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.
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.
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.
Motivated by the remarkable properties of SrCu2(BO3) 2 in a magnetic field, we use perturbative continuous unitary transformations to determine the magnetization plateaux of the Shastry-Sutherland model, unveiling an unexpected sequence of plateaux progressively appearing at 2/9, 1/6, 1/9, and 2/15 upon increasing the interdimer coupling. We predict that a 1/6 plateau should be present in SrCu2(BO3)2, even if residual interactions beyond the Shastry-Sutherland are strong enough to modify the other plateaux below 1/3. The method is extended to calculate the magnetization profile within the plateaux, leading to a local structure around triplons that agrees with NMR results on SrCu2(BO3) 2.
We present magnetic torque measurements on the Shastry-Sutherland quantum spin system SrCu 2 (BO 3 ) 2 in fields up to 31 T and temperatures down to 50 mK. A new quantum phase is observed in a 1 T field range above the 1/8 plateau, in agreement with recent NMR results. Since the presence of the DM coupling precludes the existence of a true Bose-Einstein condensation and the formation of a supersolid phase in SrCu 2 (BO 3 ) 2 , the exact nature of the new phase in the vicinity of the plateau remains to be explained. Comparison between magnetization and torque data reveals a huge contribution of the Dzyaloshinskii-Moriya interaction to the torque response. Finally, our measurements demonstrate the existence of a supercooling due to adiabatic magnetocaloric effects in pulsed field experiments.
Field-induced bound-state condensation and spin-nematic phase in SrCu2(BO3)2 revealed by neutron scattering up to 25.9 T
Bose-Einstein condensation (BEC) underpins exotic forms of order ranging from superconductivity to superfluid 4 He. In quantum magnetic materials, ordered phases induced by an applied magnetic field can be described as the BEC of magnon excitations. With sufficiently strong magnetic frustration, exemplified by the system SrCu2(BO3)2 , no clear magnon BEC is observed and the complex spectrum of multi-magnon bound states may allow a different type of condensation, but the high fields required to probe this physics have remained a barrier to detailed investigation. Here we exploit the first purpose-built high-field neutron scattering facility to measure the spin excitations of SrCu2(BO3)2 up to 25.9 T and use cylinder matrix-product-states (MPS) calculations to reproduce the experimental spectra with high accuracy. Multiple unconventional features point to a condensation of S=2 bound states into a spin-nematic phase, including the gradients of the one-magnon branches, the presence of many novel composite two- and three-triplon excitations and the persistence of a one-magnon spin gap. This gap reflects a direct analogy with superconductivity, suggesting that the spin-nematic phase in SrCu2(BO3)2 is best understood as a condensate of bosonic Cooper pairs. Our results underline the wealth of unconventional states yet to be found in frustrated quantum magnetic materials under extreme conditions.
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}.
We study a generalized Shastry-Sutherland model for the material SrCu2(BO3)(2). Along a line in the parameter space, we show rigorously that the model has a first-order phase transition between dimerized and Neel-ordered ground states. Furthermore, when a magnetic field is applied in the dimerized phase, magnetization plateaus develop at commensurate values of the magnetization. We also discuss various aspects of the phase diagram and properties of this model away from this exactly soluble line, which include gap-closing continuous transitions between dimerized and magnetically ordered phases.