Hans Rudolf Jauslin

Reaching optimally oriented molecular states by laser kicks

We present a strategy for postpulse molecular orientation aiming both at efficiency and maximal duration within a rotational period. We first identify the optimally oriented states which fulfill both requirements. We show that a sequence of half-cycle pulses of moderate intensity can be devised for reaching these target states.

Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses.

We show that a linear molecule subjected to a short specific elliptically polarized laser field yields post-pulse revivals exhibiting alignment alternatively located along the orthogonal axis and the major axis of the ellipse. The effect is experimentally demonstrated by measuring the optical Kerr effect along two different axes. The conditions ensuring an optimal field-free alternation of high alignments along both directions are derived.

Efficient and long-lived field-free orientation of molecules by a single hybrid short pulse

We show that a combination of a half-cycle pulse and a short nonresonant laser pulse produces a strongly enhanced postpulse orientation. Robust transients that display both efficient and long-lived orientation are obtained. The mechanism is analyzed in terms of optimal oriented target states in finite Hilbert subspaces and shows that hybrid pulses can prove useful for other control issues.

Time-dependent unitary perturbation theory for intense laser-driven molecular orientation

Molecular orientation dynamics by ultrashort pulses was investigated by applying a time-dependent unitary perturbation theory (TDUPT) combined with averaging techniques. A perturbative propagator was constructed which allowed to elucidate the postpulse orientation dynamics. It was observed that an effective orientation could be achieved for standard short laser pulses of zero time average. It was suggested that chosing a appropriate free parameter available in the TDUPT could help in improving the accuracy of the approximate propagator.

Control of mixed-state quantum systems by a train of short pulses

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.

Modeling of the photorefractive nonlinear response in Sn 2 P 2 S 6 crystals

We develop a theory of the photorefractive nonlinear response for Sn2P2S6 crystals. The theory incorporates two types of charge carrier (optically active and passive), provides explicit expressions for the characteristic buildup-relaxation rates and gain factors, explains naturally a big variety of accumulated experimental data, and facilitates characterization-optimization of this important nonlinear material.

Laser control for the optimal evolution of pure quantum states

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.

Pulse-driven quantum dynamics beyond the impulsive regime

We review various unitary time-dependent perturbation theories and compare them formally and numerically. We show that the Kolmogorov-Arnold-Moser technique performs better owing to both the superexponential character of correction terms and the possibility to optimize the accuracy of a given level of approximation which is explored in detail here. As an illustration, we consider a two-level system driven by short pulses beyond the sudden limit.

Four-wave-mixing coherent oscillator with frequency shifted feedback and misaligned pump waves

The effect of the pump waves misalignment on the oscillation spectra and oscillation intensity of a semilinear photorefractive oscillator is studied numerically and compared with the results of the experiment performed with a KNbO3:Fe,Ag crystal.

Optimized time-dependent perturbation theory for pulse-driven quantum dynamics in atomic or molecular systems

We present a time-dependent perturbative approach adapted to the treatment of intense pulsed interactions. We show there is a freedom in choosing secular terms and use it to optimize the accuracy of the approximation. We apply this formulation to a unitary superconvergent technique and improve the accuracy by several orders of magnitude with respect to the Magnus expansion.