We present a combined theoretical and experimental study of spin and charge dynamics on the homodinuclear compound $[{\mathrm{Ni}}_2^{\mathrm{II}}(\mathrm{L}\mathrm{\text{−}}{\mathrm{N}}_4{\mathrm{Me}}_2)(\mathrm{emb})]$. The theoretically calculated oscillator strengths of the ground-state absorption spectrum show an acceptable agreement with experiment. We predict a local ultrafast laser-induced spin-flip scenario, which involves charge-transfer states. Experimentally, we observe charge dynamics on two different time scales. The two relevant, transient electronic states and their electronic properties are also theoretically characterized. These results provide a joint investigation of the homodinuclear complex and suggest a realistic scenario for ultrafast spin dynamics and other optical-related manipulations.

• Received 24 April 2012

DOI:https://doi.org/10.1103/PhysRevLett.109.267209