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International Conference on Information Photonics

From molecular control to quantum technology with the dynamic stark effect

Philip J. Bustard, Benjamin Sussman

Published May 1, 2011• 0 citations
Publisher

Abstract

The application of nonresonant lasers to quantum systems can modify energy levels in a general way. This approach, using the nonresonant dynamic Stark effect, is an effective mechanism for modifying chemical dynamics. These molecular techniques have analogous implementations in quantum technologies. Applications include controlling vacuum fluctuations to create molecular alignment and broadband light sources, photonic catalysis, quantum memories in atomic vapours, and photonics in bulk diamond phonons. The links between these different applications are investigated.

DOI
10.1109/ico-ip.2011.5953734

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The application of nonresonant lasers to quantum systems can modify energy levels in a general way. This approach, using the nonresonant dynamic Stark effect, is an effective mechanism for modifying chemical dynamics. These molecular techniques have analogous implementations in quantum technologies. Applications include controlling vacuum fluctuations to create molecular alignment and broadband light sources, photonic catalysis, quantum memories in atomic vapours, and photonics in bulk diamond phonons. The links between these different applications are investigated.
The non-resonant dynamic Stark effect is a powerful and general way of manipulating ultrafast processes in atoms, molecules, and solids with exquisite precision. We discuss the physics behind this effect, and demonstrate its efficacy as a method of control in a variety of systems. These applications range from the control of molecular rotational dynamics to the manipulation of chemical reaction dynamics, and from the suppression of vacuum fluctuation effects in coherent preparation of matter, to the dynamic generation of bandwidth for storage of broadband quantum states of light.
Nonperturbative quantum control schemes in the intermediate field strength (nonionizing) regime are investigated. We restrict the matter-field interaction to the nonresonant dynamic Stark effect (NRDSE) as induced by infrared laser fields, which we argue is a new and general tool for quantum control of atomic and molecular dynamics. For the case of Raman coupled matter states, an effective Hamiltionian may be constructed, and quantum control via NRDSE may be thought of as reversibly modifying the effective Hamiltonian during system propagation, thus leading to control over dynamic processes. As an illustration, the creation of field-free ``switched'' wave packets through the adiabatic turn on and sudden turn off of the NRDSE is considered and experimentally demonstrated. Wave packets generated through the switched NRDSE interaction may be very different in form and content than wave packets generated via resonant transitions with Gaussian optical pulses. In order to provide an example, we discuss the specific case of rotational wave packet dynamics where the NRDSE manifests itself as molecular axis alignment. This technique is applied to the creation of field-free molecular axis alignment using an intense switched $1.064\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}$ laser pulse. This switched laser pulse was generated via a plasma shuttering technique, giving a pulse with a rise time of 150ps150\phantom{\rule{0.3em}{0ex}}\mathrm{ps}150ps and a fall time of 170fs170\phantom{\rule{0.3em}{0ex}}\mathrm{fs}170fs. The temporal evolution of the molecular axis alignment is probed via the optical Kerr effect. Field-free alignment via the switched NRDSE is demonstrated for both linear (CO2\mathrm{C}{\mathrm{O}}_{2}CO2​, CS2\mathrm{C}{\mathrm{S}}_{2}CS2​) and symmetric top (1,2-propadiene) polyatomic molecules.
The dynamic Stark effect due to a strong nonresonant but nonionizing laser field provides a route to quantum control via the creation of novel superposition states. We consider the creation of a field-free "switched" wave packet through adiabatic turn-on and sudden turn-off of a strong dynamic Stark interaction. There are two limiting cases for such wave packets. The first is a Raman-type coupling, illustrated by the creation of field-free molecular axis alignment. An experimental demonstration is given. The second case is that of dipole-type coupling, illustrated by the creation of charge localization in an array of quantum wells.
Over the past years, the development of experimental techniques for the coherent manipulation and control of isolated quantum systems has made impressive progress. Such 'quantum-logic' methods are also highly attractive in a chemical context in view of unravelling and controlling the quantum dynamics of molecular collisions and chemical reactions. Quantum technologies have the potential to transform the way chemical dynamics are investigated - by providing highly sensitive methods for state readout and spectroscopy, by opening up new pathways for the quantum-state preparation of molecules and by enabling an improved control of their microscopic behavior on the single-particle level. However, for complex quantum systems like molecules, these techniques are still in their infancy and their considerable potential remains to be unlocked. The aim of the present research program supported by an Advanced Grant of the Swiss National Science Foundation is to merge the fields of quantum science and chemical dynamics by advancing quantum technologies to polyatomic molecular ions and by applying them to the study of ion-molecule collisions and chemical reactions. In this article, we review the salient experimental methods as well as prospects and challenges in the development of molecular quantum technologies and their applications to chemistry.
We give a review on the development of quantum manipulation techniques in molecular dynamics and their technological classification and effectiveness.The analysis and comparison are based on the principles of technologies and the characteristics of implementation.The topics include the π pulse dynamics and interference path control schemes in frequency domain,and the laser pulse shaping technology.The macroscopic control theories of molecular dynamic control are also discussed and evaluated,which includes system modeling,analysis and synthesis,geometric control,control of unitary evolution matrix,quantum optimal control theory,quantum control methods based on Lyapunov method.The paper provides a panorama of the quantum manipulation techniques and the applications of control theory in molecular dynamics.