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Physical review. B, Condensed matter

Non-Markovian effects on quantum beats

J. P. Lavoine, Alex Boeglin, P. Martin, A. A. Villaeys

Published May 1, 1996• 9 citations
Publisher

Abstract

The transient four-wave mixing signal from a three-level system coupled to a bath of harmonic oscillators is calculated in the short-pulse limit. This allows an examination of the non-Markovian effects on the relaxation processes in the excited levels between which beating occurs. In particular, it is possible to distinguish between oscillations which are due to oscillatory dephasing, a consequence of the memory effects, and oscillations due to the quantum beats. This also allows one to analyze how these two kinds of oscillations are mixed together. We show that we not only have an amplitude modulation of the beats as in the Markovian case but also deformations of the beats for short delays between the exciting light pulses. These deformations are a consequence of the nonequilibrium motion of the surroundings of the system under optical excitation. \textcopyright{} 1996 The American Physical Society.

DOI
10.1103/physrevb.53.11535

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The transient four-wave mixing signal from a three-level system coupled to a bath of harmonic oscillators is calculated in the short-pulse limit. This allows an examination of the non-Markovian effects on the relaxation processes in the excited levels between which beating occurs. In particular, it is possible to distinguish between oscillations which are due to oscillatory dephasing, a consequence of the memory effects, and oscillations due to the quantum beats. This also allows one to analyze how these two kinds of oscillations are mixed together. We show that we not only have an amplitude modulation of the beats as in the Markovian case but also deformations of the beats for short delays between the exciting light pulses. These deformations are a consequence of the nonequilibrium motion of the surroundings of the system under optical excitation. \textcopyright{} 1996 The American Physical Society.
Oscillatory dephasing is a characteristic of non-Markovian relaxation phenomena when the coherence losses are essentially due to pure dephasing processes. In this paper, we wish to consider the case where the phase relaxation is essentially due to population decay. To this end, we calculate the transient four-wave mixing signal in the short pulse limit from a three-level sytem nondiagonally coupled to a bath of harmonic oscillators. We will show that no oscillatory dephasing is observed in the non-Markovian regime, only a nonexponential decay. Therefore, oscillatory dephasing appears to be a signature of pure dephasing processes.
Oscillatory dephasing is a characteristic signature of non-Markovian relaxation phenomena. From its analysis one can obtain valuable information about the dynamics of the surroundings of a given system. In this paper we calculate the transient four-wave mixing signal in the short pulse limit from two-level systems coupled to a bath of harmonic oscillators for arbitrary coupling strengths and in the presence of inhomogeneous broadening. The strong and weak coupling cases having already been analyzed, we focus on the study of the intermediate case where oscillatory dephasing is observed. We specifically show that even in the presence of inhomogeneous broadening, information about the surroundings can still be extracted in the intermediate coupling regime. The formation and the evolution of the photon echo in such experiments are also analyzed. \textcopyright{} 1996 The American Physical Society.
The transient four-wave-mixing signal from a three-level system is calculated in the short-pulse limit including a general distribution function for the energies of the levels between which beating occurs. This allows an examination of the effects of correlation between the energetic splitting of the levels. As expected, the results demonstrate that the degree of correlation can significantly alter the four-wave-mixing signal. However, the results also show that in the case where the level energies are completely correlated, in a rigorous sense, but that the correlation is not a simple offset, a strong modification of the beat amplitude occurs. This case describes the type of correlation expected in semiconductor quantum wells. Examination of several representative cases demonstrates that these effects can easily be incorrectly ascribed to dephasing.
The transient four-wave mixing signal from a three-level system coupled to a bath of harmonic oscillators is calculated in the short-pulse limit and analyzed at short times. The two excited states of the system are coupled by a constant nonadiabatic interaction V which is treated exactly. This allows an examination of the influence of V on the dynamics in the excited levels at short times. We show that the positions of the minima of the potential energy surfaces of the excited states with respect to the one of the fundamental state play an important role in the relaxation processes. We also show that for high nonadiabatic coupling it is possible to minimize the effect of the bath and hence to minimize, at short times, the coherence losses of the system. The identification of the molecular parameters required to take advantage of this effect should be of interest in the selection of materials for applications in nonlinear optics.
We analyze theoretically the quantum beat and the polarization interference phenomena observed as oscillations in pulsed four-wave mixing. We show that resolution of the signal with respect to the delay between the incoming pulses as well as the detection frequency provides valuable information on the nature of the oscillations. Most importantly, it is very simple to distinguish between polarization interference from two independent optical transitions and quantum beats from a three-level system. In case of polarization interference, the phase of the oscillations shifts \ensuremath{\pi} when the detected frequency passes any of the resonances. In case of quantum beat, the phase has little dependence on the detected frequency near the resonance.