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Field-fluctuation-independent Coherence Decay in the Transition- 1/2(^4A_2) ~ - 1/2(E^^-) of the ruby R_1 line

孝夫 村本

Published Jan 1, 1998• 0 citations
OpenAlex

Abstract

By a modified two manifold model, we explain the following experimental results performed for the test of the optical Bloch equation on the transition -1/2(4A2)~-1/2(E) of the ruby R1 line. 1)The optical hole width, including that derived from the FID increases linearly with x(Rabi frequency) under the strong excitation condition. 2)The decay of two pulse and rotary photon echo is a single exponential and the decay constant is power independent as is predicted from the ordinal optical Bloch equation. In this theory, a fluctuating local field is not assumed.

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By a modified two manifold model, we explain the following experimental results performed for the test of the optical Bloch equation on the transition -1/2(4A2)~-1/2(E) of the ruby R1 line. 1)The optical hole width, including that derived from the FID increases linearly with x(Rabi frequency) under the strong excitation condition. 2)The decay of two pulse and rotary photon echo is a single exponential and the decay constant is power independent as is predicted from the ordinal optical Bloch equation. In this theory, a fluctuating local field is not assumed.
Following a brief review of laser frequency and time domain techniques for overcoming inhomogeneous broadening of optical transitions in solids, recent studies on the failure of the optical Bloch equations (OBE) in describing saturation and coherent transient phenomena in ruby will be discussed. Experiments using free induction decay (FID), as in the original work on the system Pr3+:LaF3 by DeVoe and Brewer1, as well as extensions to rotary echos2 and hole-burning3 will be described. At low fields (~ 0.4 T), the time and frequency domain linewidth variation with Rabi frequency agree provided care is taken to avoid line broadening caused by spectral diffusion4. Recent work at high fields (~ 5 T), where Cr-Cr electron spin flipping is suppressed5, shows that spectral diffusion decreases and the dephasing time increases. Observed frequency domain hole widths as narrow as 18 kHz (FWHM) have been obtained for the 4 A2(−1/2)→E¯(−1/2) optical transition in dilute ruby using a pump-probe technique4. Work with such narrow holes emphasizes the fundamental limits imposed by the uncertainty principle and as an aside, a thought experiment where single photons are transmitted through "frequency slits" will be discussed.
Measurements of optical rotary-echo decay of the R1{R}_{1}R1​(-1/2),\ensuremath{\sigma} transition of Cr3+{\mathrm{Cr}}^{3+}Cr3+ in dilute ruby at 2 K are described and compared with predictions of two recent modifications (Gauss-Markov and random-telegraph models) of the optical Bloch equations (OBE's). While the modified OBE approximately describes the free-induction decay behavior both in Pr3+{\mathrm{Pr}}^{3+}Pr3+:LaF3{\mathrm{LaF}}_{3}LaF3​ and ruby, we show that rotary-echo decay in ruby is instead described by the standard OBE. Various aspects of the spin flip-flop model used in the theories are discussed in regard to ruby, as well as other possible dephasing contributions.
A consistent explanation of recent studies by Szabo and Muramoto [Phys. Rev. A 39, 3992 (1989); 38, 5928 (1988)] on the experimental test of modified optical Bloch equations is presented. It is shown that the observed peculiarities of optical transients in solids are connected with the mechanism of relaxation in systems with slow stochastic modulation. A theory of laser-modified relaxation and analysis of free induction decay (FID), hole burning, and rotary echo (RE) in such systems are presented. The universal character of the FID time dependence and field-independent RE decay is predicted.
Recent studies by DeVoe and Brewer [Phys. Rev. Lett. 50, 1269 (1983)] have shown that the conventional optical Bloch equations markedly fail to describe the optical saturation behavior of the D1{D}_{1}D1​ line in the solid Pr3+{\mathrm{Pr}}^{3+}Pr3+:LaF3{\mathrm{LaF}}_{3}LaF3​. In this paper we extend these studies to another solid, ruby, using free-induction-decay observations obtained by pulse excitation of the R1{R}_{1}R1​ line at 693.4 nm with an ultranarrow-linewidth dye laser. Comparison of the results with Gauss-Markov and random-telegraph-dephasing theories shows approximate agreement for a fluctuation correlation time ${\ensuremath{\tau}}_{c}$=T2{T}_{2}T2​, the dephasing time. This result is remarkably similar to that obtained for Pr3+{\mathrm{Pr}}^{3+}Pr3+:LaF3{\mathrm{LaF}}_{3}LaF3​. However, for theoretical and experimental reasons, we conclude that the theories do not consistently explain the current as well as other data. A qualitative discussion of another dephasing model is given.
Recent studies of the failure of the optical Bloch equations (OBE) in describing optical saturation in a solid are extended to test another aspect of the OBE, namely the time dependence of free-induction decay (FID) predicted by the SWB theorem on optical transients [Schenzle, Wong, and Brewer, Phys. Rev. A 22, 635 (1980)]. This theorem states that, following an arbitrarily shaped excitation pulse of length T, the FID will vanish at time T following the end of the excitation pulse. Experiments with ruby violate SWB in that FID decay at least twice as long as the excitation pulse is observed. Numerical and analytical calculations using a Gauss-Markov model for the modified OBE show an extended FID decay, however, the theoretical decay shape does not agree with experiment. Thus as with earlier studies on saturation broadening, we find that the modified OBE provides only a qualitative description of radiation-atom interaction in a solid.
Frequency-domain optical hole burning of the R1{\mathit{R}}_{1}R1​ line [4{[}^{4}[4A2{\mathit{A}}_{2}A2​(-1/2)\ensuremath{\leftrightarrows}E\ifmmode\bar\else\textasciimacron\fi{}(-1/2) transition] in dilute ruby is studied at 2 K and with a field of 3.6 kG applied along the c axis. A pump-probe (PP) technique is used with precise probe-frequency shifting obtained by an acousto-optic modulator. For sufficiently short PP pulses (50 \ensuremath{\mu}s), two holes (narrow and wide) are observed. The narrow (\ensuremath{\sim}20 kHz half width at half maximum at low power) hole-width dependence on Rabi frequency approximately agrees with that inferred from free-induction-decay measurements. For the present concentration (0.0034 wt. % Cr2{\mathrm{Cr}}_{2}Cr2​O3{\mathrm{O}}_{3}O3​) and field, the narrow hole width is determined by fluctuating fields produced by Cr-Cr spin flips [A. Szabo, T. Muramoto, and R. Kaarli, Phys. Rev. B 42, 7769 (1990)]. When the PP delay time is varied, the amplitude of the narrow hole decays with a 1/e time constant of \ensuremath{\sim}300 \ensuremath{\mu}s compared to the E\ifmmode\bar\else\textasciimacron\fi{} fluorescence lifetime of 4 ms. The wide hole (\ensuremath{\sim}500 kHz half width at half maximum) is due to Al-Cr superhyperfine interactions and is created by a spectral diffusion mechanism driven by Al-spin flipping in the host lattice.