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Physical Review A

Direct observation of two-photon optical ionizing collisions in crossed lithium atomic beams

Penelope Polak-Dingels, Regina E. Bonanno, John Keller, J. Weiner, J. C. Gauthier

Published May 1, 1982• 6 citations
Publisher

Abstract

We report here the direct observation of a two-step, ionizing "optical collision" between crossed lithium beams in which very-long-range coupling, due to van der Waals' resonance force between identical particles, is followed by photoionization: ${\mathrm{Li}}^{*}(2p)+\mathrm{Li}(2s)+\ensuremath{\hbar}\ensuremath{\omega}\ensuremath{\rightarrow}{\mathrm{Li}}^{*}(3d)+\mathrm{Li}(2s),$ ${\mathrm{Li}}^{*}(3d)+\ensuremath{\hbar}\ensuremath{\omega}\ensuremath{\rightarrow}{\mathrm{Li}}^{+}+e.$ Cross-section magnitude and form of the intensity profile are described by a simple three-level model. These results suggest that polarization of the laser field together with collisional two-photon ionization may be used to delineate the shape of individual molecular-state potential curves at long range.

DOI
10.1103/physreva.25.2539

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We report here the direct observation of a two-step, ionizing "optical collision" between crossed lithium beams in which very-long-range coupling, due to van der Waals' resonance force between identical particles, is followed by photoionization: Li∗(2p)+Li(2s)+\ensuremathℏ\ensuremathω\ensuremath→Li∗(3d)+Li(2s),{\mathrm{Li}}^{*}(2p)+\mathrm{Li}(2s)+\ensuremath{\hbar}\ensuremath{\omega}\ensuremath{\rightarrow}{\mathrm{Li}}^{*}(3d)+\mathrm{Li}(2s),Li∗(2p)+Li(2s)+\ensuremathℏ\ensuremathω\ensuremath→Li∗(3d)+Li(2s), Li∗(3d)+\ensuremathℏ\ensuremathω\ensuremath→Li++e.{\mathrm{Li}}^{*}(3d)+\ensuremath{\hbar}\ensuremath{\omega}\ensuremath{\rightarrow}{\mathrm{Li}}^{+}+e.Li∗(3d)+\ensuremathℏ\ensuremathω\ensuremath→Li++e. Cross-section magnitude and form of the intensity profile are described by a simple three-level model. These results suggest that polarization of the laser field together with collisional two-photon ionization may be used to delineate the shape of individual molecular-state potential curves at long range.
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The authors report the observation of a two-step process in which Na*(4d) is first populated by a radiative collision between Na(3s) and Ba*(6p) in the presence of an intense optical field i.e. Na(3s)+Ba*(6s6p 1 P)+h(cross) omega to Na*(4d)+Ba(6s 2 1 S) followed by photoionisation of the excited sodium Na*(4d)+h(cross) omega to Na + +e. The peak ion intensity is observed at a laser frequency close to the energy difference between Na*(4d) and Ba*(6s6p 1 P), and the magnitude of the cross section for the first step agrees well with theory.
The results of double-laser experiments in which Na2+{\mathrm{Na}}_{2}^{+}Na2+​ and Na+{\mathrm{Na}}^{+}Na+ are produced in crossed alkali beams under single-collision conditions in the presence of strong optical fields are reported. Structure in the mass-selected product ion intensity as a function laser frequency is observed when the optical field is strongly focused and tuned far off atomic or dimer transitions. These measurements are the first to show that the nuclear motion of the quasimolecular collision intermediate plays an important role in laser-induced collisional ionization.
We observe the production of Na2+ and Na+ arising from single collisions between crossed beams of sodium atoms when a laser field is tuned near the Na(3p 2P3/2) and Na(3p 2P1/2) transitions. Measurements of ion intensity vs laser intensity show that at moderately high power true laser-induced processes dominate over purely collisional effects. Relative intensity of mass-selected ions produced at either member of the Na resonance doublet shows conclusively that Na+ does not arise simply from photodissociation of Na2+ but must result from a direct, laser-induced collisional ionization.
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Abstract We study the three-photon ionization of atomic lithium by intense, short light pulses, via numerically solving the time-dependent Schrödinger equation. Two-photon Rabi oscillations are induced between the 2s and 4s states, which are damped due to single-photon ionization to the p continuum. Developing a minimal three-level model, we analyze the spectral features of the Autler–Townes (AT) doublet that is formed upon the resonant coupling with the laser pulse. Furthermore, we show that this 2 s →→ 4 s → p c o n t i n u u m pathway is the dominant process, if the duration of the laser pulse exceeds a certain value. For shorter pulses, ionization through the 2p state ( 2 s → 2 p → 4 d → f c o n t i n u u m ) gradually becomes the dominant process, provided that the pulse is strong enough to induce several Rabi floppings. Here, we trace the competition of these ionization pathways by observing the structural changes in the shape of the AT doublet.