DFT-CES2: Quantum Mechanics Based Embedding for Mean-Field QM/MM of Solid–Liquid Interfaces

The solid–liquid interface plays a crucial role
in governing
complex chemical phenomena, such as heterogeneous catalysis and (photo)electrochemical
processes. Despite its importance, acquiring atom-scale information
about these buried interfaces remains highly challenging, which has
led to an increasing demand for reliable atomic simulations of solid–liquid
interfaces. Here, we introduce an innovative first-principles-based
multiscale simulation approach called DFT-CES2, a mean-field QM/MM
method. To accurately model interactions at the interface, we developed
a quantum-mechanics-based embedding scheme that partitions complex
noncovalent interactions into Pauli repulsion, Coulomb (including
polarization), and London dispersion energies, which are described
using atom-dependent transferable parameters. As validated by comparison
with high-level quantum mechanical energies, DFT-CES2 demonstrates
chemical accuracy in describing interfacial interactions. DFT-CES2
enables the investigation of complex solid–liquid interfaces
while avoiding extensive parametrization. Therefore, we expect DFT-CES2
to be broadly applicable for elucidating atom-scale details of large
scale solid–liquid interfaces for multicomponent systems.