Second-harmonic generation tensors from high-throughput density-functional perturbation theory.

Area of Science:

• Condensed matter physics
• Materials science
• Computational chemistry

Background:

• Optical materials are crucial for modern optoelectronics, with nonlinear optical crystals enabling broader electromagnetic wave manipulation.
• Discovering new nonlinear optical crystals is challenging due to conflicting material property requirements, hindering technological advancement.

Purpose of the Study:

• To compute and provide a comprehensive dataset of static nonlinear susceptibility and dielectric tensor for 579 inorganic semiconductors.
• To facilitate the identification of novel nonlinear optical crystals for experimental investigation and technological development.

Main Methods:

• Density-functional perturbation theory (DFPT) was employed for ab initio calculations.
• A systematic computational approach was used to derive static nonlinear susceptibility and dielectric tensor values.
• The reliability of the computational methodology was validated against existing experimental and ab initio data.

Main Results:

• A database of computed static nonlinear susceptibility and dielectric tensor for 579 inorganic semiconductors has been generated.
• The data distribution and format of the database are detailed.
• The accuracy of the computed data is confirmed through comparisons with literature values.

Conclusions:

• The generated dataset serves as a valuable resource for identifying promising nonlinear optical crystal candidates.
• This work aims to stimulate further experimental research into novel nonlinear optical materials.
• The findings support the advancement of optoelectronic technologies in sectors like medicine and energy.