S-matrix theory of high harmonic generation and ionization of coherently ro-vibrating linear molecules by intense ultrashort laser pulses

A theory of high harmonic generation and ionization of coherently rotating and vibrating linear molecules by a delayed pair of intense ultrashort laser pulses is presented. It correlates the nuclear motions in real time with the modulation of the harmonic emission and ionization signals as a function of the time-delay between the exciting and the probing pulses. An illustrative analytical example of the excitation and detection of the clock-motion associated with the 0-1 vibrational oscillation of a diatomic molecule is also given.