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

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.

Emergent bound states and impurity pairs in chemically doped Shastry-Sutherland system.

Impurities often play a defining role in the ground states of frustrated quantum magnets. Studies of their effects are crucial in understanding of the phase diagram in these materials. SrCu2(BO3)2, an experimental realization of the Shastry-Sutherland (SS) lattice, provides a unique model system for such studies using both experimental and numerical approaches. Here we report effects of impurities on the crystals of bound states, and doping-induced emergent ground states in Mg-doped SrCu2(BO3)2, which remain stable in high magnetic fields. Using four complementary magnetometry techniques and theoretical simulations, a rich impurity-induced phenomenology at high fields is discovered. The results demonstrate a rare example in which even a small doping concentration interacts strongly with both triplets and bound states of triplets, and thus plays a significant role in the magnetization process even at high magnetic fields. Our findings provide insights into the study of impurity effects in geometrically frustrated quantum magnets.

Real-space localization and quantification of hole distribution in chain-ladder Sr3Ca11Cu24O41 superconductor.

Understanding the physical properties of the chain-ladder Sr3Ca11Cu24O41 hole-doped superconductor has been precluded by the unknown hole distribution among chains and ladders. We use electron energy-loss spectrometry (EELS) in a scanning transmission electron microscope (STEM) at atomic resolution to directly separate the contributions of chains and ladders and to unravel the hole distribution from the atomic scale variations of the O-K near-edge structures. The experimental data unambiguously demonstrate that most of the holes lie within the chain layers. A quantitative interpretation supported by inelastic scattering calculations shows that about two holes are located in the ladders, and about four holes in the chains, shedding light on the electronic structure of Sr3Ca11Cu24O41. Combined atomic resolution STEM-EELS and inelastic scattering calculations is demonstrated as a powerful approach toward a quantitative understanding of the electronic structure of cuprate superconductors, offering new possibilities for elucidating their physical properties.

Supercooled spin liquid state in the frustrated pyrochlore Dy2Ti2O7.

A "supercooled" liquid develops when a fluid does not crystallize upon cooling below its ordering temperature. Instead, the microscopic relaxation times diverge so rapidly that, upon further cooling, equilibration eventually becomes impossible and glass formation occurs. Classic supercooled liquids exhibit specific identifiers including microscopic relaxation times diverging on a Vogel-Tammann-Fulcher (VTF) trajectory, a Havriliak-Negami (HN) form for the dielectric function ε(ω, T), and a general Kohlrausch-Williams-Watts (KWW) form for time-domain relaxation. Recently, the pyrochlore Dy2Ti2O7 has become of interest because its frustrated magnetic interactions may, in theory, lead to highly exotic magnetic fluids. However, its true magnetic state at low temperatures has proven very difficult to identify unambiguously. Here, we introduce high precision, boundary-free magnetization transport techniques based upon toroidal geometries and gain an improved understanding of the time- and frequency-dependent magnetization dynamics of Dy2Ti2O7. We demonstrate a virtually universal HN form for the magnetic susceptibility χ (ω, T), a general KWW form for the realtime magnetic relaxation, and a divergence of the microscopic magnetic relaxation rates with the VTF trajectory. Low-temperature Dy2Ti2O7 therefore exhibits the characteristics of a supercooled magnetic liquid. One implication is that this translationally invariant lattice of strongly correlated spins may be evolving toward an unprecedented magnetic glass state, perhaps due to many-body localization of spin.

Magnetic nanopantograph in the SrCu2(BO3)2 Shastry-Sutherland lattice.

Magnetic materials having competing, i.e., frustrated, interactions can display magnetism prolific in intricate structures, discrete jumps, plateaus, and exotic spin states with increasing applied magnetic fields. When the associated elastic energy cost is not too expensive, this high potential can be enhanced by the existence of an omnipresent magnetoelastic coupling. Here we report experimental and theoretical evidence of a nonnegligible magnetoelastic coupling in one of these fascinating materials, SrCu2(BO3)2 (SCBO). First, using pulsed-field transversal and longitudinal magnetostriction measurements we show that its physical dimensions, indeed, mimic closely its unusually rich field-induced magnetism. Second, using density functional-based calculations we find that the driving force behind the magnetoelastic coupling is the CuOCu superexchange angle that, due to the orthogonal Cu(2+) dimers acting as pantographs, can shrink significantly (0.44%) with minute (0.01%) variations in the lattice parameters. With this original approach we also find a reduction of ∼ 10% in the intradimer exchange integral J, enough to make predictions for the highly magnetized states and the effects of applied pressure on SCBO.

Equation of state of zircon- and scheelite-type dysprosium orthovanadates: a combined experimental and theoretical study.

Dysprosium orthovanadate, DyVO4, belongs to a family of zircon-type orthovanadates showing a phase transition to scheelite-type structures at moderate pressures below 10 GPa. In the present study, the equations of state (EOSs) for both these phases were determined for the first time using high-pressure x-ray diffraction experiments and ab initio calculations based on the density functional theory. Structural parameters for scheelite-type DyVO4 were calculated from x-ray powder diffraction data as well. The high-pressure experiments were performed under pseudo-hydrostatic conditions at pressures up to 8.44 GPa and 5.5 GPa for the stable zircon-type and metastable (quenched) scheelite-type samples, respectively. Assuming as a compression model the Birch-Murnaghan EOS, we obtained the EOS parameters for both phases. The experimental bulk moduli (K0) for zircon-type and scheelite-type DyVO4 are 118(4) GPa and 153(6) GPa, respectively. Theoretical equations of state were determined by ab initio calculations using the PBE exchange-correlation energy functional of Perdew, Burke, and Ernzerhof. These calculations provide K0 values of 126.1 GPa and 142.9 GPa for zircon-type and scheelite-type DyVO4, respectively. The reliability of the present experimental and theoretical results is supported by (i) the consistency between the values yielded by the two methods (the discrepancy in K0 is as low as about 7% for each of the studied polymorphs) and (ii) their similarity to results obtained under similar compression conditions (hydrostatic or pseudo-hydrostatic) for other rare-earth orthovanadates, such as YVO4 and TbVO4.