Interplay between relaxational atomic fluctuations and charge density waves in La 2 − x Sr x CuO 4
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Electronic structure of high-temperature superconducting cuprates is studied by analyzing experimental data independently obtained from two complementary spectroscopies: one, quasiparticle interference (QPI) measured by scanning-tunneling microscopy, and the other, angle-resolved photoemission spectroscopy (ARPES). We combine these two sets of data in a unified theoretical analysis. Through explicit calculations of experimentally measurable quantities, we show that a simple two-component fermion model (TCFM) representing electron fractionalization succeeds in reproducing various detailed features of these experimental data: ARPES and QPI data are concomitantly reproduced by the TCFM in full energy and momentum spaces. The measured QPI pattern reveals a signature characteristic of the TCFM, distinct from the conventional single-component prediction, supporting the validity of the electron fractionalization in the cuprates. The integrated analysis also solves the puzzles of ARPES and QPI data that are seemingly inconsistent with each other. The overall success of the TCFM offers a comprehensive understanding of the electronic structure of the cuprates, in particular, the unoccupied side of the spectra, of which momentum-resolved structure has long been unexplored experimentally. We further predict that a characteristic QPI pattern should appear in the unoccupied high-energy part if the fractionalization is at work. We propose that integrated-spectroscopy analyses offer a promising way to explore challenging issues of strongly correlated electron systems.
Abstract In this paper we address the question of whether high-temperature superconductors have anything in common with BCS-BEC crossover theory. Towards this goal, we present a proposal and related predictions which provide a concrete test for the applicability of this theoretical framework. These predictions characterize the behavior of the Ginzburg-Landau coherence length, $${\xi }_{0}^{{{{\rm{coh}}}}}$$ ξ 0 coh , near the transition temperature T c , and across the entire superconducting T c dome in the phase diagram. That we are lacking a systematic characterization of $${\xi }_{0}^{{{{\rm{coh}}}}}$$ ξ 0 coh in the entire class of cuprate superconductors is perhaps surprising, as it is one of the most fundamental properties of any superconductor. This paper is written to motivate further experiments and, thus, address this shortcoming. Here we show how measurements of $${\xi }_{0}^{{{{\rm{coh}}}}}$$ ξ 0 coh contain direct indications for whether or not the cuprates are associated with BCS-BEC crossover and, if so, where within the crossover spectrum a particular superconductor lies.
Recent work has shown novel properties of twisted cuprates. In this paper, I point out that related phenomena occur intrinsically in bismuth-based cuprate superconductors due to the presence of the BiO supermodulation. As the ratio of the supermodulation potential to the superconducting energy gap increases, two critical points are found where semi-Dirac nodes form (that is, they have quadratic dispersion in one direction and linear dispersion in the orthogonal direction). The first critical point should be realized in Bi2212, the second in Bi2201. Implications of these findings are discussed.
Recent improvements in the energy resolution of resonant inelastic x-ray scattering experiments (RIXS) at the Cu-L 3 edge have enabled the study of lattice, spin, and charge excitations. Here, we report on the detection of a low-intensity signal at 140 meV, twice the energy of the bond-stretching (BS) phonon mode, in the cuprate superconductor Bi 2 Sr 2 CaCu 2 O 8+x (Bi-2212). Ultrahigh-resolution polarimetric RIXS measurements allow us to resolve the outgoing polarization of the signal and identify this feature as a two-phonon excitation. Further, here we study the connection between the two-phonon mode and the BS one-phonon mode by constructing a joint density of states toy model that reproduces the key features of the data.
Here, this Letter describes a simple mechanism for superconducting pairing with finite wave vector (pair density wave) based on weak coupling. The mechanism is illustrated with a quasi-one-dimensional model relevant to certain a class of quasi-one-dimensional materials. Within this model, pair and charge density wave order parameters are intertwined emerging as components of the same matrix field and are related by particle-hole symmetry.
The extremely overdoped cuprates are generally considered to be Fermi liquid metals without exotic orders, whereas the underdoped cuprates harbor intertwined states. Contrary to this conventional wisdom, using Cu L 3 -edge and O K-edge resonant x-ray scattering, we reveal a charge order (CO) correlation in overdoped La 2–x Sr x CuO 4 (0.35 ≤ x ≤0.6) beyond the superconducting dome. This CO has a periodicity of ~6 lattice units with correlation lengths of ~20 lattice units. It shows similar in-plane momentum and polarization dependence and dispersive excitations as the CO of underdoped cuprates, but its maximum intensity differs along the c direction and persists up to 300 K. This CO correlation cannot be explained by the Fermi surface instability and its origin remains to be understood. Finally, our results suggest that CO is prevailing in the overdoped metallic regime and requires a reassessment of the picture of overdoped cuprates as weakly correlated Fermi liquids.
