Quasimolecular electronic structure of the spin-liquid candidate Ba3InIr2O9

Publikation: Beitrag in FachzeitschriftForschungsartikelBeigetragenBegutachtung

Beitragende

  • A. Revelli - , Universität zu Köln (Autor:in)
  • M. Moretti Sala - , European Synchrotron Radiation Facility, Polytechnic University of Milan (Autor:in)
  • G. Monaco - , Università degli studi di Padova (Autor:in)
  • M. Magnaterra - , Universität zu Köln (Autor:in)
  • J. Attig - , Universität zu Köln (Autor:in)
  • L. Peterlini - , Universität zu Köln (Autor:in)
  • T. Dey - , Universität zu Köln, Indian Institute of Technology, Dhanbad, Universität Augsburg (Autor:in)
  • A. A. Tsirlin - , Universität Augsburg (Autor:in)
  • P. Gegenwart - , Universität Augsburg (Autor:in)
  • T. Fröhlich - , Universität zu Köln (Autor:in)
  • M. Braden - , Universität zu Köln (Autor:in)
  • C. Grams - , Universität zu Köln (Autor:in)
  • J. Hemberger - , Universität zu Köln (Autor:in)
  • P. Becker - , Universität zu Köln (Autor:in)
  • P. H.M. Van Loosdrecht - , Universität zu Köln (Autor:in)
  • D. I. Khomskii - , Universität zu Köln (Autor:in)
  • J. Van Den Brink - , Exzellenzcluster ct.qmat: Komplexität und Topologie in Quantenmaterialien, Professur für Festkörpertheorie (gB/IFW), Leibniz-Institut für Festkörper- und Werkstoffforschung Dresden (Autor:in)
  • M. Hermanns - , Stockholm University, KTH Royal Institute of Technology (Autor:in)
  • M. Grüninger - , Universität zu Köln (Autor:in)

Abstract

The mixed-valent iridate Ba3InIr2O9 has been discussed as a promising candidate for quantum spin-liquid behavior. The compound exhibits Ir4.5+ ions in face-sharing IrO6 octahedra forming Ir2O9 dimers with three t2g holes per dimer. Our results establish Ba3InIr2O9 as a cluster Mott insulator. Strong intradimer hopping delocalizes the three t2g holes in quasimolecular dimer states while interdimer charge fluctuations are suppressed by Coulomb repulsion. The magnetism of Ba3InIr2O9 emerges from spin-orbit entangled quasimolecular moments with yet unexplored interactions, opening up a new route to unconventional magnetic properties of 5d compounds. Using single-crystal x-ray diffraction we find the monoclinic space group C2/c already at room temperature. Dielectric spectroscopy shows insulating behavior. Resonant inelastic x-ray scattering reveals a rich excitation spectrum below 1.5 eV with a sinusoidal dynamical structure factor that unambiguously demonstrates the quasimolecular character of the electronic states. Below 0.3 eV, we observe a series of excitations. According to exact diagonalization calculations, such low-energy excitations reflect the proximity of Ba3InIr2O9 to a hopping-induced phase transition based on the condensation of a quasimolecular spin-orbit exciton. The dimer ground state roughly hosts two holes in a bonding j=12 orbital and the third hole in a bonding j=32 orbital.

Details

OriginalspracheEnglisch
Aufsatznummer155107
FachzeitschriftPhysical Review B
Jahrgang106
Ausgabenummer15
PublikationsstatusVeröffentlicht - 15 Okt. 2022
Peer-Review-StatusJa