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The occurrence of superconductivity in proximity to various strongly correlated phases of matter has drawn extensive focus on their normal state properties, to develop an understanding of the state from which superconductivity emerges1-4. The recent finding of superconductivity in layered nickelates raises similar interests5-8. However, transport measurements of doped infinite-layer nickelate thin films have been hampered by materials limitations of these metastable compounds: in particular, a high density of extended defects9-11. Here, by moving to a substrate (LaAlO3)0.3(Sr2TaAlO6)0.7 that better stabilizes the growth and reduction conditions, we can synthesize the doping series of Nd1-xSrxNiO2 essentially free from extended defects. In their absence, the normal state resistivity shows a low-temperature upturn in the underdoped regime, linear behaviour near optimal doping and quadratic temperature dependence for overdoping. This is phenomenologically similar to the copper oxides2,12 despite key distinctions-namely, the absence of an insulating parent compound5,6,9,10, multiband electronic structure13,14 and a Mott-Hubbard orbital alignment rather than the charge-transfer insulator of the copper oxides15,16. We further observe an enhancement of superconductivity, both in terms of transition temperature and range of doping. These results indicate a convergence in the electronic properties of both superconducting families as the scale of disorder in the nickelates is reduced.
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The discoveries of ferromagnetism down to the atomically thin limit in van der Waals (vdW) crystals by mechanical exfoliation have enriched the family of magnetic thin films [C. Gong et al., Nature 546, 265-269 (2017) and B. Huang et al., Nature 546, 270-273 (2017)]. However, compared to the study of traditional magnetic thin films by physical deposition methods, the toolbox of the vdW crystals based on mechanical exfoliation and transfer suffers from low yield and ambient corrosion problem and now is facing new challenges to study magnetism. For example, the formation of magnetic superlattice is difficult in vdW crystals, which limits the study of the interlayer interaction in vdW crystals [M. Gibertini, M. Koperski, A. F. Morpurgo, K. S. Novoselov, Nat. Nanotechnol. 14, 408-419 (2019)]. Here, we report a strategy of interlayer engineering of the magnetic vdW crystal Fe3GeTe2 (FGT) by intercalating quaternary ammonium cations into the vdW spacing. Both three-dimensional (3D) vdW superlattice and two-dimensional (2D) vdW monolayer can be formed by using this method based on the amount of intercalant. On the one hand, the FGT superlattice shows a strong 3D critical behavior with a decreased coercivity and increased domain wall size, attributed to the co-engineering of the anisotropy, exchange interaction, and electron doping by intercalation. On the other hand, the 2D vdW few layers obtained by over-intercalation are capped with organic molecules from the bulk crystal, which not only enhances the ferromagnetic transition temperature (TC), but also substantially protects the thin samples from degradation, thus allowing the preparation of large-scale FGT ink in ambient environment.
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The discovery of superconductivity in infinite-layer nickelates established another category of unconventional superconductors that shares structural and electronic similarities with cuprates. However, key issues of the superconducting pairing symmetry, gap amplitude and superconducting fluctuations are yet to be addressed. Here we utilize static and ultrafast terahertz spectroscopy to address these. We demonstrate that the equilibrium terahertz conductivity and non-equilibrium terahertz responses of an optimally Sr-doped nickelate film (superconducting transition temperature of Tc = 17 K) are in line with the electrodynamics of d-wave superconductivity in the dirty limit. The gap-to-Tc ratio (2Δ/kBTc) is found to be 3.4, indicating that the superconductivity falls in the weak coupling regime. In addition, we observed substantial superconducting fluctuations near Tc that do not extend into the deep normal state as the optimally hole-doped cuprates do. Our results support a d-wave system that closely resembles the electron-doped cuprates.
