Approaching Two-Dimensional Superconductivity in Ultrathin DyBa_{2}Cu_{3}O_{7-δ}.

The temperature dependence of the superfluid density ρ_{s}(T) has been measured for a series of ultrathin MBE-grown DyBa_{2}Cu_{3}O_{7-δ} superconducting (SC) films by submillimeter wave interferometry combined with time-domain terahertz spectroscopy and IR ellipsometry. We find that all films 10 u.c. and thicker show the same universal temperature dependence of ρ_{s}(T), which follows the critical behavior characteristic of single crystal YBa_{2}Cu_{3}O_{7-δ} as T approaches T_{c}. In 7 u.c. thick films, ρ_{s}(T) declines steeply upon approaching T_{c}, as expected for the Berezinskii-Kosterlitz-Thouless vortex unbinding transition. Our analysis provides evidence for a sharply defined 4 u.c. non-SC interfacial layer, leaving a quasi-2D SC layer on top. We propose that the SC state in this interfacial layer is suppressed by competing (possibly charge) order.

Stabilization of three-dimensional charge order in YBa2Cu3O6+x via epitaxial growth.

Incommensurate charge order (CO) has been identified as the leading competitor of high-temperature superconductivity in all major families of layered copper oxides, but the perplexing variety of CO states in different cuprates has confounded investigations of its impact on the transport and thermodynamic properties. The three-dimensional (3D) CO observed in YBa2Cu3O6+x in high magnetic fields is of particular interest, because quantum transport measurements have revealed detailed information about the corresponding Fermi surface. Here we use resonant X-ray scattering to demonstrate 3D-CO in underdoped YBa2Cu3O6+x films grown epitaxially on SrTiO3 in the absence of magnetic fields. The resonance profiles indicate that Cu sites in the charge-reservoir layers participate in the CO state, and thus efficiently transmit CO correlations between adjacent CuO2 bilayer units. The results offer fresh perspectives for experiments elucidating the influence of 3D-CO on the electronic properties of cuprates without the need to apply high magnetic fields.

High-temperature superconductivity at the lanthanum cuprate/lanthanum-strontium nickelate interface.

The utilization of interface effects in epitaxial systems at the nanoscale has emerged as a very powerful approach for engineering functional properties of oxides. Here we present a novel structure fabricated by a state-of-the-art oxide molecular beam epitaxy method and consisting of lanthanum cuprate and strontium (Sr)-doped lanthanum nickelate, in which interfacial high-temperature superconductivity (Tc up to 40 K) occurs at the contact between the two phases. In such a system, we are able to tune the superconducting properties simply by changing the structural parameters. By employing electron spectroscopy and microscopy combined with dedicated conductivity measurements, we show that decoupling occurs between the electronic charge carrier and the cation (Sr) concentration profiles at the interface and that a hole accumulation layer forms, which dictates the resulting superconducting properties. Such effects are rationalized in the light of a generalized space-charge theory for oxide systems that takes account of both ionic and electronic redistribution effects.

Transfer of Magnetic Order and Anisotropy through Epitaxial Integration of 3d and 4f Spin Systems.

Resonant x-ray scattering at the Dy M_{5} and Ni L_{3} absorption edges was used to probe the temperature and magnetic field dependence of magnetic order in epitaxial LaNiO_{3}-DyScO_{3} superlattices. For superlattices with 2 unit cell thick LaNiO_{3} layers, a commensurate spiral state develops in the Ni spin system below 100 K. Upon cooling below T_{ind}=18 K, Dy-Ni exchange interactions across the LaNiO_{3}-DyScO_{3} interfaces induce collinear magnetic order of interfacial Dy moments as well as a reorientation of the Ni spins to a direction dictated by the strong magnetocrystalline anisotropy of Dy. This transition is reversible by an external magnetic field of 3 T. Tailored exchange interactions between rare-earth and transition-metal ions thus open up new perspectives for the manipulation of spin structures in metal-oxide heterostructures and devices.

Long-range charge-density-wave proximity effect at cuprate/manganate interfaces.

