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1.
Sci Adv ; 8(29): eabn6882, 2022 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-35857841

RESUMO

The detection and manipulation of antiferromagnetic domains and topological antiferromagnetic textures are of central interest to solid-state physics. A fundamental step is identifying tools to probe the mesoscopic texture of an antiferromagnetic order parameter. In this work, we demonstrate that Bragg coherent diffractive imaging can be extended to study the mesoscopic texture of an antiferromagnetic order parameter using resonant magnetic x-ray scattering. We study the onset of the antiferromagnet transition in PrNiO3, focusing on a temperature regime in which the antiferromagnetic domains are dilute in the beam spot and the coherent diffraction pattern modulating the antiferromagnetic peak is greatly simplified. We demonstrate that it is possible to extract the arrangements and sizes of these domains from single diffraction patterns and show that the approach could be extended to a time-structured light source to study the motion of dilute domains or the motion of topological defects in an antiferromagnetic spin texture.

2.
Adv Mater ; 34(35): e2202971, 2022 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-35817958

RESUMO

Devices with tunable magnetic noncollinearity are important components of superconducting electronics and spintronics, but they typically require epitaxial integration of several complex materials. The spin-polarized neutron reflectometry measurements on La1-x Srx MnO3 homojunction arrays with modulated Sr concentration reported herein have led to the discovery of magnetic fan structures with highly noncollinear alignment of Mn spins and an emergent periodicity twice as large as the array's unit cell. The neutron data show that these magnetic superstructures can be fully long-range ordered, despite the gradual modulation of the doping level created by charge transfer and chemical intermixing. The degree of noncollinearity can be effectively adjusted by low magnetic fields. Notwithstanding their chemical and structural simplicity, oxide homojunctions thus show considerable promise as a platform for tunable complex magnetism and as a powerful design element of spintronic devices.

3.
Sci Rep ; 12(1): 830, 2022 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-35039561

RESUMO

We report a Spectroscopic Imaging Scanning Tunneling Microscopy (SI-STM) study of a DyBa2Cu3O7-δ (DBCO) thin film (Tc ~ 79 K) synthesized by the molecular beam epitaxy (MBE). We observed an unusual transfer of spectral weight in the local density of states (LDOS) spectra occurring only within the superconducting gap. By a systematic control of the tip-sample distance and the junction resistance, we demonstrate that the spectral weight transfer can be switched at a nano-meter length scale. These results suggest that an interaction between the STM tip and the sample alters the electronic configurations in the film. This probably originates from a combination of an intrinsic band bending at the interface between the surface and the bulk, and a tip-induced band bending. These results may open a new avenue for band engineering and applications of thin films of high-Tc cuprates.

4.
Nanoscale ; 13(48): 20663-20669, 2021 Dec 16.
Artigo em Inglês | MEDLINE | ID: mdl-34878472

RESUMO

Ruddlesden-Popper (RP) faults have emerged as a promising candidate for defect engineering in epitaxial ABO3 perovskites. Functionalities could be fine-tuned by incorporating RP faults into ABO3 thin films and superlattices. However, due to the lattice expansion at AO-AO interfaces, it is generally believed that RP faults are only energetically favorable under tensile strain. Contrary to this common cognition, here we present that compressive strain must be regarded as an alternative driving force for creating RP faults. Unlike the conventional perovskite-to-rock-salt transition, the RP faults originated from Shockley partial dislocations bounded by stacking faults on the basal plane. The edge-type partials gave rise to strain relaxation, facilitating the formation of RP faults under compressive strain. We envisage that our results will give new insights into the rational design and defect engineering in epitaxial-strained ABO3 perovskites.

