It has recently become clear that phonons generate a sizable thermal Hall effect in cuprates, whether they are undoped, electron-doped or hole-doped (inside the pseudogap phase). At higher doping, where cuprates are reasonably good metals, mobile electrons also generate a thermal Hall effect, the thermal equivalent of the standard electrical Hall effect. Here we show that in the cleanest crystals of the electron-doped cuprate Nd$_{2-x}$Ce$_{x}$CuO$_{4}$, at high doping, the phonon and electron contributions to the thermal Hall conductivity $\kappa_{\rm {xy}}$ are of comparable magnitude, but of opposite sign. In samples of lower quality, phonons dominate $\kappa_{\rm {xy}}$, resulting in a negative $\kappa_{\rm {xy}}$ at all temperatures. The fact that the negative phononic $\kappa_{\rm {xy}}$ in the metallic state is similar in magnitude and temperature dependence to that found in the insulating state at lower doping rules out any mechanism based on skew scattering of phonons off charged impurities, since a local charge should be screened in the metallic regime. The phononic $\kappa_{\rm {xy}}$ is found to persist over the entire doping range where antiferromagnetic correlations are known to be significant, suggesting that such correlations may play a role in generating the phonon thermal Hall effect in electron-doped cuprates. If the same mechanism is also at play in hole-doped cuprates, the presence of a phononic $\kappa_{\rm {xy}}$ below (and only below) the critical doping $p^{\star}$ would be evidence that spin correlations are a property of the pseudogap phase.
A Kondo insulator (KI) is a prototypical example of a highly entangled phase of matter, where many-body interactions between local moments and delocalized electrons engender the non-magnetic insulating ground state. Conventionally, the local moments arise from atomic multiplet states with a narrow bandwidth, limiting Kondo coherence to low temperatures. Here, we realize a new paradigm for constructing the KI state with hybridized molecular orbitals in FeSb2. Resonant inelastic X-ray scattering (RIXS) at the Fe L-edge reveals distinct signatures of band-like continuum states and localized states. Comparisons with first-principles calculations establish a mixed-configuration ground state with hybridized Fe d-Sb p molecular orbitals as basis states. By systematically investigating the RIXS momentum, temperature, and doping dependences, we find propagating collective modes commensurate with many-body charge and spin excitations. Our results pave the way for understanding the emerging class of unconventional d electron insulators and engineering high temperature Kondo many-body states.
Metallic systems with delocalized valence electrons host collective charge density oscillations known as plasmons. On the other hand, conventional insulators do not have free electrons and the low energy charge degrees of freedom are pinned to the ions. The fate of the collective charge excitations in the intermediate regime is an outstanding question. This problem is especially important for strongly correlated systems such as the layered cuprates, where unconventional superconductivity and other emergent phenomena arise from valence electrons on the border between Mott localization and itinerancy. Using resonant inelastic X-ray scattering, we track this evolution in the prototypical electron-doped cuprate Nd2-xCexCuO4. We find a continuous transformation of the low-energy charge response: from an acoustic plasmon in the metallic regime, to a gapped hybrid mode at intermediate doping, and finally to a nearly dispersionless 139 meV excitation at half filling. Remarkably, the 139 meV excitation has approximately twice the energy of the oxygen breathing phonon responsible for the dispersion kink observed in angle-resolved photoemission spectroscopy, and is consistent with a putative 2-phonon excitation observed in Raman spectroscopy. These results establish a unified picture of collective charge excitations across the phase diagram of electron-doped cuprates, showing that such modes persist across the Mott transition via strong coupling to lattice degrees of freedom and revealing a missing link in the charge dynamics of carrier doped Mott insulators.
Elucidating the microscopic behavior of cuprates under ultrafast photoexcitation offers critical insights into their highly correlated out-of-equilibrium states. Although quasiparticle dynamics have been investigated extensively, the behavior of collective magnetic excitations remains comparatively unexplored. Here, we use time-resolved resonant inelastic X-ray scattering (trRIXS) at the Cu L_3-edge to track the collective magnetic excitations (paramagnons) in an optimally electron-doped cuprate driven out-of-equilibrium by a femtosecond pump laser pulse. Upon pumping, we observed an anti-Stokes signal associated with paramagnon generation, which modifies the paramagnon dispersion near the zone center, although the bandwidth remained unchanged. Moreover, the spectral weight exhibits a momentum-dependent variation across the Brillouin zone. The light-driven boost of the paramagnon population and the resulting spectral-weight transfer could provide new leverage to manipulate the properties of cuprates.
