Cross-Scale Synthesis of Organic High-k Semiconductors Based on Spiro-Gridized Nanopolymers

High dielectric constants in organic semiconductors have been identified as a central challenge for the improvement in not only piexoelectric,preolecric,and freeltric efcts but also photoclecric conversion eficiency in OPVs,carrier mobility in OFETS,and charge density in charge-trapping memories.Herein,we report an ultralong persistence length(≈41 nm)efet of spiro-fused organic nanopolymers on dielectric properties,together with excitonic and charge carrier behaviors.The state-of-the-art nanopolymers,namely,nanopolyspirogrids(NPSGs),are synthesized via the simple crossscale Friedel-Crafts polygridlization of AjB-type nanomonomers.The high dielectric constant(k=8.43)of NPSG is firstly achieved by locking spiro-polygridization efect that results in the enhancement of dipole polarization.When doping into a polystyrene-based dielectric layer,such a high-k feature of NPSG increases the feld-ffct carrier mobility from 0.20 to 0.90cm^(2)Vl s'in pentacene OFET devices.Meanwhile,amorphous NPSG film exhibits an ultralow energy disorder(<50 meV)for an exellent zero-field hole mobility of 3.94×10^(-1)cm^(2)V^(-1)s^(-1).surpassing most of the amorphousπconjugated polymers Onganic nanopolymers with high dielectric constants open a new way to break through the bottleneck of eficiency and multifunctionality in the blueprint of the fourth generation semiconductors.