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From molecular control to quantum technology with the dynamic Stark effect

Philip J. Bustard, Guorong Wu, Rune Lausten, Dave Townsend, Ian A. Walmsley, Albert Stolow, Benjamin Sussman

Published Jan 1, 2011• 11 citations
Publisher

Abstract

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.

DOI
10.1039/c1fd00067e

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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.
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.
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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.
Recent advances in the ultrashort laser technology have spawned a series of new directions of research in atomic and molecular physics. This work compounds two studies on the control and probing of atomic matter by ultrafast laser pulses. The first study is concerned with the control of quantum wavepackets focusing by chirped, ultrashort laser pulses. The ability to control wavepacket focusing is important for the achievement of specific excitation pathways, for controlling chemical reactivity or even molecular synthesis. In this work, we present a general method for wavepacket control in the weak field limit. Numerical simulations involving the ICN molecule confirm our theoretical framework. The second study refers to the ionization of sodium Rydberg states via half-cycle pulses (HCPs). For this process, our full quantum-mechanical calculations demonstrate an asymmetry in both ionization rates and ionization spectrum between the downhill (Stark red-shifted) and uphill (Stark blue- shifted) states. The asymmetry is explained by appealing to a semi-classical model of the interfering ionization pathways.
Irradiation of a medium with non-resonant light leads to a shift of the energy levels in the system. This optical, or dynamical Stark effect has been studied for many years in atomic gases. It is only recently, however, that it could be detected for excitonic transitions in solids. This development has stirred considerable interest, because the optical Stark effect has inherent features which makes it well suited for applications such as in ultrafast all-optical data processing. Since the pump light beam falls in a transparency region of the medium, it experiences little loss, in contrast to optical non-linearities based on a saturation mechanism. Also, because virtual transitions are involved, the light-induced shift of exciton levels follows closely the pump pulse duration, making it possible to design ultrafast all-optical logic gates with subpicosecond switch-on and -off times.
The use of laser pulses to alter the internal quantum structure of individual atoms and molecules has applications in quantum information processing, the coherent control of chemical reactions and in quantum-state engineering. This book presents the underlying theory of such quantum-state manipulation for researchers and graduate students. The book provides the equations, and approaches for their solution, which can be applied to complicated multilevel quantum systems. It also gives the background theory for application to isolated atoms or trapped ions, simple molecules and atoms embedded in solids. Particular attention is given to the ways in which quantum changes can be displayed graphically to help readers understand how quantum changes can be controlled.