We report heat capacity measurements of SrCu_{2}(BO_{3})_{2} under high pressure along with simulations of relevant quantum spin models and map out the (P,T) phase diagram of the material. We find a first-order quantum phase transition between the low-pressure quantum dimer paramagnet and a phase with signatures of a plaquette-singlet state below T=2 K. At higher pressures, we observe a transition into a previously unknown antiferromagnetic state below 4 K. Our findings can be explained within the two-dimensional Shastry-Sutherland quantum spin model supplemented by weak interlayer couplings. The possibility to tune SrCu_{2}(BO_{3})_{2} between the plaquette-singlet and antiferromagnetic states opens opportunities for experimental tests of quantum field theories and lattice models involving fractionalized excitations, emergent symmetries, and gauge fluctuations.
We report heat capacity measurements of SrCu_{2}(BO_{3}){2} under high pressure along with simulations of relevant quantum spin models and map out the (P,T) phase diagram of the material. We find a first-order quantum phase transition between the low-pressure quantum dimer paramagnet and a phase with signatures of a plaquette-singlet state below T=2 K. At higher pressures, we observe a transition into a previously unknown antiferromagnetic state below 4 K. Our findings can be explained within the two-dimensional Shastry-Sutherland quantum spin model supplemented by weak interlayer couplings. The possibility to tune SrCu{2}(BO_{3})_{2} between the plaquette-singlet and antiferromagnetic states opens opportunities for experimental tests of quantum field theories and lattice models involving fractionalized excitations, emergent symmetries, and gauge fluctuations.
The deconfined quantum critical point (DQCP) has become a central open concept in the physics of quantum matter, and its proposed presence in the Shastry-Sutherland model was followed by the experimental observation of at least a minimal DQC scenario induced by an applied magnetic field in SrCu2(BO3)2. However, the nature of the plaquette-singlet phase in SrCu2(BO3)2 remains unresolved, and with it the identification of the DQCP symmetry from among several theoretical scenarios. Here we perform detailed high-pressure 11B NMR studies to reveal the presence of both the full-plaquette (FP) and empty-plaquette (EP) phases in SrCu2(BO3)2, phase-separated at a first-order, pressure-driven transition with a volume-fraction effect. The field-driven transition from the EP to the antiferromagnetic (AFM) phase complements our previous observations of the FP--AFM transition, with both showing deconfined quantum criticality, while the scaling of the spin-lattice relaxation rate near the EP--AFM transition, 1/T1∝T0.6, suggests a DQCP governed by a different universality class. We discuss possible extensions to the Shastry-Sutherland model that account for these pressure and field effects. The expanded phase space we discover mandates an SO(5) DQCP symmetry, and hence our results take an important step towards a complete understanding of deconfined quantum criticality in SrCu2(BO3)2.
The two-dimensional quantum spin model proposed by Shastry and Sutherland more than four decades ago is notable for its realization in SrCu2(BO3)2. Here, the authors present numerical evidence of a gapless spin liquid phase in the model and discuss its connection to a deconfined quantum critical point. The new phase exists in a parameter regime where recent high-pressure heat capacity measurements on SrCu2(BO3)2 did not detect any low-temperature order, in contrast to the antiferromagnetic and plaquette-singlet phases existing at higher and lower pressures, respectively. Thus, the elusive spin liquid may exist in SrCu2(BO3)2.
The layered material SrCu _2 2 (BO _3 3 ) _2 2 has long been studied because of its fascinating physics in a magnetic field and under pressure. Many of its properties are remarkably well described by the Shastry-Sutherland model (SSM) - a two-dimensional frustrated spin system. However, the extent of the intermediate plaquette phase discovered in SrCu _2 2 (BO _3 3 ) _2 2 under pressure is significantly smaller than predicted in theory, which is likely due to the weak interlayer coupling that is present in the material but neglected in the model. Using state-of-the-art tensor network methods we study the SSM with a weak interlayer coupling and show that the intermediate plaquette phase is destabilized already at a smaller value around J''/J\sim0.04-0.05 J ″ / J ∼ 0.04 − 0.05 than previously predicted from series expansion. Based on our phase diagram we estimate the effective interlayer coupling in SrCu _2 2 (BO _3 3 ) _2 2 to be around J''/J\sim 0.027 J ″ / J ∼ 0.027 at ambient pressure.
