Probing ultrafast photo-induced dynamics of the exchange energy in a Heisenberg antiferromagnet

Femtosecond stimulated Raman experiments on the antiferromagnetic system KNiF3 are implemented to understand how the exchange interaction — a crucial interaction that rules magnetic phenomena — is influenced by ultrafast optical excitation. Manipulating the macroscopic phases of solids using ultrashort light pulses has resulted in spectacular phenomena, including metal–insulator transitions1,2,3, superconductivity4 and subpicosecond modification of magnetic order5. The development of this research area strongly depends on the understanding and optical control of fundamental interactions in condensed matter, in particular the exchange interaction. However, disentangling the timescales relevant for the contributions of the exchange interaction and spin dynamics to the exchange energy, Eex, is a challenge. Here, we introduce femtosecond stimulated Raman scattering to unravel the ultrafast photo-induced dynamics of magnetic excitations at the edge of the Brillouin zone. We find that femtosecond laser excitation of the antiferromagnet KNiF3 triggers a spectral shift of the two-magnon line, the energy of which is proportional to Eex. By unravelling the photo-induced modification of the two-magnon line frequency from a dominating nonlinear optical effect, we find that Eex is increased by the electromagnetic stimulus.