The Joint Automated Repository for Various Integrated Simulations(JARVIS)is an integrated infrastructure to accelerate materials discovery and design using density functional theory(DFT),classical force-fields(FF),and...The Joint Automated Repository for Various Integrated Simulations(JARVIS)is an integrated infrastructure to accelerate materials discovery and design using density functional theory(DFT),classical force-fields(FF),and machine learning(ML)techniques.JARVIS is motivated by the Materials Genome Initiative(MGI)principles of developing open-access databases and tools to reduce the cost and development time of materials discovery,optimization,and deployment.展开更多
For more than three decades,nearly free-electron elemental metals have been a topic of debate because the computed bandwidths are significantly wider in the local density approximation to density-functional theory(DFT...For more than three decades,nearly free-electron elemental metals have been a topic of debate because the computed bandwidths are significantly wider in the local density approximation to density-functional theory(DFT)than indicated by angle-resolved photoemission(ARPES)experiments.Here,we systematically investigate this using first principles calculations for alkali and alkaline-earth metals using DFT and various beyond-DFT methods such as meta-GGA,G0W0,hybrid functionals(YS-PBE0,B3LYP),and LDA+eDMFT.We find that the static non-local exchange,as partly included in the hybrid functionals,significantly increase the bandwidths even compared to LDA,while the G0W0 bands are only slightly narrower than in LDA.The agreement with the ARPES is best when the local approximation to the self-energy is used in the LDA+eDMFT method.We infer that even moderately correlated systems with partially occupied s orbitals,which were assumed to approximate the uniform electron gas,are very well described in terms of short-range dynamical correlations that are only local to an atom.展开更多
Various methods going beyond density functional theory(DFT),such as DFT+U,hybrid functionals,meta-GGAs,GW,and DFTembedded dynamical mean field theory(eDMFT),have been developed to describe the electronic structure of ...Various methods going beyond density functional theory(DFT),such as DFT+U,hybrid functionals,meta-GGAs,GW,and DFTembedded dynamical mean field theory(eDMFT),have been developed to describe the electronic structure of correlated materials,but it is unclear how accurate these methods can be expected to be when applied to a given strongly correlated solid.It is thus of pressing interest to compare their accuracy as they apply to different categories of materials.Here we introduce a novel paradigm in which a chosen set of beyond-DFT methods is systematically and uniformly tested on a chosen class of materials.For a first application,we choose the target materials to be the binary transition metal oxides FeO,CoO,MnO,and NiO in their antiferromagnetic phase and present a head-to-head comparison of spectral properties as computed using the various methods.We also compare with available experimental angle-resolved photoemission spectroscopy(ARPES),inverse-photoemission spectroscopy,and with optical absorption.For the class of compounds studied here,we find that both B3LYP and eDMFT reproduce the experiments quite well,with eDMFT doing best,in particular when comparing with the ARPES data.展开更多
基金K.C.thanks the computational support from XSEDE computational resources under allocation number TGDMR 190095Contributions from K.C.were supported by the financial assistance award 70NANB19H117 from the U.S.Department of Commerce,National Institute of Standards and Technology+3 种基金Contributions by S.M.,K.H.,K.R.,and D.V.were supported by NSF DMREF Grant No.DMR-1629059 and No.DMR-1629346X.Q.was supported by NSF Grant No.OAC-1835690A.A.acknowledges partial support by CHiMaD(NIST award#70NANB19H005)G.P.was supported by the Los Alamos National Laboratory’s Laboratory Directed Research and Development(LDRD)program’s Directed Research(DR)project#20200104DR。
文摘The Joint Automated Repository for Various Integrated Simulations(JARVIS)is an integrated infrastructure to accelerate materials discovery and design using density functional theory(DFT),classical force-fields(FF),and machine learning(ML)techniques.JARVIS is motivated by the Materials Genome Initiative(MGI)principles of developing open-access databases and tools to reduce the cost and development time of materials discovery,optimization,and deployment.
基金This research was funded by NSF DMREF DMR-1629059 and NSF DMREF DMR-1629346The computations were performed at the Frontera supercomputer at the Texas Advanced Computing Center(TACC)at The University of Texas at Austin,which is supported by National Science Foundation grant number OAC-1818253 and at the Extreme Science and Engineering Discovery Environment(XSEDE),which is supported by National Science Foundation grant number ACI-1548562.
文摘For more than three decades,nearly free-electron elemental metals have been a topic of debate because the computed bandwidths are significantly wider in the local density approximation to density-functional theory(DFT)than indicated by angle-resolved photoemission(ARPES)experiments.Here,we systematically investigate this using first principles calculations for alkali and alkaline-earth metals using DFT and various beyond-DFT methods such as meta-GGA,G0W0,hybrid functionals(YS-PBE0,B3LYP),and LDA+eDMFT.We find that the static non-local exchange,as partly included in the hybrid functionals,significantly increase the bandwidths even compared to LDA,while the G0W0 bands are only slightly narrower than in LDA.The agreement with the ARPES is best when the local approximation to the self-energy is used in the LDA+eDMFT method.We infer that even moderately correlated systems with partially occupied s orbitals,which were assumed to approximate the uniform electron gas,are very well described in terms of short-range dynamical correlations that are only local to an atom.
基金The computations were performed at the Extreme Science and Engineering Discovery Environment(XSEDE),which is supported by National Science Foundation grant number ACI-1548562,Rutgers HPC(RUPC)This research also used resources from the Rutgers Discovery Informatics Institute,75 which are supported by Rutgers and the State of New Jersey+1 种基金This research was funded by NSF DMREF DMR-1629059NSF DMREF DMR-1629346.
文摘Various methods going beyond density functional theory(DFT),such as DFT+U,hybrid functionals,meta-GGAs,GW,and DFTembedded dynamical mean field theory(eDMFT),have been developed to describe the electronic structure of correlated materials,but it is unclear how accurate these methods can be expected to be when applied to a given strongly correlated solid.It is thus of pressing interest to compare their accuracy as they apply to different categories of materials.Here we introduce a novel paradigm in which a chosen set of beyond-DFT methods is systematically and uniformly tested on a chosen class of materials.For a first application,we choose the target materials to be the binary transition metal oxides FeO,CoO,MnO,and NiO in their antiferromagnetic phase and present a head-to-head comparison of spectral properties as computed using the various methods.We also compare with available experimental angle-resolved photoemission spectroscopy(ARPES),inverse-photoemission spectroscopy,and with optical absorption.For the class of compounds studied here,we find that both B3LYP and eDMFT reproduce the experiments quite well,with eDMFT doing best,in particular when comparing with the ARPES data.
