Spin-glass states generated in a van der Waals magnet by alkali-ion intercalation

Safe Khan; Eva S. Y. Aw; Liam A. V. Nagle-Cocco; Aakanksha Sud; Sukanya Ghosh; Mohammed K. B. Subhan; Zekun Xue; Charlie Freeman; Dimitrios Sagkovits; Araceli Gutierrez-Llorente; Ivan Verzhbitskiy; Daan M. Arroo; Christoph W. Zollitsch; Goki  Eda; Elton J. G. Santos; Sian E. Dutton; Steven T. Bramwell; Chris A. Howard; Hidekazu Kurebayashi

doi:10.1002/adma.202400270

Spin-glass states generated in a van der Waals magnet by alkali-ion intercalation

Safe Khan^*, Eva S. Y. Aw, Liam A. V. Nagle-Cocco, Aakanksha Sud, Sukanya Ghosh, Mohammed K. B. Subhan, Zekun Xue, Charlie Freeman, Dimitrios Sagkovits, Araceli Gutierrez-Llorente, Ivan Verzhbitskiy, Daan M. Arroo, Christoph W. Zollitsch, Goki Eda, Elton J. G. Santos, Sian E. Dutton, Steven T. Bramwell, Chris A. Howard, Hidekazu Kurebayashi^*

^*Corresponding author for this work

School of Physics and Astronomy

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

Abstract / Description of output

Tuning magnetic properties in layered van der Waals (vdW) materials has captured significant attention due to the efficient control of ground states by heterostructuring and external stimuli. Electron doping by electrostatic gating, interfacial charge transfer, and intercalation is particularly effective in manipulating the exchange and spin-orbit properties, resulting in a control of Curie temperature (TC) and magnetic anisotropy. Here, an uncharted role of intercalation is discovered to generate magnetic frustration. As a model study, Na atoms are intercalated into the vdW gaps of pristine Cr2Ge2Te6 (CGT) where generated magnetic frustration leads to emerging spin-glass states coexisting with a ferromagnetic order. A series of dynamic magnetic susceptibility measurements/analysis confirms the formation of magnetic clusters representing slow dynamics with a distribution of relaxation times. The intercalation also modifies other macroscopic physical parameters including the significant enhancement of TC from 66 to 240 K and the switching of magnetic easy-hard axis direction. This study identifies intercalation as a unique route to generate emerging frustrated spin states in simple vdW crystals.

Original language	English
Article number	2400270
Pages (from-to)	1-10
Number of pages	10
Journal	Advanced Materials
Volume	36
Issue number	36
Early online date	22 Jul 2024
DOIs	https://doi.org/10.1002/adma.202400270
Publication status	Published - 5 Sept 2024

Keywords / Materials (for Non-textual outputs)

2D materials
intercalation
magnetic frustration
magnetic materials
spin glass

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https://arxiv.org/abs/2312.17554#Licence: Creative Commons: Attribution (CC-BY)

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Khan, S., Aw, E. S. Y., Nagle-Cocco, L. A. V., Sud, A., Ghosh, S., Subhan, M. K. B., Xue, Z., Freeman, C., Sagkovits, D., Gutierrez-Llorente, A., Verzhbitskiy, I., Arroo, D. M., Zollitsch, C. W., Eda, G., Santos, E. J. G., Dutton, S. E., Bramwell, S. T., Howard, C. A., & Kurebayashi, H. (2024). Spin-glass states generated in a van der Waals magnet by alkali-ion intercalation. Advanced Materials, 36(36), 1-10. Article 2400270. https://doi.org/10.1002/adma.202400270

@article{3e908a3a77394d40bd12e0cadb2ecaca,

title = "Spin-glass states generated in a van der Waals magnet by alkali-ion intercalation",

abstract = "Tuning magnetic properties in layered van der Waals (vdW) materials has captured significant attention due to the efficient control of ground states by heterostructuring and external stimuli. Electron doping by electrostatic gating, interfacial charge transfer, and intercalation is particularly effective in manipulating the exchange and spin-orbit properties, resulting in a control of Curie temperature (TC) and magnetic anisotropy. Here, an uncharted role of intercalation is discovered to generate magnetic frustration. As a model study, Na atoms are intercalated into the vdW gaps of pristine Cr2Ge2Te6 (CGT) where generated magnetic frustration leads to emerging spin-glass states coexisting with a ferromagnetic order. A series of dynamic magnetic susceptibility measurements/analysis confirms the formation of magnetic clusters representing slow dynamics with a distribution of relaxation times. The intercalation also modifies other macroscopic physical parameters including the significant enhancement of TC from 66 to 240 K and the switching of magnetic easy-hard axis direction. This study identifies intercalation as a unique route to generate emerging frustrated spin states in simple vdW crystals.",

keywords = "2D materials, intercalation, magnetic frustration, magnetic materials, spin glass",