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The discovery of unconventional superconductivity in (La,Ba)2CuO4 (ref. 1) has motivated the study of compounds with similar crystal and electronic structure, with the aim of finding additional superconductors and understanding the origins of copper oxide superconductivity. Isostructural examples include bulk superconducting Sr2RuO4 (ref. 2) and surface-electron-doped Sr2IrO4, which exhibits spectroscopic signatures consistent with a superconducting gap3,4, although a zero-resistance state has not yet been observed. This approach has also led to the theoretical investigation of nickelates5,6, as well as thin-film heterostructures designed to host superconductivity. One such structure is the LaAlO3/LaNiO3 superlattice7-9, which has been recently proposed for the creation of an artificially layered nickelate heterostructure with a singly occupied [Formula: see text] band. The absence of superconductivity observed in previous related experiments has been attributed, at least in part, to incomplete polarization of the eg orbitals10. Here we report the observation of superconductivity in an infinite-layer nickelate that is isostructural to infinite-layer copper oxides11-13. Using soft-chemistry topotactic reduction14-20, NdNiO2 and Nd0.8Sr0.2NiO2 single-crystal thin films are synthesized by reducing the perovskite precursor phase. Whereas NdNiO2 exhibits a resistive upturn at low temperature, measurements of the resistivity, critical current density and magnetic-field response of Nd0.8Sr0.2NiO2 indicate a superconducting transition temperature of about 9 to 15 kelvin. Because this compound is a member of a series of reduced layered nickelate crystal structures21-23, these results suggest the possibility of a family of nickelate superconductors analogous to copper oxides24 and pnictides25.
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Nickel-based superconductors provide a long-awaited experimental platform to explore possible cuprate-like superconductivity. Despite similar crystal structure and d electron filling, however, superconductivity in nickelates has thus far only been stabilized in thin-film geometry, raising questions about the polar interface between substrate and thin film. Here we conduct a detailed experimental and theoretical study of the prototypical interface between Nd1-xSrxNiO2 and SrTiO3. Atomic-resolution electron energy loss spectroscopy in the scanning transmission electron microscope reveals the formation of a single intermediate Nd(Ti,Ni)O3 layer. Density functional theory calculations with a Hubbard U term show how the observed structure alleviates the polar discontinuity. We explore the effects of oxygen occupancy, hole doping and cation structure to disentangle the contributions of each for reducing interface charge density. Resolving the non-trivial interface structure will be instructive for future synthesis of nickelate films on other substrates and in vertical heterostructures.
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The recent observation of superconductivity in [Formula: see text] has raised fundamental questions about the hierarchy of the underlying electronic structure. Calculations suggest that this system falls in the Mott-Hubbard regime, rather than the charge-transfer configuration of other nickel oxides and the superconducting cuprates. Here, we use state-of-the-art, locally resolved electron energy-loss spectroscopy to directly probe the Mott-Hubbard character of [Formula: see text] Upon doping, we observe emergent hybridization reminiscent of the Zhang-Rice singlet via the oxygen-projected states, modification of the Nd 5d states, and the systematic evolution of Ni 3d hybridization and filling. These experimental data provide direct evidence for the multiband electronic structure of the superconducting infinite-layer nickelates, particularly via the effects of hole doping on not only the oxygen but also nickel and rare-earth bands.
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Freestanding films provide a versatile platform for materials engineering thanks to additional structural motifs not found in films with a substrate. A ubiquitous example is wrinkles, yet little is known about how they can develop over as fast as a few picoseconds due to a lack of experimental probes to visualize their dynamics in real time on the nanoscopic scale. Here, we use time-resolved electron diffraction to directly observe light-activated wrinkling formation in freestanding La2/3Ca1/3MnO3 films. Via a "lock-in" analysis of oscillations in the diffraction peak position, intensity, and width, we quantitatively reconstructed how wrinkles develop on the time scale of lattice vibration. Contrary to the common assumption of fixed boundary conditions, we found that wrinkle development is associated with ultrafast delamination at the film boundaries. Our work provides a generic protocol to quantify wrinkling dynamics in freestanding films and highlights the importance of the film-substrate interaction in determining the properties of freestanding structures.
