Premium
A novel ab initio approach to problems of electronic structure calculations of the gas‐solid interface
Author(s) -
Fink William H.,
Butkus Aldona M.,
Lopez Jesus P.
Publication year - 2009
Publication title -
international journal of quantum chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.484
H-Index - 105
eISSN - 1097-461X
pISSN - 0020-7608
DOI - 10.1002/qua.560160834
Subject(s) - diamond , graphite , ab initio , electronic structure , wave function , lattice (music) , projection (relational algebra) , diamond cubic , convergence (economics) , materials science , computational chemistry , chemistry , physics , quantum mechanics , mathematics , algorithm , acoustics , economics , composite material , economic growth
A calculational procedure that permits the approximation of an infinite or semi‐infinite lattice by a finite cluster is described and applied to the surfaces of the allotropes of carbon—diamond and graphite. The Hartree‐Fock‐Roothaan equations are modified to permit a portion of the wave‐function to be fixed while other parts are variationally determined in the field generated by themselves and by the fixed part. A projection technique is developed to transfer a representation of the electronic structure of the variational part to the fixed part, and self‐defining cycles are followed to convergence. Recent results for diamond and graphite surfaces suggest that for a given finite size of cluster, the procedures result in a more uniform description of electron densities than does a straightforward SCF calculation.