Charge density waves in infinite-layer NdNiO2 nickelates.

In materials science, much effort has been devoted to the reproduction of superconductivity in chemical compositions, analogous to cuprate superconductors since their discovery over 30 years ago. This approach was recently successful in realising superconductivity in infinite-layer nickelates1-6. Although differing from cuprates in electronic and magnetic properties, strong Coulomb interactions suggest that infinite-layer nickelates have a propensity towards various symmetry-breaking orders that populate cuprates7-10. Here we report the observation of charge density waves (CDWs) in infinite-layer NdNiO2 films using Ni L3 resonant X-ray scattering. Remarkably, CDWs form in Nd 5d and Ni 3d orbitals at the same commensurate wavevector (0.333, 0) reciprocal lattice units, with non-negligible out-of-plane dependence and an in-plane correlation length of up to ~60 Å. Spectroscopic studies reveal a strong connection between CDWs and Nd 5d-Ni 3d orbital hybridization. Upon entering the superconducting state at 20% Sr doping, the CDWs disappear. Our work demonstrates the existence of CDWs in infinite-layer nickelates with a multiorbital character distinct from cuprates, which establishes their low-energy physics.

Bamboo-like Vortex Chains Confined in Canals with Suppressed Superconductivity and Standing Waves of Quasiparticles.

The vortex core can be regarded as a nanoscale confined system for quasiparticles in a type-II superconductor. It is very interesting to investigate the interplay between the vortex core and other microscopic quantum confined systems. We observe band-like canals with the width of about 15 nm on the surface of KCa2(Fe1-xNix)4As4F2 (x = 0.05) by scanning tunneling microscopy. Some canals suppress superconductivity and confine parallel standing waves due to the quasiparticle interference. Upon magnetic fields being applied, some elongated vortices are formed within canals showing bamboo-like one-dimensional vortex chains. Interestingly, the confined vortex cores are elongated roughly along the perpendicular direction of canals, and the local density of states at positive and negative energies shows an in-phase oscillation at zero field; but, it becomes out-of-phase crossing the vortex cores. Our work reveals a new type of vortex patterns in confined canals and its interplay with the quasiparticle interference.

Preferred Spin Excitations in the Bilayer Iron-Based Superconductor CaK(Fe_{0.96}Ni_{0.04})_{4}As_{4} with Spin-Vortex Crystal Order.

Spin-orbit coupling (SOC) is a key to understand the magnetically driven superconductivity in iron-based superconductors, where both local and itinerant electrons are present and the orbital angular momentum is not completely quenched. Here, we report a neutron scattering study on the bilayer compound CaK(Fe_{0.96}Ni_{0.04})_{4}As_{4} with superconductivity coexisting with a noncollinear spin-vortex crystal magnetic order that preserves the tetragonal symmetry of the Fe-Fe plane. In the superconducting state, two spin resonance modes with odd and even L symmetries due to the bilayer coupling are found similar to the undoped compound CaKFe_{4}As_{4} but at lower energies. Polarization analysis reveals that the odd mode is c-axis polarized, and the low-energy spin anisotropy can persist to the paramagnetic phase at high temperature, which closely resembles other systems with in-plane collinear and c-axis biaxial magnetic orders. These results provide the missing piece of the puzzle on the SOC effect in iron-pnictide superconductors, and also establish a common picture of c-axis preferred magnetic excitations below T_{c} regardless of the details of magnetic pattern or lattice symmetry.

Friedel Oscillations of Vortex Bound States under Extreme Quantum Limit in KCa_{2}Fe_{4}As_{4}F_{2}.

We report the observation of discrete bound states with the energy levels deviating from the widely believed ratio of 1∶3∶5 in the vortices of an iron-based superconductor KCa_{2}Fe_{4}As_{4}F_{2} through scanning tunneling microscopy (STM). Meanwhile Friedel oscillations of vortex bound states are also observed for the first time in related vortices. By doing self-consistent calculations of Bogoliubov-de Gennes equations, we find that at extreme quantum limit, the superconducting order parameter exhibits a Friedel-like oscillation, which modifies the energy levels of the vortex bound states and explains why it deviates from the ratio of 1∶3∶5. The observed Friedel oscillations of the bound states can also be roughly interpreted by the theoretical calculations, however some features at high energies could not be explained. We attribute this discrepancy to the high energy bound states with the influence of nearby impurities. Our combined STM measurement and the self-consistent calculations illustrate a generalized feature of vortex bound states in type-II superconductors.

