By using aw eak modulated laser intensity we have succeeded in reversibly controlling the dynamics of the spincrossover (SC) single crystal [{Fe(NCSe)(py) 2 } 2 (m-bpypz)] inside the thermal hysteresis.The experiment could be repeated several times with ar eproducible response of the high-spin low-spin interface and without crystal damage.I n-depth investigations as af unction of the amplitude and frequency of the excitation brought to light the existence of ac ut-off frequency ca. 1.5 Hz. The results not only document the applicability of SC materials as actuators,m emory devices,or switches,but also open anew avenue for the reversible photocontrol of the spin transition inside the thermal hysteresis.
Thecontrolofthedynamicsoffirst-orderphasetransitionsisavery general and appealing problem in adiversity of fields.It concerns the irreversible character of the processes involved and makes their control of very high importance from the fundamental point of view and also for technological applications.T hus,s ystems showing propagating-interface phenomena include fluid invasion in porous media, flame fronts, cracks,d omain wall in ferroic materials.A lthough very different, their microscopic descriptions share very similar physics at the macroscopic scale and can be described under au nifying framework involving competitions between elasticity and pinning by disordered medium. In cooperative spincrossover solids, [1][2][3][4] the thermally induced first-order transition involves two spin states,n amely the low-spin (LS, diamagnetic) and the high-spin (HS,p aramagnetic) and is accompanied by as izeable volume change and thermal hysteresis loop.F or comparison, in magnetic systems,t he control of the interface between ferromagnetic and paramagnetic domains is made possible thanks to the magnetic field, which induces the domain-wall motion, [5][6][7] which may be reversible under some conditions owing to the presence of the demagnetizing field created by the dipolar magnetic interactions.Such acontrol by afield parameter is no longer possible in spin-crossover solids,s ince the macroscopic interfaces separating the LS and HS states are elastic in nature.A xial pressure might act as an efficient control parameter;h owever its practical realization faces serious challenges,s uch as the brittle nature of the spin-crossover single crystals. [8][9][10] Among the promising multifunctional materials,m ultiferroic systems are of note,t hese are studied as ar oute to harness magneto-electric coupling and enable ar ange of applications whereby magnetism (resp.f erroelectricity) can be controlled by an electric (resp.m agnetic) field. [11][12][13] Interestingly,m ultiferroic Jahn-Teller switches have been already reported for Prussian Blue analogues [14][15][16] demonstrating the important role of the elastic interactions in the control of the electronic properties of SC solids.B ut elasticity is also at the heart of many other types of phase transitions,s uch as in the Mott metal-insulator transition [17] where it has ...