0000000000181427
AUTHOR
Mamadou Ndong
Time optimization and state-dependent constraints in the quantum optimal control of molecular orientation
We apply two recent generalizations of monotonically convergent optimization algorithms to the control of molecular orientation by laser fields. We show how to minimize the control duration by a step-wise optimization and maximize the field-free molecular orientation using state-dependent constraints. We discuss the physical relevance of the different results.
Control of molecular dynamics with zero-area fields: Application to molecular orientation and photofragmentation
The constraint of time-integrated zero-area on the laser field is a fundamental, both theoretical and experimental requirement in the control of molecular dynamics. By using techniques of local and optimal control theory, we show how to enforce this constraint on two benchmark control problems, namely molecular orientation and photofragmentation. The origin and the physical implications on the dynamics of this zero-area control field are discussed.
A NOT gate in a cis-trans photoisomerization model
We numerically study the implementation of a NOT gate by laser pulses in a model molecular system presenting two electronic surfaces coupled by non adiabatic interactions. The two states of the bit are the fundamental states of the cis-trans isomers of the molecule. The gate is classical in the sense that it involves a one-qubit flip so that the encoding of the outputs is based on population analysis which does not take the phases into account. This gate can also be viewed as a double photo-switch process with the property that the same electric field controls the two isomerizations. As an example, we consider one-dimensional cuts in a model of the retinal in rhodopsin already proposed in t…
External constraints on optimal control strategies in molecular orientation and photofragmentation: Role of zero-area fields
We propose a new formulation of optimal and local control algorithms which enforces the constraint of time-integrated zero-area on the control field. The fulfillment of this requirement, crucial in many physical applications, is mathematically implemented by the introduction of a Lagrange multiplier aiming at penalizing the pulse area. This method allows to design a control field with an area as small as possible, while bringing the dynamical system close to the target state. We test the efficiency of this approach on two control purposes in molecular dynamics, namely, orientation and photodissociation.
Laser control in open molecular systems: STIRAP and Optimal Control
We examine the effect of dissipation on the laser control of a process that transforms a state into a superposed state. We consider a two-dimensional double well of a single potential energy surface. In the context of reactivity, the objective of the control is the localization in a given well, for instance the creation of an enantiomeric form whereas for quantum gates, this control corresponds to one of the transformation of the Hadamard gate. The environment is either modelled by coupling few harmonic oscillators (up to five) to the system or by an effective interaction with an Ohmic bath. In the discrete case, dynamics is carried out exactly by using the coupled harmonic adiabatic channe…
Newton algorithm for Hamiltonian characterization in quantum control
We propose a Newton algorithm to characterize the Hamiltonian of a quantum system interacting with a given laser field. The algorithm is based on the assumption that the evolution operator of the system is perfectly known at a fixed time. The computational scheme uses the Crank-Nicholson approximation to explicitly determine the derivatives of the propagator with respect to the Hamiltonians of the system. In order to globalize this algorithm, we use a continuation method that improves its convergence properties. This technique is applied to a two-level quantum system and to a molecular one with a double-well potential. The numerical tests show that accurate estimates of the unknown paramete…
Laser control in a bifurcating region
We present a complete analysis of the laser control of a model molecular system using both optimal control theory and adiabatic techniques. This molecule has a particular potential energy surface with a bifurcating region connecting three potential wells which allows a variety of processes such as isomerization, tunnelling or implementation of quantum gates on one or two qubits. The parameters of the model have been chosen so as to reproduce the main features of H3CO which is a molecule-benchmark for such dynamics. We show the feasibility of different processes and we investigate their robustness against variations of laser field. We discuss the conditions under which each method of control…
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.
Polarization shaping for unidirectional rotational motion of molecules.
Control of the orientation of the angular momentum of linear molecules is demonstrated by means of laser polarization shaping. For this purpose, we combine two orthogonally polarized and partially time-overlapped femtosecond laser pulses so as to produce a spinning linear polarization which in turn induces unidirectional rotation of N2 molecules. The evolution of the rotational response is probed by a third laser beam that can be either linearly or circularly polarized. The physical observable is the frequency shift imparted to the probe beam as a manifestation of the angular Doppler effect. Our experimental results are confirmed by theoretical computations, which allow one to gain a deep p…