Monotonically convergent algorithm for the control of molecular dynamics under non-linear interaction with the control field

Monotonically convergent optimal control theory of quantum systems with spectral constraints on the control field

We propose a new monotonically convergent algorithm which can enforce spectral constraints on the control field (and extends to arbitrary filters). The procedure differs from standard algorithms in that at each iteration the control field is taken as a linear combination of the control field (computed by the standard algorithm) and the filtered field. The parameter of the linear combination is chosen to respect the monotonic behavior of the algorithm and to be as close to the filtered field as possible. We test the efficiency of this method on molecular alignment. Using band-pass filters, we show how to select particular rotational transitions to reach high alignment efficiency. We also con…

Field-free molecular orientation by THz laser pulses at high temperature

We investigate to which extend a THz laser pulse can be used to produce field-free molecular orientation at high temperature. We consider laser pulses that can be implemented with the state of the art technology and we show that the efficiency of the control scheme crucially depends on the parameters of the molecule. We analyze the temperature effects on molecular dynamics and we demonstrate that, for some molecules, a noticeable orientation can be achieved at high temperature.

Time-optimal control of spin-1/2 particles with dissipative and generalized radiation-damping effects

We analyze the time-optimal control of spin-1/2 particles with bounded field amplitudes in the presence of dissipative and radiation damping effects. Using tools of geometric optimal control theory, we determine different optimal syntheses for specific values of the system parameters. We show the nontrivial role of the effective radiation damping effect on the optimal control law.

Monotonically convergent optimal control theory of quantum systems under a nonlinear interaction with the control field

We consider the optimal control of quantum systems interacting non-linearly with an electromagnetic field. We propose new monotonically convergent algorithms to solve the optimal equations. The monotonic behavior of the algorithm is ensured by a non-standard choice of the cost which is not quadratic in the field. These algorithms can be constructed for pure and mixed-state quantum systems. The efficiency of the method is shown numerically on molecular orientation with a non-linearity of order 3 in the field. Discretizing the amplitude and the phase of the Fourier transform of the optimal field, we show that the optimal solution can be well-approximated by pulses that could be implemented ex…

Understanding the global structure of two-level quantum systems with relaxation: Vector fields organized through the magic plane and the steady-state ellipsoid

Optimal control of the signal-to-noise ratio per unit time of a spin 1/2 particle: The crusher gradient and the radiation damping cases

We show to which extent the signal to noise ratio per unit time of a spin 1/2 particle can be maximized. We consider a cyclic repetition of experiments made of a measurement followed by a radio-frequency magnetic field excitation of the system, in the case of unbounded amplitude. In the periodic regime, the objective of the control problem is to design the initial state of the system and the pulse sequence which leads to the best signal to noise performance. We focus on two specific issues relevant in nuclear magnetic resonance, the crusher gradient and the radiation damping cases. Optimal control techniques are used to solve this non-standard control problem. We discuss the optimality of t…

Geometric optimal control of the contrast problem in Magnetic Resonance Imaging

Abstract The control of the dynamics of spin systems by magnetic fields has opened intriguing possibilities in quantum computing and in Nuclear Magnetic Resonance spectroscopy. In this framework, optimal control theory has been used to design control fields able to realize a given task while minimizing a prescribed cost such as the energy of the field or the duration of the process. However, some of the powerful tools of optimal control had not been used yet for NMR applications in medical imagery. Here, we show that the geometric control theory approach can be advantageously combined with NMR methods to crucially optimize the imaging contrast. This approach is applied to a benchmark proble…

Geometric versus numerical optimal control of a dissipative spin-12particle

We analyze the saturation of a nuclear magnetic resonance (NMR) signal using optimal magnetic fields. We consider both the problems of minimizing the duration of the control and its energy for a fixed duration. We solve the optimal control problems by using geometric methods and a purely numerical approach, the grape algorithm, the two methods being based on the application of the Pontryagin maximum principle. A very good agreement is obtained between the two results. The optimal solutions for the energy-minimization problem are finally implemented experimentally with available NMR techniques.

Simultaneous time-optimal control of the inversion of two spin-12particles

We analyze the simultaneous time-optimal control of two-spin systems. The two noncoupled spins, which differ in the value of their chemical offsets, are controlled by the same magnetic fields. Using an appropriate rotating frame, we restrict the study to the case of opposite shifts. We then show that the optimal solution of the inversion problem in a rotating frame is composed of a pulse sequence of maximum intensity and is similar to the optimal solution for inverting only one spin by using a nonresonant control field in the laboratory frame. An example is implemented experimentally using nuclear magnetic resonance techniques.

