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Arnaud Badel

Publications and source records attributed to Arnaud Badel.

5 recordsLinked to original sources

Bias-triggered conductivity relaxation (BCR): a unique tool to simultaneously investigate thermodynamics, kinetics and electrostatic effects of oxygen reactions in MIEC thin films

Mixed ionic electronic transfer (MIET) reactions, such as the oxygen reduction reaction (ORR) at oxide surfaces, are of paramount importance to manifold technologically highly relevant processes and fundamental understanding must be developed to improve performance and tailor highly efficient electrodes and catalysts. Understanding such complex multi-step reactions, requires the study of kinetic processes, underlying thermodynamic properties, i.e. ionic and electronic defect concentrations and electrostatic surface effects. However conventional techniques struggle to uncover the complete picture within the same sample/measurement. Here, we overcome this limitation by introducing bias-triggered conductivity relaxation (BCR) as a novel tool to investigate MIET reactions on oxides. It is based on alternating out-of-plane coulometric titration/polarization and in-plane electrical conductivity relaxation measurements, providing simultaneous electronic, ionic and extraordinarily rich surface kinetics information. This innovative combination of electrical and chemical driving forces synergizes information depth, with enhanced time resolution, versatility and speed, yet it lifts the weaknesses of the individual approaches, while remaining cost-effective and surprisingly simple. Furthermore, BCR allows to disentangle overpotential induced electrostatic modifications of the surface kinetics in a unique manner. We showcase the advantages of BCR in this work by studying the ORR in model (La,Sr)FeO$_{3-{\delta}}$ thin film electrodes and reporting on their thermodynamic and kinetic properties.

cond-mat.mtrl-sci

Fast track to the overdoped regime of superconducting YBa2Cu3O7-{\delta} thin films via electrochemical oxidation

High temperature superconductors, especially YBa$_2$Cu$_3$O$_{7-\delta}$ (YBCO), are considered a key enabling technology towards a clean energy future. Hole doping in YBCO is a prerequisite for the emergence of its unchallenged superconducting properties. Up to now, research was focused on the under- and optimally doped region, due to practical limitations in reaching the overdoped state, despite being highly interesting from fundamental and applied aspects as competing orders vanish and critical current densities are expected to peak. Here, we deploy for the first time an electrochemical method to access the mostly uncharted overdoped region. We demonstrate precise control over the bulk oxygen concentration in YBCO thin films across the full off-stoichiometry window (0$\le{\delta}\le$1) using electrochemical oxidation combined with in situ XRD and electrical measurements. Resulting high doping states and critical current densities are confirmed using a multi modal approach, including x-ray diffraction, electrical, Hall and magnetic characterization. Thus, this work opens a promising pathway based on electrochemical oxidation towards electronically clean, oxygen overdoped cuprate superconductors and therefore will assist to further push the critical current density to its intrinsic limit.

cond-mat.supr-con

Investigating oxides by electrochemical projection of the oxygen off-stoichiometry diagram onto a single sample

The oxygen stoichiometry is an essential key to tune functional properties of advanced oxide materials and thus has motivated numerous studies of the oxygen off-stoichiometry diagram, with the aim to determine and control structural, electronic, ionic, electrochemical and optical properties, as well as thermodynamic quantities such as the oxygen storage capacity, among others. Here, a novel approach is developed, which allows to project a broad range of oxygen chemical potentials onto a single thin film sample with unprecedented control via electrochemical polarization. Therefore, a specifically designed electrochemical cell geometry is deployed, resulting in a well-defined, linear, 1D in-plane oxygen concentration gradient, independent of variations in the materials electrical resistivity, whose endpoints can be flexibly controlled via the external pO2 and applied overpotential. This allows for an unparalleled study of materials properties as a continuous function of the oxygen content using spatially resolved tools (spectroscopic, diffraction, microscopy, local electrical probes, etc.) and thereby greatly reduces experimental efforts while also avoiding sample-to-sample variability, multi-step treatments, sample evolution effects, etc. This work presents the proof-of-concept of in-plane oxygen gradients, based on spatially resolved ex/in situ and novel fixed-energy X-ray absorption near edge spectroscopy (XANES), X-ray diffraction, ellipsometry and electrical resistivity measurements in hyper-stoichiometric La2NiO4+δ and sub-stoichiometric (La,Sr)FeO3-δ thin films. It thereby demonstrates the readiness and wide applicability of this innovative approach, which can be highly relevant for fundamental as well as applied research.

cond-mat.mtrl-sci

Oxygen incorporation in YBa$_2$Cu$_3$O$_{7-δ}$ thin films: surface activation and degradation

The oxygen off-stoichiometry plays a pivotal role for the physical properties of superconducting oxides. Yet, there is a lack of knowledge on the fundamental processes of oxygen incorporation and correlated phenomena during oxygen post annealing treatments. Here, we deployed electrical probes ($ρ(T)$ and electrical conductivity relaxation (ECR) measurements) to gain a better understanding of the kinetics of the oxygen reduction reaction (ORR) in epitaxial YBa$_2$Cu$_3$O$_{7-δ}$ (YBCO) thin films. We identified a new indicator for the onset temperature of oxygen incorporation and report for the first time drastic kinetic deactivation in bare YBCO. We demonstrate that surface decoration using silver micro islands both catalytically activates oxygen incorporation and bypasses surface degradation processes. Our results suggest that the ORR in the studied YBCO samples is limited by a surface reaction. Additionally, weak XRD signatures of the formation of extended bulk defects were identified, which have to be considered in the designing of an optimal oxygenation treatment to obtain best performing superconducting YBCO.

cond-mat.supr-con

First tests of a 800 kJ HTS SMES

SMES using high critical temperature superconductors are interesting for high power pulsed sources. Operation at temperatures above 20 K makes cryogenics easier, enhances stability and improves operation as pulsed power source. In the context of a DGA (Delegation Generate pour l'Armement) project, we have designed and constructed a 800 kJ SMES. The coil is wound with Nexans conductors made of Bi-2212 PIT tapes soldered in parallel. The coil consists in 26 superposed simple pancakes wound and bonded on sliced copper plates coated with epoxy. The rated current is 315 A for an energy of 814 kJ. The external diameter of the coil is 814 mm and its height 222 mm. The cooling at 20 K is only performed by conduction from cryocoolers to make cryogenics very friendly and invisible for the SMES users. The cooling down has been successfully carried out and the thermal system works as designed. After a brief description of the SMES design and construction, some tests will be presented. From a current of 244 A, the SMES delivered 425 kJ to a resistance with a maximum power of 175 kW.

physics.ins-det