Crystalline Porous Materials for Nonlinear Optics

Abstract Crystalline porous materials have been extensively explored for wide applications in many fields including nonlinear optics (NLO) for frequency doubling, two‐photon absorption/emission, optical limiting effect, photoelectric conversion, and biological imaging. The structural diversity and flexibility of the crystalline porous materials such as the metal–organic frameworks, covalent organic frameworks, and polyoxometalates provide numerous opportunities to orderly organize the dipolar chromophores and to systemically modify the type and concentration of these dipolar chromophores in the confined spaces, which are highly desirable for NLO. Here, the recent advances in the crystalline porous NLO materials are discussed. The second‐order NLO of crystalline porous materials have been mainly devoted to the chiral and achiral structures, while the third‐order NLO crystalline porous materials have been categorized into pure organic and hybrid organic/inorganic materials. Some representative properties and applications of these crystalline porous materials in the NLO regime are highlighted. The future perspective of challenges as well as the potential research directions of crystalline porous materials have been also proposed.