Functionalization of 2D Materials with Photosensitive Molecules: From Light‐Responsive Hybrid Systems to Multifunctional Devices

Abstract 2D materials possess exceptional physical and chemical properties that render them appealing components for numerous potential applications in (opto)electronics, energy storage, sensing, and biomedicine. However, such unique properties are hardly tunable or modifiable. The functionalization of 2D crystals with molecules constitutes a powerful strategy to adjust and modulate their properties, by also imparting them new functions. In this framework, the combination of 2D materials with photosensitive molecules is a viable route for harnessing their light‐responsive nature. The latter takes full advantage of the extremely high sensitivity of 2D materials to subtle changes in the local environment and the capacity of photosensitive molecules to modify their intrinsic properties when exposed to electromagnetic fields. The hybrid molecule–2D materials can preserve the unique optical and electrical properties of 2D layers and can exhibit additional light‐tunable features. In this Progress Report, the protocols that can be pursued for the 2D material functionalization and switching mechanisms in photosensitive systems are reviewed, followed by an in‐depth discussion on their tunable optical properties and their exploitation when integrated in novel photoswitchable electronic devices. The opportunities and associated challenges to be tackled for the development of unprecedented and high‐performance light‐responsive devices are discussed.