Abstract

By using a heated molecular beam in combination with a time-of-flight mass spectrometer, we experimentally study the ionization of vibrational-hot carbon disulfide (CS2) molecules irradiated by a linearly polarized 800-nm 50-fs strong laser field. The ion yields are measured in a laser intensity range of 7.0 × 1012 W/cm2–1.5 × 1014 W/cm2 at different molecular temperatures of up to 1400 K. Enhanced ionization yield is observed for vibrationally excited CS2 molecules. The results show that the enhancement decreases as the laser intensity increases, and exhibits non-monotonical dependence on the molecular temperature. According to the calculated potential energy curves of the neutral and ionic electronic states of CS2, as well as the theoretical models of molecular strong-field ionization available in the literature, we discuss the mechanism of the enhanced ionization of vibrational-hot molecules. It is indicated that the enhanced ionization could be attributed to both the reduced ionization potential with vibrational excitation and the Frank–Condon factors between the neutral and ionic electronic states. Our study paves the way to understanding the effect of nuclear motion on the strong-field ionization of molecules, which would give a further insight into theoretical and experimental investigations on the interaction of polyatomic molecules with strong laser fields.

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