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Science

Whither the Future of Controlling Quantum Phenomena?

HERSCHEL A. RABITZ, Regina de Vivie‐Riedle, Marcus Motzkus, Karl Ludwig Kompa

Published May 5, 2000• 1,150 citations
Publisher

Abstract

This review puts into perspective the present state and prospects for controlling quantum phenomena in atoms and molecules. The topics considered include the nature of physical and chemical control objectives, the development of possible quantum control rules of thumb, the theoretical design of controls and their laboratory realization, quantum learning and feedback control in the laboratory, bulk media influences, and the ability to utilize coherent quantum manipulation as a means for extracting microscopic information. The preview of the field presented here suggests that important advances in the control of molecules and the capability of learning about molecular interactions may be reached through the application of emerging theoretical concepts and laboratory technologies.

DOI
10.1126/science.288.5467.824

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Quantum control is concerned with active manipulation of physical and chemical processes on the atomic and molecular scale. This work presents a perspective of progress in the field of control over quantum phenomena, tracing the evolution of theoretical concepts and experimental methods from early developments to the most recent advances. Among numerous theoretical insights and technological improvements that produced the present state-of-the-art in quantum control, there have been several breakthroughs of foremost importance. On the technology side, the current experimental successes would be impossible without the development of intense femtosecond laser sources and pulse shapers. On the theory side, the two most critical insights were (i) realizing that ultrafast atomic and molecular dynamics can be controlled via manipulation of quantum interferences and (ii) understanding that optimally shaped ultrafast laser pulses are the most effective means for producing the desired quantum interference patterns in the controlled system. Finally, these theoretical and experimental advances were brought together by the crucial concept of adaptive feedback control (AFC), which is a laboratory procedure employing measurement-driven, closed-loop optimization to identify the best shapes of femtosecond laser control pulses for steering quantum dynamics towards the desired objective. Optimization in AFC experiments is guided by a learning algorithm, with stochastic methods proving to be especially effective. AFC of quantum phenomena has found numerous applications in many areas of the physical and chemical sciences, and this paper reviews the extensive experiments. Other subjects discussed include quantum optimal control theory, quantum control landscapes, the role of theoretical control designs in experimental realizations and real-time quantum feedback control. The paper concludes with a perspective of open research directions that are likely to attract significant attention in the future.
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Most quantum systems considered for control by external fields are plagued by a serious lack of complete information about the underlying Hamiltonian. Traditional feedback control techniques are generally not appropriate due to the latter problem, as well as the ultrafast nature of typical quantum dynamics phenomena and the fact that observations of the quantum system will inevitably lead to a disturbance which may often be contradictory to the desired control. In contrast, learning control techniques have a special role to play in the manipulation of quantum dynamics phenomena. The unique capabilities of quantum systems making them amenable to learning control are (a) the ability to have very large numbers of identical systems for submission to control, (b) the high duty cycle of laboratory laser controls, and (c) the ability to observe the impact of trial controls at ultrafast time scales. Various learning algorithms have been proposed to guide this control process. The paper discusses these proposals, as well as some new perspectives.
Abstract Understanding the quantum coherence effects is crucial for their promising applications, such as engineering artificial photosynthesis, manipulating chemical reactions, and designing coherence‐based functional devices. Considering that a molecule is the smallest unit that can exist independently and maintain its physical and chemical properties, investigating the quantum coherence effects of molecules is of great significance in understanding their features. In this case, exploring quantum coherence effects in the interaction of light and molecules has been one of the leading topics. This review presents an overview of state‐of‐the‐art spectroscopic techniques and deep insights into molecular quantum coherence effects. It also offers prospects for future advancement. First, the history of development and origins of quantum coherence effects are briefly introduced in molecules. Then, the principle and exciting experimental progress of sophisticated techniques for investigating molecular quantum coherence effects are discussed. Late, molecular quantum coherence effects and their promising applications in various areas have been evaluated. Finally, the challenges and potential solutions are look ahead for studying the effects of quantum coherence on molecules. This review may offer some guidance to boost the understanding and employing the molecular quantum coherence effects.