Molecular electronics offers an elegant tool to miniaturize electronic devices, reaching the nanoscale or even the single-molecule level. One of the limitations of this approach concerns the insulating character of most of the molecular systems one wants to integrate in the device. Here we show that the deposition of these functional molecules over graphene and other 2D semiconducting materials can provide an efficient way to avoid this limitation. This concept provides an entire new class of molecular/2D heterostructures in which we take advantage of using the “all surface” 2D material to sense the properties of the molecular component electrically or optically via an active control of the hybrid interface. We will illustrate this concept by choosing as molecular component spin-crossover molecules. This type of magnetic molecules provides an appealing example of molecular bistability as they can switch between two spin states upon the application of an external stimulus (temperature, light, or pressure). This spin switching can occur near room temperature and is always accompanied by a significant change of volume (by ca. 10%), so it can generate a significant strain over the 2D material. Hence, they constitute an ideal component to fabricate molecular memory devices. In this talk we show that in these heterostructures the 2D material can act as a reliable and highly sensitive spin state sensor, using the changes observed in the electrical or optical properties of the 2D material to readout the spin state.

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