摘要
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.
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
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 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-AC02-05CH11231。
