N,N′-bis(5-bromosalicylidene)propane-1,2-diamine-O,O′,N,N′)-manganese(III) chloride transition metal complex has been synthesized and characterized by elemental analysis and UV-vis spectroscopy. Its crystal structure has been determined using X-ray diffraction analysis. To provide an insight into the optical limiting (OL) behavior of the title compound, the third-order nonlinear optical (NLO) properties, one-photon absorption (OPA) and two-photon absorption (TPA) characterizations have been theoretically investigated by means of the time-dependent Hartree–Fock (TDHF), AM1 and configuration interaction (CI) methods, respectively. According to ab initio calculation results, the examined molecule exhibits second hyperpolarizabilities (γ) with non-zero values at the positions of TPA peaks, implying microscopic third-order optical nonlinearity. The maximum OPA wavelengths recorded by linear optical experiment and quantum mechanical computations are estimated in the UV region to be shorter than 400 nm, showing good optical transparency to the visible light. The TPA cross-sections (δ(ω)) at [Formula: see text] values indicate that the synthesized compound might possess OL phenomena, which are in accord with the experimental observations on the manganese complexes in the literature.