Surface-Step-Terrace Tuned Second-Order Nonlinear Optical Coefficients of Epitaxial Ferroelectric BaTiO3 Films

Ferroelectric films epitaxially grown on vicinal substrates have been widely researched in recent decades for their unprecedented performance tuned by the surface-step-terrace (SST) induced strains of substrates. Here, BaTiO3 films are epitaxially grown on miscut (001) SrTiO3 substrates with different miscut angles of 0°, 0.2°, 1°, and 2°, and the impacts of SST-induced strains on the second-order nonlinear optical coefficients are discussed by fitting the measured second harmonic generation (SHG) signals from the films. The results show that different miscut angles of the substrates can bring about different SST strain states in the BTO films, which make different contributions on the second-order nonlinear optical coefficients. These results disclose that the second-order nonlinear optical coefficients can be effectively controlled by SST induced strains, which provides a new way to tune the optical properties of functional oxide thin films.