High-pressure and high-field electron spin resonance (ESR) measurements have been performed on a single crystal of the orthogonal-dimer spin system SrCu2(BO3)2. With frequencies below 1 THz, ESR signals associated with transitions from the singlet ground state to the one-triplet excited states and the two-triplet bound state were observed at pressures up to 2.1 GPa. We obtained directly the pressure dependence of the gap energies, finding a clear first-order phase transition at Pc=1.85±0.05 GPa. By comparing this pressure dependence with the calculated excitation energies obtained from an exact diagonalization, we determined the precise pressure dependence for inter- (J′) and intra-dimer (J) exchange interactions considering the Dzyaloshinski-Moriya interaction. Thus this system undergoes a first-order quantum phase transition from the dimer singlet phase to a plaquette singlet phase above the ratio (J′/J)c=0.660±0.003.
Recent experiments [Guo et al., Phys. Rev. Lett. 124 206602 (2020)] on thermodynamic properties of the frustrated layered quantum magnet SrCu2(BO3)2 — the Shastry–Sutherland material — have provided strong evidence for a low-temperature phase transition between plaquette-singlet and antiferromagnetic order as a function of pressure. Further motivated by the recently discovered unusual first-order quantum phase transition with an apparent emergent O(4) symmetry of the antiferromagnetic and plaquette-singlet order parameters in a two-dimensional “checkerboard J-Q” quantum spin model [Zhao et al., Nat. Phys. 15 678 (2019)], we here study the same model in the presence of weak inter-layer couplings. Our focus is on the evolution of the emergent symmetry as the system crosses over from two to three dimensions and the phase transition extends from strictly zero temperature in two dimensions up to finite temperature as expected in SrCu2(BO3)2. Using quantum Monte Carlo simulations, we map out the phase boundaries of the plaquette-singlet and antiferromagnetic phases, with particular focus on the triple point where these two ordered phases meet the paramagnetic phase for given strength of the inter-layer coupling. All transitions are first-order in the neighborhood of the triple point. We show that the emergent O(4) symmetry of the coexistence state breaks down clearly when the interlayer coupling becomes sufficiently large, but for a weak coupling, of the magnitude expected experimentally, the enlarged symmetry can still be observed at the triple point up to significant length scales. Thus, it is likely that the plaquette-singlet to antiferromagnetic transition in SrCu2(BO3)2 exhibits remnants of emergent O(4) symmetry, which should be observable due to additional weakly gapped Goldstone modes.
Inspired by recent experimental measurements [Guo et al., Phys. Rev. Lett. 124, 206602 (2020PRLTAO0031-900710.1103/PhysRevLett.124.206602); Jiménez et al., Nature (London) 592, 370 (2021)NATUAS0028-083610.1038/s41586-021-03411-8] on frustrated quantum magnet SrCu_{2}(BO_{3})_{2} under combined pressure and magnetic fields, we study the related spin-1/2 Shastry-Sutherland model using state-of-the-art tensor network methods. By calculating thermodynamics, correlations, and susceptibilities, we find, in zero magnetic field, not only a line of first-order dimer-singlet to plaquette-singlet phase transition ending with a critical point, but also signatures of the ordered plaquette-singlet transition with its critical end point terminating on this first-order line. Moreover, we uncover prominent magnetic barocaloric responses, a novel type of quantum correlation induced cooling effect, in the strongly fluctuating supercritical regime. Under finite fields, we identify a quantum phase transition from the plaquette-singlet phase to the spin supersolid phase that breaks simultaneously lattice translational and spin rotational symmetries. The present findings on the Shastry-Sutherland model are accessible in current experiments and would shed new light on the critical and supercritical phenomena in the archetypal frustrated quantum magnet SrCu_{2}(BO_{3})_{2}.