First-principles Green's-function method for surface calculations: a pseudopotential localized basis set approach

摘要

We present an efficient implementation of a surface Green's-function methodfor atomistic modeling of surfaces within the framework of density functionaltheory using a pseudopotential localized basis set approach. In this method,the system is described as a truly semi-infinite solid with a surface regioncoupled to an electron reservoir, thereby overcoming several fundamentaldrawbacks of the traditional slab approach. The versatility of the method isdemonstrated with several applications to surface physics and chemistryproblems that are inherently difficult to address properly with the slabmethod, including metal work function calculations, band alignment in thin-filmsemiconductor heterostructures, surface states in metals and topologicalinsulators, and surfaces in external electrical fields. Results obtained withthe surface Green's-function method are compared to experimental measurementsand slab calculations to demonstrate the accuracy of the approach.