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Nat Commun. 2019 Mar 6;10(1):1064. doi: 10.1038/s41467-019-09071-7.

Pressure-tuning the quantum spin Hamiltonian of the triangular lattice antiferromagnet Cs2CuCl4.

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Dresden High Magnetic Field Laboratory (HLD-EMFL), Helmholtz-Zentrum Dresden-Rossendorf, 01328, Dresden, Germany.
National High Magnetic Field Laboratory, Florida State University, Tallahassee, FL, 32310, USA.
Research Facility Center for Science and Technology, Kobe University, Kobe, 657-8501, Japan.
Institute for Materials Research, Tohoku University, Sendai, 980-8578, Japan.
Dresden High Magnetic Field Laboratory (HLD-EMFL), Helmholtz-Zentrum Dresden-Rossendorf, 01328, Dresden, Germany.
Institut für Festkörper- und Materialphysik, TU Dresden, 01062, Dresden, Germany.
Molecular Photoscience Research Center, Kobe University, Kobe, 657-8501, Japan.
Department of Physical Science, Osaka Prefecture University, Osaka, 599-8531, Japan.
Department of Physics, Tokyo Institute of Technology, Tokyo, 152-8551, Japan.


Quantum triangular-lattice antiferromagnets are important prototype systems to investigate numerous phenomena of the geometrical frustration in condensed matter. Apart from highly unusual magnetic properties, they possess a rich phase diagram (ranging from an unfrustrated square lattice to a quantum spin liquid), yet to be confirmed experimentally. One major obstacle in this area of research is the lack of materials with appropriate (ideally tuned) magnetic parameters. Using Cs2CuCl4 as a model system, we demonstrate an alternative approach, where, instead of the chemical composition, the spin Hamiltonian is altered by hydrostatic pressure. The approach combines high-pressure electron spin resonance and r.f. susceptibility measurements, allowing us not only to quasi-continuously tune the exchange parameters, but also to accurately monitor them. Our experiments indicate a substantial increase of the exchange coupling ratio from 0.3 to 0.42 at a pressure of 1.8 GPa, revealing a number of emergent field-induced phases.

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