Effect of Electric-Field Fluctuations on Rotational Revival Amplitudes

We study numerically the behavior of rotational revivals in a molecular gas when subject to the fluctuating electric field of a background plasma. We model a molecule using a rigid rotor Hamiltonian and couple it to an electric field using permanent and induced multipole interaction terms. The evolution of the density matrix for the molecule is calculated for a short intense laser pulse, followed by a fluctuating background electric field. A broad superposition of angular momentum eigenstates of a molecule is created by the laser field, and the result of an ensemble average over initial molecular orientation is a set of recurring peaks in the probability density for observing a particular orientation—the so-called “rotational revivals.” The fluctuating background field is created using the dressed particle technique, and the result is a loss of coherence between the phases of the various basis states of the molecule, which causes a decreasing amplitude for subsequent alignment peaks. Modern short-pulse lasers operate with sufficient intensity to make this effect relevant to experiments in molecular alignment.