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Physical Review Letters

Strong Field Multiphoton Inversion of a Three-Level System Using Shaped Ultrafast Laser Pulses

Stephen D. Clow, Carlos A Trallero-Herrero, Thomas H. Bergeman, Thomas C. Weinacht

Published Jun 12, 2008• 34 citations
Publisher

Abstract

We demonstrate strong-field population inversion in a three-level system with single and multiphoton coupling between levels using a single shaped ultrafast laser pulse. Our interpretation of the pulse shape dependence illustrates the difference between sequential population transfer and adiabatic rapid passage in three-level systems with multiphoton coupling between levels.

DOI
10.1103/physrevlett.100.233603

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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.
In this thesis, we present work on coherent control of multilevelquantum systems in the strong field limit using shaped ultrafastlaser pulses. In recent years there have been numerous multiphotonabsorption experiments in two,three, and four-level atomic/molecularsystems and many are performed in the limit of weak fields whereperturbation theory is valid. Here, we describe a series ofexperiments aimed at exploring and understanding multiphotontransitions when the exciting field is strong and perturbationtheory breaks down. Our approach to strong field control utilizesboth parameterized scans of various pulse shapes and closed-looplearning control to identify a pulse shape that is optimal forpopulating a target quantum state. With this we will highlight thedifference between sequential population transfer and adiabaticrapid passage in multilevel systems with multiphoton couplingbetween levels. Additionally, we examine strong field control of afour-level atomic interferometer and show how interference in atarget state changes from resonant pathways in the frequency domainto time-domain interference via a singe path.Further, we use shaped femtosecond pulses to demonstrate aphenomenon in which a three-level atom becomes a modulator of anultrafast pulse. The results are based on a pump-probe scheme thatis very similar to Electromagnetically Induced Transparency (EIT).Important dynamics associated with a time-dependent coupling fieldare examined. Lastly, we extend previous work on two-photon drivensuperfluorescence from a shaped ultrafast drive laser and show howstimulated emission near threshold can turn modest coherent controlyields into essentially perfect discrimination between systems wherea control factor of about 104 is achieved between atomic andmolecular species.
We present a simple model for calculating strong-field atomic and molecular ionization dominated by Freeman resonances. Our model combines multiphoton coupling between bound states, including dynamic Stark shifts, with coupling to a discretized continuum. The simplicity of the model allows us to interpret pulse-shape-dependent strong-field ionization yields and to demonstrate the relevance of strong-field atomic or molecular phase matching to ionization, as well as bound-state population transfer. Comparison with experimental measurements demonstrates that the calculations capture the essence of the pulse-shape-dependent ionization yields.
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.
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.