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Advances in Optical Materials

Quantum Control of Strong-Field Ladder Climbing in Atomic Sodium

Sangkyung Lee, Jongseok Lim, Jaewook Ahn

Published Jan 1, 2011• 0 citations
Publisher

Abstract

We demonstrate quantum control of energy-level ladder climbing in Sodium 4s and 7p states in the strong-field regime, by spectro-temporal ultrafast pulse shaping. Dressed state picture model calculations show good agreements with the experiment.
DOI
10.1364/hilas.2011.hwc11

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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 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.
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Simple analytical approaches for implementing strong field coherent control schemes are often elusive due to the complexity of the interaction between the intense excitation field and the system of interest. Here, we demonstrate control over multiphoton excitation in a three-level resonant system using simple, analytically derived ultrafast pulse shapes. We utilize a two-dimensional spatiotemporal control technique, in which temporal focusing produces a spatially dependent quadratic spectral phase, while a second, arbitrary phase parameter is scanned using a pulse shaper. In the current work, we demonstrate weak-to-strong field excitation of 85Rb^{85}\mathrm{Rb}85Rb, with a $\ensuremath{\pi}$ phase step and the quadratic phase as the chosen control parameters. The intricate dependence of the multilevel dynamics on these parameters is exhibited by mapping the data onto a two-dimensional control landscape. Further insight is gained by simulating the complete landscape using a dressed-state, time-domain model, in which the influence of individual shaping parameters can be extracted using both exact and asymptotic time-domain representations of the dressed-state energies.