We report our results from the investigations of linear and ultrafast nonlinear optical properties of a set of pyrrolo[1,2-a]quinoxalines. Using the steady state optical techniques and density functional theory calculations the linear optical properties were investigated while the non-resonant ultrafast nonlinear optical properties were studied using the degenerate four-wave mixing technique at a wavelength of 800 nm with 70 fs pulses. The investigated molecules demonstrated large off-resonant second hyperpolarizability (γ) and nonlinear refractive index (n2) values compared to similar molecular moieties with potential application in optical devices. © 2019 Elsevier B.V.