In crystals and molecules with strong coupling between the charge carriers and atomic vibrations, high order harmonics of the vibrational excitations can be observed with intensity following the Franck-Condon envelope. Here, we uncover a new regime of electron-phonon coupling in La2-xSrxCuO4 using resonant inelastic X-ray scattering. In the undoped compound, we find sharp peaks at approximately 85±5 meV, 180±7 meV, and 330±5 meV with no observable dispersion, and an absence of appreciable intensity from other modes observed in Raman spectroscopy in this energy range. The 180 meV and 330 meV excitations have energies approximately consistent with two-phonon and four-phonon in-plane Cu-O bond stretching mode, suggesting that the resonantly excited valence electrons strongly couple to this mode. These excitations exhibit significant doping dependence, eventually becoming unresolvable at 10
Recent studies of La_{3}Ni_{2}O_{7} have identified a bilayer (2222) structure and an unexpected alternating monolayer-trilayer (1313) structure, both of which feature signatures of superconductivity near 80 K under high pressures. Using angle-resolved photoemission spectroscopy, we measure the electronic structure of 1313 samples. In contrast to the previously studied 2222 structure, we find that the 1313 structure hosts a flat band with a markedly different binding energy, as well as an additional electron pocket and band splittings. By comparison to local-density approximation calculations, we find renormalizations of the Ni-d_{z^{2}} and Ni-d_{x^{2}-y^{2}} derived bands to be about 5 to 7 and about 4, respectively, suggesting strong correlation effects. These results reveal important differences in the electronic structure brought about by the distinct structural motifs with the same stoichiometry. Such differences may be relevant to the putative high temperature superconductivity.
Signatures of superconductivity near 80 K were recently discovered in crystals of La-Ni-O with the stoichiometry of 3:2:7 under high pressures. Structural studies have shown conflicting results highlighting both the expected bilayer (2222) structure and an unexpected alternating monolayer-trilayer (1313) structure, both apparently showing superconductivity. Here, we perform angle-resolved photoemission spectroscopy on crystals with the 1313 structure to elucidate the distinct electronic features compared to the previously studied 2222 structure. Our measurements suggest that a flat band of high electron density is much closer to the Fermi energy in the 1313 structure compared to the 2222 structure. Furthermore, we observe an additional electron pocket at the Brillouin zone center with Ni-$d_{z^2}$ orbital character, highlighting the importance of the out-of-plane orbital component. In comparison to LDA+U band structure calculations, we find strong renormalization of both the Ni-$d_{z^2}$ and Ni-$d_{x^2-y^2}$ derived bands, suggesting strong correlation effects beyond that of moderate Hubbard physics. These results reveal important differences in the electronic structure brought about by the distinct structural motifs with the same stoichiometry. Such differences may contain the key to understanding superconductivity in the layered perovskite nickelates.
We present local and nonlocal electrical transport measurements of the correlated insulator FeSb_2. By employing wiring configurations that delineate between bulk- and surface-dominated conduction, we reveal the formation of a metallic surface state in FeSb_2 for temperatures ⪅ 5 K. This result is corroborated by an angular rotation study of this material's magnetotransport, which also shows signatures of the transition from bulk- to surface-dominated conduction over the same temperature interval as the local/nonlocal transport divergence. Notable similarities with the topological Kondo insulator candidate SmB_6 are discussed.
A surprising "planar" thermal Hall effect, whereby the field is parallel to the current, has recently been observed in a few magnetic insulators, and this has been attributed to exotic excitations such as Majorana fermions or chiral magnons. Here we investigate the possibility of a planar thermal Hall effect in three different cuprate materials, in which the conventional thermal Hall conductivity $\kappa_{\rm {xy}}$ (with an out-of-plane field perpendicular to the current) is dominated by either electrons or phonons. Our measurements show that the planar $\kappa_{\rm {xy}}$ from electrons in cuprates is zero, as expected from the absence of a Lorentz force in the planar configuration. By contrast, we observe a sizable planar $\kappa_{\rm {xy}}$ in those samples where the thermal Hall response is due to phonons, even though it should in principle be forbidden by the high crystal symmetry. Our findings call for a careful re-examination of the mechanisms responsible for the phonon thermal Hall effect in insulators.
