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| Naji, M. |
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| Motta, Antonella |
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| Ertürk, Emre |
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| Taccardi, Nicola |
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| Kočí, Jan | Prague |
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| Ollier, Nadège |
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| Azevedo, Nuno Monteiro |
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| Landes, Michael |
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Bette, S.
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Publications (4/4 displayed)
- 2024Microstructural Insights into the Transformation of Cubic, Low-Temperature, Disordered Cu2ZnSnS4 into the Tetragonal Formcitations
- 2022Competing spin-orbital singlet states in the 4d 4 honeycomb ruthenate Ag 3 LiRu 2 O 6citations
- 2022Competing spin-orbital singlet states in the 4d4 honeycomb ruthenate Ag3LiRu2O6citations
- 2015Real-Time Imaging System using a 12-MHz Forward-Looking Catheter with Single Chip CMUT-on-CMOS Arraycitations
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article
Competing spin-orbital singlet states in the 4d4 honeycomb ruthenate Ag3LiRu2O6
Abstract
When spin-orbit-entangled <i>d </i>electrons reside on a honeycomb lattice, rich quantum states are anticipated to emerge, as exemplified by the <i>d</i><sup>5</sup> Kitaev materials. Distinct yet equally intriguing physics may be realized with a <i>d</i>-electron count other than <i>d</i><sup>5</sup>. The magnetization, <sup>7</sup>Li-nuclear magnetic resonance (NMR), and inelastic neutron scattering measurements, together with the quantum chemistry calculation, indicate that the layered ruthenate Ag<sub>3</sub>LiRu<sub>2</sub>O<sub>6</sub> with <i>d</i><sup>4</sup>Ru<sup>4+</sup> ions at ambient pressure forms a honeycomb lattice of spin-orbit-entangled singlets, which is a playground for frustrated excitonic magnetism. Under pressure, the singlet state does not develop the expected excitonic magnetism, but two successive transitions to other nonmagnetic phases were found in <sup>7</sup>Li-NMR, neutron diffraction, and x-ray absorption fine structure measurements, first to an intermediate phase with moderate distortion of honeycomb lattice and eventually to a high-pressure phase with very short Ru-Ru dimer bonds. While the strong dimerization in the high-pressure phase originates from a molecular orbital formation as in the sister compound Li<sub>2</sub>RuO<sub>3</sub>, we argue that the intermediate phase represents a spin-orbit-coupled singlet dimer state which is stabilized by the admixture of upper-lying <i>J</i><sub>eff</sub>=1-derived states via a pseudo-Jahn-Teller effect. The emergence of competing electronic phases demonstrates rich spin-orbital physics of <i>d</i><sup>4</sup> honeycomb compounds, and this finding paves the way for realization of unconventional magnetism.