Silk Flexible Electronics: From Bombyx mori Silk Ag Nanoclusters Hybrid Materials to Mesoscopic Memristors and Synaptic Emulators

Functionalization of flexible materials based on mesoscopic reconstruction is a key strategy in fabricating biocompatible flexible electronics. This work is to acquire new mesoscopic bioelectronic hybrid materials of silk fibroin (SF)‐Ag nanoclusters (AgNCs@BSA; BSA: bovine serum albumin), which enhance significantly the performance of silk memristors. It is to build AgNCs@BSA into SF mesoscopic networks by templated β‐crystallization. Atomic force microscopy potential probing indicates that AgNCs@BSA serve as electronic potential wells that change completely the transport behavior of charge particles within the SF films. This leads to significant enhancement in the switching speed (≈10 ns), very good switching stability, extremely low set/reset voltages (0.3/−0.18 V) of SF meso‐hybrid memristors, compared with the original and other organic memristors, and displays unique synapse characteristics and the capability of synapse learning. Classical density functional theory Poisson–Nernst–Planck simulations indicate that the enhanced performance is subject to the low potential paths interconnecting the AgNCs@BSA, which guide charges' transport (Ag+) and deposition in SF films. A completely new materials engineering strategy, functionalized templated mesoscopic reconstruction, is introduced. The designed silk meso‐functional materials display significantly enhanced performance and gives rise to a new class of silk electronics (memristors and synaptic emulators). This progress represents a breakthrough in flexible materials and flexible electronics.