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Quantum triangular-lattice antiferromagnets are important prototype systemsto investigate phenomena of the geometrical frustration in condensed matter.Apart from highly unusual magnetic properties, they possess a rich phasediagram (ranging from an unfrustrated square lattice to a quantum spin liquid),yet to be confirmed experimentally. One major obstacle in this area of researchis the lack of materials with appropriate (ideally tuned) magnetic parameters.Using Cs$_2$CuCl$_4$ as a model system, we demonstrate an alternative approach,where, instead of the chemical composition, the spin Hamiltonian is altered byhydrostatic pressure. The approach combines high-pressure electron spinresonance and magnetization measurements, allowing us not only toquasi-continuously tune the exchange parameters, but also to accurately monitorthem. Our experiments indicate a substantial increase of the exchange couplingratio from 0.3 to 0.42 at a pressure of 1.8 GPa, revealing a number of emergentfield-induced phases.

Pressure-tuning the quantum spin Hamiltonian of the triangular lattice antiferromagnet Cs$_2$CuCl$_4$