Gap-Free Tuning of Second and Third Harmonic Generation in Mechanochemically Synthesized Nanocrystalline LiNb_1-xTa_xO₃ (0 x 1) Studied with Nonlinear Diffuse Femtosecond-Pulse Reflectometry

The tuning of second (SHG) and third (THG) harmonic emission is studied in the model system LiNb1-xTaxO3 (0 <= x <= 1, LNT) between the established edge compositions lithium niobate (LiNbO3, x = 0, LN) and lithium tantalate (LiTaO3, x = 1, LT). Thus, the existence of optical nonlinearities of the second and third order is demonstrated in the ferroelectric solid solution system, and the question about the suitability of LNT in the field of nonlinear and quantum optics, in particular as a promising nonlinear optical material for frequency conversion with tunable composition, is addressed. For this purpose, harmonic generation is studied in nanosized crystallites of mechanochemically synthesized LNT using nonlinear diffuse reflectometry with wavelength-tunable fundamental femtosecond laser pulses from 1200 nm to 2000 nm. As a result, a gap-free harmonic emission is validated that accords with the theoretically expected energy relations, dependencies on intensity and wavelength, as well as spectral bandwidths for harmonic generation. The SHG/THG harmonic ratio >> 1 is characteristic of the ferroelectric bulk nature of the LNT nanocrystallites. We can conclude that LNT is particularly attractive for applications in nonlinear optics that benefit from the possibility of the composition-dependent control of mechanical, electrical, and/or optical properties.