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Grand-Canonical-like adaptive resolution of molecules with electrons

Subject Area Theoretical Chemistry: Electronic Structure, Dynamics, Simulation
Term from 2020 to 2024
Project identifier Deutsche Forschungsgemeinschaft (DFG) - Project number 439321740
 
Final Report Year 2024

Final Report Abstract

The project concerns the development of a method to treat a molecular liquid in an open region at ab initio electronic resolution embedded in a classical reservoir of energy and particles. Liquid water at room conditions was chosen, because of its high relevance in chemical physics, as test system of the method. A numerical protocol based on a mathematical model of open quantum particle system, developed in this project, is applied. The corresponding results are compared with results of a full ab initio simulation of reference. The key conclusion is that one can claim the possibility of defining a numerical strategy where a quantum region can be interfaced with a classical reservoir such that (i) structural and electronic properties reproduce those of reference and (ii) the exchange of molecules with the environment takes place as expected. This work, an extension of the classical adaptive resolution method (AdResS), provides a proof of concept about the possibility to systematically define a physically well founded open quantum system embedded in a classical environment. In turn, the proof of concept for the design, in the next step, of a numerically efficient algorithm for ab initio molecular dynamics simulations of open systems.

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