A swift determination of superconductivity vs non-superconductivity of LK-99 demonstrates the importance of reproducibility in science. This has benefited from 4 decades study of high-temperature cuprate mechanism. Holy grail of room-temperature ambient-pressure superconductor remains to be pursued. Caution is needed about DFT calculations. Crucial old experimental data should be referenced. With the existing amount of experimentally discovered superconductors, could data science make a stride?
Karl Alex Mueller's intuition was that the nature of mobile charge carriers in manganates and nickelates should be like those in cuprates, which he believed were Jahn-Teller polarons, so he expected them to also host high-temperature superconductivity (HTS). Following his suggestions and persuasion, in the past, we performed several experiments that included atomic-layer-by-layer synthesis of novel, metastable manganates and nickelates. Despite our efforts and several USO sightings, here we failed to find any reproducible superconductivity and dropped the project fifteen years ago. Our results are presented here, for the first time - timely, since HTS was very recently discovered in nickelates (under pressure). So, whether his opinions were on the mark or not, Alex did guess it right - again.
Solid state chemistry has produced a plethora of materials with properties not found in nature. For example, high-temperature superconductivity in cuprates is drastically different from the superconductivity of naturally occurring metals and alloys and is frequently referred to as unconventional. Unconventional superconductivity is also found in other synthetic compounds, such as iron-based and heavy-fermion superconductors. Here, we report compelling evidence of unconventional nodal superconductivity in synthetic samples of Rh 17 S 15 (T c = 5.4 K), which is also found in nature as the mineral miassite. We investigated the temperature-dependent variation of the London penetration depth Δλ(T) and the disorder evolution of the critical superconducting temperature T c and the upper critical field H c2 (T) in single crystalline Rh 17 S 15 . We found a T - linear temperature variation of Δλ(T) below 0.3T c , which is consistent with the presence of nodal lines in the superconducting gap of Rh 17 S 15 . The nodal character of the superconducting state is supported by the observed suppression of T c and H c2 (T) in samples with a controlled level of non-magnetic disorder introduced by 2.5 MeV electron irradiation. We propose a nodal sign-changing superconducting gap in the A 1g irreducible representation, which preserves the cubic symmetry of the crystal and is in excellent agreement with the derived superfluid density. To the best of our knowledge, this establishes miassite as the only mineral known so far that reveals unconventional superconductivity in its clean synthetic form, though it is unlikely that it is present in natural crystals because of unavoidable impurities that quickly destroy nodal superconductivity.
Motivated by the recent observation of superconductivity in the pressurized trilayer Ruddlesden-Popper (RP) nickelate La 4 Ni 3 O 10 , we explore its structural, electronic, and magnetic properties as a function of hydrostatic pressure from first-principles calculations. We find that an orthorhombic (monoclinic)-to-tetragonal transition under pressure takes place concomitantly with the onset of superconductivity. The electronic structure of La 4 Ni 3 O 10 can be understood using a molecular trimer basis wherein n molecular subbands arise as the d z 2 orbitals hybridize strongly along the c axis within the trilayer. The magnetic tendencies indicate that the ground state at ambient pressure is formed by nonmagnetic inner planes and stripe-ordered outer planes that are antiferromagnetically coupled along the c axis, resulting in an unusual ↑, 0, ↓ stacking that is consistent with the spin density wave model previously suggested by neutron diffraction. Such a state is destabilized at the pressure where superconductivity arises. Despite the presence of d z 2 states at the Fermi level, the d x 2 –y 2 orbitals also play a key role in the electronic structure of La4Ni3O10. Finally, this active role of the d x 2 –y 2 states in the low-energy physics of the trilayer RP nickelate, together with the distinct electronic behavior of the inner and outer planes, resembles the physics of multilayer cuprates.
The high-temperature superconductivity in layered cuprates discovered by Bednorz and Müller arrived as a shock. Gradually, the presence of competing orders, such as antiferromagnetism and charge order, were discovered; however, the relationship to the superconductivity has been confusing. Importantly, it so happens that the original cuprate superconductor family La$_{2-x}$Ba$_x$CuO$_4$ contains all of the relevant phases, with extreme competition among them, and analysis of these phases provides strong clues to the nature of the superconductivity in cuprates.
Thermoelectric transport is widely used to study Abrikosov vortex dynamics in unconventional superconductors. However, only a few thermoelectric studies have been conducted near the dimensional crossover that occurs when the vortex-vortex interaction length scale becomes comparable to the sample size. Here, the effects of finite size on the dissipation mechanisms of the Nernst effect in the optimally doped Bi 2 Sr 2 CaCu 2 O 8 + x high-temperature superconductor are reported, down to the atomic length limit. To access this regime, a new generation of thermoelectric chips based on silicon nitride microprinted circuit boards is developed. These chips ensure optimized signals while preventing sample deterioration. The results demonstrate that lateral confinement at the nanoscale can effectively reduce vortex dissipation. Investigating vortex dissipation at the micro- and nano-scale is essential for creating stable, miniaturized superconducting circuits.
