A theory for colors of strongly correlated electronic systems

Swagata Acharya; Dimitar Pashov; Cedric Weber; Mark van Schilfgaarde; Alexander I. Lichtenstein; Mikhail I. Katsnelson

doi:10.1038/s41467-023-41314-6

A theory for colors of strongly correlated electronic systems

Swagata Acharya^*, Dimitar Pashov, Cedric Weber, Mark van Schilfgaarde, Alexander I. Lichtenstein, Mikhail I. Katsnelson

^*Corresponding author for this work

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

7 Citations (Scopus)

Abstract

Many strongly correlated transition metal insulators are colored, even though they have band gaps much larger than the highest energy photons from the visible light. An adequate explanation for the color requires a theoretical approach able to compute subgap excitons in periodic crystals, reliably and without free parameters—a formidable challenge. The literature often fails to disentangle two important factors: what makes excitons form and what makes them optically bright. We pick two archetypal cases as examples: NiO with green color and MnF₂ with pink color, and employ two kinds of ab initio many body Green’s function theories; the first, a perturbative theory based on low-order extensions of the G W approximation, is able to explain the color in NiO, while the same theory is unable to explain why MnF₂ is pink. We show its color originates from higher order spin-flip transitions that modify the optical response, which is contained in dynamical mean-field theory (DMFT). We show that symmetry lowering mechanisms may determine how ‘bright’ these excitons are, but they are not fundamental to their existence.

Original language	English
Article number	5565
Journal	Nature Communications
Volume	14
Issue number	1
Early online date	9 Sept 2023
DOIs	https://doi.org/10.1038/s41467-023-41314-6
Publication status	Published - Dec 2023

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title = "A theory for colors of strongly correlated electronic systems",

abstract = "Many strongly correlated transition metal insulators are colored, even though they have band gaps much larger than the highest energy photons from the visible light. An adequate explanation for the color requires a theoretical approach able to compute subgap excitons in periodic crystals, reliably and without free parameters—a formidable challenge. The literature often fails to disentangle two important factors: what makes excitons form and what makes them optically bright. We pick two archetypal cases as examples: NiO with green color and MnF2 with pink color, and employ two kinds of ab initio many body Green{\textquoteright}s function theories; the first, a perturbative theory based on low-order extensions of the G W approximation, is able to explain the color in NiO, while the same theory is unable to explain why MnF2 is pink. We show its color originates from higher order spin-flip transitions that modify the optical response, which is contained in dynamical mean-field theory (DMFT). We show that symmetry lowering mechanisms may determine how {\textquoteleft}bright{\textquoteright} these excitons are, but they are not fundamental to their existence.",

author = "Swagata Acharya and Dimitar Pashov and Cedric Weber and {van Schilfgaarde}, Mark and Lichtenstein, {Alexander I.} and Katsnelson, {Mikhail I.}",

note = "Funding Information: M.I.K., A.I.L., and S.A. are supported by the ERC Synergy Grant, project 854843 FASTCORR (Ultrafast dynamics of correlated electrons in solids). M.vS., D.P., and S.A. (in the later stages of the work) 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. 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 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. This work was also partly carried out on the Dutch national e-infrastructure with the support of SURF Cooperative. Funding Information: M.I.K., A.I.L., and S.A. are supported by the ERC Synergy Grant, project 854843 FASTCORR (Ultrafast dynamics of correlated electrons in solids). M.vS., D.P., and S.A. (in the later stages of the work) 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. 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 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. This work was also partly carried out on the Dutch national e-infrastructure with the support of SURF Cooperative. Publisher Copyright: {\textcopyright} 2023, Springer Nature Limited.",

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doi = "10.1038/s41467-023-41314-6",

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T1 - A theory for colors of strongly correlated electronic systems

AU - Acharya, Swagata

AU - Pashov, Dimitar

AU - Weber, Cedric

AU - van Schilfgaarde, Mark

AU - Lichtenstein, Alexander I.

AU - Katsnelson, Mikhail I.

N1 - Funding Information: M.I.K., A.I.L., and S.A. are supported by the ERC Synergy Grant, project 854843 FASTCORR (Ultrafast dynamics of correlated electrons in solids). M.vS., D.P., and S.A. (in the later stages of the work) 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. 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 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. This work was also partly carried out on the Dutch national e-infrastructure with the support of SURF Cooperative. Funding Information: M.I.K., A.I.L., and S.A. are supported by the ERC Synergy Grant, project 854843 FASTCORR (Ultrafast dynamics of correlated electrons in solids). M.vS., D.P., and S.A. (in the later stages of the work) 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. 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 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. This work was also partly carried out on the Dutch national e-infrastructure with the support of SURF Cooperative. Publisher Copyright: © 2023, Springer Nature Limited.

PY - 2023/12

Y1 - 2023/12

N2 - Many strongly correlated transition metal insulators are colored, even though they have band gaps much larger than the highest energy photons from the visible light. An adequate explanation for the color requires a theoretical approach able to compute subgap excitons in periodic crystals, reliably and without free parameters—a formidable challenge. The literature often fails to disentangle two important factors: what makes excitons form and what makes them optically bright. We pick two archetypal cases as examples: NiO with green color and MnF2 with pink color, and employ two kinds of ab initio many body Green’s function theories; the first, a perturbative theory based on low-order extensions of the G W approximation, is able to explain the color in NiO, while the same theory is unable to explain why MnF2 is pink. We show its color originates from higher order spin-flip transitions that modify the optical response, which is contained in dynamical mean-field theory (DMFT). We show that symmetry lowering mechanisms may determine how ‘bright’ these excitons are, but they are not fundamental to their existence.

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A theory for colors of strongly correlated electronic systems

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