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Physical Review Letters

Quantum Control of Tightly Competitive Product Channels

Matthias Roth, Laurent Guyon, Jonathan Roslund, Véronique Boutou, François Courvoisier, Jean‐Pierre Wolf, HERSCHEL A. RABITZ

Published Jun 22, 2009• 111 citations
Publisher

Abstract

Fundamental selectivity limits of quantum control are pushed by introducing laser driven optimal dynamic discrimination to create distinguishing excitations on two nearly identical flavin molecules. Even with modest spectral resources, significant specificity is achieved with optimal pulse shapes, which amplify small molecular differences to create distinct, identifying signals. Rather than being a hindrance, system complexity appears to aid the control process and augments control field capability, which bodes well for implementation of quantum control in a variety of demanding applications.

DOI
10.1103/physrevlett.102.253001

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Fundamental selectivity limits of quantum control are pushed by introducing laser driven optimal dynamic discrimination to create distinguishing excitations on two nearly identical flavin molecules. Even with modest spectral resources, significant specificity is achieved with optimal pulse shapes, which amplify small molecular differences to create distinct, identifying signals. Rather than being a hindrance, system complexity appears to aid the control process and augments control field capability, which bodes well for implementation of quantum control in a variety of demanding applications.
Fundamental selectivity limits of quantum control are pushed by introducing laser driven optimal dynamic discrimination to create distinguishing excitations on two nearly identical flavin molecules.Even with modest spectral resources, significant specificity is achieved with optimal pulse shapes, which amplify small molecular differences to create distinct, identifying signals.Rather than being a hindrance, system complexity appears to aid the control process and augments control field capability, which bodes well for implementation of quantum control in a variety of demanding applications.
Control of quantum phenomena has grown from a dream to a burgeoning field encompassing wide-ranging experimental and theoretical activities. Theoretical research in this area primarily concerns identification of the principles for controlling quantum phenomena, the exploration of new experimental applications and the development of associated operational algorithms to guide such experiments. Recent experiments with adaptive feedback control span many applications including selective excitation, wave packet engineering and control in the presence of complex environments. Practical procedures are also being developed to execute real-time feedback control considering the resultant back action on the quantum system. This focus issue includes papers covering many of the latest advances in the field. Focus on Quantum Control Contents Control of quantum phenomena: past, present and future Constantin Brif, Raj Chakrabarti and Herschel Rabitz Biologically inspired molecular machines driven by light. Optimal control of a unidirectional rotor Guillermo Pérez-Hernández, Adam Pelzer, Leticia González and Tamar Seideman Simulating quantum search algorithm using vibronic states of I2 manipulated by optimally designed gate pulses Yukiyoshi Ohtsuki Efficient coherent control by sequences of pulses of finite duration Götz S Uhrig and Stefano Pasini Control by decoherence: weak field control of an excited state objective Gil Katz, Mark A Ratner and Ronnie Kosloff Multi-qubit compensation sequences Y Tomita, J T Merrill and K R Brown Environment-invariant measure of distance between evolutions of an open quantum system Matthew D Grace, Jason Dominy, Robert L Kosut, Constantin Brif and Herschel Rabitz Simplified quantum process tomography M P A Branderhorst, J Nunn, I A Walmsley and R L Kosut Achieving 'perfect' molecular discrimination via coherent control and stimulated emission Stephen D Clow, Uvo C Holscher and Thomas C Weinacht A convenient method to simulate and visually represent two-photon power spectra of arbitrarily and adaptively shaped broadband laser pulses M A Montgomery and N H Damrauer Accurate and efficient implementation of the von Neumann representation for laser pulses with discrete and finite spectra Frank Dimler, Susanne Fechner, Alexander Rodenberg, Tobias Brixner and David J Tannor Coherent strong-field control of multiple states by a single chirped femtosecond laser pulse M Krug, T Bayer, M Wollenhaupt, C Sarpe-Tudoran, T Baumert, S S Ivanov and N V Vitanov Quantum-state measurement of ionic Rydberg wavepackets X Zhang and R R Jones On the paradigm of coherent control: the phase-dependent light-matter interaction in the shaping window Tiago Buckup, Jurgen Hauer and Marcus Motzkus Use of the spatial phase of a focused laser beam to yield mechanistic information about photo-induced chemical reactions V J Barge, Z Hu and R J Gordon Coherent control of multiple vibrational excitations for optimal detection S D McGrane, R J Scharff, M Greenfield and D S Moore Mode selectivity with polarization shaping in the mid-IR David B Strasfeld, Chris T Middleton and Martin T Zanni Laser-guided relativistic quantum dynamics Chengpu Liu, Markus C Kohler, Karen Z Hatsagortsyan, Carsten Muller and Christoph H Keitel Continuous quantum error correction as classical hybrid control Hideo Mabuchi Quantum filter reduction for measurement-feedback control via unsupervised manifold learning Anne E B Nielsen, Asa S Hopkins and Hideo Mabuchi Control of the temporal profile of the local electromagnetic field near metallic nanostructures Ilya Grigorenko and Anatoly Efimov Laser-assisted molecular orientation in gaseous media: