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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Contrasting c -axis and in-plane uniaxial stress effects on superconductivity and stripe order in La 1.885 Ba 0.115 CuO 4

The cuprate superconductor La 2−x Ba x CuO 4 (LBCO) near x = 0.125 is a striking example of intertwined electronic orders, where 3D superconductivity is anomalously suppressed, allowing spin and charge stripe order to develop. Understanding this interplay remains a key challenge in cuprates, highlighting the necessity of external tuning for deeper insight. While in-plane uniaxial stress enhances superconductivity and suppresses stripe order, the effects of c -axis compression remains largely unexplored. Here, we use muon spin rotation ( μ SR) and AC susceptibility with an in situ piezoelectric stress device to investigate the spin-stripe order and superconductivity in LBCO-0.115 under c-axis compression. The measurements reveal a gradual suppression of the superconducting transition temperature ( T c ) with increasing c -axis stress, in stark contrast to the strong enhancement observed under in-plane stress. We further show that while in-plane stress rapidly reduces both the magnetic volume fraction ( V m ) and the spin-stripe ordering temperature ( T so ), c-axis compression has no effect, with V m and T so exhibiting an almost unchanged behavior up to the highest applied stress of 0.21 GPa. These findings demonstrate a strong anisotropy in stress response.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Elucidation of Ce/Zr ratio effects on the physical properties and catalytic performance of CuO x /Ce y Zr 1− y O 2 catalysts

Although cerium oxide (CeO 2 ) is widely used as a catalyst support, its limited defect sites and surface oxygen vacancy/mobility should be improved. The incorporation of zirconium (Zr) in the cerium (Ce) lattice is shown to increase the number of oxygen vacancies and improve catalytic activity. Using a fixed surface density (SD) of copper (∼2.3 Cu atoms per nm 2 ) as a surface species, the role of the support (Ce y Zr 1−y O 2 (y = 1.0, 0.9, 0.6, 0.5, and 0.0)) and defect site effects in the CO oxidation reaction was investigated. Spectroscopic (e.g., Raman, XRD, XPS) and microscopic (e.g., SEM-EDX, HR-TEM) characterization techniques were applied to evaluate the defect sites, crystallite size, lattice parameters, chemical composition, oxidation states of elements and microstructure of the catalysts. Here, the CO oxidation reaction with varied CO : O 2 ratios (1 : 5, 1 : 1, and 1 : 0.5 (stoichiometric)) was used as a model reaction to describe the relationship between the structure and the catalytic performance of each catalyst. Based on the characterization results of Ce y Zr 1−y O 2 materials, the addition of Zr causes physical and chemical changes to the overall material. The inclusion of Zr into the structure of CeO 2 decreased the overall lattice parameter of the catalyst and increased the number of defect sites. The prepared catalysts were able to reach complete CO conversion (∼100%) at low temperature conditions (<200 °C), each showing varied reaction activity. The difference in CO oxidation activity was then analyzed and related to the structure, wherein Cu loading, surface oxygen vacancies, reduction–oxidation ability, CuO x –support interaction and oxygen mobility in the catalyst were the crucial descriptors.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Synthesis of La 2–x Sr x CuO 4 films via atomic layer-by-layer molecular beam epitaxy

Atomic layer-by-layer molecular beam epitaxy (ALL-MBE) is a sophisticated technique to synthesize high-temperature superconductor (HTS) materials. ALL-MBE produces single-crystal HTS films with atomically smooth surfaces and interfaces, as well as precise multilayer heterostructures engineered down to a single atomic layer level. This enables the fabrication of tunnel junctions, nanowires, nanorings, and other HTS devices of interest. Our group has focused on ALL-MBE synthesis and materials science of La 2–x Sr x CuO 4 (LSCO), a representative HTS cuprate. In the past two decades, we have synthesized over three thousand LSCO thin films and characterized them by a range of analytical techniques. Here, we present in full detail a systematic process for the synthesis and engineering of atomically perfect LSCO films. The procedure includes the preparation of substrates, calibration of the elemental sources, the recipe for ALL growth of LSCO films without any secondary-phase precipitates, post-growth annealing of the films, and ex situ film characterization. This report should aid replication and dissemination of this technique of synthesizing single-crystal LSCO films for basic research as well as for HTS electronic applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Differentiated roles of Lifshitz transition on thermodynamics and superconductivity in La 2- x Sr x CuO 4

