Tuned Range-separated Density Functional Theory and Dyson Orbital Formalism for Photoelectron Spectra

Journal of Chemical Theory and Computation
Tobias M Ouml HleSergey I Bokarev

Abstract

Photoelectron spectroscopy represents a valuable tool to analyze structural and dynamical changes in molecular systems. Comprehensive interpretation of experimental data requires, however, involvement of reliable theoretical modeling. In this communication, we present a protocol based on the combination of well-established linear-response time-dependent density functional theory and Dyson orbital formalism for the accurate prediction of both ionization energies and intensities. Essential here is the utilization of the optimally-tuned range-separated hybrid density functionals, improving the ionization potentials not only of frontier, but also of the deeper lying orbitals. In general, the protocol provides accurate results as illustrated by comparison to experiments for several gas-phase molecules, belonging to different classes. Further, we analyze possible pitfalls of this approach, and namely, discuss the ambiguities in the choice of optimal range-separation parameters, the influence of the stability of the ground state, and the spin contamination issues as possible sources of inaccuracies.

Citations

Jul 22, 2019·The Journal of Chemical Physics·Magnus W D Hanson-HeineNicholas A Besley
Feb 24, 2020·The Journal of Chemical Physics·Gilbert Grell, Sergey I Bokarev
Apr 1, 2019·The Journal of Chemical Physics·Alexey L KaledinDjamaladdin G Musaev
Jun 15, 2021·Chemical Communications : Chem Comm·Philipp DierksMatthias Bauer
Jan 4, 2020·Journal of Chemical Theory and Computation·Sascha Klawohn, Hilke Bahmann
Sep 17, 2020·Inorganic Chemistry·Philipp DierksMatthias Bauer
Sep 2, 2020·Inorganic Chemistry·J Patrick ZobelLeticia González

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