Layered Spin-Crossover Metal-Organic Frameworks for Light-Induced Control of Two-Dimensional Quantum Materials.

Metal-organic frameworks (MOFs) are widely explored for gas separation, catalysis, or energy storage, yet their integration with other electronically functional materials remains largely unexplored. Here, we integrate the layered Hofmann-type spin-crossover (SCO) MOF {FeII(pyS2Et)2[PtII(CN)4]} into electrical nanodevices to control the properties of two-dimensional (2D) quantum materials. Our molecular approach exploits the stimuli-responsive nature of SCO-layered materials as switchable building blocks. We demonstrate selective modulation of the electronic transport in van der Waals heterostructures interfacing SCO with 2D quantum materials (few-layer graphene, magnetic CrSBr, superconducting NbSe2) through the strain induced via thermal and light-induced spin transitions. In graphene, the conductivity is selectively switched by light. In spin-valves based on CrSBr bilayers, the MOF triggers magnetic hysteresis (absent in pristine CrSBr) and enables tunable non-volatile zero-field memory. In NbSe2, light modulates the superconducting critical current and transition temperature. These results establish layered stimuli-responsive SCO MOFs as active molecular control elements for 2D quantum materials, providing a route to strain-mediated control of electronic, magnetic, and superconducting functionalities, and extending MOF-based architectures beyond traditional porous-matter applications toward multifunctional electronics and spintronics.