We present what we believe to be the first experimental determination of the third-order optical susceptibility ${\chi }^{\left(3\right)}$ of bulk cuprous oxide $\left({\mathrm{Cu}}_2\mathrm{O}\right)$ crystals. The measured nonlinear refractive index, obtained with the Z-scan technique at $1064\mathrm{nm}$ , is $n_2=1.32\times {10}^{-10}\mathrm{esu},$ while the two-photon absorption coefficient is $\beta =5.0\mathrm{cm}∕\mathrm{GW}$ of ${\mathrm{Cu}}_2\mathrm{O}$ . We also observe strong third-harmonic generation (THG) from ${\mathrm{Cu}}_2\mathrm{O}$ in our detection range owing to its unique crystal and electronic structure. Considering that the first nonvanishing nonlinear term is ${\chi }^{\left(3\right)}$ , this classical semiconductor could be utilized as a promising active THG medium.

© 2009 Optical Society of America

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