Research output: Contribution to journal › Article › peer-review
Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Magnetic circular dichroism in the dd excitation in the van der Waals magnet CrI3 probed by resonant inelastic x-ray scattering
AU - Ghosh, Anirudha
AU - Jönsson, H. Johan M.
AU - Mukkattukavil, Deepak John
AU - Kvashnin, Yaroslav
AU - Phuyal, Dibya
AU - Thunström, Patrik
AU - Agåker, Marcus
AU - Nicolaou, Alessandro
AU - Jonak, Martin
AU - Klingeler, Rüdiger
AU - Kamalakar, M. Venkata
AU - Sarkar, Tapati
AU - Vasiliev, Alexander N.
AU - Butorin, Sergei M.
AU - Eriksson, Olle
AU - Abdel-Hafiez, Mahmoud
N1 - The authors would like to thank Håkan Rensmo for the fruitful discussions. A.G. and M.A.-H. acknowledge financial support from the Carl Tryggers Foundation and the Swedish Research Council (VR) under Project No. 2018-05393. D.J.M. acknowledges support from SSF Grant No. RIF14-0064. O.E. acknowledges financial support from the Knut and Alice Wallenberg Foundation, eSSENCE, the Swedish Research Council (VR), and the Foundation for Strategic Research (SSF). O.E. and P.T. acknowledge support from ERC synergy Grant No. 854843-FASTCORR. Y.K. acknowledges support from VR (Project No. 2019-03569) and the Göran Gustafsson Foundation. Support from the P220 program Project No. 075-15-2021-604 is acknowledged. The computations were enabled by resources provided by the Swedish National Infrastructure for Computing (SNIC) at the National Supercomputer Centre (NSC) partially funded by the Swedish Research Council through Grant Agreement No. 2018-05973. D.P. acknowledges support from the Swedish Research Council under Project No. 2020-00681. T.S. acknowledges financial support from the Swedish Research Council (VR Grants No. 2017-05030 and No. 2021-03675). M.H. acknowledges support by the European Union's Horizon 2020 Research and Innovation Programme, under Grant Agreement No. 824109 (European Microkelvin Platform). Work at Heidelberg has been supported by BMBF via the project SpinFun (13XP5088) and by Deutsche Forschungsgemeinschaft (DFG) under Germany's Excellence Strategy EXC2181/1-390900948 (the Heidelberg STRUCTURES Excellence Cluster). M.V.K. acknowledges support from ERC Grant No. 101002772-SPINNER.
PY - 2023
Y1 - 2023
N2 - We report on a combined experimental and theoretical study on CrI3 single crystals by employing the polarization dependence of resonant inelastic x-ray scattering (RIXS). Our investigations reveal multiple Cr 3d orbital splitting (dd excitations) as well as magnetic dichroism (MD) in the RIXS spectra. The dd excitation energies are similar on the two sides of the ferromagnetic transition temperature, TC∼61 K, although MD in RIXS is predominant at 0.4 T magnetic field below TC. This demonstrates that the ferromagnetic superexchange interaction that is responsible for the interatomic exchange field is vanishingly small compared with the local exchange field that comes from exchange and correlation interaction among the interacting Cr 3d orbitals. The recorded RIXS spectra reported here reveal clearly resolved Cr 3d intraorbital dd excitations that represent transitions between electronic levels that are heavily influenced by dynamic correlations and multiconfiguration effects. Our calculations taking into account the Cr 3d hybridization with the ligand valence states and the full multiplet structure due to intra-atomic and crystal field interactions in Oh and D3d symmetry clearly reproduced the dichroic trend in experimental RIXS spectra. © 2023 authors. Published by the American Physical Society. Published by the American Physical Society under the terms of the "https://creativecommons.org/licenses/by/4.0/"Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Funded by "https://www.kb.se/samverkan-och-utveckling/oppen-tillgang-och-bibsamkonsortiet/bibsamkonsortiet.html"Bibsam.
AB - We report on a combined experimental and theoretical study on CrI3 single crystals by employing the polarization dependence of resonant inelastic x-ray scattering (RIXS). Our investigations reveal multiple Cr 3d orbital splitting (dd excitations) as well as magnetic dichroism (MD) in the RIXS spectra. The dd excitation energies are similar on the two sides of the ferromagnetic transition temperature, TC∼61 K, although MD in RIXS is predominant at 0.4 T magnetic field below TC. This demonstrates that the ferromagnetic superexchange interaction that is responsible for the interatomic exchange field is vanishingly small compared with the local exchange field that comes from exchange and correlation interaction among the interacting Cr 3d orbitals. The recorded RIXS spectra reported here reveal clearly resolved Cr 3d intraorbital dd excitations that represent transitions between electronic levels that are heavily influenced by dynamic correlations and multiconfiguration effects. Our calculations taking into account the Cr 3d hybridization with the ligand valence states and the full multiplet structure due to intra-atomic and crystal field interactions in Oh and D3d symmetry clearly reproduced the dichroic trend in experimental RIXS spectra. © 2023 authors. Published by the American Physical Society. Published by the American Physical Society under the terms of the "https://creativecommons.org/licenses/by/4.0/"Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Funded by "https://www.kb.se/samverkan-och-utveckling/oppen-tillgang-och-bibsamkonsortiet/bibsamkonsortiet.html"Bibsam.
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U2 - 10.1103/PhysRevB.107.115148
DO - 10.1103/PhysRevB.107.115148
M3 - Article
VL - 107
JO - Physical Review B
JF - Physical Review B
SN - 2469-9950
IS - 11
M1 - 115148
ER -
ID: 37142201