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Physica Scripta

Quantum optimal control of molecular coherent states

Abdessamad Belfakir, A. Belhaj, Y. Hassouni, Randa Herzallah, Ahmed Ratnani

Published Nov 21, 2024• 0 citations
Publisher

Abstract

Abstract In this paper, we address the optimal control problem in molecular systems, focusing on transitions within coherent states characterised by complex coefficients. Employing Hölder’s inequality, we establish a mathematical relationship between the energy requirement and the distance separating the initial and the target coherent states. A key part of our study is the application of this framework to the H2O molecule, specifically examining the local OH bond. Here, we demonstrate how energy requirements for the state transitions are influenced by the distance between these states. Furthermore, we investigate the effects of a heat bath coupled to the system, by analysing its impact on transferring the molecular system to different final coherent states. These coherent states are defined as almost eigenvectors of the Generalised Heisenberg Algebra (GHA) annihilation operator. By using the Perolomov approach, another type of coherent states for the Morse potential associated with the GHA can be constructed. By leveraging the GHA structure, we revisit and analyse Morse coherent states previously established for certain diatomic molecules, offering a deeper insight into the dynamics of state transitions under various conditions.

DOI
10.1088/1402-4896/ad94ab

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Abstract In this paper, we address the optimal control problem in molecular systems, focusing on transitions within coherent states characterised by complex coefficients. Employing Hölder’s inequality, we establish a mathematical relationship between the energy requirement and the distance separating the initial and the target coherent states. A key part of our study is the application of this framework to the H2O molecule, specifically examining the local OH bond. Here, we demonstrate how energy requirements for the state transitions are influenced by the distance between these states. Furthermore, we investigate the effects of a heat bath coupled to the system, by analysing its impact on transferring the molecular system to different final coherent states. These coherent states are defined as almost eigenvectors of the Generalised Heisenberg Algebra (GHA) annihilation operator. By using the Perolomov approach, another type of coherent states for the Morse potential associated with the GHA can be constructed. By leveraging the GHA structure, we revisit and analyse Morse coherent states previously established for certain diatomic molecules, offering a deeper insight into the dynamics of state transitions under various conditions.
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.
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.
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.
Quantum optimal control theory is applied to control electric dipole transitions in a real multilevel system. The specific system studied in the present work is comprised of a multitude of hyperfine levels in the electronic ground state of the OH molecule. Spectroscopic constants are used to obtain accurate energy eigenstates and electric dipole matrix elements. The goal is to calculate the optimal time-dependent electric field that yields a maximum of the transition probability for a specified initial and final state. A further important objective was to study the detailed quantum processes that take place during such a prescribed transition in a multilevel system. Two specific transitions are studied in detail. The computed optimal electric fields as well as the paths taken through the multitude of levels reveal quite interesting quantum phenomena.
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.
A time-dependent formulation of quantum control is employed to investigate optimally controlled vibrational population transfer in a diatomic quantum system. The problem of finding the optimal laser field needed to achieve a specific quantum transition from an initial state to the desired target goal is formulated using an iterative method and the conjugate gradient method (CGM). The time-dependent Schrödinger equation is solved with interaction of laser radiation with matter included within a dipole approximation in the Hamiltonian. Appropriate boundary conditions are chosen for the evolution problem. The control objective is chosen as the value of transition probability from an initial state to a target state. A comparison is made between the results obtained using the iterative method and the CGM for optimization. Finally, quantum bits are encoded using the vibrational states of the diatomic in the regime of low-vibrational excitation.