Extreme Suppression of Antiferromagnetic Order and Critical Scaling in a Two-Dimensional Random Quantum Magnet.

Sr_{2}CuTeO_{6} is a square-lattice Néel antiferromagnet with superexchange between first-neighbor S=1/2 Cu spins mediated by plaquette centered Te ions. Substituting Te by W, the affected impurity plaquettes have predominantly second-neighbor interactions, thus causing local magnetic frustration. Here we report a study of Sr_{2}CuTe_{1-x}W_{x}O_{6} using neutron diffraction and µSR techniques, showing that the Néel order vanishes already at x=0.025±0.005. We explain this extreme order suppression using a two-dimensional Heisenberg spin model, demonstrating that a W-type impurity induces a deformation of the order parameter that decays with distance as 1/r^{2} at temperature T=0. The associated logarithmic singularity leads to loss of order for any x>0. Order for small x>0 and T>0 is induced by weak interplane couplings. In the nonmagnetic phase of Sr_{2}CuTe_{1-x}W_{x}O_{6}, the µSR relaxation rate exhibits quantum critical scaling with a large dynamic exponent, z≈3, consistent with a random-singlet state.

Neutron Spin Resonance in a Quasi-Two-Dimensional Iron-Based Superconductor.

The neutron spin resonance is generally regarded as a key to understanding the magnetically mediated Cooper pairing in unconventional superconductors. Here, we report an inelastic neutron scattering study on the low-energy spin excitations in a quasi-two-dimensional iron-based superconductor KCa_{2}Fe_{4}As_{4}F_{2}. We have discovered a two-dimensional spin resonant mode with downward dispersions, a behavior closely resembling the low branch of the hourglass-type spin resonance in cuprates. While the resonant intensity is predominant by two broad incommensurate peaks near Q=(0.5,0.5) with a sharp energy peak at E_{R}=16 meV, the overall energy dispersion of the mode exceeds the measured maximum total gap Δ_{tot}=|Δ_{k}|+|Δ_{k+Q}|. These results deeply challenge the conventional understanding of the resonance modes as magnetic excitons regardless of underlining pairing symmetry schemes, and it also points out that when the iron-based superconductivity becomes very quasi-two-dimensional, the electronic behaviors are similar to those in cuprates.

ThMnPnN (Pn = P, As): Synthesis, Structure, and Chemical Pressure Effects.

Mn-based ZrCuSiAs-type pnictides ThMnPnN (Pn = P, As) containing PbO-type Th2N2 layers were synthesized. The crystal and magnetic structures are determined using X-ray and neutron powder diffraction. While neutron diffraction indicates a C-type antiferromagnetic state at 300 K, the temperature dependence of the magnetic susceptibility shows cusps at 36 and 52 K respectively for ThMnPN and ThMnAsN. The susceptibility cusps are ascribed to a spontaneous antiferromagnetic-to-antiferromagnetic transition for Mn2+ moments, which is observed for the first time in Mn-based ZrCuSiAs-type compounds. In addition, measurements of the resistivity and specific heat suggest an abnormal increase in the density of states at the Fermi energy. The result is discussed in terms of the internal chemical pressure effect.

Unconventional Antiferromagnetic Quantum Critical Point in Ba(Fe_{0.97}Cr_{0.03})_{2}(As_{1-x}P_{x})_{2}.

