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Abstract

Photo-doped states in strongly correlated charge transfer insulators are characterized by $d-d$ and $d-p$ interactions and the resulting intertwined dynamics of charge excitations and local multiplets. Here we use femtosecond x-ray absorption spectroscopy in combination with dynamical mean-field theory to disentangle these contributions in NiO. Upon resonant optical excitation across the charge transfer gap, the Ni $L_{3}$ and O $K$ absorption edges red-shift for >10 ps, which is explained by a simultaneous Hartree shift and a renormalization of the local interactions. Furthermore, below the Ni $L_{3}$ edge an additional signature is identified for <1 ps, which reflects a transient nonthermal population of local many-body multiplets. Overall, the photo-doped state differs significantly from a chemically doped state. Our results demonstrate the ability to reveal excitation pathways in correlated materials by x-ray spectroscopies, which is relevant for ultrafast materials design.

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