J. C. Séamus Davis

Concepts relating magnetic interactions, intertwined electronic orders, and strongly correlated superconductivity

Significance This study describes a unified theory explaining the rich ordering phenomena, each associated with a different symmetry breaking, that often accompany high-temperature superconductivity. The essence of this theory is an ”antiferromagnetic interaction,” the interaction that favors the development of magnetic order where the magnetic moments reverse direction from one crystal unit cell to the next. We apply this theory to explain the superconductivity, as well as all observed accompanying ordering phenomena in the copper-oxide superconductors, the iron-based superconductors, and the heavy fermion superconductors. Unconventional superconductivity (SC) is said to occur when Cooper pair formation is dominated by repulsive electron–electron interactions, so that the symmetry of the pair wave function is other than an isotropic s-wave. The strong, on-site, repulsive electron–electron interactions that are the proximate cause of such SC are more typically drivers of commensurate magnetism. Indeed, it is the suppression of commensurate antiferromagnetism (AF) that usually allows this type of unconventional superconductivity to emerge. Importantly, however, intervening between these AF and SC phases, intertwined electronic ordered phases (IP) of an unexpected nature are frequently discovered. For this reason, it has been extremely difficult to distinguish the microscopic essence of the correlated superconductivity from the often spectacular phenomenology of the IPs. Here we introduce a model conceptual framework within which to understand the relationship between AF electron–electron interactions, IPs, and correlated SC. We demonstrate its effectiveness in simultaneously explaining the consequences of AF interactions for the copper-based, iron-based, and heavy-fermion superconductors, as well as for their quite distinct IPs.

Imaging Dirac-mass disorder from magnetic dopant atoms in the ferromagnetic topological insulator Crx(Bi0.1Sb0.9)2-xTe3.

Significance Surface states of topological insulators (TIs) should exhibit extraordinary electronic phenomena when a ‘Dirac-mass gap’ is opened in their spectrum, typically by creating a ferromagnetic state. However, our direct visualization of the Dirac-mass gap Δ(r) in a ferromagnetic TI reveals its intense disorder at the nanoscale. This is correlated with the density of magnetic dopant atoms n(r), such that Δ(r)∝n(r) as anticipated for surface-state–mediated ferromagnetism. Consequent new perspectives on ferromagnetic TI physics include that the quantum anomalous Hall effect occurs in this environment of extreme Dirac-mass disorder and that paths of associated chiral edge states must be tortuous. To achieve all the exotic physics expected of ferromagnetic TIs, greatly improved control of dopant-induced Dirac-mass gap disorder is therefore required. To achieve and use the most exotic electronic phenomena predicted for the surface states of 3D topological insulators (TIs), it is necessary to open a “Dirac-mass gap” in their spectrum by breaking time-reversal symmetry. Use of magnetic dopant atoms to generate a ferromagnetic state is the most widely applied approach. However, it is unknown how the spatial arrangements of the magnetic dopant atoms influence the Dirac-mass gap at the atomic scale or, conversely, whether the ferromagnetic interactions between dopant atoms are influenced by the topological surface states. Here we image the locations of the magnetic (Cr) dopant atoms in the ferromagnetic TI Cr0.08(Bi0.1Sb0.9)1.92Te3. Simultaneous visualization of the Dirac-mass gap Δ(r) reveals its intense disorder, which we demonstrate is directly related to fluctuations in n(r), the Cr atom areal density in the termination layer. We find the relationship of surface-state Fermi wavevectors to the anisotropic structure of Δ(r) not inconsistent with predictions for surface ferromagnetism mediated by those states. Moreover, despite the intense Dirac-mass disorder, the anticipated relationship Δ(r)∝n(r) is confirmed throughout and exhibits an electron–dopant interaction energy J* = 145 meV·nm2. These observations reveal how magnetic dopant atoms actually generate the TI mass gap locally and that, to achieve the novel physics expected of time-reversal symmetry breaking TI materials, control of the resulting Dirac-mass gap disorder will be essential.

Discovery of orbital-selective Cooper pairing in FeSe

A deeper look into iron selenide In the past 10 years, iron-based superconductors have created more puzzles than they have helped resolve. Some of the most fundamental outstanding questions are how strong the interactions are and what the electron pairing mechanism is. Now two groups have made contributions toward resolving these questions in the intriguing compound iron selenide (FeSe) (see the Perspective by Lee). Gerber et al. used photoemission spectroscopy coupled with x-ray diffraction to find that FeSe has a very sizable electron-phonon interaction. Quasiparticle interference imaging helped Sprau et al. determine the shape of the superconducting gap and find that the electron pairing in FeSe is orbital-selective. Science, this issue p. 71, p. 75; see also p. 32 Cooper pairing in iron selenide predominantly occurs between electrons from dyz orbitals of iron atoms. The superconductor iron selenide (FeSe) is of intense interest owing to its unusual nonmagnetic nematic state and potential for high-temperature superconductivity. But its Cooper pairing mechanism has not been determined. We used Bogoliubov quasiparticle interference imaging to determine the Fermi surface geometry of the electronic bands surrounding the Γ = (0, 0) and X = (π/aFe, 0) points of FeSe and to measure the corresponding superconducting energy gaps. We show that both gaps are extremely anisotropic but nodeless and that they exhibit gap maxima oriented orthogonally in momentum space. Moreover, by implementing a novel technique, we demonstrate that these gaps have opposite sign with respect to each other. This complex gap configuration reveals the existence of orbital-selective Cooper pairing that, in FeSe, is based preferentially on electrons from the dyz orbitals of the iron atoms.

