The development of large-area high-performance flexible photoelectronic synaptic devices has become a hot topic in the field of neuromorphic computing and artificial vision systems. In this work, we have successfully prepared a large-area, ultra-flexible semiconducting single-walled carbon nanotubes (sc-SWCNTs) photoelectronic synaptic thin-film transistors (TFTs) array (33×34) using solution-processable AlO_X thin film as the dielectrics by roll-to-roll gravure printing. Our photoelectronic synaptic TFTs exhibit excellent electrical properties with high switching ratio (≥10⁵), low subthreshold swing (73 mV dec^-1), excellent photoresponse properties over a wide wavelength range (from 270 nm to 650 nm), sustained photoconductivity effect (only 26.7% drop after removing light source for 36000 s) and remarkable mechanical reliability and flexibility (maintaining excellent electrical properties after bending more than 15000 cycles with a bending radius of 5 mm). In addition, concepts such as multimodal optoelectronic synaptic plasticity, optical writing speed perception simulation, and human eye self-recovery model have been successfully demonstrated using printed flexible sc-SWCNTs photoelectronic neuromorphic TFTs arrays. More importantly, we systematically investigated the response characteristics of these devices under deep ultraviolet light stimulation and, for the first time, successfully simulated bio-inspired visual perception self-recovery including the dynamic transition of the visual system from clarity to blurriness and their self-recovery over time. This work indicates that our photoelectronic neuromorphic TFT devices have great practical potential in human-computer interaction, environment perception, and visual simulation.

Monochiral single-walled carbon nanotubes (SWCNTs) can enable high-performance carbon-based electronic devices and integrated circuits. However, their fabrication often requires complex SWCNT purification and enrichment. Herein, we showed that isoindigo-based polymer derivatives (PDPPIID and PFIID) directly enriched (9,8) nanotubes from as-synthesized SWCNT powders selectively and efficiently to yield high concentration (9,8) nanotube inks. The selective wrapping mechanism was elucidated by classical full-atomistic molecular dynamic (MD) simulations. Thin-film transistors (TFTs) were fabricated by depositing the SWCNT ink into device channels using aerosol jet printing. TFT performance was strongly influenced by polymer residues, the deposition condition (humidity), and ink concentration. Optimized TFTs showed excellent device-to-device uniformity with 10⁸ on/off ratios. Further, optoelectronic transistors were fabricated, and their photoelectrical neuromorphic characteristics, storage, memory, and logic functions were characterized under the pulsed light and voltage stimulations, demonstrating excellent application potentials.