Magnetic evolution induced by freezing of Ag+ fluctuations in an intercalated transition metal dichalcogenide

J. Qi; H. Wang; Q. Zhang; Y. Kawakita; K. Shibata; P. Miao; S. Torii; Y. K. Huang; D. Li; K. Singh; R. Rawat; T. Kamiyama; D. Vaknin; E. P. Gilbert; Z. D. Zhang; K. Nakajima; B. Li

doi:10.1103/PhysRevMaterials.9.044411

Magnetic evolution induced by freezing of Ag+ fluctuations in an intercalated transition metal dichalcogenide

J. Qi, H. Wang, Q. Zhang, Y. Kawakita, K. Shibata, P. Miao, S. Torii, Y. K. Huang, D. Li, K. Singh, R. Rawat, T. Kamiyama, D. Vaknin, E. P. Gilbert, Z. D. Zhang, K. Nakajima, B. Li

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Abstract

Here, we present a comprehensive study on the magnetic evolution processes in AgCrSe2 using both neutron scattering and theoretical calculations. The development of magnetic short-range correlation with decoupled interlayer interactions is confirmed between 55 and 200 K. Significant magneto-crystalline anisotropy energy around 0.1 meV of Cr3+ is identified that mainly contributes to the robust existence of the in-plane magnetic correlations in the magnetic short-order regime. Furthermore, the indirect superexchange interactions through Cr-Se-Ag-Se-Cr path between the adjacent CrSe6 octahedral layers is also demonstrated. In combination with the mutual coupling among multiple degrees of freedom (spin, phonon, lattice, and dipole), we reveal the key role of the freezing of Ag+ fluctuations in preventing interlayer exchange interactions from decoupling.

Original language	English
Article number	044411
Journal	Physical Review Materials
Volume	9
Issue number	4
DOIs	https://doi.org/10.1103/PhysRevMaterials.9.044411
State	Published - Apr 2025

Funding

We thank Dr. José Ignacio Robledo at Forschungszentrum Jülich for his valuable contribution to the small angle neutron scattering data analysis. B.L. was supported by the Ministry of Science and Technology of China (Grant 2021YFB3501201) and the National Natural Science Foundation of China (Grants No. 52425107 and No. 11934007). H.W. acknowledges support from State Key Laboratory of Powder Metallurgy and Innovation-Driven Plan (2019CX023) of Central South University, Project of High-Level Talents of Hunan Province (2018RS3021) and National Natural Science Foundation of China (11874429). Q.Z. was supported by the US Department of Energy, office of Basic Energy Sciences, Scientific User Facilities Division. Ames Laboratory is operated for the U.S. Department of Energy by Iowa State University under Contract No. DE-AC02-07CH11358. We acknowledge the award of beam time from J-PARC via Proposals No. 2012P0906, No. 2015A0123, No. 2015A0075 and No. 2016B0057, and from ANSTO via Proposal No. 14264.

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Qi, J., Wang, H., Zhang, Q., Kawakita, Y., Shibata, K., Miao, P., Torii, S., Huang, Y. K., Li, D., Singh, K., Rawat, R., Kamiyama, T., Vaknin, D., Gilbert, E. P., Zhang, Z. D., Nakajima, K., & Li, B. (2025). Magnetic evolution induced by freezing of Ag+ fluctuations in an intercalated transition metal dichalcogenide. Physical Review Materials, 9(4), Article 044411. https://doi.org/10.1103/PhysRevMaterials.9.044411

