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Development of novel 2D materials with singular and thrilling properties has aroused large interest due to the novel unexpected applications that can be derived from there. In this sense, coordination polymers (CPs) have appeared as matching candidates thanks to their rational chemical design and the added-value properties given by the presence of metal ions. This is the case of switchable spin crossover systems that have been proposed as excellent candidates for data storage or sensing, among others. Here we report the delamination of crystals of the 2D spin-crossover (SCO) {[Fe(L1)(2)](ClO4)(2)}(alpha) (1) CP by liquid-phase exfoliation (LPE) in water. The application of this top-down technique down to 1-2 nm thick (mostly mono- and bilayer), that retain the chemical composition and SCO interconversion of the bulk material. Moreover, these flakes can be handled as stable colloidal dispersions for many days. This allows for a controlled transfer to solid substrates and the formation of thermochromic polymeric films as a proof-of-concept of device. These first results will definitely open new venues and opportunities for the investigation and future integration of these original switchable 2D materials in devices.

Spin-Crossover in an Exfoliated 2D Coordination Polymer and Its Implementation in Thermochromic Films