Structure-dependent optical nonlinearity of indium tin oxide

We use post-deposition vacuum annealing of epsilon-near-zero (ENZ) indium tin oxide (ITO) nanolayers in order to modify their structural properties and enhance the third-order optical nonlinear response around the ENZ wavelength. We find that room temperature magnetron sputtering deposition results in polycrystalline thin films with an intrinsic tensile strain and a ⟨110⟩ fiber axis preferentially oriented normal to the substrate. Moreover, we demonstrate that post-deposition vacuum annealing treatments produce a secondary anisotropic phase characterized by compressive strain that increases with the annealing temperature. Finally, we use the Z-scan optical technique to accurately measure the complex nonlinear susceptibility χ ( 3 ) and the intensity-dependent refractive index change Δ n for samples with different structural properties despite featuring similar ENZ wavelengths. Our intensity-dependent analysis demonstrates that an enhancement of the optical nonlinearity can be achieved by tuning the structure of ENZ nanolayers with values as large as χ R ( 3 ) = ( 5.2 ± 0.3 ) × 10 − 17 m 2 / V 2. This study unveils the importance of structural control and secondary phase formation in ITO nanolayers with ENZ optical dispersion properties for the engineering of integrated highly nonlinear devices and metamaterials that are compatible with the scalable silicon photonics platform.