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Journal of the Optical Society of America B

Adaptive real-time femtosecond pulse shaping

Doron Meshulach, Dvir Yelin, Yaron R. Silberberg

Published May 1, 1998• 89 citations
Publisher

Abstract

Experimental results of a practical self-learning pulse-shaping system are presented. Real-time adaptive pulse shaping of uncharacterized pulses is achieved. A cross-correlation feedback measurement of the output pulses is used by a simulated-annealing algorithm to modify the pulses iteratively toward target shapes. This scheme can readily be used for coherent control of quantum dynamics.

DOI
10.1364/josab.15.001615

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Experimental results of a practical self-learning pulse-shaping system are presented. Real-time adaptive pulse shaping of uncharacterized pulses is achieved. A cross-correlation feedback measurement of the output pulses is used by a simulated-annealing algorithm to modify the pulses iteratively toward target shapes. This scheme can readily be used for coherent control of quantum dynamics.
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We have constructed an automated learning apparatus to control quantum systems. By directing intense shaped ultrafast laser pulses into a variety of samples and using a measurement of the system as a feedback signal, we are able to reshape the laser pulses to direct the quantum system into a desired physical state. The feedback signal is the input to an adaptive learning algorithm. This algorithm programs a computer-controlled, acousto-optic modulator (AOM) pulse shaper. The learning algorithm generates new shaped laser pulses based on the success of previous pulses in achieving a predetermined goal.
Coherent control of quantum phenomena can be achieved by using phase- and amplitude modulated laser pulses. With a self-learning loop, which combines a femtosecond pulse shaper, an optimization algorithm and an experimental feedback signal, it is possible to automatically steer the interaction between system and electric field. This approach allows control even without any knowledge of the Hamiltonian. We have successfully implement this learning loop for the coherent control of the nonresonant two-photon excitation in sodium. New solutions for 'bright' and 'dark' pulses could be designed for this two-photon resonance without previous knowledge of the resonances. In a further experiment we combined the self-learning loop with degenerate four-wave-mixing spectroscopy in order to study the influence of phase and amplitude modulated pulses on the molecular FWM response of the prototype system K2. The obtained control pulses typically show a complex structure which hides the responsible physical mechanism. In order to extract the applied mechanism the concept of parameterization has been introduced which allows the learning algorithm to optimize already known control processes. Therefore the control of vibrational wavepacket motion in the electronic ground and excited state could be attributed to chirped pulse excitation, impulsive Raman excitation by pulse trains and phase-related double pulses representing the well-known Tannor-Rice-Kosloff control scheme.
Summary form only given. Many realized or potential applications of optically driven ultrafast quantum dynamics require specially shaped quantum states, with the ability to detect these shapes and modify them using active feedback. We have developed methods to sculpt wave packets using shaped ultrafast optical pulses. We can also view these wave packets using quantum interference methods that have been adapted from holographic techniques used to characterize classical light. These quantum state holograms have been used as feedback to sculpt specific target shapes.
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.