Correlating Valence and 2p3d RIXS Spectroscopies: A Ligand-Field Study of Spin-Crossover Iron(II)

Spin-crossover complexes also provide a unique opportunity to study the ligand field properties of a system in both HS and LS states while maintaining the same ligand environment. Presently, we employ complementing valence and core-level spectroscopic methods to probe the electronic excited state manifolds of the spin-crossover complex [FeII(H2B(pz)2)2phen]0.

Light-induced excited spin state trapping (LIESST) at liquid He temperatures is exploited to characterize magnetic and spectroscopic properties of the photo-induced HS state using SQUID and MCD spectroscopy. In parallel, Fe 2p3d RIXS spectroscopy is employed to examine the S = 0, 1 excited ligand-field (LF) states. These experimental studies are combined with state-of-the-art CASSCF/NEVPT2 and CASCI/NEVPT2 calculations characterizing the ground and LF excited states.