Ultrafast manipulation of the NiO antiferromagnetic order via sub gap optical excitation

Wide band gap insulators such as NiO offer the exciting prospect of coherently manipulating electronic correlations with strong optical fields. Contrary to metals where rapid dephasing of optical excitation via electronic processes occurs, the sub gap excitation in charge transfer insulators has been shown to couple to low energy bosonic excitations. However, it is currently unknown if the bosonic dressing field is composed of phonons or magnons. Here we use the prototypical charge transfer insulator NiO to demonstrate that 1.5 eV sub gap optical excitation leads to a renormalised NiO band gap in combination with a significant reduction of the antiferromagnetic order. We employ element specific X ray reflectivity at the FLASH free electron laser to demonstrate the reduction of the upper band edge at the O 1s 2p core valence resonance K edge whereas the antiferromagnetic order is probed via X ray magnetic linear dichroism XMLD at the Ni 2p 3d resonance L2 edge . Comparing the transient XMLD spectral line shape to ground state measurements allows us to extract a spin temperature rise of 65 5 K for time delays longer than 400 fs while at earlier times a non equilibrium spin state is formed. We identify transient mid gap states being formed during the first 200 fs accompanied by a band gap reduction lasting at least up to the maximum measured time delay of 2.4 ps. Electronic structure calculations indicate that magnon excitations significantly contribute to the reduction of the NiO band ga