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Physical Review A

Robust optimal control of quantum molecular systems in the presence of disturbances and uncertainties

Hong Zhang, HERSCHEL A. RABITZ

Published Apr 1, 1994• 69 citations
Publisher

Abstract

Recently, systematic optimal control theory has been successfully applied to design optical fields which act on a molecule to guide or transform it into a specifically prescribed state. Under realistic laboratory conditions and for real molecules, it is inevitable that there will exist disturbances and uncertainties in the control optical field, in the molecular Hamiltonian, and in the field-coupling coefficient (e.g., the dipole moment), etc. Therefore, it is important to design an optimal field which is robust to disturbances. In this paper, we provide a method through which the worst possible disturbance to the control process, under certain possible constraints, can be calculated and a corresponding optimal control field designed to be robust to the disturbances. Under disturbances of small amplitude, a perturbation solution to this problem can be applied. Illustrations are given for control of the wave-packet evolution of a diatomic molecule in the presence of disturbances.

DOI
10.1103/physreva.49.2241

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This thesis details work performed on the improvement of experimental control of quantum systems through the use of optimal control theory. We pursue this objective through both conceptual and practical routes. We first devise improved methods of optimal control for quantum systems. We then apply them, as well as more established methods, to experimental situations where robustness to inaccuracy and error is sought. We develop a method for improving the computational efficiency of optimal control theory in the context of quantum control. This approach makes use of the iterative nature of optimisation algorithms, by using perturbation theory to minimise the effort needed to calculate the time propagator associated with a controlled Hamiltonian. We also create a new way of defining a figure of merit when optimising for robustness against error in an experiment. This method specifically applies to errors that have a relatively small effect on the controlled system's Hamiltonian. We compare this with an ensemble method based around randomly sampling several points on the control landscape, and find these methods to be largely equivalent for small errors, with the ensemble method being superior for larger error. On the applied side, we design radio frequency magnetic pulses that create robustness in spin ensembles to inhomogeneous broadening and variations of coupling strength to the control field for two applications. In the first, we create reliable gates in a situation where limitations are imposed on the control that can be applied. In the second application, we design controls for radio frequency magnetic pulses to create a superradiant state in a spin ensemble. Finally, we collaborate with the experiment to measure the electrons electric dipole moment that is being performed at Imperial College London. For this collaboration, we shape the envelope of the radio frequency control pulses used in the experiment to create superpositions of Zeeman and Stark-shifted excited states in YbF molecules. This shaping allows us to impart pre-determined phases to these superpositions, in a manner that is robust to errors in the control pulse envelope. We obtain sets of robust and sensitive pulses that have been sent to the experiment for testing purposes.

