We investigate experimentally and numerically the field-free orientation of the symmetric top molecule of methyl-iodide at high temperature using a terahertz radiation generated by a plasma induced by a two-color laser beam. The degree of orientation is measured from the free-induction decay emitted by the sample. The observed experimental signal is reproduced with a good accuracy by numerical simulations.

We study the classical and quantum rotation numbers of the free rotation of asymmetric top molecules. We show numerically that the quantum rotation number converges to its classical analog in the semi-classical limit. Different asymmetric molecules such as the water molecule are taken as illustrative example. A simple approximation of the classical rotation number is derived in a neighborhood of the separatrix connecting the two unstable fixed points of the system. Furthermore, a signature of the classical tennis racket effect in the spectrum of asymmetric molecules is identified.The variables (K, α K ) describe the dynamics of the angular momentum J in the body-fixed frame. With the convention:we deduce the following identification:The Hamiltonian H can be expressed in terms of the new set of coordinates as follows:A first action of the system is given by J, the second I can be written as: