Orbital-selective time-domain signature of nematicity dynamics in the charge-density-wave phase of La1.65Eu0.2Sr0.15CuO4.

Understanding the interplay between charge, nematic, and structural ordering tendencies in cuprate superconductors is critical to unraveling their complex phase diagram. Using pump-probe time-resolved resonant X-ray scattering on the (0 0 1) Bragg peak at the Cu [Formula: see text] and O [Formula: see text] resonances, we investigate nonequilibrium dynamics of [Formula: see text] nematic order and its association with both charge density wave (CDW) order and lattice dynamics in La[Formula: see text]Eu[Formula: see text]Sr[Formula: see text]CuO[Formula: see text]. The orbital selectivity of the resonant X-ray scattering cross-section allows nematicity dynamics associated with the planar O 2[Formula: see text] and Cu 3[Formula: see text] states to be distinguished from the response of anisotropic lattice distortions. A direct time-domain comparison of CDW translational-symmetry breaking and nematic rotational-symmetry breaking reveals that these broken symmetries remain closely linked in the photoexcited state, consistent with the stability of CDW topological defects in the investigated pump fluence regime.

Two superconducting states with broken time-reversal symmetry in FeSe1-xSx.

Iron-chalcogenide superconductors FeSe1-xSx possess unique electronic properties such as nonmagnetic nematic order and its quantum critical point. The nature of superconductivity with such nematicity is important for understanding the mechanism of unconventional superconductivity. A recent theory suggested the possible emergence of a fundamentally new class of superconductivity with the so-called Bogoliubov Fermi surfaces (BFSs) in this system. However, such an ultranodal pair state requires broken time-reversal symmetry (TRS) in the superconducting state, which has not been observed experimentally. Here, we report muon spin relaxation (µSR) measurements in FeSe1-xSx superconductors for 0 ≤ x ≤ 0.22 covering both orthorhombic (nematic) and tetragonal phases. We find that the zero-field muon relaxation rate is enhanced below the superconducting transition temperature Tc for all compositions, indicating that the superconducting state breaks TRS both in the nematic and tetragonal phases. Moreover, the transverse-field µSR measurements reveal that the superfluid density shows an unexpected and substantial reduction in the tetragonal phase (x > 0.17). This implies that a significant fraction of electrons remain unpaired in the zero-temperature limit, which cannot be explained by the known unconventional superconducting states with point or line nodes. The TRS breaking and the suppressed superfluid density in the tetragonal phase, together with the reported enhanced zero-energy excitations, are consistent with the ultranodal pair state with BFSs. The present results reveal two different superconducting states with broken TRS separated by the nematic critical point in FeSe1-xSx, which calls for the theory of microscopic origins that account for the relation between nematicity and superconductivity.

Optically Probing Unconventional Superconductivity in Atomically Thin Bi2Sr2Ca0.92Y0.08Cu2O8+δ.

Atomically thin cuprates exhibiting a superconducting phase transition temperature similar to that of the bulk have recently been realized, although the device fabrication remains a challenge and limits the potential for many novel studies and applications. Here, we use an optical pump-probe approach to noninvasively study the unconventional superconductivity in atomically thin Bi2Sr2Ca0.92Y0.08Cu2O8+δ (Y-Bi2212). Apart from finding an optical response due to the superconducting phase transition that is similar to that of bulk Y-Bi2212, we observe that the sign and amplitude of the pump-probe signal in atomically thin flakes vary significantly in different dielectric environments depending on the nature of the optical excitation. By exploiting the spatial resolution of the optical probe, we uncover the exceptional sensitivity of monolayer Y-Bi2212 to the environment. Our results provide the first optical evidence for the intralayer nature of the superconducting condensate in Bi2212 and highlight the role of double-sided encapsulation in preserving superconductivity in atomically thin cuprates.

Comparative Electronic Structures of the Chiral Helimagnets Cr1/3NbS2 and Cr1/3TaS2.

Magnetic materials with noncollinear spin textures are promising for spintronic applications. To realize practical devices, control over the length and energy scales of such spin textures is imperative. The chiral helimagnets Cr1/3NbS2 and Cr1/3TaS2 exhibit analogous magnetic-phase diagrams with different real-space periodicities and field dependence, positioning them as model systems for studying the relative strengths of the microscopic mechanisms giving rise to exotic spin textures. Although the electronic structure of the Nb analogue has been experimentally investigated, the Ta analogue has received far less attention. Here, we present a comprehensive suite of electronic structure studies on both Cr1/3NbS2 and Cr1/3TaS2 using angle-resolved photoemission spectroscopy and density functional theory. We show that bands in Cr1/3TaS2 are more dispersive than their counterparts in Cr1/3NbS2, resulting in markedly different Fermi wavevectors. The fact that their qualitative magnetic phase diagrams are nevertheless identical shows that hybridization between the intercalant and host lattice mediates the magnetic exchange interactions in both of these materials. We ultimately find that ferromagnetic coupling is stronger in Cr1/3TaS2, but larger spin-orbit coupling (and a stronger Dzyaloshinskii-Moriya interaction) from the heavier host lattice ultimately gives rise to shorter spin textures.

