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Spin-orbital Jahn-Teller bipolarons.

Lorenzo Celiberti1,2, Dario Fiore Mosca1,3,4, Giuseppe Allodi5

  • 1Faculty of Physics and Center for Computational Materials Science, University of Vienna, 1090, Vienna, Austria.

Nature Communications
|March 19, 2024
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Summary
This summary is machine-generated.

This study reveals spin-orbital bipolarons in doped osmium oxides, where polarons and spin-orbit coupling interact. This entanglement preserves the Mott gap across doping, impacting charge transport and spin-orbitronics.

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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Quantum Mechanics

Background:

  • Polarons arise from electron-phonon interactions and electron localization, common in 3d transition metal oxides.
  • Spin-orbit coupling is significant in heavy atoms (5d transition metal oxides) with delocalized electrons.
  • These phenomena are typically considered distinct and mutually exclusive in charge transport and spin-orbitronics.

Purpose of the Study:

  • To investigate the interplay between polarons and spin-orbit coupling in electron-doped osmium oxides.
  • To demonstrate the formation of spin-orbital bipolarons in Ba₂Na₁₋ₓCaₓOsO₆.
  • To understand the impact of these entangled interactions on material properties and electronic phase transitions.

Main Methods:

  • Combined ab initio calculations to model electronic structure and interactions.
  • Experimental magnetic measurements to characterize material properties.
  • Analysis of electron doping effects on the Os 5d electronic configuration and spin-orbital states.

Main Results:

  • Demonstrated entanglement of polarons and spin-orbit coupling, forming spin-orbital bipolarons in Ba₂Na₁₋ₓCaₓOsO₆.
  • Observed conversion of Os 5d¹ J_eff=3/2 levels to a 5d² J_eff=2 bipolaron manifold due to polaron trapping.
  • Showcased the coexistence of different J-effective states within a single phase and the preservation of the Mott gap across the doping range.

Conclusions:

  • The study unveils a novel quantum effect: spin-orbital bipolarons, arising from the entanglement of polarons and spin-orbit coupling.
  • Polaron charge trapping and Jahn-Teller activity are key mechanisms driving this phenomenon in the studied osmium oxides.
  • The formation of spin-orbital bipolarons prevents metallization, maintaining the Mott gap even at high doping levels.