Strong-field molecular ionization beyond the single active electron approximation.

This work explores quantitative limits to the single-active electron approximation, often used to deal with strong-field ionization and subsequent attosecond dynamics. Using a time-dependent, multiconfiguration approach, specifically the time-dependent configuration interaction method, we solve the time-dependent Schrödinger equation for the two-electron dihydrogen molecule with the possibility of tuning at will the electron-electron interaction by an adiabatic switch-on/switch-off function. We focus on signals of the single ionization of H2 under a strong near-infrared, four-cycle, linearly polarized laser pulse of varying intensity and within a vibrationally frozen molecular model. The observables we address are post-pulse total ionization probability profiles as a function of the laser peak intensity. Three values of the internuclear distance R taken as a parameter are considered, R = Req = 1.4 a.u. for the equilibrium geometry of the molecule, R = 5.0 a.u. for an elongated molecule, and R = 10.2 a.u. for a dissociating molecule. The most striking observation is the non-monotonous behavior of the ionization probability profiles at intermediate elongation distances with an instance of enhanced ionization and one of partial ionization quenching. We give an interpretation of this in terms of a resonance-enhanced-multiphoton ionization mechanism with interfering overlapping resonances resulting from excited electronic states.

Dissociation quenching using exceptional points.

We examine a short way to reach an exceptional point that corresponds to a coalescence of two resonance energies. The application concerns the photodissociation of the Na2 molecule exposed to a laser field. In this case, the resonances can be correlated with the field-free vibrational states of the diatomic species. The resonances are due to the field-induced coupling with the continuum of a repulsive potential. We also draw attention to a new kind of exceptional point involving a resonance originating from a vibrational state coalescing with a shape-type resonance of the repulsive potential. A laser control scenario, aiming at the adiabatic transport from this field-free decaying state to a stable field-free vibrational state, is discussed in terms of field-induced dissociation quenching.

Proposal for a laser control of vibrational cooling in Na(2) using resonance coalescence.

With a specific choice of laser parameters resulting in a so-called exceptional point (EP) in the wavelength-intensity parameter plane, it is possible to produce the coalescence of two Floquet resonances describing the photodissociation of the Na(2) molecule, which is one of the candidates for the formation of samples of translationally cold molecules. By appropriately tuning laser parameters along a contour encircling the exceptional point, the resonances exchange their quantum nature. Thus a laser-controlled transfer of the probability density from one field-free vibrational level to another is achieved through adiabatic transport involving these resonances. We propose an efficient scenario for vibrational cooling of Na(2) referring to cascade transfers involving multiple EPs and predicted to be robust up to a 78% rate against laser-induced dissociation.

Laser control of vibrational transfer based on exceptional points.

The coalescence of two Floquet resonances with complex quasi-energies in the photodissociation of a molecule can be reached through an appropriate choice of laser parameters (wavelength and intensity). The corresponding point in the parameter plane is called exceptional. We show that a condition for two resonances to yield such a point is that they correspond, respectively, to a shape-like resonance and a Feshbach-like resonance. We examine how the resonances behave along a contour in the parameter plane, which goes around the exceptional point. The resonances exchange their labels. This amounts to a laser control of the vibrational transfer of the undissociated molecules from one field-free state to another.

Resonance coalescence in molecular photodissociation.

We study theoretically the photodissociation dynamics of the H_{2};{+} molecular ion exposed to a linearly polarized laser light. It is shown that it is possible to choose a laser wavelength and intensity so as to produce a coalescence of two photodissociation vibronic resonance states. At such a coalescence point, also called an exceptional point, the photodissociative resonance wave function is self-orthogonal. This unique phenomenon which is presented here for light induced molecular dynamics enables us to transfer completely the nondissociated molecules from one vibronic state to another by varying adiabatically the laser frequency and intensity along a closed contour which encircles the exceptional point.

Molecular dissociative ionization and wave-packet dynamics studied using two-color XUV and IR pump-probe spectroscopy.

We present a combined theoretical and experimental study of ultrafast wave-packet dynamics in the dissociative ionization of H_{2} molecules as a result of irradiation with an extreme-ultraviolet (XUV) pulse followed by an infrared (IR) pulse. In experiments where the duration of both the XUV and IR pulses are shorter than the vibrational period of H_{2};{+}, dephasing and rephasing of the vibrational wave packet that is formed in H_{2};{+} upon ionization of the neutral molecule by the XUV pulse is observed. In experiments where the duration of the IR pulse exceeds the vibrational period of H_{2};{+} (15 fs), a pronounced dependence of the H;{+} kinetic energy distribution on XUV-IR delay is observed that can be explained in terms of the adiabatic propagation of the H_{2};{+} wave packet on field-dressed potential energy curves.

Bell-type inequalities for cold heteronuclear molecules.

We introduce Bell-type inequalities allowing for nonlocality and entanglement tests with two cold heteronuclear molecules. The proposed inequalities are based on correlations between each molecule spatial orientation, an observable which can be experimentally measured with present day technology. Orientation measurements are performed on each subsystem at different times. These times play the role of the polarizer angles in Bell tests realized with photons. We discuss the experimental implementations of the proposed tests, which could also be adapted to other high dimensional quantum angular momenta systems.