The effect of pressure on the dinuclear spin crossover material [{Fe(bpp)(NCS)(2)}(2)(4,4'-bipy)]·2MeOH (where bpp = 2,6-bis(pyrazol-3-yl)pyridine and 4,4'-bipy = 4,4'-bipyridine, 1) has been investigated with single crystal X-ray diffraction and Raman spectroscopy using diamond anvil cell techniques. The very gradual pressure-induced spin crossover occurs between 7 and 25 kbar, and shows no evidence of crystallographic phase transitions. The pressure-induced spin transition leads to a complete LS state which is not thermally accessible. This structural evolution under pressure is in stark contrast to the previously reported thermal spin crossover behaviour, in which a symmetry-breaking, purely structural phase transition results in only partial conversion to the low spin state. This observation is attributed to the symmetry-breaking phase transition becoming unfavourable under pressure.
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