Theoretical Investigations of Structural, Electronic, and Nonlinear Optical Properties of 2‐Methoxy‐N, N‐diphenylbenzamide (2MNNDPB)

ABSTRACT Density functional theory (DFT) is a versatile method for predicting the properties of Nonlinear optical (NLO) materials. Different studies have employed the DFT approach to investigate NLO materials at the molecular level. Moving in the same line, we have selected a newly synthesized benzamide derivative, 2‐Methoxy‐N, N‐diphenylbenzamide (2MNNDPB), which is an organic NLO molecule for DFT investigation. The DFT approach is used to investigate the structural, electronic, and nonlinear optical behavior of the 2MNNDPB molecule theoretically. Geometry optimization calculations are performed to determine the values of optimized structural parameters of 2MNNDPB. Intra‐molecular charge transfer and its effect on hyperpolarizability are studied by Natural bond analysis. Further, the inter‐molecular charge transfer [ICT] and its impact on the nonlinear behavior of the material, stability, and reactivity of 2MNNDPB were investigated through HOMO‐LUMO energy gap analysis and molecular electrostatic potential mapping. NCI analysis is performed to understand inter‐ and intramolecular noncovalent interactions. Finally, the nonlinear optical behavior of 2MNNDPB is evaluated by determining the values of nonlinear optical parameters. The calculated first‐order hyperpolarizability(β tot ) of 2MNNDPB is 2.445014 × 10 −30 esu, which is approximately 12 times greater than that of urea. Therefore, the relatively high value of hyperpolarizability (β tot ) of 2MNNDPB promises its applicability in nonlinear optical applications.