First-principles calculation of the ultrafast spin manipulation of two-center metallic clusters with a CO molecule attached to one center as an infrared marker

Abstract

We present a fully ab initio ultrafast spin manipulation calculation in two-magnetic-center clusters with CO attached to one of the magnetic centers. CO serves as an experimental marker for certain magnetic states between which spin flip and transfer can be achieved. The predicted spin-state-dependent CO vibrational frequencies indicate that spin manipulation can be readily monitored through the infrared spectrum. The feasibility is demonstrated by two charged clusters ${[{\text{CoMg}}_{2}\text{Ni-CO}]}^{+}$ and ${[\text{NiCo-CO}]}^{+}$. Spin transfer between magnetic centers is achieved with a fidelity of 99.8%.