Projected Wave Function Extrapolation Scheme to Accelerate Plane-Wave Hybrid Functional-Based Born-Oppenheimer...

Area of Science:

• Computational Chemistry and Physics
• Materials Science
• Quantum Mechanics

Background:

• Born-Oppenheimer molecular dynamics (BOMD) simulations are crucial for understanding molecular and solid system dynamics.
• Hybrid functional-based BOMD (H-BOMD) simulations, particularly with plane-wave basis sets, are computationally expensive due to frequent self-consistent-field (SCF) calculations.
• Accelerating these simulations is essential for broader applicability and efficiency.

Purpose of the Study:

• To develop an efficient wave function extrapolation method to accelerate plane-wave H-BOMD simulations.
• To reduce the number of SCF iterations required per molecular dynamics (MD) step.
• To maintain or improve the accuracy of BOMD simulations.

Main Methods:

• Introduction of the Projected Always Stable Predictor-Corrector (PASPC) method for wave function extrapolation.
• Investigation of convergence properties of different extrapolation schemes for both molecular and solid systems.
• Evaluation of energy drift and simulation accuracy using PASPC in plane-wave H-BOMD.

Main Results:

• PASPC significantly accelerates plane-wave H-BOMD simulations by reducing SCF iterations.
• The method yields wave functions closer to the true solution space, enhancing convergence.
• PASPC demonstrates reduced energy drift oscillations, enabling larger time steps, especially for systems with heavy atoms.
• Simulations show improved accuracy in power and infrared spectra for silicon dioxide and liquid water, comparable to experimental data.

Conclusions:

• The PASPC method offers a substantial speedup for plane-wave H-BOMD simulations without compromising accuracy.
• PASPC enhances the reliability and efficiency of BOMD simulations for complex molecular and solid systems.
• This advancement facilitates more accurate predictions of material properties and dynamic behaviors.