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Journal of the Physical Society of Japan

The Effect of Optical Pumping and Cross Relaxation in the Stark Switching Experiment in Ruby

Shunsuke Nakanishi, 孝夫 村本, O. Tamura, Tsuneo Hashi

Published Dec 1, 1980• 3 citations
Publisher

Abstract

We have found that the amplitudes of the optical FID, two-pulse photon echoes and stimulated photon echoes in ruby measured as a function of applied magnetic field exhibit sharp increases at the magnetic fields where two Zeeman splittings in the ground state 4 A 2 or in the excited state \bar E ( 2 E ) are harmonically related. The phenomena are confirmed to be inherent in the Stark (or frequency) switching experiment where the sample is subjected to the cw irradiation, and the origin of the sharp increases be the change of the steady state population in 4 A 2 of the nonresonant Cr ions caused by a combined action of the cw optical pumping and the spin-spin cross relaxation. The mechanism involved is successfully explained by the analysis based on the rate equations.

DOI
10.1143/jpsj.49.2305

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Observation of Various Photon Echoes and FID in Ruby by Stark Switching Technique

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Journal of the Physical Society of Japan•Oct 1, 1978•6 citations
We have found that the amplitudes of the optical FID, two-pulse photon echoes and stimulated photon echoes in ruby measured as a function of applied magnetic field exhibit sharp increases at the magnetic fields where two Zeeman splittings in the ground state 4 A 2 or in the excited state \bar E ( 2 E ) are harmonically related. The phenomena are confirmed to be inherent in the Stark (or frequency) switching experiment where the sample is subjected to the cw irradiation, and the origin of the sharp increases be the change of the steady state population in 4 A 2 of the nonresonant Cr ions caused by a combined action of the cw optical pumping and the spin-spin cross relaxation. The mechanism involved is successfully explained by the analysis based on the rate equations.
A time varying macroscopic magnetization of ruby is observed at room temperature by selectively exciting the Cr 3+ ions with a right- and a left circularly polarized light of a Q -switched ruby laser from one of the ground 4 A 2 multiplets to a proper component of the upper \bar E ( 2 E ) multiplets. Dependence of such a magnetization in the Z -direction on the irradiation power, the ellipticity and the magnetic field was measured with a pick-up coil. The signal had a value of 1.7×10 -4 emu/g at the irradiation of 67 mJ. The relaxation time of the ground state was estimated from the decay to be about 180 ns in zero magnetic field. The signal changed with the ellipticity of the exciting light, and the amplitude of the signal was always proportional to the intensity of the excitation. These experimental results were quantitatively explained by a theoretical analysis for the time varying optically induced magnetization.
A large number of small but sharp changes (increases and decreases) of the R 1 fluorescence in ruby are observed as a function of applied magnetic field between 2 K and 77 K. At liquid helium temperatures, these signals have linewidths much narrower than the inhomogeneous linewidth (∼0.1 cm -1 ) of the R 1 line. All of these signals appear at the fields where the Zeeman splittings in the excited state \bar E ( 2 E ) and the ground state 4 A 2 satisfy an energy-matching condition for simultaneous transitions of two or more ions. Two distinct mechanisms are found to be responsible for the signals: spin-spin cross-relaxation between \bar E ( 2 E ) and 4 A 2 , and resonant self-trapping of the R 1 line. From the temperature dependence of the linewidths of the signals, thermal broadening of \bar E ( 2 E ) is measured below 77 K. Similar signals are observed in the N lines due to energy transfer from isolated ions to pairs.
The magnetization of ruby in a magnetic field at 300\ifmmode^\circ\else\textdegree\fi{}K is changed when the ruby is optically pumped with linearly polarized radiation from a QQQ-switched ruby laser. With a magnetic field parallel to the trigonal axis, laser light polarized parallel to this axis induces transitions from the spin \ifmmode\pm\else\textpm\fi{}\textonehalf{} levels of the 4A2^{4}A_{2}4A2​ ground state to the levels of the E‾(2E)\overline{E}(^{2}E)E(2E) excited state. The change in Mz{M}_{z}Mz​ is linearly proportional to HHH except near the anticrossing points of the 4A2^{4}A_{2}4A2​ spin levels at 2.07 and 4.14 kG. At these field strengths, there is an enhancement of the magnetization caused by state mixing of the 4A2^{4}A_{2}4A2​ wave functions. When HHH has a small component perpendicular to the zzz axis, a magnetization is detected parallel to this component in the vicinity of 4.14 kG. The effect requires a long ground-state relaxation time. In a separate experiment, the relaxation of Mz{M}_{z}Mz​ was found to vary from 0.13 \ensuremath{\mu}sec in zero magnetic field to a constant value of 0.57 \ensuremath{\mu}sec for fields above 60 G.
Direct relaxation within the optically excited E‾(2E)\overline{E}(^{2}E)E(2E) level of 700-ppm ruby is investigated in magnetic fields up to 65 kG making an angle to the ccc axis. At low pump intensities, the experimental relaxation rates are found to be in excellent agreement with the theory by Blume et al., predicting a fifth-power dependence on field and a ${cos}^{3}\ensuremath{\theta}{sin}^{2}\ensuremath{\theta}$ dependence on orientation. The observed proportionality constant of 4.7 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}19}$ ${\mathrm{G}}^{\ensuremath{-}5}$${\mathrm{s}}^{\ensuremath{-}1}$ is close to the theoretical estimate based on static experiments in ruby. When increasing optical pumping, the phonon-bath conduction is demonstrated to become the limiting process due to resonant trapping of the phonons. Following pulsed excitation, a prolonging of the decay time by a factor up to 13 is attained at excited-state concentrations ${N}^{*}\ensuremath{\sim}2\ifmmode\times\else\texttimes\fi{}{10}^{17}/{\mathrm{cm}}^{3}$. In stationary experiments, a nonlinear increase with N∗{N}^{*}N∗ is observed of the equilibrium population of the upper Zeeman level of E‾\overline{E}E to over a decade above the nonbottlenecked value, corresponding to bottlenecking factors of over \ensuremath{\sim}200. Under the assumption of a constant phonon lifetime of the order of the flight time through the illuminated region, rate equations appear to consistently account for the experiments. A Gaussian-type resonance line, fully homogenized supposedly by magnetic interactions with the surrounding Al nuclei and Cr3+{\mathrm{Cr}}^{3+}Cr3+ ions, explains the lattice-bath equilibration. Finally, the prospect is discussed of using the E‾\overline{E}E direct transition in ruby as a tunable phonon generator and detector with bandwidth 0.002 ${\mathrm{cm}}^{\ensuremath{-}1}$ in the practical frequency range of 2-15 ${\mathrm{cm}}^{\ensuremath{-}1}$.
A relative phase shift between the different groups of excited dipoles, which appears as result of its frequency splitting due to action of a pulse of electric or magnetic fields, depends on a time, if the pulse overlaps in time with echo-pulse. As а consequence, the echo waveform is changed. The echo time form is modulated. The inverse modulation period well enough approximates Zeeman and pseudo-Stark splitting in the cases of magnetic and, therefore, electrical fields. Thus the g-factors of ground 4I15/2 and excited 4F9/2 optical states of Er3+ ion in LuLiF4 and YLiF4 have been measured and pseudo-Stark shift of R1 line in ruby has been determined.