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Annual Meeting Optical Society of America

Stimulated photon echo modulation in praseodymium-doped crystals

P. Talagala, M. K. Kim, Ravinder Kachru

Published Jan 1, 1990• 0 citations
Publisher

Abstract

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.

DOI
10.1364/oam.1990.tuy32

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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.
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.
We study the optical properties of rare-earth-ion-doped inorganic crystals with an emphasis on the dependence of two-pulse photon echoes on the excitation density in the system. The experimental investigations concentrate on Pr3+{\mathrm{Pr}}^{3+}Pr3+:Nd3+{\mathrm{Nd}}^{3+}Nd3+:Eu3+{\mathrm{Eu}}^{3+}Eu3+ codoped Y2{\mathrm{Y}}_{2}Y2​SiO5{\mathrm{O}}_{5}O5​ and YAlO3{\mathrm{O}}_{3}O3​ crystals at low temperatures. With two pulses of one laser the echo is induced in one ion species and with a third, "scrambler" pulse of a second laser another species is excited. These scrambler excitations lead to a dephasing and thus to an echo attenuation which depends on the strength, frequency, and time of the scrambler pulse. The spectral sensitivity of the echo attenuation is used for a spectroscopic technique: "photon-echo attenuation spectroscopy." As a function of the delay time ts{t}_{s}ts​ between the scrambler pulse and the onset of the two-pulse echo sequence the attenuation shows a very specific behavior dictated by the excitation-induced frequency shifts (EFS's). For ts{t}_{s}ts​ between the two echo-inducing pulses the echo intensity is partially regained by the "dephasing-rephasing balancing" of the reversible EFS's. For the theoretical description a stochastic model is introduced and the dephasing by excitation-induced lattice vibrations and by EFS's are analyzed in detail. The present results are discussed in the light of previous experimental and theoretical investigations.
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.
A novel coherent transient spectroscopy, cw photon echo, is described. A medium is exposed to broadband cw laser radiation and then to a pulsed laser, resulting in a continuous emission signal from the medium. The temporal profile of this signal is studied using full density-matrix theory for the cases of a two-level system and a multilevel system. It is shown that such signal decays with a homogeneous dephasing time T2{\mathit{T}}_{2}T2​ and can have a quantum-beat-type modulation, reproducing in a single shot the conventional two-pulse photon echo plot versus first-to-second pulse separation. Experimental demonstrations are given for the 7^{7}7F0{\mathit{F}}_{0}F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathit{D}}_{0}D0​ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ and the 3^{3}3H4{\mathit{H}}_{4}H4​${\mathrm{\ensuremath{-}}}^{1}$D2{\mathit{D}}_{2}D2​ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+; both ions are doped in YAlO3{\mathrm{YAlO}}_{3}YAlO3​. The Eu ions exhibit a single exponential decay with a slight modulation due to the ground-state hyperfine splittings. The temperature dependence of the signal is also studied. The Pr ions show a very deep modulation pattern, which provides excellent agreement with the independent two pulse echo measurement. A numerical simulation based on the modulation theory also agrees with the observed decay curves and the nuclear axis configuration in this crystal is discussed.
The signals of photon echo (PE) are investigated firstly in a ruby crystal doped only by the 53 Cr isotope ions in a concentration of 0.03 – 0,05 wt%. The optical experiments were performed in backward regime at the wavelength of 693.4 nm both with a low magnetic field (200 G) and without it. Since the 53 Cr isotope ions have hyperfine structure of levels the special attention was paid to the study of the stimulated photon echo and primarily to the investigation of its decay kinetics. It is established that this decay has a form which is typical to the signals of long-lived PE. But in contrast to the long-lived PE the decay time in our case is less than the lifetime of the excited 2E(Ē) state. The signals of primary photon echo and stimulated photon echo at a low longitudinal magnetic field and their decay curves are investigated. We observed the beats of temporal shape of these signals with a period of several tens of nanoseconds. Theoretical analysis shows that they are due to the hyperfine interaction of valence electrons of 53 Cr isotope ions with their own nuclei. The obtained decay curves allow us to estimate the phase relaxation time at the presence of a magnetic field. It proves to be equal to 98 ns. The spectrum of stimulated photon echo signal in the doped ruby exposed to a magnetic field is measured.