An effective strategy for tuning nonlinear optical response of N-atom functionalized corannulene by alkali metals doping: First theoretical insight.

[Display omitted] • 13 stable isomers of N -atom functionalized corannulene by alkali metals (Li, Na, K) doping are investigated. • All doped complexes exhibited significant thermodynamic stability. • Significant reduction of HOMO-LUMO gap is observed upon alkali metals doping. • Isomer V of Na@Cora-1N series exhibited eye-catching NLO response of 4.84x104 au. • The studied compounds are proposed to be better entrants for modern NLO applications. • This theoretical framework is a novel strategy to develop new NLO materials. Nonlinear optical (NLO) materials are gaining immense scientific attention in recent years due to their applications in diverse domains. An attempt is made for the first time in this study to theoretically design alkali metals (Li, Na, and K) doped 1 N -functionalized corannulene molecules. DFT method is used to investigate their geometric, thermodynamic stability, electronic and NLO properties. The E H-L gap is significantly reduced upto1.17 eV for doped isomers. The highest calculated first hyperpolarizability of the designed complexes is found to be 4.84x10⁴ au. NBO, NCI, TDOS and PDOS analyses are used to confirm the charge transfer, type of the interaction and the participation of different fragments, respectively. TD-DFT calculations show that these molecules are transparent in the UV region and almost all isomers show λ max in the visible region. This novel approach with comparatively higher static first hyperpolarizability values will open up new possibilities for both theoretical and experimental researchers to develop novel NLO materials. [ABSTRACT FROM AUTHOR]