Chen Weilin, Chen An, Liu Xue, Shu Fan, Zeng Jianmin, Zhang Jinying, Xu Hongbo, Peng Gaoliang, Yang Zhi, Li Jinjin, Liu Gang
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai, 200240, China.
QIANYUAN National Laboratory, Hangzhou, 310024, China.
Adv Mater. 2024 Nov;36(46):e2410097. doi: 10.1002/adma.202410097. Epub 2024 Sep 27.
Manipulating the properties of 2D materials through meticulously engineered artificial heterojunctions holds great promise for novel device applications. However, existing research on the crucial charge-transfer interactions and energy profile regulation is predominantly focused on 2D van der Waals structures formed via weak van der Waals forces, limiting regulatory efficiency at high costs. Herein, a refined atomic-molecular heterojunction strategy featuring strong covalent bonds between organic molecule and 2D violet phosphorus (VP) atomic crystal is developed, which enables enhanced charge-transfer dynamics and customizable band structure regulation at the molecular level. Both experimentally and theoretically, it is demonstrated that grafting efficiency, charge redistribution, and energy gap regulation critically depend on organic electronegativity, providing a low-cost yet high-efficiency regulatory effect on a large scale. As a proof of concept, the novel VP-molecular heterojunctions exhibit optimized performance in diverse application domains, presenting a general platform for future high-performance device applications.
通过精心设计的人工异质结来调控二维材料的性质，对于新型器件应用具有巨大潜力。然而，现有的关于关键电荷转移相互作用和能量分布调控的研究主要集中在通过弱范德华力形成的二维范德华结构上，这限制了调控效率且成本高昂。在此，开发了一种精细的原子 - 分子异质结策略，其特点是有机分子与二维紫磷（VP）原子晶体之间形成强共价键，这能够在分子水平上增强电荷转移动力学并实现可定制的能带结构调控。实验和理论均表明，接枝效率、电荷重新分布和能隙调控关键取决于有机电负性，从而在大规模上提供了低成本但高效的调控效果。作为概念验证，新型VP - 分子异质结在不同应用领域展现出优化性能，为未来高性能器件应用提供了一个通用平台。
