Giant valley-Zeeman coupling in the surface layer of an intercalated transition metal dichalcogenide

Brendan Edwards; O Dowinton; A Hall; Philip  Murgatroyd; Sebastian Buchberger; Tommaso Antonelli; Gesa-Roxanne Siemann; Akhil  Rajan; Edgar Abarca Morales; Andela Zivanovic; Chiara Bigi; R Belosludov; M Polley; D Carbone; D Mayoh; G Balakrishnan; M Bahramy; Phil King

doi:10.1038/s41563-022-01459-z

Giant valley-Zeeman coupling in the surface layer of an intercalated transition metal dichalcogenide

Brendan Edwards, O Dowinton, A Hall, Philip Murgatroyd, Sebastian Buchberger, Tommaso Antonelli, Gesa-Roxanne Siemann, Akhil Rajan, Edgar Abarca Morales, Andela Zivanovic, Chiara Bigi, R Belosludov, M Polley, D Carbone, D Mayoh, G Balakrishnan, M Bahramy^*, Phil King^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

Abstract

Spin–valley locking is ubiquitous among transition metal dichalcogenides with local or global inversion asymmetry, in turn stabilizing properties such as Ising superconductivity, and opening routes towards ‘valleytronics’. The underlying valley–spin splitting is set by spin–orbit coupling but can be tuned via the application of external magnetic fields or through proximity coupling. However, only modest changes have been realized to date. Here, we investigate the electronic structure of the V-intercalated transition metal dichalcogenide V1/3NbS2 using microscopic-area spatially resolved and angle-resolved photoemission spectroscopy. Our measurements and corresponding density functional theory calculations reveal that the bulk magnetic order induces a giant valley-selective Ising coupling exceeding 50 meV in the surface NbS₂ layer, equivalent to application of a ~250 T magnetic field. This energy scale is of comparable magnitude to the intrinsic spin–orbit splittings, and indicates how coupling of local magnetic moments to itinerant states of a transition metal dichalcogenide monolayer provides a powerful route to controlling their valley–spin splittings.

Original language	English
Pages (from-to)	459-465
Number of pages	7
Journal	Nature Materials
Volume	22
Issue number	4
Early online date	19 Jan 2023
DOIs	https://doi.org/10.1038/s41563-022-01459-z
Publication status	Published - 1 Apr 2023

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Copyright © 2023 the Authors. This work has been made available online in accordance with the Rights Retention Strategy This accepted manuscript is distributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. The final published version of this work is available at https://doi.org/10.1038/s41563-022-01459-z.
Accepted author manuscript, 4.25 MBLicence: CC BY

Strain-tuning electronic structure: Strain-tuning electronic structure and quantum many-body interactions
King, P. (PI)
EPSRC
1/11/20 → 31/10/24
Project: Standard
Engineered Quantum States: Engineered quantum states via atmoic-scale assembly of artificial 2D heterostructures
King, P. (PI)
The Leverhulme Trust
1/08/17 → 31/07/22
Project: Standard
ERC Starting Grant QUESTDO: H2020 ERC Starting Grant QUESTDO
King, P. (PI)
European Research Council
1/01/17 → 31/12/21
Project: Fellowship

Imaging the effects of magnetic proximity coupling on the electronic structure of transition metal dichalcogenides (thesis data)
Edwards, B. M. (Creator) & King, P. (Supervisor), University of St Andrews, 12 Jan 2026
DOI: 10.17630/a31d1eec-63c1-41ce-bd9e-8ad3439603f0, https://doi.org/10.17630/sta/698
Dataset: Thesis dataset
Giant valley-Zeeman coupling in the surface layer of an intercalated transition metal dichalcogenide (dataset)
Edwards, B. (Creator), Dowinton, O. (Creator), Hall, A. (Creator), Murgatroyd, P. (Creator), Buchberger, S. (Creator), Antonelli, T. (Creator), Siemann, G.-R. (Creator), Rajan, A. (Creator), Abarca Morales, E. (Creator), Zivanovic, A. (Creator), Bigi, C. (Creator), Belosludov, R. (Creator), Polley, C. (Creator), Carbone, D. (Creator), Mayoh, D. (Creator), Balakrishnan, G. (Creator), Bahramy, M. (Creator) & King, P. (Creator), University of St Andrews, 20 Jan 2023
DOI: 10.17630/fb5496ed-6eae-49fa-9214-cd3507265f2b
Dataset

