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Reviews of Modern Physics

Coherent population transfer among quantum states of atoms and molecules

Klaas Bergmann, H. Theuer, Bruce W. Shore

Published Jul 1, 1998• 2,227 citations
Publisher

Abstract

The authors discuss the technique of stimulated Raman adiabatic passage (STIRAP), a method of using partially overlapping pulses (from pump and Stokes lasers) to produce complete population transfer between two quantum states of an atom or molecule. The procedure relies on the initial creation of a coherence (a population-trapping state) with subsequent adiabatic evolution. The authors present the basic theory, with some extensions, and then describe examples of experimental utilization. They note some applications of the technique not only to preparation of selected states for reaction studies, but also to quantum optics and atom optics.

DOI
10.1103/revmodphys.70.1003

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We discuss a simple scheme for preparing atoms and molecules in an arbitrary preselected coherent superposition of quantum states. The technique, which we call fractional stimulated Raman adiabatic passage ({\it f-STIRAP}), is based upon (incomplete) adiabatic population transfer between an initial state $ψ_1$ and state $ψ_3$ through an intermediate state $ψ_2$. As in STIRAP, the Stokes pulse arrives before the pump pulse, but unlike STIRAP, the two pulses terminate simultaneously while maintaining a constant ratio of amplitudes. The independence of f-STIRAP from details of pulse shape and pulse area makes it the analog of conventional STIRAP in the creation of coherent superpositions of states. We suggest a smooth realization of f-STIRAP which requires only two laser pulses (which can be derived from a single laser) and at the same time ensures the automatic fulfillment of the asymptotic conditions at early and late times. Furthermore, we provide simple analytic estimates of the robustness of f-STIRAP against variations in the pulse intensity, the pulse delay, and the intermediate-state detuning, and discuss its possible extension to multistate systems.

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The technique of stimulated Raman adiabatic passage (STIRAP) is used to transfer potassium atoms from the 22p state to the 21p Rydberg state through the intermediate state 22s. The results show that complete population transfer is related to pulse duration and overlap, and occurs when the pulse duration and overlap have adequate values. At the same time, population trapping is also formed. Complete population transfer can also occurs when the two-photon resonance condition ( Δ s = Δ p ) is met.

