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Conference on Lasers and Electro-Optics

Intensity Invariance of Strong-Field Two-Photon Absorption

Sangkyung Lee, Jongseok Lim, Vahe Hakobyan, S. Guérin, Jaewook Ahn

Published Jan 1, 2010• 0 citations
Publisher

Abstract

We demonstrate experimentally and theoretically the intensity - invariant scaling formula of coherent control of two - photon absorption as a function of pulse–shape parameters of ultrafast laser field in the strong - interaction regime .
DOI
10.1364/qels.2010.qtue6

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We demonstrate the ultrafast coherent control of a nonlinear two-photon absorption in a dynamically shifted energy level structure. We use a spectrotemporal laser-pulse shaping that is programed to preserve the resonant absorption condition during the intense laser-field interaction. Experiments carried out in the strong-field regime of two-photon absorption in the ground state of atomic cesium reveal that the analytically obtained offset and curvature of a laser spectrum compensate the effect of both static and dynamic energy shifts of the given light-atom interaction.
We have considered an analytical control of two-photon absorption process of atoms in the strong-field interaction regime. The experiment was performed on gaseous cesium atoms strongly interacting with a shaped laser-pulse from a femtosecond laser amplifier and a programmable pulse-shaper. When this shaped laser-pulse transfers the atomic population from the 6s ground state to the 8s excited state, we have found that both positively- and negatively-chirped laser pulses, compared with a Gaussian pulse, enhance this excitation in the strong-field regime of laser-atom interaction. This unusual phenomena is explained because the temporal shape of the laser intensity compensates the effect of dynamic Stark shift for the two-photon resonant condition to be optimally maintained. We provide analytic calculations using the strong-field phase matching, which show good agreement with the experiment.
Coherent control of femtosecond two-photon absorption in the intermediate-field regime is analyzed in detail in the powerful frequency domain using an extended 4th-order perturbative description. The corresponding absorption is coherently induced by the weak-field non-resonant two-photon transitions as well as by four-photon transitions involving three absorbed photons and one emitted photons. The interferences between these two groups of transitions lead to a difference between the intermediate-field and weak-field absorption dynamics. The corresponding interference nature (constructive or destructive) strongly depends on the detuning direction of the pulse spectrum from half the two-photon transition frequency. The model system of the study is atomic sodium, for which both experimental and theoretical results are obtained. The detailed understanding obtained here serves as a basis for coherent control with rationally-shaped femtosecond pulses in a regime of sizable absorption yields.