*Nat Commun ; 13(1): 2301, 2022 Apr 28.*

##### RESUMO

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.

*Phys Rev Lett ; 127(20): 207202, 2021 Nov 12.*

##### RESUMO

We directly measure the low energy excitation modes of the quantum Ising magnet LiHoF_{4} using microwave spectroscopy. Instead of a single electronic mode, we find a set of collective electronuclear modes, in which the spin-1/2 Ising electronic spins hybridize with the bath of spin-7/2 Ho nuclear spins. The lowest-lying electronuclear mode softens at the approach to the quantum critical point, even in the presence of disorder. This softening is rapidly quenched by a longitudinal magnetic field. Similar electronuclear structures should exist in other spin-based quantum Ising systems.

*Sci Rep ; 11(1): 16181, 2021 Aug 10.*

##### RESUMO

We investigate the low-temperature complex impedance of disordered insulating thin TiN and NbTiN films in the frequency region 400 Hz-1 MHz in close proximity to the superconductor-insulator transition (SIT). The frequency, temperature, and magnetic field dependencies of the real and imaginary parts of the impedance indicate that in full accord with the theoretical predictions and earlier observations, the films acquire self-induced electronic granularity and become effectively random arrays of superconducting granules coupled via Josephson links. Accordingly, the inductive component of the response is due to superconducting droplets, while the capacitive component results from the effective Josephson junctions capacitances. The impedance crosses over from capacitive to inductive behavior as films go across the transition.

*Nat Commun ; 12(1): 2779, 2021 May 13.*

##### RESUMO

While Mott insulators induced by Coulomb interactions are a well-recognized class of metal-insulator transitions, insulators purely driven by spin correlations are much less common, as the reduced energy scale often invites competition from other degrees of freedom. Here, we demonstrate a clean example of a spin-correlation-driven metal-insulator transition in the all-in-all-out pyrochlore antiferromagnet Cd2Os2O7, where the lattice symmetry is preserved by the antiferromagnetism. After the antisymmetric linear magnetoresistance from conductive, ferromagnetic domain walls is removed experimentally, the bulk Hall coefficient reveals four Fermi surfaces of both electron and hole types, sequentially departing the Fermi level with decreasing temperature below the Néel temperature, TN = 227 K. In Cd2Os2O7, the charge gap of a continuous metal-insulator transition opens only at T ~ 10 K << TN. The insulating mechanism parallels the Slater picture, but without a folded Brillouin zone, and contrasts sharply with Mott insulators and spin density waves, where the electronic gap opens above and at TN, respectively.

*Rev Sci Instrum ; 91(11): 113902, 2020 Nov 01.*

##### RESUMO

The application of giga-Pascal scale pressures has been widely used as a tool to systematically tune the properties of materials in order to access such general questions as the driving mechanisms underlying phase transitions. While there is a large and growing set of experimental tools successfully applied to high-pressure environments, the compatibility between diamond anvil cells and optical probes offers further potential for examining lattice, magnetic, and electronic states, along with their excitations. Here, we describe the construction of a highly efficient optical Raman spectrometer that enables measurements of magnetic excitations in single crystals down to energies of 9 cm-1 (1.1 meV or 13 K) at cryogenic temperatures and under pressures of tens of GPa.

*Nat Commun ; 11(1): 216, 2020 Jan 10.*

##### RESUMO

The phenomena of antisymmetric magnetoresistance and the planar Hall effect are deeply entwined with ferromagnetism. The intrinsic magnetization of the ordered state permits these unusual and rarely observed manifestations of Onsager's theorem when time reversal symmetry is broken at zero applied field. Here we study two classes of ferromagnetic materials, rare-earth magnets with high intrinsic coercivity and antiferromagnetic pyrochlores with strongly-pinned ferromagnetic domain walls, which both exhibit antisymmetric magnetoresistive behavior. By mapping out the peculiar angular variation of the antisymmetric galvanomagnetic response with respect to the relative alignments of the magnetization, magnetic field, and electrical current, we experimentally distinguish two distinct underlying microscopic mechanisms: namely, spin-dependent scattering of a Zeeman-shifted Fermi surface and anomalous electron velocities. Our work demonstrates that the anomalous electron velocity physics typically associated with the anomalous Hall effect is prevalent beyond the ρxy(Hz) channel, and should be understood as a part of the general galvanomagnetic behavior.

