Herein, it is reported the influence of solution processing and treatments, such as adding marginal solvent, ultrasonication, and UV treatment, on the resulting perovskite (CsPbBr3) quantum dot (QD)/poly(3‐hexylthiophene) (P3HT) composite nanofibril films (CNFs) to improve the charge dissociation and photonic synaptic performance. A photonic synaptic transistor with CNFs can perform fundamental functions, including short‐term plasticity, long‐term plasticity, spike‐number‐dependent, and spike‐time‐dependent plasticity, to mimic sensing, computing, and memory functions. Notably, a synaptic device with CNFs presents an ultralow energy consumption of 0.18 fJ and zero‐gate operation. The superior performance of synaptic devices with CNFs can be attributed to two factors: (i) homogeneous axial distribution of the QDs and (ii) the formation of P3HT nanofibrils and co‐aggregates. Therefore, enhanced interfacial charge transfer between QDs and P3HT, ensuring decent carrier transport capability, is achieved. Collectively, the composite artificial synapse successfully provides an effective guide that offers a new perspective for the fabrication of one‐dimensional self‐assembled nanostructure‐based artificial synapses emulating human‐like memory, neuromorphic computing, and artificial intelligent systems.

Neuromorphic computation possesses the advantages of self-learning, highly parallel computation, and low energy consumption, and is of great promise to overcome the bottleneck of von Neumann computation. In this work, a series of poly(3-hexylthiophene) (P3HT)-based block copolymers (BCPs) with different coil segments, including polystyrene, poly(2-vinylpyridine) (P2VP), poly(2-vinylnaphthalene), and poly(butyl acrylate), are utilized in photosynaptic transistor to emulate paired-pulse facilitation, spike time/rate-dependent plasticity, short/long-term neuroplasticity, and learning−forgetting−relearning processes. P3HT serves as a carrier transport channel and a photogate, while the insulating coils with electrophilic groups are for charge trapping and preservation. Three main factors are unveiled to govern the properties of these P3HT-based BCPs: i) rigidity of the insulating coil, ii) energy levels between the constituent polymers, and iii) electrophilicity of the insulating coil. Accordingly, P3HT-b-P2VP-based photosynaptic transistor with a sought-after BCP combination demonstrates long-term memory behavior with current contrast up to 10 5 , short-term memory behavior with high paired-pulse facilitation ratio of 1.38, and an ultralow energy consumption of 0.56 fJ at an operating voltage of −0.0003 V. As far as it is known, this is the first work to utilize conjugated BCPs in an electret-free photosynaptic transistor showing great potential to the artificial intelligence technology.

We report the synthesis, morphology and photo-memory device applications of a block copolymer (BCP) consisting of poly(9,9-dioctylfluorene) (PFO) and polystyrene (PS).

To date, few studies of the mobility–stretchability properties of N-type semiconductors, including naphthalenediimide (NDI)-based polymers, have been conducted, and the preparation of intrinsically stretchable N-type semiconducting polymers is very important in the construction of stretchable electronics. In this study, three NDI-based random terpolymers are synthesized by introducing functionalized conjugation break spacers (CBSs) with ester, sulfone, and amide groups. N-type semiconducting polymers with ester and amide-based CBSs undergo conformational reorganization during stretching, as evidenced by the progressive evolution of mixed edge-on and face-on orientations, as well as the increased UV–vis dichroic ratio. This phenomenon is attributed to the improved chain conformability and ductility from the randomized distribution of the CBSs along the polymer backbone with more planar CBSs. Therefore, polymers with ester-based CBSs achieve superior orthogonal electron mobility (μe) >0.005 cm2 V–1 s–1 and an average μe retention of 61% after 400 cyclic stretching at 60% strain. To the best of our knowledge, this study is the first to decipher the mobility–stretchability properties of N-type semiconducting polymers that warrant further investigation for constructing intrinsically stretchable and wearable electronics.

The mechanical properties and structural design flexibility of charge-trapping polymer electrets has led to their widespread use in organic field-effect transistor (OFET) memories. For example, in the electrets of polyfluorene-based conjugated/insulating block copolymers (BCPs), the confined fiber-like polyfluorene nanostructures in the insulating polymer matrix act as effective hole-trapping sites, leading to controllable memory performance through the design of BCP. However, few studies have reported intrinsically stretchable charge-trapping materials and their memory device applications, and a practical method to correlate thin film morphology of BCP electrets with their charge-trapping ability has not yet been developed. In this study, a series of new conjugated/insulating BCPs, poly(9,9-di-n-hexyl-2,7-fluorene)-block-poly(δdecanolactone)s (PF-b-PDLx, x = 1-3) as stretchable hole-trapping materials are reported. The linear and branched PDL blocks with the comparable molecular weight were used to investigate the effect of polymer architecture on morphology and device performance. Moreover, coverage area of the polyfluorene nanofibers on the BCP films was extracted from atomic force microscopy images, which can be correlated with the trapping density of the polymer electrets. The branched PDL segments not only improve stretchability but also tailor crystallinity and phase separation of the BCPs, thus increasing their charge-trapping ability. The OFET memory device with PF-b-PDL3 as electret layer exhibited the largest memory window (102 V), and could retain its performance at up to 100% strain. This research highlights the importance of BCP design for developing stretchable charge-trapping materials.