5.
Proc Natl Acad Sci U S A ; 118(30)2021 Jul 27.
Artigo em Inglês | MEDLINE | ID: mdl-34301905

RESUMO

We have used atomic layer-by-layer oxide molecular beam epitaxy to grow epitaxial thin films of [Formula: see text] with x up to 0.5, greatly exceeding the solubility limit of Ca in bulk systems ([Formula: see text]). A comparison of the optical conductivity measured by spectroscopic ellipsometry to prior predictions from dynamical mean-field theory demonstrates that the hole concentration p is approximately equal to x. We find superconductivity with [Formula: see text] of 15 to 20 K up to the highest doping levels and attribute the unusual stability of superconductivity in [Formula: see text] to the nearly identical radii of La and Ca ions, which minimizes the impact of structural disorder. We conclude that careful disorder management can greatly extend the "superconducting dome" in the phase diagram of the cuprates.

6.
ACS Nano ; 15(10): 16228-16235, 2021 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-34592093

RESUMO

Strain engineering of complex oxide heterostructures has provided routes to explore the influence of the local perturbations to the physical properties of the material. Due to the challenge of disentangling intrinsic and extrinsic effects at oxide interfaces, the combined effects of epitaxial strain and charge transfer mechanisms have been rarely studied. Here, we reveal the local charge distribution in manganite slabs by means of high-resolution electron microscopy and spectroscopy via investigating how the strain locally alters the electronic and magnetic properties of La0.5Sr0.5MnO3-La2CuO4 heterostructures. The charge rearrangement results in two different magnetic phases: an interfacial ferromagnetically reduced layer and an enhanced ferromagnetic metallic region away from the interfaces. Further, the magnitude of the charge redistribution can be controlled via epitaxial strain, which further influences the macroscopic physical properties in a way opposed to strain effects reported on single-phase films. Our work highlights the important role played by epitaxial strain in determining the spatial distribution of microscopic charge and spin interactions in manganites and provides a different perspective for engineering interface properties.

7.
Nat Commun ; 11(1): 1793, 2020 Apr 14.
Artigo em Inglês | MEDLINE | ID: mdl-32286291

RESUMO

In high-energy physics, the Higgs field couples to gauge bosons and fermions and gives mass to their elementary excitations. Experimentally, such couplings can be inferred from the decay product of the Higgs boson, i.e., the scalar (amplitude) excitation of the Higgs field. In superconductors, Cooper pairs bear a close analogy to the Higgs field. Interaction between the Cooper pairs and other degrees of freedom provides dissipation channels for the amplitude mode, which may reveal important information about the microscopic pairing mechanism. To this end, we investigate the Higgs (amplitude) mode of several cuprate thin films using phase-resolved terahertz third harmonic generation (THG). In addition to the heavily damped Higgs mode itself, we observe a universal jump in the phase of the driven Higgs oscillation as well as a non-vanishing THG above Tc. These findings indicate coupling of the Higgs mode to other collective modes and potentially a nonzero pairing amplitude above Tc.

8.
ACS Appl Mater Interfaces ; 10(26): 22786-22792, 2018 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-29927575

RESUMO

Transition metal oxides exhibit a high potential for application in the field of electronic devices, energy storage, and energy conversion. The ability of building these types of materials by atomic layer-by-layer techniques provides a possibility to design novel systems with favored functionalities. In this study, by means of the atomic layer-by-layer oxide molecular beam epitaxy technique, we designed oxide heterostructures consisting of tetragonal K2NiF4-type insulating La2CuO4 (LCO) and perovskite-type conductive metallic LaNiO3 (LNO) layers with different thicknesses to assess the heterostructure-thermoelectric property-relationship at high temperatures. We observed that the transport properties depend on the constituent layer thickness, interface intermixing, and oxygen-exchange dynamics in the LCO layers, which occurs at high temperatures. As the thickness of the individual layers was reduced, the electrical conductivity decreased and the sign of the Seebeck coefficient changed, revealing the contribution of the individual layers where possible interfacial contributions cannot be ruled out. High-resolution scanning transmission electron microscopy investigations showed that a substitutional solid solution of La2(CuNi)O4 was formed when the thickness of the constituent layers was decreased.

