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Fluorescence diagnostics in two-step laser excitation of high J atoms

Richard C. Stern, Bruce W. Shore, Norbert Lang

Published Apr 5, 1979• 0 citations

Abstract

Using a pair of lasers near 6000 A, the J = 6 ground state is excited to a J = 6 intermediate level and then to a J = 5 upper state. Non-resonant fluorescences from both excited states are separately detected. Results of a set of model calculations are tabulated. Level 3 average populations are always very small, since the system decays rapidly into inaccessible metastable states. This means that chemistry experiments are difficult. The differences between parallel and perpendicular polarization are modest. The fluorescence dips converge to a value near 50%. The level 3 populations do not approach a common value. This means that the most reliable experimental measurement does not determine the level populations. The most striking changes appear in the last two, most exact, models. The difference between the models is that one includes, for the first time, the linear frequency chirp produced by the fanlike spread of the focussed laser beams. This seemingly innocuous change halves the population left in the ground state. It appears that analogues of adiabatic passage and adiabatic rapid passage respectively are being observed.

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Using a pair of lasers near 6000 A, the J = 6 ground state is excited to a J = 6 intermediate level and then to a J = 5 upper state. Non-resonant fluorescences from both excited states are separately detected. Results of a set of model calculations are tabulated. Level 3 average populations are always very small, since the system decays rapidly into inaccessible metastable states. This means that chemistry experiments are difficult. The differences between parallel and perpendicular polarization are modest. The fluorescence dips converge to a value near 50%. The level 3 populations do not approach a common value. This means that the most reliable experimental measurement does not determine the level populations. The most striking changes appear in the last two, most exact, models. The difference between the models is that one includes, for the first time, the linear frequency chirp produced by the fanlike spread of the focussed laser beams. This seemingly innocuous change halves the population left in the ground state. It appears that analogues of adiabatic passage and adiabatic rapid passage respectively are being observed.

The stark-chirped rapid adiabatic passage (SCRAP) is analyzed, which can give a complete transfer of atomic or molecular population between two bound states in the two level states and Λ(-three)-level state, by means of level-crossing technique and dressed states theory. SCRAP uses two laser pulses: a nearly-resonant pump laser pulse drives the population between a ground state and an excited state, and an intense far-off-resonance Stark laser pulse modifies the transition frequency and resonates with the Bohr transition frequency for two level crossings. A population-transfer maximal efficiency approaching unity is provided from the ground state to the excited state, when the delay of the Stark-shifting pulse with respect to the pulse of the coupling-laser frequency is appropriate and guarantees the pump pulse is strong at one of these crossings and is weak at second one.

The authors describe a method for producing a fast atomic hydrogen beam with a large amount of population selected in 3l j, mod mj mod levels. This is realized by a one-step tunable laser excitation of the metastable component of the atomic beam inside a nonhomogeneous static electric field. The linear laser polarization is taken either parallel or perpendicular with respect to the external field. It allows the selective excitation of all the states of the n=3 Stark manifold (with the exception of the mod mj mod =5/2 state). The electric field strength vanishes immediately after the laser excitation. At this point the population of the excited states are better referred to the atomic basis. The shapes of the resonant lines show that two transient effects are leading the excitation process. The first is of an optical kind (i.e. Rabi oscillation and rapid adiabatic passage) and the second is the intra Stark manifold state mixing due to the nonadiabatic time evolution of the external field strength. The internal state of the atoms crossing these fields is completely described by the density matrix evolution calculated independently on two bases (the atomic basis and the Stark instantaneous basis).

We suggest that infrared stimulated Raman adiabatic passage, a coherent multiple excitation process, can be used to create a superposition of (2J+1) highly correlated M-state sublevels of a rigid rotor molecule with vibrational level v and rotational level J. This method employs the (v=0,J-2) to (v=2,J) S-branch transition, which is carried out in a counterintuitive manner in which the v=1 to v=2 transition is pumped prior to the v=0 to v=1 transition, causing nearly complete population transfer to the v=2 final level. We use perpendicular and parallel linearly polarized infrared excitation (biaxial excitation). Specifically, the perpendicular polarization connects the v=1 intermediate level to the final vibrational level v=2, and the parallel polarization connects the initial level v=0 to the intermediate level v=1. By this means we break the cylindrical symmetry for an ensemble of vibrationally excited molecules in a rovibrational eigenstate (v=2,J). The angular momentum polarization is determined by the relative phases rather than by the populations of the magnetic M-sublevels. For the phase correlated ensemble, the angular momentum polarization can be considered as a purely quantum mechanical effect. Using a fully general density matrix treatment, we illustrate this approach by considering a beam of carbon monoxide (CO) molecules. We find that significant polarization for J=2, 5, and 10 can be achieved with a cw infrared laser source having modest power (∼100 mW/mm(2)). We believe that this technique is a general one and may offer an experimentally accessible new platform for different applications, from scattering studies with M-state entangled ensembles of molecules to logic gate operations of a quantum computer.