Abstract
A systematic method is presented for determining the ground state of absorbed species on a substrate based on a cluster expansion of the configurational energy. It is shown that the method can determine the ground state of a strongly relaxing system using a few first-principles total energy calculations of small cells only. The method is applied to a particularly challenging case, the two-sided hydrogen chemisorption on a free standing graphene sheet, where, as a function of hydrogen coverage, the carbon hybridization goes from to The method should require still fewer calculations and yield still more accurate results in the case of physisorption where longer-ranged strain effects are less important.
- Received 20 April 2003
DOI:https://doi.org/10.1103/PhysRevB.68.085410
©2003 American Physical Society