2020/10/07 by Daniel R. Nascimento, Elisa Biasin, Nascimento, Daniel R. +10
Chemistry · Materials Science · Medicine · Physics and Astronomy · #Advanced NMR Techniques and Applications #Atomic physics #Chemical Physics (physics.chem-ph) #Crystallography and Radiation Phenomena #Density functional theory #FOS: Physical sciences #Inelastic neutron scattering #Inelastic scattering #Medicine #Nuclear physics #Physics #Protocol (science) #Quantum mechanics #Resonant inelastic X-ray scattering #Scattering #X-ray #X-ray Diffraction in Crystallography #physics.chem-ph
paper · pdf · doi:10.48550/arxiv.2010.03092
arxiv created 2020/10/07 · openalex publication_date 2020/10/07 · arxiv updated 2020/10/08 · openalex created_date 2020/10/15 · openalex updated_date 2026/07/28
We present a time-dependent density functional theory (TDDFT) based approach to compute the light-matter couplings between two different manifolds of excited states relative to a common ground state. These quantities are the necessary ingredients to solve the Kramers--Heisenberg equation for resonant inelastic X-ray scattering (RIXS) and several other types of two-photon spectroscopies. The procedure is based on the pseudo-wavefunction approach, where TDDFT eigenstates are treated as a configuration interaction wavefunction with single excitations, and on the restricted energy window approach, where a manifold of excited states can be rigorously defined based on the energies of the occupied molecular orbitals involved in the excitation process. We illustrate the applicability of the method by calculating the 2p4d RIXS maps of three representative Ruthenium complexes and comparing them to experimental results. The method is able to accurately capture all the experimental features in all three complexes, with relative energies correct to within 0.6 eV at the cost of two independent TDDFT calculations.