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

https://iopscience.iop.org/article/10.1088/1367-2630/12/7/075008/pdf

Control of quantum phenomena: past, present and future

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. The current experimental successes would be impossible without the development of intense femtosecond laser sources and pulse shapers. The two most critical theoretical insights were (1) realizing that ultrafast atomic and molecular dynamics can be controlled via manipulation of quantum interferences and (2) 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, 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 adaptive feedback control experiments is guided by a learning algorithm, with stochastic methods proving to be especially effective. Adaptive feedback control 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 prospective of open research directions that are likely to attract significant attention in the future.

Control of quantum phenomena: Past, present, and future

Beyond the Floquet theorem: generalized Floquet formalisms and quasienergy methods for atomic and molecular multiphoton processes in intense laser fields

The active steering of the pathways taken by chemical reactions and the optimization of energy conversion processes provide striking examples of the coherent control of quantum interference through the use of shaped laser pulses. Experimentally, coherence is usually established by synchronizing a subset of molecules in an ensemble with ultra-short laser pulses. But in complex systems where even chemically identical molecules exist with different conformations and in diverse environments, the synchronized subset will have an intrinsic inhomogeneity that limits the degree of coherent control that can be achieved. A natural-and, indeed, the ultimate-solution to overcoming intrinsic inhomogeneities is the investigation of the behaviour of one molecule at a time. The single-molecule approach has provided useful insights into phenomena as diverse as biomolecular interactions, cellular processes and the dynamics of supercooled liquids and conjugated polymers. Coherent state preparation of single molecules has so far been restricted to cryogenic conditions, whereas at room temperature only incoherent vibrational relaxation pathways have been probed. Here we report the observation and manipulation of vibrational wave-packet interference in individual molecules at ambient conditions. We show that adapting the time and phase distribution of the optical excitation field to the dynamics of each molecule results in a high degree of control, and expect that the approach can be extended to achieve single-molecule coherent control in other complex inhomogeneous systems.

Visualizing and controlling vibrational wave packets of single molecules

The dissociative ionization of ethanol C2H5OH in an intense laser field is investigated with a chirped laser pulse. From the sensitive dependence of the relative yields of the fragment ions on the absolute values of the linear chirp rate, it is shown that the light-dressed potential-energy surface (LDPES) at the singly charged stage governs the nuclear dynamics, and that the nuclear wave packet flow into the breaking of either of the C–C and C–O chemical bonds could be characterized by the holding time thold during which the LDPESs are maintained. It is also understood in term of the holding time that the enhanced ionization into the doubly charged stage followed by the Coulomb explosion at C–C or C–O proceeds when the nuclear wave packet at the singly charged stage reaches the critical distance for the further ionization.

/pdf/dissociative-ionization-of-ethanol-in-chirped-intense-laser-202rqretuq.pdf

Dissociative ionization of ethanol in chirped intense laser fields

Part 1: Coherent - Optimal Control 1. Controlling Molecular Motion: The Molecule Knows Best 2. Variations on the Theme of STIRAP: Control of Chemical Reactions 3. Laser Control of Selective Preparation of Pre-oriented Enantiomers from their Racemate 4. Experimental and Theoretical Studies of the Channel Phase in the Coherent Control of Molecular Processes 5. Four-Wave Mixing and Coherent Control 6. Control of Chemical Reactions by Using Chirped Laser Pulses 7. Selective Excitation Among Closely Lying Multi-Levels 8. Laser Manipulation of Differential Autoionization Yields: Pump-Dump Control Through Coupled Channels 9. Optimal Quantum Control in Dissipative Environments: General Formalism and Pertubative Limits 10. Manifestation of Coherence on Laser Pulse Propagation 11. Double-Pulse Manipulation of Vibrational Wavepackets in HgAr van der Waals Complex 12. Real-time Spectroscopy of Molecular Vibration Using Sub-5-fs Pulses Part 2: Intense Fields 13. Quantum Control by Adaptive Femtosecond Pulse Shaping 14. The Mechanisms of Strong-Field Control of Chemical Reactivity Using Tailored Laser Pulses 15. Laser-Phase Control of Dissociative Ionization of Molecules: Exact Non-Born Oppenheimer Simulations for H +2 16. Molecular Restructuring in Intense Infra-Red Laser Fields 17. Ultrafast Dynamics of Molecules in Intense Laser-light Fields: New Research Directions 18. Intense-Laser-Induced Electron Transfer and Structure Deformation of Molecules Part 3: Alignment and Manipulation 19. Manipulating Molecules via Combined Electrostatic and Pulsed Resonant Laser Fields 20. Prospects for All-Optical Alignment and Quantum State Control of Nonpolar Molecules 21. Alignment of Neutral Molecules by a Strong Nonresonant Linearly-Polarized Laser Field 22. Propensity of Molecules to Spatially Align in Linearly-Polarized, Intense Light Fields

Laser Control and Manipulation of Molecules

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Laser Control and Manipulation of Molecules