Linear and Nonlinear Optics in Coherently Spinning Molecules

Abstract

Over the last two decades, coherently spinning molecules induced by laser have been a subject of current growing interest motivated by their unique individual and collective properties. From a fundamental aspect, spinning molecules had also led to a better understanding of the mechanisms at play when molecular rotors are strongly driven by an external field. In this chapter, we describe new strategies for designing laser pulses enabling the production of spinning molecules. Two rationalized approaches are first discussed highlighting major assets and flaws. In order to implement them, simple and compact optical arrangements are proposed together with the use of a pulse shaper device that provides a greater flexibility. A more sophisticated strategy relying on a non-standard pulse shaper arrangement is also discussed. Laser pulses exhibiting a twisted linear polarization are then applied to control the rotation of linear molecules subsequently used as ultrafast phase modulators. The rotational Doppler shifts resulting from the linear and nonlinear scattering of a circularly polarized laser pulse with fast spinning molecules are investigated both experimentally and numerically.