Combining optical control theory with ab initio quantum chemistry and electronic crystal field theory we explore the laser induced femtosecond spin dynamics. We propose a scenario for ultrafast all-optical magnetic switching that results from the combination of spin-orbit coupling with appropriately shaped short laser pulses. We find that the application of the theory to the multiplet states within the gap of NiO(001) predicts for the first time the possibility of all-optical spin switching within 100 fs. The switching can be observed using any of the multiplets as the intermediate state.

• Received 5 May 2003

DOI:https://doi.org/10.1103/PhysRevLett.92.227402