Detection of a Cooper-Pair Density Wave in Bi

The quantum condensate of Cooper pairs forming a superconductor was originally conceived as being translationally invariant. In theory, however, pairs can exist with finite momentum Q, thus generating a state with a spatially modulated Cooper-pair density. Such a state has been created in ultracold 6Li gas but never observed directly in any superconductor. It is now widely hypothesized that the pseudogap phase of the copper oxide superconductors contains such a ‘pair density wave’ state. Here we report the use of nanometre-resolution scanned Josephson tunnelling microscopy to image Cooper pair tunnelling from a d-wave superconducting microscope tip to the condensate of the superconductor Bi2Sr2CaCu2O8+x. We demonstrate condensate visualization capabilities directly by using the Cooper-pair density variations surrounding zinc impurity atoms and at the Bi2Sr2CaCu2O8+x crystal supermodulation. Then, by using Fourier analysis of scanned Josephson tunnelling images, we discover the direct signature of a Cooper-pair density modulation at wavevectors QP ≈ (0.25, 0)2π/a0 and (0, 0.25)2π/a0 in Bi2Sr2CaCu2O8+x. The amplitude of these modulations is about five per cent of the background condensate density and their form factor exhibits primarily s or s′ symmetry. This phenomenology is consistent with Ginzburg–Landau theory when a charge density wave with d-symmetry form factor and wavevector QC = QP coexists with a d-symmetry superconductor; it is also predicted by several contemporary microscopic theories for the pseudogap phase.

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The quantum condensate of Cooper pairs forming a superconductor was originally conceived as being translationally invariant. In theory, however, pairs can exist with finite momentum Q, thus generating a state with a spatially modulated Cooper-pair density. Such a state has been created in ultracold 6Li gas but never observed directly in any superconductor. It is now widely hypothesized that the pseudogap phase of the copper oxide superconductors contains such a ‘pair density wave’ state. Here we report the use of nanometre-resolution scanned Josephson tunnelling microscopy to image Cooper pair tunnelling from a d-wave superconducting microscope tip to the condensate of the superconductor Bi2Sr2CaCu2O8+x. We demonstrate condensate visualization capabilities directly by using the Cooper-pair density variations surrounding zinc impurity atoms and at the Bi2Sr2CaCu2O8+x crystal supermodulation. Then, by using Fourier analysis of scanned Josephson tunnelling images, we discover the direct signature of a Cooper-pair density modulation at wavevectors QP ≈ (0.25, 0)2π/a0 and (0, 0.25)2π/a0 in Bi2Sr2CaCu2O8+x. The amplitude of these modulations is about five per cent of the background condensate density and their form factor exhibits primarily s or s′ symmetry. This phenomenology is consistent with Ginzburg–Landau theory when a charge density wave with d-symmetry form factor and wavevector QC = QP coexists with a d-symmetry superconductor; it is also predicted by several contemporary microscopic theories for the pseudogap phase.

Sr

In solid-state physics two different paradigms are typically applied. The first is a local picture, in which one visualizes the quantum states of electrons in atomic orbitals or at impurity atoms in real space ( r -space). The second is the momentum or reciprocal space ( k -space) picture, where electrons are viewed as de Broglie waves completely delocalized throughout the material. Understanding these two separate paradigms is essential for a complete understanding of the physics of condensed matter, but rarely has it been as necessary to combine both pictures as it has been to gain insight into the electronic structure of the high-temperature superconductors (HTSCs). In this article, we review recent developments in the understanding of the relationship between the r -space and k -space electronic spectroscopies used to explore high-temperature superconductivity.

