High‐Performance Photodetector and Angular‐Dependent Random Lasing from Long‐Chain Organic Diammonium Sandwiched 2D Hybrid Perovskite Non‐Linear Optical Single Crystal

Three-dimensional organic-inorganic metal halide perovskites are excellent materials for optoelectronic applications due to their exceptional properties, solution processability, and cost-effectiveness. However, the lack of environmental stability highly restricts them from practical applications. Herein, the authors report a stable centimeter-long two-dimensional (2D) hybrid perovskite (N-MPDA)[PbBr4] single crystal using divalent N1-methylpropane1,3-diammonium (N-MPDA) cation as an organic spacer. The as-grown single crystal exhibits stable optoelectronic performance, low threshold random lasing, and multi-photon luminescence/multi-harmonic generation. A photoconductive device fabricated using (NMPDA)[PbBr4] single crystal exhibits an excellent photoresponsivity (≈124 AW-1 at 405 nm) that is ≈4 orders of magnitudes higher than that of monovalent organic spacer-assisted 2D perovskites, such as (BA)2PbBr4 and (PEA)2PbBr4, and large specific detectivity (≈1012 Jones). As an optical gain media, the (N-MPDA)[PbBr4] single crystal exhibits a low threshold random lasing (≈6.5 µJcm-2 ) with angular dependent narrow linewidth (≈0.1 nm) and high-quality factor (Q≈2673). Based on our results, the outstanding optoelectronic merits of (N-MPDA)[PbBr4] single crystal will offer a high-performance device and act as a dynamic material to construct stable future electronics and optoelectronic-based applications.