An Assessment of Different Electronic Structure Approaches for Modeling Time-Resolved X-ray Absorption Spectroscopy

Abstract

We assess the performance of different protocols for simulating excited-state X-ray absorption spectra. We consider three different protocols based on equation-of-motion coupled-cluster singles and doubles, two of them combined with the maximum overlap method. The three protocols differ in the choice of a reference configuration used to compute target states. Maximum-overlap-method time-dependent density functional theory is also considered. The performance of the different approaches is illustrated using uracil, thymine, and acetylacetone as benchmark systems. The results provide guidance for selecting an electronic structure method for modeling time-resolved X-ray absorption spectroscopy.

arXiv commentRevised version submitted to Structural Dynamics (January 2021)

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• Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy
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• Generalization of one-center non orthogonal configuration interaction singles to open shell singlet reference states: Theory and application to valence-core pump-probe states in acetylacetone
• Ultrafast Charge Migration Dynamics in Enol Keto Tautomerization Monitored with a Local Soft-X-Ray Probe
• Resolving Competing Conical Intersection Pathways: Time-Resolved X-ray Absorption Spectroscopy of trans-1,3-Butadiene