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Physical Review A

Multipulse photon echoes in LaF3 : Pr3+

Lynden E. Erickson

Published Nov 1, 1992• 4 citations
Publisher

Abstract

Multipulse photon echoes are observed from ${\mathrm{LaF}}_{3}$:${\mathrm{Pr}}^{3+}$ 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.

DOI
10.1103/physreva.46.5899

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Physical review. B, Condensed matter•Nov 1, 1991•13 citations
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.
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 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.
A strong decreasing of the intensity of the inverse 2-pulse, 3-pulse and long lived 3-pulse photon echo was observed when a current pulse passed through the strip evaporated onto the surface of the sample (current pulse was applied before or after the laser pulses). The strip is heated by the current pulse and there is the voltage difference at the ends of the strip. The voltage difference creates instantly the nonuniform electric field in the region of optical excitation so the echo intensity is decreased by the short-lived nonuniform line width rise. The line width rise is differentiated for the distinct type ion sites in the LaF3 unit cell. The strip current-heating gives rise to a phonon pulse. When phonon pulse reaches the optically excited volume it causes the shift of energy levels of Pr3+ ions, effecting a phase accumulation and the echo intensity change as a consequence.
We have observed various types of photon echoes in a rare-earth doped crystal using a broad-band c.w. dye laser. Even at the very low spectral power density of the laser, the quantum efficiency of photon echo generation is as large as those using high-power or narrow-band lasers. We have observed Carr-Purcell type photon echo series for the first time in a rare-earth doped crystal. We have measured relaxation of two-pulse photon echo, three-pulse stimulated photon echo, and many-pulse Carr-Purcell photon echo, and found some new features.
When the intensity of photon echo in a two-level system is measured as a function of delay time of the two input pulses, one obtains a simple exponential decay with the characteristic phase relaxation time. When the two levels contain hyperfine structures, the interference among the hyperfine levels gives rise to modulation of the decay envelope. The Fourier transform of the modulation pattern reveals the hyperfine structure of the rare-earth ions. The hyperfine structure, and therefore the modulation pattern, are both sensitively affected by the crystal environment of the ionic site. We extend photon-echo modulation spectroscopy to three-pulse, stimulated photon-echo modulation, and we find that the stimulated echo modulation patterns are quite distinct from the two-pulse, photon-echo case and are affected by a different set of atomic and crystal interaction parameters. The modulation is measured, in several photon-echo transitions of praseodymium ions in lanthanum trifluoride and yttrium aluminum garnet crystals, as functions of delay times between first and second pulses and between first and third pulses. Comparison of the experimental results with density-matrix calculations allows us to determine hyperfine parameters that are not easily observed with two-pulse echo modulation.
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.