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Photoinduced Bidirectional Magnetism against Monodirectional Electronics in Square-Antiprismatic Octacyanometalates

Irradiating ${\rm Cu}_2{\rm Mo}({\rm CN})_8\cdot 8{\rm H}_2{\rm O}$ with blue light induces a global magnetization, whereas succeeding irradiations with red or longer-wavelength light demagnetize this material. We solve the time-dependent Schrödinger equation for an extended Hubbard model to reproduce the photoreversible magnetism. Monitoring the photoinduced optical-conductivity and angle-resolved-photoemission spectra, we reveal that the magnetic round trip by way of ferromagnetism is far from a return in terms of electronics. While visible-light-induced magnetization has never been observed in the tungsten analog ${\rm Cu}_2{\rm W}({\rm CN})_8\cdot 5{\rm H}_2{\rm O}$, infrared-light irradiation may magnetize this material as well.