4-spin plaquette singlet state in the Shastry–Sutherland compound SrCu₂(BO₃)₂

The study of interacting spin systems is of fundamental importance for modern condensed-matter physics. On frustrated lattices, magnetic exchange interactions cannot be simultaneously satisfied, and often give rise to competing exotic ground states. The frustrated two-dimensional Shastry–Sutherland lattice realized by SrCu₂(BO₃)₂ is an important test to our understanding of quantum magnetism. It was constructed to have an exactly solvable 2-spin dimer singlet ground state within a certain range of exchange parameters and frustration. While the exact dimer state and the antiferromagnetic order at both ends of the phase diagram are well known, the ground state and spin correlations in the intermediate frustration range have been widely debated. We report here the first experimental identification of the conjectured plaquette singlet intermediate phase in SrCu₂(BO₃)₂. It is observed by inelastic neutron scattering after pressure tuning at 21.5kbar. This gapped singlet state leads to a transition to an ordered Neel state above 40 kbar, which can realize a deconfined quantum critical point.