Electronic structure of chromium trihalides beyond density functional theory

Swagata Acharya; Dimitar Pashov; Brian Cunningham; Alexander N. Rudenko; Malte Rösner; Myrta Grüning; Mark van Schilfgaarde; Mikhail I. Katsnelson

doi:10.1103/PhysRevB.104.155109

Electronic structure of chromium trihalides beyond density functional theory

Swagata Acharya, Dimitar Pashov, Brian Cunningham, Alexander N. Rudenko, Malte Rösner, Myrta Grüning, Mark van Schilfgaarde, Mikhail I. Katsnelson

Research output: Contribution to journal › Article › peer-review

22 Citations (Scopus)

Abstract

We explore the electronic band structure of freestanding monolayers of chromium trihalides , = Cl, Br, I, within an advanced ab initio theoretical approach based on the use of Green's function functionals. We compare the local density approximation with the quasiparticle self-consistent GW (QSGW) approximation and its self-consistent extension by solving the particle-hole ladder Bethe-Salpeter equations to improve the effective interaction . We show that, at all levels of theory, the valence band consistently changes shape in the sequence , and the valence band maximum shifts from the point to the point. By analyzing the dynamic and momentum-dependent self-energy, we show that adds to the localization of the systems in comparison with QSGW, thereby leading to a narrower band and reduced amount of halogens in the valence band manifold. Further analysis shows that = Cl is most strongly correlated, and = I is least correlated (most bandlike) as the hybridization between Cr and enhances in the direction . For and , we observe remarkable differences between the QSGW and valence band structures, while their eigenfunctions are very similar. We show that weak perturbations, like moderate strain, weak changes to the hybridization, and adding small , can flip the valence band structures between these two solutions in these materials.

Original language	English
Article number	155109
Journal	Physical Review B
Volume	104
Issue number	15
DOIs	https://doi.org/10.1103/PhysRevB.104.155109
Publication status	Published - 15 Oct 2021

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10.1103/PhysRevB.104.155109

https://arxiv.org/abs/2106.06564

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@article{45ef3eda5ad048c7be307fd50d262c4f,

title = "Electronic structure of chromium trihalides beyond density functional theory",

abstract = "We explore the electronic band structure of freestanding monolayers of chromium trihalides , = Cl, Br, I, within an advanced ab initio theoretical approach based on the use of Green's function functionals. We compare the local density approximation with the quasiparticle self-consistent GW (QSGW) approximation and its self-consistent extension by solving the particle-hole ladder Bethe-Salpeter equations to improve the effective interaction . We show that, at all levels of theory, the valence band consistently changes shape in the sequence , and the valence band maximum shifts from the point to the point. By analyzing the dynamic and momentum-dependent self-energy, we show that adds to the localization of the systems in comparison with QSGW, thereby leading to a narrower band and reduced amount of halogens in the valence band manifold. Further analysis shows that = Cl is most strongly correlated, and = I is least correlated (most bandlike) as the hybridization between Cr and enhances in the direction . For and , we observe remarkable differences between the QSGW and valence band structures, while their eigenfunctions are very similar. We show that weak perturbations, like moderate strain, weak changes to the hybridization, and adding small , can flip the valence band structures between these two solutions in these materials.",

author = "Swagata Acharya and Dimitar Pashov and Brian Cunningham and Rudenko, {Alexander N.} and Malte R{\"o}sner and Myrta Gr{\"u}ning and {van Schilfgaarde}, Mark and Katsnelson, {Mikhail I.}",

note = "Funding Information: M.I.K., A.N.R., and S.A. are supported by the ERC Synergy Grant, Project No. 854843 FASTCORR (ultrafast dynamics of correlated electrons in solids). M.v.S. and D.P. are supported by the Simons Many-Electron Collaboration. We acknowledge PRACE for awarding us access to Irene-Rome hosted by TGCC, France, and Juwels Booster and Clusters, Germany; STFC Scientific Computing Department's SCARF cluster, Cambridge Tier-2 system operated by the University of Cambridge Research Computing Service funded by EPSRC Tier-2 capital Grant No. EP/P020259/1. M.v.S. was supported by DOE grant KC0310010-ERW7246. Funding Information: European Research Council Science and Technology Facilities Council University of Cambridge Research Computing Service Engineering and Physical Sciences Research Council U.S. Department of Energy Publisher Copyright: {\textcopyright} 2021 American Physical Society",

year = "2021",

month = oct,

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doi = "10.1103/PhysRevB.104.155109",

language = "English",

volume = "104",

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T1 - Electronic structure of chromium trihalides beyond density functional theory