Towards the time-optimal control of dissipative spin-1/2 particles in nuclear magnetic resonance

International audience; We consider the time-optimal control of a spin 1/2 particle whose dynamics is governed by the Bloch equations with both longitudinal and transverse relaxation terms. We solve this control problem by using geometric optimal control techniques. We show the crucial role of singular extremals in the time-optimal synthesis. This role can mainly be attributed to the presence of dissipation. We also analyze the robustness of the optimal control sequence when both the maximum amplitude of the control field and the dissipative parameters are varied. Finally, we present an experimental implementation of the different solutions using techniques of Nuclear Magnetic Resonance.

Field-free permanent molecular planar alignment

We show the existence of a permanent molecular planar alignment in field-free conditions. We present different control strategies using shaped laser pulses to reach this state. The strategies are robust with respect to the temperature and can be implemented with the state of the art technology. They can be applied not only to linear molecules but also to symmetric or asymmetric top molecules along the most polarizable molecular axis. We propose potential applications of this planar alignment such as the increase of the adsorption on a surface.

Saturation of a spin-1/2 particle by generalized local control

We show how to apply a generalization of Local control design to the problem of saturation of a spin 1/2 particle by magnetic fields in Nuclear Magnetic Resonance. The generalization of local or Lyapunov control arises from the fact that the derivative of the Lyapunov function does not depend explicitly on the control field. The second derivative is used to determine the local control field. We compare the efficiency of this approach with respect to the time-optimal solution which has been recently derived using geometric methods.

Singular Extremals for the Time-Optimal Control of Dissipative Spin 1/2 Particles

We consider the time-optimal control by magnetic fields of a spin 1/2 particle in a dissipative environment. This system is used as an illustrative example to show the role of singular extremals in the control of quantum systems. We analyze a simple case where the control law is explicitly determined. We experimentally implement the optimal control using techniques of nuclear magnetic resonance. To our knowledge, this is the first experimental demonstration of singular extremals in quantum systems with bounded control amplitudes.

Observation of laser-induced field-free permanent planar alignment of molecules

International audience; Permanent planar alignment of gas-phase linear molecules is achieved by a pair of delayed perpendicularly polarized short laser pulses. The experiment is performed in a supersonic jet, ensuring a relatively high number density of molecules with moderately low rotational temperature. The effect is optically probed on a femtosecond time scale by the use of a third short pulse, enabling a time-resolved birefringence detection performed successively in two perpendicular planes of the laboratory frame. The technique allows for an unambiguous estimation of the molecular planar delocalization produced within the polarization plane of the pulse pair after the turn-off of the…

Exploring the Physical Limits of Saturation Contrast in Magnetic Resonance Imaging

International audience; Magnetic Resonance Imaging has become nowadays an indispensable tool with applications ranging from medicine to material science. However, so far the physical limits of the maximum achievable experimental contrast were unknown. We introduce an approach based on principles of optimal control theory to explore these physical limits, providing a benchmark for numerically optimized robust pulse sequences which can take into account experimental imperfections. This approach is demonstrated experimentally using a model system of two spatially separated liquids corresponding to blood in its oxygenated and deoxygenated forms.

Optimal control of quantum superpositions in a bosonic Josephson junction

We show how to optimally control the creation of quantum superpositions in a bosonic Josephson junction within the two-site Bose-Hubbard model framework. Both geometric and purely numerical optimal control approaches are used, the former providing a generalization of the proposal of Micheli et al [Phys. Rev. A 67, 013607 (2003)]. While this method is shown not to lead to significant improvements in terms of time of formation and fidelity of the superposition, a numerical optimal control approach appears more promising, as it allows to create an almost perfect superposition, within a time short compared to other existing protocols. We analyze the robustness of the optimal solution against at…

Comparative study of monotonically convergent optimization algorithms for the control of molecular rotation

We apply two different monotonically convergent optimization algorithms to the control of molecular rotational dynamics by laser pulses. This example represents a quantum control problem where the interaction of the system with the external field is non-linear. We test the validity and accuracy of the two methods on the key control targets of producing molecular orientation and planar delocalization at zero temperature, and maximizing permanent alignment at non-zero temperature.

Discrete-valued-pulse optimal control algorithms: Application to spin systems

International audience; This article is aimed at extending the framework of optimal control techniques to the situation where the control field values are restricted to a finite set. We propose generalizations of the standard GRAPE algorithm suited to this constraint. We test the validity and the efficiency of this approach for the inversion of an inhomogeneous ensemble of spin systems with different offset frequencies. It is shown that a remarkable efficiency can be achieved even for a very limited number of discrete values. Some applications in nuclear magnetic resonance are discussed.