The role of electron correlations in the electronic structure of putative Chern magnet TbMn6Sn6

Abdulgani Annaberdiyev; Subhasish Mandal; Lubos Mitas; Jaron T. Krogel; Panchapakesan Ganesh

doi:10.1038/s41535-023-00583-6

The role of electron correlations in the electronic structure of putative Chern magnet TbMn₆Sn₆

Abdulgani Annaberdiyev, Subhasish Mandal, Lubos Mitas, Jaron T. Krogel, Panchapakesan Ganesh

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4 Scopus citations

Abstract

A member of the RMn₆Sn₆ rare-earth family materials, TbMn₆Sn₆, recently showed experimental signatures of the realization of a quantum-limit Chern magnet. In this work, we use quantum Monte Carlo (QMC) and density functional theory with Hubbard U (DFT + U) calculations to examine the electronic structure of TbMn₆Sn₆. To do so, we optimize accurate, correlation-consistent pseudopotentials for Tb and Sn using coupled-cluster and configuration–interaction (CI) methods. We find that DFT + U and single-reference QMC calculations suffer from the same overestimation of the magnetic moments as meta-GGA and hybrid density functional approximations. Our findings point to the need for improved orbitals/wavefunctions for this class of materials, such as natural orbitals from CI, or for the inclusion of multi-reference effects that capture the static correlations for an accurate prediction of magnetic properties. DFT + U with Mn magnetic moments adjusted to the experiment predict the Dirac crossing in bulk to be close to the Fermi level, within ~120 meV, in agreement with the experiments. Our non-stoichiometric slab calculations show that the Dirac crossing approaches even closer to the Fermi level, suggesting the possible realization of Chern magnetism in this limit.

Original language	English
Article number	50
Journal	npj Quantum Materials
Volume	8
Issue number	1
DOIs	https://doi.org/10.1038/s41535-023-00583-6
State	Published - Dec 2023

Funding

This work has been supported by the U.S. 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. An award for computer time was provided by the Innovative and Novel Computational Impact on Theory and Experiment (INCITE) program. This research used resources from the Oak Ridge Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract No. DE-AC05-00OR22725. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231. S.M. acknowledges the support from the Air Force Office of Scientific Research by the Department of Defense under the award number FA9550-23-1-0498 of the DEPSCoR program and 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 No. OAC-1818253. This paper describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the U.S. Department of Energy or the United States Government. Notice: This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains, and the publisher, by accepting the article for publication, acknowledges that the US 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. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). We thank P.R.C. Kent, Anand Bhattacharya, and Jeonghwan Ahn for reading the manuscript and providing helpful suggestions. This work has been supported by the U.S. 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. An award for computer time was provided by the Innovative and Novel Computational Impact on Theory and Experiment (INCITE) program. This research used resources from the Oak Ridge Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract No. DE-AC05-00OR22725. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231. S.M. acknowledges the support from the Air Force Office of Scientific Research by the Department of Defense under the award number FA9550-23-1-0498 of the DEPSCoR program and 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 No. OAC-1818253. This paper describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the U.S. Department of Energy or the United States Government. Notice: This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains, and the publisher, by accepting the article for publication, acknowledges that the US 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. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).

Funders	Funder number
DOE Public Access Plan
Texas Advanced Computing Center
National Science Foundation	OAC-1818253
U.S. Department of Defense	FA9550-23-1-0498
U.S. Department of Energy
Air Force Office of Scientific Research
Office of Science	DE-AC05-00OR22725
Basic Energy Sciences
Lawrence Berkeley National Laboratory	DE-AC02-05CH11231
University of Texas at Austin
Division of Materials Sciences and Engineering

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title = "The role of electron correlations in the electronic structure of putative Chern magnet TbMn6Sn6",

abstract = "A member of the RMn6Sn6 rare-earth family materials, TbMn6Sn6, recently showed experimental signatures of the realization of a quantum-limit Chern magnet. In this work, we use quantum Monte Carlo (QMC) and density functional theory with Hubbard U (DFT + U) calculations to examine the electronic structure of TbMn6Sn6. To do so, we optimize accurate, correlation-consistent pseudopotentials for Tb and Sn using coupled-cluster and configuration–interaction (CI) methods. We find that DFT + U and single-reference QMC calculations suffer from the same overestimation of the magnetic moments as meta-GGA and hybrid density functional approximations. Our findings point to the need for improved orbitals/wavefunctions for this class of materials, such as natural orbitals from CI, or for the inclusion of multi-reference effects that capture the static correlations for an accurate prediction of magnetic properties. DFT + U with Mn magnetic moments adjusted to the experiment predict the Dirac crossing in bulk to be close to the Fermi level, within ~120 meV, in agreement with the experiments. Our non-stoichiometric slab calculations show that the Dirac crossing approaches even closer to the Fermi level, suggesting the possible realization of Chern magnetism in this limit.",

author = "Abdulgani Annaberdiyev and Subhasish Mandal and Lubos Mitas and Krogel, {Jaron T.} and Panchapakesan Ganesh",

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AU - Annaberdiyev, Abdulgani

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AU - Mitas, Lubos

AU - Krogel, Jaron T.

AU - Ganesh, Panchapakesan

PY - 2023/12

Y1 - 2023/12

N2 - A member of the RMn6Sn6 rare-earth family materials, TbMn6Sn6, recently showed experimental signatures of the realization of a quantum-limit Chern magnet. In this work, we use quantum Monte Carlo (QMC) and density functional theory with Hubbard U (DFT + U) calculations to examine the electronic structure of TbMn6Sn6. To do so, we optimize accurate, correlation-consistent pseudopotentials for Tb and Sn using coupled-cluster and configuration–interaction (CI) methods. We find that DFT + U and single-reference QMC calculations suffer from the same overestimation of the magnetic moments as meta-GGA and hybrid density functional approximations. Our findings point to the need for improved orbitals/wavefunctions for this class of materials, such as natural orbitals from CI, or for the inclusion of multi-reference effects that capture the static correlations for an accurate prediction of magnetic properties. DFT + U with Mn magnetic moments adjusted to the experiment predict the Dirac crossing in bulk to be close to the Fermi level, within ~120 meV, in agreement with the experiments. Our non-stoichiometric slab calculations show that the Dirac crossing approaches even closer to the Fermi level, suggesting the possible realization of Chern magnetism in this limit.

AB - A member of the RMn6Sn6 rare-earth family materials, TbMn6Sn6, recently showed experimental signatures of the realization of a quantum-limit Chern magnet. In this work, we use quantum Monte Carlo (QMC) and density functional theory with Hubbard U (DFT + U) calculations to examine the electronic structure of TbMn6Sn6. To do so, we optimize accurate, correlation-consistent pseudopotentials for Tb and Sn using coupled-cluster and configuration–interaction (CI) methods. We find that DFT + U and single-reference QMC calculations suffer from the same overestimation of the magnetic moments as meta-GGA and hybrid density functional approximations. Our findings point to the need for improved orbitals/wavefunctions for this class of materials, such as natural orbitals from CI, or for the inclusion of multi-reference effects that capture the static correlations for an accurate prediction of magnetic properties. DFT + U with Mn magnetic moments adjusted to the experiment predict the Dirac crossing in bulk to be close to the Fermi level, within ~120 meV, in agreement with the experiments. Our non-stoichiometric slab calculations show that the Dirac crossing approaches even closer to the Fermi level, suggesting the possible realization of Chern magnetism in this limit.

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The role of electron correlations in the electronic structure of putative Chern magnet TbMn₆Sn₆

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