Highly Strained\nPolymeric Monolayer Stacked for Wafer-Scale\nand Transferable Nanodielectrics

As the keystones of molecular electronics,\nhigh-quality\nnanodielectric\nlayers are challenging to assemble due to the strictest criteria for\ntheir reliability and uniformity over a large area. Here, we report\na strained poly(4-vinylphenol) monolayer, ready to be stacked to form\ndefect-free wafer-scale nanodielectrics. The thickness of the nanodielectrics\ncan be precisely adjusted in integral multiples of the 1.2 nm thick\nPVP monolayer. By employing a double cross-linking strategy, an exceptional\ndielectric performance is achieved with a leakage current of 10<sup>–7</sup>–10<sup>–8</sup> A/cm<sup>2</sup> at\n2 MV/cm across the low-<i>k</i> PVP layers as thin as 3.6\nnm. Furthermore, the obtained nanodielectric layers could be laminated\nonto various substrates on demand via polydimethylsiloxane soft stamps,\nenabling its application in organic field-effect transistors of both\nbottom-gate and top-gate configurations. This work represents a pivotal\ndevelopment in (opto-)electronic molecular materials and heralds an\nemerging avenue for the exploration of functional nanodielectrics\nin the field of nanoelectronics.