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J. C. Séamus Davis

Publications and source records attributed to J. C. Séamus Davis.

At least 19 recordsLinked to original sources

Spinon mediation of witness spin dynamics in herbertsmithite

The kagome lattice of spin-1/2 copper atoms in herbertsmithite is conjectured to sustain a quantum spin liquid state with spinon quasiparticles. Ideally, the kagome crystal planes are each separated by a plane of spinless zinc atoms. However, in real crystals some spin-1/2 copper atoms substitute randomly onto these inter-kagome zinc sites. Here we reconceptualize such 'impurity' atoms as quantum witness spins whose dynamics is designed to probe the spin liquid state. We then introduce spin noise spectroscopy to measure the frequency and temperature dependence of witness spin dynamics, demonstrating that their phenomenology is consistent with extensive interactions between witness spins mediated by propagation of spinons through a quantum spin liquid. Ultimately, a sharp transition occurs at around 260 mK, below which the properties of both spin noise and magnetic susceptibility suggest that the witness spins form a spin glass phase. Among theoretical models considered, we demonstrate that our observations are only consistent with spinon-mediated interactions between witness spins by either a Z2 or U(1) quantum spin liquid, with the former model more closely matching the data. Our work demonstrates that quantum mechanical witness spins may now conceivably be used as a widely applicable probe of quantum spin liquid physics.

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Discovery of Dynamical Heterogeneity in a Supercooled Magnetic Monopole Fluid

Dynamical heterogeneity, in which transitory local fluctuations occur in the conformation and dynamics of constituent particles, is widely hypothesized to be essential to evolution of supercooled liquids into the structural glass state. Yet its microscopic spatiotemporal phenomenology is challenging to detect directly in molecular glass forming liquids. Because recent theoretical advances predict that corresponding dynamical heterogeneity could occur in supercooled magnetic monopole fluids (Proc. Nat. Acad. Sci. 112, 8549 (2015)), we searched for such phenomena in Dy2Ti2O7. By measuring its microsecond-resolved spontaneous magnetization fluctuations $M(t,T)$ we discovered a sharp bifurcation in monopole noise characteristics below $T \approx 1500$ mK, with the appearance of powerful spontaneous monopole current bursts. This intense dynamics emerges upon entering the supercooled monopole fluid regime, reaches maximum strength near $T \approx 750$ mK and then collapses along with coincident loss of ergodicity approaching $T_g \approx 750$ mK. Moreover, when the four-point dynamical susceptibility $χ_4(τ, T)$ is determined directly from temperature dependence of correlations in $M(t,T)$, it evolves as predicted when dynamical heterogeneity is present, revealing its simultaneously and rapidly escalating length and time scales, $ξ(T)$. and $τ_4(T)$. This overall phenomenology 2 greatly expands our empirical knowledge of supercooled monopole fluids and, more generally, demonstrates direct detection of the time sequence, magnitude, statistics and correlations of dynamical heterogeneity, access to which may greatly accelerate fundamental vitrification studies.

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Visualizing the Odd-parity Superconducting Order Parameter and its Quasiparticle Surface Band in UTe2

A distinctive identifier of nodal intrinsic topological superconductivity (ITS) would the appearance of an Andreev bound state on crystal surfaces parallel to the nodal axis, in the form of a topological quasiparticle surface band (QSB) appearing only for $T < T_C$. Moreover, theory shows that specific QSB characteristics observable in tunneling to an s-wave superconductor can distinguish between chiral and non-chiral ITS order parameter $Δ_k$. To search for such phenomena in $\text{UTe}_2$, s-wave superconductive scan-tip scanning tunneling microscopy (STM) imaging was employed. It reveals an intense zero-energy Andreev conductance maximum at the $\text{UTe}_2$ (0-11) crystal termination. Development of the zero-energy Andreev conductance peak into two finite-energy particle-hole symmetric conductance maxima as the tunnel barrier is reduced, then signifies that $\text{UTe}_2$ superconductivity is non-chiral. Quasiparticle interference imaging (QPI) for an ITS material should be dominated by the QSB for energies within the superconductive energy gap $|E| \le Δ$, so that bulk $Δ(k)$ characteristics of the ITS can only be detected excursively. Again using a superconducting scan-tip, the in-gap quasiparticle interference patterns of the QSB of $\text{UTe}_2$ were visualized. Specifically, a band of Bogoliubov quasiparticles appears as a characteristic sextet $q_i$ :$i = 1-6$ of interference wavevectors showing that QSB dispersions $k(E)$ occur only for energies $|E| \le Δ_{max}$ and only within the range of Fermi momenta projected onto the (0-11) crystal surface. In combination, these phenomena are consistent with a bulk $Δ(k)$ exhibiting spin triplet, time-reversal conserving, odd-parity, a-axis nodal, $B_{3u}$ symmetry in $\text{UTe}_2$.

