Hong Huilong, Guo Songhao, Jin Leyang, Mao Yuhong, Chen Yuguang, Gu Jiazhen, Chen Shaochuang, Huang Xu, Guan Yan, Li Xiaotong, Li Yan, Lü Xujie, Fu Yongping
Beijing National Laboratory for Molecular Science, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China.
Center for High Pressure Science and Technology Advanced Research, Shanghai, 201203, China.
Nat Commun. 2024 Apr 11;15(1):3164. doi: 10.1038/s41467-024-47406-1.
Two-dimensional organic-inorganic hybrid halide perovskites possess diverse structural polymorphs with versatile physical properties, which can be controlled by order-disorder transition of the spacer cation, making them attractive for constructing semiconductor homojunctions. Here, we demonstrate a space-cation-dopant-induced phase stabilization approach to creating a lateral homojunction composed of ordered and disordered phases within a two-dimensional perovskite. By doping a small quantity of pentylammonium into (butylammonium)PbI or vice versa, we effectively suppress the ordering transition of the spacer cation and the associated out-of-plane octahedral tilting in the inorganic framework, resulting in phase pining of the disordered phase when decreasing temperature or increasing pressure. This enables epitaxial growth of a two-dimensional perovskite homojunction with tunable optical properties under temperature and pressure stimuli, as well as directional exciton diffusion across the interface. Our results demonstrate a previously unexplored strategy for constructing two-dimensional perovskite heterostructures by thermodynamic tuning and spacer cation doping.
二维有机-无机杂化卤化物钙钛矿具有多种结构多晶型物,具备多样的物理性质,这些性质可通过间隔阳离子的有序-无序转变来控制,这使得它们在构建半导体同质结方面具有吸引力。在此,我们展示了一种空间阳离子掺杂诱导的相稳定方法,用于在二维钙钛矿中创建由有序相和无序相组成的横向同质结。通过将少量戊基铵掺杂到(丁基铵)PbI中,反之亦然,我们有效地抑制了间隔阳离子的有序转变以及无机框架中相关的面外八面体倾斜,导致在温度降低或压力增加时无序相的相钉扎。这使得二维钙钛矿同质结能够在温度和压力刺激下实现具有可调光学性质的外延生长,以及激子跨界面的定向扩散。我们的结果展示了一种通过热力学调控和间隔阳离子掺杂构建二维钙钛矿异质结构的前所未有的策略。