Published March 31, 2021 | Version v1

Gapped magnetic ground state in quantum-spin-liquid candidate κ-(BEDT-TTF)_2Cu_2(CN)_3

  • 1. 1. Physikalisches Institut, Universität Stuttgart, Pfaffenwaldring 57, 70569 Stuttgart, Germany
  • 2. 1. Physikalisches Institut, Universität Stuttgart, Pfaffenwaldring 57, 70569 Stuttgart, Germany and Department of Physics and Astronomy, UCLA, Los Angeles, California 90095, USA
  • 3. Institut of Problems of Chemical Physics, Russian Academy of Sciences, Chernogolovka, Moscow Region 142432, Russia
  • 4. Department of Applied Physics, University of Tokyo, Tokyo 113-8656, Japan
  • 5. Material Science Division, Argonne National Laboratory, Argonne, Illinois 60439-4831, USA and National Science Foundation, Alexandria, Virginia 2223, USA

Description

Geometrical frustration, quantum entanglement and disorder may prevent long-range ordering of localized spins with strong exchange interactions, resulting in an exotic state of matter. κ-(BEDT-TTF)2Cu2(CN)3 is considered the prime candidate for this elusive quantum-spin-liquid state, but its ground-state properties remain puzzling. Here we present a multi-frequency electron-spin-resonance (ESR) study down to millikelvin temperatures, revealing a rapid drop of the spin susceptibility at T= 6 K. This opening of a spin gap, accompanied by structural modifications, is consistent with the formation of a valence-bond-solid ground state. We identify an impurity contribution to the ESR response that becomes dominant when the intrinsic spins form singlets. Probing the electrons directly manifests the pivotal role of defects for the low-energy properties of quantum-spin systems without magnetic order.

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Preprint: arXiv:2010.16155 (arXiv)