Abstract

A fully ab initio controlled ultrafast magnetooptical switching mechanism in small magnetic clusters is achieved through exploiting spin-orbit-coupling enabled Λ processes. The idea is that in the magnetic molecules a fast transition between two almost degenerate states with different spins can be triggered by a laser pulse, which leads to an electron excitation from one of the degenerate states to a highly spin-mixed state and a deexcitation to the state of opposite spin. In this paper a CO molecule is attached to one magnetic center of the clusters, which serves as an experimental marker to map the laser-induced spin manipulation to the IR spectrum of CO. The predicted spin-state-dependent CO frequencies can facilitate experimental monitoring of the processes. We show that spin flip in magnetic atoms can be achieved in structurally optimized magnetic clusters in a subpicosecond regime with linearly polarized light.

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