RESUMEN
Crystalline solids are generally known as excellent heat conductors, amorphous materials or glasses as thermal insulators. It has thus come as a surprise that certain crystal structures defy this paradigm. A prominent example are type-I clathrates and other materials with guest-host structures. They sustain low-energy Einstein-like modes in their phonon spectra, but are also prone to various types of disorder and phonon-electron scattering and thus the mechanism responsible for their ultralow thermal conductivities has remained elusive. Our thermodynamic and transport measurements on various clathrate single crystal series and their comparison with ab initio simulations reveal an all phononic Kondo effect as origin. This insight devises design strategies to further suppress the thermal conductivity of clathrates and other related materials classes, with relevance for thermoelectric waste heat recovery and, more generally, phononic applications. It may also trigger theoretical work on strong correlation effects in phonon systems.
RESUMEN
Recent theoretical studies of topologically nontrivial electronic states in Kondo insulators have pointed to the importance of spin-orbit coupling (SOC) for stabilizing these states. However, systematic experimental studies that tune the SOC parameter λ_{SOC} in Kondo insulators remain elusive. The main reason is that variations of (chemical) pressure or doping strongly influence the Kondo coupling J_{K} and the chemical potential µ-both essential parameters determining the ground state of the material-and thus possible λ_{SOC} tuning effects have remained unnoticed. Here, we present the successful growth of the substitution series Ce_{3}Bi_{4}(Pt_{1-x}Pd_{x})_{3} (0≤x≤1) of the archetypal (noncentrosymmetric) Kondo insulator Ce_{3}Bi_{4}Pt_{3}. The Pt-Pd substitution is isostructural, isoelectronic, and isosize, and it therefore is likely to leave J_{K} and µ essentially unchanged. By contrast, the large mass difference between the 5d element Pt and the 4d element Pd leads to a large difference in λ_{SOC}, which thus is the dominating tuning parameter in the series. Surprisingly, with increasing x (decreasing λ_{SOC}), we observe a Kondo insulator to semimetal transition, demonstrating an unprecedented drastic influence of the SOC. The fully substituted end compound Ce_{3}Bi_{4}Pd_{3} shows thermodynamic signatures of a recently predicted Weyl-Kondo semimetal.
RESUMEN
The increasing worldwide energy consumption calls for the design of more efficient energy systems. Thermoelectrics could be used to convert waste heat back to useful electric energy if only more efficient materials were available. The ideal thermoelectric material combines high electrical conductivity and thermopower with low thermal conductivity. In this regard, the intermetallic type-I clathrates show promise with their exceedingly low lattice thermal conductivities. Here we report the successful incorporation of cerium as a guest atom into the clathrate crystal structure. In many simpler intermetallic compounds, this rare earth element is known to lead, through the Kondo interaction, to strong correlation phenomena including the occurrence of giant thermopowers at low temperatures. Indeed, we observe a 50% enhancement of the thermopower compared with a rare-earth-free reference material. Importantly, this enhancement occurs at high temperatures and we suggest that a rattling-enhanced Kondo interaction underlies this effect.
RESUMEN
In surface-roughened metallic implant materials, the topography, chemistry and energy of the surfaces play an important role for the cell and tissue attachment. The highly reactive commercially pure metals niobium, tantalum and titanium were analysed after microblasting (with Al2O3 powder and consecutive shot-peening with ZrSiO2), and after additional reactive ion etching (RIE, with CF4). Scanning electron microscopy in combination with energy-dispersive X-ray analysis and surface roughness measurements showed, for all microblasted surfaces, a heterogeneous roughening (Ra about 0.7 microm), and a contamination with blasting particles. RIE resulted in a further roughening (Ra about 1.1 microm), and a total cleaning from contaminations, except for traces of aluminium. Determination of surface energy by dynamic contact angle measurements showed an increase in surface energy after microblasting, which further increased after RIE, most pronounced for commercially pure niobium. In conjunction with superior electrochemical properties, this makes niobium and tantalum promising candidates for implant purposes, at least equal to the generally used titanium.
RESUMEN
When the surface of a solid sample is irradiated under vacuum by x-rays an electron emission, owing to photoabsorption, can be measured. As the electrons are detected under neglection of their kinetic energies the total electron yield (TEY) is determined. With a tuneable x-ray monochromator the TEY is measured below and above of one of the absorption edges of a given element. A jumplike increase of the TEY signal, due to the additional photoabsorptions in the corresponding atomic level, can be observed - qualitative analysis. The height of this jump can be correlateted to the concentration - quantitative analysis. It can be shown by a fundamental parameter approach for primary and secondary excitations how to use TEY for a quantitative analysis. The information depth lambda of this new method is approximately 2-400 nm depending on the chemical elements and on the original kinetic energies of Auger and photoelectrons. Thus, TEY is located between photoelectron spectrometry and x-ray fluorescence analysis.
RESUMEN
A method of nondestructive depth profiling in near surface regions of solids is described. Models have been discussed from which algorithms for evaluation of measured data are obtained. The algorithms, based on standard profiles with free parameters, have been adjusted to the data resulting from angle resolved XPS (ARXPS) by means of least squares fits. Depth profile analyses and segregation studies were performed on Pt-Ni and Fe-S specimens.