We have systematically studied physical properties of Ba(Fe_{0.97}Cr_{0.03})_{2}(As_{1-x}P_{x})_{2}, where superconductivity in BaFe_{2}(As_{1-x}P_{x})_{2} is fully suppressed by just 3% of Cr substitution of Fe. A quantum critical point is revealed at x∼0.42, where non-Fermi-liquid behaviors similar to those in BaFe_{2}(As_{1-x}P_{x})_{2} are observed. Neutron diffraction and inelastic neutron scattering measurements suggest that the quantum critical point is associated with the antiferromagnetic order, which is not of conventional spin-density-wave type as evidenced by the ω/T scaling of spin excitations. On the other hand, no divergence of low-temperature nematic susceptibility is observed when x is decreased to 0.42 from higher doping level, demonstrating that there are no nematic quantum critical fluctuations. Our results suggest that non-Fermi-liquid behaviors in iron-based superconductors can be solely resulted from the antiferromagnetic quantum critical fluctuations, which cast doubts on the role of nematic fluctuations played in the normal-state properties in iron-based superconductors.

Odd and Even Modes of Neutron Spin Resonance in the Bilayer Iron-Based Superconductor CaKFe_{4}As_{4}.

We report an inelastic neutron scattering study on the spin resonance in the bilayer iron-based superconductor CaKFe_{4}As_{4}. In contrast to its quasi-two-dimensional electron structure, three strongly L-dependent modes of spin resonance are found below T_{c}=35 K. The mode energies are below and linearly scale with the total superconducting gaps summed on the nesting hole and electron pockets, essentially in agreement with the results in cuprate and heavy fermion superconductors. This observation supports the sign-reversed Cooper pairing mechanism under multiple pairing channels and resolves the long-standing puzzles concerning the broadening and dispersive spin resonance peak in iron pnictides. More importantly, the triple resonant modes can be classified into odd and even symmetries with respect to the distance of Fe-Fe planes within the Fe-As bilayer unit. Thus, our results closely resemble those in the bilayer cuprates with nondegenerate spin excitations, suggesting that these two high-T_{c} superconducting families share a common nature.

Spin Waves in Detwinned BaFe_{2}As_{2}.

Understanding magnetic interactions in the parent compounds of high-temperature superconductors forms the basis for determining their role for the mechanism of superconductivity. For parent compounds of iron pnictide superconductors such as AFe_{2}As_{2} (A=Ba, Ca, Sr), although spin excitations have been mapped out throughout the entire Brillouin zone, the respective measurements were carried out on twinned samples and did not allow for a conclusive determination of the spin dynamics. Here we use inelastic neutron scattering to completely map out spin excitations of ∼100% detwinned BaFe_{2}As_{2}. By comparing observed spectra with theoretical calculations, we conclude that the spin excitations can be well described by an itinerant model when taking into account moderate electronic correlation effects.

Neutron Spin Resonance in the 112-Type Iron-Based Superconductor.

We use inelastic neutron scattering to study the low-energy spin excitations of the 112-type iron pnictide Ca_{0.82}La_{0.18}Fe_{0.96}Ni_{0.04}As_{2} with bulk superconductivity below T_{c}=22 K. A two-dimensional spin resonance mode is found around E=11 meV, where the resonance energy is almost temperature independent and linearly scales with T_{c} along with other iron-based superconductors. Polarized neutron analysis reveals the resonance is nearly isotropic in spin space without any L modulations. Because of the unique monoclinic structure with additional zigzag arsenic chains, the As 4p orbitals contribute to a three-dimensional hole pocket around the Γ point and an extra electron pocket at the X point. Our results suggest that the energy and momentum distribution of the spin resonance does not directly respond to the k_{z} dependence of the fermiology, and the spin resonance intrinsically is a spin-1 mode from singlet-triplet excitations of the Cooper pairs in the case of weak spin-orbital coupling.

Two-Dimensional Massless Dirac Fermions in Antiferromagnetic AFe_{2}As_{2} (A=Ba,Sr).

