Fundamental gap of fluorographene by many-body GW and fixed-node diffusion Monte Carlo methods
Abstract
Fluorographene (FG) is a promising graphene-derived material with a large bandgap. Currently existing predictions of its fundamental gap (Δf) and optical gap (Δopt) significantly vary when compared with experiment. We provide here an ultimate benchmark of Δf for FG by many-body GW and fixed-node diffusion Monte Carlo (FNDMC) methods. Both approaches independently arrive at Δf ≈ 7.1 ± 0.1 eV. In addition, the Bethe–Salpeter equation enabled us to determine the first exciton binding energy, Eb = 1.92 eV. We also point to the possible misinterpretation problem of the results obtained for gaps of solids by FNDMC with single-reference trial wave functions of Bloch orbitals. We argue why instead of Δopt, in the thermodynamic limit, such an approach results in energy differences that rather correspond to Δf, and we also outline conditions when this case actually applies.
- Authors:
-
[1];
[2];
[3];
[4]
- Univ. of Ostrava, Ostrava (Czech Republic). Faculty of Science. Dept. of Physics; Slovak Univ. of Technology in Bratislava, Trnava (Slovakia). Faculty of Materials Science and Technology in Trnava. ATRI
- Univ. of Ostrava, Ostrava (Czech Republic). Faculty of Science. Dept. of Physics
- Slovak Univ. of Technology in Bratislava, Trnava (Slovakia). Faculty of Materials Science and Technology in Trnava. ATRI
- North Carolina State Univ., Raleigh, NC (United States). Dept. of Physics and CHiPS
- Publication Date:
- Research Org.:
- North Carolina State University, Raleigh, NC (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; Czech Science Foundation; Slovak Research and Development Agency; European Regional Development Fund; USDOE
- OSTI Identifier:
- 1851609
- Alternate Identifier(s):
- OSTI ID: 1712504
- Grant/Contract Number:
- SC0012314; 18-25128S; 18-24321Y; APVV-18-0161; ITMS2014+:313011W085; de-sc0012314
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 153; Journal Issue: 18; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Chemistry; physics; quasiparticle; graphene; GW-approximation; Bethe-Salpeter equation; Monte Carlo methods; correlation energy; triplet state; excitonic effects
Citation Formats
Dubecký, Matúš, Karlický, František, Minárik, Stanislav, and Mitas, Lubos. Fundamental gap of fluorographene by many-body GW and fixed-node diffusion Monte Carlo methods. United States: N. p., 2020.
Web. doi:10.1063/5.0030952.
Dubecký, Matúš, Karlický, František, Minárik, Stanislav, & Mitas, Lubos. Fundamental gap of fluorographene by many-body GW and fixed-node diffusion Monte Carlo methods. United States. https://doi.org/10.1063/5.0030952
Dubecký, Matúš, Karlický, František, Minárik, Stanislav, and Mitas, Lubos. Sat .
"Fundamental gap of fluorographene by many-body GW and fixed-node diffusion Monte Carlo methods". United States. https://doi.org/10.1063/5.0030952. https://www.osti.gov/servlets/purl/1851609.
@article{osti_1851609,
title = {Fundamental gap of fluorographene by many-body GW and fixed-node diffusion Monte Carlo methods},
author = {Dubecký, Matúš and Karlický, František and Minárik, Stanislav and Mitas, Lubos},
abstractNote = {Fluorographene (FG) is a promising graphene-derived material with a large bandgap. Currently existing predictions of its fundamental gap (Δf) and optical gap (Δopt) significantly vary when compared with experiment. We provide here an ultimate benchmark of Δf for FG by many-body GW and fixed-node diffusion Monte Carlo (FNDMC) methods. Both approaches independently arrive at Δf ≈ 7.1 ± 0.1 eV. In addition, the Bethe–Salpeter equation enabled us to determine the first exciton binding energy, Eb = 1.92 eV. We also point to the possible misinterpretation problem of the results obtained for gaps of solids by FNDMC with single-reference trial wave functions of Bloch orbitals. We argue why instead of Δopt, in the thermodynamic limit, such an approach results in energy differences that rather correspond to Δf, and we also outline conditions when this case actually applies.},
doi = {10.1063/5.0030952},
journal = {Journal of Chemical Physics},
number = 18,
volume = 153,
place = {United States},
year = {Sat Nov 14 00:00:00 EST 2020},
month = {Sat Nov 14 00:00:00 EST 2020}
}
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