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arXiv:quant-ph/0510008 · Physical Review A

Laser control for the optimal evolution of pure quantum states

Dominique Sugny, Arne Keller, Osman Atabek, D. Daems, Claude M. Dion, S. Guérin, Hans Rudolf Jauslin

Published Jun 7, 2005• 38 citations
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Abstract

Starting from an initial pure quantum state, we present a strategy for reaching a target state corresponding to the extremum (maximum or minimum) of a given observable. We show that a sequence of pulses of moderate intensity, applied at times when the average of the observable reaches its local or global extremum, constitutes a strategy transferable to different control issues. Among them, postpulse molecular alignment and orientation are presented as examples. The robustness of such strategies with respect to experimentally relevant parameters is also examined.

DOI
10.1103/physreva.71.063402

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•Nov 28, 2017•0 citations
Starting from an initial pure quantum state, we present a strategy for reaching a target state corresponding to the extremum (maximum or minimum) of a given observable. We show that a sequence of pulses of moderate intensity, applied at times when the average of the observable reaches its local or global extremum, constitutes a strategy transferable to different control issues. Among them, postpulse molecular alignment and orientation are presented as examples. The robustness of such strategies with respect to experimentally relevant parameters is also examined.
We investigate how and to what extent molecular alignment can be controlled in a dissipative medium by a suitable train of laser pulses. We focus primarily on the extension of a scheme of control originally constructed for unitary evolution. The procedure is applied to control the alignment of CO molecules in an Ar gas. The parameters of the train of kicks---i.e., the intensity of each kick and the delay between them---are either obtained by a systematic procedure (maximum strategy) or by optimization by evolutionary algorithms.
This paper introduces the optimization of a quantum control application, the so-called molecular alignment problem, subject to a dynamic environment. Given the relative simplicity of optimized pulse-shapes in the low-intensity variant of the problem, versus the high complexity of the optimized pulse-shapes in the high-intensity case, a dynamic-intensity environment is simulated in a noise-free calculation. Specific evolution strategies, natural candidates for optimization in dynamic environments, are applied to this task. The calculations reveal the evolution of the pulse-shapes and their underlying evolving structures, that allow a complete physical interpretation. The combination of an optimization in a dynamic environment with the examination of the intermediate optimized solutions offers a sharper physics view of the problem, and accomplishes a fruitful interdisciplinary study.
A density matrix approach is developed for the control of a mixed-state quantum system using a time-dependent external field such as a train of pulses. This leads to the definition of a target density matrix constructed in a reduced Hilbert space as a specific combination of the eigenvectors of a given observable through weighting factors related to the initial statistics of the system. A train of pulses is considered as a possible strategy to reach this target. An illustration is given by considering the laser control of molecular alignment and orientation in thermal equilibrium.
The lack of a direct map between control fields and desired control objectives poses a significant challenge in applying quantum control theory to quantum technologies. Here, we propose an analytical framework to precisely control a limited set of quantum states and construct desired coherent superpositions using a well-designed laser pulse sequence with optimal amplitudes, phases, and delays. This theoretical framework that corresponds to a multilevel pulse-area theorem establishes a straightforward mapping between the control parameters of the pulse sequence and the amplitudes and phases of rotational states within a specific subspace. As an example, we utilize this approach to generate 15 distinct and desired rotational superpositions of ultracold polar molecules, leading to 15 desired field-free molecular orientations. By optimizing the superposition of the lowest 16 rotational states, we demonstrate that this approach can achieve a maximum orientation value of | 〈 cos θ 〉 | max above 0.99, which is very close to the global optimal value of 1 that could be achieved in an infinite-dimensional state space. This work marks a significant advancement in achieving precise control over multilevel subsystems within molecules. It holds potential applications in molecular alignment and orientation, as well as in various interdisciplinary fields related to the precise quantum control of ultracold polar molecules, opening up considerable opportunities in molecular-based quantum techniques.
Structured decompositions of a desired unitary operator are employed to derive control schemes that achieve certain control objectives for finite-level quantum systems using only sequences of simple control pulses such as square waves with finite rise and decay times or Gaussian wavepackets. The technique is applied to find control schemes that achieve population transfers for pure-state systems, complete inversions of the ensemble populations for mixed-state systems, create arbitrary superposition states and optimize the ensemble average of observables.
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.