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Physical Review A

Linear theory for optimal control of molecular wave packets

Jianshu Cao, Kent R. Wilson

Published Jun 1, 1997• 4 citations
Publisher

Abstract

A linear theory for optimizing optical fields to achieve a molecular configuration at a chosen time is formulated with an emphasis on the symmetric transformation between time domain and space domain representations. Based on two different measures of control, the yield and achievement functions, two parallel but distinct optimization schemes are derived in a unified algebraic format. Connections are then established to a more conventional optimization procedure as well as the optimization procedure for squeezing wave packets used by Averbukh and Shapiro [Phys. Rev. A 47, 5086 (1993)]. A numerical example of the production of localized wave packets (i.e., squeezed states) demonstrates the effectiveness and feasibility of the proposed scheme.

DOI
10.1103/physreva.55.4477

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•Jan 1, 1997•3 citations
A linear theory for optimizing optical fields to achieve a molecular configuration at a chosen time is formulated with an emphasis on the symmetric transformation between time domain and space domain representations. Based on two different measures of control, the yield and achievement functions, two parallel but distinct optimization schemes are derived in a unified algebraic format. Connections are then established to a more conventional optimization procedure as well as the optimization procedure for squeezing wave packets used by Averbukh and Shapiro [Phys. Rev. A 47, 5086 (1993)]. A numerical example of the production of localized wave packets (i.e., squeezed states) demonstrates the effectiveness and feasibility of the proposed scheme.
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 look at time evolution of a physical system from the point of view of dynamical control theory. Normally we solve motion equation with a given external potential and we obtain time evolution. Standard examples are the trajectories in classical mechanics or the wave functions in Quantum Mechanics. In the control theory, we have the configurational variables of a physical system, we choose a velocity field and with a suited strategy we force the physical system to have a well defined evolution. The evolution of the system is the 'premium' that the controller receives if he has adopted the right strategy. The strategy is given by well suited laboratory devices. The control mechanisms are in many cases non linear; it is necessary, namely, a feedback mechanism to retain in time the selected evolution. Our aim is to introduce a scheme to obtain Quantum wave packets by control theory. The program is to choose the characteristics of a packet, that is, the equation of evolution for its centre and a controlled dispersion, and to give a building scheme from some initial state (for example a solution of stationary Schroedinger equation). It seems natural in this view to use stochastic approach to Quantum Mechanics, that is, Stochastic Mechanics [S.M.]. It is a quantization scheme different from ordinary ones only formally. This approach introduces in quantum theory the whole mathematical apparatus of stochastic control theory. Stochastic Mechanics, in our view, is more intuitive when we want to study all the classical-like problems. We apply our scheme to build two classes of quantum packets both derived generalizing some properties of coherent states.
A general local control theory for manipulating quantum system dynamics is developed. Basic concept of the present theory is lying in the realization of monotonous increasing condition of the performance index, which is locally (in time domain) defined to major how the present quantum state satisfies the current objective. The local control field is designed to satisfy the above condition taking into account the equation of motion of the system. It is found, through the formulation, that the monotonous increasing condition can be achieved as long as the performance index is given as a function of expectation values of time-dependent observable operators, whose equation of motion is governed by the field-free system Hamiltonian or Liouvillian. It is also shown that the present theory is a generalization of the local optimization approach which has been successfully applied to many of molecular dynamics control problems. As for the special cases, performance indices for “transition path control,” “population distribution control,” and “wave packet shaping” are proposed. The theory is applied to vibrational control problems of the one-dimensional model system of hydrogen fluoride. The results show that the present method works effectively for the population dynamics control as well as the wave packet shaping.
By combining the theories of optimal control and coherent control, we derive an analytical formulation to evaluate the optimal 1-photon and n -photon fields together with their relative phase and intensity in the optimal “1 + n ”-coherent control scheme. The optimal coherent control exploits tailored light pulses to produce the best overlap with a predefined nuclear target in an electronically degenerate region. It also exploits explicitly the quantum interference between two optimal excitation pathways to achieve the product electronic selectivity. Numerical demonstrations are carried out to selectively control a minimum-uncertainty outgoing wave packet target in a molecular system. The electronically degenerate byproduct is shown to be completely discriminated against via the destructive interference between two optimal excitation pathways. The target considered in this paper would neither be achievable via the conventional continuous-wave coherent control nor via a single optimal control pathway in the weak response regime. Proposed is also a time-dependent excitation frequency degeneracy condition that incorporates the evolution of carrier frequencies in the optimal coherent control with tailored light fields.
We introduce a general formalism, based on the stochastic formulation of quantum mechanics, to obtain localized quasi-classical wave packets as dynamically controlled systems, for arbitrary anharmonic potentials. The control is in general linear, and it amounts to introduce additional quadratic and linear time-dependent terms to the given potential. In this way one can construct for general systems either coherent packets moving with constant dispersion, or dynamically squeezed packets whose spreading remains bounded for all times. In the standard operatorial framework our scheme corresponds to a suitable generalization of the displacement and scaling operators that generate the coherent and squeezed states of the harmonic oscillator.