Abstract

AbstractWe construct a microscopic theory on the photomagnetism in the cyano‐bridged bimetallic assemblies Cu2[Mo(CN)8]·��H2O. Going through a grouptheoretical analysis on the ground‐state properties, we simulate photoirradiation and the resultant magnetization dynamics with a time‐dependent Hartree‐Fock method.It is not c‐axis‐polarized photons but those polarized in the ab plane that induce a macroscopic magnetization. Absorption of the photon energy is double‐stepped and the occurrence of a significant magnetization is simultaneous with the second stage (© 2012 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

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