9.
Sci Rep ; 7(1): 453, 2017 03 28.
Artigo em Inglês | MEDLINE | ID: mdl-28352070

RESUMO

Among the range of complex interactions, especially at the interfaces of epitaxial oxide systems, contributing to the occurrence of intriguing effects, a predominant role is played by the local structural parameters. In this study, oxide molecular beam epitaxy grown lanthanum cuprate-based bilayers (consisting of a metallic (M) and an insulating phase (I)), in which high-temperature superconductivity arises as a consequence of interface effects, are considered. With the aim of assessing the role of the dopant size on local crystal structure and chemistry, and on the interface functionalities, different dopants (Ca2+, Sr2+ and, Ba2+) are employed in the M-phase, and the M-I bilayers are investigated by complementary techniques, including spherical-aberration-corrected scanning transmission electron microscopy. A series of exciting outcomes are found: (i) the average out-of-plane lattice parameter of the bilayers is linearly dependent on the dopant ion size, (ii) each dopant redistributes at the interface with a characteristic diffusion length, and (iii) the superconductivity properties are highly dependent on the dopant of choice. Hence, this study highlights the profound impact of the dopant size and related interface chemistry on the functionalities of superconducting oxide systems.

10.
Sci Rep ; 7: 40621, 2017 01 13.
Artigo em Inglês | MEDLINE | ID: mdl-28084444

RESUMO

The magneto-optical activity of high quality transparent thin films of insulating EuTiO3 (ETO) deposited on a thin SrTiO3 (STO) substrate, both being non-magnetic materials, are demonstrated to be a versatile tool for light modulation. The operating temperature is close to room temperature and allows for multiple device engineering. By using small magnetic fields birefringence of the samples can be switched off and on. Similarly, rotation of the sample in the field can modify its birefringence Δn. In addition, Δn can be increased by a factor of 4 in very modest fields with simultaneously enhancing the operating temperature by almost 100 K.

11.
ACS Appl Mater Interfaces ; 8(40): 27368-27375, 2016 Oct 12.
Artigo em Inglês | MEDLINE | ID: mdl-27648928

RESUMO

The exploration of interface effects in complex oxide heterostructures has led to the discovery of novel intriguing phenomena in recent years and has opened the path toward the precise tuning of material properties at the nanoscale. One recent example is space-charge superconductivity. Among the complex range of effects which may arise from phase interaction, a crucial role is played by cationic intermixing, which defines the final chemical composition of the interface. In this work, we performed a systematic study on the local cationic redistribution of two-dimensionally doped lanthanum cuprate films grown by oxide molecular beam epitaxy, in which single LaO layers in the epitaxial crystal structure were substituted by layers of differently sized and charged dopants (Ca, Sr, Ba, and Dy). In such a model system, in which the dopant undergoes an asymmetric redistribution across the interface, the evolution of the cationic concentration profile can be effectively tracked by means of atomically resolved imaging and spectroscopic methods. This allowed for the investigation of the impact of the dopant chemistry (ionic size and charge) and of the growth conditions (temperature) on the final superconducting and structural properties. A qualitative model for interface cationic intermixing, based on thermodynamic considerations, is proposed. This work highlights the key role which cationic redistribution may have in the definition of the final interface properties and represents a further step forward the realization of heterostructures with improved quality.

