Applications of quantum-classical and quantum-stochastic molecular dynamics simulations for proton transfer processes

Abstract

Quantum-classical and quantum-stochastic molecular dynamics models (QCMD/QSMD) are formulated and applied to describe proton transfer processes in three model systems - the proton bound ammonia-ammonia dimer in an external electrostatic field; malonaldehyde, which undergoes a quantum tautomeric rearrangement; and phospholipase A 2, an enzyme which induces a water dissociation process in its active site followed by proton hopping to a histidine imidazole ring. The proton dynamics are described by the time-dependent Schrödinger equation. The dynamics of the classical atoms are described using classical molecular dynamics. Coupling between the quantum proton (s) and the classical atoms is accomplished via conventional or extended Hellmann-Feynman forces, as well as the time-dependence of the potential energy function in the Schrödinger equation. The interaction of the system with its environment is described by stochastic forces. Possible extensions of the models as well as future applications in molecular structure and dynamics analysis will be briefly discussed.