arXiv subjects

Bruce Normand

Publications and source records attributed to Bruce Normand.

At least 19 recordsLinked to original sources

arXiv2025

Universal dynamics of a pair condensate

Pair condensates appear in multiple branches of physics, always introducing exotic phenomena. The pair condensate in quantum magnetism is the spin nematic, whose static (quadrupolar) order is difficult to access, favoring dynamical probes. Here, we perform high-resolution neutron spectroscopy to obtain direct evidence for the presence of two spin-nematic phases induced in the triangular-lattice antiferromagnet Na2BaNi(PO4)2 by controlling the applied magnetic field. By combining precise experiments with quantitative theoretical and numerical analysis, we identify universal dynamics arising from the pair condensate. We show explicitly how the gapless Goldstone mode influences the dispersion and induces Cherenkov-like velocity-selective decay of the gapped single-quasiparticle band. These common spectral features shed new light on spin-nematic dynamics and underline the universal phenomenology shared by pair condensates across different physical systems.

cond-mat.str-el↗

arXiv2024

Coexistence of insulator-like paramagnon and metallic spin-orbit exciton modes in SrIrO$_3$

We probe the spectrum of elementary excitations in SrIrO$_3$ by using heterostructured [(SrIrO$_3$)$_m$/(SrTiO$_3$)$_l$] samples to approach the bulk limit. Our resonant inelastic x-ray scattering (RIXS) measurements at the Ir $L_3$-edge reveal a robust low-lying collective magnetic mode with an antiferromagnetic (AF) dispersion similar to the insulators Sr$_2$IrO$_4$ and Sr$_3$Ir$_2$O$_7$, albeit with a large gap and much larger linewidth. At higher energies we find the spin-orbit exciton, also strongly broadened, but with an inverted dispersion and doubled periodicity that are controlled by the charge hopping. These results demonstrate that the AF paramagnon persists, somewhat counterintuitively, far into the metallic regime of the insulator-metal transition driven by the degree of confinement in the heterostructure. We conclude that these two excitations, which are contrasting but coexisting hallmarks of strong AF pseudospin and charge fluctuations in a spin-orbit-coupled Mott-Slater material, are properties intrinsic to the ground state of semimetallic perovskite SrIrO$_3$.

cond-mat.str-el↗

arXiv2024

Two Plaquette-Singlet Phases and Emergent SO(5) Deconfined Quantum Criticality in SrCu2(BO3)2

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 SrCu$_2$(BO$_3$)$_2$. However, the nature of the plaquette-singlet phase in SrCu$_2$(BO$_3$)$_2$ remains unresolved, and with it the identification of the DQCP symmetry from among several theoretical scenarios. Here we perform detailed high-pressure $^{11}$B NMR studies to reveal the presence of both the full-plaquette (FP) and empty-plaquette (EP) phases in SrCu$_2$(BO$_3$)$_2$, 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, $1/T_1 \propto T^{0.6}$, 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 SrCu$_2$(BO$_3$)$_2$.

cond-mat.str-el↗

arXiv2024

Fingerprints of supersymmetric spin and charge dynamics observed by inelastic neutron scattering

Supersymmetry is an algebraic property of a quantum Hamiltonian that, by giving every boson a fermionic superpartner and vice versa, may underpin physics beyond the Standard Model. Fractional bosonic and fermionic quasiparticles are familiar in condensed matter, as in the spin and charge excitations of the $t$-$J$ model describing electron dynamics in one-dimensional materials, but this type of symmetry is almost unknown. However, the triplet excitations of a quantum spin ladder in an applied magnetic field provide a supersymmetric analogue of the $t$-$J$ chain. Here we perform neutron spectroscopy on the spin-ladder compounds (C$_5$D$_{12}$N)$_2$CuBr$_4$ and (C$_5$D$_{12}$N)$_2$CuCl$_4$ over a range of applied fields and temperatures, and apply matrix-product-state methods to the ladder and equivalent chain models. From the momentum-resolved dynamics of a single charge-like excitation in a bath of fractional spins, we find essential differences in thermal broadening between the supersymmetric and non-supersymmetric sectors. The persistence of a strict zone-centre pole at all temperatures constitutes an observable consequence of supersymmetry that marks the beginning of supersymmetric studies in experimental condensed matter.

