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Two self-healing-type supramolecular Ni(II)-metallogels are achieved. The choice of proper low-molecular-weight organic gelators such as trans -butenedioic acid ( i.e. , trans -BDA) and cis -butenedioic acid ( i.e. , cis -BDA) and triethylamine in N , N '-dimethylformamide solvent facilitates the metallogelation process. Through rheological investigations the mechanical robustness and viscoelastic properties of synthesized metallogels are explored. An in-depth exploration of thixotropic behavior also supports their self-healing features. Notably, distinct variations in morphologies of metallogels are also ascertained through field emission scanning electron microscopy studies. Furthermore, the existence of versatile noncovalent supramolecular interactions operating throughout the metallogel network is clearly revealed via Fourier transform infrared spectroscopy. Electrospray ionization-mass studies also explore the construction protocol of individual Ni(II)-metallogels. The Z-scan measurements with a 532 nm continuous wave laser were employed to unveil the nonlinear thermo-optical response of two synthesized self-healing metallogels, i.e. , trans -BDA-TEA@Ni(II) and cis -BDA-TEA@Ni(II). Crucial parameters like the nonlinear refractive index, nonlinear absorption coefficient, thermo-optical coefficient, and third-order susceptibility of these metallogels are obtained. Metallogels show negative signs for the nonlinear refractive index and the nonlinear absorption coefficient. The real parts of the third-order susceptibility for these metallogels are much greater than the imaginary parts ( i.e. , χ R (3) > χ I (3) ), making such metallogels very promising for all optical-switching applications.

The generation of solvent-directed self-healing supramolecular Ni(II) metallogels of glutaric acid (i.e., Ni-Glu-DMF and Ni-Glu-DMSO ) is described in this article. Polar aprotic solvents like N , N '-dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) are separately entrapped into the Ni(II)-acetate salt and glutaric acid-mediated networks to attain the semisolid flexible scaffolds. The gel nature of the fabricated materials is experimentally proven through different rheological tests such as amplitude sweep, frequency sweep, and thixotropic (time sweep) measurements. The self-repairing strategy and load-bearing features of the synthesized metallogel are studied in this work. The different supramolecular noncovalent interactions working within the soft scaffold are clearly explored. The formation strategy and the microstructural features of these synthesized metallogels are scrutinized through a Fourier transform infrared (FT-IR) spectroscopy study and field-emission scanning electron microscopy (FESEM) morphological analyses. The FT-IR spectroscopy observation displays a considerable amount of shifting of the infrared (IR) peaks of the xerogel samples of both the metallogels Ni-Glu-DMF and Ni-Glu-DMSO . The electrospray ionization (ESI)-mass spectroscopy result demonstrates the plausible construction of the metallogel network. In order to examine the nonlinear optical characteristics of the two synthesized self-healing metallogels Ni-Glu-DMSO and Ni-Glu-DMF , Z-scan measurements are carried out with a continuous wave (CW) diode-pumped solid-state (DPSS) laser at 532 nm. The nonlinear refractive index, nonlinear absorption coefficient, thermo-optical coefficient, and third-order susceptibility of these metallogels were evaluated by analyzing the experimental data from the Sheik-Bahae formalism. The nonlinear thermo-optical study reveals that these solvent-dependent metallogels show negative signs of nonlinear refractive index and nonlinear absorption coefficient. The figure of merit calculated for these compounds shows good agreement for their use in nonlinear photonic devices.