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Edwards, B., Dowinton, O., Hall, A., Murgatroyd, P., Buchberger, S., Antonelli, T., Siemann, G.-R., Rajan, A., Abarca Morales, E., Zivanovic, A., Bigi, C., Belosludov, R., Polley, M., Carbone, D., Mayoh, D., Balakrishnan, G., Bahramy, M., & King, P. (2023). Giant valley-Zeeman coupling in the surface layer of an intercalated transition metal dichalcogenide. Nature Materials, 22(4), 459-465. https://doi.org/10.1038/s41563-022-01459-z

@article{f169ba3251d9413588a03eb2457188d8,

title = "Giant valley-Zeeman coupling in the surface layer of an intercalated transition metal dichalcogenide",

abstract = "Spin–valley locking is ubiquitous among transition metal dichalcogenides with local or global inversion asymmetry, in turn stabilizing properties such as Ising superconductivity, and opening routes towards {\textquoteleft}valleytronics{\textquoteright}. The underlying valley–spin splitting is set by spin–orbit coupling but can be tuned via the application of external magnetic fields or through proximity coupling. However, only modest changes have been realized to date. Here, we investigate the electronic structure of the V-intercalated transition metal dichalcogenide V1/3NbS2 using microscopic-area spatially resolved and angle-resolved photoemission spectroscopy. Our measurements and corresponding density functional theory calculations reveal that the bulk magnetic order induces a giant valley-selective Ising coupling exceeding 50 meV in the surface NbS2 layer, equivalent to application of a ~250 T magnetic field. This energy scale is of comparable magnitude to the intrinsic spin–orbit splittings, and indicates how coupling of local magnetic moments to itinerant states of a transition metal dichalcogenide monolayer provides a powerful route to controlling their valley–spin splittings.",

author = "Brendan Edwards and O Dowinton and A Hall and Philip Murgatroyd and Sebastian Buchberger and Tommaso Antonelli and Gesa-Roxanne Siemann and Akhil Rajan and {Abarca Morales}, Edgar and Andela Zivanovic and Chiara Bigi and R Belosludov and M Polley and D Carbone and D Mayoh and G Balakrishnan and M Bahramy and Phil King",

note = "Funding: The authors gratefully acknowledge support from the Leverhulme Trust (Grant No. RL-2016-006 [P.D.C.K., B.E., T.A., A.R., C.B.]), the European Research Council (through the QUESTDO project, 714193 [P.D.C.K., G.R.S.]), the Engineering and Physical Sciences Research Council (Grant Nos. EP/T02108X/1 [P.D.C.K., P.A.E.M.] and EP/N032128/1 [D.A.M., G.B.]), and the Center for Computational Materials Science at the Institute for Materials Research for allocations on the MASAMUNE-IMR supercomputer system (Project No. 202112-SCKXX-0510 [R.B.V., M.S.B.]). S.B., E.A.M. and A.Z. gratefully acknowledge studentship support from the International Max-Planck Research School for Chemistry and Physics of Quantum Materials. Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research council under contract 2018-07152, the Swedish Governmental Agency for Innovation Systems under contract 2018-04969, and Formas under contract 2019-02496. The research leading to this result has been supported by the project CALIPSOplus under the Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020.",

year = "2023",

month = apr,

day = "1",

doi = "10.1038/s41563-022-01459-z",

language = "English",

volume = "22",

pages = "459--465",

journal = "Nature Materials",

issn = "1476-1122",

publisher = "Nature publishing group",

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Edwards, B, Dowinton, O, Hall, A, Murgatroyd, P, Buchberger, S, Antonelli, T, Siemann, G-R, Rajan, A, Abarca Morales, E, Zivanovic, A, Bigi, C, Belosludov, R, Polley, M, Carbone, D, Mayoh, D, Balakrishnan, G, Bahramy, M & King, P 2023, 'Giant valley-Zeeman coupling in the surface layer of an intercalated transition metal dichalcogenide', Nature Materials, vol. 22, no. 4, pp. 459-465. https://doi.org/10.1038/s41563-022-01459-z

TY - JOUR

T1 - Giant valley-Zeeman coupling in the surface layer of an intercalated transition metal dichalcogenide