12.
ACS Appl Mater Interfaces ; 8(10): 6763-9, 2016 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-26909681

RESUMO

Using spherical aberration corrected high-resolution and analytical scanning transmission electron microscopy, we have quantitatively studied the lattice distortion and the redistribution of charges in two-dimensionally strontium (Sr)-doped La2CuO4 superlattices, in which single LaO planes are periodically replaced by SrO planes. As shown previously, such structures show Tc up to 35 K as a consequence of local charge accumulation on both sides of the nominal SrO planes position. This is caused by two distinct mechanisms of doping: heterogeneous doping at the downward side of the interface (space-charge effect) and "classical" homogeneous doping at the upward side. The comparative chemical and atomic-structural analyses reveal an interrelation between local CuO6 octahedron distortions, hole spatial distribution, and chemical composition. In particular we observe an anomalous expansion of the apical oxygen-oxygen distance in the heterogeneously doped (space-charge) region, and a substantial shrinkage of the apical oxygen-oxygen distance in the homogeneously doped region. Such findings are interpreted in terms of different Jahn-Teller effects occurring at the two interface sides (downward and upward).

13.
Adv Mater ; 26(38): 6554-9, 2014 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-25103570

RESUMO

The electronic phase behavior and functionality of interfaces and surfaces in complex materials are strongly correlated to chemical composition profiles, stoichiometry and intermixing. Here a novel analysis scheme for resonant X-ray reflectivity maps is introduced to determine such profiles, which is element specific and non-destructive, and which exhibits atomic-layer resolution and a probing depth of hundreds of nanometers.


Assuntos
Nanoestruturas/química , Análise Espectral , Fenômenos Ópticos , Raios X
14.
Beilstein J Nanotechnol ; 5: 596-602, 2014.
Artigo em Inglês | MEDLINE | ID: mdl-24995148

RESUMO

In this paper we present the atomic-layer-by-layer oxide molecular beam epitaxy (ALL-oxide MBE) which has been recently installed in the Max-Planck Institute for Solid State Research and we report on its present status, providing some examples that demonstrate its successful application in the synthesis of different layered oxides, with particular reference to superconducting La2CuO4 and insulator-to-metal La2- x Sr x NiO4. We briefly review the ALL-oxide MBE technique and its unique capabilities in the deposition of atomically smooth single-crystal thin films of various complex oxides, artificial compounds and heterostructures, introducing our goal of pursuing a deep investigation of such systems with particular emphasis on structural defects, with the aim of tailoring their functional properties by precise defects control.

15.
Adv Mater ; 26(2): 258-62, 2014 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-24155253

RESUMO

A combined synchrotron X-ray diffraction and transmission electron microscopy study reveals a structural phase transition controlled by the overall thickness of epitaxial nickelate-aluminate superlattices. The transition between uniform and twin-domain states is confined to the nickelate layers and leaves the aluminate layers unaffected.

16.
ACS Nano ; 6(10): 9175-81, 2012 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-23009148

RESUMO

Lately, fluorescence quenching microscopy (FQM) has been introduced as a new tool to visualize graphene-based sheets. Even though quenching of the emission from a dye molecule by fluorescence resonance energy transfer (FRET) to graphene happens on the nanometer scale, the resolution of FQM so far is still limited to several hundreds of nanometers due to the Abbe limit restricting the resolution of conventional light microscopy. In this work, we demonstrate an advancement of FQM by using a super-resolution imaging technique for detecting fluorescence of color centers used in FQM. The technique is similar to stimulated emission depletion microscopy (STED). The combined "FRET+STED" technique introduced here for the first time represents a substantial improvement to FQM since it exhibits in principle unlimited resolution while still using light in the visible spectral range. In the present case we demonstrate all-optical imaging of graphene with resolution below 30 nm. The performance of the technique in terms of imaging resolution and contrast is well described by a theoretical model taking into account the general distance dependence of the FRET process and the distance distribution of donor centers with respect to the flake. In addition, the change in lifetime for partially quenched emitters allows extracting the quenching distance from experimental data for the first time.