Spin- and charge-lattice interactions are potential key factors in the microscopic mechanism of high-temperature superconductivity in cuprates. Although both interactions can dramatically shape the low-energy electronic structure, their phenomenological roles in superconductivity are usually investigated independently. Employing angle-resolved photoemission spectroscopy, we reveal the spectroscopic fingerprint of short-range antiferromagnetic order in conjunction with enhanced electron-phonon interaction in the electron-doped cuprate superconductor Nd_1.85Ce_0.15CuO_4. The observed mode coupling exhibits a strong momentum dependence that is in striking contrast to the node-antinode dichotomy previously observed in the hole-doped cuprates. Our results reveal an intimate relationship between electron-phonon coupling and antiferromagnetic fluctuations, which collectively sets the stage for unconventional superconductivity in the electron-doped cuprates.
In the underdoped n-type cuprate Nd 2- x Ce x CuO 4 , long-range antiferromagnetic order reconstructs the Fermi surface, resulting in a putative antiferromagnetic metal with small Fermi pockets. Using angle-resolved photoemission spectroscopy, we observe an anomalous energy gap, an order of magnitude smaller than the antiferromagnetic gap, in a wide portion of the underdoped regime and smoothly connecting to the superconducting gap at optimal doping. After considering all the known ordering tendencies in tandem with the phase diagram, we hypothesize that the normal-state gap in the underdoped n-type cuprates originates from Cooper pairing. The high temperature scale of the normal-state gap raises the prospect of engineering higher transition temperatures in the n-type cuprates comparable to those of the p-type cuprates.
Electron-doped cuprates consistently exhibit strong antiferromagnetic correlations, leading to the prevalent belief that antiferromagnetic spin fluctuations mediate Cooper pairing in these unconventional superconductors. However, early investigations showed that although antiferromagnetic spin fluctuations create the largest pseudogap at hot spots in momentum space, the superconducting gap is also maximized at these locations. This presented a paradox for spin-fluctuation-mediated pairing: Cooper pairing is strongest at momenta where the normal-state low-energy spectral weight is most suppressed. Here we investigate this paradox and find evidence that a gossamer—meaning very faint—Fermi surface can provide an explanation for these observations. We study Nd 2– x Ce x CuO 4 using angle-resolved photoemission spectroscopy and directly observe the Bogoliubov quasiparticles. First, we resolve the previously observed reconstructed main band and the states gapped by the antiferromagnetic pseudogap around the hot spots. Within the antiferromagnetic pseudogap, we also observe gossamer states with distinct dispersion, from which coherence peaks of Bogoliubov quasiparticles emerge below the superconducting critical temperature. Moreover, the direct observation of a Bogoliubov quasiparticle permits an accurate determination of the superconducting gap, yielding a maximum value an order of magnitude smaller than the pseudogap, establishing the distinct nature of these two gaps. We propose that orientation fluctuations in the antiferromagnetic order parameter are responsible for the gossamer states.
Measurements of the thermal Hall conductivity in hole-doped cuprates have shown that phonons acquire chirality in a magnetic field both in the pseudogap phase and in the Mott insulator state. The microscopic mechanism at play is still unclear. A number of theoretical proposals are being considered including skew scattering of phonons by various defects, the coupling of phonons to spins, and a state of loop-current order with the appropriate symmetries, but more experimental information is required to constrain theoretical scenarios. Here we present our study of the thermal Hall conductivity kappa xy in the electron-doped cuprates Nd2-xCexCuO4 and Pr2-xCexCuO4 for dopings across the phase diagram, from x = 0 in the insulating antiferromagnetic phase up to x = 0.17 in the metallic phase above optimal doping. We observe a large negative thermal Hall conductivity at all dopings in both materials. Since heat conduction perpendicular to the CuO2 planes is dominated by phonons, the large thermal Hall conductivity we observe in electron-doped cuprates for a heat current in that direction must also be due to phonons, as in hole-doped cuprates. However, the degree of chirality, measured as the ratio |kappa xy/kappa xx| where kappa xx is the longitudinal thermal conductivity, is much larger in the electron-doped cuprates. We discuss various factors that may be involved in the mechanism that confers chirality to phonons in cuprates, including short-range spin correlations.
