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Physical Review A

Detrimental consequences of small rapid laser fluctuations on stimulated Raman adiabatic passage

Леонід Петрович Яценко, Bruce W. Shore, Klaas Bergmann

Published Jan 23, 2014• 33 citations

Abstract

We discuss the detrimental effect of small rapid random fluctuations of laser-field amplitude and phase upon the efficiency of stimulated Raman adiabatic passage (STIRAP). Such fluctuations typically accompany the laser stabilization procedures that produce nearly monochromatic light on top of a much broader bandwidth Lorentz-profile pedestal which may carry only a few percent or less of the total power. As we will show, their effects differ qualitatively from the fluctuations that have hitherto been considered (for example, phase diffusion). We present analytic expressions for the population transfer efficiency of STIRAP when limited by stochastic fluctuations of this type. These expressions show, in contrast to situations discussed in the past in which population transfer improves with increasing peak Rabi frequencies, that for the weak broadband noise that accompanies a strong narrow-spectral component, there is an optimum value for the peak Rabi frequency and that the effect of fluctuations, although small, cannot be entirely eliminated in practice. The mission of the current work is to point out that, under the given circumstances, efforts in experiments trying to overcome the detrimental consequences of fluctuations by increasing the intensity, which is the intuitively proper approach, will not be successful.

DOI: 10.1103/physreva.89.013831

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We discuss the detrimental effect of small rapid random fluctuations of laser-field amplitude and phase upon the efficiency of stimulated Raman adiabatic passage (STIRAP). Such fluctuations typically accompany the laser stabilization procedures that produce nearly monochromatic light on top of a much broader bandwidth Lorentz-profile pedestal which may carry only a few percent or less of the total power. As we will show, their effects differ qualitatively from the fluctuations that have hitherto been considered (for example, phase diffusion). We present analytic expressions for the population transfer efficiency of STIRAP when limited by stochastic fluctuations of this type. These expressions show, in contrast to situations discussed in the past in which population transfer improves with increasing peak Rabi frequencies, that for the weak broadband noise that accompanies a strong narrow-spectral component, there is an optimum value for the peak Rabi frequency and that the effect of fluctuations, although small, cannot be entirely eliminated in practice. The mission of the current work is to point out that, under the given circumstances, efforts in experiments trying to overcome the detrimental consequences of fluctuations by increasing the intensity, which is the intuitively proper approach, will not be successful.

In this paper we discuss the effect of phase noise upon the efficiency of population transfer produced by stimulated Raman adiabatic passage (STIRAP). To allow an adjustable cross-correlation of the two fields we consider the pump and Stokes pulses to be derived from a single phase-diffusing exponentially correlated laser, but we allow some time delay T between the noise signals. We present examples of Monte Carlo simulations, showing unexpected regularities in the dependence of efficiency upon pulse area for partially cross-correlated fields: efficiency does not monotonically increase with increasing pulse area, as would be expected. We explain these, and other properties, by using a simple model of pulse shapes to derive analytic expressions for efficiency. Although derived for a specific analytic form, the formulas also provide a useful description of transfer efficiency by other pulse shapes. We also obtain an estimate of the fundamental limit on the transfer efficiency with STIRAP, based on the Schawlow-Townes limit to laser bandwidths.

This work explores the effect of phase relaxation on the population transfer efficiency in stimulated Raman adiabatic passage (STIRAP). The study is based on the Liouville equation, which is solved analytically in the adiabatic limit. The transfer efficiency of STIRAP is found to decrease exponentially with the dephasing rate; this effect is stronger for shorter pulse delays and weaker for larger delays, since the transition time is found to be inversely proportional to the pulse delay. Moreover, it is found that the transfer efficiency of STIRAP in the presence of dephasing does not depend on the peak Rabi frequencies at all, as long as they are sufficiently large to enforce adiabatic evolution; hence increasing the field intensity cannot reduce the dephasing losses. It is shown also that for any dephasing rate, the final populations of the initial state and the intermediate state are equal. For strong dephasing all three populations tend to

\frac{1}{3}

.

This work explores the effect of spontaneous emission on the population transfer efficiency in stimulated Raman adiabatic passage (STIRAP). The approach uses adiabatic elimination of weakly coupled density matrix elements in the Liouville equation, from which a very accurate analytic approximation is derived. The loss of population transfer efficiency is found to decrease exponentially with the factor ${\ensuremath{\Omega}}_{0}^{2}∕\ensuremath{\Gamma}$, where $\ensuremath{\Gamma}$ is the spontaneous emission rate and ${\ensuremath{\Omega}}_{0}$ is the peak Rabi frequency. The transfer efficiency increases with the pulse delay and reaches a steady value. For large pulse delay and large spontaneous emission rate STIRAP degenerates into optical pumping.

This paper begins with the premise that stimulated Raman adiabatic passage (STIRAP) from one state to another by coupling to an intermediate state necessarily requires some population of that intermediate state. The usual view of the process depends on having no population in the intermediate state, but a simple argument from the time-dependent Schr\"odinger equation shows that such adiabatic transfer cannot occur. From another perspective, removing the time dependence of the Hamiltonian by making the rotating frame transformation cancels the optical frequency oscillations but does not account for the envelopes of the pulses commonly used for STIRAP. By assuming a small but finite intermediate state amplitude ${\ensuremath{\varepsilon}}_{1}$ in the wave function, the propagator for the evolution between initial and final states is derived. Applying the propagator to the initial state produces a single compact formula for the final intermediate-state population that is readily evaluated for an arbitrary choice of laser pulse parameters. Several plots for various experimental conditions show that under the conditions normally used for STIRAP experiments the effects are typically a few percent or less, but in the end this effect puts an ultimate limit on total efficiency.

A theoretical analysis is presented of the effect of correlation between fluctuations of laser pulse amplitudes on population transfer between the states of a three-level atom coupled by the laser field. The carrier frequencies of the pulses are tuned to resonance with the transitions between the ground and excited states, |〈 and | 2〈, and the excited and metastable states, |2〈 and |3〈, in a lambda-type configuration. The laser pulses are timed so that population transfer between states |1〈 and | 3〈 is made possible by stimulated Raman adiabatic passage (STIRAP) in the absence of fluctuations. STIRAP does not occur when the laser fields are not correlated. When the fluctuations of one pulse amplitude duplicate those of the other, STIRAP can be observed for pulse amplitudes larger than those required in the absence of fluctuations.

The feasability of selective and complete population transfer between atomic or molecular levels by stimulated Raman scattering with delayed pulses involving spectrally broad light with characteristics typical for pulsed lasers is investigated. In extension of previous work, the effect on the transfer efficiency of phase fluctuations and of the detuning ΔR of the laser frequencies from the two-photon resonance is analyzed. The minimum pulse energy Pmin required to achieve a transfer efficiency of nearly unity is derived analytically, with some restrictions imposed on the type of phase fluctuations. Pmin increases approximately proportional to the square of the bandwidth of the laser radiation and to the square of ΔR. The conclusions are confirmed by the results of extensive numerical calculations. These studies also reveal a high sensitivity of the transfer efficiency to the autocorrelation of the fluctuating light.