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

Abstract

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)[PbBr 4 ] 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)[PbBr 4 ] 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) 2 PbBr 4 and (PEA) 2 PbBr 4 , and large specific detectivity (≈10 12 Jones). As an optical gain media, the (N-MPDA)[PbBr 4 ] 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)[PbBr 4 ] single crystal will offer a highperformance device and act as a dynamic material to construct stable future electronics and optoelectronic-based applications.

Influence of O−H⋅⋅⋅Pt interactions on photoluminescent response in the (Et4N)2{[Pt(bph)(CN)2][phenylene‐1,4‐diresorcinol]} framework

“…For example, cations or dedicated cation pairs are used for tuning the stability of hybrid metal halides and optical properties inherent in the metal halide skeleton via conditioning inorganic subnetwork dimensionality and topology, lattice or local symmetry, van der Waals separation and overall nanospace for electronic interaction. [1][2][3][4][5][6] In parallel, non-covalently bonded organic-inorganic systems (salts, double salts, co-crystal salts and solvates) involving functional discrete d-metallate complexes (polycyanidometallates, [7][8][9][10][11][12][13][14][15] polyoxometallates, [16][17][18] polyhalidometallates, [6,19] etc.) emerged to offer switchable dielectric properties, [7,8,10,12] piezo-and ferroelectric properties, [9] charge transfer (CT) and/or photoinduced electron transfer (PET) phenomena, [6,14,16,17,19] as well as nonlinear optical effects, [12] photoluminescence (PL) [12,17] and molecular waveguides functions.…”

“…The underlying properties are inscribed in the individual features of building blocks and/or in the way that building blocks become arranged in molecular architecture, in parallel with their frequently observed positioning and function. For example, cations or dedicated cation pairs are used for tuning the stability of hybrid metal halides and optical properties inherent in the metal halide skeleton via conditioning inorganic subnetwork dimensionality and topology, lattice or local symmetry, van der Waals separation and overall nanospace for electronic interaction [1–6] . In parallel, non‐covalently bonded organic‐inorganic systems (salts, double salts, co‐crystal salts and solvates) involving functional discrete d‐metallate complexes (polycyanidometallates, [7–15] polyoxometallates, [16–18] polyhalidometallates, [6,19] etc.)…”

Nonlinear and Emissive {[MIII(CN)6]3–···Polyresorcinol} (M = Fe, Co, Cr) Cocrystals Exhibiting an Ultralow Frequency Raman Response

“…This process relies on the interaction between matter and the incident beam, specifically, its polarization and orientation. The advantage of SHG lies in its narrow operating band, which allows for the precise control and manipulation of the generated signal. , The SHG function in the solid state requires a noncentrosymmetric space group and proper light absorption cutoff, which stimulated extended studies on the relevant inorganic, , organic, − as well as hybrid inorganic–organic − phases. In particular, the two latter composition strategies have recently been employed within the cocrystallization approach , considering the tunable intrinsic features of organic counterparts, e.g .…”