Introducing open boundary conditions in modeling nonperiodic materials and interfaces

Simulations are essential to accelerate the discovery of new materials. We introduce the first method of open boundary conditions in material and interface modeling. The new method, which we named ROBIN (recursive open boundary and interfaces) allows for discretizing millions of atoms in real space, thereby avoiding any symmetry or order of the atom distribution. The computational costs are limited to solving quantum properties in a focus area. It is verified in detail that the impact of the infinite environment on that area is included exactly. Calculations of graphene with the same amount of 1) periodic (currently available methods) and 2) randomly distributed silicon atoms shows that assuming periodicity elevates a small perturbation into a strong impact on the material property prediction. Graphene was confirmed to produce a band gap with periodic substitution of 3% carbon with silicon in agreement with published periodic boundary condition calculations. Instead, 3% randomly distributed silicon in graphene only shifts the energy spectrum. The predicted shift agrees quantitatively with published experimental data. Periodic boundary conditions can be applied on truly periodic systems only. Other systems should apply an open boundary method.