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Nearly linear orbital molecules on a pyrochlore lattice.

Aleksandra Krajewska1,2,3, Alexander N Yaresko1, Jürgen Nuss1

  • 1Max Planck Institute for Solid State Research, 70569 Stuttgart, Germany.

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|October 9, 2024
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Indium ruthenate (In2Ru2O7) exhibits a unique nonmagnetic ground state due to covalent In-O bonds, forming Ru2O molecules. This discovery challenges existing models of excitonic magnets and geometrical frustration in pyrochlore ruthenates.

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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Solid-State Chemistry

Background:

  • Complex ruthenates with octahedrally coordinated Ru4+ exhibit phase competition driven by spin-orbit coupling (SOC).
  • SOC can stabilize a nonmagnetic Jeff = 0 state locally.
  • Intersite interactions lead to either excitonic magnets or Ru2 molecular orbital dimers at low temperatures.

Purpose of the Study:

  • To synthesize and characterize In2Ru2O7, a pyrochlore ruthenate, to investigate its low-temperature magnetic and structural properties.
  • To understand the role of covalent In-O bonds in determining the ground state of this material.
  • To explore deviations from typical A2Ru2O7 behavior, particularly regarding excitonic magnetism and geometrical frustration.

Main Methods:

  • Synthesis of In2Ru2O7 with covalent In-O bonds.
  • High-temperature and low-temperature characterization of the pyrochlore ruthenate.
  • Analysis of structural and magnetic properties to determine the ground state.

Main Results:

  • In2Ru2O7 exhibits a local Jeff = 0 state at high temperatures.
  • At low temperatures, it forms a unique nonmagnetic ground state characterized by nearly linear Ru-O-Ru molecules.
  • Covalent In-O bond disproportionation drives the formation of Ru2O molecules, quenching both the local spin-orbit singlet and geometrical frustration.

Conclusions:

  • In2Ru2O7 presents a novel nonmagnetic ground state distinct from other pyrochlore ruthenates.
  • The formation of Ru2O molecules via covalent bond disproportionation is the key mechanism driving this unique state.
  • This finding offers new insights into the interplay of SOC, intersite interactions, and bonding in complex oxides, challenging existing paradigms of excitonic magnetism and frustration.