The interplay between charge density waves (CDWs) and high-temperature superconductivity is currently under intense investigation. Experimental research on this issue is difficult because CDW formation in bulk copper oxides is strongly influenced by random disorder, and a long-range-ordered CDW state in high magnetic fields is difficult to access with spectroscopic and diffraction probes. Here we use resonant X-ray scattering in zero magnetic field to show that interfaces with the metallic ferromagnet La2/3Ca1/3MnO3 greatly enhance CDW formation in the optimally doped high-temperature superconductor YBa2Cu3O6+δ (δ ∼ 1), and that this effect persists over several tens of nanometres. The wavevector of the incommensurate CDW serves as an internal calibration standard of the charge carrier concentration, which allows us to rule out any significant influence of oxygen non-stoichiometry, and to attribute the observed phenomenon to a genuine electronic proximity effect. Long-range proximity effects induced by heterointerfaces thus offer a powerful method to stabilize the charge-density-wave state in the cuprates and, more generally, to manipulate the interplay between different collective phenomena in metal oxides.

High-temperature superconductivity in space-charge regions of lanthanum cuprate induced by two-dimensional doping.

The exploitation of interface effects turned out to be a powerful tool for generating exciting material properties. Such properties include magnetism, electronic and ionic transport and even superconductivity. Here, instead of using conventional homogeneous doping to enhance the hole concentration in lanthanum cuprate and achieve superconductivity, we replace single LaO planes with SrO dopant planes using atomic-layer-by-layer molecular beam epitaxy (two-dimensional doping). Electron spectroscopy and microscopy, conductivity measurements and zinc tomography reveal such negatively charged interfaces to induce layer-dependent superconductivity (Tc up to 35 K) in the space-charge zone at the side of the planes facing the substrate, where the strontium (Sr) profile is abrupt. Owing to the growth conditions, the other side exhibits instead a Sr redistribution resulting in superconductivity due to conventional doping. The present study represents a successful example of two-dimensional doping of superconducting oxide systems and demonstrates its power in this field.

Tunable Charge and Spin Order in PrNiO_{3} Thin Films and Superlattices.

We use polarized Raman scattering to probe lattice vibrations and charge ordering in 12 nm thick, epitaxially strained PrNiO_{3} films, and in superlattices of PrNiO_{3} with the band insulator PrAlO_{3}. A carefully adjusted confocal geometry is used to eliminate the substrate contribution to the Raman spectra. In films and superlattices under tensile strain which undergo a metal-insulator transition upon cooling, the Raman spectra reveal phonon modes characteristic of charge ordering. These anomalous phonons do not appear in compressively strained films, which remain metallic at all temperatures. For superlattices under compressive strain, the Raman spectra show no evidence of anomalous phonons indicative of charge ordering, while complementary resonant x-ray scattering experiments reveal antiferromagnetic order associated with a modest increase in resistivity upon cooling. This confirms theoretical predictions of a spin density wave phase driven by spatial confinement of the conduction electrons.

Sequence of hole resonances in complex oxide heterostructures.

Resonant soft x-ray scattering measurements at the O K edge on Sr2CuO4-ν/La2NiO4+δ (SCO/LNO) complex oxide superlattices show resonances for holes in the two constituent layers, in a sequence of energy levels. The observation of well defined resonances, on a superlattice with layers one unit cell thick, indicates that the resonance energy is largely unaffected by atoms outside a cluster extending half a unit cell along the c axis, consistent with calculations for bulk materials. Comparison to measurements on related superlattices confirms that the order of resonances at the O K edge reflects the order of hole ground-state energies in the heterostructure buried layers. For the SCO/LNO superlattices, the measurements show that the ground-state energies remain different in very thin SCO and LNO layers, which is a contributing factor when considering electronic reconstruction at interfaces, in addition to the areal density of ionic charges in the atomic planes. Different hole energy levels in the SCO/LNO superlattice also imply that holes do not spread into SCO from LNO layers.

Form factor dispersion at La M5,4 edges and average density of resonant atoms.

Resonant soft x-ray scattering on complex oxide superlattices shows very large variations in the superlattice reflection position and intensity near La M5,4 edges. Resonant dispersion of the La x-ray form factor describes the observations well. We determine the average density of resonant La atoms and the thickness of superlattice layers.

Anomalous independence of interface superconductivity from carrier density.