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Quasiparticle interference and spectral function of the UTe$_2$ superconductive surface band

We compute the (0-11) surface spectral function, the surface density of states (DOS), and the quasiparticle interference (QPI) patterns, both in the normal state and superconducting (SC) state of UTe$_2$. We consider all possible non-chiral and chiral order parameters (OPs) that could in principle describe the superconductivity in this compound. We describe the formation of surface states whose maximum intensity energy depends on the nature of the pairing. We study also the QPI patterns resulting from the scattering of these surface states. We show that the main feature distinguishing between various OPs is a QPI peak that is only observed experimentally in the superconducting state. The energy dispersion and the stability of this peak is consistent among the non-chiral OPs only with a $B_{3u}$ pairing. Moreover, $B_{3u}$ is the only non-chiral pairing that shows a peak at zero energy in the DOS, consistent with the experimental observations.

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Odd-Parity Quasiparticle Interference in the Superconductive Surface State of UTe2

Although no known material exhibits intrinsic topological superconductivity, wherein spin-triplet odd-parity electron pairing occurs, UTe2 is now the leading representative of this class. Conventionally, the parity of the superconducting order parameter may be established by using Bogoliubov quasiparticle interference (QPI) imaging. However, odd-parity superconductors should support a topological quasiparticle surface band (QSB) at energies within the maximum superconducting energy gap. QPI would then be dominated by the electronic structure of the QSB and only reveal the characteristics of the bulk order parameter excursively. Here, we visualize quasiparticle interference patterns of UTe2 and find that, at the (0-11) cleave surface, a new band of Bogoliubov quasiparticles appears only in the superconducting state. QPI visualization then allows study of dispersion of states within this QSB, which we demonstrate exists only within the range of Fermi momenta projected onto the (0-11) surface. Finally, we develop a theoretical framework to predict the QPI signatures of such a QSB at the (0-11) surface of UTe2. Its predictions are most consistent with the experimental results if the bulk superconducting gap function exhibits time-reversal conserving, odd-parity, a-axis nodal, B3u symmetry.

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Pair Wavefunction Symmetry in UTe2 from Zero-Energy Surface State Visualization

Although nodal spin-triplet topological superconductivity appears probable in UTe2, its superconductive order-parameter $Δ_k$ remains unestablished. In theory, a distinctive identifier would be the existence of a superconductive topological surface band (TSB), which could facilitate zero-energy Andreev tunneling to an s-wave superconductor, and also distinguish a chiral from non-chiral $Δ_k$ via enhanced s-wave proximity. Here we employ s-wave superconductive scan-tips and detect intense zero-energy Andreev conductance at the UTe2 (0-11) termination surface. Imaging reveals sub-gap quasiparticle scattering interference signatures with a-axis orientation. The observed zero-energy Andreev peak splitting with enhanced s-wave proximity, signifies that $Δ_k$ of UTe2 is a non-chiral state: B1u, B2u or B3u. However, if the quasiparticle scattering along the a-axis is internodal, then a non-chiral B3u state is the most consistent for UTe2.

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Spiral Spin Liquid Noise

An emerging concept for identification of different types of spin liquids is through the use of spontaneous spin noise. Here we develop spin noise spectroscopy for spin liquid studies by considering Ca$_{10}$Cr$_7$O$_{28}$, a material hypothesized to be either a quantum or a spiral spin liquid. By enhancing techniques introduced for magnetic monopole noise studies we measure the time and temperature dependence of spontaneous flux $\varPhi(t, T)$ and thus magnetization $M(t, T)$ of Ca$_{10}$Cr$_7$O$_{28}$ samples. The resulting power spectral density of magnetization noise $S_M(ω,T)$ reveals intense spin fluctuations with $S_M(ω,T) \propto ω^{-α(T)}$ and 0.84 < $α(T)$ < 1.04 . Both the variance $σ_M^2(T)$ and the correlation function $C_M(t,T)$ of this spin noise undergo crossovers at a temperature $T^* \approx$ 450 mK. While predictions for quantum spin liquids are inconsistent with this phenomenology, those from Monte-Carlo simulations of a 2D spiral spin liquid state in Ca$_{10}$Cr$_7$O$_{28}$ yield overall quantitative correspondence with the measured frequency and temperature dependences of $S_M(ω,T), C_M(t,T)$ and $σ_M^2(T)$, thus indicating that Ca$_{10}$Cr$_7$O$_{28}$ is a spiral spin liquid.

