1 research outputs found
Grand Canonical Adaptive Resolution Simulation for Molecules with Electrons: A Theoretical Framework based on Physical Consistency
A theoretical scheme for the treatment of an open molecular system with
electrons and nuclei is proposed. The idea is based on the Grand Canonical
description of a quantum region embedded in a classical reservoir of molecules.
Electronic properties of the quantum region are calculated at constant
electronic chemical potential equal to that of the corresponding (large) bulk
system treated at full quantum level. Instead, the exchange of molecules
between the quantum region and the classical environment occurs at the chemical
potential of the macroscopic thermodynamic conditions. T he Grand Canonical
Adaptive Resolution Scheme is proposed for the treatment of the classical
environment; such an approach can treat the exchange of molecules according to
first principles of statistical mechanics and thermodynamic. The overall scheme
is build on the basis of physical consistency, with the corresponding
definition of numerical criteria of control of the approximations implied by
the coupling. Given the wide range of expertise required, this work has the
intention of providing guiding principles for the construction of a well
founded computational protocol for actual multiscale simulations from the
electronic to the mesoscopic scale.Comment: Computer Physics Communications (2017), in pres