cond-mat.str-el↗

arXiv2023

Superconductivity in nickelate and cuprate superconductors with strong bilayer coupling

The discovery of superconductivity at 80 K under high pressure in La$_3$Ni$_2$O$_7$ presents the groundbreaking confirmation that high-$T_c$ superconductivity is a property of strongly correlated materials beyond cuprates. We use density functional theory (DFT) calculations of the band structure of La$_3$Ni$_2$O$_7$ under pressure to verify that the low-energy bands are composed almost exclusively of Ni 3$d_{x^2-y^2}$ and O 2$p$ orbitals. We deduce that the Ni 3$d_{z^2}$ orbitals are essentially decoupled by the geometry of the high-pressure structure and by the effect of the Ni Hund coupling being strongly suppressed, which results from the enhanced interlayer antiferromagnetic interaction between $d_{z^2}$ orbitals and the strong intralayer hybridization of the $d_{x^2-y^2}$ orbitals with O 2$p$. By introducing a tight-binding model for the Fermi surfaces and low-energy dispersions, we arrive at a bilayer $t$-$t_\perp$-$J$ model with strong interlayer hopping, which we show is a framework unifying La$_3$Ni$_2$O$_7$ with cuprate materials possessing similar band structures, particularly the compounds La$_2$CaCu$_2$O$_6$, Pb$_2$Sr$_2$YCu$_3$O$_8$, and EuSr$_2$Cu$_2$NbO$_8$. We use a renormalized mean-field theory to show that these systems should have ($d$+$is$)-wave superconductivity, with a dominant $d$-wave component and the high $T_c$ driven by the near-optimally doped $\beta$ band, while the $\alpha$ band adds an $s$-wave component that should lead to clear experimental signatures.

cond-mat.supr-con↗

arXiv2023

Emergent criticality in fully frustrated quantum magnets

Phase transitions in condensed matter are often linked to exotic emergent properties. We study the fully frustrated bilayer Heisenberg antiferromagnet to demonstrate that an applied magnetic field creates a novel emergent criticality. The quantum phase diagram contains four states, the DS (singlets on every interlayer dimer bond), DTAF (all triplets with antiferromagnetic order), TC (a singlet-triplet checkerboard) and FM (saturated ferromagnet). The thermal phase diagram is dominated by a wall of discontinuities extending from the zero-field DTAF-DS transition to a quantum critical endpoint where the field drives the DTAF and TC into the FM. This first-order wall is terminated at finite temperatures by a line of critical points, where the Berezinskii-Kosterlitz-Thouless (BKT) transition of the DTAF and the thermal Ising transition of the TC also terminate. We demonstrate by quantum Monte Carlo simulations that the BKT transition does not change the Ising nature of the DTAF-DS critical line. By contrast, the combination of symmetries merging on the multicritical DTAF-TC line leads to a 4-state Potts universality not contained in the microscopic Hamiltonian, which we associate with the Ashkin-Teller model. Our results represent a systematic step in understanding emergent phenomena in quantum magnetic materials including the ``Shastry-Sutherland compound'' SrCu$_2$(BO$_3$)$_2$.

cond-mat.str-el↗

arXiv2023

Ultrafast Frustration-Breaking and Magnetophononic Driving of Singlet Excitations in a Quantum Magnet

