We present a fully ab initio theory for coherent laser-induced ultrafast spin manipulation on the homodinuclear magnetic clusters FeOFe, FeOOFe, NiONi, and NiOONi. With the oxygen atom(s) bridging the magnetically active centers, the clusters tend to adopt asymmetric geometries due to the Jahn-Teller effect. Therefore they have well-defined spin localization which is required for local spin manipulation. We find that both spin-flip and spin-transfer scenarios can be achieved on the clusters FeOFe and FeOOFe while only spin flip is realized on NiONi and NiOONi, based on which we predict that the Fe-containing clusters are quite promising for logic operations. The different dynamical behavior on these systems is analyzed in detail from the viewpoint of their distinct electronic structures and related spectra. In striving for better magnetization dynamics control, the results obtained on these prototypic systems strongly indicate their great potential in spintronic device design and future practical applications.

• Received 20 September 2013
• Revised 11 December 2013

DOI:https://doi.org/10.1103/PhysRevB.89.024419