Abstract
Metal-organic molecular systems are fascinating alternatives to conventional spintronic materials such as transition-metal oxides and diluted magnetic semiconductors, having the advantage of their structural diversity and chemical sensitivity. Here we demonstrate, based on advanced density functional theory calculations, that a cobalt-organic-molecular crystal exhibits particular spin-crossover phenomenon, which is extremely sensitive to external pressure as well as the surrounding water ligands' coordination. We found keen competition between crystal-field splitting and on-site Hund's exchange interaction, resulting in the highly-sensitive spin-crossover transition. Our finding paves the way to soft spintronics, in which molecular spin representing a bit can be easily flipped by small changes in external pressure and temperature at low energy cost.
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