Energy Decomposition Scheme for Rectangular Graphene Flakes

Abstract

We show—to our own surprise—that total electronic energies for a family of m × n rectangular graphene flakes can be very accurately represented by a simple function of the structural parameters m and n with errors not exceeding 1 kcal/mol. The energies of these flakes, usually referred to as multiple zigzag chains Z(m,n), are computed for m, n < 21 at their optimized geometries using the DFTB3 methodology. We have discovered that the structural parameters m and n (and their simple algebraic functions) provide a much better basis for the energy decomposition scheme than the various topological invariants usually used in this context. Most terms appearing in our energy decomposition scheme seem to have simple chemical interpretations. Our observation goes against the well-established knowledge stating that many-body energies are complicated functions of molecular parameters. Our observations might have far-reaching consequences for building accurate machine learning models.