Optical-field-induced pendular states and pendular band contours in symmetric tops

The pendular states that arise from the interaction between a polarizable symmetric top and a strong, polarized optical field are investigated. Analytical solutions to the Schrödinger equation for this situation are presented corresponding to the limit of large field-polarizability interaction. The eigenfunctions and eigenvalues obtained are used to explore the manifestations of pendular states in nonlinear Raman and electric-dipole-allowed spectroscopies—that is, pendular band contours. The theoretical expectations regarding pendular band contours are compared with direct numerical simulations of the contours and with experimental results from nonlinear Raman spectroscopy on benzene–Ar and naphthalene trimer.