Exploration of Nonlinear Optical Properties for the First Theoretical Framework of Non-Fullerene DTS(FBTTh(2))(2)-Based Derivatives

[Image: see text] Organic compounds having significant nonlinear optical (NLO) applications are being employed in the optoelectronics field. In the current work, a series of non-fullerene acceptor (NFA) based compounds are designed by modifying the acceptors with different substituents using DTS(FBTTh(2))(2)R1 as a reference compound. To study the NLO responses to the tuning of various acceptors, DFT and TD-DFT based parameters were calculated at the M06 level along with the 6-31G(d,p) basis set. The designed compounds (MSTD2–MSTD7) showed smaller values of the energy gap in comparison to the reference compound. The energy gaps of the title compounds were linked to global reactivity insights; MSTD7 provided a lower band gap, with smaller and larger quantities for hardness and softness characteristics, respectively. Further, UV–vis analyses were performed for all of the designed compounds, displaying wavelengths red-shifted from that of DTS(FBTTh(2))(2)R1(.) The intraelectron transfer (ICT) process and stability of the title compounds were explored via frontier molecular orbital (FMO) and natural bond orbital (NBO) studies, respectively. Out of all the designed compounds, the highest value of linear polarizability ⟨α⟩ of 3.485 × 10(–22) esu, first hyperpolarizability (β(total)) of 13.44 × 10(–27) esu and second-order hyperpolarizability ⟨γ⟩ of 3.66 × 10(–31) esu were exhibited by MSTD7. In short, all of the designed compounds exhibited promising NLO properties because of their low charge transport resistance. These NLO properties may be useful for experimental researchers to uncover NLO materials for modern applications.