INTENSE-FIELD MOLECULAR-SPECTROSCOPY - VIBRATIONAL AND ROTATIONAL EFFECTS IN HARMONIC-GENERATION BY H-2+

We present results of a complete treatment of electronic, vibrational, and rotational motion in numerical calculation of harmonic generation (HG) of 1064-nm laser radiation by the H-2+ molecular ion for intensities 10(13) less-than-or-equal-to I less-than-or-equal-to 10(14) W/cm2. We show that efficient HG can be enhanced by suppression of photodissociation, a phenomenon which results from vibrational trapping in laser-field-induced potential wells. The HG spectra exhibit peaks clustered around even and odd harmonic orders. All peaks can be assigned to Raman-like transitions between dressed eigenstates of the field-molecule system. Rotational excitation is shown to compete with HG. Thus harmonic generation and photon scattering in molecules holds the promise of a potential diagnostic for molecular stabilization by intense laser fields.