Abstract
We present a fully ab initio theory of ultrafast spin switching in nanostructures using optical control theory and including spin-orbit coupling thus realizing Λ processes. These processes are investigated using high-level quantum chemistry in structures with one, two, and three magnetic centers, where the spin localization and transferability are discussed with respect to their geometry. In particular we study metallic chains with two and three magnetic centers interconnected with Na atoms. We discuss the prerequisites for such scenarios for all structures.
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