A new reciprocal space based treatment of long range interactions on surfaces

A new formalism designed to treat long range interactions on surfaces, systems which are infinitely replicated in two spatial directions but have finite extent in the third, is developed. The new formalism is based in reciprocal space and, thus, permits the facile extension of standard plane-wave based density functional theory, Ewald summation, and smooth particle-mesh Ewald methods to handle surfaces efficiently. The method is tested on both model (body centered cubic lattices) and realistic problems (an ice surface with a defect and the 2×1 surface reconstruction of silicon) and found to be accurate, efficient, and a marked improvement on existing formulations in speed, accuracy, and utility.

[1]  M. Parrinello,et al.  Ab-Initio Molecular Dynamics: Principles and Practical Implementation , 1991 .

[2]  Mark E. Tuckerman,et al.  A reciprocal space based method for treating long range interactions in ab initio and force-field-based calculations in clusters , 1999 .

[3]  P. Hohenberg,et al.  Inhomogeneous Electron Gas , 1964 .

[4]  M. Dixon,et al.  Interionic potentials in alkali halides and their use in simulations of the molten salts , 1976 .

[5]  D. Remler,et al.  Molecular dynamics without effective potentials via the Car-Parrinello approach , 1990 .

[6]  Jim Glosli,et al.  Comments on P3M, FMM, and the Ewald method for large periodic Coulombic systems , 1996 .

[7]  Lee G. Pedersen,et al.  Long-range electrostatic effects in biomolecular simulations , 1997 .

[8]  M. Klein,et al.  An Ewald summation method for planar surfaces and interfaces , 1992 .

[9]  Parr,et al.  Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density. , 1988, Physical review. B, Condensed matter.

[10]  D. A. Dunnett.  Classical Electrodynamics , 2020, Nature.

[11]  M. Yin,et al.  Theoretical determination of surface atomic geometry: Si(001)-(2×1) , 1981 .

[12]  M. Klein,et al.  Quantum simulation studies of singlet and triplet bipolarons in liquid ammonia , 1993 .

[13]  Masuhiro Mikami,et al.  Rapid calculation of two-dimensional Ewald summation , 2001 .

[14]  G. Somorjai,et al.  Progress in our understanding of structure bonding and reactivity of metal surfaces and adsorbed monolayers at the molecular level: A 25 year perspective , 1995 .

[15]  R W Hockney,et al.  Computer Simulation Using Particles , 1966 .

[16]  S. Bent,et al.  Diels-Alder reactions of butadienes with the Si(100)-2×1 surface as a dienophile: Vibrational spectroscopy, thermal desorption and near edge x-ray absorption fine structure studies , 1998 .

[17]  J. Perram,et al.  Simulation of electrostatic systems in periodic boundary conditions. I. Lattice sums and dielectric constants , 1980, Proceedings of the Royal Society of London. A. Mathematical and Physical Sciences.

[18]  Arieh Warshel,et al.  The extended Ewald method: A general treatment of long‐range electrostatic interactions in microscopic simulations , 1988 .

[19]  W. Kohn,et al.  Self-Consistent Equations Including Exchange and Correlation Effects , 1965 .

[20]  Martins,et al.  Efficient pseudopotentials for plane-wave calculations. , 1991, Physical review. B, Condensed matter.

[21]  D. R. Hamann,et al.  Pseudopotentials that work: From H to Pu , 1982 .

[22]  Car,et al.  Unified approach for molecular dynamics and density-functional theory. , 1985, Physical review letters.

[23]  D. Heyes.  Molecular dynamics of ionic solid and liquid surfaces , 1984 .

[24]  A. Becke,et al.  Density-functional exchange-energy approximation with correct asymptotic behavior. , 1988, Physical review. A, General physics.

[25]  T. Darden,et al.  A smooth particle mesh Ewald method , 1995 .

[26]  G. Ciccotti,et al.  Non-Hamiltonian molecular dynamics: Generalizing Hamiltonian phase space principles to non-Hamiltonian systems , 2001 .