Giant Optical Activity and Second Harmonic Generation in 2D Hybrid Copper Halides

Abstract

Hybrid organic–inorganic metal halides have emerged as highly promising materials for a wide range of applications in optoelectronics. Incorporating chiral organic molecules into metal halides enables the extension of their unique optical and electronic properties to chiral optics. By using chiral (R)‐ or (S)‐methylbenzylamine (R‐/S‐MBA) as the organic component, we synthesized chiral hybrid copper halides, (R‐/S‐MBA)2CuCl4, and investigated their optical activity. Thin films of this material showed a record anisotropic g‐factor as high as approximately 0.06. We discuss the origin of the giant optical activity observed in (R‐/S‐MBA)2CuCl4 by theoretical modeling based on density functional theory (DFT) and demonstrate highly efficient second harmonic generation (SHG) in these samples. Our study provides insight into the design of chiral materials by structural engineering, creating a new platform for chiral and nonlinear photonic device applications of the chiral hybrid copper halides.

Reversible phase transition for switchable second harmonic generation in 2D perovskite microwires

“…The complexity and high cost of nanophotonics processing, fabricated by chemical vapor deposition and electron‐beam lithography techniques, hinder the broad applications of SHG switching. In contrast, low‐cost solution‐processable semiconductors with stimuli‐responsive properties offer a feasible approach to constructing reversible solid‐state SHG switching, but the fabrication of large SHG switching contrast is still challenging 13–18 . Based on the single crystallinity of self‐assembled CsPbBr 3 perovskite microwires, Xiong and his colleagues 19 demonstrate all‐optical switching on a picosecond time scale.…”

Multi‐Stimuli Responsive Luminescence and Domino Phase Transition of Hybrid Copper Halides with Nonlinear Optical Switching Behavior

“…The Cu I ion has attracted much attention due to its significant 3d 10 ‐3d 9 4s 1 electron transition. In addition, compared with Pb 2+ , coordination engineering of Cu I halide enriches the connection mode of the halide center, providing a broad exploration space for various structural types of copper halide materials such as linear, triangular, tetrahedron, dimer consist of two edged/faced‐shared tetrahedrons, octahedron and so on [9–12] . The structural variability makes it possible for copper halides to become very promising PTMs.…”