Paramagnetic electronic structure of CrSBr: Comparison between ab initio GW theory and angle-resolved photoemission spectroscopy

Marco Bianchi; Swagata Acharya; Florian Dirnberger; Julian Klein; Dimitar Pashov; Kseniia Mosina; Zdenek Sofer; Alexander N. Rudenko; Mikhail I. Katsnelson; Mark Van Schilfgaarde; Malte Rösner; Philip Hofmann

doi:10.1103/PhysRevB.107.235107

Paramagnetic electronic structure of CrSBr: Comparison between ab initio GW theory and angle-resolved photoemission spectroscopy

Marco Bianchi, Swagata Acharya, Florian Dirnberger, Julian Klein, Dimitar Pashov, Kseniia Mosina, Zdenek Sofer, Alexander N. Rudenko, Mikhail I. Katsnelson, Mark Van Schilfgaarde, Malte Rösner, Philip Hofmann

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Abstract

We explore the electronic structure of paramagnetic CrSBr by comparative first-principles calculations and angle-resolved photoemission spectroscopy. We theoretically approximate the paramagnetic phase using a supercell hosting spin configurations with broken long-range order and applying quasiparticle self-consistent GW theory, without and with the inclusion of excitonic vertex corrections to the screened Coulomb interaction (QSGW and QSGW, respectively). Comparing the quasiparticle band-structure calculations to angle-resolved photoemission data collected at 200 K results in excellent agreement. This allows us to qualitatively explain the significant broadening of some bands as arising from the broken magnetic long-range order and/or electronic dispersion perpendicular to the quasi-two-dimensional layers of the crystal structure. The experimental band gap at 200 K is found to be at least 1.51 eV at 200 K. At lower temperature, no photoemission data can be collected as a result of charging effects, pointing towards a significantly larger gap, which is consistent with the calculated band gap of approximately 2.1 eV.

Original language	English
Article number	235107
Journal	Physical Review B
Volume	107
Issue number	23
DOIs	https://doi.org/10.1103/PhysRevB.107.235107
Publication status	Published - 15 Jun 2023

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10.1103/PhysRevB.107.235107

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Bianchi, M., Acharya, S., Dirnberger, F., Klein, J., Pashov, D., Mosina, K., Sofer, Z., Rudenko, A. N., Katsnelson, M. I., Van Schilfgaarde, M., Rösner, M., & Hofmann, P. (2023). Paramagnetic electronic structure of CrSBr: Comparison between ab initio GW theory and angle-resolved photoemission spectroscopy. Physical Review B, 107(23), Article 235107. https://doi.org/10.1103/PhysRevB.107.235107

@article{747f830ab8db47629563cd66aaa91be2,

title = "Paramagnetic electronic structure of CrSBr: Comparison between ab initio GW theory and angle-resolved photoemission spectroscopy",

abstract = "We explore the electronic structure of paramagnetic CrSBr by comparative first-principles calculations and angle-resolved photoemission spectroscopy. We theoretically approximate the paramagnetic phase using a supercell hosting spin configurations with broken long-range order and applying quasiparticle self-consistent GW theory, without and with the inclusion of excitonic vertex corrections to the screened Coulomb interaction (QSGW and QSGW, respectively). Comparing the quasiparticle band-structure calculations to angle-resolved photoemission data collected at 200 K results in excellent agreement. This allows us to qualitatively explain the significant broadening of some bands as arising from the broken magnetic long-range order and/or electronic dispersion perpendicular to the quasi-two-dimensional layers of the crystal structure. The experimental band gap at 200 K is found to be at least 1.51 eV at 200 K. At lower temperature, no photoemission data can be collected as a result of charging effects, pointing towards a significantly larger gap, which is consistent with the calculated band gap of approximately 2.1 eV.",

author = "Marco Bianchi and Swagata Acharya and Florian Dirnberger and Julian Klein and Dimitar Pashov and Kseniia Mosina and Zdenek Sofer and Rudenko, {Alexander N.} and Katsnelson, {Mikhail I.} and {Van Schilfgaarde}, Mark and Malte R{\"o}sner and Philip Hofmann",

note = "Funding Information: This work was supported by VILLUM FONDEN via the Centre of Excellence for Dirac Materials (Grant No. 11744) and the Independent Research Fund Denmark (Grant No. 1026-00089B). M.R. and M.I.K. acknowledge the research program Materials for the Quantum Age (QuMat) for financial support. This program (registration number 024.005.006) is part of the Gravitation program financed by the Dutch Ministry of Education, Culture and Science (OCW). Z.S. was supported by ERC-CZ program (Project No. LL2101) from the Ministry of Education Youth and Sports (MEYS). M.v.S., S.A., and D.P. were supported by the Computational Chemical Sciences program within the Office of Basic Energy Sciences, U.S. Department of Energy under Contract No. DE-AC36-08GO28308. F.D. was supported by the W{\"u}rzburg-Dresden Cluster of Excellence on Complexity and Topology in Quantum Matter ct.qmat (EXC 2147, ProjectID 390858490). M.I.K. and S.A. are supported by the ERC Synergy Grant, Project No. 854843 FASTCORR (Ultrafast dynamics of correlated electrons in solids). 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 using NERSC Award No. BES-ERCAP0021783. S.A. and M.I.K. acknowledge PRACE for awarding us access to Irene-Rome hosted by TGCC, France and Juwels Booster and Cluster, Germany. Publisher Copyright: {\textcopyright} 2023 American Physical Society.",

