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AIP conference proceedings

Efficient coherent population transfer in NO-molecules using pulsed lasers

S. Steuerwald, S. Schiemann, Axel Kuhn, Klaas Bergmann

Published Jan 1, 1995• 1 citation
Publisher

Abstract

Highly efficient and selective population transfer in NO molecules in the electronic ground state (X2Π1/2) from the vibrational level v‘=0 to the level v‘=6 is demonstrated. A rather generally applicable scheme for complete control over the level population in atoms and molecules is now available. The efficiency relies on a counter‐intuitive interaction sequence of two lasers with the molecule in a process of stimulated Raman scattering involving adiabatic passage (STIRAP).

DOI
10.1063/1.47627

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Highly efficient and selective population transfer in NO molecules in the electronic ground state (X2Π1/2) from the vibrational level v‘=0 to the level v‘=6 is demonstrated. A rather generally applicable scheme for complete control over the level population in atoms and molecules is now available. The efficiency relies on a counter‐intuitive interaction sequence of two lasers with the molecule in a process of stimulated Raman scattering involving adiabatic passage (STIRAP).
Highly efficient and selective population transfer in NO molecules in the electronic ground state (X2{\mathit{X}}^{2}X2${\mathrm{\ensuremath{\Pi}}}_{1/2}$) from the vibrational level v''=0 to the level v''=6 is demonstrated. It shows, for the first time with pulsed lasers, that a rather generally applicable scheme for complete control over the level population in atoms and molecules is now available. The efficiency relies on a counterintuitive interaction sequence of two lasers with the molecule in a process of stimulated Raman scattering involving adiabatic passage.
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.
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.
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.