The NLO property of a few designed inorganic-organic hybrid materials based on Nickel dithiolenes endcapped with donor-acceptor groups has been studied theoretically. All the designed molecules possess high rst hyperpolarizability values indicating their potential use in optics, photonics, and as photosensitizers. Among the four designed systems, the BODIPY-containing systems signi cantly reduce the HOMO-LUMO energy gap resulting in a massive trek in the rst hyperpolarizability (β) values. To judge their high NLO response, transition dipole moment (TDM) density has been plotted and it has been found that electron dissipation occurs through the molecular network with a large Δr index value. It is to be noted that high Δr index values are quantitative measurements to understand the type of transitions, and we noticed that a charge transfer transition occurs in all of our designed systems. Hence a nice correlation between the rst hyperpolarizability, TDM density, and Δr index value has been observed. The global reactivity parameters are also studied and correlated nicely with polarizability and hole-electron transport ability.

The NLO property of a few designed inorganic-organic hybrid materials based on Nickel dithiolenes end-capped with donor-acceptor groups has been studied theoretically. All the designed molecules possess high first hyperpolarizability values indicating their potential use in optics, photonics, and as photosensitizers. Among the four designed systems, the BODIPY-containing systems significantly reduce the HOMO-LUMO energy gap resulting in a massive trek in the first hyperpolarizability (β) values. To judge their high NLO response, transition dipole moment (TDM) density has been plotted and it has been found that electron dissipation occurs through the molecular network with a large Δr index value. It is to be noted that high Δr index values are quantitative measurements to understand the type of transitions, and we noticed that a charge transfer transition occurs in all of our designed systems. Hence a nice correlation between the first hyperpolarizability, TDM density, and Δr index value has been observed. The global reactivity parameters are also studied and correlated nicely with polarizability and hole-electron transport ability.