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

Autor:	Kenneth Lopata, Mette B. Gaarde, Kyle A. Hamer, Timothy D. Scarborough, Kenneth J. Schafer, Daniel R. Tuthill, Louis F. DiMauro, Francois Mauger
Rok vydání:	2021
Předmět:	Physics Harmonic spectrum Dipole Atomic orbital Scattering Ab initio quantum chemistry methods Triatomic molecule Density functional theory Time-dependent density functional theory Physics::Chemical Physics Molecular physics
Zdroj:	Physical Review A. 104
ISSN:	2469-9934 2469-9926
DOI:	10.1103/physreva.104.033114
Popis:	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.
Databáze:	OpenAIRE
Externí odkaz:	https://explore.openaire.eu/search/publication?articleId=doi_________::54c812050e190ef80ec42086506d523a https://doi.org/10.1103/physreva.104.033114 Zobrazit plný text záznamu