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Bulletin of the American Physical Society

Population transfer, alignment and orientation by stimulated adiabatic passage

Y. B. Band

Published May 1, 1993• 0 citations
OpenAlex

Abstract

We review and compare recent experiments and theoretical models demonstrating complete population transfer to selected states in atoms and molecules using (1) Stimulated Raman Adiabatic Rapid Passage (STIRAP) with temporally delayed but partially overlapping time dependent fundamental and Stokes fields and (2) Chirped Adiabatic Passage (CHIRAP) using frequency chirped field with the frequency swept through the resonance frequency of transitions. The transfer efficiency in these processes is unity when the adiabatic criteria are satisfied. Alignment and orientation of the initial and terminals levels of the transitions can be obtained using these methods. The dynamics involve the atomic or molecular internal angular momentum states because the Rabi frequencies for the transitions depend on the magnetic quantum numbers of the states. Full wavefunction and density matrix (necessary when spontaneous emission of the excited states plays a role) calculations are presented and adiabatic-following wavefunction and density matrix descriptions are advanced to explain unexpected experimental results.

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We review and compare recent experiments and theoretical models demonstrating complete population transfer to selected states in atoms and molecules using (1) Stimulated Raman Adiabatic Rapid Passage (STIRAP) with temporally delayed but partially overlapping time dependent fundamental and Stokes fields and (2) Chirped Adiabatic Passage (CHIRAP) using frequency chirped field with the frequency swept through the resonance frequency of transitions. The transfer efficiency in these processes is unity when the adiabatic criteria are satisfied. Alignment and orientation of the initial and terminals levels of the transitions can be obtained using these methods. The dynamics involve the atomic or molecular internal angular momentum states because the Rabi frequencies for the transitions depend on the magnetic quantum numbers of the states. Full wavefunction and density matrix (necessary when spontaneous emission of the excited states plays a role) calculations are presented and adiabatic-following wavefunction and density matrix descriptions are advanced to explain unexpected experimental results.
We study the dynamics of chirped adiabatic passage (CHIRAP) with temporally delayed pulses to selectively and fully transfer population in atoms and molecules. We show that the transfer of population via stimulated Raman adiabatic passage (STIRAP) and stimulated two-photon adiabatic absorption with temporally delayed laser pulses is not adversely affected by applying a chirp to the pulses, provided the intensity of the laser is sufficiently large to allow adiabatic passage. We then proceed to consider systems in which a near degeneracy of terminal state levels results in nonselective population of the terminal levels using nonchirped STIRAP or two-photon absorption stimulated passage, because the dynamics within the nearly degenerate pair of levels is not adiabatic. However, the CHIRAP process selectively populates only one of the terminal levels.
We describe a technique for totally transferring the population of a molecular vibronic level to another optically accessible level by chirped pulse absorption. The method can be applied even for nonvanishing angular momentum states where the Rabi frequencies for the transitions depend on the magnetic quantum number M of the states. The population of a large J initial state can be totally transferred to a J′=J+1 state by R branch transitions with linearly or circularly polarized light pulses with negative or positive frequency chirp if the bandwidth of the chirped pulse is sufficiently small. For an initial state with small J, having P(Q) and R transitions that are closely spaced in energy and within the chirped pulse bandwidth, the situation is complicated by the presence of transitions involving additional nearby J states which can participate in transitions induced by the chirped pulse. For positive frequency chirp, population can be totally transferred to the excited electronic state, whereas for the negative frequency chirp case the population distribution depends on the details of the energy levels and laser pulse. The technique can be employed to align and orient states in which not all the M states of the initial level are transferred to the same branch, but each M state is totally transferred from the initial state. Criteria for this type of population transfer and alignment and orientation are described and the conditions under which adiabatic passage is maintained are discussed.
The technique of stimulated Raman adiabatic passage (STIRAP) has become an established procedure for producing complete population inversion in atoms or molecules via application of Stokes and pump pulses in a counterintuitive sequence. Previously we reported on numerical and analytical investigations showing some of the additional and important phenomena that arise when some of the levels involved have nonzero angular momentum, the field polarization directions have no simplifying symmetries, and Zeeman splitting lifts the magnetic sublevel degeneracy. Here we verify our theoretical findings using the metastable neon system: 3^{3}3P0{\mathit{P}}_{0}P0​?3{\mathrm{?}}^{3}?3P1{\mathit{P}}_{1}P1​?3{\mathrm{?}}^{3}?3P2{\mathit{P}}_{2}P2​ with the corresponding angular momentum sequence J=0?J=1?J=2. In particular, we demonstrate that it is possible to transfer all population from the single initial state to any single selectable final magnetic sublevel M. Selectivity can be achieved either by choosing special laser polarization angles or, for fixed polarizations, by tuning the two lasers into two-photon resonance between the initial and desired final state. The complete control of magnetic sublevel population enabled by this procedure extends the customary experimental methods for producing oriented or aligned beams of atoms. In addition, we demonstrate very clearly the previous prediction that population transfer may fail for certain sets of parameters (detunings, Rabi frequencies, and polarization angles). \textcopyright{} 1996 The American Physical Society.
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.
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.