Alignment of asymmetric-top molecules using multiple-pulse trains

We theoretically analyze the effectiveness of multiple-pulse laser alignment methods for asymmetric-top molecules. As an example, we choose SO2 and investigate the alignment dynamics induced by two different sequences, each consisting of four identical laser pulses. Each sequence differs only in the time delay between the pulses. Equally spaced pulses matching the alignment revival of the symmetrized SO2 rotor model are exploited in the first sequence. The pulse separations in the second sequence are short compared to the rotation dynamics of the molecule and monotonically increase the degree of alignment until the maximum alignment is reached. We point out the significant differences between the alignment dynamics of SO2 treated as an asymmetric-top and a symmetric-top rotor, respectively. We also explain why the fast sequence of laser pulses creates considerably stronger one-dimensional molecular alignment for asymmetric-top molecules. In addition, we show that multiple-pulse trains with elliptically polarized pulses do not enhance one-dimensional alignment or create three-dimensional alignment.