Two-photon absorption (TPA) and nonlinear refraction in AlN single crystals are revealed with the single beam Z-scan technique. A large TPA coefficient of 13±3cm/GW at 355nm and third-order nonlinear refractive indices of −1.91±0.38×10−13 cm2/W at 355 nm, 1.79±0.36×10−13 cm2/W at 532 nm and 1.61±0.32×10−12 cm2/W at 1064 nm are derived. It is inferred that the TPA-generated free carriers are responsible for the large negative nonlinear refractive index at 355 nm, while the oxygen impurity induced bandgap narrowing may account for the large third-order nonlinear refractive indices at 532 nm and 1064 nm. The large nonlinear optical responses of AlN promise wide applications in the deep ultraviolet nonlinear optical devices.
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