title: Calibration of Energy-Specific TDDFT for Modeling K-edge XAS Spectra of Light Elements.
abstract: X-ray absorption spectroscopy (XAS) has become a powerful technique in chemical physics, because of advances in synchrotron technology that have greatly improved its temporal and spectroscopic resolution. Our recent work on energy-specific time-dependent density functional theory (ES-TDDFT) allows for the direct calculation of excitation energies in any region of the absorption spectrum, from UV-vis to X-ray. However, the ability of different density functional theories to model X-ray absorption spectra (XAS) of light elements has not yet been verified for ES-TDDFT. This work is a calibration of the ability of existing DFT kernels and basis sets to reproduce experimental K-edge excitation energies. Results were compared against 30 different transitions from gas-phase experiments. We focus on six commonly used density functionals (BHandHLYP, B3LYP, PBE1PBE, BP86, HSE06, LC-ωPBE) and various triple-ζ basis sets. The effects of core and diffuse functions are also investigated.
authors.affiliation: Department of Chemistry, University of Washington , Seattle, Washington 98195, United States.
authors.forename: Patrick J
authors.initials: PJ
authors.lastname: Lestrange
authors.affiliation: Department of Chemistry, University of Washington , Seattle, Washington 98195, United States.
authors.forename: Phu D
authors.initials: PD
authors.lastname: Nguyen
authors.affiliation: Department of Chemistry, University of Washington , Seattle, Washington 98195, United States.
authors.forename: Xiaosong
authors.initials: X
authors.lastname: Li