AU - Acharya, Swagata

AU - Pashov, Dimitar

AU - Cunningham, Brian

AU - Rudenko, Alexander N.

AU - Rösner, Malte

AU - Grüning, Myrta

AU - van Schilfgaarde, Mark

AU - Katsnelson, Mikhail I.

N1 - Funding Information: M.I.K., A.N.R., and S.A. are supported by the ERC Synergy Grant, Project No. 854843 FASTCORR (ultrafast dynamics of correlated electrons in solids). M.v.S. and D.P. are supported by the Simons Many-Electron Collaboration. We acknowledge PRACE for awarding us access to Irene-Rome hosted by TGCC, France, and Juwels Booster and Clusters, Germany; STFC Scientific Computing Department's SCARF cluster, Cambridge Tier-2 system operated by the University of Cambridge Research Computing Service funded by EPSRC Tier-2 capital Grant No. EP/P020259/1. M.v.S. was supported by DOE grant KC0310010-ERW7246. Funding Information: European Research Council Science and Technology Facilities Council University of Cambridge Research Computing Service Engineering and Physical Sciences Research Council U.S. Department of Energy Publisher Copyright: © 2021 American Physical Society

PY - 2021/10/15

Y1 - 2021/10/15

N2 - We explore the electronic band structure of freestanding monolayers of chromium trihalides , = Cl, Br, I, within an advanced ab initio theoretical approach based on the use of Green's function functionals. We compare the local density approximation with the quasiparticle self-consistent GW (QSGW) approximation and its self-consistent extension by solving the particle-hole ladder Bethe-Salpeter equations to improve the effective interaction . We show that, at all levels of theory, the valence band consistently changes shape in the sequence , and the valence band maximum shifts from the point to the point. By analyzing the dynamic and momentum-dependent self-energy, we show that adds to the localization of the systems in comparison with QSGW, thereby leading to a narrower band and reduced amount of halogens in the valence band manifold. Further analysis shows that = Cl is most strongly correlated, and = I is least correlated (most bandlike) as the hybridization between Cr and enhances in the direction . For and , we observe remarkable differences between the QSGW and valence band structures, while their eigenfunctions are very similar. We show that weak perturbations, like moderate strain, weak changes to the hybridization, and adding small , can flip the valence band structures between these two solutions in these materials.

AB - We explore the electronic band structure of freestanding monolayers of chromium trihalides , = Cl, Br, I, within an advanced ab initio theoretical approach based on the use of Green's function functionals. We compare the local density approximation with the quasiparticle self-consistent GW (QSGW) approximation and its self-consistent extension by solving the particle-hole ladder Bethe-Salpeter equations to improve the effective interaction . We show that, at all levels of theory, the valence band consistently changes shape in the sequence , and the valence band maximum shifts from the point to the point. By analyzing the dynamic and momentum-dependent self-energy, we show that adds to the localization of the systems in comparison with QSGW, thereby leading to a narrower band and reduced amount of halogens in the valence band manifold. Further analysis shows that = Cl is most strongly correlated, and = I is least correlated (most bandlike) as the hybridization between Cr and enhances in the direction . For and , we observe remarkable differences between the QSGW and valence band structures, while their eigenfunctions are very similar. We show that weak perturbations, like moderate strain, weak changes to the hybridization, and adding small , can flip the valence band structures between these two solutions in these materials.

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DO - 10.1103/PhysRevB.104.155109

M3 - Article

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SN - 2469-9950

VL - 104

JO - Physical Review B

JF - Physical Review B

IS - 15

M1 - 155109

ER -

Electronic structure of chromium trihalides beyond density functional theory

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