Development of Real-Time TDDFT Program with k-Point Sampling and DFT + U in a Gaussian and Plane Waves Framework

Area of Science:

• Computational Chemistry
• Materials Science
• Condensed Matter Physics

Background:

• Real-time time-dependent density functional theory (RT-TDDFT) is crucial for simulating material dynamics.
• Large-scale RT-TDDFT calculations are computationally demanding, limiting their application.
• Simulating systems with strong electron correlations requires advanced methods like DFT + U.

Purpose of the Study:

• To develop a scalable RT-TDDFT program within the Gaussian and plane waves (GPW) framework.
• To implement DFT + U for RT-TDDFT, enabling simulations of strongly correlated systems.
• To validate the efficiency and robustness of the developed methods for solid-state materials.

Main Methods:

• Development of a k-point sampling RT-TDDFT program integrated into the CP2K software suite.
• Implementation of symmetry-based k-point reduction and parallelization for computational efficiency.
• Extension of the "tensorial" subspace representation approach for DFT + U to k-point sampling RT-TDDFT.

Main Results:

• The developed RT-TDDFT program in the GPW framework is feasible for large-scale calculations.
• The extended DFT + U approach for k-point sampling RT-TDDFT is robust and efficient.
• The method shows promise for RT-TDDFT + U simulations of solid materials with small additional computational cost.

Conclusions:

• The new RT-TDDFT program with k-point sampling and DFT + U extension is a significant advancement for computational materials science.
• The implementation offers an efficient and robust approach for simulating complex electronic properties of solids.
• This work paves the way for more accurate and large-scale real-time simulations of materials.