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The Journal of Chemical Physics

General formulation of locally designed coherent control theory for quantum system

Michihiko Sugawara

Published Apr 3, 2003• 86 citations
Publisher

Abstract

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.

DOI
10.1063/1.1559680

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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.
Quantum optimal control theory is applied to find optimal pulses for controlling the motion of an ion and a molecule for two different applications. Those optimal pulses enable the control of the dynamics of the system by driving the atom or the molecule from an initial state to desired states.The evolution equations obtained by means of the quantum optimal control theory are resolved iteratively using a monotonic convergent algorithm. A number of simulation parameters are varied in order to get the optimal pulses including the duration of the pulses, the time step of the time grid, a penalty factor that limits the maximal intensity of the fields, and a guess pulse which is used to start the optimal control.The optimal pulses obtained for each application are analyzed by Fourier transform, and also by looking at the time evolution of the populations that they generate in the system.The first application is the preparation of specific vibrational states of acetylene that are usually not reachable from the ground state, and that would remain unpopulated by usual spectroscopy. Relevant state energies and transition dipole moments are extracted from the experimental literature and especially from the global acetylene Hamiltonian conferring an uncommon precision to the control simulation. The control starts from the ground state. The target states belongs to the polyad Ns=1, Nr=5 of acetylene which includes two vibrational dark states and one vibrational bright state. First, the simulation is performed with the Schrödinger equation and in a second step, with the Liouville--von Neumann equation, as mixed states are prepared. Indeed, the control starts from a Boltzmann distribution of population in the rotational levels of the vibrational ground state chosen in order to simulate an experimental condition. But the distribution is truncated to limit the computational effort. One of the dark states appears to be a potential target for a realistic experimental investigation because the average population of the Rabi oscillation remains high and decoherence is expected to be weak. The optimal pulses obtained have a high fidelity, have a spectrum with well-resolved peak frequencies, and their experimental feasibility seems achievable within the current abilities of experimental laboratories.The second application is to propose an experimental realization of a microscopic physical device able to simulate quantum dynamics. The idea is to use the motional states of a Cd^+ ion trapped in an anharmonic potential to realize a quantum dynamics simulator of a single-particle Schrödinger equation. In this way, the motional states store the information and the optimal pulse manipulates this information to realize operations. In the present case, the simulated dynamics was the propagation of a wave packet in a harmonic potential. Starting from an initial quantum state, the pulse acts on the system to modify the motional states of the ion in such a way that the final superposition of motional states corresponds to the results of the dynamics. This simulation is performed with the Liouville--von Neumann equation and also with the Lindblad equation as dissipation is included to test the robustness of the pulse against perturbations of the potential. The optimal pulses that are obtained have a high fidelity which shows that the ion trap system has correctly realized the quantum dynamics simulation. The optimal pulses are valid for any initial condition if the potential of the simulation or the mass of the propagated wave packet is unchanged.
Applies the invertibility of a quantum mechanical systems concept to design open loop controls of molecular systems. The inverse quantum-mechanical control of molecules is studied using the equation of motion for the expectation value of an operator. With this method a requisite external field is obtained to exactly track a prescribed molecular objective expectation value as a function of time. Applications to diatomic molecules are formulated. While the method is directly applicable as a test of physical intuition, it can in principle be used to design fields for specific objectives including reactive selectivity. Results are presented for energy tracking in the hydrogen fluoride molecular system. The numerical calculations show that seemingly benign objective tracks may give rise to singularities in the field. However, these singularities do not present problems in the evolution of the dynamical quantities and instead provide useful hints for designing robust fields.>
Local time control methods are used in the simulation of quantum control phenomena because they conveniently ensure an increase of a predefined performance index and also avoid singularities associated with tracking procedures. However, the drawback of the existing implementations is that they only take into account one-photon, direct transitions and may stop at nonoptimal values of the index. We propose in this paper a modification of the currently used algorithms that addresses this issue and explain how the convergence is improved. Furthermore, when iterations are required, we show that this approach can be inserted into a monotonically convergent algorithm.
The opportunities offered by utilizing time-independent Hamiltonian structure as controls are explored for manipulating quantum dynamics. Two scenarios are investigated using different manifestations of Hamiltonian structure to illustrate the generality of the concept. In scenario I, optimally shaped electrostatic potentials are generated to flexibly control electron scattering in a two-dimensional subsurface plane of a semiconductor. A simulation is performed showing the utility of optimally setting the individual voltages applied to a multi-pixel surface gate array in order to produce a spatially inhomogeneous potential within the subsurface scattering plane. The coherent constructive and destructive electron wave interferences are manipulated by optimally adjusting the potential shapes to alter the scattering patterns. In scenario II, molecular vibrational wave packets are controlled by means of optimally selecting the Hamiltonian structure in cooperation with an applied field. As an illustration of the concept, a collection (i.e., a level set) of dipole functions is identified where each member serves with the same applied electric field to produce the desired final transition probability. The level set algorithm additionally found Hamiltonian structure controls exhibiting desirable physical properties. The prospects of utilizing the applied field and Hamiltonian structure simultaneously as controls is also explored. The control scenarios I and II indicate the gains offered by algorithmically guided molecular or material discovery for manipulating quantum dynamics phenomenon.
The control of quantum dynamics via specially tailored laser pulses is a long-standing goal in physics and chemistry. Partly, this dream has come true, as sophisticated pulse-shaping experiments allow us to coherently control product ratios of chemical reactions. The theoretical design of the laser pulse to transfer an initial state to a given final state can be achieved with the help of quantum optimal control theory (QOCT). This tutorial provides an introduction to QOCT. It shows how the control equations defining such an optimal pulse follow from the variation of a properly defined functional. We explain the most successful schemes to solve these control equations and show how to incorporate additional constraints in the pulse design. The algorithms are then applied to simple quantum systems and the obtained pulses are analysed. Besides the traditional final-time control methods, the tutorial also presents an algorithm and an example to handle time-dependent control targets.
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.