Electron-Nuclear Dynamics on Amplitude and Frequency Modulation of Molecular High-Order Harmonic Generation from H2 + and its Isotopes

Abstract

Abstract Electron-nuclear dynamics of molecular high-order harmonic generation from H2 + and its isotopes has been theoretically investigated beyond the Born-Oppenheimer approximations. The results show that (i) due to the different ionisation probabilities and the harmonic emission times, the intensities of the harmonics from H2 + and its isotopes are very sensitive to the initial vibrational state, the pulse duration, and the pulse intensity. (ii) Due to the nonadiabatic effects in molecular high-order harmonic generation, the red-shifts of the harmonics can be found in the lower pulse intensity. With the increase of the pulse intensity, the harmonics are from the red-shifts to the blue-shifts. Moreover, as the pulse duration increases, the blue-shifts of the harmonics can be enhanced. As the initial vibrational state increases, the red-shifts of the harmonics can be decreased, whereas the blue-shifts of the harmonics can be enhanced. However, the shifts of the harmonics are decreased as the nuclear mass increases. (iii) Due to the coupled electron-nuclear dynamics in molecules, the spatial symmetry of the system is broken. As a result, non-odd harmonics can be generated at the larger internuclear distance. With the increase of the initial vibrational state or the nuclear mass, the generation of the non-odd harmonics can be enhanced and reduced, respectively. As the pulse duration or the pulse intensity increase, the generation of the non-odd harmonics can be enhanced. However, the intensities of the non-odd harmonics are decreased when using the longer pulse duration with the much higher laser intensity.