“…With the rapid development of nonlinear optics, nonlinear optical (NLO) materials are profoundly important in the fields of optical communications, optical machining, ultrafast photonics, etc. − Especially in recent years, materials with third-order NLO properties have been generally used in optical switching, mode-locking systems, laser protection, and other fields. − Compared to conventional third-order NLO materials, which mainly include inorganic and organic materials, such as metal nanoparticles, carbon materials, organic dye molecules, etc., − metal–organic frameworks (MOFs) composed of metal nodes and conjugated organic linkers not only combine the advantages of both inorganic and organic components but also have designable structures and tunable functions, ,− exhibiting fascinating third-order NLO properties. − For example, large conjugated porphyrin-based ligands have been used for the construction of new MOF materials with highly third-order NLO properties. − Moreover, the third-order NLO performances of MOFs have been optimized and improved by assembling MOFs into films, , or by adjusting the types of metal-chelated ligands, constructing interpenetrated networks, and encapsulating guest species . Although static third-order NLO properties of some MOF materials have been reported, the study of their dynamic NLO performance is limited.…”