Effects of basis set quality on the prediction of structures, energies, and properties of amorphous tetrahedral carbon

Peter A. Schultz, Ellen Stechel

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23 Citations (Scopus)

Abstract

We systematically investigate the effects of basis set quality on the prediction of a representative amorphous tetrahedral (a-tC) carbon structure. In fully self-consistent first-principles calculations, variations in the quality of the basis set do result in significant variations in predicted structure. Substantial differences between the calculations, ranging from a minimum basis to a high-quality double-zeta plus polarization (DZP) basis, for amorphous carbon stem from two sources. We discover that to properly relax candidate a-tC structures requires a high-quality basis set in the calculation. A minimum basis set is inadequate to negotiate the transition geometries involved in the making and breaking of bonds while relaxing a structure. Relaxation of an a-tC structure proposed by Drabold, Fedders, and Stumm [Phys. Rev. B 49, 16 415 (1994)] using a minimum, and a DZP basis demonstrates this point. The minimum basis set calculation leaves the bonding topology essentially unchanged, while relaxation using a DZP basis removes most of the small rings and triples the number of threefold bonded atoms. In addition, we find that to accurately represent the energetics of highly defected local structures, as found in a-tC, also requires a high-quality basis set. We demonstrate this point by using molecular analogs of local structures found in a-tC. Notable is how little rebonding and energy separates a-tC structures that have qualitatively different densities of threefold atoms.

Original languageEnglish
Pages (from-to)3295-3304
Number of pages10
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume57
Issue number6
Publication statusPublished - Feb 1 1998

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Amorphous carbon
carbon
Polarization
predictions
polarization
Atoms
energy
stems
Carbon
leaves
Topology
atoms
topology
Geometry
analogs
rings
geometry

ASJC Scopus subject areas

  • Condensed Matter Physics

Cite this

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abstract = "We systematically investigate the effects of basis set quality on the prediction of a representative amorphous tetrahedral (a-tC) carbon structure. In fully self-consistent first-principles calculations, variations in the quality of the basis set do result in significant variations in predicted structure. Substantial differences between the calculations, ranging from a minimum basis to a high-quality double-zeta plus polarization (DZP) basis, for amorphous carbon stem from two sources. We discover that to properly relax candidate a-tC structures requires a high-quality basis set in the calculation. A minimum basis set is inadequate to negotiate the transition geometries involved in the making and breaking of bonds while relaxing a structure. Relaxation of an a-tC structure proposed by Drabold, Fedders, and Stumm [Phys. Rev. B 49, 16 415 (1994)] using a minimum, and a DZP basis demonstrates this point. The minimum basis set calculation leaves the bonding topology essentially unchanged, while relaxation using a DZP basis removes most of the small rings and triples the number of threefold bonded atoms. In addition, we find that to accurately represent the energetics of highly defected local structures, as found in a-tC, also requires a high-quality basis set. We demonstrate this point by using molecular analogs of local structures found in a-tC. Notable is how little rebonding and energy separates a-tC structures that have qualitatively different densities of threefold atoms.",
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