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Reports on Progress in Physics

Coherent control of molecular dynamics

Moshe Shapiro, Paul W. Brumer

Published May 13, 2003• 213 citations
Publisher

Abstract

We review the principles and some recent advances in the theory of coherent control of molecular processes and discuss some of its experimental realizations. Amongst the topics discussed are: bichromatic and pump-dump control; the interference between N-photons and M-photon processes; the optical conversion of a mixture of left- and right-handed chiral molecules into an ensemble containing molecules of the handedness of choice; control of collisional processes; control over chaotic dynamics; effects of decoherence; the solution of the non-degenerate quantum control problem; and control over spontaneous emission and other decay processes.

DOI
10.1088/0034-4885/66/6/201

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We review the principles and some recent advances in the theory of coherent control of molecular processes and discuss some of its experimental realizations. Amongst the topics discussed are: bichromatic and pump-dump control; the interference between N-photons and M-photon processes; the optical conversion of a mixture of left- and right-handed chiral molecules into an ensemble containing molecules of the handedness of choice; control of collisional processes; control over chaotic dynamics; effects of decoherence; the solution of the non-degenerate quantum control problem; and control over spontaneous emission and other decay processes.
Preface.Preliminaries of the Interaction of Light with Matter.Weak-Field Photodissociation.Weak-Field Coherent Control.Optimal Control Theory.Decoherence and Loss of Control.Case Studies in Coherent Control.Coherent Control of Bimolecular Processes.Coherent Control of the Synthesis and Purification of Chiral Molecules.Coherent Control Beyond the Weak-Field Regime: Bound States and Resonances.Photodissociation Beyond the Weak-Field Regime.Coherent Control Beyond the Weak-Field Regime: The Continuum.Strong-Field Coherent Control.Case Studies in Optimal Control.References.Author Index.Subject Index.
Abstract Rather different problems can be lumped together under the general term 'laser control of atoms and molecules'. They include the laser selection of atomic and molecular velocities for the purpose of Doppler-free spectroscopy, laser control of the position and velocity of atoms (i.e. laser trapping and cooling of atoms), and laser control of atomic and molecular processes (ionization, dissociation) with a view of detecting single atoms and molecules and particularly separating isotopes and nuclear isomers. Over the last decades the principal problems posed have been successfully solved, and many of them have evolved remarkably in the subsequent investigations of the international research community. For example, the solution of the problem of laser cooling and trapping of atoms has given birth to the new field of the physics of ultracold matter, i.e. quantum atomic and molecular gases. The laser non-coherent control of uni-molecular processes has found an interesting extension in the field of laser coherent control of molecules. The concept of laser control of position has been successfully demonstrated with microparticles (optical tweezers), concurrently with investigations into atomic control. The laser photo-ionization of molecules on surfaces has led to the development of novel techniques of laser-assisted mass spectrometry of macromolecules, and so on. The aim of this book is to review these topics from a unified or 'coherent' point of view. It will be useful for many readers in various fields of laser science and its applications.
We review recent applications of quantum control on molecular switches by optical means. We discuss diverse examples, as detection and automatic switching between nucleotide base-pairs and their undesired mutants, controlled operation of multi-configurational molecular devices for quantum information storage, and switching between the two enantiomeric forms of a chiral molecule. The variety of examples discussed demonstrates the wide range of applicability and the power of optical quantum control techniques in the fast emerging field of molecular devices.
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.