AU - Edwards, Brendan

AU - Dowinton, O

AU - Hall, A

AU - Murgatroyd, Philip

AU - Buchberger, Sebastian

AU - Antonelli, Tommaso

AU - Siemann, Gesa-Roxanne

AU - Rajan, Akhil

AU - Abarca Morales, Edgar

AU - Zivanovic, Andela

AU - Bigi, Chiara

AU - Belosludov, R

AU - Polley, M

AU - Carbone, D

AU - Mayoh, D

AU - Balakrishnan, G

AU - Bahramy, M

AU - King, Phil

N1 - Funding: The authors gratefully acknowledge support from the Leverhulme Trust (Grant No. RL-2016-006 [P.D.C.K., B.E., T.A., A.R., C.B.]), the European Research Council (through the QUESTDO project, 714193 [P.D.C.K., G.R.S.]), the Engineering and Physical Sciences Research Council (Grant Nos. EP/T02108X/1 [P.D.C.K., P.A.E.M.] and EP/N032128/1 [D.A.M., G.B.]), and the Center for Computational Materials Science at the Institute for Materials Research for allocations on the MASAMUNE-IMR supercomputer system (Project No. 202112-SCKXX-0510 [R.B.V., M.S.B.]). S.B., E.A.M. and A.Z. gratefully acknowledge studentship support from the International Max-Planck Research School for Chemistry and Physics of Quantum Materials. Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research council under contract 2018-07152, the Swedish Governmental Agency for Innovation Systems under contract 2018-04969, and Formas under contract 2019-02496. The research leading to this result has been supported by the project CALIPSOplus under the Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020.

PY - 2023/4/1

Y1 - 2023/4/1

N2 - Spin–valley locking is ubiquitous among transition metal dichalcogenides with local or global inversion asymmetry, in turn stabilizing properties such as Ising superconductivity, and opening routes towards ‘valleytronics’. The underlying valley–spin splitting is set by spin–orbit coupling but can be tuned via the application of external magnetic fields or through proximity coupling. However, only modest changes have been realized to date. Here, we investigate the electronic structure of the V-intercalated transition metal dichalcogenide V1/3NbS2 using microscopic-area spatially resolved and angle-resolved photoemission spectroscopy. Our measurements and corresponding density functional theory calculations reveal that the bulk magnetic order induces a giant valley-selective Ising coupling exceeding 50 meV in the surface NbS2 layer, equivalent to application of a ~250 T magnetic field. This energy scale is of comparable magnitude to the intrinsic spin–orbit splittings, and indicates how coupling of local magnetic moments to itinerant states of a transition metal dichalcogenide monolayer provides a powerful route to controlling their valley–spin splittings.

AB - Spin–valley locking is ubiquitous among transition metal dichalcogenides with local or global inversion asymmetry, in turn stabilizing properties such as Ising superconductivity, and opening routes towards ‘valleytronics’. The underlying valley–spin splitting is set by spin–orbit coupling but can be tuned via the application of external magnetic fields or through proximity coupling. However, only modest changes have been realized to date. Here, we investigate the electronic structure of the V-intercalated transition metal dichalcogenide V1/3NbS2 using microscopic-area spatially resolved and angle-resolved photoemission spectroscopy. Our measurements and corresponding density functional theory calculations reveal that the bulk magnetic order induces a giant valley-selective Ising coupling exceeding 50 meV in the surface NbS2 layer, equivalent to application of a ~250 T magnetic field. This energy scale is of comparable magnitude to the intrinsic spin–orbit splittings, and indicates how coupling of local magnetic moments to itinerant states of a transition metal dichalcogenide monolayer provides a powerful route to controlling their valley–spin splittings.

U2 - 10.1038/s41563-022-01459-z

DO - 10.1038/s41563-022-01459-z

M3 - Article

SN - 1476-1122

VL - 22

SP - 459

EP - 465

JO - Nature Materials

JF - Nature Materials

IS - 4

ER -

Giant valley-Zeeman coupling in the surface layer of an intercalated transition metal dichalcogenide

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Projects

Strain-tuning electronic structure: Strain-tuning electronic structure and quantum many-body interactions

Engineered Quantum States: Engineered quantum states via atmoic-scale assembly of artificial 2D heterostructures

ERC Starting Grant QUESTDO: H2020 ERC Starting Grant QUESTDO

Datasets

Imaging the effects of magnetic proximity coupling on the electronic structure of transition metal dichalcogenides (thesis data)

Giant valley-Zeeman coupling in the surface layer of an intercalated transition metal dichalcogenide (dataset)

Cite this