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Japanese Journal of Applied Physics

Theory of Optical-Microwave Double Resonance I. Fundamentals and Double Resonance of Microwave Detection

Michio Takami

Published Jun 1, 1976• 41 citations
Publisher

Abstract

The effect of optical pumping on the lineshapes and the peak values of microwave absorption line is calculated by a density matrix method in the Doppler limit approximation. The calculated double resonance signal consists of two terms. One is proportional to the unperturbed population difference of the optical transition and has a Lorentzian lineshape at weak microwave saturation. In this term the two-photon processes cause broadening of the line. The other is proportional to the population difference of the microwave transition and gives the higher-order dynamic Stark effect. At moderate optical saturation the former term is much greater than the latter. At strong optical saturation the latter term becomes noticeable and lineshape anomaly occurs. The peak values of the double resonance signals are also calculated and compared with an experimental result.

DOI
10.1143/jjap.15.1063

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Annual Meeting Optical Society of America•Jan 1, 1985•0 citations
The effect of optical pumping on the lineshapes and the peak values of microwave absorption line is calculated by a density matrix method in the Doppler limit approximation. The calculated double resonance signal consists of two terms. One is proportional to the unperturbed population difference of the optical transition and has a Lorentzian lineshape at weak microwave saturation. In this term the two-photon processes cause broadening of the line. The other is proportional to the population difference of the microwave transition and gives the higher-order dynamic Stark effect. At moderate optical saturation the former term is much greater than the latter. At strong optical saturation the latter term becomes noticeable and lineshape anomaly occurs. The peak values of the double resonance signals are also calculated and compared with an experimental result.
The theory of optical-microwave double resonance is extended to the case of the off-resonant optical field. Line shapes for fixed optical and variable microwave frequencies are calculated under various conditions by the density matrix method. Analytical expressions are given for small microwave or small optical saturation. When the off-resonance is much greater than the Doppler width of the optical transition, optical Stark effect and optical-microwave two-photon transition are the principal effects. When the signal is observed as a variation of microwave absorption, the former effect is much stronger than the latter. When the signal is detected optically, the two-photon and the stepwise transitions for small microwave saturation are the effects with the same order of magnitude, while the optical Stark effect is a secondary effect. The line shapes are also calculated numerically for arbitrary microwave and optical saturation.
This paper presents a theory of lineshapes for molecular Optical-Optical Double Resonance (DR) Spectroscopy with arbitrary strength for both pump and probe fields using the steady-state solutions for the 3-level density matrix. When Doppler broadening can be neglected, the results are analytical, and the probe spectrum is a pair of Lorentzian lines that display Autler-Townes splitting, each with an angular frequency half-width half maximum equal to the relaxation rates, which are assumed to be equal. When Doppler broadening is introduced, one must resort to numerical integration except for the limit of weak pump and probe fields. When the Doppler width is assumed to be much larger than the pump and probe Rabi frequencies and the probe frequency is higher than that of the pump, the calculated DR lineshapes are found to be Lorentzian with a strong pump field limit width that is proportional to the pump Rabi frequency, which is commonly known as power broadening. However, the width does not equal that Rabi frequency and is different for co- and counter-propagating pump and probe fields. Furthermore, that broadening is largely inhomogeneous, despite the Lorentzian shape. The saturation power is found to be about 4 times higher than for the bare probe transition with the same relaxation rate, dramatically lower than that expected if the width is interpreted as homogeneous.
A theoretical study on double-resonance optical pumping for the transitions $5{S}_{1/2}\text{\ensuremath{-}}5{P}_{3/2}\text{\ensuremath{-}}4{D}_{3/2,5/2}$ of 87Rb^{87}\text{R}\text{b}87Rb atoms is presented. The full-density-matrix equations in the presence the probe and the coupling laser beams for all relevant magnetic sublevels of the hyperfine levels were solved numerically, and the absorption of a probe beam was calculated as a function of the detuning of the coupling beam. The calculated results were compared with experimental data, and they showed an excellent agreement. The results were also compared with the approximate results calculated when the coherence between the ground and the highest excited levels was neglected. We found that the dominant operating mechanism for double-resonance signals was the optical pumping rather than the two-photon coherence, although the latter affected the signals significantly.
Novel spectral line shapes of optical-microwave double resonance with an extremely narrow line width were observed in a rubidium atomic clock pumped by a semiconductor laser. It was confirmed that these novel spectral line shapes of double resonance were due to the modulation-transfer effect. These spectral line shapes were calculated by solving the equation of motion of the density matrix that describes the modulation-transfer process. The calculated results agree with the experimental results. By using the calculated results of the influence of the optical Stark effect on these spectral line shapes, characteristics of the inhomogeneous light shift were evaluated quantitatively for the frequency-modulated microwave. Furthermore, optimum values of modulation parameters were found by computer simulation in order to obtain the highest microwave frequency stability of the atomic clocks. An experiment was carried out employing these optimum parameters, and a short-term frequency stability as high as σy(τ) = 7.9 × 10−13τ−1/2 was obtained, where τ is an integration time of measurement.
Previously derived equations describing recoil effects in saturated absorption by a gas of two-level atoms or molecules are solved numerically for the case of standing plane-wave excitation and large Doppler broadening. The numerical techniques and accuracy estimates are discussed briefly. The lineshapes obtained are well approximated by the superposition of two Lorentzian functions whose width, heights, and separation parametrise the lineshape. The dependence of these parameters on saturation, recoil splitting, and relaxation rates is described and compared with corresponding results in the rate equation approximation and in the weak-probe-beam approximation. Saturation broadening depends strongly on these latter approximations, but very little on recoil splitting. When multiphoton processes are retained in the equations, increasing saturation causes a slight decrease in the fitted separation of the peaks. The ratio of the heights of the two Lorentzians is closely related to the ratio of relaxation rates for the level populations.
Reference 1 derives the two-photon probe-absorption coefficient for a homogeneously broadened medium subjected to an arbitrarily intense saturator wave. We have generalized this theory to allow for Doppler broadening with a counterrunning probe and saturator waves. We have carried out integrals over a Lorentzian Doppler distribution analytically and have specialized to a number of limits, such as extreme Doppler broadening. In this limit, we find the simple probe absorption coefficient α 1 ≃ 2 α 0 ( γ D 1 I 2 − i ω s T 1 ) , where α0 is the unsaturated two-photon absorption coefficient, I2 is the saturator intensity, γ is the two-photon coherence decay rate constant, ω s is the Stark shift parameter, T1 is the population difference decay time, and D 1 = 1 / [ γ+ i ( ω+ω s I 2 − ν 2 − ν 1 ) ] . For vanishing Stark shifts (ω s = 0), this is the standard two-photon probe absorption coefficient, but for large ω s , the complex Lorentzian D 1 becomes detuned. In the homogeneously broadened limit, the absorption spectrum resembles the one-photon case. In this paper we show the transition between these two limits.