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Physical Review A

Coherent control of strong field multiphoton absorption in the presence of dynamic Stark shifts

Carlos A Trallero-Herrero, David Cardoza, Thomas C. Weinacht, J. L. Cohen

Published Jan 28, 2005• 70 citations
Publisher

Abstract

We show that coherent control of multiphoton transitions is possible in the strong field limit, even in the presence of large dynamic Stark shifts. By tailoring the phase of an ultrafast laser pulse, one can compensate for the dynamic Stark shift during the atom-field interaction to achieve efficient population transfer in two-photon absorption. Numerical simulations for atomic sodium reveal efficient population transfer from the $\ensuremath{\mid}3s⟩$ ground state to the $\ensuremath{\mid}4s⟩$ excited state using an appropriately shaped ultrafast laser pulse. The theory and simulations provide insight into coherent control of more complicated multiphoton processes.

DOI
10.1103/physreva.71.013423

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We show that coherent control of multiphoton transitions is possible in the strong field limit, even in the presence of large dynamic Stark shifts. By tailoring the phase of an ultrafast laser pulse, one can compensate for the dynamic Stark shift during the atom-field interaction to achieve efficient population transfer in two-photon absorption. Numerical simulations for atomic sodium reveal efficient population transfer from the \ensuremath∣3s⟩\ensuremath{\mid}3s⟩\ensuremath∣3s⟩ ground state to the \ensuremath∣4s⟩\ensuremath{\mid}4s⟩\ensuremath∣4s⟩ excited state using an appropriately shaped ultrafast laser pulse. The theory and simulations provide insight into coherent control of more complicated multiphoton processes.
We trace out the transition from weak- to strong-field coherent control, focusing on multiphoton population transfer in atomic sodium. We show how dynamic Stark shifts and ground-state depletion mark the departure from perturbative to strong-field excitation, and how a time-domain picture yields insight into the dynamics when a static resonance, frequency-domain approach breaks down. Experimental measurements are interpreted with the help of calculations that numerically integrate the Schr\"odinger equation.
We demonstrate ultrafast coherent control of multiphoton absorption in a dynamically shifted energy level structure. In a three-level system that models optical interactions with sodium atoms, we control the quantum interference of sequential 2 + 1 photons and direct three-photon transitions. Dynamic change in energy levels predicts an enormous enhancement of |7p>-state excitation in the strong-field regime by a negatively chirped pulse. In addition, the |4s>-state excitation is enhanced symmetrically by nonzero linear chirp rates given as a function of laser peak intensity and laser detuning. Experiments performed by ultrafast shaped-pulse excitation of ground-state atomic sodium verifies the various strong-field contributions to |3s>-|7p> and |3s>-|4s> transitions. The result suggests that for systems of molecular level understanding adiabatic control approach with analytically shaped pulses becomes a more direct control than feedback-loop black-box approaches.
We demonstrate a population inversion in a three-level system via three-photon absorption from a single shaped ultrafast laser pulse. The optimal pulse shape for the inversion is discovered using closed-loop learning control and interpreted via pulse shape parameter scans and numerical integration of the Schrödinger equation. The population inversion is measured using a combination of spontaneous and stimulated emissions. Our results illustrate the importance of dynamic Stark shifts in coherent multi-photon excitation.
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.
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