Highly Tunable Ru-dimer Molecular Orbital State in 6H-perovskite Ba_3MRu_2O_9
arxiv(2024)
摘要
Molecular orbital (MO) systems with clusters of heavy transition metal (TM)
ions are one of the most important classes of model materials for studying the
interplay between local physics and effects of itinerancy. Despite a large
number of candidates identified in the family of 4d TM materials, an
understanding of their physics from competing microscopic energy
scales is still missing. We bridge this gap by reporting the first resonant
inelastic X-ray scattering (RIXS) measurement on a well-known series of Ru
dimer systems with a 6H-perovskite structure, Ba_3MRu_2O_9
(M^3+=In^3+, Y^3+, La^3+). Our RIXS measurements reveal an
extremely fragile MO state in these Ru dimer compounds, evidenced by an abrupt
change in the RIXS spectrum accompanying a tiny change in the local structure
tuned by the M-site ion. By modelling the RIXS spectra, we attribute the
enhanced electronic instability in Ba_3MRu_2O_9 to the combined effect of
a large hopping and a small spin-orbit coupling in the Ru dimers. The unique
combination of energy scales uncovered in the present study make Ru MO systems
ideal model systems for studying quantum phase transitions with molecular
orbitals.
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