Abstract
The evolution of the electronic structures of strongly correlated insulators with doping has long been a central fundamental question in condensed matter physics; it is also of great practical relevance for applications. We have studied the evolution of NiO under hole and electron doping at low doping levels such that the system remains insulating using high-quality thin film and a wide range of experimental and theoretical methods. The evolution is in both cases very smooth with dopant concentration. The band gap is asymmetric under electron and hole doping, consistent with a charge-transfer insulator picture, and is reduced faster under hole doping than under electron doping. For both electron and hole doping, occupied states are introduced at the top of the valence band. The formation of deep donor levels under electron doping and the inability to pin otherwise empty states near the conduction-band edge are indicative that local electron addition and removal energies are dominated by a Mott-like Hubbard U interaction even though the global band gap is predominantly a charge-transfer-type gap.
Original language | English |
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Article number | 195128 |
Journal | Physical Review B |
Volume | 101 |
Issue number | 19 |
DOIs | |
State | Published - May 15 2020 |
Funding
F.W, C.S., H.S, H.N.L., P.G., J.T.K., A.Be., P.R.C.K., O.H., and A.Bh. were supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, as part of the Computational Materials Sciences Program and Center for Predictive Simulation of Functional Materials. H.P. (DMFT calculations) was supported by US Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. C.S. was supported in part (optical analysis) by the Creative Materials Discovery Program through the National Research Foundation of Korea funded by Ministry of Science and ICT (Grant No. NRF-2017M3D1A1040828). An award of computer time was provided by the Innovative and Novel Computational Impact on Theory and Experiment program. This research used resources of the Argonne Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract No. DE-AC02-06CH11357. We gratefully acknowledge the computing resources provided on Bebop, a high-performance computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory. Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. This paper has been authored by UT-Battelle, LLC, under Contract No. DE-AC0500OR22725 with the US Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this paper, or allow others to do so, for US Government purposes. The US Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan . Data are available from the authors upon request. F.W,?C.S., H.S, H.N.L., P.G., J.T.K., A.Be., P.R.C.K., O.H., and A.Bh. were supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, as part of the Computational Materials Sciences Program and Center for Predictive Simulation of Functional Materials. H.P. (DMFT calculations) was supported by US Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. C.S. was supported in part (optical analysis) by the Creative Materials Discovery Program through the National Research Foundation of Korea funded by Ministry of Science and ICT (Grant No. NRF-2017M3D1A1040828). An award of computer time was provided by the Innovative and Novel Computational Impact on Theory and Experiment program. This research used resources of the Argonne Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract No. DE-AC02-06CH11357. We gratefully acknowledge the computing resources provided on Bebop, a high-performance computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory. Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. This paper has been authored by UT-Battelle, LLC, under Contract No. DE-AC0500OR22725 with the US Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this paper, or allow others to do so, for US Government purposes. The US Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan [48]. Data are available from the authors upon request.