Assuntos
Grafite/análise , Grafite/química , Aumento da Imagem/métodos , Microscopia de Fluorescência/métodos , Nanoestruturas/química , Nanoestruturas/ultraestrutura , Tamanho da Partícula
17.
Nat Commun ; 2: 272, 2011.
Artigo em Inglês | MEDLINE | ID: mdl-21505428

RESUMO

The Meissner effect and associated perfect 'bulk' diamagnetism together with zero resistance and gap opening are characteristic features of the superconducting state. In the pseudogap state of cuprates, unusual diamagnetic signals and anomalous proximity effects have been detected, but a Meissner effect has never been observed. Here we probe the local diamagnetic response in the normal state of an underdoped La(1.94)Sr(0.06)CuO(4) layer (T(c)'≤5 K), which is brought into close contact with two nearly optimally doped La(1.84)Sr(0.16)CuO(4) layers (T(c)≈32 K). We show that the entire 'barrier' layer of thickness, much larger than the typical c axis coherence lengths of cuprates, exhibits a Meissner effect at temperatures above T(c)' but below T(c). The temperature dependence of the effective penetration depth and superfluid density in different layers indicates that superfluidity with long-range phase coherence is induced in the underdoped layer by the proximity to optimally doped layers, but this induced order is sensitive to thermal excitation.


Assuntos
Cobre/química , Campos Eletromagnéticos , Nanotecnologia/métodos , Temperatura , Lantânio/química , Modelos Químicos , Estrôncio/química
18.
Nat Nanotechnol ; 5(7): 516-9, 2010 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-20543834

RESUMO

Measurements on nanoscale structures constructed from high-temperature superconductors are expected to shed light on the origin of superconductivity in these materials. To date, loops made from these compounds have had sizes of the order of hundreds of nanometres(8-11). Here, we report the results of measurements on loops of La(1.84)Sr(0.16)CuO(4), a high-temperature superconductor that loses its resistance to electric currents when cooled below approximately 38 K, with dimensions down to tens of nanometres. We observe oscillations in the resistance of the loops as a function of the magnetic flux through the loops. The oscillations have a period of h/2e, and their amplitude is much larger than the amplitude of the resistance oscillations expected from the Little-Parks effect. Moreover, unlike Little-Parks oscillations, which are caused by periodic changes in the superconducting transition temperature, the oscillations we observe are caused by periodic changes in the interaction between thermally excited moving vortices and the oscillating persistent current induced in the loops. However, despite the enhanced amplitude of these oscillations, we have not detected oscillations with a period of h/e, as recently predicted for nanoscale loops of superconductors with d-wave symmetry, or with a period of h/4e, as predicted for superconductors that exhibit stripes.

19.
Proc Natl Acad Sci U S A ; 107(18): 8103-7, 2010 May 04.
Artigo em Inglês | MEDLINE | ID: mdl-20404212

RESUMO

We have introduced an improved x-ray phase-retrieval method with unprecedented speed of convergence and precision, and used it to determine with sub-Angstrom resolution the complete atomic structure of epitaxial La(2-x)Sr(x)CuO(4) ultrathin films. We focus on superconducting heterostructures built from constituent materials that are not superconducting in bulk samples. Single-phase metallic or superconducting films are also studied for comparison. The results show that this phase-retrieval diffraction method enables accurate measurement of structural modifications in near-surface layers, which may be critically important for elucidation of surface-sensitive experiments. Specifically we find that, while the copper-apical-oxygen distance remains approximately constant in single-phase films, it shows a dramatic increase from the metallic-insulating interface of the bilayer towards the surface by as much as 0.45 A. The apical-oxygen displacement is known to have a profound effect on the superconducting transition temperature.

20.
Phys Rev Lett ; 101(24): 247004, 2008 Dec 12.
Artigo em Inglês | MEDLINE | ID: mdl-19113657

RESUMO

We have measured quasiparticle tunneling across a junction perpendicular to the superconducting copper oxide planes. The tunneling spectra show peaks in the density of states. There are 11 minima in the second derivative d2I/dV2, where I is the current and V the voltage, suggesting multiple boson-quasiparticle interactions. These minima match precisely with the published Raman scattering data, leading us to conclude that the relevant bosons in superconducting La1.84Sr0.16CuO4 films are phonons.

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