Chiral hybrid organic−inorganic perovskites (HOIPs) with intrinsic noncentrosymmetry have shown great potentials for chiroptoelectronic applications including second‐order nonlinear optics (NLO). Ideal NLO materials should simultaneously feature a large NLO coefficient, wide optical transparency, high laser damage threshold, and physicochemical stability. However, the development of applicable second‐order NLO materials has been largely restricted due to their strict requirement on structural noncentrosymmetry. Here, chiral amino acids abundant in nature have been adopted to synthesize hybrid lead halide perovskites (D‐/L‐Pro)PbI3·H2O (Pro = Proline) with resonance enhanced second‐harmonic generation (SHG). Their crystals feature balanced NLO performances with a large NLO coefficient, wide transparent region, high laser damage threshold, and high polarization ratio. This work demonstrates the promise of naturally abundant amino acids for the construction of hybrid chiral metal halide perovskites for next generation optoelectronic materials.

Chiral metal halides have shown great potential for applications in next generation nonlinear optics (NLO) devices owing to their intrinsic non-centrosymmetry. However, the structures and properties of chiral hybrid indium...

Recently, chiral hybrid organic-inorganic perovskites (HOIPs) are drawing wide attention due to their intrinsic noncentrosymmetric structures which result in fascinating properties such as ferroelectronics and second-order nonlinear optics (NLO). However,...

Organic -conjugated materials have demonstrated superior nonlinear optical (NLO) performance and serve as ideal candidates for the photonic devices. However, the design of organic NLO materials with well-defined architectures and...