Search

We present the first test of the implementation of a characterization method whose aim is to study the interfaces of magnetic and periodic hetero-structures. The methodology relies on the combination of two techniques, generation of x-ray standing waves and dichroism in x-ray emission. The first one gives the depth selectivity since the maximum of the electric field can be put in specific locations of the stack, the centre of layers or their interfaces, while the second one enables being sensitive to the magnetic character of the atoms present within the stack. To concentrate on the methodology, the well-studied Mg/Co multilayer is analysed by using incident photon of monochromatic energies across the Co L2,3 absorption edge and measuring the intensity of the Co Lαβ emission. Despite large dispersive effects preventing the maxima of the electric field to reach the interfaces of the stack, it has been possible to observe the dichroic signal in the angular distribution of the Co emission intensity, i.e. in the so-called x-ray standing wave curve.

International audience; A method for the reciprocal space treatment of high-resolution transmission electron microscopy (HR-TEM) and high-resolution scanning transmission electron microscopy (HR-STEM) images has been developed. Named “Absolute strain” (AbStrain), it allows for quantification and mapping of interplanar distances and angles, displacement fields and strain tensor components with reference to a user-defined Bravais lattice and with their corrections from the image distortions specific to HR-TEM and HR-STEM imaging. We provide the corresponding mathematical formalism. AbStrain goes beyond the restriction of the existing method known as geometric phase analysis by enabling direct analysis of the area of interest without the need for reference lattice fringes of a similar crystal structure on the same field of view. In addition, for the case of a crystal composed of two or more types of atoms, each with its own sub-structure constraint, we developed a method named “Relative displacement” for extracting sub-lattice fringes associated to one type of atom and measuring atomic columns displacements associated to each sub-structure with reference to a Bravais lattice or to another sub-structure. The successful application of AbStrain and Relative displacement to HR-STEM images of functional oxide ferroelectric heterostructures is demonstrated.

11th Region Workshop of the European-Microbeam-Analysis-Society (EMAS), Leoben, AUSTRIA, SEP 21-24, 2014; International audience; This work presents a series of three-dimensional computational methods with the objective of analyzing and quantifying some important structural characteristics in a collection of low-density polyolefin-based foams. First, the solid phase tortuosity, local thickness, and surface curvature, have been determined over the solid phase of the foam. These parameters were used to quantify the presence of wrinkles located at the cell walls of the foams under study. In addition, a novel segmentation technique has been applied to the continuous solid phase. This novel method allows performing a separate analysis of the constituting elements of this phase, that is, cell struts and cell walls. The methodology is based on a solid classification algorithm and evaluates the local topological dissimilarities existing between these elements. Thanks to this method it was possible to perform a separate analysis of curvature, local thickness, and corrugation ratio in the solid constituents that reveals additional differences that were not detected in the first analysis of the continuous structure. The methods developed in this work are applicable to other types of porous materials in fields such as geoscience or biomedicine.

The determination of depth profiles across interfaces is of primary importance in many scientific and technological areas. Photoemission spectroscopy is in principle well suited for this purpose, yet a quantitative implementation for investigations of liquid-vapor interfaces is hindered by the lack of understanding of electron-scattering processes in liquids. Previous studies have shown, however, that core-level photoelectron angular distributions (PADs) are altered by depth-dependent elastic electron scattering and can, thus, reveal information on the depth distribution of species across the interface. Here, we explore this concept further and show that the anisotropy parameter characterizing the PAD scales linearly with the average distance of atoms along the surface normal. This behavior can be accounted for in the low-collision-number regime. We also show that results for different atomic species can be compared on the same length scale. We demonstrate that atoms separated by about 1~\AA~along the surface normal can be clearly distinguished with this method, achieving excellent depth resolution., Comment: Submitted to Phys. Rev. Lett