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.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Orbital-selective time-domain signature of nematicity dynamics in the charge-density-wave phase of La 1.65 Eu 0.2 Sr 0.15 CuO 4

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 L 3 and O K resonances, we investigate nonequilibrium dynamics of Q a = Q b = 0 nematic order and its association with both charge density wave (CDW) order and lattice dynamics in La 1.65 Eu 0.2 Sr 0.15 CuO 4 . The orbital selectivity of the resonant X-ray scattering cross-section allows nematicity dynamics associated with the planar O 2 p and Cu 3 d 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.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Ultra-thin ZrO 2 overcoating on CuO-ZnO-Al 2 O 3 catalyst by atomic layer deposition for improved catalytic performance of CO 2 hydrogenation to dimethyl ether

Abstract An ultra-thin overcoating of zirconium oxide (ZrO 2 ) film on CuO-ZnO-Al 2 O 3 (CZA) catalysts by atomic layer deposition (ALD) was proved to enhance the catalytic performance of CZA/HZSM-5 (H form of Zeolite Socony Mobil-5) bifunctional catalysts for hydrogenation of CO 2 to dimethyl ether (DME). Under optimal reaction conditions (i.e. 240 °C and 2.8 MPa), the yield of product DME increased from 17.22% for the bare CZA/HZSM-5 catalysts, to 18.40% for the CZA catalyst after 5 cycles of ZrO 2 ALD with HZSM-5 catalyst. All the catalysts modified by ZrO 2 ALD displayed significantly improved catalytic stability of hydrogenation of CO 2 to DME reaction, compared to that of CZA/HZSM-5 bifunctional catalysts. The loss of DME yield in 100 h of reaction was greatly mitigated from 6.20% (loss of absolute value) to 3.01% for the CZA catalyst with 20 cycles of ZrO 2 ALD overcoating. Characterizations including hydrogen temperature programmed reduction, x-ray powder diffraction, and x-ray photoelectron spectroscopy revealed that there was strong interaction between Cu active centers and ZrO 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Scaling behavior of low-temperature orthorhombic domains in the prototypical high-temperature superconductor La 1.875 Ba 0.125 CuO 4

Structural symmetry breaking and recovery in condensed-matter systems are closely related to exotic physical properties such as superconductivity (SC), magnetism, spin density waves, and charge density waves (CDWs). The interplay between different order parameters is intricate and often subject to intense debate, as in the case of CDW order and superconductivity. In La 1.875 Ba 0.125 CuO 4 (LBCO), the low-temperature structural domain walls are hypothesized as nanometer-scale pinning sites for the CDWs. Coherent x-ray diffraction techniques have been employed here to visualize the domain structures associated with these symmetry changes directly during phase transition. We have pushed Bragg coherent diffractive imaging (BCDI) into the cryogenic regime where most phase transitions in quantum materials reside. Utilizing BCDI, we image the structural evolution of LBCO microcrystal samples during the high-temperature tetragonal to low-temperature orthorhombic (LTO) phase transition. Our results show the formation of LTO domains close to the transition temperature and how the domain size decreases with temperature. In conclusion, the number of domains follows the secondary order parameter (or orthorhombic strain) measurement with a critical exponent that is consistent with the three-dimensional universality class.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Phonon spectrum of underdoped HgBa 2 CuO 4+δ investigated by neutron scattering

The cuprates exhibit a prominent charge-density-wave (CDW) instability with a wave vector along [100], i.e., the Cu-O bond direction. Whereas CDW order is most prominent at moderate doping and low temperature, there exists increasing evidence for dynamic charge correlations throughout a large portion of the temperature-doping phase diagram. In particular, the signatures of incipient charge order have been observed as phonon softening and/or broadening near the CDW wave vector approximately halfway through the Brillouin zone. Most of this work is focused on moderately doped cuprates, for which the CDW order is robust, or on optimally doped samples, for which the superconducting transition temperature (T c ) attains its maximum. Here we present a time-of-flight neutron scattering study of phonons in simple-tetragonal HgBa 2 CuO 4+δ (T c = 55 K) at a low doping level where prior work showed the CDW order to be weak. We employ and showcase a new software-based technique that mines a large number of measured Brillouin zones for useful data in order to improve accuracy and counting statistics. Density-functional theory has not provided an accurate description of phonons in HgBa2CuO4+δ, yet we find the right set of parameters to qualitatively reproduce the data. The notable exception is a dispersion minimum in the longitudinal Cu-O bond-stretching branch along [100]. Here, this discrepancy suggests that, while CDW order is weak, there exist significant dynamic charge correlations in the optic phonon range at low doping, near the edge of the superconducting dome.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Unexpected magnetic phase in the weakly ordered spin- 1 2 chain cuprate Sr 2 CuO 3