Fano interference between collective modes in cuprate high-Tc superconductors.

Cuprate high-Tc superconductors are known for their intertwined interactions and the coexistence of competing orders. Uncovering experimental signatures of these interactions is often the first step in understanding their complex relations. A typical spectroscopic signature of the interaction between a discrete mode and a continuum of excitations is the Fano resonance/interference, characterized by the asymmetric light-scattering amplitude of the discrete mode as a function of the electromagnetic driving frequency. In this study, we report a new type of Fano resonance manifested by the nonlinear terahertz response of cuprate high-Tc superconductors, where we resolve both the amplitude and phase signatures of the Fano resonance. Our extensive hole-doping and magnetic field dependent investigation suggests that the Fano resonance may arise from an interplay between the superconducting fluctuations and the charge density wave fluctuations, prompting future studies to look more closely into their dynamical interactions.

High-order replica bands in monolayer FeSe/SrTiO3 revealed by polarization-dependent photoemission spectroscopy.

The mechanism of the enhanced superconductivity in monolayer FeSe/SrTiO3 has been enthusiastically studied and debated over the past decade. One specific observation has been taken to be of central importance: the replica bands in the photoemission spectrum. Although suggestive of electron-phonon interaction in the material, the essence of these spectroscopic features remains highly controversial. In this work, we conduct angle-resolved photoemission spectroscopy measurements on monolayer FeSe/SrTiO3 using linearly polarized photons. This configuration enables unambiguous characterization of the valence electronic structure with a suppression of the spectral background. We consistently observe high-order replica bands derived from various Fe 3d bands, similar to those observed on bare SrTiO3. The intensity of the replica bands is unexpectedly high and different between dxy and dyz bands. Our results provide new insights on the electronic structure of this high-temperature superconductor and the physical origin of the photoemission replica bands.

2D-Berry-Curvature-Driven Large Anomalous Hall Effect in Layered Topological Nodal-Line MnAlGe.

Topological magnets comprising 2D magnetic layers with Curie temperatures (TC ) exceeding room temperature are key for dissipationless quantum transport devices. However, the identification of a material with 2D ferromagnetic planes that exhibits an out-of-plane-magnetization remains a challenge. This study reports a ferromagnetic, topological, nodal-line, and semimetal MnAlGe composed of square-net Mn layers that are separated by nonmagnetic Al-Ge spacers. The 2D ferromagnetic Mn layers exhibit an out-of-plane magnetization below TC  ≈ 503 K. Density functional calculations demonstrate that 2D arrays of Mn atoms control the electrical, magnetic, and therefore topological properties in MnAlGe. The unique 2D distribution of the Berry curvature resembles the 2D Fermi surface of the bands that form the topological nodal line near the Fermi energy. A large anomalous Hall conductivity of ≈700 S cm-1 is obtained at 2 K and related to this nodal-line-induced 2D Berry curvature distribution. The high transition temperature, large anisotropic out-of-plane magnetism, and natural heterostructure-type atomic arrangements consisting of magnetic Mn and nonmagnetic Al/Ge elements render nodal-line MnAlGe one of the few, unique, and layered topological ferromagnets that have ever been observed.

Separation between low-energy hole dynamics and spin dynamics in a frustrated magnet.

An angle-resolved photoemission spectroscopy (ARPES) study is reported on a Mott insulator NiGa2S4 in which Ni2+ (S=1) ions form a triangular lattice and the Ni spins do not order even in its ground state. The first ARPES study on the two-dimensional spin-disordered system shows that low-energy hole dynamics at high temperatures is characterized by wave vectors Q(E) which are different from wave vectors Q(M) dominating low-energy spin excitations at low temperatures. The unexpected difference between Q(E) and Q(M) is deeply related to charge fluctuation across the Mott gap in the frustrated lattice and is a key issue to understand the spin-disordered ground states in Mott insulators.

Dynamics of correlation-frozen antinodal quasiparticles in superconducting cuprates.

Many puzzling properties of high-critical temperature (Tc) superconducting (HTSC) copper oxides have deep roots in the nature of the antinodal quasiparticles, the elementary excitations with wave vector parallel to the Cu-O bonds. These electronic states are most affected by the onset of antiferromagnetic correlations and charge instabilities, and they host the maximum of the anisotropic superconducting gap and pseudogap. We use time-resolved extreme-ultraviolet photoemission with proper photon energy (18 eV) and time resolution (50 fs) to disclose the ultrafast dynamics of the antinodal states in a prototypical HTSC cuprate. After photoinducing a nonthermal charge redistribution within the Cu and O orbitals, we reveal a dramatic momentum-space differentiation of the transient electron dynamics. Whereas the nodal quasiparticle distribution is heated up as in a conventional metal, new quasiparticle states transiently emerge at the antinodes, similarly to what is expected for a photoexcited Mott insulator, where the frozen charges can be released by an impulsive excitation. This transient antinodal metallicity is mapped into the dynamics of the O-2p bands, thus directly demonstrating the intertwining between the low- and high-energy scales that is typical of correlated materials. Our results suggest that the correlation-driven freezing of the electrons moving along the Cu-O bonds, analogous to the Mott localization mechanism, constitutes the starting point for any model of high-Tc superconductivity and other exotic phases of HTSC cuprates.

