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Optics Express

Strong-field quantum control of 2 + 1 photon absorption of atomic sodium

Sangkyung Lee, Jongseok Lim, Chang Yong Park, Jaewook Ahn

Published Jan 24, 2011• 17 citations
Publisher

Abstract

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.

DOI
10.1364/oe.19.002266

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•Aug 1, 2010•1 citation
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 present a joint experimental and theoretical study on strong-field photo-ionization of sodium atoms using chirped femtosecond laser pulses. By tuning the chirp parameter, selectivity among the population in the highly excited states 5p, 6p, 7p and 5f, 6f is achieved. Different excitation pathways enabling control are identified by simultaneous ionization and measurement of photoelectron angular distributions employing the velocity map imaging technique. Free electron wave packets at an energy of around 1 eV are observed. These photoelectrons originate from two channels. The predominant 2 + 1 + 1 resonance enhanced multi-photon ionization (REMPI) proceeds via the strongly driven two-photon transition 4s←←3s, and subsequent ionization from the states 5p, 6p and 7p whereas the second pathway involves 3 + 1 REMPI via the states 5f and 6f. In addition, electron wave packets from two-photon ionization of the non-resonant transiently populated state 3p are observed close to the ionization threshold. A mainly qualitative five-state model for the predominant excitation channel is studied theoretically to provide insights into the physical mechanisms at play. Our analysis shows that by tuning the chirp parameter the dynamics is effectively controlled by dynamic Stark shifts and level crossings. In particular, we show that under the experimental conditions the passage through an uncommon three-state 'bow-tie' level crossing allows the preparation of coherent superposition states.
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 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 compare the results of two strong field coherent control experiments: one which optimizes multi-photon population transfer in atomic sodium (from the 3s to the 4s state, measured by spontaneous emission from the 3p-3s transition) with one that optimizes stimulated emission on the 3p-3s transition in an ensemble of sodium atoms. Both experiments make use of intense, shaped ultrafast laser pulses discovered by a Genetic Algorithm inside a learning control loop. Optimization leads to improvements in the spontaneous and stimulated emission yields of about 444 and 104{10}^{4}104, respectively, over an unshaped pulse. We interpret these results by modeling both the single atom dynamics as well as the stimulated emission buildup through numerical integration of Schr\"odinger's and Maxwell's equations. Our interpretation leads to the conclusion that modest yields for controlling single quantum systems can lead to dramatic effects whenever an ensemble of such systems acts collectively following controlled impulsive 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.