Computational insights into the static, solvent and frequency-dependent nonlinear optical properties of head-to-tail novel non-fullerene compounds for modern electro-optic applications

[Display omitted] •Solvent-dependent NLO properties have been calculated by employing DFT and TDDFT.•Band gap of studied systems lies in the range of 2.54 to 1.56 eV.•Acceptor modification results in an increase in static polarizability.•Investigated chromophores showed substantial SHG and EOPE values at 532 nm and 1064 nm lasers.•Studied chromophores are recommended as excellent NLO materials for future cutting-edge optoelectronic applications. Addressing the growing demand of novel nonlinear optical (NLO) materials, hyper-rayleigh-scattering (HRS) in solution, static and frequency-dependent NLO properties of novel IsoIDTC-based derivatives (AFS1-AFS9) are computed at laser frequencies of 1064 nm and 532 nm to explore SHG β (−2ω, ω, ω) and EOPE β (−ω, ω, 0) for modern electro-optic applications. Structural, electrical, and NLO features were calculated using DFT, and TDDFT modeling, HRS, and DR measurement. The polar, non-polar solvent, and gas phase NLO properties show the highest linear polarizability of 8.92 × 102 a.u. (AFS8) in water, 9.68 × 102 a.u. (AFS5) in gas, and 9.56 × 102 a.u. (AFS) in benzene. AFS8 push-pulls exhibit the highest first hyper-polarizability (βtot) at 1.05 × 105 a.u. and 1.47 × 105 a.u. in gas and benzene solvent, respectively. The proposed chromophores showed substantial SHG and EOPE values at 532 nm and 1064 nm lasers compared toIDT, hence, allowed the successful synthesis of NLO materials for future cutting-edge optoelectronic applications.