Paramagnetic electronic structure of CrSBr: Comparison between ab initio G W theory and angle-resolved photoemission spectroscopy
- Aarhus Univ. (Denmark)
- National Renewable Energy Laboratory (NREL), Golden, CO (United States); Radboud Univ., Nijmegen (Netherlands)
- Technische Univ. Dresden (Germany)
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Kings College London (United Kingdom)
- University of Chemistry and Technology, Prague (Czech Republic)
- Radboud Univ., Nijmegen (Netherlands)
- Kings College London (United Kingdom); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Here, 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 (QS GW and QS $$G\widehat{W}$$, 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.
- Research Organization:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
- Grant/Contract Number:
- AC36-08GO28308; AC02-05CH11231
- OSTI ID:
- 1991207
- Report Number(s):
- NREL/JA-5F00-85865; MainId:86638; UUID:041e6302-3078-4827-8e98-985715460c0b; MainAdminID:69944; TRN: US2404017
- Journal Information:
- Physical Review. B, Vol. 107, Issue 23; ISSN 2469-9950
- Publisher:
- American Physical Society (APS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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SUPERCONDUCTIVITY AND SUPERFLUIDITY
angle-resolved photoemission spectroscopy
broken magnetic
Coulomb interaction
excitonic vertex corrections
paramagnetic CrSBr
quasiparticle self-consistent GW theory
supercell hosting spin configurations
electronic structure
layered crystals
magnetic insulators
GW method