*Nat Commun ; 10(1): 4001, 2019 Sep 05.*

##### RESUMO

Quantum states cohere and interfere. Atoms arranged imperfectly in a solid rarely display these properties. Here we demonstrate an exception in a disordered quantum magnet that divides itself into nearly isolated subsystems. We probe these coherent spin clusters by driving the system nonlinearly and measuring the resulting hole in the linear spectral response. The Fano shape of the hole encodes the incoherent lifetime as well as coherent mixing of the localized excitations. For the Ising magnet LiHo0.045Y0.955F4, the quality factor Q for spectral holes can be as high as 100,000. We tune the dynamics by sweeping the Fano mixing parameter q through zero via the ac pump amplitude as well as a dc transverse field. The zero crossing of q is associated with a dissipationless response at the drive frequency. Identifying localized two-level systems in a dense and disordered magnet advances the search for qubit platforms emerging from strongly interacting, many-body systems.

*IUCrJ ; 6(Pt 4): 507-520, 2019 Jul 01.*

##### RESUMO

Advances in both non-resonant and resonant X-ray magnetic diffraction since the 1980s have provided researchers with a powerful tool for exploring the spin, orbital and ion degrees of freedom in magnetic solids, as well as parsing their interplay. Here, we discuss key issues for performing X-ray magnetic diffraction on single-crystal samples under high pressure (above 40â GPa) and at cryogenic temperatures (4â K). We present case studies of both non-resonant and resonant X-ray magnetic diffraction under pressure for a spin-flip transition in an incommensurate spin-density-wave material and a continuous quantum phase transition of a commensurate all-in-all-out antiferromagnet. Both cases use diamond-anvil-cell technologies at third-generation synchrotron radiation sources. In addition to the exploration of the athermal emergence and evolution of antiferromagnetism discussed here, these techniques can be applied to the study of the pressure evolution of weak charge order such as charge-density waves, antiferro-type orbital order, the charge anisotropic tensor susceptibility and charge superlattices associated with either primary spin order or softened phonons.

*Proc Natl Acad Sci U S A ; 116(23): 11201-11206, 2019 Jun 04.*

##### RESUMO

The magnetoresistance (MR) of a material is typically insensitive to reversing the applied field direction and varies quadratically with magnetic field in the low-field limit. Quantum effects, unusual topological band structures, and inhomogeneities that lead to wandering current paths can induce a cross-over from quadratic to linear MR with increasing magnetic field. Here we explore a series of metallic charge- and spin-density-wave systems that exhibit extremely large positive linear MR. By contrast to other linear MR mechanisms, this effect remains robust down to miniscule magnetic fields of tens of Oersted at low temperature. We frame an explanation of this phenomenon in a semiclassical narrative for a broad category of materials with partially gapped Fermi surfaces due to density waves.

*Nat Commun ; 9(1): 3677, 2018 09 05.*

##### RESUMO

The original PDF version of the Article contained an error in the last sentence of the author affiliation information, which incorrectly read 'Correspondence and requests for materials should be addressed to T.$.R. (e-mail: tfr@caltech.edu) or to Y.F. (e-mail: yejun@oist.jp)'. The correct version states 'T.F.R.' in place of "T.$.R.'. This has been corrected in the PDF version of the Article. The HTML version was correct from the time of publication.

