Effect of different end-capped donor moieties on non-fullerenes based non-covalently fused-ring derivatives for achieving high-performance NLO properties

series of derivatives ( DOCD2–DOCD6 ) with D–π–A configuration was designed by substituting various efficient donor moieties via the structural tailoring of o-DOC6-2F . Quantum-chemical approaches were used to analyze the optoelectronic properties of the designed chromophores. Particularly, M06/6-311G(d,p) functional was employed to investigate the non-linear optical (NLO) response (linear polarizability ⟨α⟩, first ( β tot ) and second ( tot ) order hyperpolarizabilities) of the designed derivatives. A variety of analyses such as frontier molecular orbital (FMO), absorption spectra, transition density matrix (TDMs), density of states (DOS), natural bond orbital (NBO) and global reactivity parameters (GRPs) were employed to explore the optoelectronic response of aforementioned chromophores. FMO investigation revealed that DOCD2 showed the least energy gap (1.657 eV) among all the compounds with an excellent transference of charge towards the acceptor from the donor. Further, DOS pictographs and TDMs heat maps also supported FMO results, corroborating the presence of charge separation states along with efficient charge transitions. NBO analysis showed that π-linker and donors possessed positive charges while acceptors retained negative charges confirming the D–π–A architecture of the studied compounds. The λ max values of designed chromophores (659.070–717.875 nm) were found to have broader spectra. The GRPs were also examined utilizing energy band gaps of E HOMO and E LUMO for the entitled compounds. Among all the derivatives, DOCD2 showed the highest values of β tot (7.184 × 10 –27 esu) and tot (1.676 × 10 –31 esu), in coherence with the reduced band gap (1.657 eV), indicating future potentiality for NLO materials.