Lattice mold technique for the calculation of crystal nucleation rates.

We present a new simulation method for the calculation of crystal nucleation rates by computer simulation. The method is based on the use of molds to induce crystallization in state points where nucleation is a rare event. The mold is a cluster of potential energy wells placed in the lattice positions of the solid.

Nonresonant electronic transitions induced by vibrational motion in light-induced potentials.

We find a new mechanism of electronic population inversion using strong femtosecond pulses, where the transfer is mediated by vibrational motion on a light-induced potential. The process can be achieved with a single pulse tuning its frequency to the red of the Franck-Condon window. We show the determinant role that the gradient of the transition dipole moment can play on the dynamics, and extend the method to multiphoton processes with odd number of pulses.

Protecting and accelerating adiabatic passage with time-delayed pulse sequences.

Using numerical simulations of two-photon electronic absorption with femtosecond pulses in Na2 we show that: (i) it is possible to avoid the characteristic saturation or dumped Rabi oscillations in the yield of absorption by time-delaying the laser pulses; (ii) it is possible to accelerate the onset of adiabatic passage by using the vibrational coherence starting in a wave packet; and (iii) it is possible to prepare the initial wave packet in order to achieve full state-selective transitions with broadband pulses. The findings can be used, for instance, to achieve ultrafast adiabatic passage by light-induced potentials and understand its intrinsic robustness.