*Nat Commun ; 9(1): 2953, 2018 07 27.*

##### RESUMO

Dimensionality and symmetry play deterministic roles in the laws of Nature. They are important tools to characterize and understand quantum phase transitions, especially in the limit of strong correlations between spin, orbit, charge, and structural degrees of freedom. Here, using newly-developed, high-pressure resonant X-ray magnetic and charge diffraction techniques, we have discovered a quantum critical point in Cd2Os2O7 as the all-in-all-out antiferromagnetic order is continuously suppressed to zero temperature and, concomitantly, the cubic lattice structure continuously changes from space group Fd-3m to F-43m. Surrounded by three phases of different time reversal and spatial inversion symmetries, the quantum critical region anchors two phase lines of opposite curvature, with striking departures from a mean-field form at high pressure. As spin fluctuations, lattice breathing modes, and quasiparticle excitations interact in the quantum critical region, we argue that they present the necessary components for strongly-coupled quantum criticality in this three-dimensional compound.

*Nat Commun ; 7: 13037, 2016 10 06.*

##### RESUMO

Magnetic and superconducting ground states can compete, cooperate and coexist. MnP provides a compelling and potentially generalizable example of a material where superconductivity and magnetism may be intertwined. Using a synchrotron-based non-resonant X-ray magnetic diffraction technique, we reveal a spiral spin order in MnP and trace its pressure evolution towards superconducting order via measurements in a diamond anvil cell. Judging from the magnetostriction, ordered moments vanish at the quantum phase transition as pressure increases the electron kinetic energy. Spins remain local in the disordered phase, and the promotion of superconductivity is likely to emerge from an enhanced coupling to residual spiral spin fluctuations and their concomitant suppression of phonon-mediated superconductivity. As the pitch of the spiral order varies across the 3d transition metal compounds in the MnP family, the magnetic ground state switches between antiferromagnet and ferromagnet, providing an additional tuning parameter in probing spin-fluctuation-induced superconductivity.

*Nat Commun ; 7: 11956, 2016 06 20.*

##### RESUMO

An exact mapping between quantum spins and boson gases provides fresh approaches to the creation of quantum condensates and crystals. Here we report on magnetization measurements on the dimerized quantum magnet SrCu2(BO3)2 at cryogenic temperatures and through a quantum-phase transition that demonstrate the emergence of fractionally filled bosonic crystals in mesoscopic patterns, specified by a sequence of magnetization plateaus. We apply tens of Teslas of magnetic field to tune the density of bosons and gigapascals of hydrostatic pressure to regulate the underlying interactions. Simulations help parse the balance between energy and geometry in the emergent spin superlattices. The magnetic crystallites are the end result of a progression from a direct product of singlet states in each short dimer at zero field to preferred filling fractions of spin-triplet bosons in each dimer at large magnetic field, enriching the known possibilities for collective states in both quantum spin and atomic systems.

*Rev Sci Instrum ; 86(9): 093901, 2015 Sep.*

##### RESUMO

We discuss techniques for performing continuous measurements across a wide range of pressure-field-temperature phase space, combining the milli-Kelvin temperatures of a helium dilution refrigerator with the giga-Pascal pressures of a diamond anvil cell and the Tesla magnetic fields of a superconducting magnet. With a view towards minimizing remnant magnetic fields and background magnetic susceptibility, we characterize high-strength superalloy materials for the pressure cell assembly, which allows high fidelity measurements of low-field phenomena such as superconductivity below 100 mK at pressures above 10 GPa. In situ tunability and measurement of the pressure permit experiments over a wide range of pressure, while at the same time making possible precise steps across abrupt phase transitions such as those from insulator to metal.

*J Phys Condens Matter ; 27(29): 296001, 2015 Jul 29.*

##### RESUMO

The geometrically frustrated triangular antiferromagnet Gadolinium Gallium Garnet (Gd3Ga5O12 or GGG) exhibits a rich mix of short-range order and isolated quantum states. We investigate the effects of up to 1% neodymium substitution for gallium on the ac magnetic response at temperatures below 1 K in both the linear and nonlinear regimes. Substitutional disorder actually drives the system toward a more perfectly frustrated state, apparently compensating for the effects of imperfect gadolinium/gallium stoichiometry, while at the same time more closely demarcating the boundaries of isolated, coherent clusters composed of hundreds of spins. Optical measurements of the local Nd environment substantiate the picture of an increased frustration index with doping.

