<br>利用带有极性有机阳离子的 2D Ruddlesden-Popper 钙钛矿用于超灵敏多位非易失性晶体管型光忆阻器,ACS Nano

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利用带有极性有机阳离子的 2D Ruddlesden-Popper 钙钛矿用于超灵敏多位非易失性晶体管型光忆阻器
ACS Nano ( IF 15.8 ) Pub Date : 2023-12-14 , DOI: 10.1021/acsnano.3c09595
Po-Ting Lai, Cheng-Yueh Chen, Hao-Cheng Lin, Bo-Yuan Chuang, Kai-Hua Kuo, Christopher R. Greve, Tsung-Kai Su, Guang-Hsun Tan, Chia-Feng Li, Sheng-Wen Huang, Kai-Yuan Hsiao, Eva M. Herzig, Ming-Yen Lu, Yu-Ching Huang, Ken-Tsung Wong, Hao-Wu Lin

由于其快速数据传输和低功耗的潜力，光忆阻器被认为是下一代基于硬件的神经拟态计算最有前途的候选者之一。然而有趣的是，到目前为止，光忆阻器很少表现出真正具有高光敏感性的非易失性存储特性。在此，我们展示了利用二维（2D）Ruddlesden-Popper（RP）钙钛矿和高极性供体-受体型推拉有机阳离子4-（5-（2-氨基乙基）噻吩-2-基）的超灵敏光忆阻器)苯甲腈⁺ (EATPCN ⁺ )，作为电荷俘获层。在(EATPCN) ₂ PbI ₄器件中观察到高线性度和几乎零衰减的保留，这与由非极性有机阳离子组成的传统2D RP钙钛矿器件非常不同，例如苯乙胺⁺ (PEA ⁺ ) 和辛胺⁺ ( OA ⁺ )，以及由甲胺⁺ (MA ⁺ ) 组成的传统 3D 钙钛矿器件。双重优势，包括理想的空间晶体排列和工程能带排列，阐明了 (EATPCN) ₂ PbI ₄器件卓越性能的机制。优化的 (EATPCN) ₂ PbI ₄光忆阻器还显示出 87.9 V 的存储窗口和 10 ⁶的开/关比，保留时间至少为 2.4 × 10 ⁵ s，并且在 >10 ⁵写入-读取-擦除后保持不变–阅读耐力周期。光刺激和每次状态更新的读取过程的能耗也非常低，分别为 1.12 和 6 fJ。同时实现了极低的功耗和高光响应性。高光敏度超过最先进的商用脉冲能量计几个数量级。凭借出色的线性度和保留能力，兔子图像由 (EATPCN) ₂ PbI ₄光忆阻器重建，真实地呈现图像，不会随着时间的推移而褪色。最后，利用(EATPCN) ₂ PbI ₄光忆阻器强大的~8位非易失性增强和抑制水平，CIFAR-10图像分类和MNIST手写数字分类的识别任务准确率分别达到89%和94.8% 。这项研究首次报告了利用 2D RP 钙钛矿中的功能性供体-受体型有机阳离子来制备高性能光忆阻器，其特性在当前卤化物钙钛矿中不存在。

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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)₂PbI₄ 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)₂PbI₄ devices. The optimized (EATPCN)₂PbI₄ photomemristor also shows a memory window of 87.9 V and an on/off ratio of 10⁶ with a retention time of at least 2.4 × 10⁵ s and remains unchanged after >10⁵ 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)₂PbI₄ 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)₂PbI₄ 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.

更新日期：2023-12-14

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