title: From Classical to Quantum and Back: A Hamiltonian Scheme for Adaptive Multiresolution Classical/Path-Integral Simulations.
abstract: Quantum delocalization of atomic nuclei affects the physical properties of many hydrogen-rich liquids and biological systems even at room temperature. In computer simulations, quantum nuclei can be modeled via the path-integral formulation of quantum statistical mechanics, which implies a substantial increase in computational overhead. By restricting the quantum description to a small spatial region, this cost can be significantly reduced. Herein, we derive a bottom-up, rigorous, Hamiltonian-based scheme that allows molecules to change from quantum to classical and vice versa on the fly as they diffuse through the system, both reducing overhead and making quantum grand-canonical simulations possible. The method is validated via simulations of low-temperature parahydrogen. Our adaptive resolution approach paves the way to efficient quantum simulations of biomolecules, membranes, and interfaces.
authors.affiliation: Max Planck Institute for Polymer Research , Ackermannweg 10, 55128 Mainz, Germany.|Graduate School Materials Science in Mainz, Johannes Gutenberg University Mainz , Staudinger Weg 9, 55128 Mainz, Germany.
authors.forename: Karsten
authors.initials: K
authors.lastname: Kreis
authors.affiliation: Department of Chemistry, New York University (NYU) , New York, New York 10003, United States.|Courant Institute of Mathematical Sciences, NYU , New York, New York 10012, United States.|NYU-East China Normal University Center for Computational Chemistry at NYU Shanghai , Shanghai 200062, China.
authors.forename: Mark E
authors.initials: ME
authors.lastname: Tuckerman
authors.affiliation: Max Planck Institute for Polymer Research , Ackermannweg 10, 55128 Mainz, Germany.|Department of Chemistry, University of California at Davis , One Shields Avenue, Davis, California 95616, United States.
authors.forename: Davide
authors.initials: D
authors.lastname: Donadio
authors.affiliation: Max Planck Institute for Polymer Research , Ackermannweg 10, 55128 Mainz, Germany.
authors.forename: Kurt
authors.initials: K
authors.lastname: Kremer
authors.affiliation: Max Planck Institute for Polymer Research , Ackermannweg 10, 55128 Mainz, Germany.
authors.forename: Raffaello
authors.initials: R
authors.lastname: Potestio