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arXiv:2107.02929 · Nature Communications

Discovery of quantum phases in the Shastry-Sutherland compound SrCu2(BO3)2 under extreme conditions of field and pressure

Zhenzhong Shi, Sachith Dissanayake, Philippe Corboz, William Steinhardt, David E Graf, D. M. Silevitch, H. A. Dabkowska, T. F. Rosenbaum, Frédéric Mila, Sara Haravifard

Published Apr 28, 2022• 69 citations
arXivHTMLPDF

Abstract

Abstract The 2-dimensional layered oxide material SrCu2(BO3)2, long studied as a realization of the Shastry-Sutherland spin topology, exhibits a range of intriguing physics as a function of both hydrostatic pressure and magnetic field, with a still debated intermediate plaquette phase appearing at approximately 20 kbar and a possible deconfined critical point at higher pressure. Here, we employ a tunnel diode oscillator (TDO) technique to probe the behavior in the combined extreme conditions of high pressure, high magnetic field, and low temperature. We reveal an extensive phase space consisting of multiple magnetic analogs of the elusive supersolid phase and a magnetization plateau. In particular, a 10 × 2 supersolid and a 1/5 plateau, identified by infinite Projected Entangled Pair States (iPEPS) calculations, are found to rely on the presence of both magnetic and non-magnetic particles in the sea of dimer singlets. These states are best understood as descendants of the full-plaquette phase, the leading candidate for the intermediate phase of SrCu2(BO3)2.

DOI
10.1038/s41467-022-30036-w

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Abstract The 2-dimensional layered oxide material SrCu2(BO3)2, long studied as a realization of the Shastry-Sutherland spin topology, exhibits a range of intriguing physics as a function of both hydrostatic pressure and magnetic field, with a still debated intermediate plaquette phase appearing at approximately 20 kbar and a possible deconfined critical point at higher pressure. Here, we employ a tunnel diode oscillator (TDO) technique to probe the behavior in the combined extreme conditions of high pressure, high magnetic field, and low temperature. We reveal an extensive phase space consisting of multiple magnetic analogs of the elusive supersolid phase and a magnetization plateau. In particular, a 10 × 2 supersolid and a 1/5 plateau, identified by infinite Projected Entangled Pair States (iPEPS) calculations, are found to rely on the presence of both magnetic and non-magnetic particles in the sea of dimer singlets. These states are best understood as descendants of the full-plaquette phase, the leading candidate for the intermediate phase of SrCu2(BO3)2.
Abstract Under magnetic fields, quantum magnets often undergo exotic phase transitions with various kinds of order. The discovery of a sequence of fractional magnetization plateaus in the Shastry-Sutherland compound SrCu 2 (BO 3 ) 2 has played a central role in the high-field research on quantum materials, but so far this system could only be probed up to half the saturation value of the magnetization. Here, we report the first experimental and theoretical investigation of this compound up to the saturation magnetic field of 140 T and beyond. Using ultrasound and magnetostriction techniques combined with extensive tensor-network calculations (iPEPS), several spin-supersolid phases are revealed between the 1/2 plateau and saturation (1/1 plateau). Quite remarkably, the sound velocity of the 1/2 plateau exhibits a drastic decrease of -50%, related to the tetragonal-to-orthorhombic instability of the checkerboard-type magnon crystal. The unveiled nature of this paradigmatic quantum system is a new milestone for exploring exotic quantum states of matter emerging in extreme conditions.
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_22​(BO3_33​)2_22​. However, the nature of the plaquette-singlet phase in SrCu2_22​(BO3_33​)2_22​ remains unresolved, and with it the identification of the DQCP symmetry from among several theoretical scenarios. Here we perform detailed high-pressure 11^{11}11B NMR studies to reveal the presence of both the full-plaquette (FP) and empty-plaquette (EP) phases in SrCu2_22​(BO3_33​)2_22​, 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∝T0.61/T_1 \propto T^{0.6}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_22​(BO3_33​)2_22​.
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}.
The Shastry-Sutherland model is an effective model of the layered material SrCu_{2}(BO_{3})_{2}, which exhibits an extremely rich phase diagram as a function of pressure and magnetic field. Motivated by the recent controversy regarding its phase diagram at zero magnetic field, we perform large-scale simulations based on infinite projected entangled-pair states, a two-dimensional tensor network Ansatz to represent the ground state directly in the thermodynamic limit. By employing the latest optimization techniques, we obtain variational states with lower energy than previous results obtained from other methods. Using systematic extrapolations to the exact infinite bond dimension limit, our simulations reveal a narrow quantum spin liquid phase between the plaquette and antiferromagnetic phases in the range 0.785(5)≤J^{'}/J≤0.82(1).
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.
Building on the growing evidence based on NMR, magnetization, neutron scattering, electron spin resonance, and specific heat that, under pressure, SrCu2(BO3)2{\mathrm{SrCu}}_{2}{({\mathrm{BO}}_{3})}_{2}SrCu2​(BO3​)2​ has an intermediate phase between the dimer and the N\'eel phase, we study the competition between two candidate phases in the context of a minimal model that includes two types of intra- and interdimer interactions without enlarging the unit cell. We show that the empty plaquette phase of the Shastry-Sutherland model is quickly replaced by a quasi-one-dimensional full plaquette phase when intra- and/or interdimer couplings take different values, and that this full plaquette phase is in much better agreement with available experimental data than the empty plaquette one.