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Charge correlations and magnetoelastic coupling in intercalated transition metal dichalcogenides

A. Kar1,2,*, R. Basak3,*, Xue Li4,5,*, A. Korshunov1,*, D. Subires1,6, J. Phillips7,8, C. Lim1, Feng Zhou4,9, Linxuan Song4,9 et al.

Wenhong Wang9, Yong-Chang Lau4,5, G. Garbarino10, P. Gargiani11, C. Plueckthun12, S. Francoual12, A. Jana13,14, I. Vobornik13, T. Valla1,15, A. Rajapitamahuni16, James G. Analytis17,18, Robert J. Birgeneau17,19,20, E. Vescovo16, A. Bosak10, J. Dai11, M. Tallarida11, A. Frano3, V. Pardo7,8, S. Wu21, and S. Blanco-Canosa1,22,†

  • *These authors contributed equally to this work.
  • †Contact author: sblanco@dipc.org

Phys. Rev. Materials 10, 034006 – Published 23 March, 2026

DOI: https://doi.org/10.1103/gyfq-2c26

Abstract

The large van der Waals gap in transition metal dichalcogenides (TMDs) offers an avenue to tune the ground state of 2D materials through the intercalation of magnetic atoms. Here, we investigate the charge correlations in Fe1/3TaS2, Co1/3TaS2, and Fe0.35NbS2 by combining angle-resolved photoemission spectroscopy (ARPES), x-ray scattering, magnetometry, and density functional theory (DFT). We find that, while short-range charge fluctuations develop in Ta-based compounds, Fe0.35NbS2 exhibits long-range charge order which is strongly coupled with magnetic order and tunable by external magnetic field. Our electronic structure analysis reveals that intercalation reconstructs the Fermi surface via charge transfer and band renormalization, yet does not generate the nesting conditions compatible with the observed ordering vectors. Complementary phonon calculations further exclude a conventional electron-phonon origin of charge order. Together, these results establish magnetoelastic coupling as the dominant mechanism behind charge ordering in Fe0.35NbS2 and highlight the contrasting role of Nb and Ta hosts in stabilizing correlated ground states in intercalated TMDs.

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