Relativistic Orbital Optimized Density Functional Theory for Accurate Core-Level Spectroscopy

• URL: http://arxiv.org/abs/2111.08405v2
• Date: Wed, 30 Mar 2022 22:40:15 GMT
• Title: Relativistic Orbital Optimized Density Functional Theory for Accurate Core-Level Spectroscopy
• Authors: Leonardo A. Cunha, Diptarka Hait, Richard Kang, Yuezhi Mao, Martin Head-Gordon
• Abstract summary: Core-level spectra of 1s electrons of elements heavier than Ne show significant relativistic effects. We combine advances in orbital optimized DFT (OO-DFT) with the spin-free exact two-component (X2C) model for scalar relativistic effects.
• Score: 0.0
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: Core-level spectra of 1s electrons of elements heavier than Ne show significant relativistic effects. We combine advances in orbital optimized DFT (OO-DFT) with the spin-free exact two-component (X2C) model for scalar relativistic effects, to study K-edge spectra of third period elements. OO-DFT/X2C is found to be quite accurate at predicting energies, yielding $\sim 0.5$ eV RMS error vs experiment with the modern SCAN (and related) functionals. This marks a significant improvement over the $>50$ eV deviations that are typical for the popular time-dependent DFT (TDDFT) approach. Consequently, experimental spectra are quite well reproduced by OO-DFT/X2C, sans empirical shifts for alignment. OO-DFT/X2C combines high accuracy with ground state DFT cost and is thus a promising route for computing core-level spectra of third period elements. We also explored K and L edges of 3d transition metals to identify limitations of the OO-DFT/X2C approach in modeling the spectra of heavier atoms.

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