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Recently, systematic optimal control theory has been successfully applied to design optical fields which act on a molecule to guide or transform it into a specifically prescribed state. Under realistic laboratory conditions and for real molecules, it is inevitable that there will exist disturbances and uncertainties in the control optical field, in the molecular Hamiltonian, and in the field-coupling coefficient (e.g., the dipole moment), etc. Therefore, it is important to design an optimal field which is robust to disturbances. In this paper, we provide a method through which the worst possible disturbance to the control process, under certain possible constraints, can be calculated and a corresponding optimal control field designed to be robust to the disturbances. Under disturbances of small amplitude, a perturbation solution to this problem can be applied. Illustrations are given for control of the wave-packet evolution of a diatomic molecule in the presence of disturbances.
The design of optimal final-state controllers of quantum-mechanical systems that are insensitive to errors in the molecular Hamiltonian or to errors in the initial state of the system is considered. Control arises through the interaction of the system with an external field; the goal is optimal design of these latter fields for various physical objectives in the presence of system uncertainty. Sensitivity to modeling errors and other uncertainties in the molecular Hamiltonian is minimized by considering averaged costs for a family of Hamiltonian functions H0{\mathit{H}}_{0}H0​(\ensuremath{\alpha}) indexed by the random variable \ensuremath{\alpha} taking values on a compact set in Euclidean space. Similarly, sensitivity of the optimal control to the initial state is minimized by viewing the initial condition as a Hilbert-space-valued random variable and considering an optimization problem with a cost functional that is averaged over the class of initial conditions. A precise formulation of the control problem is given, and its well-posedness is established. Cost propagators are defined to display the dependence of the performance index on the initial conditions explicitly, which allows analytic averaging of initial conditions.The constrained optimization problem is reduced to an unconstrained optimization problem by the introduction of Lagrange-multiplier operators. Necessary conditions for the unconstrained problem provide the basis for a gradient search for an optimal solution. Finite-difference schemes are utilized to provide a numerical approximation of the optimal control problem. Numerical examples are given for final-state control of a diatomic molecule represented by a Morse potential illustrating design for systems with initial-phase uncertainty and parametric uncertainty. The resultant insensitive controllers execute different strategies depending on the design requirements. The controller designed to be insensitive to errors in the initial phases adopts a strategy of phase imprinting during the initial stages of the control interval to compensate for a lack of knowledge of the initial phases. It is also shown that it is not possible to coerce a system from a state with completely random initial phases to a correlated state using the class of averaged controllers considered here. The controller designed to be insensitive to parametric Hamiltonian errors adopts a strategy of amplitude restraint to prevent the wave packet from taking significant excursions into the regions where the potential is uncertain. The interesting structure exhibited by the controllers in response to the different design requirements, and the superior performance of the insensitive controllers when compared with controllers designed at nominal phases and parameters, illustrate the usefulness of the cost-averaging technique for design in the presence of uncertainties.
The optimal control of the path to a specified final state of a quantum-mechanical system is investigated. The problem is formulated as a minimization problem over appropriate function spaces, and the well-posedness of this problem is is established by proving the existence of an optimal solution. A Lagrange-multiplier technique is used to reduce the problem to an equivalent optimization problem and to derive necessary conditions for a minimum. These necessary conditions form the basis for a gradient iterative procedure to search for a minimum. A numerical scheme based on finite differences is used to reduce the infinite-dimensional minimization problem to an approximate finite-dimensional problem. Numerical examples are provided for final-state control of a diatomic molecule represented by a Morse potential. Within the context of this optimal control formulation, numerical results are given for the optimal pulsing strategy to demonstrate the feasibility of wave-packet control and finally to achieve a specified dissociative wave packet at a given time. The optimal external optical fields generally have a high degree of structure, including an early time period of wave-packet phase adjustment followed by a period of extensive energy deposition to achieve the imposed objective. Constraints on the form of the molecular dipole (e.g., a linear dipole) are shown to limit the accessibility (i.e., controllability) of certain types of molecular wave-packet objectives. The nontrivial structure of the optimal pulse strategies emphasizes the ultimate usefulness of an optimal-control approach to the steering of quantum systems to desired objectives.
The control of multilevel quantum systems is sensitive to implementation errors in the control field and uncertainties associated with system Hamiltonian parameters. A small variation in the control field spectrum or the system Hamiltonian can cause an otherwise optimal field to deviate from controlling desired quantum state transitions and reaching a particular objective. An accurate analysis of robustness is thus essential in understanding and achieving model-based quantum control, such as in the control of chemical reactions based on ab initio or experimental estimates of the molecular Hamiltonian. In this paper, theoretical foundations for quantum control robustness analysis are presented from both a distributional perspective---in terms of moments of the transition amplitude, interferences, and transition probability---and a worst-case perspective. Based on this theory, analytical expressions and a computationally efficient method for determining the robustness of coherently controlled quantum dynamics are derived. The robustness analysis reveals that there generally exists a set of control pathways that are more resistant to destructive interferences in the presence of control field and system parameter uncertainty. These robust pathways interfere and combine to yield a relatively accurate transition amplitude and high transition probability when uncertainty is present.