The magnetic phase diagram of a spin-$\frac{1}{2}$ chain antiferromagnet Sr 2 CuO 3 is studied by an ultrasound phase-sensitive detection technique. The system is in the extreme proximity of the Luttinger-liquid quantum-critical point and we observe an unusually strong effect of magnetic field, which is very weak compared to the in-chain interaction, on the Néel ordering temperature. Inside the ordered phase, we detect an unexpected, field-induced continuous phase transition. The transition is accompanied by softening of magnetic excitation observed by electron-spin resonance, which in previous work [E. G. Sergeicheva et al., Phys. Rev. B 95, 020411(R) (2017)] was associated with a longitudinal (amplitude) mode of the order parameter. These results suggest a transition from a transverse collinear antiferromagnet to an amplitude-modulated spin-density-wave phase in a very weak magnetic field, which is unexpected for a system of weakly coupled Heisenberg spin-$\frac{1}{2}$ chains.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Mobile orbitons in Ca 2 CuO 3 : Crucial role of Hund's exchange

We investigate the Cu L 3 edge resonant inelastic x-ray scattering (RIXS) spectra of a quasi-1D antiferromagnet Ca 2 CuO 3 . In addition to the magnetic excitations, which are well-described by the two-spinon continuum, we observe two dispersive orbital excitations, the 3d xy and the 3d yz orbitons. We carry out a quantitative comparison of the RIXS spectra, obtained with two distinct incident polarizations, with a theoretical model. We show that any realistic spin-orbital model needs to include a finite, but realistic, Hund's exchange J H ≈ 0.5 eV . Its main effect is an increase in orbiton velocities, so that their theoretically calculated values match those observed experimentally. Even though Hund's exchange also mediates some interaction between spinon and orbiton, the picture of spin-orbit separation remains intact and describes orbiton motion in this compound.

1-dimensional spin chains↗
DOE OSTI2021

Nature of the magnetic stripes in fully oxygenated La 2 CuO 4+y

We present triple-axis neutron scattering studies of static and dynamic magnetic stripes in an optimally oxygen-doped cuprate superconductor, La 2 CuO 4+y , which exhibits a clean superconducting transition at T c = 42 K. Polarization analysis reveals that the magnetic stripe structure is equally represented along both of the tetragonal crystal axes and that the fluctuating stripes display significant weight for in-plane as well as out-of-plane spin components. Both static magnetic order as well as low-energy fluctuations are fully developed in zero applied magnetic field and the low-energy spin fluctuations at ℏω = 0.3 – 10 meV intensify on cooling. We interpret this as an indication that superconductivity and low-energy spin fluctuations coexist microscopically in spatial regions which are separated from domains with static magnetic order.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Observation of cyclotron resonance and measurement of the hole mass in optimally doped La 2–x Sr x CuO 4

Using time-domain terahertz spectroscopy in pulsed magnetic fields up to 31 T, we measure the terahertz optical conductivity in an optimally doped thin film of the high-temperature superconducting cuprate La 1.84 Sr 0.16 CuO 4 . We observe systematic changes in the circularly polarized complex optical conductivity that are consistent with cyclotron absorption of p-type charge carriers characterized by a cyclotron mass of 4.9m e ± 0.8m e and a scattering rate that increases with magnetic field. Furthermore, these results open the door to studies aimed at characterizing the degree to which electron-electron interactions influence carrier masses in cuprate superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Experimental evidence that zinc impurities pin pair-density-wave order in La 2-x Ba x CuO 4

Both Zn doping and c-axis magnetic fields have been observed to increase the spin stripe order in La 2-x Ba x CuO 4 with x close to 1/8. For x = 0.095, the applied magnetic field also causes superconducting layers to decouple, presumably by favoring pair-density-wave order that consequently frustrates interlayer Josephson coupling. Here we show that introducing 1% Zn also leads to an initial onset of two-dimensional (2D) superconductivity, followed by 3D superconductivity at lower temperatures, even in zero field. Overall, we infer that the Zn pins pair-density-wave order locally, establishing the generality of such behavior.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Implications of second harmonic generation for hidden order in Sr 2 CuO 2 Cl 2

