Orbital-resolved calculations of two-center interferences in linear triatomic molecules

Kyle A. Hamer, Louisiana State University
Daniel R. Tuthill, The Ohio State University
Timothy D. Scarborough, The Ohio State University
Louis F. DiMauro, The Ohio State University
Kenneth Lopata, Louisiana State University
Kenneth J. Schafer, Louisiana State University
Mette B. Gaarde, Louisiana State University
François Mauger, Louisiana State University


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.