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Journal of Theoretical and Computational Chemistry

OPTIMALLY CONTROLLED VIBRATIONAL POPULATION TRANSFER IN A DIATOMIC QUANTUM SYSTEM

Praveen Kumar, Sitansh Sharma, Harjinder Singh

Published Feb 1, 2009• 11 citations
Publisher

Abstract

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.

DOI
10.1142/s0219633609004605

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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.
We discuss recent advances in optimal control theory (OCT) related to the investigation of the impact of control field noise on controllability of quantum dynamics. Two numerical methods, the gradient method and the iteration method, are paid particular attention. We analyze the problem of designing noisy control fields to maximize the vibrational transition probability in diatomic quantum systems, e.g. the HF and OH molecules. White noise is used as an additive random variable in the amplitude of the control field. It is demonstrated that the convergence is faster in the presence of noise and population transfer is increased by 0.04% for small values of noise compared to the field amplitude.
We derive a simple approximate analytic solution for the driving field that will generate a desired target vibrational wavepacket in a diatomic molecule. This solution is valid for arbitrary population transfer from the initial to the final electronic states. Analytic solutions to the control problem are possible when the control field is of shorter duration than the characteristic time scale of the system being manipulated. For target states that are localized wavepackets, our technique yields multiple solutions for the control field. We describe a procedure to choose from the set of solutions one that achieves both the target state and population transfer with high accuracy, for a large class of target states. The fidelity of each solution is tested by comparing the state obtained from a direct numerical integration of Schrödinger's equation using the analytic solution with the specified target state.
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.
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.
This paper considers the optimal control of quantum systems. The controlled quantum systems are described by the probability-density-matrix-based Liouville–von Neumann equation. Using projection operators, the states of the quantum system are decomposed into two sub-spaces, namely the 'main state' space and the 'remaining state' space. Since the control energy is limited, a solution for optimizing the external control force is proposed in which the main state is brought to the desired main state at a certain target time, while the population of the remaining state is simultaneously suppressed in order to diminish its effects on the final population of the main state. The optimization problem is formulated by maximizing a general cost functional of states and control force. An efficient algorithm is developed to solve the optimization problem. Finally, using the hydrogen fluoride (HF) molecular population transfer problem as an illustrative example, the effectiveness of the proposed scheme for a quantum system initially in a mixed state or in a pure state is investigated through numerical simulations.
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.