Journal des nanomatériaux et de la nanotechnologie moléculaire

Electronic Theory of Ultrafast Spin Dynamics in NiO

Chun Li, Georgios Lefkidis and Wolfgang H?bner

Electronic Theory of Ultrafast Spin Dynamics in NiO

NiO is a good candidate for ultrafast magnetic switching because of its large spin density, antiferromagnetic order, and clearly separated intragap states. In order to detect and monitor the switching dynamics, we develop a systematic approach to study optical second harmonic generation (SHG) in NiO, both at the (001) surface and in the bulk. In our calculations NiO is modeled as a doubly embedded cluster. All intragap d-states of the bulk and the (001) surface are obtained with highly-correlational quantum chemistry and propagated in time under the influence of a static magnetic field and a laser pulse. We find that demagnetization and switching can be best achieved in a subpicosecond regime with linearly rather than circularly polarized light. We also show the importance of including an external magnetic field in order to distinguish spin-up and spin-down states and the necessity of including magnetic-dipole transitions in order to realize the process in the centrosymmetric bulk. Having already shown the effects of phonons in the SHG for the bulk NiO within the frozen-phonon approximation, and following the same trail of thoughts, we discuss the role of phonons in a fully quantized picture as a symmetrylowering mechanism in the switching scenario and investigate the electronic and lattice temperature effects.