2023/03/07 by Yu Zhang, Zhang, Yu, M. J. Cawkwell +7
Earth and Planetary Sciences · Physics and Astronomy · #Advanced Chemical Physics Studies #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #High-pressure geophysics and materials #Quantum, superfluid, helium dynamics
paper · pdf · doi:10.48550/arxiv.2303.03655
openalex publication_date 2023/03/07 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
Extended Lagrangian Born-Oppenheimer molecular dynamics (XL-BOMD) [Phys. Rev. Lett. vol. 100, 123004 (2008)] is combined with Kohn-Sham density functional theory (DFT) using a DFT+U correction based on the Hubbard model. This combined XL-BOMD and DFT+U approach allows efficient Born-Oppenheimer molecular dynamics simulations with orbital-dependent corrections beyond regular Kohn-Sham density functional theory. The extended Lagrangian formulation eliminates the need for the iterative self-consistent-field optimization of the electronic ground state prior to the force evaluations, which is required in regular direct Born-Oppenheimer molecular dynamics simulations. This method provides accurate and stable molecular trajectories, while reducing the computational cost per time step. The combined XL-BOMD and DFT+U approach is demonstrated with molecular dynamics simulations of a nitromethane molecular liquid and a system of solid nuclear fuel, UO2, using self-consistent-charge density functional based tight-binding theory.