Ideal magnetic frustration forms the basis for the emergence of exotic quantum spin states that are entirely nonmagnetic. Such singlet spin states are the defining feature of the Shastry-Sutherland model, and of its faithful materials realization in the quantum antiferromagnet SrCu$_2$(BO$_3$)$_2$. To address these states on ultrafast timescales, despite their lack of any microscopic order parameter, we introduce a nonlinear magnetophononic mechanism to alter the quantum spin dynamics by driving multiple optical phonon modes coherently and simultaneously. We apply intense terahertz pulses to create a nonequilibrium modulation of the magnetic interactions that breaks the ideal frustration of SrCu$_2$(BO$_3$)$_2$, such that previously forbidden physics can be driven in a coherent manner. Specifically, this driving populates a purely magnetic excitation, the singlet branch of the two-triplon bound state, by resonance with the difference frequency of two pumped phonons. Our results demonstrate how light-driven phonons can be used for the ultrafast and selective manipulation of interactions in condensed matter, even at frequencies far from those of the pump spectrum, offering valuable additional capabilities for the dynamical control of quantum many-body phenomena.

cond-mat.str-el↗

arXiv2023

Field-induced bound-state condensation and spin-nematic phase in SrCu$_2$(BO$_3$)$_2$ 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 SrCu$_2$(BO$_3$)$_2$ , 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 SrCu$_2$(BO$_3$)$_2$ 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 SrCu$_2$(BO$_3$)$_2$ 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.

cond-mat.str-el↗

arXiv2022

Randomness and Frustration in a S = 1/2 Square-Lattice Heisenberg Antiferromagnet

We explore the interplay between randomness and magnetic frustration in the series of $S = 1/2$ Heisenberg square-lattice compounds Sr$_2$CuTe$_{1-x}$W$_x$O$_6$. Substituting W for Te alters the magnetic interactions dramatically, from strongly nearest-neighbor to next-nearest-neighbor antiferromagnetic coupling. We perform neutron scattering measurements to probe the magnetic ground state and excitations over a range of $x$. We propose a bond-disorder model that reproduces ground states with only short-ranged spin correlations in the mixed compounds. The calculated neutron diffraction patterns and powder spectra agree well with the measured data and allow detailed predictions for future measurements. We conclude that quenched randomness plays the major role in defining the physics of Sr$_2$CuTe$_{1-x}$W$_x$O$_6$ with frustration being less significant.

cond-mat.str-el↗

arXiv2022

Spin dynamics in the square-lattice cupola system Ba(TiO)Cu$_4$(PO$_4$)$_4$

We report high-resolution single-crystal inelastic neutron scattering measurements on the spin-1/2 antiferromagnet Ba(TiO)Cu$_4$(PO$_4$)$_4$. This material is formed from layers of four-site \cupola" structures, oriented alternately upwards and downwards, which constitute a rather special realization of two-dimensional (2D) square-lattice magnetism. The strong Dzyaloshinskii-Moriya (DM) interaction within each cupola, or plaquette, unit has a geometry largely unexplored among the numerous studies of magnetic properties in 2D Heisenberg models with spin and spatial anisotropies. We have measured the magnetic excitations at zero field and in fields up to 5 T, finding a complex mode structure with multiple characteristic features that allow us to extract all the relevant magnetic interactions by modelling within the linear spin-wave approximation. We demonstrate that Ba(TiO)Cu$_4$(PO$_4$)$_4$ is a checkerboard system with almost equal intra- and inter-plaquette couplings, in which the intra-plaquette DM interaction is instrumental both in enforcing robust magnetic order and in opening a large gap at the Brillouin-zone center. We place our observations in the perspective of generalized phase diagrams for spin-1/2 square-lattice models and materials, where exploring anisotropies and frustration as routes to quantum disorder remains a frontier research problem.

cond-mat.str-el↗

arXiv2022

Systematic extraction of crystal electric-field effects and quantum magnetic model parameters in triangular rare-earth magnets

