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Physical Review A

Coherent population transfer in multilevel systems with magnetic sublevels. III. Experimental results

J. Martin, Bruce W. Shore, Klaas Bergmann

Published Aug 1, 1996• 108 citations
Publisher

Abstract

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}$${\mathit{P}}_{0}$${\mathrm{?}}^{3}$${\mathit{P}}_{1}$${\mathrm{?}}^{3}$${\mathit{P}}_{2}$ 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.

DOI
10.1103/physreva.54.1556

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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}$${\mathit{P}}_{0}$${\mathrm{?}}^{3}$${\mathit{P}}_{1}$${\mathrm{?}}^{3}$${\mathit{P}}_{2} 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.
The technique of stimulated Raman adiabatic passage 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. We discuss here some of the new and important phenomena that arise when some of the states involved have nonzero angular momentum, the field polarization directions have no simplifying symmetries, and Zeeman splitting lifts the magnetic sublevel degeneracy. We consider the effects of the linkage structure of the Hamiltonian, the effects of various polarization directions, and the effects of various choices for carrier frequencies, as expressed by detunings from single-photon resonance. In particular, we consider an example with angular momentum J=0\ensuremath{\leftrightarrows}J=1\ensuremath{\leftrightarrows}J=2 in which nine magnetic sublevels occur. We show that under suitable conditions it is possible, simply through the appropriate tuning of pump and Stokes carrier frequencies, to place the entire population into any specified single magnetic sublevel.
We present experimental demonstrations of a technique, based on multistate variants of the stimulated Raman adiabatic passage (STIRAP) process, that allows efficient and robust preparation of a preselected superposition of two or three degenerate states (magnetic sublevels of an atom) and the measurement of their relative amplitudes and phases. The experiments verify theoretical results described in the preceding paper. We perform our experiments with neon atoms in a supersonic beam: atoms in the metastable 3P0^{3}{P}_{0}3P0​ state are transferred to a superposition of the metastable 3P2^{3}{P}_{2}3P2​ magnetic sublevels, using four different linkage patterns. Because the preparation utilizes adiabatic passage, it is robust against small fluctuations of the Rabi frequencies and temporal shape of the coupling fields. The relative phases and the amplitude ratios of the components of the prepared superpositions are experimentally analyzed using a technique termed phase-to-population mapping. Phase-to-population mapping is based on laser-induced fluorescence after the atoms have undergone optical pumping cycles induced by an additional laser. The optical pumping process maps the superposition phases into populations of a subset of levels by means of a filtering laser field, and is robust against variations in the intensity and detuning of that field.
We extend previous theoretical work on coherent population transfer by stimulated Raman adiabatic passage for states involving nonzero angular momentum. The pump and Stokes fields are either copropagating or counterpropagating with the corresponding linearly polarized electric-field vectors lying in a common plane with the magnetic-field direction. Zeeman splitting lifts the magnetic sublevel degeneracy. We present an algebraic analysis of dressed-state properties to explain the behavior noted in numerical studies. In particular, we discuss conditions which are likely to lead to a failure of complete population transfer. The applied strategy, based on simple methods of linear algebra, will also be successful for other types of discrete multilevel systems, provided the rotating-wave and adiabatic approximation are valid.
We examine the conditions needed to accomplish stimulated Raman adiabatic passage (STIRAP) when the three levels (ground ggg, excited eee, and final fff) are degenerate, with arbitrary couplings contributing to the pump-pulse interaction $(g\text{\ensuremath{-}}e)$ and to the Stokes-pulse interaction $(e\text{\ensuremath{-}}f)$. We show that in general a sufficient condition for complete population removal from the ggg set of degenerate states for arbitrary, pure or mixed, initial state is that the degeneracies should not decrease along the sequence ggg, eee, and fff. Using a sequence of unitary transformations we demonstrate that when this condition holds it is possible to achieve the degenerate counterpart of conventional STIRAP, whereby adiabatic passage produces complete population transfer. Indeed, the system is equivalent to a set of independent three-state systems, in each of which a STIRAP procedure can be implemented. We also examine the cases when this degeneracy constraint does not hold and show what can be accomplished in those cases. For example, for angular momentum states when the degeneracy of the ggg and fff levels is less than that of the eee level we show how a special choice for the pulse polarizations and phases can produce complete removal of population from the ggg set. Our scheme can be a powerful tool for coherent control in degenerate systems, because of its robustness, when selective addressing of the states is not required or impossible. We illustrate the analysis with several analytically solvable examples, in which the degeneracies originate from angular momentum orientation, as expressed by magnetic sublevels.
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.
It introduced several methods to transfer population,including two-level system and three-level system, and gave some comparisons on transfer efficiency and transfer velocity of them in theory. It is shown that population transfer by coherent pulse sequence is better than incoherence one. Numerical simulation results showed that when using Stimulated Raman Adiabatic Rapid Passage (STIRAP), in which the pump laser pulse fully overlaps the Stokes pulse with the Stokes preceding the pump, population can be transferred completely and rapidly. Robust control of population transfer among Zeeman sublevels in the ground states of three-level system is investigated using adiabatic rapid passage in theory. The laser pulse widths are supposed to be short compared to the lifetime of the excited level, which means adiabatic. We demonstrated that techniques of STIRAP can be found to optimize population transfer in the ground states of three-level Λ system.