The recent discovery of superconductivity at the interface of two non-superconducting materials has received much attention. In cuprate bilayers, the critical temperature (Tc) can be significantly enhanced compared with single-phase samples. Several explanations have been proposed, invoking Sr interdiffusion, accumulation and depletion of mobile charge carriers, elongation of the copper-to-apical-oxygen bond length, or a beneficial crosstalk between a material with a high pairing energy and another with a large phase stiffness. From each of these models, one would predict Tc to depend strongly on the carrier density in the constituent materials. Here, we study combinatorial libraries of La(2-x)Sr(x)CuO4-La2CuO4 bilayer samples--an unprecedentedly large set of more than 800 different compositions. The doping level x spans a wide range, 0.15 < x < 0.47, and the measured Hall coefficient varies by one order of magnitude. Nevertheless, across the entire sample set, Tc stays essentially constant at about 40 K. We infer that doping up to the optimum level does not shift the chemical potential, unlike in ordinary Fermi liquids. This result poses a new challenge to theory--cuprate superconductors have not run out of surprises.

Emergence of superconductivity from the dynamically heterogeneous insulating state in La(2-x)Sr(x)CuO4.

A central issue for copper oxides is the nature of the insulating ground state at low carrier densities and the emergence of high-temperature superconductivity from that state with doping. Even though this superconductor-insulator transition (SIT) is a zero-temperature transition, measurements are not usually carried out at low temperatures. Here we use magnetoresistance to probe both the insulating state at very low temperatures and the presence of superconducting fluctuations in La(2-x)Sr(x)CuO(4) films, for doping levels that range from the insulator to the superconductor (x = 0.03-0.08). We observe that the charge glass behaviour, characteristic of the insulating state, is suppressed with doping, but it coexists with superconducting fluctuations that emerge already on the insulating side of the SIT. The unexpected quenching of the superconducting fluctuations by the competing charge order at low temperatures provides a new perspective on the mechanism for the SIT.

Orbital control of noncollinear magnetic order in nickel oxide heterostructures.

We have used resonant x-ray diffraction to develop a detailed description of antiferromagnetic ordering in epitaxial superlattices based on two-unit-cell thick layers of the strongly correlated metal LaNiO3. We also report reference experiments on thin films of PrNiO3 and NdNiO3. The resulting data indicate a spiral state whose polarization plane can be controlled by adjusting the Ni d-orbital occupation via two independent mechanisms: epitaxial strain and spatial confinement of the valence electrons. The data are discussed in light of recent theoretical predictions.

Insights from the study of high-temperature interface superconductivity.

A brief overview is given of the studies of high-temperature interface superconductivity based on atomic-layer-by-layer molecular beam epitaxy (ALL-MBE). A number of difficult materials science and physics questions have been tackled, frequently at the expense of some technical tour de force, and sometimes even by introducing new techniques. ALL-MBE is especially suitable to address questions related to surface and interface physics. Using this technique, it has been demonstrated that high-temperature superconductivity can occur in a single copper oxide layer-the thinnest superconductor known. It has been shown that interface superconductivity in cuprates is a genuine electronic effect-it arises from charge transfer (electron depletion and accumulation) across the interface driven by the difference in chemical potentials rather than from cation diffusion and mixing. We have also understood the nature of the superconductor-insulator phase transition as a function of doping. However, a few important questions, such as the mechanism of interfacial enhancement of the critical temperature, are still outstanding.

Two-dimensional magnetic and superconducting phases in metal-insulator La(2-x)Sr(x)CuO(4) superlattices measured by muon-spin rotation.

We show, by means of low-energy muon-spin rotation measurements, that few-unit-cells thick La(2)CuO(4) layers synthesized digitally by molecular beam epitaxy are antiferromagnetically ordered. Below a thickness of about 5 CuO(2) layers the long-range ordered state breaks down, and a magnetic state appears with enhanced quantum fluctuations and a reduced spin stiffness. This magnetic state can exist in close proximity (few Å) to high-temperature superconducting layers, without transmitting supercurrents.

High-temperature superconductivity in a single copper-oxygen plane.

The question of how thin cuprate layers can be while still retaining high-temperature superconductivity (HTS) has been challenging to address, in part because experimental studies require the synthesis of near-perfect ultrathin HTS layers and ways to profile the superconducting properties such as the critical temperature and the superfluid density across interfaces with atomic resolution. We used atomic-layer molecular beam epitaxy to synthesize bilayers of a cuprate metal (La(1.65)Sr(0.45)CuO4) and a cuprate insulator (La2CuO4) in which each layer is just three unit cells thick. We selectively doped layers with isovalent Zn atoms, which suppress superconductivity and act as markers, to show that this interface HTS occurs within a single CuO2 plane. This approach may also be useful in fabricating HTS devices.

