Liu Xiaolong, Wang Kang, Zhang Tongjin, Liu Haidi, Ren Ang, Ren Shizhe, Li Penghao, Zhang Chuang, Yao Jiannian, Zhao Yong Sheng
Key Laboratory of Photochemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China.
Adv Mater. 2023 Dec;35(52):e2305260. doi: 10.1002/adma.202305260. Epub 2023 Nov 20.
Spin-polarized lasers, arising from stimulated emission of imbalanced spin populations, play a vital role in spin-optoelectronics. It is usually tackled by external spin injection, inevitably suffering from additional losses across the barriers from injection sources to gain materials. Herein, spin-polarized coherent light emission is self-triggered from the 1D-anchoring-3D perovskites, where the imbalanced populations in achiral 3D perovskites are endowed with the spin selectivity of exciton chirality (EC) underpinned by chiral 1D perovskites. Efficient transfer of EC is enabled by rapid energy transfer, thereby creating an imbalance of the spin population of excited states. Stimulated emission of such populations brings self-triggered spin-polarized amplified spontaneous emission in the composite perovskites, yielding a higher degree of polarization (DOP) than that based on optical spin injection into bare achiral 3D perovskites. Chemical diversity of composite perovskites not only enables to adjust band gap for broadband output of spin-polarized light signals but also promises to manipulate radiative decay and spin relaxation toward remarkably increased DOP. These results highlight the importance of EC transfer mechanism for spin-polarized lasing and represent a crucial step toward the development of chiral-spintronics.
自旋极化激光器源于不平衡自旋态的受激发射，在自旋光电子学中起着至关重要的作用。它通常通过外部自旋注入来解决，不可避免地会在从注入源到增益材料的势垒处遭受额外的损耗。在此，自旋极化相干光发射是由一维锚定三维钙钛矿自触发的，其中非手性三维钙钛矿中的不平衡态被赋予了由手性一维钙钛矿支撑的激子手性（EC）的自旋选择性。快速的能量转移实现了EC的有效转移，从而造成激发态自旋态的不平衡。这种态的受激发射在复合钙钛矿中产生了自触发的自旋极化放大自发发射，产生的偏振度（DOP）高于基于向裸非手性三维钙钛矿中进行光自旋注入所产生的偏振度。复合钙钛矿的化学多样性不仅能够调整带隙以实现自旋极化光信号的宽带输出，还有望控制辐射衰减和自旋弛豫，从而显著提高DOP。这些结果突出了EC转移机制对自旋极化激光的重要性，并代表了手性自旋电子学发展的关键一步。
