Study of double core hole excitations in molecules by X-ray double-quantum-coherence signals: a multi-configuration simulation.

ABSTRACT: The multi-configurational self-consistent field method is employed to simulate the two-dimensional all-X-ray double-quantum-coherence (XDQC) spectroscopy, a four-wave mixing signal that provides direct signatures of double core hole (DCH) states. The valence electronic structure is probed by capturing the correlation between the single (SCH) and double core hole states. The state-averaged restricted-active-space self-consistent field (SA-RASSCF) approach is used which can treat the valence, SCH, and DCH states at the same theoretical level, and applies to all types of DCHs (located on one or two atoms, K-edge or L-edge), with both accuracy and efficiency. Orbital relaxation introduced by the core hole(s) and the static electron correlation is properly accounted for. The XDQC process can ta

SUBMITTER: Hua W 

PROVIDER: S-EPMC6022231 | biostudies-literature | 2016 Sep

REPOSITORIES: biostudies-literature