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Optics Letters

Concentration independence of photon echo lifetimes in Pr^3+:LaF_3

Akio Yamagishi, Arthur G. Szabo

Published Jun 1, 1978• 14 citations
Publisher

Abstract

Photon echo studies of the concentration dependence of the homogeneous lifetime, T2′, of the 3H4 → 3P0 transition of Pr3+ in LaF3 indicate no dependence over the range 0.01 to 1.0 at. %. This shows that multipolar, exchange, and spin-flip effects on T2′ are much smaller than the measured value, T2′ = 515 ± 11 nsec. Also, additional experimental confirmation of earlier theories of echo energy dependence on optical thickness is obtained.

DOI
10.1364/ol.2.000160

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Low Temperature Physics•Sep 1, 1997•1 citation
Photon echo studies of the concentration dependence of the homogeneous lifetime, T2′, of the 3H4 → 3P0 transition of Pr3+ in LaF3 indicate no dependence over the range 0.01 to 1.0 at. %. This shows that multipolar, exchange, and spin-flip effects on T2′ are much smaller than the measured value, T2′ = 515 ± 11 nsec. Also, additional experimental confirmation of earlier theories of echo energy dependence on optical thickness is obtained.
Temperature dependences of backward photon echo intensity have been measured from 5°K to 13°K on the 3P0–3H4 (4778 Å) and 1D2–3H4 (5925 Å) transitions of LaF3:Pr3+. Over six orders of magnitude (on the 3P0–3H4 transition) and three orders of magnitude (on the 1D2–3H4 transition) of the photon echo intensity, the experimental results are explained by the one-phonon process (the direct process) taking into account the energy differences between the echo levels and their adjacent levels. Preliminary measurements have also been made on the 4G7/2–4I9/2 (5221 Å) and 4G5/2–4I9/2 (5775 Å) transitions of LaF3:Nd3+.
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.
Photon echo measurements made at 2 °K on the 3H4 - 1D2 transition in Pr3+:LaF3 show that magnetic dipolar couplings between the Pr and F nuclei account for the 56 kHz homogeneous linewidth of this transition.1 The homogeneous broadening arises from the enhanced 141Pr nuclear moment (I=5/2) interacting with the local field fluctuations of the 19F nuclear moments undergoing mutual spin flip transitions. Such resonant fluctuations should, in the absence of a fluorine spin diffusion barrier, produce a homogeneous linewidth of about 200 kHz which is, in fact, roughly what is observed for the inhomogeneous broadening of the Pr3+ hyperfine levels and is considerably broader than that obtained by the photon echo measurements. Shelby et al2 proposed a simple model analogous to the spin diffusion barriers responsible for narrowing the homogeneous lines in certain electron paramagnetic resonance transitions3. In such systems, the field produced by the electron magnetic dipole moment (2-3 orders of magnitude larger than the enhanced nuclear moment associated with the ground state of Pr3+ in LaF3) de-tunes the nearest neighbors from each other, prohibiting mutual spin flips among them. Thus, the fields produced by the neighboring spins are static and their interaction with the paramagnetic ion contributes to the inhomogeneous linewidth and not to homogeneous broadening. The de-tuned neighbors are referred to as the "frozen core." Application of this picture to the case of Pr3+:LaF3 is supported by the calculation of Devoe et al.4 Their Monte Carlo calculation of the Pr3+ optical dephasing times shows that the observed homogeneous linewidth could be explained by deleting the nearest neighbor F spins from the lattice of rapidly fluctuating fluorine moments, in effect, treating them as part of a frozen core.
Optical and hyperfine parameters of the 3H4–1D2 transition are investigated in Pr3 +:La2(WO4)3 for doping concentrations ranging from 0.02 to 3 at.%, at liquid helium temperatures. This includes optical inhomogeneous and homogeneous linewidths, peak absorption, excited-state population decays, spectral hole lifetime and inhomogeneous and homogeneous hyperfine linewidths. Optical inhomogeneous broadening with increasing Pr3 + concentration is limited due to close atomic radii between Pr3 + and La3 +. The peak absorption coefficient increases with increasing Pr3 + doping, reaching up to 28 cm−1. At the highest Pr3 + concentration, optical coherence lifetime is 4.6 μs and hole lifetime 2 s, which should allow one to transfer coherences and tailor the optical inhomogeneous linewidth, as required for rare earth-based optical quantum memories. Raman echo experiments show that hyperfine inhomogeneous linewidth and coherence lifetime (50 kHz and 250 μs respectively) are independent of Pr3 + concentration. These results suggest that highly doped crystals are useful for efficient and long-storage time quantum memories.
Experimental results on the investigation of low-temperature optical absorption spectra and temperature dependence of the photon echo (PE) amplitude signal in Y2SiO5:Pr3+ and LaF3:Pr3+ crystals at the transition H43(0)−3P0 of the Pr3+ ion are presented. It is shown that additional relaxation channels exist for PE in addition to the known phonon mechanisms. This is associated in a LaF3:Pr3+ crystal with the temperature variation of dipole moment at the Pr3+ ion transition. In a Y2SiO5:Pr3+ crystal, this is due to the thermally activated transitions for the Pr3+ ion between nonequivalent positions in the crystal lattice.