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A new synthetic approach has recently been developed for the fabrication of freestanding crystalline perovskite oxide nanomembranes, which involves the epitaxial growth of a water-soluble sacrificial layer. By utilizing an ultrathin capping layer of SrTiO3, here we show that this sacrificial layer, as grown by pulsed laser deposition, can be stabilized in air and therefore be used as transferrable templates for ex situ epitaxial growth using other techniques. We find that the stability of these templates depends on the thickness of the capping layer. On these templates, freestanding superconducting SrTiO3 membranes were synthesized ex situ using molecular beam epitaxy, enabled by the lower growth temperature which preserves the sacrificial layer. This study paves the way for the synthesis of an expanded selection of freestanding oxide membranes and heterostructures with a wide variety of ex situ growth techniques.
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A variety of nickel oxide compounds have long been studied for their manifestation of various correlated electron phenomena. Recently, superconductivity was observed in nanoscale infinite layer nickelate thin films of Nd0.8Sr0.2NiO2, epitaxially stabilized on SrTiO3 substrates via topotactic reduction from the perovskite precursor phase. Here, we present the synthesis and properties of PrNiO2 thin films on SrTiO3. Upon doping in Pr0.8Sr0.2NiO2, we observe superconductivity with a transition temperature of 7-12 K and robust critical current density at 2 K of 334 kA/cm2. These findings indicate that superconductivity in the infinite layer nickelates is relatively insensitive to the details of the rare earth 4f configuration. Furthermore, they motivate the exploration of a broader family of compounds based on two-dimensional NiO2 planes, which will enable systematic investigation of the superconducting and normal state properties and their underlying mechanisms.
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We report the phase diagram of Nd_{1-x}Sr_{x}NiO_{2} infinite layer thin films grown on SrTiO_{3}. A superconducting dome spanning 0.125
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Terpenoids constitute the largest class of natural products with complex structures, essential functions, and versatile applications. Creation of new building blocks beyond the conventional five-carbon (C5) units, dimethylallyl diphosphate (DMAPP) and isopentenyl diphosphate, expands significantly the chemical space of terpenoids. Structure-guided engineering of an S-adenosylmethionine-dependent geranyl diphosphate (GPP) C2-methyltransferase from Streptomyces coelicolor yielded variants converting DMAPP to a new C6 unit, 2-methyl-DMAPP. Mutation of the Gly residue at the position 202 resulted in a smaller substrate-binding pocket to fit DMAPP instead of its native substrate GPP. Replacement of Phe residue at the position 222 with a Tyr residue contributed to DMAPP binding via hydrogen bond. Furthermore, using Escherichia coli as the chassis, we demonstrated that 2-methyl-DMAPP was accepted as a start unit to generate noncanonical trans- and cis-prenyl diphosphates (C5n+1) and terpenoids. This work provides insights into substrate recognition of prenyl diphosphate methyltransferases, and strategies to diversify terpenoids by expanding the building block portfolio.
RESUMEN
The search for superconductivity in infinite-layer nickelates was motivated by analogy to the cuprates, and this perspective has framed much of the initial consideration of this material. However, a growing number of studies have highlighted the involvement of rare-earth orbitals; in that context, the consequences of varying the rare-earth element in the superconducting nickelates have been much debated. Here, we show notable differences in the magnitude and anisotropy of the superconducting upper critical field across the La-, Pr-, and Nd-nickelates. These distinctions originate from the 4f electron characteristics of the rare-earth ions in the lattice: They are absent for La3+, nonmagnetic for the Pr3+ singlet ground state, and magnetic for the Nd3+ Kramer's doublet. The unique polar and azimuthal angle-dependent magnetoresistance found in the Nd-nickelates can be understood to arise from the magnetic contribution of the Nd3+ 4f moments. Such robust and tunable superconductivity suggests potential in future high-field applications.
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Lithium intercalation of MoS2 is generally believed to introduce a phase transition from H phase (semiconducting) to T phase (metallic). However, during the intercalation process, a spatially sharp boundary is usually formed between the fully intercalated T phase MoS2 and non-intercalated H phase MoS2. The intermediate state, i.e., lightly intercalated H phase MoS2 without a phase transition, is difficult to investigate by optical-microscope-based spectroscopy due to the narrow size. Here, we report the stabilization of the intermediate state across the whole flake of twisted bilayer MoS2. The twisted bilayer system allows the lithium to intercalate from the top surface and enables fast Li-ion diffusion by the reduced interlayer interaction. The E2g Raman mode of the intermediate state shows a peak splitting behavior. Our simulation results indicate that the intermediate state is stabilized by lithium-induced symmetry breaking of the H phase MoS2. Our results provide an insight into the non-uniform intercalation during battery charging and discharging, and also open a new opportunity to modulate the properties of twisted 2D systems with guest species doping in the Moiré structures.
