Observation of <i>T</i>_LIESST above Liquid Nitrogen Temperature and Disclosure of Hidden Hysteresis in Multiresponsive Hofmann-type Coordination Polymers

Photoresponsive spin-crossover (SCO) molecules are an important class of bistable magnetic molecules with intriguing potential in device applications. The light-induced excited spin state trapping (LIESST) and the combined application of light and temperature can provide access to the metastable region of the SCO profile. The primary obstacle in utilizing light stimuli is the manifestation of light-induced trappings at extremely low temperatures. Herein, we report two novel multiresponsive 2D Hofmann-type coordination polymers exhibiting light-induced excited spin state trapping above liquid nitrogen temperature (<i>T</i>_LIESST = 82 and 81 K). Stimulating the samples in conjugation with light and temperature successfully unveils hysteresis, which is otherwise concealed. Apart from light and temperature, we found that the SCO phenomenon is also responsive to external hydrostatic pressure and exhibits modulation of the hysteresis width and transition temperature shifts with changes in pressure.