Details

Autor(en) / Beteiligte

• Jenkins, Andrew J
• Hu, Hang
• Lu, Lixin
• Frisch, Michael J
• Li, Xiaosong

Titel

Two-Component Multireference Restricted Active Space Configuration Interaction for the Computation of L‑Edge X‑ray Absorption Spectra

Ist Teil von

• Journal of chemical theory and computation, 2022-01, Vol.18 (1), p.141-150

Ort / Verlag

United States: American Chemical Society

Erscheinungsjahr

2022

Link zum Volltext

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• X-ray absorption spectroscopy is a powerful probe of local electronic and nuclear structures, providing insights into chemical processes. The theoretical prediction and interpretation of metal L-edge X-ray absorption spectra are complicated by both relativistic effects, including spin–orbit coupling and the multiconfigurational nature of the states involved. This work details an exact two-component multireference restricted active space (RAS) configuration interaction scheme that uses an exact two-component state-averaged complete active space self-consistent-field method, which includes the spin–orbit coupling in a variational manner, for the accurate description of the electronic structure before using a RAS configuration interaction method to describe the core excited states of the X-ray spectrum. Benchmark calculations are presented for a series of iron-containing complexes, with results showing key features of the spectrum being reproduced, including ligand-to-metal charge transfer and shake-up excitations.