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Principles of the Quantum Control of Molecular Processes

Moshe Shapiro, Paul W. Brumer

Published Mar 7, 2003• 575 citations
OpenAlex

Abstract

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.

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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.
Written by two of the world's leading researchers in the field, this is a systematic introduction to the fundamental principles of coherent control, and to the underlying physics and chemistry.This fully updated second edition is enhanced by 80% and covers the latest techniques and applications, including nanostructures, attosecond processes, optical control of chirality, and weak and strong field quantum control. Developments and challenges in decoherence-sensitive condensed phase control as well as in bimolecular control are clearly described.Indispensable for atomic, molecular and chemical
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. Part I: Atomic and Molecular systems. Scenarios in Coherent Control P. Brumer, M. Shapiro. Quantum Control in Atomic Systems D. Charalambidis, et al. Laser-phase-sensitive Coherent Control of Photoion Product States in 2-Photon vs. 2-Photon Ionization of Atomic Barium, F. Wang, et al. Coherent Phase control of Photoionization and Photodissociation R.J. Gordon, et al. Coherent Control of Atomic Photoionization and Autoionization P. Lambropoulos, T. Nakajima. Lasing Without Inversion via Interference of Double-Dark Resonances in Atomic and Quantum Well Systems M.O. Scully, et al. Part II: Coherent Control in Semiconductors. Coherence Control of Free Carriers in Bulk Semiconductors H.M. van Driel, et al. Coherent Control of 2D Excitons Probed by Time-Resolved Secondary Emission X. Marie, et al. Many-Body Effects in the Ultrafast Population Transfer in p-Doped Semiconductor Quantum Wells R. Binder, M. Lindberg. Coherent Control of Heavy-Light Hole and Phonon Quantum Beats T. Kuhn, et al. Coherent Control Schemes in Semiconductor Double Wells X. Hu, W. Poetz. Terahertz-Control of Charge-Carrier Wavepackets in Semiconductor Quantum Wells S. Hughes, D.S. Citrin. Microcavity Exciton-Polariton H. Cao. Part III: Coherent Phenomena and Related Topics. Coherent Control of Quantum Localization M. Holthaus. Tunneling of Low-Energetic Electrons in the Presence of Intense Laser Fields: The Formation of Dynamical Barrier States M. Wagner. Hopping Mechanism of Coherent Photovoltaic Effect and Photoinduced Polar Anisotropy in Glass E.M. Baskin, M.V. Entin. Heterodyning Scheme Employing Quantum Interference J.B. Khurgin, et al. Generation of Widely Tunable THz-Wave Using Nonlinear Optics K. Kawase, H.Ito. List of Participants.
The subtle and fundamental issue of indistinguishability and interference between independent pathways to the same target state is examined in the context of coherent control of atomic and molecular processes, with emphasis placed on possible "which-way" information due to quantum entanglement established in the quantum dynamics. Because quantum interference between independent pathways to the same target state occurs only when the independent pathways are indistinguishable, it is first shown that creating useful coherence between nondegenerate states of a molecule for subsequent quantum interference manipulation cannot be achieved by collisions between atoms or molecules that are prepared in momentum and energy eigenstates. Coherence can, however, be transferred from light fields to atoms or molecules. Using a particular coherent control scenario, it is shown that this coherence transfer and the subsequent coherent phase control can be readily realized by the most classical states of light, i.e., coherent states of light. It is further demonstrated that quantum states of light may suppress the extent of phase-sensitive coherent control by leaking out some which-way information while "incoherent interference control" scenarios proposed in the literature have automatically ensured the indistinguishability of multiple excitation pathways. The possibility of quantum coherence in photodissociation product states is also understood in terms of the disentanglement between photodissociation fragments. Results offer deeper insights into quantum coherence generation in atomic and molecular processes.
The interaction of strong laser fields with matter causes light-shifts that play an important role in many fields as quantum optics, molecular physics and chemistry. Here the control results from the interference between two excitation quantum paths, corresponding to the absorption and to the emission by the dressed atomic system of one photon from/on the weak field mode respectively. This effect paves the way to many applications and we will describe a new method to slow the light in an atomic medium.
Chemical reactions at temperatures near absolute zero require a full quantum description of the reaction pathways and enable enhanced control of the products via quantum state selection. Ultracold molecule experiments have provided initial insight into the quantum nature of basic chemical processes involving diatomic molecules, for example from studies of bimolecular reactions, but complete control over the reactants and products has remained elusive. The half-collision process of photodissociation is an indispensable tool in molecular physics and offers significantly more control than the reverse process of photoassociation. Here we reach a fully quantum regime with photodissociation of ultracold 88^{88}88Sr2_22​ molecules where the initial bound state of the molecule and the target continuum state of the fragments are strictly controlled. Detection of the photodissociation products via optical absorption imaging reveals the hallmarks of ultracold chemistry: resonant and nonresonant barrier tunneling, importance of quantum statistics, presence of forbidden reaction pathways, and matter wave interference of reaction products. In particular, this interference yields fragment angular distributions with a strong breaking of cylindrical symmetry, so far unobserved in photodissociation. We definitively show that the quasiclassical description of photodissociation fails in the ultracold regime. Instead, a quantum model accurately reproduces our results and yields new intuition.