摘要： In this study, first attempt has been made for theoretical designing of quinacridone (QA) dye and new QA-based compounds (QA-1 to QA-9) were proposed by installing auxiliary donors (dimethylvinyl, methoxy, and N,N-dimethylamine), donor (diphenylamine) and acceptors (cyanoacrylic acid, CN and NO2) segments into fixed π-bridge QA. DFT and TDDFT calculations with B3LYP/6-31G(d,p) and CAM-B3LYP/6-31G(d,p) functional were used to shed light on the promising structure, charge transport and NLO properties. Introduction of auxiliary donors/donor and acceptor successfully modified the structure which led to superior NLO properties. An eye-catching NLO response was observed in all designed compounds. Interestingly, QA-9 exhibits appealingly large enhancement in NLO properties through ICT process with < α > and βtot computed to be 716.02 (a.u) and 128082.15 (a.u) respectively. UV–Vis results indicates the QA-9 most red shifted among all studied compounds with λmax = 489.02 nm. QA-1 to QA-9 showed narrow HOMO-LUMO energy gap as compared to QA which results in enhanced NLO response. NBO analysis confirms the formation of charge separation state in QA-1 to QA-9 due to successful migration of electrons from auxiliary donors/donor to acceptors via π-bridge. The present research evokes the scientific interest regarding the development of QA based tempting NLO compounds that can be beneficial in modern hi-tech applications.