Retrieval of Angle-Dependent Strong-Field Ionization by Using High Harmonics Generated from Aligned N2 Molecules

We propose a method to retrieve the angle-dependent strong-field ionization of highest occupied molecular orbital (HOMO) from high-order harmonic generation (HHG) of aligned molecules. This method is based on the single-molecule quantitative rescattering model with known alignment distribution and photo-recombination cross sections of fixed-in-space molecules. With the macroscopic HHG of aligned N-2 molecules, we show that angle-dependent ionization of HOMO can be successfully retrieved at both low and high degrees of alignment. We then show that the error in the retrieved angular dependence of ionization becomes larger if the uncertainty in the alignment distribution is introduced in the retrieval procedure. We also examine that the retrieved ionization of HOMO is much deviated from the accurate one if the intensity of probe laser becomes higher such that inner HOMO-1 can contribute to HHG.

Automated summary

This study presents a method to retrieve the angle-dependent strong-field ionization of aligned molecules' highest occupied molecular orbital (HOMO) from high-order harmonic generation (HHG). The research shows that the angle-dependent ionization of HOMO can be successfully retrieved at low and high degrees of alignment, but the error in retrieval increases with uncertainty in the alignment distribution.