Oxidized dichloromethane solutions of cis-Mo(CO)4(PPh3)2 stabilized by the addition of excess PPh3 exhibit unusual large molecular second-order hyperpolarizabilities with minimal linear absorption. To better understand the mechanism by which this occurs, DFWM, Z-scan and optical limiting experiments have been carried out on oxidized dichloromethane solutions of cis-Mo(CO)4(PPh3)2 using 5.8 ns laser pulses at 532 nm. Our results demonstrate that the mechanism by which the oxidized species enhance the third-order nonlinear response is not dominated by thermal effects, but is instead due to the strong nonlinear absorption and nonlinear refraction of the oxidized species. Moreover, the oxidized species shows very strong optical limiting properties. Such complexes would be very interesting third-order nonlinear optical materials for optical limiting applications.