cond-mat.str-el↗

Dichotomous Dynamics of Magnetic Monopole Fluids

A recent advance in the study of emergent magnetic monopoles was the discovery that monopole motion is restricted to dynamical fractal trajectories (J. Hallén et al, Science 378, 1218 (2022)) thus explaining the characteristics of magnetic monopole noise spectra (Dusad, R. et al. Nature 571, 234 (2019); Samarakoon, A. M. et al. Proc. Natl. Acad. Sci. 119, e2117453119 (2022)). Here we apply this new theory to explore the dynamics of field-driven monopole currents, finding them comprised of two quite distinct transport processes: initially swift fractal rearrangements of local monopole configurations followed by conventional monopole diffusion. This theory also predicts a characteristic frequency dependence of the dissipative loss-angle for AC-field-driven currents. To explore these novel perspectives on monopole transport, we introduce simultaneous monopole current control and measurement techniques using SQUID-based monopole current sensors. For the canonical material Dy2Ti2O7, we measure $Φ(t)$, the time-dependence of magnetic flux threading the sample when a net monopole current $J(t) = \dotΦ(t)/μ_0$ is generated by applying an external magnetic field $B_0(t)$. These experiments find a sharp dichotomy of monopole currents, separated by their distinct relaxation time-constants before and after $t \approx 600 μs$ from monopole current initiation. Application of sinusoidal magnetic fields $B_0(t) = Bcos(ωt)$ generates oscillating monopole currents whose loss angle $θ(f)$ exhibits a characteristic transition at frequency $f \approx 1.8$ kHz over the same temperature range. Finally, the magnetic noise power is also dichotomic, diminishing sharply after $t \approx 600 μs$. This complex phenomenology represents a new form of heterogeneous dynamics generated by the interplay of fractionalization and local spin configurational symmetry.

cond-mat.mes-hall↗

Discovery of Orbital Ordering in Bi2Sr2CaCu2O8+x

The primordial ingredient of cuprate superconductivity is the CuO2 unit cell. Here, theoretical attention usually concentrates on the intra-atom Coulombic interactions dominating the 3d^9 and 3d^10 configurations of each copper ion. However, if Coulombic interactions also occur between electrons of the 2p^6 orbitals of each planar oxygen atom, spontaneous orbital ordering may split their energy levels. This long predicted intra-unit cell symmetry breaking should then generate an orbital ordered phase, for which the charge-transfer energy E separating the 2p^6 and 3d^10orbitals is distinct for the two oxygen atoms. Here we introduce sublattice resolved E(r) imaging techniques to CuO2 studies and discover intra-unit-cell rotational symmetry breaking of E(r), with energy-level splitting between the two oxygen atoms on the 50 meV scale. Spatially, this state is arranged in disordered Ising domains of orthogonally oriented orbital order that appear bounded by dopant ions, and within whose domain walls low energy electronic quadrupolar two-level systems occur. Overall, these data reveal a Q=0 orbitally ordered state that splits the energy levels of the oxygen orbitals by ~50 meV, in underdoped CuO2.

cond-mat.supr-con↗

Interplay of Hidden Orbital Order and Superconductivity in CeCoIn5

Visualizing atomic-orbital degrees of freedom is a frontier challenge in scanned microscopy. Some types of orbital order are virtually imperceptible to normal scattering techniques because they do not reduce the overall crystal lattice symmetry. A good example is dxz/dyz (π,π) orbital order in tetragonal lattices. For enhanced detectability, here we consider the quasiparticle scattering interference (QPI) signature of such (π,π) orbital order in both normal and superconducting phases. The theory reveals that sublattice-specific QPI signatures generated by the orbital order should emerge strongly in the superconducting phase. Sublattice-resolved QPI visualization in superconducting CeCoIn5 then reveals two orthogonal QPI patterns at lattice-substitutional impurity atoms. We analyze the energy dependence of these two orthogonal QPI patterns and find the intensity peaked near E=0, as predicted when such (π) orbital order is inte,πrtwined with d-wave superconductivity. Sublattice-resolved superconductive QPI techniques thus represent a new approach for study of hidden orbital order.