Quasi-particle interference of heavy fermions in resonant x-ray scattering.

Resonant x-ray scattering (RXS) has recently become an increasingly important tool for the study of ordering phenomena in correlated electron systems. Yet, the interpretation of RXS experiments remains theoretically challenging because of the complexity of the RXS cross section. Central to this debate is the recent proposal that impurity-induced Friedel oscillations, akin to quasi-particle interference signals observed with a scanning tunneling microscope (STM), can lead to scattering peaks in RXS experiments. The possibility that quasi-particle properties can be probed in RXS measurements opens up a new avenue to study the bulk band structure of materials with the orbital and element selectivity provided by RXS. We test these ideas by combining RXS and STM measurements of the heavy fermion compound CeMIn5 (M = Co, Rh). Temperature- and doping-dependent RXS measurements at the Ce-M4 edge show a broad scattering enhancement that correlates with the appearance of heavy f-electron bands in these compounds. The scattering enhancement is consistent with the measured quasi-particle interference signal in the STM measurements, indicating that the quasi-particle interference can be probed through the momentum distribution of RXS signals. Overall, our experiments demonstrate new opportunities for studies of correlated electronic systems using the RXS technique.

Doping-dependent charge order correlations in electron-doped cuprates.

Understanding the interplay between charge order (CO) and other phenomena (for example, pseudogap, antiferromagnetism, and superconductivity) is one of the central questions in the cuprate high-temperature superconductors. The discovery that similar forms of CO exist in both hole- and electron-doped cuprates opened a path to determine what subset of the CO phenomenology is universal to all the cuprates. We use resonant x-ray scattering to measure the CO correlations in electron-doped cuprates (La2-x Ce x CuO4 and Nd2-x Ce x CuO4) and their relationship to antiferromagnetism, pseudogap, and superconductivity. Detailed measurements of Nd2-x Ce x CuO4 show that CO is present in the x = 0.059 to 0.166 range and that its doping-dependent wave vector is consistent with the separation between straight segments of the Fermi surface. The CO onset temperature is highest between x = 0.106 and 0.166 but decreases at lower doping levels, indicating that it is not tied to the appearance of antiferromagnetic correlations or the pseudogap. Near optimal doping, where the CO wave vector is also consistent with a previously observed phonon anomaly, measurements of the CO below and above the superconducting transition temperature, or in a magnetic field, show that the CO is insensitive to superconductivity. Overall, these findings indicate that, although verified in the electron-doped cuprates, material-dependent details determine whether the CO correlations acquire sufficient strength to compete for the ground state of the cuprates.

Charge ordering in the electron-doped superconductor Nd(2-x)Ce(x)CuO4.

In cuprate high-temperature superconductors, an antiferromagnetic Mott insulating state can be destabilized toward unconventional superconductivity by either hole or electron doping. In hole-doped (p-type) cuprates, a charge ordering (CO) instability competes with superconductivity inside the pseudogap state. We report resonant x-ray scattering measurements that demonstrate the presence of charge ordering in the n-type cuprate Nd(2-x)Ce(x)CuO4 near optimal doping. We find that the CO in Nd(2-x)Ce(x)CuO4 occurs with similar periodicity, and along the same direction, as in p-type cuprates. However, in contrast to the latter, the CO onset in Nd(2-x)Ce(x)CuO4 is higher than the pseudogap temperature, and is in the temperature range where antiferromagnetic fluctuations are first detected. Our discovery opens a parallel path to the study of CO and its relationship to antiferromagnetism and superconductivity.

Revealing the high-energy electronic excitations underlying the onset of high-temperature superconductivity in cuprates.

In strongly correlated systems the electronic properties at the Fermi energy (E(F)) are intertwined with those at high-energy scales. One of the pivotal challenges in the field of high-temperature superconductivity (HTSC) is to understand whether and how the high-energy scale physics associated with Mott-like excitations (|E-E(F)|>1 eV) is involved in the condensate formation. Here, we report the interplay between the many-body high-energy CuO(2) excitations at 1.5 and 2 eV, and the onset of HTSC. This is revealed by a novel optical pump-supercontinuum-probe technique that provides access to the dynamics of the dielectric function in Bi(2)Sr(2)Ca(0.92)Y(0.08)Cu(2)O(8+δ) over an extended energy range, after the photoinduced suppression of the superconducting pairing. These results unveil an unconventional mechanism at the base of HTSC both below and above the optimal hole concentration required to attain the maximum critical temperature (T(c)).