The discovery of superconductivity in square-planar nickelates has offered a rich materials platform to explore the origins of high-temperature superconductivity. However, experimental investigations have largely been limited to the infinite-layer R NiO 2 ( R , rare earth) nickelates. For this work we constructed a phase diagram of multilayer square-planar Nd n+1 Ni n O 2n+2 compounds and found signatures of superconductivity for dimensionality n = 4 to 8. Upon decreasing n , the superconducting anisotropy evolves owing to 4ƒ electron effects, and electronic structure characteristics approach cuprate-like behavior. Magnetic fluctuations persist from within the superconducting regime and into the overdoped, nonsuperconducting regime. The superconducting regime overlaps with that of chemically doped infinite-layer nickelates, demonstrating underlying commonalities as well as differences across varying structural realizations of square-planar nickelates. Our work establishes this layered template for creating new nickel-based superconductors.
In order to fully utilize the technological potential of unconventional superconductors, an enhanced understanding of the superconducting mechanism is necessary. In the best performing superconductors, the cuprates, superconductivity is intimately linked with magnetism, although the details of this coupling remain elusive. Here, we address this gap by studying the electron-doped cuprate Nd 1.85 Ce 0.15 CuO 4−δ that has an antiferromagnetic ground state when synthesized and only becomes superconducting after a reductive annealing process. Using neutron spectroscopy, we show that the as-grown crystal exhibits a large spin pseudogap in the magnetic fluctuation spectrum. Annealing removes defects introduced by the commonly employed synthesis method and significantly reduces the spin pseudogap. While the spin pseudogap in the annealed sample likely arises from superconductivity, in the as-grown sample it results from the absence of long-wavelength spin waves. These results reveal a direct connection between defects, magnetism, and superconductivity, offering new insight into the mechanisms underlying high-temperature superconductivity and guiding the design of improved superconducting materials.
Elucidating spin correlations in the parent compounds of high-temperature superconductors is crucial for understanding superconductivity. We used neutron scattering to study spin correlations in Li 1–x Fe x ODFeSe, an insulating material with reduced electron carriers compared to its superconducting counterpart (T c = 41 K), serving as the undoped parent compound. Our findings show a reduced total fluctuating moment in this insulator relative to FeSe and 122 iron pnictides, likely due to increased interlayer distances from intercalation, which enhance fluctuations and reduce the intensity of spin excitations. Moreover, we observed a V-shaped spin wavelike excitation dispersion, contrasting with the twisted hourglass pattern in the superconducting counterpart. Electron doping shifts spin excitation from (π,0) point to an incommensurate position towards (π,π) direction below 65 meV. In conclusion, this transition from V-shaped to hourglasslike dispersion, akin to behaviors in hole-doped cuprates, suggests a potential shared mechanism in magnetism and superconductivity across these diverse systems.
In this study, the pursuit of discovering new high-temperature superconductors that diverge from the copper-based model has profound implications for explaining mechanisms behind superconductivity and may also enable new applications. Here our investigation shows that the application of pressure effectively suppresses the spin–charge order in trilayer nickelate La 4 Ni 3 O 10-δ single crystals, leading to the emergence of superconductivity with a maximum critical temperature (T c ) of around 30 K at 69.0 GPa. The d.c. susceptibility measurements confirm a substantial diamagnetic response below T c , indicating the presence of bulk superconductivity with a volume fraction exceeding 80%. In the normal state, we observe a strange metal behaviour, characterized by a linear temperature-dependent resistance extending up to 300 K. Furthermore, the layer-dependent superconductivity observed hints at a unique interlayer coupling mechanism specific to nickelates, setting them apart from cuprates in this regard. Our findings provide crucial insights into the fundamental mechanisms underpinning superconductivity, while also introducing a new material platform to explore the intricate interplay between the spin–charge order, flat band structures, interlayer coupling, strange metal behaviour and high-temperature superconductivity.
Large Language Models (LLMs) show great promise as a powerful tool for scientific literature exploration. However, their effectiveness in providing scientifically accurate and comprehensive answers to complex questions within specialized domains remains an active area of research. Using the field of high-temperature cuprates as an exemplar, we evaluate the ability of LLM systems to understand the literature at the level of an expert. We construct an expert-curated database of 1,726 scientific papers that covers the history of the field, and a set of 67 expert-formulated questions that probe deep understanding of the literature. We then evaluate six different LLM-based systems for answering these questions, including both commercially available closed models and a custom retrieval-augmented generation (RAG) system capable of retrieving images alongside text. Experts then evaluate the answers of these systems against a rubric that assesses balanced perspectives, factual comprehensiveness, succinctness, and evidentiary support. Among the six systems, two using RAG on curated literature outperformed existing closed models across key metrics, particularly in providing comprehensive and well-supported answers. We discuss promising aspects of LLM performances as well as critical short-comings of all the models. The set of expert-formulated questions and the rubric will be valuable for assessing expert level performance of LLM based reasoning systems.