Radiative transitions induced by short laser pulses in atomic collisions: Nonperturbative study of pulse shape effects

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Abstract
A time-dependent adiabatic electronic representation is defined by solving the local N-level electronic time-dependent Schrödinger equations at each nuclear configuration of a general N-channel, laser-driven molecular system. These solutions are eigenstates of a time-dependent effective Hamiltonian with respect to which the exact time-evolution of the N-state system is adiabatic. For a two-channel system, the time-dependent adiabatic electronic representation depends on an effective area of the laser pulse and geometrical phases that are also functionals of the laser pulse shape. This adiabatic representation is used in constructing an algorithm for the generation and propagation of wavepackets in a two-channel system irradiated by a short laser pulse. The algorithm is applied to the study of the wavepacket dynamics in the Na–Ar collisional system excited by short laser pulses. The dynamics of the channel populations are analyzed as functions of the shape, duration, and intensity of the laser pulses.