Convergence of defect energetics calculations

Abstract

Determination of the chemical and spectroscopic natures of defects in materials such as hexagonal boron nitride (h-BN) remains a serious challenge for both experiment and theory. To establish basics needs for reliable calculations, we consider a model defect $V_N{N}_B$ in h-BN in which a boron-for-nitrogen substitution is accompanied by a nitrogen vacancy, examining its lowest-energy transition, (1)2B1 to (1)2A1. This provides a relatively simple test system as open-shell and charge-transfer effects, that are difficult to model and can dominate defect spectroscopy, are believed to be small. We establish calculation convergence with respect to sample size using both cluster and 2D-periodic models, convergence with respect to numerical issues such as use of plane-wave or Gaussian-basis-set expansions, and convergence with respect to the treatment of electron correlation. The results strongly suggest that poor performance of computational methods for defects of other natures arise through intrinsic methodological shortcomings.

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Cited by in corpus (6)

• First-principles identification of single photon emitters based on carbon clusters in hexagonal boron nitride
• Photoluminescence and photochemistry of the $V_B^{-}$ defect in hexagonal boron nitride
• Accurate prediction of the properties of materials using the CAM-B3LYP Density Functional
• Possible nanophotonics applications of the $V_N{N}_B$ defect in hexagonal boron nitride
• Density functionals with asymptotic-potential corrections are required for the simulation of spectroscopic properties of materials
• First-principles computational methods for quantum defects in two-dimensional materials: A perspective