Orthogonal Lithography for Halide Perovskite Optoelectronic Nanodevices

3D organic–inorganic hybrid halide perovskites have attracted great interest due to their impressive optoelectronic properties. Recently, the emergence of 2D layered hybrid perovskites, with their excellent and tunable optoelectronic behavior, has encouraged researchers to develop the next generation of optoelectronics based on these 2D materials. However, device fabrication methods of scalable patterning on both types of hybrid perovskites are still lacking as these materials are readily damaged by the organic solvents in standard lithographic processes. We conceived the orthogonal processing and patterning method: Chlorobenzene and hexane, which are orthogonal to hybrid perovskites, are utilized in modified electron beam lithography (EBL) processes to fabricate perovskite-based devices without compromising their electronic or optical characteristics. As a proof-of-concept, we used the orthogonal EBL technique to fabricate a 2D layered single-crystal (C₆H₅C₂H₄NH₃)₂PbI₄ photodetector featuring nanoscale patterned electrodes and superior photodetection ability with responsivity of 5.4 mA/W and detectivity of 1.07 × 10¹³ cm Hz^1/2/W. Such orthogonal processing and patterning methods are believed to fully enable the high-resolution, high-throughput fabrication of complex perovskite-based electronics in the near future.