author = "Safe Khan and Aw, {Eva S. Y.} and Nagle-Cocco, {Liam A. V.} and Aakanksha Sud and Sukanya Ghosh and Subhan, {Mohammed K. B.} and Zekun Xue and Charlie Freeman and Dimitrios Sagkovits and Araceli Gutierrez-Llorente and Ivan Verzhbitskiy and Arroo, {Daan M.} and Zollitsch, {Christoph W.} and Goki Eda and Santos, {Elton J. G.} and Dutton, {Sian E.} and Bramwell, {Steven T.} and Howard, {Chris A.} and Hidekazu Kurebayashi",

note = "31 pages, 18 figures",

year = "2024",

month = sep,

day = "5",

doi = "10.1002/adma.202400270",

language = "English",

volume = "36",

pages = "1--10",

journal = "Advanced Materials",

issn = "0935-9648",

publisher = "Wiley-VCH",

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}

Khan, S, Aw, ESY, Nagle-Cocco, LAV, Sud, A, Ghosh, S, Subhan, MKB, Xue, Z, Freeman, C, Sagkovits, D, Gutierrez-Llorente, A, Verzhbitskiy, I, Arroo, DM, Zollitsch, CW, Eda, G, Santos, EJG, Dutton, SE, Bramwell, ST, Howard, CA & Kurebayashi, H 2024, 'Spin-glass states generated in a van der Waals magnet by alkali-ion intercalation', Advanced Materials, vol. 36, no. 36, 2400270, pp. 1-10. https://doi.org/10.1002/adma.202400270

TY - JOUR

T1 - Spin-glass states generated in a van der Waals magnet by alkali-ion intercalation

AU - Khan, Safe

AU - Aw, Eva S. Y.

AU - Nagle-Cocco, Liam A. V.

AU - Sud, Aakanksha

AU - Ghosh, Sukanya

AU - Subhan, Mohammed K. B.

AU - Xue, Zekun

AU - Freeman, Charlie

AU - Sagkovits, Dimitrios

AU - Gutierrez-Llorente, Araceli

AU - Verzhbitskiy, Ivan

AU - Arroo, Daan M.

AU - Zollitsch, Christoph W.

AU - Eda, Goki

AU - Santos, Elton J. G.

AU - Dutton, Sian E.

AU - Bramwell, Steven T.

AU - Howard, Chris A.

AU - Kurebayashi, Hidekazu

N1 - 31 pages, 18 figures

PY - 2024/9/5

Y1 - 2024/9/5

N2 - Tuning magnetic properties in layered van der Waals (vdW) materials has captured significant attention due to the efficient control of ground states by heterostructuring and external stimuli. Electron doping by electrostatic gating, interfacial charge transfer, and intercalation is particularly effective in manipulating the exchange and spin-orbit properties, resulting in a control of Curie temperature (TC) and magnetic anisotropy. Here, an uncharted role of intercalation is discovered to generate magnetic frustration. As a model study, Na atoms are intercalated into the vdW gaps of pristine Cr2Ge2Te6 (CGT) where generated magnetic frustration leads to emerging spin-glass states coexisting with a ferromagnetic order. A series of dynamic magnetic susceptibility measurements/analysis confirms the formation of magnetic clusters representing slow dynamics with a distribution of relaxation times. The intercalation also modifies other macroscopic physical parameters including the significant enhancement of TC from 66 to 240 K and the switching of magnetic easy-hard axis direction. This study identifies intercalation as a unique route to generate emerging frustrated spin states in simple vdW crystals.

AB - Tuning magnetic properties in layered van der Waals (vdW) materials has captured significant attention due to the efficient control of ground states by heterostructuring and external stimuli. Electron doping by electrostatic gating, interfacial charge transfer, and intercalation is particularly effective in manipulating the exchange and spin-orbit properties, resulting in a control of Curie temperature (TC) and magnetic anisotropy. Here, an uncharted role of intercalation is discovered to generate magnetic frustration. As a model study, Na atoms are intercalated into the vdW gaps of pristine Cr2Ge2Te6 (CGT) where generated magnetic frustration leads to emerging spin-glass states coexisting with a ferromagnetic order. A series of dynamic magnetic susceptibility measurements/analysis confirms the formation of magnetic clusters representing slow dynamics with a distribution of relaxation times. The intercalation also modifies other macroscopic physical parameters including the significant enhancement of TC from 66 to 240 K and the switching of magnetic easy-hard axis direction. This study identifies intercalation as a unique route to generate emerging frustrated spin states in simple vdW crystals.

KW - 2D materials

KW - intercalation

KW - magnetic frustration

KW - magnetic materials

KW - spin glass

U2 - 10.1002/adma.202400270

DO - 10.1002/adma.202400270

M3 - Article

SN - 0935-9648

VL - 36

SP - 1

EP - 10

JO - Advanced Materials

JF - Advanced Materials

IS - 36

M1 - 2400270

ER -

Spin-glass states generated in a van der Waals magnet by alkali-ion intercalation

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Keywords / Materials (for Non-textual outputs)

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