Abstract
Previous investigations have shown that the instantaneous eigenstates of a molecule interacting via its polarizability with a strong electric field of a nonresonant laser pulse are pendular hybrids of field-free rotational states, aligned along the field direction. However, nonadiabatic effects during the time evolution of the initial field-free rotational state could cause the molecule to end up in a state described by a linear combination of pendular states (a rotational wavepacket) whose alignment properties are not a priori known. We report a computational study of the time evolution of these states. We solve the reduced time-dependent Schrödinger equation for an effective Hamiltonian acting within the vibronic ground state. Our numerical results show that the time evolution and the achievement of adiabatic behavior depend critically on the detailed characteristics of the laser pulse and the rotational constant of the molecule.
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