Density functional theory in classical explicit solvents: Mean-field QM/MM method for simulating solid-liquid interfaces

Solid-liquid interfaces are ubiquitous in scientifically and technologically important systems, and they govern complex chemophysical processes such as those in electrochemistry and heterogeneous catalysis. Atomic-level elucidation of interfacial structures has been extensively pursued; however, related research is still limited. A major obstacle lies in the intrinsic character of interfaces: they are located between two bulk phases that make the application of spectroscopic or surface-science techniques be difficult. Although this suggests the possibility of employing computational approaches to explore interfacial structures, modern molecular simulation methods suffer from an inability to simulate large interfacial systems in a sufficient time scale at the all-atom resolution. To develop a method capable of simulating solid-liquid interfaces, we have been developing a mean-field quantum mechanics/molecular mechanics (QM/MM) method. This Review briefly summarizes the theoretical background of mean-field QM/MM, as well as recent efforts to advance it. Furthermore, we summarize several studies performed based on this method.

Automated summary

Solid-liquid interfaces play a crucial role in various scientific and technological systems. However, the research on interfacial structures is still limited due to the difficulties in experimental techniques. Computational methods provide a possible solution, but current molecular simulation methods have limitations in simulating large interfacial systems. In order to overcome these limitations, a mean-field quantum mechanics/molecular mechanics (QM/MM) method has been developed.