A variety of new inorganic and organic materials have emerged to advance laser technologies and optical engineering. A rational design approach can contribute significantly to fabricating nonlinear optically active metal−organic frameworks (MOFs) by considering the underlying structure−property linkage. Here, it has been embarked on a study of novel samarium(III) MOF, ([Sm2(ata)3(DMF)4]·DMF (ata2−: 2- aminoterephthalate), abbreviated as NH2-Sm-MUM-4) with enhanced nonlinear optical (NLO) properties. The crystal structure of this MOF represents a 6-connected framework with a pcu topology and distinctive characteristics, including open metal sites, free amine groups, and great stability, making it suitable for third-order NLO activity. The nonlinear index of refraction (n2) revealed the self-focusing impacts of NH2-Sm- MUM-4 at different incident intensities. The highest value of n2 and β related to 10 mw power of incident intensity are 5.15 cm2/W and 2.65 cm/W, respectively. As far as the authors know, this is the first study examining the potential systematic structural−property associations in Sm-MOFs considering improved third-order NLO properties.
