Calculations of point defect energetics with Density Functional Theory(DFT)can provide valuable insight into several optoelectronic,thermodynamic,and kinetic properties.These calculations commonly use methods ranging ...Calculations of point defect energetics with Density Functional Theory(DFT)can provide valuable insight into several optoelectronic,thermodynamic,and kinetic properties.These calculations commonly use methods ranging from semi-local functionals with a-posteriori corrections to more computationally intensive hybrid functional approaches.For applications of DFT-based high-throughput computation for data-driven materials discovery,point defect properties are of interest,yet are currently excluded from available materials databases.This work presents a benchmark analysis of automated,semi-local point defect calculations with a-posteriori corrections,compared to 245“gold standard”hybrid calculations previously published.We consider three different a-posteriori correction sets implemented in an automated workflow,and evaluate the qualitative and quantitative differences among four different categories of defect information:thermodynamic transition levels,formation energies,Fermi levels,and dopability limits.We highlight qualitative information that can be extracted from high-throughput calculations based on semi-local DFT methods,while also demonstrating the limits of quantitative accuracy.展开更多
基金This work was primarily funded by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences,Materials Sciences and Engineering Division under Contract No.DE-AC02-05-CH11231:Materials Project program KC23MPThis research used resources of the National Energy Research Scientific Computing Center,which is supported by the Office of Science of the U.S.Department of Energy under Contract No.DE-AC02-05-CH11231+1 种基金This work was partially performed under the auspices of the U.S.DOE by Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344DB would like to thank Chris G.Van de Walle,Nick Adamski,Andrew Rowberg,and Mark Turiansky along with all of the attendees of the 2018 Gordon Research Conference for Point Defects in Semiconductors for many constructive discussions on this paper’s topic.
文摘Calculations of point defect energetics with Density Functional Theory(DFT)can provide valuable insight into several optoelectronic,thermodynamic,and kinetic properties.These calculations commonly use methods ranging from semi-local functionals with a-posteriori corrections to more computationally intensive hybrid functional approaches.For applications of DFT-based high-throughput computation for data-driven materials discovery,point defect properties are of interest,yet are currently excluded from available materials databases.This work presents a benchmark analysis of automated,semi-local point defect calculations with a-posteriori corrections,compared to 245“gold standard”hybrid calculations previously published.We consider three different a-posteriori correction sets implemented in an automated workflow,and evaluate the qualitative and quantitative differences among four different categories of defect information:thermodynamic transition levels,formation energies,Fermi levels,and dopability limits.We highlight qualitative information that can be extracted from high-throughput calculations based on semi-local DFT methods,while also demonstrating the limits of quantitative accuracy.