Abstract Quantum robust control—which can employ fast leading order approximations, slower but more accurate asymptotic methods, or a combination thereof for quantification of robustness—enables control of moments of quantum observables and gates in the presence of Hamiltonian uncertainty or field noise. In this paper, we present a generalized quantum robust control theory that extends the previously described theory of quantum robust control in several important ways. We present robust control theory for control of any moment of arbitrary quantum control objectives, introducing moment-generating functions and transfer functions for quantum robust control that generalize the tools of frequency domain response theory to quantum systems, and extend the Pontryagin maximum principle for quantum control to control optimization in the presence of noise in the manipulated amplitudes or phases used to shape the control field. To provide guidelines as to the types of quantum control systems and control objectives for which asymptotic robustness analysis is important for accuracy, we introduce methods for assessing the Lie algebraic depth of quantum control systems, and illustrate through examples drawn from quantum information processing how such accurate methods for quantification of robustness to noise and uncertainty are more important for control strategies that exploit higher order quantum pathways. In addition, we define the relationship between leading order Taylor expansions and asymptotic estimates for quantum control moments in the presence of Hamiltonian uncertainty and field noise, and apply such leading order approximations to significant pathways analysis and dimensionality reduction of asymptotic quantum robust control calculations, describing numerical methods for implementation of these calculations.
Advances in quantum control theory and optimization techniques have made possible a new phenomena of quantum engineering. Chemical reactions can now be dynamically manipulated using first-principles quantum chemical models, in which a laser field, rather than a catalyst, serve as photonic reagents to selectively break a chemical bond and yield products via intramolecular rearrangement. A field pulse may also be designed to perform ultrasensitive spectroscopy, where compounds with very similar chemical properties are differentiated through their unique interaction with resonant and off-resonant photons. Despite significant progress in theoretical and laboratory quantum control, however, quantum engineering remains principally challenging due to manifestation of noise and uncertainties associated with the input and system parameters. Specifically, a small magnitude of variation in the field and Hamiltonian parameters would cause an otherwise optimal field to deviate from controlling desired quantum state transitions and reaching a particular objective. Thus, an accurate analysis of robustness of controlled quantum dynamics followed by a robust control framework is essential in achieving quantum control in a practical setting. In this work, theoretical foundations for quantum control robustness analysis are presented from both a distributional perspective - in terms of moments of the transition amplitude, interferences, and transition probability - and a worst-case perspective. In addition, an evolutionary control strategy for achieving robust control via open- and closed-loop approach are described with its mechanism of convergence elucidated using the robustness analysis method.
This thesis details work performed on the improvement of experimental control of quantum systems through the use of optimal control theory. We pursue this objective through both conceptual and practical routes. We first devise improved methods of optimal control for quantum systems. We then apply them, as well as more established methods, to experimental situations where robustness to inaccuracy and error is sought. We develop a method for improving the computational efficiency of optimal control theory in the context of quantum control. This approach makes use of the iterative nature of optimisation algorithms, by using perturbation theory to minimise the effort needed to calculate the time propagator associated with a controlled Hamiltonian. We also create a new way of defining a figure of merit when optimising for robustness against error in an experiment. This method specifically applies to errors that have a relatively small effect on the controlled system's Hamiltonian. We compare this with an ensemble method based around randomly sampling several points on the control landscape, and find these methods to be largely equivalent for small errors, with the ensemble method being superior for larger error. On the applied side, we design radio frequency magnetic pulses that create robustness in spin ensembles to inhomogeneous broadening and variations of coupling strength to the control field for two applications. In the first, we create reliable gates in a situation where limitations are imposed on the control that can be applied. In the second application, we design controls for radio frequency magnetic pulses to create a superradiant state in a spin ensemble. Finally, we collaborate with the experiment to measure the electrons electric dipole moment that is being performed at Imperial College London. For this collaboration, we shape the envelope of the radio frequency control pulses used in the experiment to create superpositions of Zeeman and Stark-shifted excited states in YbF molecules. This shaping allows us to impart pre-determined phases to these superpositions, in a manner that is robust to errors in the control pulse envelope. We obtain sets of robust and sensitive pulses that have been sent to the experiment for testing purposes.