Time dependent density functional theory is used to systematically examine the band gap variation of Li-substituted adamantanes upon fluorination. It is realized that the absorption wavelength of Li-Adamantane can be fine tuned within UV–Visible region by changing the degree of fluorination. The static and dynamic hyperpolarizabilities of fluorinated Li-Adamantane derivatives were computed using coupled perturbed Kohn Sham theory. In this article, we report Pockel, dc-Kerr, ESHG, degenerate four wave mixing coefficients and nonlinear refractive indices from the first and second order hyperpolarizability calculations. A high positive nonlinear refractive index and significant second harmonic generation efficiency at Nd:YAG Laser wavelength are observed in F3Li-Adm derivative. © 2018 Elsevier B.V.