Silver iodide (AgI) thin films offer a compelling platform for studying nonlinear optical phenomena due to their intrinsic noncentrosymmetric lattice and direct band gap. Here, we investigate the nonlinear optical properties of AgI thin films grown by physical vapor deposition that selectively produce zinc-blende $\left(\gamma \text{−}\mathrm{AgI}\right)$ and wurtzite $\left(\beta \text{−}\mathrm{AgI}\right)$ phases. Using a combination of polarization-resolved second-harmonic generation (SHG) and two-photon photoluminescence (2PPL) spectroscopy, we identify clear phase- and morphology-dependent anisotropic nonlinear responses. Triangular $\gamma \text{−}\mathrm{AgI}\left(111\right)$ flakes exhibit sixfold SHG symmetry and isotropic 2PPL emission, while rod-shaped $\beta \text{−}\mathrm{AgI}\left(101\right)$ samples display twofold-symmetric patterns in both SHG and 2PPL, which are explained by theories that integrate explicit polarization analysis using second- and third-order nonlinear susceptibilities. We estimate ${\chi }_{\mathrm{eff}}^{\left(2\right)}$ of 0.45 pm/V $\left(\gamma \text{−}\mathrm{AgI}\right)$ and 0.16 pm/V $\left(\beta \text{−}\mathrm{AgI}\right)$, respectively, after correcting for multiple internal reflections and generation of SHG within the AgI film and optical interference effect in the dielectric layers. These results identify AgI as a useful single-composition halide platform for studying phase-dependent nonlinearity and establish a realistic methodology for evaluating nonlinear susceptibilities in layered materials or thin films supported by a substrate.

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• Nonlinear optics
• Third order nonlinear optical processes
• Thin films
• Optical second-harmonic generation