Intense terahertz radiation via the transverse thermoelectric effect

Terahertz (THz) radiation is a powerful tool with widespread applications ranging from imaging, sensing, and broadband communications to spectroscopy and nonlinear control of materials. Future progress in THz technology depends on the development of efficient, structurally simple THz emitters that can be implemented in advanced miniaturized devices. Here we show how the natural electronic anisotropy of layered conducting transition metal oxides enables the generation of intense terahertz radiation via the transverse thermoelectric effect. In thin films grown on offcut substrates, femtosecond laser pulses generate ultrafast out-of-plane temperature gradients, which in turn launch in-plane thermoelectric currents, thus allowing efficient emission of the resulting THz field out of the film structure. We demonstrate this scheme in experiments on thin films of the layered metals PdCoO2 and La1.84Sr0.16CuO4, and present model calculations that elucidate the influence of the material parameters on the intensity and spectral characteristics of the emitted THz field. Due to its simplicity, the method opens up a promising avenue for the development of highly versatile THz sources and integrable emitter elements.Comment: 27 pages, 11 figure

Orbital reflectometry

The occupation of d-orbitals controls the magnitude and anisotropy of the inter-atomic electron transfer in transition metal oxides and hence exerts a key influence on their chemical bonding and physical properties. Atomic-scale modulations of the orbital occupation at surfaces and interfaces are believed to be responsible for massive variations of the magnetic and transport properties, but could thus far not be probed in a quantitative manner. Here we show that it is possible to derive quantitative, spatially resolved orbital polarization profiles from soft x-ray reflectivity data, without resorting to model calculations. We demonstrate that the method is sensitive enough to resolve differences of 3 % in the occupation of Ni e_g orbitals in adjacent atomic layers of a LaNiO3-LaAlO3 superlattice, in good agreement with ab-initio electronic-structure calculations. The possibility to quantitatively correlate theory and experiment on the atomic scale opens up many new perspectives for orbital physics in d-electron materials

Transient increase of Tc and Jc in superconducting/metallic heterostructures

The presence of a metallic layer can influence the properties of high-temperature superconductors underneath. We investigate the influence of metallic structures deposited in form of nanoparticles or continuous layers by electron beam evaporation or ion beam sputtering on the properties of Y1Ba2Cu3O7-x (YBCO) thin films. To generally avoid diffusion of metal atoms an additional barrier layer is introduced. Detailed measurements of the magnetic moment of the superconductor as a function of temperature and magnetic field have been performed using SQUID magnetometry. It is found that the modification of the superconducting properties of coated YBCO strongly depends on the deposition method of the metal on top rather than the type of metal (Ni or Ag), its magnetic properties (ferromagnetic or paramagnetic) or its morphology (nanoparticles or thin film). The main result is a transient increase of the critical temperature Tc and critical current density Jc that was observed for samples prepared by electron beam evaporation

Atomic-Scale Quantitative Analysis of Lattice Distortions at Interfaces of Two-Dimensionally Sr-Doped La₂CuO₄ Superlattices

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 <i>T</i>_c 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)

Cationic Redistribution at Epitaxial Interfaces in Superconducting Two-Dimensionally Doped Lanthanum Cuprate Films

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

High-Temperature Thermoelectricity in LaNiO₃–La₂CuO₄ Heterostructures

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