Birefringence arising from the reorientation of the polarizability anisotropy of molecules in collisionless gases

The refractive-index change in a collisionless gas is evaluated from the Stark shifts of the rotational energy levels that arise from the polarizability anisotropy. In the limit of an extremely-short-duration excitation, a multilevel coherent effect results in delayed refractive-index bursts. Both stationary and transient responses of this birefringence to an optical field are considered for symmetric-top molecules, with particular emphasis on the special case of linear molecules.