title: First principles molecular dynamics without self-consistent field optimization.
abstract: We present a first principles molecular dynamics approach that is based on time-reversible extended Lagrangian Born-Oppenheimer molecular dynamics [A. M. N. Niklasson, Phys. Rev. Lett. 100, 123004 (2008)] in the limit of vanishing self-consistent field optimization. The optimization-free dynamics keeps the computational cost to a minimum and typically provides molecular trajectories that closely follow the exact Born-Oppenheimer potential energy surface. Only one single diagonalization and Hamiltonian (or Fockian) construction are required in each integration time step. The proposed dynamics is derived for a general free-energy potential surface valid at finite electronic temperatures within hybrid density functional theory. Even in the event of irregular functional behavior that may cause a dynamical instability, the optimization-free limit represents a natural starting guess for force calculations that may require a more elaborate iterative electronic ground state optimization. Our optimization-free dynamics thus represents a flexible theoretical framework for a broad and general class of ab initio molecular dynamics simulations.
authors: Department of Physics and Astronomy, Division of Materials Theory, Uppsala University, Box 516, SE-75120 Uppsala, Sweden.
authors: Petros
authors: P
authors: Souvatzis
authors: Theoretical Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA.
authors: Anders M N
authors: AM
authors: Niklasson
mesh_terms: D004583:Electrons; D004980:Ethane / Q000737:chemistry; D007700:Kinetics; D056004:Molecular Dynamics Simulation; D011789:Quantum Theory; D012399:Rotation; D013302:Streptomyces / Q000737:chemistry; D013696:Temperature; D014732:Vibration; D014867:Water / Q000737:chemistry
chemical_list: D014867:Water; D004980:Ethane