Abstract

Two-dimensional materials have recently attracted attention due to their unique physical properties and promising applications. This work reports the electronic, linear and second-order nonlinear optical properties of aluminum nitride (AlN) monolayer by using a real-time first-principles approach based on Green's function theory. In this approach, quasi-particle corrections, crystal local field effects, and excitonic contributions are considered for investigating the linear and nonlinear responses. As a two-dimensional material with a wide direct gap of around 6.45 eV, the AlN monolayer exhibits strong resonances of absorption and second-harmonic spectra in the ultraviolet range. In the transparent spectral range from blue to deep ultraviolet (2.8-5.3 eV), strong peaks of second-order nonlinear susceptibility appear in the AlN monolayer with a large peak value of around 430 pm/V, which is one or two orders-of-magnitude larger than the nonlinear materials used in the ultraviolet range. The results presented in this work will find important applications for nonlinear imaging, spectroscopy, and nonlinear nanophotonics in the ultraviolet range.

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