*Proc Natl Acad Sci U S A ; 112(5): E383-4, 2015 Feb 03.*

*Proc Natl Acad Sci U S A ; 111(40): 14372-7, 2014 Oct 07.*

##### RESUMO

Quantum spins placed on the corners of a square lattice can dimerize and form singlets, which then can be transformed into a magnetic state as the interactions between dimers increase beyond threshold. This is a strictly 2D transition in theory, but real-world materials often need the third dimension to stabilize long-range order. We use high pressures to convert sheets of Cu(2+) spin 1/2 dimers from local singlets to global antiferromagnet in the model system SrCu2(BO3)2. Single-crystal neutron diffraction measurements at pressures above 5 GPa provide a direct signature of the antiferromagnetic ordered state, whereas high-resolution neutron powder and X-ray diffraction at commensurate pressures reveal a tilting of the Cu spins out of the plane with a critical exponent characteristic of 3D transitions. The addition of anisotropic, interplane, spin-orbit terms in the venerable Shastry-Sutherland Hamiltonian accounts for the influence of the third dimension.

*Nat Commun ; 5: 4218, 2014 Jun 18.*

##### RESUMO

Pressure can transform a transparent material into an opaque one, quench the moments in a magnet and force solids to flow like liquids. At 15 GPa, the pressure found 500 km below the earth's surface, the semiconductors silicon and germanium superconduct. Yet, at this same pressure, we show here that the magnetism in metallic GdSi remains completely robust even as it shrinks by one-seventh of its volume. Non-resonant X-ray magnetic diffraction in a specially designed diamond anvil cell, combined with band structure calculations, reveal the stability of the incommensurate spin density wave, which can be traced to a persistently nested portion of the Fermi surface that becomes increasingly one-dimensional under pressure. A cooperative interaction between nested, itinerant spins and local magnetic moments provides the organizing principle for the modulated magnetic order, salient both for its insights into the role of topology in ordered states and its potential functionality.

*Rev Sci Instrum ; 85(3): 033901, 2014 Mar.*

##### RESUMO

We present the design of an efficient bellows-controlled diamond anvil cell that is optimized for use inside the bores of high-field superconducting magnets in helium-3 cryostats, dilution refrigerators, and commercial physical property measurement systems. Design of this non-magnetic pressure cell focuses on in situ pressure tuning and measurement by means of a helium-filled bellows actuator and fiber-coupled ruby fluorescence spectroscopy, respectively. We demonstrate the utility of this pressure cell with ac susceptibility measurements of superconducting, ferromagnetic, and antiferromagnetic phase transitions to pressures exceeding 8 GPa. This cell provides an opportunity to probe charge and magnetic order continuously and with high resolution in the three-dimensional Magnetic Field-Pressure-Temperature parameter space.

*Proc Natl Acad Sci U S A ; 111(10): 3689-94, 2014 Mar 11.*

##### RESUMO

The degree of contact between a system and the external environment can alter dramatically its proclivity to quantum mechanical modes of relaxation. We show that controlling the thermal coupling of cubic-centimeter-sized crystals of the Ising magnet LiHo(x)Y(1-x)F4 to a heat bath can be used to tune the system between a glassy state dominated by thermal excitations over energy barriers and a state with the hallmarks of a quantum spin liquid. Application of a magnetic field transverse to the Ising axis introduces both random magnetic fields and quantum fluctuations, which can retard and speed the annealing process, respectively, thereby providing a mechanism for continuous tuning between the destination states. The nonlinear response of the system explicitly demonstrates quantum interference between internal and external relaxation pathways.