Sr 2 CuO 2 Cl 2 (SCOC) is a model undoped cuprate with I4/mmm crystallographic symmetry, and a simple magnetic space group CAmca with associated magnetic point group mmm1'. However, recent second harmonic spectroscopy in the antiferromagnetic phase has challenged this picture, suggesting instead a magnetic point group 4/mm'm' that coexists with the antiferromagnetism and breaks the two orthogonal mirror planes containing the tetragonal c axis. Here, we analyze the symmetry of SCOC in light of the second harmonic results, and discuss possible ground states that are consistent with the data.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Effect of the electronic charge gap on LO bond-stretching phonons in undoped La 2 CuO 4 calculated using LDA + U

Typical density-functional theory calculations that wrongly predict undoped cuprates to be metallic also predict Cu-O half- and full-breathing phonon energies that are significantly softer than observed, presumably because of weak on-site Coulomb repulsion on the Cu 3d orbitals. We used DFT+U calculations with antiferromagnetic supercells of La 2 CuO 4 to establish correlation between the on-site repulsion strength, tuned via adjusting the value of U, and phonon dispersions. Here, we find that breathing and half-breathing phonons reach experimental values when U is tuned to obtain the correct optical gap and magnetic moments. We demonstrate that using distorted supercells within DFT+U is a promising framework to model phonons in undoped cuprates and other perovskite oxides with complex, interrelated structural and electronic degrees of freedom.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Effect of radiation-induced defects on the superfluid density and optical conductivity of overdoped La 2 - x Sr x CuO 4

Using a combination of time-domain THz spectroscopy (TDTS) and mutual inductance measurements, we have investigated the low-energy electrodynamic response of overdoped La$_{2-x}$Sr$_x$CuO$_4$ films that have been exposed to ion irradiation. Films went through three rounds of irradiation (2, 4, and 6 $\times 10^{13}$ ions/cm$^2$) and mututal inductance and TDTS experiments were performed between each step. Together with the as-grown film, this gives four different levels of disorder. The transport scattering rate that is measured directly in the THz experiments is an approximately linear function of the radiation dose at all temperatures. This is consistent with a proportionate increase in elastic scattering from point-like 2D disorder. Here, in the superconducting state we find that the relation between T$_c$, the superfluid density, and the scattering rates are quantitatively at odds with the predictions based on the extant theory of Abrikosov-Gorkov-like pair breaking in a dirty d-wave superconductor. Increasing disorder causes only a small change in T$_c$ for the overdoped films, but the changes to the $\omega \sim 0$ superfluid density are much larger.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Strongly-overdoped $\mathrm{La}$ 2- $_{x}$$\mathrm{Sr}$$_{x}$$\mathrm{CuO}$ 4 : Evidence for Josephson-coupled grains of strongly-correlated superconductor

The interpretation of how superconductivity disappears in cuprates at large hole doping has been controversial. To address this issue, here we present an experimental study of single-crystal and thin film samples of La 2-x Sr x CuO 4 (LSCO) with x ≥0.25. In particular, measurements of bulk susceptibility on LSCO crystals with x = 0.25 indicate an onset of diamagnetism at T c1 =38.5 K, with a sharp transition to a phase with full bulk shielding at T c2 =18 K, independent of field direction. Strikingly, the in-plane resistivity only goes to zero at T c2 . Inelastic neutron scattering on 0.25 crystals confirms the presence of low-energy incommensurate magnetic excitations with reduced strength compared to lower doping levels. The ratio of the spin gap to T c2 is anomalously large. Our results are consistent with a theoretical prediction for strongly overdoped cuprates by Spivak, Oreto, and Kivelson, in which superconductivity initially develops within disconnected self-organized grains characterized by a reduced hole concentration, with bulk superconductivity occurring only after superconductivity is induced by proximity effect in the surrounding medium of higher hole concentration. Beyond the superconducting-to-metal transition, local differential conductance measurements on an LSCO thin film suggest that regions with pairing correlations survive, but are too dilute to support superconducting order. Future experiments will be needed to test the degree to which these results apply to overdoped cuprates in general.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