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AIP conference proceedings

Collisions of atoms and molecules with laserfields

Klaas Bergmann

Published Jan 1, 1991• 0 citations
Publisher

Abstract

It is shown theoretically and confirmed by experiments that very efficient and highly selective population transfer between atomic or molecular levels can be achieved by stimulated Raman scattering with partially overlapping pulses. It is a particular interesting feature of this method, called STIRAP, that the particles must interact first with the Stokes laser and then with the pump laser, provided there is a sufficient overlap between the interaction with the two lasers. The striking similarity of this transfer process with phenomena well known in atom‐atom collisions is emphasized.

DOI
10.1063/1.40974

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It is shown theoretically and confirmed by experiments that very efficient and highly selective population transfer between atomic or molecular levels can be achieved by stimulated Raman scattering with partially overlapping pulses. It is a particular interesting feature of this method, called STIRAP, that the particles must interact first with the Stokes laser and then with the pump laser, provided there is a sufficient overlap between the interaction with the two lasers. The striking similarity of this transfer process with phenomena well known in atom‐atom collisions is emphasized.
The feasibility of a novel technique for efficient and selective population transfer from a thermally populated level 1 via an intermediate state 2 to level 3 is experimentally demonstrated. It is shown for sodium dimers that the process of on- or near-resonance stimulated Raman scattering with only partially overlapping laser beams is, in particular, useful for the selective population of high vibrational levels of particles in a molecular beam. This is achieved when the interaction with the Stokes laser, coupling levels 2 and 3, begins earlier than the interaction with the pump laser. The phenomenon, which is closely related to the formation of ‘‘trapped states,’’ is quantitatively explained using the basis of eigenstates of molecules strongly coupled to the radiation fields. The similarity and difference to related techniques such as rapid adiabatic passage phenomena in two-level systems, off-resonant stimulated Raman scattering, or stimulated emission pumping is briefly discussed.
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.
Stimulated Raman scattering involving adiabatic passage (STIRAP) is a proven technique for population transfer in three-level systems with strong oscillator strengths. We show that the STIRAP process should also yield high transfer efficiencies when the densities of states near the intermediate and final levels are high, provided certain criteria for the experimentally controllable parameters are met. We also show that high transfer efficiencies may even be possible when the pump and Stokes lasers can access levels outside of the three-level system. The criteria are derived with an approach that emphasizes the adiabatic nature of the transfer process in an eigenvector of the interaction Hamiltonian that resembles a trapped state. The results are compared to density matrix calculations.
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.