A primary goal at the interface of theoretical and experimental quantum magnetism is the investigation of exotic spin states, most notably quantum spin liquids (QSLs). Magnetic rare-earth ions go beyond the straightforward paradigm of geometrical frustration in Heisenberg antiferromagnets by introducing competing energy scales, and in particular their strong spin-orbit coupling creates multiple split crystal electric-field (CEF) levels, leading to anisotropic effective spin models with intrinsic frustration. While rare-earth delafossites have a triangular-lattice geometry, and thus have gained recent attention as candidates for hosting spin-1/2 QSL physics, the reliable extraction of effective spin models from the initial many-parameter CEF spectrum is a hard problem. Using the example of CsYbSe2, we demonstrate the unambiguous extraction of the Stevens-operators coefficients dictating the full CEF spectrum of Yb$^{3+}$ by translating these into parameters with a direct physical interpretation. Specifically, we combine low-field susceptibility measurements with resonant torsion magnetometry experiments in fields up to 60 T to determine a sufficiently large number of physical parameters -- effective Zeeman splittings, anisotropic van Vleck coefficients, and magnetotropic coefficients -- that the set of Stevens-operator coefficients is unique. Our crucial identification of the strong corrections to the Zeeman splitting of Kramers doublets as van Vleck coefficients has direct consequences for the interpretation of all anisotropic magnetic susceptibility measurements. Our results allow us to determine the nature and validity of an effective spin-1/2 model for CsYbSe2, to provide input for theoretical studies of such models on the triangular lattice, and to provide additional materials insight into routes for achieving magnetic frustration and candidate QSL systems in rare-earth compounds.

cond-mat.str-el↗

arXiv2021

Revealing three-dimensional quantum criticality by Sr-substitution in Han Purple

Classical and quantum phase transitions (QPTs), with their accompanying concepts of criticality and universality, are a cornerstone of statistical thermodynamics. An exemplary controlled QPT is the field-induced magnetic ordering of a gapped quantum magnet. Although numerous "quasi-one-dimensional" coupled spin-chain and -ladder materials are known whose ordering transition is three-dimensional (3D), quasi-2D systems are special for several physical reasons. Motivated by the ancient pigment Han Purple (BaCuSi$_{2}$O$_{6}$), a quasi-2D material displaying anomalous critical properties, we present a complete analysis of Ba$_{0.9}$Sr$_{0.1}$CuSi$_{2}$O$_{6}$. We measure the zero-field magnetic excitations by neutron spectroscopy and deduce the magnetic Hamiltonian. We probe the field-induced transition by combining magnetization, specific-heat, torque and magnetocalorimetric measurements with low-temperature nuclear magnetic resonance studies near the QPT. By a Bayesian statistical analysis and large-scale Quantum Monte Carlo simulations, we demonstrate unambiguously that observable 3D quantum critical scaling is restored by the structural simplification arising from light Sr-substitution in Han Purple.

cond-mat.str-el↗

arXiv2021

Triplons, Magnons, and Spinons in a Single Quantum Spin System: SeCuO3

Quantum spin systems exhibit an enormous range of collective excitations, but their spin waves, gapped triplons, fractional spinons, or yet other modes are generally held to be mutually exclusive. Here we show by neutron spectroscopy on SeCuO$_3$ that magnons, triplons, and spinons are present simultaneously. We demonstrate that this is a consequence of a structure consisting of two coupled subsystems and identify all the interactions of a minimal magnetic model. Our results serve qualitatively to open the field of multi-excitation spin systems and quantitatively to constrain the complete theoretical description of one member of this class of materials.

cond-mat.str-el↗

arXiv2019

Thermodynamic properties of the Shastry-Sutherland model throughout the dimer-product phase

