Dissociation under ultrashort intense laser fields differs from the process occurring in the presence of a weak field by two main characteristics. In the strong field regime, the force exerted by the laser on the molecule is comparable to the intermolecular forces. In addition, this force is varying on a time scale comparable to that of the molecular vibration. The combination of these two effe...

The real time photodissociation dynamics of CH(3)I from the A band has been studied experimentally and theoretically. Femtosecond pump-probe experiments in combination with velocity map imaging have been carried out to measure the reaction times (clocking) of the different (nonadiabatic) channels of this photodissociation reaction yielding ground and spin-orbit excited states of the I fragment ...

Tight-binding molecular dynamics simulations of the adsorption of O2/Pt(111) have been performed based on an ab initio potential energy surface. We demonstrate that, contrary to common belief, in this system the whole adsorption probability as a function of the kinetic energy can be understood in terms of trapping into chemisorbed molecular precursor states. This provides a novel unified pictur...

A space warping method, facilitating the modeling of large-scale conformational changes in mesoscopic systems, is presented. The method uses a set of "global (or collective) coordinates" that capture overall behavior, in conjunction with the set of atomic coordinates. Application of the space warping method to energy minimization is discussed. Several simulations where the method is used to det...

High-resolution spectroscopy measures the transitions between energy levels with high accuracy; typically, uncertainties are in the region of 1 part in 108. Although it is possible, under favorable circumstances, to obtain this sort of accuracy by fitting effective Hamiltonians to observed spectra (see Bauder 2011: Fundamentals of Rotational Spectroscopy, this handbook), such ultrahigh accuracy...

We present ‘BYTe’, a comprehensive ‘hot’ line list for the ro-vibrational transitions of ammonia, NH3, in its ground electronic state. This line list has been computed variationally using the program suite TROVE, a new spectroscopically determined potential energy surface and an ab initio dipole moment surface. BYTe, is designed to be used at all temperatures up to 1500 K. It comprises 1138 323...

In this paper we present a deenition of \connguration controllability" for mechanical systems whose Lagrangian is kinetic energy with respect to a Riemannian metric minus potential energy. A computable test for this new version of controllability is also derived. This condition involves a new object which we call the symmetric product. Of particular interest is a deenition of \equilibrium contr...

To predict the branching between energetically allowed product channels, chemists often rely on statistical transition state theories or exact quantum scattering calculations on a single adiabatic potential energy surface. The potential energy surface gives the energetic barriers to each chemical reaction and allows prediction of the reaction rates. Yet, chemical reactions evolve on a single po...

Interferences are genuine quantum phenomena that appear whenever two seemingly distinct classical trajectories lead to the same outcome. They are common in elastic scattering but are seldom observable in chemical reactions. Here we report experimental measurements of the state-to-state angular distribution for the H + D2 reaction using the 'photoloc' technique. For products in low rotational an...