Harnessing 2D Ruddlesden–Popper Perovskite with Polar Organic Cation for Ultrasensitive Multibit Nonvolatile Transistor-Type Photomemristors

Photomemristors have been regarded as one of the most promising candidates for next-generation hardware-based neuromorphic computing due to their potentials of fast data transmission and low power consumption. However, intriguingly, so far, photomemristors seldom display truly nonvolatile memory characteristics with high light sensitivity. Herein, we demonstrate ultrasensitive photomemristors utilizing two-dimensional (2D) Ruddlesden–Popper (RP) perovskites with a highly polar donor–acceptor-type push–pull organic cation, 4-(5-(2-aminoethyl)thiophen-2-yl)benzonitrile + (EATPCN + ), as charge-trapping layers. High linearity and almost zero-decay retention are observed in (EATPCN) 2 PbI 4 devices, which are very distinct from that of the traditional 2D RP perovskite devices consisting of nonpolar organic cations, such as phenethylamine + (PEA + ) and octylamine + (OA + ), and traditional 3D perovskite devices consisting of methylamine + (MA + ). The 2-fold advantages, including desirable spatial crystal arrangement and engineered energetic band alignment, clarify the mechanism of superior performance in (EATPCN) 2 PbI 4 devices. The optimized (EATPCN) 2 PbI 4 photomemristor also shows a memory window of 87.9 V and an on/off ratio of 10 6 with a retention time of at least 2.4 × 10 5 s and remains unchanged after >10 5 writing–reading–erasing–reading endurance cycles. Very low energy consumptions of 1.12 and 6 fJ for both light stimulation and the reading process of each status update are also demonstrated. The extremely low power consumption and high photoresponsivity were simultaneously achieved. The high photosensitivity surpasses that of a state-of-the-art commercial pulse energy meter by several orders of magnitude. With their outstanding linearity and retention, rabbit images have been rebuilt by (EATPCN) 2 PbI 4 photomemristors, which truthfully render the image without fading over time. Finally, by utilizing the powerful ∼8 bits of nonvolatile potentiation and depression levels of (EATPCN) 2 PbI 4 photomemristors, the accuracies of the recognition tasks of CIFAR-10 image classification and MNIST handwritten digit classification have reached 89% and 94.8%, respectively. This study represents the first report of utilizing a functional donor–acceptor type of organic cation in 2D RP perovskites for high-performance photomemristors with characteristics that are not found in current halide perovskites.