Reaching optimally oriented molecular states by laser kicks

We present a strategy for post-pulse 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.Comment: 4 pages, 3 figure

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 postpulse 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.Comment: 5 pages, 4 color figure

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, post-pulse molecular alignment and orientation are presented as examples. The robustness of such strategies with respect to experimentally relevant parameters is also examined.Comment: 16 pages, 9 figure

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.Comment: 4 pages, 2 figure

Unitary time-dependent superconvergent technique for pulse-driven quantum dynamics

We present a superconvergent Kolmogorov-Arnold-Moser type of perturbation theory for time-dependent Hamiltonians. It is strictly unitary upon truncation at an arbitrary order and not restricted to periodic or quasiperiodic Hamiltonians. Moreover, for pulse-driven systems we construct explicitly the KAM transformations involved in the iterative procedure. The technique is illustrated on a two-level model perturbed by a pulsed interaction for which we obtain convergence all the way from the sudden regime to the opposite adiabatic regime

Non-intersecting squared Bessel paths and multiple orthogonal polynomials for modified Bessel weights

We study a model of $n$ non-intersecting squared Bessel processes in the confluent case: all paths start at time $t = 0$ at the same positive value $x = a$, remain positive, and are conditioned to end at time $t = T$ at $x = 0$. In the limit $n \to \infty$, after appropriate rescaling, the paths fill out a region in the $tx$-plane that we describe explicitly. In particular, the paths initially stay away from the hard edge at $x = 0$, but at a certain critical time $t^*$ the smallest paths hit the hard edge and from then on are stuck to it. For $t \neq t^*$ we obtain the usual scaling limits from random matrix theory, namely the sine, Airy, and Bessel kernels. A key fact is that the positions of the paths at any time $t$ constitute a multiple orthogonal polynomial ensemble, corresponding to a system of two modified Bessel-type weights. As a consequence, there is a $3 \times 3$ matrix valued Riemann-Hilbert problem characterizing this model, that we analyze in the large $n$ limit using the Deift-Zhou steepest descent method. There are some novel ingredients in the Riemann-Hilbert analysis that are of independent interest.Comment: 59 pages, 11 figure

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

We apply a time-dependent perturbation theory based on unitary transformations combined with averaging techniques, on molecular orientation dynamics by ultrashort pulses. We test the validity and the accuracy of this approach on LiCl described within a rigid-rotor model and find that it is more accurate than other approximations. Furthermore, it is shown that a noticeable orientation can be achieved for experimentally standard short laser pulses of zero time average. In this case, we determine the dynamically relevant parameters by using the perturbative propagator, that is derived from this scheme, and we investigate the temperature effects on the molecular orientation dynamics.Comment: 16 pages, 6 figure

Simple deterministic dynamical systems with fractal diffusion coefficients

We analyze a simple model of deterministic diffusion. The model consists of a one-dimensional periodic array of scatterers in which point particles move from cell to cell as defined by a piecewise linear map. The microscopic chaotic scattering process of the map can be changed by a control parameter. This induces a parameter dependence for the macroscopic diffusion coefficient. We calculate the diffusion coefficent and the largest eigenmodes of the system by using Markov partitions and by solving the eigenvalue problems of respective topological transition matrices. For different boundary conditions we find that the largest eigenmodes of the map match to the ones of the simple phenomenological diffusion equation. Our main result is that the difffusion coefficient exhibits a fractal structure by varying the system parameter. To understand the origin of this fractal structure, we give qualitative and quantitative arguments. These arguments relate the sequence of oscillations in the strength of the parameter-dependent diffusion coefficient to the microscopic coupling of the single scatterers which changes by varying the control parameter.Comment: 28 pages (revtex), 12 figures (postscript), submitted to Phys. Rev.

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 details here. As an illustration, we consider a two-level system driven by short pulses beyond the sudden limit.Comment: 15 pages, 5 color figure