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The occurrence of unconventional superconductivity in cuprates has long motivated the search for manifestations in other layered transition metal oxides. Recently, superconductivity is found in infinite-layer nickelate (Nd,Sr)NiO2 and (Pr,Sr)NiO2 thin films, formed by topotactic reduction from the perovskite precursor phase. A topic of much current interest is whether rare-earth moments are essential for superconductivity in this system. In this study, it is found that with significant materials optimization, substantial portions of the La1- x Srx NiO2 phase diagram can enter the regime of coherent low-temperature transport (x = 0.14 - 0.20), with subsequent superconducting transitions and a maximum onset of ≈9 K at x = 0.20. Additionally, the unexpected indication of a superconducting ground state in undoped LaNiO2 is observed, which likely reflects the self-doped nature of the electronic structure. Combining the results of (La/Pr/Nd)1- x Srx NiO2 reveals a generalized superconducting dome, characterized by systematic shifts in the unit cell volume and in the relative electron-hole populations across the lanthanides.
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A defining feature of emergent phenomena in complex oxides is the competition and cooperation between ground states. In manganites, the balance between metallic and insulating phases can be tuned by the lattice; extending the range of lattice control would enhance the ability to access other phases. We stabilized uniform extreme tensile strain in nanoscale La0.7Ca0.3MnO3 membranes, exceeding 8% uniaxially and 5% biaxially. Uniaxial and biaxial strain suppresses the ferromagnetic metal at distinctly different strain values, inducing an insulator that can be extinguished by a magnetic field. Electronic structure calculations indicate that the insulator consists of charge-ordered Mn4+ and Mn3+ with staggered strain-enhanced Jahn-Teller distortions within the plane. This highly tunable strained membrane approach provides a broad opportunity to design and manipulate correlated electron states.
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Advances in complex oxide heteroepitaxy have highlighted the enormous potential of utilizing strain engineering via lattice mismatch to control ferroelectricity in thin-film heterostructures. This approach, however, lacks the ability to produce large and continuously variable strain states, thus limiting the potential for designing and tuning the desired properties of ferroelectric films. Here, we observe and explore dynamic strain-induced ferroelectricity in SrTiO3 by laminating freestanding oxide films onto a stretchable polymer substrate. Using a combination of scanning probe microscopy, optical second harmonic generation measurements, and atomistic modeling, we demonstrate robust room-temperature ferroelectricity in SrTiO3 with 2.0% uniaxial tensile strain, corroborated by the notable features of 180° ferroelectric domains and an extrapolated transition temperature of 400 K. Our work reveals the enormous potential of employing oxide membranes to create and enhance ferroelectricity in environmentally benign lead-free oxides, which hold great promise for applications ranging from non-volatile memories and microwave electronics.
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OBJECTIVE: To observe clinical therapeutic effect of moxibustion and acupuncture at Zusanli (ST 36) on refractory facial paralysis. METHODS: Sixty cases were randomly divided into a test group and a control group, 30 cases in each group. The control group were treated with acupuncture at Hegu (LI 4), Taichong (LR 3), Touwei (ST 8), etc. , and the test group with acupuncture at the same points as those in the control group plus moxibustion and acupuncture at Zusanli (ST 36) with a warm-heat sense transmitting into the depth of the point along the needle body for the patient. RESULTS: The total effective rate of 93.3% in the test group was significantly better than 76.7 in the control group (P < 0.05); in the test group, the total effective rate for the patients with needling sensation propagating along the channel was 100%, which was significantly superior to 80.00% in the patients with no needling sensation propagating along the channel (P < 0.05). CONCLUSION: Moxibustion and acupuncture at Zusanli (ST 36) activating sensation propagating along channel as main way has a better therapeutic effect on refractory facial paralysis.