Shadow Molecular Dynamics for a Charge-Potential Equilibration Model

Abstract: We introduce a shadow molecular dynamics (MD) approach based on the Atom-Condensed Kohn-Sham second-order (ACKS2) charge-potential equilibration model. In contrast to regular flexible charge models, the ACKS2 model includes both flexible atomic charges and potential fluctuation parameters that allow for physically correct charge fragmentation and scaling of the polarizability. Our shadow MD scheme is based on an approximation of the ACKS2's flexible charge-potential energy function, in combination with extended Lagrangian Born-Oppenheimer MD. Utilizing this shadow charge-potential equilibration approach mitigates the costly overhead and stability problems associated with finding well-converged iterative solutions to the charges and potential fluctuations of the ACKS2 model in an MD simulation. Our work provides a robust and versatile framework for efficient, high-fidelity MD simulations of diverse physical phenomena and applications.