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

• Published in: Advanced functional materials Vol. 33; no. 17
• Main Authors: Ulaganathan, Rajesh Kumar, Roy, Pradip Kumar, Mhatre, Swapnil Milind, Murugesan, Raghavan Chinnambedu, Chen, Wei‐Liang, Lai, Man‐Hong, Subramanian, Ambika, Lin, Chang‐Yu, Chang, Yu‐Ming, Canulescu, Stela, Rozhin, Alex, Liang, Chi‐Te, Sankar, Raman
• Format: Journal Article
• Language: English
• Published: Hoboken Wiley Subscription Services, Inc 01.04.2023
• Subjects: Crystal growth; Harmonic generations; Lasing; long‐chain spacers; Materials science; Metal halides; Optoelectronics; Perovskites; random lasing; responsivity; second‐harmonic generation; Single crystals
• ISSN: 1616-301X; 1616-3028
• DOI: 10.1002/adfm.202214078

3D 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, a stable centimeter‐long 2D hybrid perovskite (N‐MPDA)[PbBr4] single crystal using divalent N1‐methylpropane‐1,3‐diammonium (N‐MPDA) cation as an organic spacer, is reported. 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 (N‐MPDA)[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 µJ cm−2) with angular dependent narrow linewidth (≈0.1 nm) and high‐quality factor (Q ≈ 2673). Based on these 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. Asymmetric diammonium di‐cation assisted nonlinear optical 2D (N‐MPDA)[PbBr4] hybrid perovskite single crystal shows a stable photodetector performance with high responsivity, large specific detectivity, and functions as an optical gain medial for random lasing with high “Q” factor. The above features promising the asymmetric diammonium spacer will be highly beneficial in advancing 2D perovskite materials for steady optoelectronic applications.