A polarizable three-layer frozen density embedding/molecular mechanics approach

We present a novel multilayer polarizable embedding approach in which the system is divided into three portions, two of which are treated using density functional theory and their interaction is based on frozen density embedding (FDE) theory, and both also mutually interact with a polarizable classical layer described using an atomistic model based on fluctuating charges (FQ). The efficacy of the model is demonstrated by extending the formalism to linear response properties and applying it to the simulation of the excitation energies of organic molecules in aqueous solution, where the solute and the first solvation shell are treated using FDE, while the rest of the solvent is modeled using FQ charges.

Automated summary

This study introduces a novel multilayer polarizable embedding approach, dividing the system into three portions, with two parts treated using density functional theory and their interaction based on frozen density embedding theory, while both interact with a classical layer described using fluctuating charges. The model's efficacy is demonstrated by extending the formalism to linear response properties and applying it to the simulation of excitation energies of organic molecules in aqueous solution.