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Zinc (Zn) has arisen as a significant suppressor of vacancy formation in halide perovskites, establishing its pivotal role in defect engineering for these materials. Herein, the Zn‐catalyzed vapor‐liquid‐solid (VLS) route is reported to render black‐phase CsPbI3 nanowires (NWs) operationally stable at room temperature. Based on first‐principle calculations, the doped Zn2+ can not only lead to the partial crystal lattice distortion but also reduce the formation energy (absolute value) from the black phase to the yellow phase, improving the stability of the desired black‐phase CsPbI3 NWs. A series of contrast tests further confirm the stabilization effect of the Zn‐doped strategy. Besides, the polarization‐sensitive characteristics of black‐phase CsPbI3 NWs are revealed. This work highlights the importance of phase stabilization engineering for CsPbI3 NWs and their potential applications in anisotropic optoelectronics. [ABSTRACT FROM AUTHOR]

The surface of low‐dimensional perovskites play a crucial role in determining their intrinsic property. Understanding their characteristics and the influence of certain surfaces is valuable in designing functional surface‐engineered structures. Meanwhile, surface passivation can also be applied to stabilize and optimize the state‐of‐the‐art perovskite‐based optoelectronics. Herein, cesium lead bromide (CsPbBr3) microwire parallel arrays are designed and fabricated with specific (100)‐terminated crystal planes, which exhibit excellent photodetection performance with long‐term environment stability >3000 h. Notably, it is uncovered experimentally and theoretically that environmental oxygen can not only passivate the Br‐vacancy‐related trap states on the (100) surface, but also create charge carrier nanochannels to enhance the (opto)electronic properties. The coupling effects between oxygen species and the specific terminated crystal planes of perovskites highlight the importance of surface engineering for designing and optimizing perovskite‐based devices. [ABSTRACT FROM AUTHOR]