The values of the nonlinear refractive index coefficient for various materials in the terahertz frequency range exceed the ones in both visible and NIR ranges by several orders of magnitude. We report the direct measurement of the nonlinear refractive index coefficient of liquid water by using the Z-scan method with broadband pulsed THz beam. Our experimental result shows that nonlinear refractive index coefficient in water is positive and can be as large as 3.5×10 −10 cm 2 /W in the THz frequency range, which exceeds the ones for the visible and NIR ranges by 6 orders of magnitude.

Polar liquids are strong absorbers of electromagnetic waves in the terahertz range, therefore, historically such liquids have not been considered as good candidates for terahertz sources. However, flowing liquid medium has explicit advantages, such as a higher damage threshold compared to solid-state sources and more efficient ionization process compared to gases. Here we report systematic study of efficient generation of terahertz radiation in flat liquid jets under sub-picosecond single-color optical excitation. We demonstrate how medium parameters such as molecular density, ionization energy and linear absorption contribute to the terahertz emission from the flat liquid jets. Our simulation and experimental measurements reveal that the terahertz energy has quasi-quadratic dependence on the optical excitation pulse energy. Moreover, the optimal pump pulse duration, which depends on the thickness of the jet is theoretically predicted and experimentally confirmed. The obtained optical-to-terahertz energy conversion efficiency is more than 0.05%. It is comparable to the commonly used optical rectification in most of electro-optical crystals and two-color air filamentation. These results, significantly advancing prior research, can be successfully applied to create a new alternative source of terahertz radiation.

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Despite the growing interest in nonlinear devices and components for light by light control in the terahertz range, there is a shortage of such materials and media used for these purposes. Here, we present the calculated values of low-inertia nonlinear refractive index coefficient for electro-optical crystals used in THz time-domain spectroscopy systems such as ZnSe, ZnTe, CdTe, GaP, and LiNbO3. The medium parameters affecting the cubic nonlinearity of the vibrational nature increase in the range of 0.5–1 THz have been determined. Comparison of theoretical calculations with known experimental results confirm the theoretical model as well as our analysis of media parameter influence on the cubic nonlinearity. In terms of applications, results obtained open up new perspectives for studying various materials in the THz frequency range.

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