Chinese Physics•Jul 1, 2007•2 citations
The authors discuss the technique of stimulated Raman adiabatic passage (STIRAP), a method of using partially overlapping pulses (from pump and Stokes lasers) to produce complete population transfer between two quantum states of an atom or molecule. The procedure relies on the initial creation of a coherence (a population-trapping state) with subsequent adiabatic evolution. The authors present the basic theory, with some extensions, and then describe examples of experimental utilization. They note some applications of the technique not only to preparation of selected states for reaction studies, but also to quantum optics and atom optics.
We discuss a simple scheme for preparing atoms and molecules in an arbitrary preselected coherent superposition of quantum states. The technique, which we call fractional stimulated Raman adiabatic passage ({\it f-STIRAP}), is based upon (incomplete) adiabatic population transfer between an initial state ψ1ψ_1ψ1​ and state ψ3ψ_3ψ3​ through an intermediate state ψ2ψ_2ψ2​. As in STIRAP, the Stokes pulse arrives before the pump pulse, but unlike STIRAP, the two pulses terminate simultaneously while maintaining a constant ratio of amplitudes. The independence of f-STIRAP from details of pulse shape and pulse area makes it the analog of conventional STIRAP in the creation of coherent superpositions of states. We suggest a smooth realization of f-STIRAP which requires only two laser pulses (which can be derived from a single laser) and at the same time ensures the automatic fulfillment of the asymptotic conditions at early and late times. Furthermore, we provide simple analytic estimates of the robustness of f-STIRAP against variations in the pulse intensity, the pulse delay, and the intermediate-state detuning, and discuss its possible extension to multistate systems.
Techniques for population transfer are needed to gain more complete insight into the collision dynamics of thermally unpopulated levels, e.g. highly vibrationally excited states of molecules. Very promising new techniques are now becoming available. They invoke coherence properties of the radiation field and rely on the phenomena of adiabatic following. In this presentation, I will discuss one of them, the STIRAP method, which induces efficient and highly selective flow of population from an initially populated level 1 to a final level 3. These levels are coupled by a pump and a Stokes laser, with both laser frequencies tuned to resonance with an intermediate level 2. Despite the resonance, spontaneous emission, which may populate levels other than level 3, is eliminated. The method can be implemented with cw as well as with pulsed lasers. First results from a study of the effect of initial vibrational excitation of a molecule on a chemical reaction will be presented. It will also be shown how this technique allows the orientation of electronic or molecular angular moments. The prospects of using this technique for efficient transfer of photon momenta to an atom may be mentioned.
Abstract The population transfer of a NaH molecule from the ground state X 1 Σ + to the target state A 1 Σ + via stimulated Raman adiabatic passage (STIRAP) is investigated. The results show that the intensity, delay time and detuning have a significant effect on population transfer. A large population transfer is observed with increased pump and Stokes intensity, especially when the pump and Stokes intensity match. Population transfer also depends on the delay time between the pump laser pulse and the Stokes laser pulse. The detuning of the two pulses influences the population transfer. Efficient population transfer can be realized under the resonant or two-photon resonant condition.
We discuss the properties of a simple and robust scheme for preparing atoms and molecules in an arbitrary preselected coherent superposition of quantum states - fractional stimulated Raman adiabatic passage (fractional STIRAP) - first proposed by Marte et al (1991 Phys. Rev. A 44 R4118). As in STIRAP, the Stokes pulse arrives before the pump pulse, but unlike STIRAP, here the two pulses terminate simultaneously, while maintaining a constant ratio of amplitudes. We extend earlier research and suggest a realization of this scheme with two smoothly varying delayed laser pulses (which can be derived from a single laser), the parameters of the created superposition being controlled by the polarization of the delayed pulse. Furthermore, we provide simple analytic estimates of the robustness of this process against variations in the laser intensity, laser frequency and pulse delay. Finally, we discuss an extension to multistate systems which provides a possibility for creating coherent superpositions of more than two states.
We describe a technique for creating superpositions of degenerate quantum states, such as are needed for beam splitters used in matter-wave optics, by manipulating the timing of three orthogonally polarized laser beams through which moving atoms (or molecules) pass; motion across the laser beams produces pulses in the atomic rest frame. As illustrated with representative simulations for transitions in metastable neon, a single pass through three overlapping laser beams can produce superpositions (with preselected phase) of atomic beams differing by transverse momentum corresponding to the momentum of four photons. Like the two-photon momentum transfer of the tripod linkage pattern which it extends, the method relies on controlled adiabatic time evolution in the Hilbert subspace of two degenerate dark states. It is thus a generalization to multiple dark states (and larger transfers of linear momentum to the atomic beam) of the single dark state occurring with the stimulated Raman adiabatic passage (STIRAP) technique, and therefore it is potentially insensitive to decoherence due to spontaneous emission. By extending the tripod-linkage system to more numerous degenerate states, the technique not only increases the atomic beam deflections but, as we demonstrate, allows control over the superposition phase and amplitudes. LIke other techniques based on adiabatic time evolution, the technique is robust with respect to variations of the intensity, timing, and other characteristics of the laser fields. Unlike STIRAP, the same robust partial population transfer occurs for opposite timings of the pulse sequence, as is needed for such procedures as Hadamard gates.
The technique of stimulated Raman adiabatic passage (STIRAP) is used to transfer potassium atoms from the 22p state to the 21p Rydberg state through the intermediate state 22s. The results show that complete population transfer is related to pulse duration and overlap, and occurs when the pulse duration and overlap have adequate values. At the same time, population trapping is also formed. Complete population transfer can also occurs when the two-photon resonance condition ( Δ s = Δ p ) is met.