Organic field-effect transistors (OFETs) are crucial elements for the fabrication of flexible, wearable, and biocompatible electronic devices. As miniaturization is approaching its limits, bringing an end to Moore’s law, beyond−CMOS devices, “More-than-Moore” technologies aimed at functional diversification are emerging as a technologically viable strategy to boost data storage capacity in tomorrow’s digital electronics. Two-dimensional covalent organic frameworks (2D COFs) are tailored by covalently tethering suitably designed small organic units to form planar π-conjugated 2D networks. Since 2D COFs are constructed through the chemical tethering of different building blocks (cornerstones and linkers) via dynamic covalent organic chemistry approaches, they can be seen as ideal platforms to simultaneously incorporate different switchable units into a given 2D skeleton exhibiting a precise and robust structure. In this framework, the making of multi-responsive semiconducting 2D COFs represents a grand challenge, which can offer major technological advancement for the next generation of electronic devices. In the MS2DCOFO project, we have synthesized a novel photo-switchable 2D COF, and also developed unique methodology to synthesize 2D COF films with smooth bottom surface, which can be coated on MoS2 to achieve heterostructure-based semiconductors. The newly developed nanotechnology offers an alternative approach for fabricating multi-switchable semiconducting devices. The overall objectives of this project were to incorporate different stimuli responsive organic building blocks into highly crystalline 2D COFs, and further integrate the 2D COF films into semiconducting devices for complex logic operations. In summary, the MS2DCOFO project provides a guideline to design and synthesize photo-switchable 2D COFs, offers a new methodology for the fabrication of 2D COF-based semiconducting devices, and achieved 2D COF-based multi-responsive semiconductors for the first time. These new findings have the potential to bring technology revolution in the materials and electronic industry.
