Reversible Control by Light of the High‐Spin Low‐Spin Elastic Interface inside the Bistable Region of a Robust Spin‐Transition Single Crystal

By using a weak modulated laser intensity we have succeeded in reversibly controlling the dynamics of the spin-crossover (SC) single crystal [{Fe(NCSe)(py)2 }2 (m-bpypz)] inside the thermal hysteresis. The experiment could be repeated several times with a reproducible response of the high-spin low-spin interface and without crystal damage. In-depth investigations as a function of the amplitude and frequency of the excitation brought to light the existence of a cut-off frequency ca. 1.5 Hz. The results not only document the applicability of SC materials as actuators, memory devices, or switches, but also open a new avenue for the reversible photo-control of the spin transition inside the thermal hysteresis.