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    Critical behavior and evidence of dimensional crossover in quasi-two-dimensional Li2FeSiO4

    W. Hergett1,*, K. Ackermann2,*, E. Walendy1, S. Spachmann1, M. Jonak1, M. Abdel-Hafiez1,3,4, M. W. Haverkort2, and R. Klingeler1,†

    • *These authors contributed equally to this work.
    • †Contact author: klingeler@kip.uni-heidelberg.de

    Phys. Rev. B 113, 024435 – Published 28 January, 2026

    DOI: https://doi.org/10.1103/x66l-7vsx

    Abstract

    We report thermal-expansion and heat-capacity studies on Li2FeSiO4 single crystals which enable us to investigate critical behavior in magnetically quasi-two-dimensional (2D) material. Pronounced λ-shaped anomalies at the magnetic ordering temperature TN imply significant magnetoelastic coupling. Our analysis of both the thermal-expansion and the specific heat data implies the crossover from 2D Ising-like behavior for |(T−TN)/TN|>0.3 to 3D Ising behavior below ≃1.3×TN. The 2D-like behavior is further supported by density functional calculations which show minimal dispersion perpendicular to the crystallographic ac planes of the layered structure, thereby indicating the 2D nature of magnetism at higher temperatures. Our results extend the available model materials of quasi-2D magnetism to a high-spin S=2 system with tetrahedrally coordinated Fe2+ ions, thereby illustrating how magnetic order evolves in a 2D Ising-like system with orbital degrees of freedom.

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