We report infrared studies of AFe_{2}As_{2} (A=Ba, Sr), two representative parent compounds of iron-arsenide superconductors, at magnetic fields (B) up to 17.5 T. Optical transitions between Landau levels (LLs) were observed in the antiferromagnetic states of these two parent compounds. Our observation of a sqrt[B] dependence of the LL transition energies, the zero-energy intercepts at B=0 T under the linear extrapolations of the transition energies and the energy ratio (∼2.4) between the observed LL transitions, combined with the linear band dispersions in two-dimensional (2D) momentum space obtained by theoretical calculations, demonstrates the existence of massless Dirac fermions in the antiferromagnet BaFe_{2}As_{2}. More importantly, the observed dominance of the zeroth-LL-related absorption features and the calculated bands with extremely weak dispersions along the momentum direction k_{z} indicate that massless Dirac fermions in BaFe_{2}As_{2} are 2D. Furthermore, we find that the total substitution of the barium atoms in BaFe_{2}As_{2} by strontium atoms not only maintains 2D massless Dirac fermions in this system, but also enhances their Fermi velocity, which supports that the Dirac points in iron-arsenide parent compounds are topologically protected.

Unified Phase Diagram for Iron-Based Superconductors.

High-temperature superconductivity is closely adjacent to a long-range antiferromagnet, which is called a parent compound. In cuprates, all parent compounds are alike and carrier doping leads to superconductivity, so a unified phase diagram can be drawn. However, the properties of parent compounds for iron-based superconductors show significant diversity and both carrier and isovalent dopings can cause superconductivity, which casts doubt on the idea that there exists a unified phase diagram for them. Here we show that the ordered moments in a variety of iron pnictides are inversely proportional to the effective Curie constants of their nematic susceptibility. This unexpected scaling behavior suggests that the magnetic ground states of iron pnictides can be achieved by tuning the strength of nematic fluctuations. Therefore, a unified phase diagram can be established where superconductivity emerges from a hypothetical parent compound with a large ordered moment but weak nematic fluctuations, which suggests that iron-based superconductors are strongly correlated electron systems.

Effect of Nematic Order on the Low-Energy Spin Fluctuations in Detwinned BaFe_{1.935}Ni_{0.065}As_{2}.

The origin of nematic order remains one of the major debates in iron-based superconductors. In theories based on spin nematicity, one major prediction is that the spin-spin correlation length at (0,π) should decrease with decreasing temperature below the structural transition temperature T_{s}. Here, we report inelastic neutron scattering studies on the low-energy spin fluctuations in BaFe_{1.935}Ni_{0.065}As_{2} under uniaxial pressure. Both intensity and spin-spin correlation start to show anisotropic behavior at high temperature, while the reduction of the spin-spin correlation length at (0,π) happens just below T_{s}, suggesting the strong effect of nematic order on low-energy spin fluctuations. Our results favor the idea that treats the spin degree of freedom as the driving force of the electronic nematic order.

Nematic Quantum Critical Fluctuations in BaFe_{2-x}Ni_{x}As_{2}.

We have systematically studied the nematic fluctuations in the electron-doped iron-based superconductor BaFe_{2-x}Ni_{x}As_{2} by measuring the in-plane resistance change under uniaxial pressure. While the nematic quantum critical point can be identified through the measurements along the (110) direction, as studied previously, quantum and thermal critical fluctuations cannot be distinguished due to similar Curie-Weiss-like behaviors. Here we find that a sizable pressure-dependent resistivity along the (100) direction is present in all doping levels, which is against the simple picture of an Ising-type nematic model. The signal along the (100) direction becomes maximum at optimal doping, suggesting that it is associated with nematic quantum critical fluctuations. Our results indicate that thermal fluctuations from striped antiferromagnetic order dominate the underdoped regime along the (110) direction. We argue that either there is a strong coupling between the quantum critical fluctuations and the fermions, or more exotically, a higher symmetry may be present around optimal doping.

Nematic Crossover in BaFe(2)As(2) under Uniaxial Stress.

