With charge-based electronics getting to their limits in storage density, speed and energy consumption, spin-based electronics (spintronics) is now a central research topic and promises significant improvements in device performances. Controlling spins with an electric field is a major goal in spintronics since it is an industry-compatible, low-energy-consumption degree-of-freedom to act on an elusive, fundamental property of matter. Taking advantage of the predicted giant Rashba effect at their interfaces, transition metal dichalcogenides (TMDCs) monolayers gated by a ferroelectric oxide layer can achieve this goal. By combining advanced angle- and spin- resolved photoemission spectroscopy, the CORNFLAKE project aims at a thorough characterization of the spin-split bands of TMDCs deposited on ferroelectric ultrathin films via molecular beam epitaxy. This project will give quantitative values for the band energy and momentum spin-splitting as a function of the ferroelectric polarization magnitude and direction. The ultimate goal of the project is to provide a ferroelectric polarization dependent measure of the 3D spin-texture of the TMDCs. Such knowledge is necessary for a better understanding of gated TMDCs and their potential use in realistic spin devices. Also, by focusing on strong spin-orbit-coupled materials and hybrid interfaces, this project falls within the more general field of Quantum Materials, a fascinating venue to uncover the roles of symmetry, topology, dimensionality and strong correlations in macroscopic observables.

The research objective of the project SPECTROSCOPE is the in operando X-ray Absorption Spectroscopy (XAS) study of novel non-precious metal electrocatalysts in low temperature polymer-electrolyte-membrane fuel cells (PEMFC) and electrolyzers (PEMEL), also involving the development of a synchrotron platform for such cells. The investigated materials will be metal-nitrogen-carbon and metal-chalcogenide catalysts for oxygen reduction and hydrogen evolution, respectively. A combined experimental-theoretical approach by employing operando X-ray absorption synchrotron techniques (XANES, EXAFS) with advanced ab initio modelling tools will provide unprecedented structural and electronic information on the nature, number and modifications of active sites during oxygen reduction and hydrogen evolution under operation in PEMFC and PEMEL, respectively. Novel structural and mechanistic insights governing the activity and, even more critical, the degradation of such materials will be acquired for the first time under operating conditions and in the environment of PEM-based cells, characterized with a polymer electrolyte, moving the field beyond liquid-electrolyte XAS studies performed hitherto. This will allow us establishing novel understanding and guidelines for durable PEM cells catalyzed by non-precious metal electrocatalysts in the near future.

Carbon dioxide (CO2) is a major exhaust product of transportation and industrial processes in industrial societies. The deleterious effect of this gas on our environment is becoming a serious concern, but our societies remain dependent on fossil fuels as one of their main energy source. The transformation of this by-product into added-value chemicals or energy-rich fuels is a highly interesting valorization route, both from environmental and industrial perspectives. In this context, the electrochemical reduction of CO2 is an interesting approach, which allows synthesizing simple molecules such as methanol or formaldehyde or more complex ones such as butanol. These chemicals can be used either as building blocks for commodity chemicals or directly as fuels. Although a lot of research has been done in the last years to improve them, catalytic CO2 reduction reactions suffer from one of the two following problems: i) Low selectivity: metallic copper, for example, has been largely studied for its ability to reduce CO2 electrochemically in aqueous media. This catalyst is appreciated for the variety of compounds it can produce: CO, CH4, C2H4, HCOOH. Despite the progresses made over the last years to improve its selectivity, it is not satisfactory yet, with 4 to 5 major products (representing at least 10% each of the total products) and no simple way of separating them. ii) The formation of low added value products: several molecular catalysts (rhenium bipyridine/CO or manganese bipyridine/CO complexes, iron porphyrins) are efficient for the electrochemical or photochemical reduction of CO2, but their only product is carbon monoxide, which added value or energetic potential is quite low. To circumvent these issues, we propose to develop microfluidic systems that will feature successive electrocatalytic reactors in order to perform CO2 reduction reactions sequentially. Our bet is that a series of well-controlled cascade reactions is more efficient and easier to handle than trying to optimize a single catalyst for the synthesis of added-value hydrocarbons all at once. These systems will allow optimizing independent catalysts for a given reaction involving CO2 or its reduction products. Once the catalytic conditions of each single microreactor will be optimized, they will be incorporated in complex, multi-step reaction schemes. The use of microfluidic systems will allow controlling the availability of substrate independently for each catalyst and also offer parallelization possibilities, which can speed up the optimization of catalytic conditions. Because of its industrial significance and its synthetic versatility (in particular the presence of and electrophilic carbon), our main target is formaldehyde. This synthetic building block will be obtained by the electrochemical reduction of CO2 into CO in aqueous medium and the subsequent electrocatalytic reduction of CO into formaldehyde in acidic medium. We will use well known and commercially available catalysts for each of these steps, which will be set in the microreactors developed in the course of the project. Specific microfluidic tools will also be developed for the detection of reaction products and parameters optimization. This project proposes to demonstrate the feasibility of sequential multi-step electrosynthetic reactions applied to the reduction of CO2. Its completion will showcase the benefits of microfluidic in electrosynthetic reactions by the control it allows on the availability and circulation of reactants and products. The knowledge and the microfluidic electrosynthetic devices developed along this project will be applied to other reactions involving CO2 and will benefit the entire community interested in such reactions.

We propose to trace back the origin of biomolecular asymmetry to interstellar asymmetric processes. Therefore, we concretely envisage the measurement of circular dichroism spectra of amino acids in the solid state applying circularly polarized radiation at the ISA (Århus) and enantioselective photolysis of these samples at the SOLEIL (Gif-sur-Yvette) synchrotron centers. For ultra-modern analytical resolution of enantiomers in the above samples an enantioselective GCxGC system is required.