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title = "Magnetic evolution induced by freezing of Ag+ fluctuations in an intercalated transition metal dichalcogenide",

abstract = "Here, we present a comprehensive study on the magnetic evolution processes in AgCrSe2 using both neutron scattering and theoretical calculations. The development of magnetic short-range correlation with decoupled interlayer interactions is confirmed between 55 and 200 K. Significant magneto-crystalline anisotropy energy around 0.1 meV of Cr3+ is identified that mainly contributes to the robust existence of the in-plane magnetic correlations in the magnetic short-order regime. Furthermore, the indirect superexchange interactions through Cr-Se-Ag-Se-Cr path between the adjacent CrSe6 octahedral layers is also demonstrated. In combination with the mutual coupling among multiple degrees of freedom (spin, phonon, lattice, and dipole), we reveal the key role of the freezing of Ag+ fluctuations in preventing interlayer exchange interactions from decoupling.",

author = "J. Qi and H. Wang and Q. Zhang and Y. Kawakita and K. Shibata and P. Miao and S. Torii and Huang, \{Y. K.\} and D. Li and K. Singh and R. Rawat and T. Kamiyama and D. Vaknin and Gilbert, \{E. P.\} and Zhang, \{Z. D.\} and K. Nakajima and B. Li",

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Qi, J, Wang, H, Zhang, Q, Kawakita, Y, Shibata, K, Miao, P, Torii, S, Huang, YK, Li, D, Singh, K, Rawat, R, Kamiyama, T, Vaknin, D, Gilbert, EP, Zhang, ZD, Nakajima, K & Li, B 2025, 'Magnetic evolution induced by freezing of Ag+ fluctuations in an intercalated transition metal dichalcogenide', Physical Review Materials, vol. 9, no. 4, 044411. https://doi.org/10.1103/PhysRevMaterials.9.044411

TY - JOUR

T1 - Magnetic evolution induced by freezing of Ag+ fluctuations in an intercalated transition metal dichalcogenide

AU - Qi, J.

AU - Wang, H.

AU - Zhang, Q.

AU - Kawakita, Y.

AU - Shibata, K.

AU - Miao, P.

AU - Torii, S.

AU - Huang, Y. K.

AU - Li, D.

AU - Singh, K.

AU - Rawat, R.

AU - Kamiyama, T.

AU - Vaknin, D.

AU - Gilbert, E. P.

AU - Zhang, Z. D.

AU - Nakajima, K.

AU - Li, B.

PY - 2025/4

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N2 - Here, we present a comprehensive study on the magnetic evolution processes in AgCrSe2 using both neutron scattering and theoretical calculations. The development of magnetic short-range correlation with decoupled interlayer interactions is confirmed between 55 and 200 K. Significant magneto-crystalline anisotropy energy around 0.1 meV of Cr3+ is identified that mainly contributes to the robust existence of the in-plane magnetic correlations in the magnetic short-order regime. Furthermore, the indirect superexchange interactions through Cr-Se-Ag-Se-Cr path between the adjacent CrSe6 octahedral layers is also demonstrated. In combination with the mutual coupling among multiple degrees of freedom (spin, phonon, lattice, and dipole), we reveal the key role of the freezing of Ag+ fluctuations in preventing interlayer exchange interactions from decoupling.

AB - Here, we present a comprehensive study on the magnetic evolution processes in AgCrSe2 using both neutron scattering and theoretical calculations. The development of magnetic short-range correlation with decoupled interlayer interactions is confirmed between 55 and 200 K. Significant magneto-crystalline anisotropy energy around 0.1 meV of Cr3+ is identified that mainly contributes to the robust existence of the in-plane magnetic correlations in the magnetic short-order regime. Furthermore, the indirect superexchange interactions through Cr-Se-Ag-Se-Cr path between the adjacent CrSe6 octahedral layers is also demonstrated. In combination with the mutual coupling among multiple degrees of freedom (spin, phonon, lattice, and dipole), we reveal the key role of the freezing of Ag+ fluctuations in preventing interlayer exchange interactions from decoupling.

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DO - 10.1103/PhysRevMaterials.9.044411

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JO - Physical Review Materials

JF - Physical Review Materials

IS - 4

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ER -

Magnetic evolution induced by freezing of Ag+ fluctuations in an intercalated transition metal dichalcogenide

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