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Significance Strong Coulomb interactions between electrons on adjacent Cu atoms result in charge localization in the cuprate Mott-insulator state. When a few percent of electrons are removed, both high-temperature superconductivity and exotic charge density modulations appear. Identifying the correct fundamental theory for superconductivity requires confidence on whether a particle-like or a wave-like concept of electrons describes this physics. To address this issue, here we take the approach of using the phase of charge modulations, available only from atomic-scale imaging. It reveals a universal periodicity of the charge modulations of four crystal unit cells. These results indicate that the particle-like concept of strong interactions in real-space provides the intrinsic organizational principle for cuprate charge modulations, implying the equivalent for the superconductivity. Theories based upon strong real space (r-space) electron–electron interactions have long predicted that unidirectional charge density modulations (CDMs) with four-unit-cell (4a0) periodicity should occur in the hole-doped cuprate Mott insulator (MI). Experimentally, however, increasing the hole density p is reported to cause the conventionally defined wavevector QA of the CDM to evolve continuously as if driven primarily by momentum-space (k-space) effects. Here we introduce phase-resolved electronic structure visualization for determination of the cuprate CDM wavevector. Remarkably, this technique reveals a virtually doping-independent locking of the local CDM wavevector at |Q0|=2π/4a0 throughout the underdoped phase diagram of the canonical cuprate Bi2Sr2CaCu2O8. These observations have significant fundamental consequences because they are orthogonal to a k-space (Fermi-surface)–based picture of the cuprate CDMs but are consistent with strong-coupling r-space–based theories. Our findings imply that it is the latter that provides the intrinsic organizational principle for the cuprate CDM state.

CaCu

Significance In heavy-fermion materials, the magnetic moment of an f-electron atom, such as Ce, is screened via the Kondo effect resulting in the splitting of a conventional light band into two heavy bands within few millielectron volts of the Fermi energy. For decades it has been hypothesized that Cooper pairing and superconductivity of the resulting heavy electrons are mediated by the f-electron magnetism. By extracting the magnetic interactions of CeCoIn5 from heavy-fermion scattering interference, and by then predicting quantitatively a variety of characteristics expected for unconventional superconductivity driven by them, we provide direct evidence that the heavy-fermion Cooper pairing in this material is indeed mediated by f-electron magnetism. To identify the microscopic mechanism of heavy-fermion Cooper pairing is an unresolved challenge in quantum matter studies; it may also relate closely to finding the pairing mechanism of high-temperature superconductivity. Magnetically mediated Cooper pairing has long been the conjectured basis of heavy-fermion superconductivity but no direct verification of this hypothesis was achievable. Here, we use a novel approach based on precision measurements of the heavy-fermion band structure using quasiparticle interference imaging to reveal quantitatively the momentum space (k-space) structure of the f-electron magnetic interactions of CeCoIn5. Then, by solving the superconducting gap equations on the two heavy-fermion bands Ekα,β with these magnetic interactions as mediators of the Cooper pairing, we derive a series of quantitative predictions about the superconductive state. The agreement found between these diverse predictions and the measured characteristics of superconducting CeCoIn5 then provides direct evidence that the heavy-fermion Cooper pairing is indeed mediated by f-electron magnetism.

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Atomic-scale imaging reveals how individual impact sites of high-energy ions prevent the disruptive motion of magnetic vortices. Maximizing the sustainable supercurrent density, JC, is crucial to high-current applications of superconductivity. To achieve this, preventing dissipative motion of quantized vortices is key. Irradiation of superconductors with high-energy heavy ions can be used to create nanoscale defects that act as deep pinning potentials for vortices. This approach holds unique promise for high-current applications of iron-based superconductors because JC amplification persists to much higher radiation doses than in cuprate superconductors without significantly altering the superconducting critical temperature. However, for these compounds, virtually nothing is known about the atomic-scale interplay of the crystal damage from the high-energy ions, the superconducting order parameter, and the vortex pinning processes. We visualize the atomic-scale effects of irradiating FeSexTe1−x with 249-MeV Au ions and find two distinct effects: compact nanometer-sized regions of crystal disruption or “columnar defects,” plus a higher density of single atomic site “point” defects probably from secondary scattering. We directly show that the superconducting order is virtually annihilated within the former and suppressed by the latter. Simultaneous atomically resolved images of the columnar crystal defects, the superconductivity, and the vortex configurations then reveal how a mixed pinning landscape is created, with the strongest vortex pinning occurring at metallic core columnar defects and secondary pinning at clusters of point-like defects, followed by collective pinning at higher fields.

O

We review the current state of efforts to use resonant soft X-ray scattering (RSXS), which is an elastic, momentum-resolved, valence band probe of strongly correlated electron systems, to study stripe-like phenomena in copper-oxide superconductors and related materials. We review the historical progress including RSXS studies of Wigner crystallization in spin ladder materials, stripe order in 214-phase nickelates, 214-phase cuprates, and other systems. One of the major outstanding issues in RSXS concerns its relationship to more established valence band probes, namely angle-resolved photoemission (ARPES) and scanning tunneling microscopy (STM). These techniques are widely understood as measuring a one-electron spectral function, yet a relationship between RSXS and a spectral function has so far been unclear. Using physical arguments that apply at the oxygen K edge, we show that RSXS measures the square modulus of an advanced version of the Green’s function measured with STM. This indicates that, despite being a momentum space probe, RSXS is more closely related to STM than to ARPES techniques. Finally, we close with some discussion of the most promising future directions for RSXS. We will argue that the most promising area lies in high magnetic field studies, particularly of edge states in strongly correlated heterostructures, and the vortex state in superconducting cuprates, where RSXS may clarify the anomalous periodicities observed in recent quantum oscillation experiments.