Linear and Nonlinear Optical Properties of SiO2/TiO2 Heterostructures Grown by Plasma-Enhanced Atomic Layer Deposition

Second harmonic (SH) radiation can only be generated in non-centrosymmetric bulk crystals under electric dipole approximation. Nonlinear thin films made from bulk crystals are technologically challenging because of complex and high-temperature fabrication processes. In this work, heterostructures made of two distinct amorphous materials, namely SiO2 and TiO2, were prepared through plasma-enhanced atomic layer deposition (PEALD) with deposition temperature of 100 °C. By using the uniaxial dispersion model, we characterized the form birefringence of the deposited films, which can play a crucial role for the phase-matching condition in nonlinear waveguides or other nonlinear optical applications. By applying a fringe-based technique, we determined the largest diagonal component of the effective bulk second-order susceptibility, χzzz(2) = 1.30 ± 0.13 pm/V, at a wavelength of 1032 nm. Noteworthy, we observed strong SHG signals from two-component nanolaminates, which are several orders of magnitude larger than those from single layers. The SHG signals from our samples only require the broken inversion symmetry at the interface. Here, optical properties of nanocomposites can be precisely engineered using the promising PEALD technology.