Weinvestigate the atomic and electronic structures of ferroelectric perovskite oxides,BaTiO_(3),PbTiO_(3),LiNbO_(3),and BiFeO_(3) using ab initio extended Hubbard functionals(DFT+U+V),where on-site and inter-site Hubb...Weinvestigate the atomic and electronic structures of ferroelectric perovskite oxides,BaTiO_(3),PbTiO_(3),LiNbO_(3),and BiFeO_(3) using ab initio extended Hubbard functionals(DFT+U+V),where on-site and inter-site Hubbard parameters are self-consistently determined via a pseudohybrid density functional by Agapito-Curtarolo-Buongiorno Nardelli.We compute band structures,ferroelectric distortions,polarization,Born effective charges,and switching barriers,compared with local density approximation,generalized gradient approximation(GGA),meta-GGA,and hybrid(HSE06)functionals.Results from DFT+U+V closely match experimental data,with the inter-site Hubbard terms significantly increasing band gaps,making closer alignment with GWresults.The crucial role of the inter-site Coulomb interactions,restoring polar distortions suppressed by on-site U is discussed.Our approach yields accuracy comparable to HSE06 at over an order-of-magnitude lower computational cost.This combination of accuracy and efficiency makes DFT+U+V well suited for high-throughput calculations and properties such as bulk photovoltaic effect and band alignments of ferroelectric heterostructures.展开更多
基金supported by the National Research Foundation of Korea(NRF) grant funded by the Korea government(MSIT) (No. RS-2024-00358551)by the Basic Science Research Program through the National Research Foundation of Korea(NRF) funded by the Ministry of Education (No. RS-2021-NR060129)+2 种基金S.Y.P. and M.C.C. were supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF) funded by the Ministry of Education (No. RS-2021-NR060140)Y.-W.S. was supported by KIAS individual Grant (No. CG031509)W.Y. was supported by KIAS individual Grant (No. QP090102). Computations were also supported by the CAC of KIAS.
文摘Weinvestigate the atomic and electronic structures of ferroelectric perovskite oxides,BaTiO_(3),PbTiO_(3),LiNbO_(3),and BiFeO_(3) using ab initio extended Hubbard functionals(DFT+U+V),where on-site and inter-site Hubbard parameters are self-consistently determined via a pseudohybrid density functional by Agapito-Curtarolo-Buongiorno Nardelli.We compute band structures,ferroelectric distortions,polarization,Born effective charges,and switching barriers,compared with local density approximation,generalized gradient approximation(GGA),meta-GGA,and hybrid(HSE06)functionals.Results from DFT+U+V closely match experimental data,with the inter-site Hubbard terms significantly increasing band gaps,making closer alignment with GWresults.The crucial role of the inter-site Coulomb interactions,restoring polar distortions suppressed by on-site U is discussed.Our approach yields accuracy comparable to HSE06 at over an order-of-magnitude lower computational cost.This combination of accuracy and efficiency makes DFT+U+V well suited for high-throughput calculations and properties such as bulk photovoltaic effect and band alignments of ferroelectric heterostructures.
