Li Penghao, Zhou Zhonghao, Ran Guangliu, Zhang Tongjin, Jiang Zhengjun, Liu Haidi, Zhang Wenkai, Yan Yongli, Yao Jiannian, Dong Haiyun, Zhao Yong Sheng
Key Laboratory of Photochemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China.
School of Chemical Science, University of Chinese Academy of Sciences, Beijing, China.
Nat Commun. 2024 Dec 30;15(1):10880. doi: 10.1038/s41467-024-55234-6.
Spin-polarized lasers have demonstrated many superiorities over conventional lasers in both performance and functionalities. Hybrid organic-inorganic perovskites are emerging spintronic materials with great potential for advancing spin-polarized laser technology. However, the rapid carrier spin relaxation process in hybrid perovskites presents a major bottleneck for spin-polarized lasing. Here we report the identification and successful suppression of the spin relaxation mechanism in perovskites for the experimental realization of spin-polarized perovskite lasers. The electron-hole exchange interaction is identified as the decisive spin relaxation mechanism hindering the realization of spin-polarized lasing in perovskite microcrystals. An ion doping strategy is employed accordingly to introduce a new energy level in perovskites, which enables a long carrier spin lifetime by suppressing the electron-hole exchange interaction. As a result, spin-polarized lasing is achieved in the doped perovskite microcrystals. Moreover, the doped cation is a magnetic species allowing for the magnetic field control of the spin-polarized perovskite lasing. This work unlocks the potential of perovskites for spin-polarized lasers, providing guidance for the design of perovskites towards spintronic devices.
自旋极化激光器在性能和功能方面已展现出许多优于传统激光器的优势。有机-无机杂化钙钛矿是新兴的自旋电子材料,在推动自旋极化激光技术发展方面具有巨大潜力。然而,杂化钙钛矿中快速的载流子自旋弛豫过程是自旋极化激光发射的一个主要瓶颈。在此,我们报告了对钙钛矿中自旋弛豫机制的识别和成功抑制,以实现自旋极化钙钛矿激光器的实验。电子-空穴交换相互作用被确定为阻碍钙钛矿微晶中自旋极化激光发射实现的决定性自旋弛豫机制。相应地采用离子掺杂策略在钙钛矿中引入新的能级,通过抑制电子-空穴交换相互作用实现长的载流子自旋寿命。结果,在掺杂的钙钛矿微晶中实现了自旋极化激光发射。此外,掺杂阳离子是一种磁性物质,可实现对自旋极化钙钛矿激光发射的磁场控制。这项工作开启了钙钛矿用于自旋极化激光器的潜力,为面向自旋电子器件的钙钛矿设计提供了指导。