Pressure-tuning of α-RuCl3 towards a quantum spin liquid

The layered material α-RuCl₃ is a promising candidate to realize the Kitaev quantum spin liquid (QSL) state. However, at ambient pressure, deviations from the perfect Kitaev geometry prevent the existence of the QSL state at low temperatures. Here we present the discovery of a pressure-induced high-symmetry phase in α-RuCl₃, which creates close to ideal conditions for the emergence of a QSL. Employing a novel approach based on Bragg and diffuse scattering of synchrotron radiation, we reveal a pressure-induced reorganization of the RuCl₃-layers. Most importantly, this reorganization affects the structure of the layers themselves, which acquire a high trigonal symmetry. For this trigonal phase the largest ratio between the Kitaev (K) and the Heisenberg exchange (J) ever encountered is found: K/J = 124. Additionally, we demonstrate that this phase can also be stabilized by a slight biaxial pressure. This not only resolves the conflicting reports of low-temperature structures in the literature, but also facilitates the investigation of the high-symmetry phase and its potential QSL using a range of experimental techniques.