Highly Strained Polymeric Monolayer Stacked for Wafer-Scale and Transferable Nanodielectrics

As the keystones of molecular electronics, high-quality nanodielectric layers are challenging to assemble due to the strictest criteria for their reliability and uniformity over a large area. Here, we report a strained poly(4-vinylphenol) monolayer, ready to be stacked to form defect-free wafer-scale nanodielectrics. The thickness of the nanodielectrics can be precisely adjusted in integral multiples of the 1.2 nm thick PVP monolayer. By employing a double cross-linking strategy, an exceptional dielectric performance is achieved with a leakage current of 10^-7-10^-8 A/cm² at 2 MV/cm across the low-<i>k</i> PVP layers as thin as 3.6 nm. Furthermore, the obtained nanodielectric layers could be laminated onto various substrates on demand via polydimethylsiloxane soft stamps, enabling its application in organic field-effect transistors of both bottom-gate and top-gate configurations. This work represents a pivotal development in (opto-)electronic molecular materials and heralds an emerging avenue for the exploration of functional nanodielectrics in the field of nanoelectronics.