Acceleration of self-consistent-field convergence in ab initio molecular dynamics and Monte Carlo simulations and geometry optimization

We propose a novel acceleration method for self-consistent-field calculations in direct ab initio molecular dynamics/Monte Carlo (AIMD/AIMC) simulations and geometry optimization. This acceleration method, so-called LSMO, predicts an initial guess of molecular orbitals (MOs) for the next simulation step by using the geometric information with the least-squares technique. Numerical tests confirm that the LSMO method is both effective and feasible in the AIMD/AIMC simulations and geometry optimization.