Raman scattering can detect spontaneous point-group symmetry breaking without resorting to single-domain samples. Here, we use this technique to study BaFe(2)As(2), the parent compound of the "122" Fe-based superconductors. We show that an applied compression along the Fe-Fe direction, which is commonly used to produce untwinned orthorhombic samples, changes the structural phase transition at temperature T(s) into a crossover that spans a considerable temperature range above T(s). Even in crystals that are not subject to any applied force, a distribution of substantial residual stress remains, which may explain phenomena that are seemingly indicative of symmetry breaking above T(s). Our results are consistent with an onset of spontaneous nematicity only below T(s).

Structural and Magnetic Phase Transitions near Optimal Superconductivity in BaFe2(As(1-x)Px)2.

We use nuclear magnetic resonance (NMR), high-resolution x-ray, and neutron scattering studies to study structural and magnetic phase transitions in phosphorus-doped BaFe2(As(1-x)P(x)2. Previous transport, NMR, specific heat, and magnetic penetration depth measurements have provided compelling evidence for the presence of a quantum critical point (QCP) near optimal superconductivity at x=0.3. However, we show that the tetragonal-to-orthorhombic structural (T{s}) and paramagnetic to antiferromagnetic (AF, TN) transitions in BaFe2(As(1-x)Px)2 are always coupled and approach T{N}≈T{s}≥T{c} (≈29 K) for x=0.29 before vanishing abruptly for x≥0.3. These results suggest that AF order in BaFe_{2}(As(1-x)Px)2 disappears in a weakly first-order fashion near optimal superconductivity, much like the electron-doped iron pnictides with an avoided QCP.

Spin excitation anisotropy as a probe of orbital ordering in the paramagnetic tetragonal phase of superconducting BaFe1.904Ni0.09As2.

We use polarized neutron scattering to demonstrate that in-plane spin excitations in electron doped superconducting BaFe1.904Ni0.096As2 (Tc=19.8 K) change from isotropic to anisotropic in the tetragonal phase well above the antiferromagnetic (AFM) ordering and tetragonal-to-orthorhombic lattice distortion temperatures (TN≈Ts=33±2 K) without an uniaxial pressure. While the anisotropic spin excitations are not sensitive to the AFM order and tetragonal-to-orthorhombic lattice distortion, superconductivity induces further anisotropy for spin excitations along the [110] and [110] directions. These results indicate that the spin excitation anisotropy is a probe of the electronic anisotropy or orbital ordering in the tetragonal phase of iron pnictides.

Avoided quantum criticality and magnetoelastic coupling in BaFe(2-x)Ni(x)As2.

We study the structural and magnetic orders in electron-doped BaFe(2-x)Ni(x)As2 by high-resolution synchrotron x-ray and neutron scatterings. Upon Ni doping x, the nearly simultaneous tetragonal-to-orthorhombic structural (T(s)) and antiferromagnetic (T(N)) phase transitions in BaFe2As2 are gradually suppressed and separated, resulting in T(s)>T(N) with increasing x, as was previously observed. However, the temperature separation between T(s) and T(N) decreases with increasing x for x≥0.065, tending toward a quantum bicritical point near optimal superconductivity at x≈0.1. The zero-temperature transition is preempted by the formation of a secondary incommensurate magnetic phase in the region 0.088≲x≲0.104, resulting in a finite value of T(N)≈T(c) + 10 K above the superconducting dome around x≈0.1. Our results imply an avoided quantum critical point, which is expected to strongly influence the properties of both the normal and superconducting states.

Coexistence and competition of the short-range incommensurate antiferromagnetic order with the superconducting state of BaFe(2-x)Ni(x)As2.

Superconductivity in the iron pnictides develops near antiferromagnetism, and the antiferromagnetic (AF) phase appears to overlap with the superconducting phase in some materials such as BaFe(2-x)T(x)As2 (where T=Co or Ni). Here we use neutron scattering to demonstrate that genuine long-range AF order and superconductivity do not coexist in BaFe(2-x)Ni(x)As2 near optimal superconductivity. In addition, we find a first-order-like AF-to-superconductivity phase transition with no evidence for a magnetic quantum critical point. Instead, the data reveal that incommensurate short-range AF order coexists and competes with superconductivity, where the AF spin correlation length is comparable to the superconducting coherence length.