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Visualizing the atomic-scale origin of metallic behavior in Kondo insulators

A Kondo lattice is often electrically insulating at low temperatures. However, several recent experiments have detected signatures of bulk metallicity within this Kondo insulating phase. Here we visualize the real-space charge landscape within a Kondo lattice with atomic resolution using a scanning tunneling microscope. We discover nanometer-scale puddles of metallic conduction electrons centered around uranium-site substitutions in the heavy-fermion compound URu$_2$Si$_2$, and around samarium-site defects in the topological Kondo insulator SmB$_6$. These defects disturb the Kondo screening cloud, leaving behind a fingerprint of the metallic parent state. Our results suggest that the mysterious 3D quantum oscillations measured in SmB$_6$ could arise from these Kondo-lattice defects, although we cannot rule out other explanations. Our imaging technique could enable the development of atomic-scale charge sensors using heavy-fermion probes.

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Detection of a Pair Density Wave State in UTe$_2$

Spin-triplet topological superconductors should exhibit many unprecedented electronic properties including fractionalized electronic states relevant to quantum information processing. Although UTe$_2$ may embody such bulk topological superconductivity, its superconductive order-parameter $Δ(\mathbf{k})$ remains unknown. Many diverse forms for $Δ(\mathbf{k})$ are physically possible in such heavy fermion materials. Moreover, intertwined density waves of spin (SDW), charge (CDW) and pairs (PDW) may interpose, with the latter state exhibiting spatially modulating superconductive order-parameter $Δ(\mathbf{r})$, electron pair density and pairing energy-gap. Hence, the newly discovered CDW state in UTe$_2$ motivates the prospect that a PDW state may exist in this material. To search for it, we visualize the pairing energy-gap with $μ$$eV$-scale energy-resolution using superconductive STM tips. We detect three PDWs, each with peak-peak gap modulations circa 10 $μ$$eV$ and at incommensurate wavevectors $\mathbf{P}_{i=1,2,3}$ that are indistinguishable from the wavevectors $\mathbf{Q}_{i=1,2,3}$ of the prevenient CDW. Concurrent visualization of the UTe$_2$ superconductive PDWs and the non-superconductive CDWs reveals that every $\mathbf{P}_i$ : $\mathbf{Q}_i$ pair exhibits a relative phase $δϕ\approx π$. From these observations, and given UTe$_2$ as a spin-triplet superconductor, this PDW state should be a spin-triplet pair density wave. While such states do exist in superfluid $^{3}$He, for superconductors they are unprecedented.

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Scattering Interference Signature of a Pair Density Wave State in the Cuprate Pseudogap Phase

An unidentified quantum fluid designated as the pseudogap (PG) phase is produced by electron-density depletion in the CuO$_2$ antiferromagnetic insulator. Current theories suggest that the PG phase may be a pair density wave (PDW) state characterized by a spatially modulating density of electron pairs. Such a state should exhibit a periodically modulating energy gap $Δ_P(\pmb r)$ in real-space, and a characteristic quasiparticle scattering interference (QPI) signature $Λ_P(\pmb q)$ in wavevector space. By studying strongly underdoped Bi$_2$Sr$_2$CaDyCu$_2$O$_8$ at hole-density ~0.08 in the superconductive phase, we detect the $8a_0$-periodic $Δ_P(\pmb r)$ modulations signifying a PDW coexisting with superconductivity. Then, by visualizing the temperature dependence of this electronic structure from the superconducting into the pseudogap phase, we find evolution of the scattering interference signature $Λ(\pmb q)$ that is predicted specifically for the temperature dependence of an $8a_0$-periodic PDW. These observations are consistent with theory for the transition from a PDW state coexisting with d-wave superconductivity to a pure PDW state in the Bi$_2$Sr$_2$CaDyCu$_2$O$_8$ pseudogap phase.

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Atomic-scale Visualization of Electronic Fluid Flow

The most essential characteristic of any fluid is the velocity field v(r) and this is particularly true for macroscopic quantum fluids. Although rapid advances have occurred in quantum fluid v(r) imaging, the velocity field of a charged superfluid - a superconductor - has never been visualized. Here we use superconductive-tip scanning tunneling microscopy to image the electron-pair density \r{ho}_S(r) and velocity v_S(r) fields of the flowing electron-pair fluid in superconducting NbSe2. Imaging v_S(r) surrounding a quantized vortex finds speeds reaching 10,000 km/hr. Together with independent imaging of \r{ho}_S(r) via Josephson tunneling, we visualize the supercurrent density j_S(r)=\r{ho}_S(r)v_S(r), which peaks above 3 x 10^7 A/cm^2. The spatial patterns in electronic fluid flow and magneto-hydrodynamics reveal hexagonal structures co-aligned to the crystal lattice and quasiparticle bound states, as long anticipated. These novel techniques pave the way for electronic fluid flow visualization in many other quantum fluids.

