Contribution of the pre-ionized H$_2$ and the ionized H$_2^+$ subsystems to the HHG Spectra of H$_2$ in intense laser fields

TL;DR

This study investigates how pre-ionized and ionized subsystems of H₂ contribute to high-order harmonic generation under intense ultrafast laser pulses, revealing intensity-dependent spectral features and the influence of nuclear dynamics.

Contribution

It provides a detailed analysis of the roles of pre-ionized and ionized H₂ subsystems in HHG, highlighting the effects of laser intensity, wavelength, and nuclear motion on the spectra.

Findings

PI-H₂ dominates HHG at lower intensities.

Both subsystems contribute at higher intensities.

Even and odd harmonics vary with intensity and wavelength.

Abstract

Contributions of the pre-ionized H$_2$ (PI-H$_2$) and ionized H$_2^+$ subsystems of the two-electron H$_2$ system to its high-order harmonic generation in 8-cycle $\sin^{2}$-like ultrafast intense laser pulses are calculated and analyzed based on the solution of the time-dependent Schr\"{o}dinger equation (TDSE) for the one-dimensional two-electronic H$_2$ system with fixed nuclei. The laser pulses have $\lambda\ =\ 390\ \&\ 532$ nm wavelengths and $I=1\times 10^{14}$, 5$\times 10^{14}$, 1$\times 10^{15}$ \&\ 5$\times 10^{15}$ Wcm$^{-2}$ intensities. It is found that at the two lower intensities, the PI-H$_2$ subsystem dominantly produces the HHG spectra. While, at the two higher intensities, both PI-H$_2$ and ionized H$_2^+$ subsystems contribute comparably to the HHG spectra. In the H$_2^+$ subsystem, the symmetry of the populations of H$_2^+$(I) and H$_2^+$(II) regions (left and right regions of H$_2^+$ subsystem) is broken by increasing the laser intensity. Complex patterns and even harmonics also appear at these two higher intensities. For instance, at $1\times 10^{15}$ Wcm$^{-2}$ intensity and $\lambda$ = 532 nm, the even harmonics are appeared near cut-off region. Interestingly, at $5\times 10^{15}$ Wcm$^{-2}$ intensity and $\lambda$ = 390 nm, the even harmonics replaced by the odd harmonics with red shift. At $\lambda$ = 390 \&\ 532 nm and $I=1\times 10^{15}$ intensity, the two-electron cutoffs corresponding to nonsequential double-recombination (NSDR) with maximum return kinetic energy of 4.70$U_p$ are detected. The HHG spectra of the whole H$_2$ system obtained with and without nuclear dynamics treated classically are approximately similar. However, at $1\times 10^{15}$ Wcm$^{-2}$ intensity and $\lambda$ = 532 nm, if we take into account nuclear dynamics, the even harmonics which are appeared near cutoff region, replaced by the odd harmonics with blue shift.