Orbital-resolved calculations of two-center interferences in linear triatomic molecules
We perform ab initio calculations of high-harmonic spectroscopy (HHS) of two-center interference phenomena in oriented carbon-dichalcogen molecules, using time-dependent density functional theory (TDDFT). We show that by resolving the harmonic response into contributions from individual Kohn-Sham orbitals, we can extract target-specific characteristics for both the spectral amplitude and phase. We also discuss that this extraction is predicated on a careful analysis and normalization of the harmonic spectrum. Finally, we present field-free scattering calculations that mimic the recollision step in high-order-harmonic generation and allow the calculation of recombination dipole matrix elements without explicitly calculating the scattering states of a molecule. We show that the orbital-resolved TDDFT HHS results and results based on our field-free scattering calculations are in very good agreement with each other.
Publication Source (Journal or Book title)
Physical Review A
Hamer, K., Tuthill, D., Scarborough, T., DiMauro, L., Lopata, K., Schafer, K., Gaarde, M., & Mauger, F. (2021). Orbital-resolved calculations of two-center interferences in linear triatomic molecules. Physical Review A, 104 (3) https://doi.org/10.1103/PhysRevA.104.033114