Abstract
Nonlinear optical (NLO) materials are essential for the advancement of ultrashort laser pulses, optoelectronics, and high-speed optical communications. In this study, we investigate the NLO properties of a perylenediimide derivative, N,N'-di(2-(trimethylammonium iodide) ethylene) perylenediimide (TAIPDI), immobilized within two zirconium-based metal-organic frameworks (MOFs): UiO-66 and UiO-66-NH2. Using femtosecond laser pulses, we observed enhanced NLO responses in the MOF-dye composites compared to the TAIPDI dye. Characterization techniques, including steady-state absorption and fluorescence spectroscopy, revealed stronger interactions between TAIPDI and the amino-functionalized UiO66-NH2 compared to UiO-66. Key NLO parameters were measured, including nonlinear refractive index (n2), nonlinear absorption (NLA) coefficient (β), and third-order NLO susceptibility (χ(3)). The results demonstrated: (i) Both TAIPDI-UiO-66 and TAIPDI-UiO66-NH2 exhibited significantly higher NLA and NLR coefficients compared to the free TAIPDI dye. (ii) TAIPDI-UiO66-NH2 composite showed the most pronounced NLO enhancement, with n2 approximately 2.5 times higher than that of TAIPDI-UiO-66. (iii) The observed NLA behavior was attributed to RSA. (iv) The incorporation of TAIPDI into both MOFs resulted in significantly improved optical limiting properties. (v) TAIPDI-UiO-66 and TAIPDI-UiO66-NH2 exhibited 2PACS values of 2.78 × 107 GM and 3.25 × 107 GM, respectively. These results highlight the synergistic effects of MOF encapsulation and framework functionalization, positioning these composites as highly promising materials for advanced photonic devices and optical power limiting applications.
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