Superconducting transition at 38 K in insulating-overdoped La2CuO4-La1.64Sr0.36CuO4 superlattices: evidence for interface electronic redistribution from resonant soft X-ray scattering.

We use resonant soft x-ray scattering (RSXS) to quantify the hole distribution in a superlattice of insulating La2CuO4 (LCO) and overdoped La2-xSrxCuO4 (LSCO). Despite its nonsuperconducting constituents, this structure is superconducting with T_{c}=38 K. We found that the conducting holes redistribute electronically from LSCO to the LCO layers. The LCO layers were found to be optimally doped, suggesting they are the main drivers of superconductivity. Our results demonstrate the utility of RSXS for separating electronic from structural effects at oxide interfaces.

High-temperature interface superconductivity between metallic and insulating copper oxides.

The realization of high-transition-temperature (high-T(c)) superconductivity confined to nanometre-sized interfaces has been a long-standing goal because of potential applications and the opportunity to study quantum phenomena in reduced dimensions. This has been, however, a challenging target: in conventional metals, the high electron density restricts interface effects (such as carrier depletion or accumulation) to a region much narrower than the coherence length, which is the scale necessary for superconductivity to occur. By contrast, in copper oxides the carrier density is low whereas T(c) is high and the coherence length very short, which provides an opportunity-but at a price: the interface must be atomically perfect. Here we report superconductivity in bilayers consisting of an insulator (La(2)CuO(4)) and a metal (La(1.55)Sr(0.45)CuO(4)), neither of which is superconducting in isolation. In these bilayers, T(c) is either approximately 15 K or approximately 30 K, depending on the layering sequence. This highly robust phenomenon is confined within 2-3 nm of the interface. If such a bilayer is exposed to ozone, T(c) exceeds 50 K, and this enhanced superconductivity is also shown to originate from an interface layer about 1-2 unit cells thick. Enhancement of T(c) in bilayer systems was observed previously but the essential role of the interface was not recognized at the time.

Combinatorial measurements of Hall effect and resistivity in oxide films.

A system for the simultaneous measurement of the Hall effect in 31 different locations as well as the measurement of the resistivity in 30 different locations on a single oxide thin film grown with a composition gradient is described. Considerations for designing and operating a high-throughput system for characterizing highly conductive oxides with Hall coefficients as small as 10(-10) m3/C are discussed. Results from measurements on films grown using combinatorial molecular beam epitaxy show the usefulness of characterizing combinatorial libraries via both the resistivity and the Hall effect.

Giant proximity effect in cuprate superconductors.

Using an advanced molecular beam epitaxy system, we have reproducibly synthesized atomically smooth films of high-temperature superconductors and uniform trilayer junctions with virtually perfect interfaces. We found that supercurrent runs through very thick barriers. We can rule out pinholes and microshorts; this "giant proximity effect" (GPE) is intrinsic. It defies the conventional explanation; it might originate in resonant tunneling through pair states in an almost-superconducting barrier. GPE may also be significant for superconducting electronics, since thick barriers are easier to fabricate.

No mixing of superconductivity and antiferromagnetism in a high-temperature superconductor.

There is still no universally accepted theory of high-temperature superconductivity. Most models assume that doping creates 'holes' in the valence band of an insulating, antiferromagnetic 'parent' compound, and that antiferromagnetism and high-temperature superconductivity are intimately related. If their respective energies are nearly equal, strong antiferromagnetic fluctuations (temporally and spatially restricted antiferromagnetic domains) would be expected in the superconductive phase, and superconducting fluctuations would be expected in the antiferromagnetic phase; the two states should 'mix' over an extended length scale. Here we report that one-unit-cell-thick antiferromagnetic La2CuO4 barrier layers remain highly insulating and completely block a supercurrent; the characteristic decay length is 1 A, indicating that the two phases do not mix. We likewise found that isolated one-unit-cell-thick layers of La1.85Sr0.15CuO4 remain superconducting. The latter further implies that, on doping, new electronic states are created near the middle of the bandgap. These two findings are in conflict with most proposed models, with a few notable exceptions that include postulated spin-charge separation.