We present systematic ab initio calculations of the charge carrier correlations between adjacent layers of two-dimensional materials in the presence of both charged impurity and strain disorder potentials using the examples of monolayer and bilayer graphene. For the first time, our analysis yields unambiguous first-principles quantum corrections to the Thomas-Fermi densities for interacting two-dimensional systems described by orbital-free density functional theory. Specifically, using density-potential functional theory, we find that quantum corrections to the quasi-classical Thomas-Fermi approximation have to be taken into account even for heterostructures of mesoscopic size. In order for the disorder-induced puddles of electrons and holes to be anti-correlated at zero average carrier density for both layers, the strength of the strain potential has to exceed that of the impurity potential by at least a factor of ten, with this number increasing for smaller impurity densities. Furthermore, our results show that quantum corrections have a larger impact on puddle correlations than exchange does, and they are necessary for properly predicting the experimentally observed Gaussian energy distribution at charge neutrality.
PhySH: Two-dimensional electron system, Density functional approximations, HeterostructuresThe most severe obstacle for OF-DFT in taking over as the workhorse of theoretical chemistry and materials science is the lack of accurate, reliable, systematic, and preferably universal quantum corrections to the quasi-classical TF approximation, in particular for the kinetic energy of low-dimensional systems [13][14][15]48,49 . While ad-hoc corrections to the quasiclassical limit and heuristic approximations are available for kinetic energy and particle density of low-dimensional systems 50,51 , successful derivations of systematic and consistent corrections are scarce 15,49,[52][53][54] . One promising route towards systematic orbital-free quantum corrections is provided by density-potential functional theory (DPFT) 15,49,54-57 , a more flexible reformulation of the original Hohenberg-Kohn DFT 4,58 , which circumvents the need for an explicit kineticenergy density-functional and provides natural ways for sys-arXiv:1902.02525v2 [cond-mat.mtrl-sci]