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Physical Review A

Optimal control of quantum systems by chirped pulses

Bjarne Amstrup, Jimmie D. Doll, Roland A. Sauerbrey, G. Szabó, András Lörincz

Published Nov 1, 1993• 61 citations
Publisher

Abstract

Research on optimal control of quantum systems has been severely restricted by the lack of experimentally feasible control pulses. Here, to overcome this obstacle, optimal control is considered with the help of chirped pulses. Simulated annealing is used as the optimizing procedure. The examples treated are pulsed population inversion between electronic levels, and optimization of vibronic excitation in the presence of another electronic level. In the problem of population inversion effective potentials of displaced harmonic oscillators are used. For optimizing vibronic excitation the CsI model potential is used.

DOI
10.1103/physreva.48.3830

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Research on optimal control of quantum systems has been severely restricted by the lack of experimentally feasible control pulses. Here, to overcome this obstacle, optimal control is considered with the help of chirped pulses. Simulated annealing is used as the optimizing procedure. The examples treated are pulsed population inversion between electronic levels, and optimization of vibronic excitation in the presence of another electronic level. In the problem of population inversion effective potentials of displaced harmonic oscillators are used. For optimizing vibronic excitation the CsI model potential is used.
This paper considers vibronic population inversion in the presence of molecular rotation. The objective is to invert the population of a vibronic level with populated rotational levels to a specific vibrational level in the excited electronic state regardless of the detailed population distribution in the final rotational levels. The control of the multilevel population inversion is achieved by design of a pump pulse through optimal control theory. The total energy fluence and the pulse peak intensity are imposed as physical constraints in the design cost functional. A model diatomic molecule is used as an example to investigate molecular rotational effects on the vibronic population inversion and the control properties at different target times. The numerical results indicate that the shape-optimized pulses can achieve nearly complete population inversion and largely overcome the difficulty that a rectangular pulse faces due to energy mismatches and multiple dipole transition moments.
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.
We investigate the effect of chirped excitation and the excitation detuning on the coherent control of population transfer and vibrational states in a four-level system. Density matrix equations are studied for optimally enhanced processes by considering specific parameters typical of oxazine systems. Our simulations show a strong dependence on the interplay between chirp and excitation detuning and predict enhancement factors up to 3.2 for population transfer and up to 38.5 for vibrational coherences of electronic excited states. The study of the dynamics of the populations and vibrational coherences involved in the four-level system allows an interpretation of the different enhancement/suppression processes observed.
Detailed theoretical analysis and numerical simulation indicate that nearly complete electronic population inversion of molecular systems can be achieved with intense positively chirped broadband laser pulses. To provide a simple physical picture, a two-level model is used to examine the condition for the so-called π pulses and a four-level model is designed to demonstrate for molecular systems the correlation between the sign of the chirp and the excited state population. The proposed molecular π pulse is the combined result of vibrational coherence in the femtosecond regime and adiabatic inversion in the picosecond regime. Numerical results for a displaced oscillator, for LiH and for I2, show that the proposed molecular π pulse scheme is robust with respect to changes in field parameters such as the linear positive chirp rate, field intensity, bandwidth, and carrier frequency, and is stable with respect to thermal and condensed phase conditions including molecular rotation, rovibronic coupling, and electronic dephasing.
A new scheme of controlling molecular processes by a sequence of linearly chirped pulses is proposed and is applied to selective excitation of an energy level among closely lying ones and to complete electronic excitation of a diatomic molecule. The basic idea is quite different from the conventional ones utilizing chirped pulses in the sense that the present one does not rely on the idea of adiabatic rapid passage at all, but tries to control basic nonadiabatic transitions explicitly. Control of molecular processes can be achieved by controlling nonadiabatic transitions among Floquet (or dressed) states with use of the interference effects. The scheme can be formulated with use of the analytical theories of nonadiabatic transitions, and the proper control parameters can be estimated theoretically. Numerical demonstrations are provided to confirm the robustness of the method in comparison with the other conventional ones. Namely, the present scheme is shown to be stable against the variation of pulse area, complete and selective in population transfer, and fast to accomplish the transition. It is expected that the method can be applied to general multilevel systems and various types of wave packet dynamics. Its experimental realizability can also be expected, since linear chirping can now be relatively easily realized and manipulated.
Abstract Quantum control methods, like rapid adiabatic passage, stimulated Raman adiabatic passage, shortcuts to adiabaticity and optimal control, have become an integral part of modern quantum technologies, for example quantum computation and sensing, where they are exploited in order to find the optimal pulse sequences which drive quantum systems to the desired target state in minimum time or with maximum fidelity, overcoming decoherence and dissipation. In this perspective, we use the basic example of adiabatic population inversion in a two-level system in order to present these methods and review the latest developments in the field, while we touch upon the emerging method of reinforcement learning.