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Hidden Charge-Order in the Mixed-Valent K0.75Li2Cr6O12 High-Pressure Oxide.

Angel M Arévalo-López1, Clemens Ritter2, Marielle Huvé1

  • 1UMR-8181-UCCS-Unité de Catalyse et Chimie du Solide (UCCS), CNRS, Université de Lille, Centrale Lille/ENSCL, Lille, 59000, France.

Advanced Science (Weinheim, Baden-Wurttemberg, Germany)
|December 5, 2025
PubMed
Summary

A novel high-pressure oxide, K₀.₇₅Li₂Cr₆³·⁵⁴O₁₂, exhibits a unique helical magnetic structure. Pressure-induced changes drive a transition from paramagnetic to antiferromagnetic states, revealing strong spin-lattice coupling.

Keywords:
charge‐orderhigh‐pressure oxidemagnetismmixed‐valencyneutron diffraction

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Area of Science:

  • Materials Science
  • Solid State Chemistry
  • Magnetism

Background:

  • Mixed-valent chromium oxides with channel structures are of interest due to their complex magnetic and electronic properties.
  • Understanding the relationship between crystal structure, cation disorder, and magnetic transitions is crucial for designing new functional materials.

Purpose of the Study:

  • To synthesize and characterize a novel mixed-valent high-pressure chromium oxide, K₀.₇₅Li₂Cr₆³·⁵⁴O₁₂.
  • To elucidate the crystal structure, magnetic properties, and the nature of the magnetic transition in this compound.
  • To investigate the influence of pressure and structural disorder on the magnetic interactions.

Main Methods:

  • High-pressure synthesis at 12 GPa and 1373 K.
  • Synchrotron X-ray diffraction and powder neutron diffraction (PND) for structural analysis.
  • Electron microscopy and pair distribution function analysis for local structure.
  • Low-temperature PND to determine magnetic structure.
  • Density functional theory (DFT) calculations for electronic structure and magnetic exchange interactions.

Main Results:

  • A P6₃/m average crystal structure was determined, featuring a corner-sharing CrO₆ octahedra framework with Li⁺ and K⁺ in channels.
  • Evidence of K⁺ disorder and loss of correlation in the K⁺ channels was observed.
  • A magnetostrictive paramagnetic-to-antiferromagnetic transition occurred at T<0xE2><0x82><0x99> = 75 K.
  • A commensurate helical magnetic structure with a propagation vector k = [⅓ ⅓ ¼] was resolved at low temperatures.
  • DFT calculations confirmed the role of c-axis compression in mediating magnetic exchange interactions, leading to a charge-ordered antiferromagnetic state.

Conclusions:

  • K₀.₇₅Li₂Cr₆³·⁵⁴O₁₂ exhibits a pressure-stabilized helical antiferromagnetic structure.
  • Despite K⁺ disorder, the material displays significant spin-lattice coupling, where structural changes strongly influence magnetic properties.
  • The findings provide insights into pressure-induced magnetic transitions in related hollandite structures.