<p>The prospect of merging the paradigms of geometric frustration on a triangular lattice and bond anisotropies in the strong spin-orbit coupling limit holds tremendous promise in the search for exotic quantum materials. Here we identify a new candidate system to realize such physics, the organic quantum antiferromagnet (CD<sub>3</sub>ND<sub>3</sub>)<sub>2</sub>NaRuCl<sub>6</sub>. We report a combination of thermodynamic, magneto-elastic and neutron scattering experiments on single-crystals to determine the phase diagram in axial magnetic fields <b>H</b>∥<b>c</b> and propose a minimal model Hamiltonian. (CD<sub>3</sub>ND<sub>3</sub>)<sub>2</sub>NaRuCl<sub>6</sub> displays an ideal triangular arrangement of Ru<sup>3+</sup> ions adopting the spin-orbital entangled <i>j</i><sub>eff</sub> = 1/2 state. It hosts residual magnetic order below <i>T</i><sub>N</sub> = 0.23 K and a highly unusual <i>H</i> − <i>T</i> phase diagram including three different incommensurate states. Spin-waves in the high-field polarized regime are described by a Heisenberg triangular lattice Hamiltonian with a potential sub-leading bond dependent anisotropy term <i>J</i><sub>±±</sub>. We argue that the multi-<b>q</b> ground state in zero magnetic field is a prime candidate for hosting the <InlineEquation ID="IEq2"><EquationSource Format="TEX">\({{\mathbb{Z}}}_{2}\)</EquationSource><EquationSource Format="MATHML"><math><msub><mrow><mi mathvariant="double-struck">Z</mi></mrow><mrow><mn>2</mn></mrow></msub></math></EquationSource></InlineEquation> vortex crystal proposed on the triangular Heisenberg-Kitaev model. (CD<sub>3</sub>ND<sub>3</sub>)<sub>2</sub>NaRuCl<sub>6</sub> is the first member in an extended family of quantum triangular lattice magnets, providing a new playground to study the interplay of geometric frustration and spin-orbit effects.</p>

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\({{\mathbb{Z}}}_{2}\) vortex crystal candidate in the triangular S = 1/2 quantum antiferromagnet

  • Jakob Nagl,
  • Kirill Yu. Povarov,
  • Benjamin Duncan,
  • Catharina Näppi,
  • Dmitry Khalyavin,
  • Pascal Manuel,
  • Fabio Orlandi,
  • Jeremy Sourd,
  • Beat Valentin Schwarze,
  • Freya Husstedt,
  • Sergei A. Zvyagin,
  • Oksana Zaharko,
  • Paul Steffens,
  • Arno Hiess,
  • David R. Allan,
  • Sarah A. Barnett,
  • Zewu Yan,
  • Severian Gvasaliya,
  • Andrey Zheludev

摘要

The prospect of merging the paradigms of geometric frustration on a triangular lattice and bond anisotropies in the strong spin-orbit coupling limit holds tremendous promise in the search for exotic quantum materials. Here we identify a new candidate system to realize such physics, the organic quantum antiferromagnet (CD3ND3)2NaRuCl6. We report a combination of thermodynamic, magneto-elastic and neutron scattering experiments on single-crystals to determine the phase diagram in axial magnetic fields Hc and propose a minimal model Hamiltonian. (CD3ND3)2NaRuCl6 displays an ideal triangular arrangement of Ru3+ ions adopting the spin-orbital entangled jeff = 1/2 state. It hosts residual magnetic order below TN = 0.23 K and a highly unusual HT phase diagram including three different incommensurate states. Spin-waves in the high-field polarized regime are described by a Heisenberg triangular lattice Hamiltonian with a potential sub-leading bond dependent anisotropy term J±±. We argue that the multi-q ground state in zero magnetic field is a prime candidate for hosting the \({{\mathbb{Z}}}_{2}\)Z2 vortex crystal proposed on the triangular Heisenberg-Kitaev model. (CD3ND3)2NaRuCl6 is the first member in an extended family of quantum triangular lattice magnets, providing a new playground to study the interplay of geometric frustration and spin-orbit effects.