The accurate modeling of adsorbates on periodic surfaces at low or intermediate coverages is computationally inefficient with current methodologies, typically requiring large unit cells to minimize unphysical intercell interactions. We propose novel composite methods that effectively cancel any unphysical adsorbate-adsorbate interactions that may otherwise be present in such slab calculations. Our composite approach provides a good description of the entire potential energy surface, and yields geometrical relaxations at low, intermediate and high coverages of adsorbates on small, computationally efficient unit cells. The methods are applied to investigate radical-initiated chain reactions as well as atomic layer deposition reactions on semiconductor surfaces. The foundations of the method, along with possible extensions and  performance will be discussed.

Novel composite methods for investigating structures and chemical reactions at semiconductor surfaces

246th National Meeting (2013)

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