Thermochromic Meltable Materials with Reverse Spin Transition Controlled by Chemical Design

We report a series of meltable Fe II complexes, which, depending on the length of aliphatic chains, display abrupt forward low‐spin to high‐spin transition or unprecedented melting‐triggered reverse high‐spin to low‐spin transition on temperature rise. The reverse spin transition is perfectly reproducible on thermal cycling and the obtained materials are easily processable in the form of thin film owing to their soft‐matter nature. We found that the discovered approach represents a potentially generalizable new avenue to control both the location in temperature and the direction of the spin transition in meltable compounds.