Field Free Dimensional Algnment of Molecules with Varying Degrees of Symmetry

A number of methods have been developed to achieve aligned or oriented distributions of polyatomic molecules. Nonetheless, achieving strong alignment of all three molecular axes remains a challenge. Furthermore, most studies have focused on prolate-type asymmetric top molecules with their most polarizable and fastest axis being the same, such as Iodobenzne. Here, we computationally investigate the application of multiple laser pulses with different polarizations to molecules with varying symmetry in their moment inertia and polarizability tensors. We find that a pulse sequence previously demonstrated to produce three-dimensional alignment (3DA) of Iodobenzene under field-free conditions fails do so in general. We find new pulse sequences that generate 3DA for molecules with different symmetry properties, and prescribe a strategy for 3DA of asymmetric top molecules.