Optical and magneto-optical properties of ferromagnetic monolayer CrBr 3 : A first-principles G W and G W plus Bethe-Salpeter equation study
Abstract
The discovery of atomically thin two-dimensional (2D) magnetic semiconductors has triggered enormous research interest recently. In this paper, we use first-principles many-body perturbation theory to study a prototypical 2D ferromagnetic semiconductor, monolayer chromium tribromide (CrBr3). With broken time-reversal symmetry, spin-orbit coupling, and excitonic effects included through the full-spinor GW and GW plus Bethe-Salpeter equation (GW-BSE) methods, we compute the frequency-dependent layer polarizability tensor and dielectric function tensor that govern the optical and magneto-optical (MO) properties. In addition, we provide a detailed theoretical formalism for simulating magnetic circular dichroism, MO Kerr effect, and Faraday effect, demonstrating the approach with monolayer CrBr3. Due to reduced dielectric screening in 2D and the localized nature of the Cr d orbitals, we find strong self-energy effects on the quasiparticle band structure of monolayer CrBr3 that give a 3.8 eV indirect bandgap. Also, excitonic effects dominate the low-energy optical and MO responses in monolayer CrBr3 where a large exciton binding energy of 2.3 eV is found for the lowest bright exciton state with excitation energy at 1.5 eV. We further find that the MO signals demonstrate strong dependence on the excitation frequency and substrate refractive index. Furthermore, our theoretical framework for modeling optical and MO effectsmore »
- Authors:
-
[1];
[1];
[1]
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), High Energy Physics (HEP); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1892024
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Materials
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 1; Journal ID: ISSN 2475-9953
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Electronic structure; Excitons; First-principles calculations; Magneto-optical effect; Quasiparticles & collective excitations; Spin-orbit coupling; Ferromagnets; Magnetic semiconductors; Monolayer films; Two-dimensional electron system; Bethe-Salpeter equation; Density functional theory; GW method
Citation Formats
Wu, Meng, Li, Zhenglu, and Louie, Steven G. Optical and magneto-optical properties of ferromagnetic monolayer CrBr3: A first-principles GW and GW plus Bethe-Salpeter equation study. United States: N. p., 2022.
Web. doi:10.1103/physrevmaterials.6.014008.
Wu, Meng, Li, Zhenglu, & Louie, Steven G. Optical and magneto-optical properties of ferromagnetic monolayer CrBr3: A first-principles GW and GW plus Bethe-Salpeter equation study. United States. https://doi.org/10.1103/physrevmaterials.6.014008
Wu, Meng, Li, Zhenglu, and Louie, Steven G. Wed .
"Optical and magneto-optical properties of ferromagnetic monolayer CrBr3: A first-principles GW and GW plus Bethe-Salpeter equation study". United States. https://doi.org/10.1103/physrevmaterials.6.014008. https://www.osti.gov/servlets/purl/1892024.
@article{osti_1892024,
title = {Optical and magneto-optical properties of ferromagnetic monolayer CrBr3: A first-principles GW and GW plus Bethe-Salpeter equation study},
author = {Wu, Meng and Li, Zhenglu and Louie, Steven G.},
abstractNote = {The discovery of atomically thin two-dimensional (2D) magnetic semiconductors has triggered enormous research interest recently. In this paper, we use first-principles many-body perturbation theory to study a prototypical 2D ferromagnetic semiconductor, monolayer chromium tribromide (CrBr3). With broken time-reversal symmetry, spin-orbit coupling, and excitonic effects included through the full-spinor GW and GW plus Bethe-Salpeter equation (GW-BSE) methods, we compute the frequency-dependent layer polarizability tensor and dielectric function tensor that govern the optical and magneto-optical (MO) properties. In addition, we provide a detailed theoretical formalism for simulating magnetic circular dichroism, MO Kerr effect, and Faraday effect, demonstrating the approach with monolayer CrBr3. Due to reduced dielectric screening in 2D and the localized nature of the Cr d orbitals, we find strong self-energy effects on the quasiparticle band structure of monolayer CrBr3 that give a 3.8 eV indirect bandgap. Also, excitonic effects dominate the low-energy optical and MO responses in monolayer CrBr3 where a large exciton binding energy of 2.3 eV is found for the lowest bright exciton state with excitation energy at 1.5 eV. We further find that the MO signals demonstrate strong dependence on the excitation frequency and substrate refractive index. Furthermore, our theoretical framework for modeling optical and MO effects could serve as a powerful theoretical tool for future study of optoelectronic and spintronics devices consisting of van der Waals 2D magnets.},
doi = {10.1103/physrevmaterials.6.014008},
journal = {Physical Review Materials},
number = 1,
volume = 6,
place = {United States},
year = {Wed Jan 26 00:00:00 EST 2022},
month = {Wed Jan 26 00:00:00 EST 2022}
}
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