We develop an open-source python workflow package,pyGWBSE to perform automated first-principles calculations within the GW-BSE(Bethe-Salpeter)framework.GW-BSE is a many body perturbation theory based approach to explo...We develop an open-source python workflow package,pyGWBSE to perform automated first-principles calculations within the GW-BSE(Bethe-Salpeter)framework.GW-BSE is a many body perturbation theory based approach to explore the quasiparticle(QP)and excitonic properties of materials.GW approximation accurately predicts bandgaps of materials by overcoming the bandgap underestimation issue of the more widely used density functional theory(DFT).BSE formalism produces absorption spectra directly comparable with experimental observations.pyGWBSE package achieves complete automation of the entire multi-step GW-BSE computation,including the convergence tests of several parameters that are crucial for the accuracy of these calculations.pyGWBSE is integrated with Wannier90,to generate QP bandstructures,interpolated using the maximally-localized wannier functions.pyGWBSE also enables the automated creation of databases of metadata and data,including QP and excitonic properties,which can be extremely useful for future material discovery studies in the field of ultra-wide bandgap semiconductors,electronics,photovoltaics,and photocatalysis.展开更多
The formation and disassociation of excitons play a crucial role in any photovoltaic or photocatalytic application.However,excitonic effects are seldom considered in materials discovery studies due to the monumental c...The formation and disassociation of excitons play a crucial role in any photovoltaic or photocatalytic application.However,excitonic effects are seldom considered in materials discovery studies due to the monumental computational cost associated with the examination of these properties.Here,we study the excitonic properties of nearly 50 photocatalysts using state-of-the-art Bethe–Salpeter formalism.These~50 materials were recently recognized as promising photocatalysts for CO_(2) reduction through a data-driven screening of 68,860 materials.Here,we propose three screening criteria based on the optical properties of these materials,taking excitonic effects into account,to further down select six materials.Furthermore,we study the correlation between the exciton binding energies obtained from the Bethe–Salpeter formalism and those obtained from the computationally much lessexpensive Wannier–Mott model for these chemically diverse~50 materials.This work presents a paradigm towards the inclusion of excitonic effects in future materials discovery for solar-energy harvesting applications.展开更多
基金This work was supported by ULTRA,an Energy Frontier Research Center funded by the U.S.Department of Energy(DOE),Office of Science,Basic Energy Sciences(BES),under Award#DE-SC0021230In addition,Singh acknowledges support by the Arizona State University start-up funds.The authors acknowledge the San Diego Supercomputer Center under the NSF-XSEDE Award No.DMR150006+1 种基金the Research Computing at Arizona State University for providing HPC resources.This research used resources of the National Energy Research Scientific Computing Center,a DOE Office of Science User Facility supported by the Office of Science of the U.S.Department of Energy under Contract No.DE-AC02-05CH11231The authors also thank Tara M.Boland,Adway Gupta,Akash Patel,and Cody Milne for testing the code and for helpful discussions.
文摘We develop an open-source python workflow package,pyGWBSE to perform automated first-principles calculations within the GW-BSE(Bethe-Salpeter)framework.GW-BSE is a many body perturbation theory based approach to explore the quasiparticle(QP)and excitonic properties of materials.GW approximation accurately predicts bandgaps of materials by overcoming the bandgap underestimation issue of the more widely used density functional theory(DFT).BSE formalism produces absorption spectra directly comparable with experimental observations.pyGWBSE package achieves complete automation of the entire multi-step GW-BSE computation,including the convergence tests of several parameters that are crucial for the accuracy of these calculations.pyGWBSE is integrated with Wannier90,to generate QP bandstructures,interpolated using the maximally-localized wannier functions.pyGWBSE also enables the automated creation of databases of metadata and data,including QP and excitonic properties,which can be extremely useful for future material discovery studies in the field of ultra-wide bandgap semiconductors,electronics,photovoltaics,and photocatalysis.
基金This work was supported by the Arizona State University start-up funds and in part as part of ULTRA,an Energy Frontier Research Center funded by the U.S.Department of Energy(DOE),Office of Science,Basic Energy Sciences(BES),under Award#DESC0021230(GW-BSE high-throughput simulations)In addition,Singh acknowledges support by the NSF DMR-grant NSF-DMR#1906030+1 种基金The authors acknowledge the San Diego Supercomputer Center under the NSF-XSEDE Award No.DMR150006 and the Research Computing at Arizona State University for providing HPC resourcesThis research used resources of the National Energy Research Scientific Computing Center,a DOE Office of Science User Facility supported by the Office of Science of the U.S.Department of Energy under Contract No.DE-AC02-05CH11231。
文摘The formation and disassociation of excitons play a crucial role in any photovoltaic or photocatalytic application.However,excitonic effects are seldom considered in materials discovery studies due to the monumental computational cost associated with the examination of these properties.Here,we study the excitonic properties of nearly 50 photocatalysts using state-of-the-art Bethe–Salpeter formalism.These~50 materials were recently recognized as promising photocatalysts for CO_(2) reduction through a data-driven screening of 68,860 materials.Here,we propose three screening criteria based on the optical properties of these materials,taking excitonic effects into account,to further down select six materials.Furthermore,we study the correlation between the exciton binding energies obtained from the Bethe–Salpeter formalism and those obtained from the computationally much lessexpensive Wannier–Mott model for these chemically diverse~50 materials.This work presents a paradigm towards the inclusion of excitonic effects in future materials discovery for solar-energy harvesting applications.