiments in Pr3+{\mathrm{Pr}}^{3+}Pr3+:LaF3{\mathrm{LaF}}_{3}LaF3​ on the three transitions, 3P0^{3}\mathrm{P}_{0}3P0​-(3{(}^{3}(3H5{\mathrm{H}}_{5}H5​)1{)}_{1})1​, 3P0^{3}\mathrm{P}_{0}3P0​-(3{(}^{3}(3H5{\mathrm{H}}_{5}H5​)2{)}_{2})2​, and 3P0^{3}\mathrm{P}_{0}3P0​-(3{(}^{3}(3H6{\mathrm{H}}_{6}H6​)1{)}_{1})1​ [none of which, therefore, involves the (3{(}^{3}(3H4{\mathrm{H}}_{4}H4​)1{)}_{1})1​ ground state] at liquid-He temperatures have revealed the presence of anomalously large residual homogeneous linewidths. The subscripts (e.g., 1,2) denote the crystal-field-split levels of the Pr3+{\mathrm{Pr}}^{3+}Pr3+ ion states. Amplitude-modulated trilevel echoes were observed involving the 3P0^{3}\mathrm{P}_{0}3P0​-(3{(}^{3}(3H5{\mathrm{H}}_{5}H5​)1{)}_{1})1​ and 3P0^{3}\mathrm{P}_{0}3P0​-(3{(}^{3}(3H5{\mathrm{H}}_{5}H5​)2{)}_{2})2​ transitions while no trilevel echoes were observed involving the 3P0^{3}\mathrm{P}_{0}3P0​-(3{(}^{3}(3H4{\mathrm{H}}_{4}H4​)1{)}_{1})1​ and 3P0^{3}\mathrm{P}_{0}3P0​-(3{(}^{3}(3H6{\mathrm{H}}_{6}H6​)1{)}_{1})1​ transitions. Photon echoes were observed on many of the satellite lines of the principal resonance 3P0^{3}\mathrm{P}_{0}3P0​-(3{(}^{3}(3H4{\mathrm{H}}_{4}H4​)1{)}_{1})1​ transitions.
We report a systematic study of the stimulated-photon-echo relaxation on the 3^{3}3P0{\mathit{P}}_{0}P0​${\mathrm{\ensuremath{-}}}^{3}$H4{\mathit{H}}_{4}H4​ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+:LaF3{\mathrm{LaF}}_{3}LaF3​ and the 3^{3}3P0{\mathit{P}}_{0}P0​${\mathrm{\ensuremath{-}}}^{3}$H4{\mathit{H}}_{4}H4​ and 1^{1}1D2{\mathit{D}}_{2}D2​${\mathrm{\ensuremath{-}}}^{3}$H4{\mathit{H}}_{4}H4​ transitions of Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAG (yttrium aluminum garnet). The stimulated-echo intensity is measured as a function of the delay between the first and the second pulses and the delay between the second and the third pulses. The stimulated-echo relaxation is modulated by the hyperfine interaction in the ground and the excited electronic states. We find that the modulation patterns can be quite distinct from those for two-pulse photon-echo relaxation and give complementary information about the hyperfine structures. We use the density-matrix theory of stimulated-photon-echo modulation, and the resulting simulation shows satisfactory agreement with the experimental data.