The thermodynamic properties of the Shastry-Sutherland model have posed one of the longest-lasting conundrums in frustrated quantum magnetism. Over a wide range on both sides of the quantum phase transition (QPT) from the dimer-product to the plaquette-based ground state, neither analytical nor any available numerical methods have come close to reproducing the physics of the excited states and thermal response. We solve this problem in the dimer-product phase by introducing two qualitative advances in computational physics. One is the use of thermal pure quantum (TPQ) states to augment dramatically the size of clusters amenable to exact diagonalization. The second is the use of tensor-network methods, in the form of infinite projected entangled pair states (iPEPS), for the calculation of finite-temperature quantities. We demonstrate convergence as a function of system size in TPQ calculations and of bond dimension in our iPEPS results, with complete mutual agreement even extremely close to the QPT. Our methods reveal a remarkably sharp and low-lying feature in the magnetic specific heat around the QPT, whose origin appears to lie in a proliferation of excitations composed of two-triplon bound states. The surprisingly low energy scale and apparently extended spatial nature of these states explain the failure of less refined numerical approaches to capture their physics. Both of our methods will have broad and immediate application in addressing the thermodynamic response of a wide range of highly frustrated magnetic models and materials.

cond-mat.str-el↗

arXiv2019

Finite-Temperature Charge Dynamics and the Melting of the Mott Insulator

The Mott insulator is the quintessential strongly correlated electronic state. We obtain complete insight into the physics of the two-dimensional Mott insulator by extending the slave-fermion (holon-doublon) description to finite temperatures. We first benchmark its predictions against state-of-the-art quantum Monte Carlo simulations, demonstrating quantitative agreement. Qualitatively, the short-ranged spin fluctuations both induce holon-doublon bound states and renormalize the charge sector to form the Hubbard bands. The Mott gap is understood as the charge gap renormalized downwards by these spin fluctuations. As temperature increases, the Mott gap closes before the charge gap, causing a pseudogap regime to appear naturally during the melting of the Mott insulator.

cond-mat.str-el↗

arXiv2018

Thermal Critical Points and Quantum Critical End Point in the Frustrated Bilayer Heisenberg Antiferromagnet

We consider the finite-temperature phase diagram of the $S = 1/2$ frustrated Heisenberg bilayer. Although this two-dimensional system may show magnetic order only at zero temperature, we demonstrate the presence of a line of finite-temperature critical points related to the line of first-order transitions between the dimer-singlet and -triplet regimes. We show by high-precision quantum Monte Carlo simulations, which are sign-free in the fully frustrated limit, that this critical point is in the Ising universality class. At zero temperature, the continuous transition between the ordered bilayer and the dimer-singlet state terminates on the first-order line, giving a quantum critical end point, and we use tensor-network calculations to follow the first-order discontinuities in its vicinity.

cond-mat.str-el↗

arXiv2018

Dirac and Chiral Quantum Spin Liquids on the Honeycomb Lattice in a Magnetic Field

Motivated by recent experimental observations in $α$-RuCl$_3$, we study the $K$-$Γ$ model on the honeycomb lattice in an external magnetic field. By a slave-particle representation and Variational Monte Carlo calculations, we reproduce the phase transition from zigzag magnetic order to a field-induced disordered phase. The nature of this state depends crucially on the field orientation. For particular field directions in the honeycomb plane, we find a gapless Dirac spin liquid, in agreement with recent experiments on $α$-RuCl$_3$. For a range of out-of-plane fields, we predict the existence of a Kalmeyer-Laughlin-type chiral spin liquid, which would show an integer-quantized thermal Hall effect.

cond-mat.str-el↗

arXiv2018

Giant pressure dependence and dimensionality switching in a metal-organic quantum antiferromagnet

We report an extraordinary pressure dependence of the magnetic interactions in the metal-organic system [(CuF$_2$(H$_2$O)$_2$)$_2$pyrazine]. At zero pressure, this material realizes a quasi-two-dimensional (Q2D) spin-1/2 square-lattice Heisenberg antiferromagnet. By high-pressure, high-field susceptibility measurements we show that the dominant exchange parameter is reduced continuously by a factor of 2 upon compression. Above 18 kbar, a phase transition occurs, inducing an orbital re-ordering that switches the dimensionality, transforming the Q2D lattice into weakly coupled chains (Q1D). We explain the microscopic mechanisms for both phenomena by combining detailed x-ray and neutron diffraction results with quantitative modeling using spin-polarized density functional theory.

cond-mat.mtrl-sci↗