Competing spin-orbital singlet states in the honeycomb ruthenate
T. Takayama et al.
Phys. Rev. Research 4, 043079 (2022) - Published 7 November, 2022
When spin-orbit-entangled electrons reside on a honeycomb lattice, rich quantum states are anticipated to emerge, as exemplified by the Kitaev materials. Distinct yet equally intriguing physics may be realized with a -electron count other than . The magnetization, -nuclear magnetic resonance (NMR), and inelastic neutron scattering measurements, together with the quantum chemistry calculation, indicate that the layered ruthenate with 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 -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 , we argue that the intermediate phase represents a spin-orbit-coupled singlet dimer state which is stabilized by the admixture of upper-lying -derived states via a pseudo-Jahn-Teller effect. The emergence of competing electronic phases demonstrates rich spin-orbital physics of honeycomb compounds, and this finding paves the way for realization of unconventional magnetism.




