Rotational Doppler effect in harmonic generation from spinning molecules

We present an observation of the rotational Doppler shift in the frequency of optical harmonic generated in fast rotating molecules. Conservation of energy and angular momentum in the light-molecule interaction suggests four different kinds of shifts depending on the mutual handedness of the circularly polarized fundamental and harmonic fields, as well as the handedness of the molecular rotation. All four types of the frequency shifts were observed in our experiments on third-harmonic generation in a gas of fast spinning O₂ molecules.