Chiral Lead Halide Perovskite Nanowires for Second-Order Nonlinear Optics

Abstract

Hybrid organic/inorganic lead halide perovskites (LHPs) have recently emerged as extremely promising photonic materials. However, the exploration of their optical nonlinearities has been mainly focused on the third- and higher-order nonlinear optical (NLO) effects. Strong second-order NLO responses are hardly expected from ordinary LHPs due to their intrinsic centrosymmetric structures, but are highly desirable for advancing their applications in the next generation integrated photonic circuits. Here we demonstrate the fabrication of a novel noncentrosymmetric LHP material by introducing chiral amines as the organic component. The nanowires grown from this new LHP material crystallize in a noncentrosymmetric P1 space group and demonstrate highly efficient second harmonic generation (SHG) with high polarization ratios and chiroptical NLO effects. Such a chiral perovskite skeleton could provide a new platform for future engineering of optoelectronic functionalities of hybrid perovskite materials.

Chiral Perovskites: Promising Materials toward Next‐Generation Optoelectronics

“…The chiral arrangement of ligands significantly affected the chiroptical properties of the chiral perovskites, and the electronic coupling between chiral enantiomer ligand and the quantum‐confined axis induced the circular dichroism signal. Recently, our group implemented the antisolvent vapor‐assisted crystallization (AVC), where an antisolvent (CHCl 3 ) gradually diffused into the solvent containing the crystal precursors and influenced the growth process . The 2D hybrid perovskite capped with R ‐ or S ‐β‐methylphenethylamine ( R ‐ or S ‐MPEA) was constructed in a ternary solvent system by using a mixture of N,N ‐dimethylformamide (DMF) and dimethyl sulfoxide (DMSO), which resulted in a chiral perovskite with a chemical constitution of (MPEA) 1.5 PbBr 3.5 (DMSO) 0.5 .…”

“…Excitation and detection wavelengths are 850 and 425 nm, respectively. Reproduced with permission . Copyright 2018, American Chemical Society.…”

“…Image of second harmonic generation. Reproduced with permission . Copyright 2018, American Chemical Society.…”

Spintronics of Hybrid Organic–Inorganic Perovskites: Miraculous Basis of Integrated Optoelectronic Devices

“…In addition, while the CD spectra are widely used in observation of the linear optical properties, new types of low‐dimensional perovskites are emerging for studies of the nonlinear optical effect induced by polarized light excitation. Researchers have also observed second‐order nonlinear responses in both 2D HOPs and higher‐order materials . They measured the second‐harmonic generation intensities of fabricated nanowires under different degrees of light polarization.…”

“…In 2018, Yuan et al crystallized a new lead halide perovskite material into nanowires by introducing chiral amines as organic components. These nanowires belong to the noncentrosymmetric P 1 space group and have a high polarization ratio and a higher‐order nonlinear optical effect that allow them to generate second harmonics efficiently …”