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The Journal of Chemical Physics

Stimulated Raman adiabatic passage in the presence of dephasing

Qiang Shi, Eitan Geva

Published Nov 22, 2003• 50 citations

Abstract

The prospect of employing the stimulated Raman adiabatic Passage (STIRAP) technique under the influence of pure dephasing is explored. A general analysis of how decoherence influences the performance of STIRAP is provided. Starting from a general and fully quantum-mechanical system–bath Hamiltonian, we derive a quantum master equation (QME) that describes the reduced dynamics of a dissipative STIRAP system. The derivation is based on the standard assumptions of (1) weak system–bath coupling; (2) Markovity, in the sense that the relaxation times are long in comparison to the bath correlation time, τc; and (3) weak field–matter interaction, in the sense that the Rabi period of the driving laser fields, Ω−1, is longer than τc. The dissipative term in this QME is the same as it would have been in the absence of the driving fields, because of the assumption of weak field–matter interaction. This type of uncontrollable dephasing is seen to diminish the efficiency of STIRAP, although the actual loss strongly depends on the specific dephasing mechanism. We also derive a more general QME, which is applicable to driving fields of arbitrary intensity. The dissipative term in the new QME is explicitly dependent on the driving fields, and therefore controllable. Intense fields are shown to effectively slow down the dephasing when Ωτc>1, which suggests that it may be possible to use STIRAP in order to transfer population between the quantum states of a solute molecule embedded in a solvent.

DOI: 10.1063/1.1623482

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The prospect of employing the stimulated Raman adiabatic Passage (STIRAP) technique under the influence of pure dephasing is explored. A general analysis of how decoherence influences the performance of STIRAP is provided. Starting from a general and fully quantum-mechanical system–bath Hamiltonian, we derive a quantum master equation (QME) that describes the reduced dynamics of a dissipative STIRAP system. The derivation is based on the standard assumptions of (1) weak system–bath coupling; (2) Markovity, in the sense that the relaxation times are long in comparison to the bath correlation time, τc; and (3) weak field–matter interaction, in the sense that the Rabi period of the driving laser fields, Ω−1, is longer than τc. The dissipative term in this QME is the same as it would have been in the absence of the driving fields, because of the assumption of weak field–matter interaction. This type of uncontrollable dephasing is seen to diminish the efficiency of STIRAP, although the actual loss strongly depends on the specific dephasing mechanism. We also derive a more general QME, which is applicable to driving fields of arbitrary intensity. The dissipative term in the new QME is explicitly dependent on the driving fields, and therefore controllable. Intense fields are shown to effectively slow down the dephasing when Ωτc>1, which suggests that it may be possible to use STIRAP in order to transfer population between the quantum states of a solute molecule embedded in a solvent.

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}

.

We propose a method to improve the stimulated Raman adiabatic passage (STIRAP) via dissipative quantum dynamics, taking into account the dephasing effects. Fast and robust population transfer can be obtained with the scheme by the designed pulses and detuning, even though the initial state of the system is imperfect. With a concrete three-level system as an example, the influences of the imperfect initial state, variations in the control parameters, and various dissipation effects are discussed in detail. The numerical simulation shows that the scheme is insensitive to moderate fluctuations of experimental parameters and the relatively large dissipation effects of the excited state. Furthermore, the dominant dissipative factors, namely, the dephasing effects of the ground states and the imperfect initial state are no longer undesirable, in fact, they are the important resources to the scheme. Therefore, the scheme could provide more choices for the realization of the complete population transfer in the strong dissipative fields where the standard stimulated Raman adiabatic passage or shortcut schemes are invalid.

Using our recently developed quantum dissipation theory, we study the influence of dissipation on the population transfer efficiency between the stimulated Raman adiabatic passage (STIRAP) and the pump-dump passage in a simple three-level Λ system. By comparison, STIRAP is found to be relatively insensitive to the relaxation and fluctuation of the intermediate state. Numerical results also demonstrate the applicability of the new quantum dissipation theory for studying the correlated driving-dissipation dynamics problems.

A master equation approach to the study of environmental effects in the adiabatic population transfer in three-state systems is presented. A systematic comparison with the non-Hermitian Hamiltonian approach [Vitanov and Stenholm, Phys. Rev. A 56, 1463 (1997)] shows that, in the weak-coupling limit, the two treatments lead to essentially the same results. In contrast, in the strong-damping limit the predictions are quite different: In particular, the counterintuitive sequences in the STIRAP scheme turn out to be much more efficient than expected before. This point is explained in terms of quantum Zeno dynamics.

Abstract Stimulated Raman adiabatic passage (STIRAP) is a widely used technique for efficient population transfer between quantum states. However, the adiabatic nature of STIRAP requires slow evolution, leading to long operation times, which limits its practical applications. The superadiabatic method has been introduced to accelerate the STIRAP process, but it often necessitates additional couplings between the initial and target states, which may not be available in the original Hamiltonian. In this work, we present a novel approach to implement superadiabatic STIRAP (sa-STIRAP) between dressed states in a three-level quantum system. By modulating the amplitude and phase of the original driving fields, the initial and target states in dressed-state space can be effectively coupled. This approach provides a practical means of realizing sa-STIRAP in experimental setups, making it convenient to accelerate adiabatic quantum state transfer.

The technique of stimulated Raman adiabatic passage (STIRAP) is a highly efficient tool for coherent population transfer in a chainwise-connected three-state quantum system. It is widely accepted that the two-photon resonance between the two end states of the chain is a crucial condition for STIRAP. This assumption is indeed correct when the two driving fields, pump and Stokes, produce nearly equal couplings for their respective transitions. We show analytically, supported by numeric examples, that when the pump and Stokes couplings differ significantly, the two-photon population transfer profile is distorted and its center is shifted away from the two-photon resonance; hence, the optimal operation of STIRAP demands a two-photon detuning. We derive simple analytic estimates for the center and the width of the two-photon profile. The results are of potential importance in situations when the pump and Stokes fields are of different physical natures (e.g., laser and cavity fields) or when two-photon resonance is unwanted (e.g., in the presence of residual light).