Covalent mixing in the two-dimensional ferromagnet CrSiTe₃ evidenced by magnetic x-ray circular dichroism

<p>The low-temperature electronic structure of the van der Waals ferromagnet CrSiTe3 has been investigated. This ferromagnetic semiconductor has a magnetic bulk transition temperature of 33 K, which can reach up to 80 K in single- and few-layer flakes. X-ray absorption spectroscopy (XAS) and x...

Full description

Bibliographic Details
Main Authors: Achinuq, B, Fujita, R, Xia, W, Guo, Y, Bencok, P, van der Laan, G, Hesjedal, T
Format: Journal article
Language:English
Published: Wiley 2021
_version_ 1826307941602426880
author Achinuq, B
Fujita, R
Xia, W
Guo, Y
Bencok, P
van der Laan, G
Hesjedal, T
author_facet Achinuq, B
Fujita, R
Xia, W
Guo, Y
Bencok, P
van der Laan, G
Hesjedal, T
author_sort Achinuq, B
collection OXFORD
description <p>The low-temperature electronic structure of the van der Waals ferromagnet CrSiTe3 has been investigated. This ferromagnetic semiconductor has a magnetic bulk transition temperature of 33 K, which can reach up to 80 K in single- and few-layer flakes. X-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) measurements, carried out at the Cr&nbsp;<em>L</em><sub>2,3</sub>&nbsp;and Te&nbsp;<em>M</em><sub>b</sub>&nbsp;edges on in vacuo cleaved single crystals, give strong evidence for hybridization-mediated super-exchange between the Cr atoms. The observed chemical shift in the XAS, as well as the comparison of the XMCD with the calculated Cr L<sub>2,3</sub>&nbsp;multiplet spectra, confirm a strongly covalent bond between the Cr&nbsp;<em>3d</em>(<em>e</em><sub>g</sub>) and Te 5<em>p</em>&nbsp;states. Application of the XMCD sum rules gives a non-vanishing orbital moment, supporting a partial occupation of the&nbsp;<em>e<sub>g</sub></em>&nbsp;states, apart from the&nbsp;<em>t</em><sub>2<em>g</em></sub>. Also, the presence of a non-zero XMCD signal at the Te Mb edge confirms a Te 5<em>p</em>&nbsp;spin polarization due to mixing with the Cr&nbsp;<em>e<sub>g</sub></em>&nbsp;bonding states. The results strongly suggest that superexchange, instead of the previously suggested single ion anisotropy, is responsible for the low-temperature ferromagnetic ordering of 2D materials such as CrSiTe<sub>3</sub>&nbsp;and CrGeTe<sub>3</sub>. This demonstrates the interplay between electron correlation and ferromagnetism in insulating two-dimensional materials.</p>
first_indexed 2024-03-07T07:10:43Z
format Journal article
id oxford-uuid:5f2eaf0e-d2fa-49ae-9bfe-1e2f320dd530
institution University of Oxford
language English
last_indexed 2024-03-07T07:10:43Z
publishDate 2021
publisher Wiley
record_format dspace
spelling oxford-uuid:5f2eaf0e-d2fa-49ae-9bfe-1e2f320dd5302022-06-22T11:53:08ZCovalent mixing in the two-dimensional ferromagnet CrSiTe₃ evidenced by magnetic x-ray circular dichroismJournal articlehttp://purl.org/coar/resource_type/c_545buuid:5f2eaf0e-d2fa-49ae-9bfe-1e2f320dd530EnglishSymplectic ElementsWiley2021Achinuq, BFujita, RXia, WGuo, YBencok, Pvan der Laan, GHesjedal, T<p>The low-temperature electronic structure of the van der Waals ferromagnet CrSiTe3 has been investigated. This ferromagnetic semiconductor has a magnetic bulk transition temperature of 33 K, which can reach up to 80 K in single- and few-layer flakes. X-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) measurements, carried out at the Cr&nbsp;<em>L</em><sub>2,3</sub>&nbsp;and Te&nbsp;<em>M</em><sub>b</sub>&nbsp;edges on in vacuo cleaved single crystals, give strong evidence for hybridization-mediated super-exchange between the Cr atoms. The observed chemical shift in the XAS, as well as the comparison of the XMCD with the calculated Cr L<sub>2,3</sub>&nbsp;multiplet spectra, confirm a strongly covalent bond between the Cr&nbsp;<em>3d</em>(<em>e</em><sub>g</sub>) and Te 5<em>p</em>&nbsp;states. Application of the XMCD sum rules gives a non-vanishing orbital moment, supporting a partial occupation of the&nbsp;<em>e<sub>g</sub></em>&nbsp;states, apart from the&nbsp;<em>t</em><sub>2<em>g</em></sub>. Also, the presence of a non-zero XMCD signal at the Te Mb edge confirms a Te 5<em>p</em>&nbsp;spin polarization due to mixing with the Cr&nbsp;<em>e<sub>g</sub></em>&nbsp;bonding states. The results strongly suggest that superexchange, instead of the previously suggested single ion anisotropy, is responsible for the low-temperature ferromagnetic ordering of 2D materials such as CrSiTe<sub>3</sub>&nbsp;and CrGeTe<sub>3</sub>. This demonstrates the interplay between electron correlation and ferromagnetism in insulating two-dimensional materials.</p>
spellingShingle Achinuq, B
Fujita, R
Xia, W
Guo, Y
Bencok, P
van der Laan, G
Hesjedal, T
Covalent mixing in the two-dimensional ferromagnet CrSiTe₃ evidenced by magnetic x-ray circular dichroism
title Covalent mixing in the two-dimensional ferromagnet CrSiTe₃ evidenced by magnetic x-ray circular dichroism
title_full Covalent mixing in the two-dimensional ferromagnet CrSiTe₃ evidenced by magnetic x-ray circular dichroism
title_fullStr Covalent mixing in the two-dimensional ferromagnet CrSiTe₃ evidenced by magnetic x-ray circular dichroism
title_full_unstemmed Covalent mixing in the two-dimensional ferromagnet CrSiTe₃ evidenced by magnetic x-ray circular dichroism
title_short Covalent mixing in the two-dimensional ferromagnet CrSiTe₃ evidenced by magnetic x-ray circular dichroism
title_sort covalent mixing in the two dimensional ferromagnet crsite₃ evidenced by magnetic x ray circular dichroism
work_keys_str_mv AT achinuqb covalentmixinginthetwodimensionalferromagnetcrsite3evidencedbymagneticxraycirculardichroism
AT fujitar covalentmixinginthetwodimensionalferromagnetcrsite3evidencedbymagneticxraycirculardichroism
AT xiaw covalentmixinginthetwodimensionalferromagnetcrsite3evidencedbymagneticxraycirculardichroism
AT guoy covalentmixinginthetwodimensionalferromagnetcrsite3evidencedbymagneticxraycirculardichroism
AT bencokp covalentmixinginthetwodimensionalferromagnetcrsite3evidencedbymagneticxraycirculardichroism
AT vanderlaang covalentmixinginthetwodimensionalferromagnetcrsite3evidencedbymagneticxraycirculardichroism
AT hesjedalt covalentmixinginthetwodimensionalferromagnetcrsite3evidencedbymagneticxraycirculardichroism