The effect of Lifshitz transition on thermodynamics and superconductivity in hole-doped cuprates has been heavily debated but remains an open question. In particular, an observed peak of electronic specific heat is proposed to originate from fluctuations of a putative quantum critical point p* (e.g., the termination of pseudogap at zero temperature), which is close to but distinguishable from the Lifshitz transition in overdoped La-based cuprates where the Fermi surface transforms from hole-like to electron-like. Here we report an in situ angle-resolved photoemission spectroscopy study of three-dimensional Fermi surfaces in La 2- x Sr x CuO 4 thin films ( x = 0.06 to 0.35). With accurate k z dispersion quantification, the said Lifshitz transition is determined to happen within a finite range around x = 0.21. Normal state electronic specific heat, calculated from spectroscopy-derived band parameters, reveals a doping-dependent profile with a maximum at x = 0.21 that agrees with previous thermodynamic microcalorimetry measurements. The account of the specific heat maximum by underlying band structures excludes the need for additionally dominant contribution from the quantum fluctuations at p* . A d -wave superconducting gap smoothly across the Lifshitz transition demonstrates the insensitivity of superconductivity to the dramatic density of states enhancement.
Since its discovery as a Kondo insulator 50 years ago, SmB6 recently received a revival of interest due to detection of unexpected quantum oscillations in the insulating state, discovery of disorder-immune bulk transport, and proposals of correlation-driven topological physics. While recent transport results attribute the anomalous low temperature conduction to two-dimensional surface states, important alternatives, such as conduction channel residing in one-dimensional dislocation lines, have not been adequately explored. Here we study SmB6 with scanning microwave impedance microscopy and uncover evidence for conducting one-dimensional states terminating at surface step edges. These states remain conducting up to room temperature, indicating unusual robustness against scattering and an unconventional origin. Our results bring to light a heretofore undetected conduction route in SmB6 that contributes to the low temperature transport. The unique scenario of intrinsic one-dimensional conducting channels in a highly insulating correlated bulk offers a one-dimensional platform that may host exotic physics.
The resistance of a conventional insulator diverges as temperature approaches zero. The peculiar low temperature resistivity saturation in the 4f Kondo insulator (KI) SmB6 has spurred proposals of a correlation-driven topological Kondo insulator (TKI) with exotic ground states. However, the scarcity of model TKI material families leaves difficulties in disentangling key ingredients from irrelevant details. Here we use angle-resolved photoemission spectroscopy (ARPES) to study FeSb2, a correlated d-electron KI candidate that also exhibits a low temperature resistivity saturation. On the (010) surface, we find a rich assemblage of metallic states with two-dimensional dispersion. Measurements of the bulk band structure reveal band renormalization, a large temperature-dependent band shift, and flat spectral features along certain high symmetry directions, providing spectroscopic evidence for strong correlations. Our observations suggest that exotic insulating states resembling those in SmB6 and YbB12 may also exist in systems with d instead of f electrons.
Time- and angle-resolved photoemission spectroscopy is a powerful probe of electronic band structures out of equilibrium. Tuning time and energy resolution to suit a particular scientific question has become an increasingly important experimental consideration. Many instruments use cascaded frequency doubling in nonlinear crystals to generate the required ultraviolet probe pulses. We demonstrate how calculations clarify the relationship between laser bandwidth and nonlinear crystal thickness contributing to experimental resolutions and place intrinsic limits on the achievable time-bandwidth product. Experimentally, we tune time and energy resolution by varying the thickness of nonlinear $\beta$-BaB$_2$O$_4$ crystals for frequency up-conversion, providing for a flexible experiment design. We achieve time resolutions of 58 to 103 fs and corresponding energy resolutions of 55 to 27 meV.