In Silico Modeling of New “Y-Series”-Based Near-Infrared Sensitive Non-Fullerene Acceptors for Efficient Organic Solar Cells

[Image: see text] This work was inspired by a previous report [Janjua, M. R. S. A. Inorg. Chem. 2012, 51, 11306–11314] in which the optoelectronic properties were improved with an acceptor bearing heteroaromatic rings. Herein, we have designed four novel Y-series non-fullerene acceptors (NFAs) by end-capped acceptor modifications of a recently synthesized 15% efficient Y21 molecule for better optoelectronic properties and their potential use in solar cell applications. Density functional theory (DFT) along with time-dependent density functional theory (TDDFT) at the B3LYP/6-31G(d,p) level of theory is used to calculate the band gap, exciton binding energy along with transition density matrix (TDM) analysis, reorganizational energy of electrons and holes, and absorption maxima and open-circuit voltage of investigated molecules. In addition, the PM6:YA1 complex is also studied to understand the charge shifting from the donor polymer PM6 to the NFA blend. Results of all parameters suggest that the DA’D electron-deficient core and effective end-capped acceptors in YA1–YA4 molecules form a perfect combination for effective tuning of optoelectronic properties by lowering frontier molecular orbital (FMO) energy levels, reorganization energy, and binding energy and increasing the absorption maximum and open-circuit voltage values in selected molecules (YA1–YA4). The combination of extended conjugation and excellent electron-withdrawing capability of the end-capped acceptor moiety in YA1 makes YA1 an excellent organic solar cell (OSC) candidate owing to promising photovoltaic properties including the lowest energy gap (1.924 eV), smallest electron mobility (λ(e) = 0.0073 eV) and hole mobility (λ(h) = 0.0083 eV), highest λ(max) values (783.36 nm (in gas) and 715.20 nm (in chloroform) with lowest transition energy values (E(x)) of 1.58 and 1.73 eV, respectively), and fine open-circuit voltage (V(oc) = 1.17 V) with respect to HOMO(PM6)–LUMO(acceptor). Moreover, selected molecules are observed to have better photovoltaic properties than Y21, thus paving the way for experimentalists to look for future developments of Y-series-based highly efficient solar cells.