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Discovery of a Cooper-Pair Density Wave State in a Transition-Metal Dichalcogenide

Pair density wave (PDW) states are defined by a spatially modulating superconductive order-parameter. To search for such states in transition metal dichalcogenides (TMD) we use high-speed atomic-resolution scanned Josephson-tunneling microscopy (SJTM). We detect a PDW state whose electron-pair density and energy-gap modulate spatially at the wavevectors of the preexisting charge density wave (CDW) state. The PDW couples linearly to both the s-wave superconductor and to the CDW, and exhibits commensurate domains with discommensuration phase-slips at the boundaries, conforming to those of the lattice-locked commensurate CDW. Nevertheless, we find a global $δΦ\sim \pm2π/3$ phase difference between the PDW and CDW states, possibly owing to the Cooper-pair wavefunction orbital content. Our findings presage pervasive PDW physics in the many other TMDs that sustain both CDW and superconducting states.

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Multi-Atom Quasiparticle Scattering Interference for Superconductor Energy-Gap Symmetry Determination

Complete theoretical understanding of the most complex superconductors requires a detailed knowledge of the symmetry of the superconducting energy-gap $Δ_\mathbf{k}^α$, for all momenta $\mathbf{k}$ on the Fermi surface of every band $α$. While there are a variety of techniques for determining $|Δ_\mathbf{k}^α|$, no general method existed to measure the signed values of $Δ_\mathbf{k}^α$. Recently, however, a new technique based on phase-resolved visualization of superconducting quasiparticle interference (QPI) patterns centered on a single non-magnetic impurity atom, was introduced. In principle, energy-resolved and phase-resolved Fourier analysis of these images identifies wavevectors connecting all k-space regions where $Δ_\mathbf{k}^α$ has the same or opposite sign. But use of a single isolated impurity atom, from whose precise location the spatial phase of the scattering interference pattern must be measured is technically difficult. Here we introduce a generalization of this approach for use with multiple impurity atoms, and demonstrate its validity by comparing the $Δ_\mathbf{k}^α$ it generates to the $Δ_\mathbf{k}^α$ determined from single-atom scattering in FeSe where $s_{\pm}$ energy-gap symmetry is established. Finally, to exemplify utility, we use the multi-atom technique on LiFeAs and find scattering interference between the hole-like and electron-like pockets as predicted for $Δ_\mathbf{k}^α$ of opposite sign.

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Severe Dirac Mass Gap Suppression in Sb_2Te_3-based Quantum Anomalous Hall Materials

Quantum anomalous Hall (QAH) effect appears in ferromagnetic topological insulators (FMTI) when a Dirac mass gap opens in the spectrum of the topological surface states (SS). Unaccountably, although the mean mass gap can exceed 28 meV (or ~320 K), the QAH effect is frequently only detectable at temperatures below 1 K. Using atomic-resolution Landau level spectroscopic imaging, we compare the electronic structure of the archetypal FMTI Cr_0.08(Bi_0.1Sb_0.9)_1.92Te_3 to that of its non-magnetic parent (Bi_0.1Sb_0.9)_2Te_3, to explore the cause. In (Bi_0.1Sb_0.9)_2Te_3, we find spatially random variations of the Dirac energy. Statistically equivalent Dirac energy variations are detected in Cr_0.08(Bi_0.1Sb_0.9)_1.92Te_3 with concurrent but uncorrelated Dirac mass gap disorder. These two classes of SS electronic disorder conspire to drastically suppress the minimum mass gap to below 100 μeV for nanoscale regions separated by <1 μm. This fundamentally limits the fully quantized anomalous Hall effect in Sb_2Te_3-based FMTI materials to very low temperatures.

cond-mat.mes-hall↗

Phase-sensitive determination of nodal $\mathbf{d}$-wave order parameter in single-band and multiband superconductors

Determining the exact pairing symmetry of the superconducting order parameter in candidate unconventional superconductors remains an important challenge. Recently a new method, based on phase sensitive quasiparticle interference measurements, was developed to identify gap sign changes in isotropic multiband systems. Here we extend this approach to the single-band and multiband nodal $d$-wave superconducting cases relevant, respectively, for the cuprates and likely for the infinite-layer nickelate superconductors. Combining analytical and numerical calculations, we show that the antisymmetrized correction to the tunneling density of states due to nonmagnetic impurities in the Born and intermediate-scattering limits shows characteristic features for sign-changing and sign-preserving scattering wavevectors, as well as for the momentum-integrated quantity. Furthermore, using a realistic approach accounting for the Wannier orbitals, we model scanning tunneling microscopy data of $\text{Bi}_2\text{Sr}_2\text{CaCu}_2\text{O}_{8+δ}$, which should allow the comparison of our theory with experimental data.

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