Wafer-Scale Patterning Integration of Chiral 3D Perovskite Single Crystals toward High-Performance Full-Stokes Polarimeter

Wafer-Scale Patterning Integration of Chiral 3D Perovskite Single Crystals toward High-Performance Full-Stokes Polarimeter Junli Bai,∇Hebin Wang,∇Jianpeng Ma, Yingjie Zhao,* Haolin Lu, Yunxin Zhang, Sehrish Gull, Tianjiao Qiao, Wei Qin, Yongsheng Chen, Lei Jiang, Guankui Long,* and Yuchen Wu* Cite This: J. Am. Chem. Soc. 2024, 146, 18771−18780 Read Online ACCESS Metrics & More Article Recommendations * sı Supporting Information ABSTRACT: Chiral three-dimensional (3D) perovskites exhibit exceptional optoelectronic characteristics and inherent chiroptical activity, which may overcome the limitations of low-dimensional chiral optoelectronic devices and achieve superior performance. The integrated chip of high-performance arbitrary polarized light detection is one of the aims of chiral optoelectronic devices and may be achieved by chiral 3D perovskites. Herein, we first fabricate the wafer-scale integrated full-Stokes polarimeter by the synergy of unprecedented chiral 3D perovskites (R/S-PyEA)Pb2Br6 and one- step capillary-bridge assembly technology. Compared with the chiral low-dimensional perovskites, chiral 3D perovskites present smaller exciton binding energies of 57.3 meV and excellent circular dichroism (CD) absorption properties, yielding excellent circularly polarized light (CPL) photodetectors with an ultrahigh responsivity of 86.7 A W−1, an unprecedented detectivity exceeding 4.84 × 1013 Jones, a high anisotropy factor of 0.42, and high-fidelity CPL imaging with 256 pixels. Moreover, the anisotropic crystal structure also enables chiral 3D perovskites to have a large linear-polarization response with a polarized ratio of 1.52. The combination of linear-polarization and circular-polarization discrimination capabilities guarantees the achievement of a full-Stokes polarimeter. Our study provides new research insights for the large-scale patterning wafer integration of high-performance chiroptical devices. ■INTRODUCTION Hybrid organic−inorganic metal halide perovskites gain substantial attention due to the large absorption coefficients, tunable band gaps, high carrier mobility, long carrier diffusion lengths, and low-cost solution processing, which greatly accelerate the development of solar cells,1−3 light-emitting diodes,4−6 photodetectors,7−9 and lasers.10−12 In particular, the construction of chiral perovskites yields numerous exotic properties, including circular dichroism (CD),13,14 nonlinear chiroptical properties,15,16 ferroelectricity,17,18 and chirality- induced spin selectivity (CISS) effect,19,20 which significantly broadens the applications of perovskites in various fields including circularly polarized light (CPL) photodetectors,21,22 nonlinear optics,23 memories,24 and spin-LEDs.25 The current fabrication of chiral perovskite optoelectronic devices is usually based on the chiral low-dimensional perovskite materials, such as (R/S-α-PEA)PbI3,26 (R/S-α-PEA)2PbI4,27 (R/S-β- MPA)2MAPb2I7,28 and (R/S-BPEA)2PbI4.29 These devices expose some intrinsic limitations, such as poor charge carrier mobility, low responsivity, and small anisotropy factor. The manufacturing of chiral three-dimensional (3D) perovskites represents a promising approach to address these limitations and achieve superior performance in chiral optoelectronic devices, but the incorporation of large chiral cations typically breaks down the structure of chiral 3D perovskite due to an undesirable structure tolerance factor.30,31 Furthermore, thermodynamically stabilized chiral 3D perovskites have been predicted by theoretical calculations, but they have not been explored experimentally.32 Therefore, it is absolutely necessary to design appropriate A-site chiral cations, which will be helpful in composing stable chiral 3D perovskites for the advancement of chiral optoelectronic devices. The performance of perovskite devices greatly relies on the crystallization quality and orientation of the perovskite crystals along with optoelectronic features such as c