Lagrangian descriptor and escape time as tools to investigate the dynamics of laser-driven polar molecules.

We consider the nonlinear dynamics of a diatomic polar molecule under a linearly polarized laser field. We assume a model in which the molecule dipole is coupled with a time-dependent electric field. This system presents a bound energy region where the atoms are bound, and a free-energy region where the atoms are dissociated. Due to the nonalignment between the dipole axis and the laser direction, and the time dependence of the external field, this system presents two and a half degrees of freedom, namely the vibrational degree, the rotation degree, and the time. To investigate the system dynamics, instead of using the Poincaré surface-of-section technique, we propose the use of the Lagrangian descriptor associated with the escape times. The Lagrangian descriptor is a quantity that reveals complex structures in the phase space, whereas the escape times are the time span in which a trajectory is initially in the bound region before escaping to the unbound region. The combination of these two quantities allows us to distinguish between real stability regions from other complex structures, including stickiness regions, and a different formation, which we call escape islands. With the help of these tools, we find that for high-field amplitudes the inclusion of rotation leads to an increase of the stability regions, which implies a decrease of the dissociation in comparison with the one-dimensional case.

Nonlinear photoassociation through exotic orbits.

We investigate the effects of a particular kind of orbits, which we call exotic orbits, on the process of classical molecular photoassociation. As a starting model system, we consider the process described by the Morse potential with a time-dependent perturbation consisting of the interaction of an external laser field with the molecular dipole. When the external perturbation is turned off, the bound molecular states are classically represented by librational motion, whereas the unbound, the collisional states, are represented by unbound motion, and in both cases, the energy is a constant of motion. When the perturbation is turned on, the total energy is no longer a constant of motion and initial conditions in the unbound region can reach the bound region, and vice versa, through chaotic orbits. Alternatively, we have found that the connection between the bound and unbound sectors can be achieved through exotic orbits, which are comprised by librationlike parts, a localized chaotic region, and an unbounded constant-energy part. Thus, if a colliding atomic pair is in an exotic orbit, it penetrates a chaotic region coming from the unbound sector, subsequently performing librationlike motion, during which the molecule with constant bound energy is formed. Afterwards, the molecule returns to the chaotic region and from this region, it can either access a distinct bound energy or dissociate. We call this phenomenon, in which a metastable molecule is formed, intermittent photoassociation. We show that the key for the emergence of exotic orbits is the relatively short range of the dipole as compared to the interacting potential range. In order to further verify our results, we have considered realistic forms for the potentials and dipole functions of several molecules and found the emergence of exotic orbits, and consequently of intermittent photoassociation, for the MgLi and SrLi molecular parameters.

Nonchaotic laser pulse dissociation through deformed tori.

We consider the nonlinear classical dynamics of a diatomic molecule under the action of a laser field in the framework of the driven Morse oscillator model. We investigate the influence of the dipole function and the laser field on the deformations of the surviving, invariant tori. For intense and high-frequency fields, some invariant tori traverse the separatrix of motion, visiting both the bound and unbound regions of the interatomic potential. Based on this fact, we propose the use of appropriately designed laser pulses to induce dissociation of trajectories on such invariant tori. This mechanism constitutes a controlled nonchaotic route for dissociation, which is an alternative to chaotic multiphoton dissociation and to chirped pulse dissociation.

Role of the range of the dipole function in the classical dynamics of molecular dissociation.

The dissociation dynamics of heteronuclear diatomic molecules induced by infrared laser pulses is investigated within the framework of the classical driven Morse oscillator. The interaction between the molecule and the laser field described in the dipole formulation is given by the product of a time-dependent external field with a position-dependent permanent dipole function. The effects of changing the spatial range of the dipole function in the classical dissociation dynamics of large ensembles of trajectories are studied. Numerical calculations have been performed for distinct amplitudes and carrier frequencies of the external pulses and also for ensembles with different initial energies. It is found that there exist a set of values of the dipole range for which the dissociation probability can be completely suppressed. The dependence of the dissociation on the dipole range is explained through the examination of the Fourier series coefficients of the dipole function in the angle variable of the free system. In particular, the suppression of dissociation corresponds to dipole ranges for which the Fourier coefficients associated with nonlinear resonances are null and the chaotic region in the phase space is reduced to thin layers. In this context, it is shown that the suppression of dissociation of heteronuclear molecules for certain frequencies of the external field is a consequence of the finite range of the corresponding permanent dipole.

The Morse oscillator under time-dependent external fields.

A method to solve the equations for the Morse oscillator under intense time-dependent external fields is presented. Exact analytical formulas for the dipole matrix elements are calculated by the use of the hypergeometric algebra. The continuum is described by an expansion using Laguerre functions. The full algorithm for the calculation of wave functions can be controlled by the convergence of series and by the errors of a first order integration method. We apply our technique to the selective preparation of high overtones by femtosecond laser pulses. The population of the target state is optimized as a function of the intensity and frequency. Introducing a second simultaneous laser, we study the effects of relative frequency and phase over the target state population and dissociation channels. The calculations exhibit a rich interference pattern showing the enhancement and the suppression of the target population by varying the laser parameters.