The new tetracarbonyl -chromium-triphenyl phosphine complex was synthesized and characterized using ultraviolet (UV)-visible, Fourier transform infrared (FTIR), and nuclear magnetic resonance (NMR) techniques. The characterization results confirm the molecular structure of the new complex. The z-scan measurements were done by diode laser [continuous wave (CW)] to estimate the nonlinear optical parameter (χ 3 ). The results led to calculate three parameters: the groundstate cross sections (σ g ), the excited-state cross sections (σ ex ), and thermo-optic coefficient of the new complex. This study indicated that our complex is a suitable for photonic applications.