Halide perovskite ferroelectrics endowed with a distinctive spontaneous polarization effect have been regarded as prospective electroactive materials and are prevalently utilized in solar cells, photoelectric detection, and other domains. Among them, multipolar-axis ferroelectrics featuring multiple equivalent polarization directions are particularly desirable for diverse areas of applications. Nevertheless, the design and regulation of multipolar axis perovskite ferroelectrics remains a significant challenge. Here, guided by the strategy of layer regulation, we successfully designed and regulated a series of 2D homologous perovskites OA2Csn-1PbnBr3n+1 (OA = n-octylammonium, n = 1-3). Notably, OA2Csn-1PbnBr3n+1 exhibits layer-dependent ferroelectricity: OA2PbBr4 exhibits non-ferroelectricity, OA2CsPb2Br7 displays uniaxial ferroelectricity, while OA2Cs2Pb3Br10 with multiaxial ferroelectricity. Moreover, the devices fabricated based on OA2Cs2Pb3Br10 achieve high-performance self-driven photodetection in multiple directions. This precise layer-regulation strategy offers an efficient approach to obtaining and regulating multipolar-axis perovskite ferroelectrics, presenting the potential for next-generation optoelectronic devices.
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