English

Formation of orbital molecules on a pyrochlore lattice induced by A-O bond covalency

Strongly Correlated Electrons 2021-11-10 v1

Abstract

The pyrochlore ruthenate In2_2Ru2_2O7_7 displays a subtle competition between spin-orbital entanglement and molecular orbital formation. At room temperature, a spin-orbit-entangled singlet state was identified. With decreasing temperature, In2_2Ru2_2O7_7 undergoes multiple structural transitions and eventually forms a nonmagnetic ground state with semi-isolated Ru2_2O units on the pyrochlore lattice. The dominant hopping through the Ru-O-Ru linkage leads to molecular orbital formation within the Ru2_2O units. This molecular orbital formation is unique in that it involves the O2^{2-} anions, unlike the transition-metal dimers observed in systems with edge-sharing octahedra. We argue that the covalent character of In-O bonds plays a pivotal role in the structural transitions and molecular orbital formation and such bonding character of "AA-site" ions is an important ingredient for electronic phase competition in complex transition metal oxides.

Keywords

Cite

@article{arxiv.2111.05057,
  title  = {Formation of orbital molecules on a pyrochlore lattice induced by A-O bond covalency},
  author = {A. Krajewska and A. Yaresko and J. Nuss and A. S. Gibbs and S. Bette and M. Blankenhorn and R. E. Dinnebier and D. P. Sari and I. Watanabe and J. Bertinshaw and H. Gretarsson and K. Ishii and D. Matsumura and T. Tsuji and M. Isobe and B. Keimer and H. Takagi and T. Takayama},
  journal= {arXiv preprint arXiv:2111.05057},
  year   = {2021}
}