year = "2023",

month = jun,

day = "15",

doi = "10.1103/PhysRevB.107.235107",

language = "English",

volume = "107",

journal = "Physical Review B",

issn = "2469-9950",

publisher = "American Physical Society",

number = "23",

}

Bianchi, M, Acharya, S, Dirnberger, F, Klein, J, Pashov, D, Mosina, K, Sofer, Z, Rudenko, AN, Katsnelson, MI, Van Schilfgaarde, M, Rösner, M & Hofmann, P 2023, 'Paramagnetic electronic structure of CrSBr: Comparison between ab initio GW theory and angle-resolved photoemission spectroscopy', Physical Review B, vol. 107, no. 23, 235107. https://doi.org/10.1103/PhysRevB.107.235107

TY - JOUR

T1 - Paramagnetic electronic structure of CrSBr

T2 - Comparison between ab initio GW theory and angle-resolved photoemission spectroscopy

AU - Bianchi, Marco

AU - Acharya, Swagata

AU - Dirnberger, Florian

AU - Klein, Julian

AU - Pashov, Dimitar

AU - Mosina, Kseniia

AU - Sofer, Zdenek

AU - Rudenko, Alexander N.

AU - Katsnelson, Mikhail I.

AU - Van Schilfgaarde, Mark

AU - Rösner, Malte

AU - Hofmann, Philip

N1 - Funding Information: This work was supported by VILLUM FONDEN via the Centre of Excellence for Dirac Materials (Grant No. 11744) and the Independent Research Fund Denmark (Grant No. 1026-00089B). M.R. and M.I.K. acknowledge the research program Materials for the Quantum Age (QuMat) for financial support. This program (registration number 024.005.006) is part of the Gravitation program financed by the Dutch Ministry of Education, Culture and Science (OCW). Z.S. was supported by ERC-CZ program (Project No. LL2101) from the Ministry of Education Youth and Sports (MEYS). M.v.S., S.A., and D.P. were supported by the Computational Chemical Sciences program within the Office of Basic Energy Sciences, U.S. Department of Energy under Contract No. DE-AC36-08GO28308. F.D. was supported by the Würzburg-Dresden Cluster of Excellence on Complexity and Topology in Quantum Matter ct.qmat (EXC 2147, ProjectID 390858490). M.I.K. and S.A. are supported by the ERC Synergy Grant, Project No. 854843 FASTCORR (Ultrafast dynamics of correlated electrons in solids). 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 using NERSC Award No. BES-ERCAP0021783. S.A. and M.I.K. acknowledge PRACE for awarding us access to Irene-Rome hosted by TGCC, France and Juwels Booster and Cluster, Germany. Publisher Copyright: © 2023 American Physical Society.

PY - 2023/6/15

Y1 - 2023/6/15

N2 - We explore the electronic structure of paramagnetic CrSBr by comparative first-principles calculations and angle-resolved photoemission spectroscopy. We theoretically approximate the paramagnetic phase using a supercell hosting spin configurations with broken long-range order and applying quasiparticle self-consistent GW theory, without and with the inclusion of excitonic vertex corrections to the screened Coulomb interaction (QSGW and QSGW, respectively). Comparing the quasiparticle band-structure calculations to angle-resolved photoemission data collected at 200 K results in excellent agreement. This allows us to qualitatively explain the significant broadening of some bands as arising from the broken magnetic long-range order and/or electronic dispersion perpendicular to the quasi-two-dimensional layers of the crystal structure. The experimental band gap at 200 K is found to be at least 1.51 eV at 200 K. At lower temperature, no photoemission data can be collected as a result of charging effects, pointing towards a significantly larger gap, which is consistent with the calculated band gap of approximately 2.1 eV.

AB - We explore the electronic structure of paramagnetic CrSBr by comparative first-principles calculations and angle-resolved photoemission spectroscopy. We theoretically approximate the paramagnetic phase using a supercell hosting spin configurations with broken long-range order and applying quasiparticle self-consistent GW theory, without and with the inclusion of excitonic vertex corrections to the screened Coulomb interaction (QSGW and QSGW, respectively). Comparing the quasiparticle band-structure calculations to angle-resolved photoemission data collected at 200 K results in excellent agreement. This allows us to qualitatively explain the significant broadening of some bands as arising from the broken magnetic long-range order and/or electronic dispersion perpendicular to the quasi-two-dimensional layers of the crystal structure. The experimental band gap at 200 K is found to be at least 1.51 eV at 200 K. At lower temperature, no photoemission data can be collected as a result of charging effects, pointing towards a significantly larger gap, which is consistent with the calculated band gap of approximately 2.1 eV.

UR - http://www.scopus.com/inward/record.url?scp=85163285064&partnerID=8YFLogxK

U2 - 10.1103/PhysRevB.107.235107

DO - 10.1103/PhysRevB.107.235107

M3 - Article

AN - SCOPUS:85163285064

SN - 2469-9950

VL - 107

JO - Physical Review B

JF - Physical Review B

IS - 23

M1 - 235107

ER -

Paramagnetic electronic structure of CrSBr: Comparison between ab initio GW theory and angle-resolved photoemission spectroscopy

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