new possibilities and applications Dmitry V Zhdanov and Victor N Zadkov Optimization of laser field-free orientation of a state-selected NO molecular sample Arnaud Rouzee, Arjan Gijsbertsen, Omair Ghafur, Ofer M Shir, Thomas Back, Steven Stolte and Marc J J Vrakking Controlling the sense of molecular rotation Sharly Fleischer, Yuri Khodorkovsky, Yehiam Prior and Ilya Sh Averbukh Optimal control of interacting particles: a multi-configuration time-dependent Hartree-Fock approach Michael Mundt and David J Tannor Exact quantum dissipative dynamics under external time-dependent driving fields Jian Xu, Rui-Xue Xu and Yi Jing Yan Pulse trains in molecular dynamics and coherent spectroscopy: a theoretical study J Voll and R de Vivie-Riedle Quantum control of electron localization in molecules driven by trains of half-cycle pulses Emil Persson, Joachim Burgdorfer and Stefanie Grafe Quantum control design by Lyapunov trajectory tracking for dipole and polarizability coupling Jean-Michel Coron, Andreea Grigoriu, Catalin Lefter and Gabriel Turinici Sliding mode control of quantum systems Daoyi Dong and Ian R Petersen Implementation of fault-tolerant quantum logic gates via optimal control R Nigmatullin and S G Schirmer Generalized filtering of laser fields in optimal control theory: application to symmetry filtering of quantum gate operations Markus Schroder and Alex Brown
Similar molecules or materials have comparable composition, structure, and other properties thus making them difficult to discriminate for purposes of detection. Although the species may be spectrally similar, they each could have significantly different (quantum) dynamical behavior for detection. Optimal dynamic discrimination (ODD) aims to maximally draw out the differences among similar species by manipulating their molecular dynamics with optimized radiation resources. The highest degrees of discrimination arise upon exploiting control of the quantum dynamics of the species. Theoretical analysis shows that quantum systems differing even infinitesimally in character may be distinguished by means of their dynamics when acted upon by a suitably shaped control field. Simulations have demonstrated the capabilities of optimal discrimination in the presence of laser-pulse noise, signal detection errors, and imperfect signal detection resolution. Recent experiments have demonstrated the feasibility of ODD.
Optimal dynamic discrimination (ODD) uses closed-loop learning control techniques to discriminate between similar quantum systems. ODD achieves discrimination by employing a shaped control (laser) pulse to simultaneously exploit the unique quantum dynamics particular to each system, even when they are quite similar. In this work, ODD is viewed in the context of multiobjective optimization, where the competing objectives are the degree of similarity of the quantum systems and the level of controlled discrimination that can be achieved. To facilitate this study, the D-MORPH gradient algorithm is extended to handle multiple quantum systems and multiple objectives. This work explores the trade-off between laser resources (e.g., the length of the pulse, fluence, etc.) and ODD's ability to discriminate between similar systems. A mechanism analysis is performed to identify the dominant pathways utilized to achieve discrimination between similar systems.
We investigate the problem of control of quantum systems. Various notions of controllability of quantum systems are discussed and Lie algebraic techniques are employed to derive necessary and sufficient conditions for the resulting degrees of controllability. The results are employed to study the degree of controllability for various model systems. The problem of optimal control is formulated as a problem of maximisation of the expectation value of an observable of the system subject to dynamical constraints and costs. A class of iterative algorithms is discussed, and shown to converge to a solution of the Euler-Lagrange equations, which is a necessary condition for optimality of a solution. A numerical realisation of the algorithm is presented and potential implementation of the resulting control fields in the laboratory is discussed. The algorithm is applied to find optimal control fields for a variety of applications including selective and simultaneous excitation of individual quantum dots in a globally addressed ensemble, creation of superposition states, and selective excitation of certain vibrational modes of a simple molecule such as Hydrogen Fluoride. In each case we systematically explore the parameter space of the algorithm to select solutions with desirable physical features from the multitude of possible choices. As there are many possible optimal control fields which give similar yields the question of whether some are more robust than others is investigated. A number of optimal fields are analysed quantitatively in terms of robustness with regard to temporal and spectral noise affecting the fields, uncertainty in the model parameters and the effect of experimental limitations such as restrictions on the bandwidth of the fields. It is shown that whilst the solutions tend to be sensitive to uncertainty in the energy levels chosen for the model, they appear to be surprisingly tolerant to even severe bandwidth limitations.
Selective resonant excitations can be realized with a shaped ultrashort pulse in an optically dense collection of multilevel individual atoms, where the near dipole-dipole interactions induce intrinsic frequency shifts of the atomic resonance. A proper transform-limited pulse and modulation of excitation pulses can be controlled to establish constructive or destructive quantum interference between different excitation pathways towards a desired selective resonant excitation, even driven by pulses with broadband spectral components.