Ultrafast coupled charge and spin dynamics in strongly correlated NiO

Abstract

Charge excitations across an electronic band gap play an important role in opto-electronics and light harvesting. In contrast to conventional semiconductors, studies of above-band-gap photoexcitations in strongly correlated materials are still in their infancy. Here we reveal the ultrafast dynamics controlled by Hund’s physics in strongly correlated photoexcited NiO. By combining time-resolved two-photon photoemission experiments with state-of-the-art numerical calculations, an ultrafast (≲10 fs) relaxation due to Hund excitations and related photo-induced in-gap states are identified. Remarkably, the weight of these in-gap states displays long-lived coherent THz oscillations up to 2 ps at low temperature. The frequency of these oscillations corresponds to the strength of the antiferromagnetic superexchange interaction in NiO and their lifetime vanishes slightly above the Néel temperature. Numerical simulations of a two-band t-J model reveal that the THz oscillations originate from the interplay between local many-body excitations and antiferromagnetic spin correlations.