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Physical Review A

Spectroscopy and multiwave mixing in Pr3+ : LaF3

Fred Moshary, R. Kichinski, Raymond John Beach, Sven R. Hartmann

Published Oct 1, 1989• 3 citations
Publisher

Abstract

Photon-echo and stimulated-photon-echo experiments in ${\mathrm{Pr}}^{3+}$:${\mathrm{LaF}}_{3}$ on the three transitions, $^{3}\mathrm{P}_{0}$-${(}^{3}$${\mathrm{H}}_{5}$${)}_{1}$, $^{3}\mathrm{P}_{0}$-${(}^{3}$${\mathrm{H}}_{5}$${)}_{2}$, and $^{3}\mathrm{P}_{0}$-${(}^{3}$${\mathrm{H}}_{6}$${)}_{1}$ [none of which, therefore, involves the ${(}^{3}$${\mathrm{H}}_{4}$${)}_{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 ${\mathrm{Pr}}^{3+}$ ion states. Amplitude-modulated trilevel echoes were observed involving the $^{3}\mathrm{P}_{0}$-${(}^{3}$${\mathrm{H}}_{5}$${)}_{1}$ and $^{3}\mathrm{P}_{0}$-${(}^{3}$${\mathrm{H}}_{5}$${)}_{2}$ transitions while no trilevel echoes were observed involving the $^{3}\mathrm{P}_{0}$-${(}^{3}$${\mathrm{H}}_{4}$${)}_{1}$ and $^{3}\mathrm{P}_{0}$-${(}^{3}$${\mathrm{H}}_{6}$${)}_{1}$ transitions. Photon echoes were observed on many of the satellite lines of the principal resonance $^{3}\mathrm{P}_{0}$-${(}^{3}$${\mathrm{H}}_{4}$${)}_{1}$ transitions.

DOI
10.1103/physreva.40.4426

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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}$${\mathrm{H}}_{5}$${)}_{1}, 3P0^{3}\mathrm{P}_{0}3P0​-{(}^{3}$${\mathrm{H}}_{5}$${)}_{2}, and 3P0^{3}\mathrm{P}_{0}3P0​-{(}^{3}$${\mathrm{H}}_{6}$${)}_{1} [none of which, therefore, involves the {(}^{3}$${\mathrm{H}}_{4}$${)}_{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}$${\mathrm{H}}_{5}$${)}_{1} and 3P0^{3}\mathrm{P}_{0}3P0​-{(}^{3}$${\mathrm{H}}_{5}$${)}_{2} transitions while no trilevel echoes were observed involving the 3P0^{3}\mathrm{P}_{0}3P0​-{(}^{3}$${\mathrm{H}}_{4}$${)}_{1} and 3P0^{3}\mathrm{P}_{0}3P0​-{(}^{3}$${\mathrm{H}}_{6}$${)}_{1} transitions. Photon echoes were observed on many of the satellite lines of the principal resonance 3P0^{3}\mathrm{P}_{0}3P0​-{(}^{3}$${\mathrm{H}}_{4}$${)}_{1} transitions.
Stimulated-photon-echo measurements as a function of both the first-to-second (\ensuremath{\tau}) and the second-to-third (T) pulse separations were conducted to study the echo-modulation behavior for the 3^{3}3H4{\mathit{H}}_{4}H4​${\mathrm{\ensuremath{-}}}^{1}$D2{\mathit{D}}_{2}D2​ transition of a cryogenic Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ sample. When T is shorter than the excited-state lifetime T1{\mathit{T}}_{1}T1​, deep echo modulations along both the \ensuremath{\tau} and T axes are observed, the frequencies of which correspond to the excited-state sublevel splittings. When T exceeds T1{\mathit{T}}_{1}T1​, the modulation is still observed, although only along the \ensuremath{\tau} axis. A density-matrix theory is developed in a perturbative manner to explain these coherent dynamical properties. The numerically simulated three-dimensional plots of the echo intensity versus \ensuremath{\tau} and T are presented, predicting quite satisfactorily the seemingly complicated experimental modulation patterns.
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.
Multipulse photon echoes are observed from LaF3{\mathrm{LaF}}_{3}LaF3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+ and are shown to be primarily stimulated echoes. The various contributions to the echoes were measured using a three-pulse photon-echo sequence that resolved the image of the echo generated by the first two pulses, and the echo generated by the second and third pulses and that of the first and third pulses from the stimulated echo. By use of a theoretical model of Shoemaker [in Laser and Coherence Spectroscopy, edited by J. I. Steinfeld (Plenum, New York, 1978)] and relaxation theory of Hu and Hartmann [Phys. Rev. B 9, 1 (1974)], the image echo contributions to the third echo is shown to be less than 10% of the total for the pulse widths and Rabi frequencies used in the measurements. As a result, multipulse photon echoes will find limited use in measuring coherence decay until very short high-intensity pulses are used to excite the echoes.
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 photon echo technique was used to investigate the 3P0‐3H6 (5985Å) and the two 3P0‐3H5 (5333.0 Å 5333.5 Å) transitions in Pr3+:LaF3 at 4.6 K. On the 3P0‐3H6 transition, the data displayed modulation and spanned a dynamic range of nine decades in intensity. Echo relaxation rates were anomalously fast in view of previous experiments in this sample. We also report observation of ‘Satellite Echoes’ on the satellite lines of the 3P0‐3H4(4778 Å) transition and present photon echo data obtained on one of the satellite lines. Lasing was observed at 4.6 K and at 77 K during pulse excitation of the 3P0‐3H4 and 3P1(2I6)‐3H4(4633 Å) transitions.