Considering the problem of the control of a two-state quantum system by an external field, we establish a general and versatile method allowing the derivation of smooth pulses which feature the properties of high fidelity, robustness, and low area. Such shaped pulses can be interpreted as a single-shot generalization of the composite pulse-sequence technique with a time-dependent phase.

We apply the techniques of control theory and of sub-Riemannian geometry to laser-induced population transfer in two- and three-level quantum systems. The aim is to induce complete population transfer by one or two laser pulses minimizing the pulse fluences. Sub-Riemannian geometry and singular-Riemannian geometry provide a natural framework for this minimization, where the optimal control is expressed in terms of geodesics. We first show that in two-level systems the well-known technique of “π-pulse transfer” in the rotating wave approximation emerges naturally from this minimization. In three-level systems driven by two resonant fields, we also find the counterpart of the “π-pulse transfer.” This geometrical picture also allows one to analyze the population transfer by adiabatic passage.

We present a method for optimization of the technique of adiabatic passage between two quantum states by composite sequences of frequency-chirped pulses with specific relative phases: composite adiabatic passage (CAP). By choosing the composite phases appropriately the nonadiabatic losses can be canceled to any desired order with sufficiently long sequences, regardless of the nonadiabatic coupling. The values of the composite phases are universal for they do not depend on the pulse shapes and the chirp. The accuracy of the CAP technique and its robustness against parameter variations make CAP suitable for high-fidelity quantum information processing.

We report a direct nonintrusive observation of alignment and planar delocalization of ${\mathrm{C}\mathrm{O}}_2$ after an intense linearly polarized femtosecond laser pulse excitation. The effects are measured by a polarization technique involving a perturbative probe that itself does not induce appreciable alignment. We show that this technique allows one to measure a signal proportional to $⟨{cos}^2\theta ⟩-1/3$, with $\theta$ the angle between the molecular axis and the laser polarization. Simulations that support this analysis allow one to characterize the experimentally observed alignment and planar delocalization quantitatively.

We develop an inverse geometric optimization technique that allows the derivation of optimal and robust exact solutions of low-dimension quantum control problems driven by external fields. We determine in the dynamical variable space optimal trajectories constrained to robust solutions by Euler-Lagrange optimization; the control fields are then derived from the obtained robust geodesics and the inverted dynamical equations. We apply this method, referred to as robust inverse optimization (RIO), to design optimal control fields producing a complete or half population transfer and a not quantum gate robust with respect to the pulse inhomogeneities. The method is versatile and can be applied to numerous quantum control problems, e.g., other gates, other types of imperfections, Raman processes, or dynamical decoupling of undesirable effects.