English

Accurate QM/MM Molecular Dynamics for Periodic Systems in \textsc{GPU4PySCF} with Applications to Enzyme Catalysis

Chemical Physics 2024-11-26 v2 Biological Physics

Abstract

We present an implementation of the quantum mechanics/molecular mechanics (QM/MM) method for periodic systems using GPU accelerated QM methods, a distributed multipole formulation of the electrostatics, and a pseudo-bond treatment of the QM/MM boundary. We demonstrate that our method has well-controlled errors, stable self-consistent QM convergence, and energy-conserving dynamics. We further describe an application to the catalytic kinetics of chorismate mutase. Using an accurate hybrid functional reparametrized to coupled cluster energetics, our QM/MM simulations highlight the sensitivity in the calculated rate to the choice of quantum method, quantum region selection, and local protein conformation. Our work is provided through the open-source \textsc{PySCF} package using acceleration from the \textsc{GPU4PySCF} module.

Keywords

Cite

@article{arxiv.2408.03273,
  title  = {Accurate QM/MM Molecular Dynamics for Periodic Systems in \textsc{GPU4PySCF} with Applications to Enzyme Catalysis},
  author = {Chenghan Li and Garnet Kin-Lic Chan},
  journal= {arXiv preprint arXiv:2408.03273},
  year   = {2024}
}