Pressure-tuning the quantum spin Hamiltonian of the triangular lattice antiferromagnet Cs 2 CuCl 4

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. Theoretical studies of quantum magnetism typically assume idealised lattices with freely tunable parameters, which are difficult to realise experimentally. Zvyagin et al. perform challenging measurements at high pressures to tune and to accurately monitor the exchange parameters of a triangular lattice antiferromagnet.