Dynamical control of the spin transition inside the thermal hysteresis loop of a spin-crossover single crystal

We have succeeded to achieve experimentally, using an adapted optical microscopy setup, the reversible control of the front transformation between the low-spin (LS)–high-spin (HS) interface in the spin-crossover (SC) single crystal [{Fe(NCSe)(py)2}2(m-bpypz)] undergoing a first-order transition at 112 K with a 7 K hysteresis width. For that, we first generate a phase separation state (a HS/LS interface at equilibrium) inside the hysteresis loop by tuning the light intensity of the microscope. In the second step, this intensity is monitored in such a way to drive, through a photo-heating process, the interface motion. This photo-control is found to be reversible, accurate and requiring a very small amount of energy. In addition the integrity of the crystal is maintained even after a large number of cycling. The experimental observations, are well described as a reaction diffusion process accounting for the front propagation and the photo-heating effects.