Study of diatomic molecules under short intense laser pulses

TL;DR

This study uses ab initio calculations and a novel resolvent operator method to analyze the correlated electronic and nuclear dynamics of the H2+ molecule under ultrashort intense laser pulses, revealing detailed energy sharing and harmonic generation phenomena.

Contribution

It introduces the resolvent operator method for molecules, enabling detailed analysis of correlated spectra and angular distributions in strong field molecular ionization.

Findings

Correlated spectra provide more detailed information than integrated spectra.

Energy sharing differs between multiphoton and tunneling ionization regimes.

Even harmonic generation observed in light molecules with long pulses.

Abstract

In this work we report ab initio calculations for the $H_2^+$ molecule interacting with ultrashort intense laser pulses. We analyse several observables that can, in principle, be available experimentally, in order to get a deeper understanding of the strong field molecular dynamics. In particular, we will focus our attention to the interplay between electronic and nuclear dynamics and how the two motions are correlated. We have extended the Resolvent Technique to molecules and we have extracted the correlated energy spectra in different regimes of ionization: from the perturbative regime to the tunneling ionization regime. We have applied this new method, called resolvent operator method (ROM), to a 1+1D model of the $H_2^+$ molecule. We have applied this method to several photoionization regimes and we have compared with previous results in the literature. We show that the correlated spectra can provide us much more information than the integrated spectra on the electron or nuclear energy. We report the correlated energy spectrum from the multiphoton ionization to the tunneling ionization regime and how the sharing of the excess energy is different for the two regimes. We have also applied the ROM to a 3D model of the $H_2^+$ molecule in which angular distributions can be obtained. With these angular correlated spectra we show that the contributions of electrons coming from absorption of different number of photons can be disentangled. We have calculated the high harmonic spectra for a 3D model of the $H_2^+$ molecule and its isotopes. In these calculations we have observed that for sufficiently long pulses and for light molecules we observe even harmonic generation, a phenomenon that is not expected in a centrosymmetric molecule.

Full text

See pages 1-last of impressao.pdf