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Area of Science:

Materials Science
Nonlinear Optics
Solid State Physics

Background:

Third harmonic generation (THG) is a key nonlinear optical process.
Understanding nonlinear optical properties of dielectric materials is crucial for photonic applications.
Previous studies have focused on lower-order nonlinearities in thin films.

Purpose of the Study:

To investigate third harmonic generation (THG) in HfO2 dielectric layers.
To quantify the third-order nonlinear susceptibility (χ(3)) and the fifth-order nonlinear susceptibility (χ(5)) in HfO2.
To elucidate the influence of the substrate on THG in layered dielectric materials.

Main Methods:

Fabrication of a thin gradient of Hafnium Oxide (HfO2) with continuously increasing thickness.
Detailed investigation of the third harmonic generation process.
Spectroscopic analysis at a fundamental wavelength of 1030 nm.

Main Results:

Successfully quantified the third-order nonlinear susceptibility (χ(3)) of the HfO2 layers.
Achieved the first measurement of the fifth-order nonlinear susceptibility (χ(5)) in thin dielectric layers.
Demonstrated the influence of the substrate on the THG process.

Conclusions:

The gradient HfO2 layer technique provides a detailed method for studying nonlinear optical properties.
The fifth-order nonlinear susceptibility (χ(5)) in thin dielectric layers can be measured.
Substrate effects play a significant role in third harmonic generation from dielectric layers.