International audience; Solvated electrons are among the most reductive species in an aqueous environment. Diamond materials have been proposed as a promising source of solvated electrons, but the underlying emission process in water remains elusive so far. Here, we show spectroscopic evidence for the emission of solvated electrons from detonation nanodiamonds upon excitation with both deep ultraviolet (225 nm) and visible (400 nm) light using ultrafast transient absorption. The crucial role of surface termination in the emission process is evidenced by comparing hydrogenated, hydroxylated and carboxylated nanodiamonds. In particular, a transient response that we attribute to solvated electrons is observed on hydrogenated nanodiamonds upon visible light excitation, while it shows a sub-ps recombination due to trap states when excited with deep ultraviolet light. The essential role of surface reconstructions on the nanodiamonds in these processes is proposed based on density functional theory calculations. These results open new perspectives for solar-driven emission of solvated electrons in an aqueous phase using nanodiamonds.

The creation, transfer, and stabilization of localized excitations are studied in a donor-acceptor Frenkel exciton model in an atomistic treatment of reduced-size double quantum dots (QDs) of various sizes. The explicit time-dependent dynamics simulations carried out by hybrid time-dependent density functional theory/configuration interaction show that laser-controlled hole trapping in stacked, coupled germanium/silicon quantum dots can be achieved by a UV/IR pump-dump pulse sequence. The first UV excitation creates an exciton localized on the topmost QD and after some coherent transfer time, an IR pulse dumps and localizes an exciton in the bottom QD. While hole trapping is observed in each excitation step, we show that the stability of the localized electron depends on its multiexcitonic character. We present how size and geometry variations of three Ge/Si nanocrystals influence transfer times and thus the efficiency of laser-driven populations of the electron-hole pair states.

International audience; Functional nanostructures can exhibit tunable physical properties and hold great promise for future application in nanoelectronics. These properties are largely governed by their size, surface, and geometry; hence accurate and damage-free fabrication techniques are key to reliable device functionalities. In contrast to other nanofabrication methods, focused ion beam (FIB) milling has proven to be a powerful machining method, offering the advantage of precision, rapid prototyping, and an operational capability on many materials. Light ion sources with helium (He) and neon(Ne) yield low ablation rates and less milling damage near the surface. A low surface damage is of particular interest for the fabrication of ferroelectric nanostructures, in which polarization patterns are largely governed by the boundary conditions.Here, we investigate Ne ion milling (NIM) of BaTiO3 single crystals and epitaxial thin films on Si substrate. A Zeiss Orion NanoFab microscope was used. BaTiO3 nanopillars and nanodisks of ~sub-500 nm dimensions were fabricated. The pillars were characterized by Raman spectroscopy, transmission electron microscopy (TEM) and scanning electron microscopy (SEM). Different processing conditions were investigated for neon ion milling on (001) BaTiO3 single crystals. We will first examine the effect of ion beam energy (in the range 15-30 keV) and fluence on the sputter rate and on the damaged depth in BaTiO3. Then, we will discuss the evolution of the pillar geometry and damage of the single crystalline structure with different milling conditions based on the Raman, TEM and SEM analyses. The effects of the milling sequence (in-out, out-in or alternating), beam spacing, beam dwell time and number of repetitions were investigated. Finally, we will consider the case of BaTiO3 nanopillars fabricated in BaTiO3 epitaxial thin films (20 nm)on SrTiO3-buffered silicon with different aspect ratios

We have studied the laser induced ultrafast quenching of Gd 4f magnetic order in ferrimagnetic Co100-xGdx alloys to highlight the role of the inter-atomic exchange coupling. We have taken advantage of the ultrashort soft X-ray pulses deliver by the femtoslicing beamline at the BESSY II synchrotron radiation source at the Helmholtz-Zentrum Berlin to perform element- and time-resolved X-ray Magnetic Circular Dichroism spectroscopy.Our results show that the laser induced quenching of Gd 4f magnetic order occurs on very different time-scales for the Co72Gd28, the Co77Gd23 and the Co79Gd21 alloys. Most of the magnetic moment losses occur within the first picosecond (ps) while the electron distribution is strongly out of equilibrium. After the equilibration of the electrons and lattice temperatures (t > 1 ps), the magnetic losses occur on slower rates that depend on the alloy composition: increasing the Co composition speeds up the demagnetization of Gd 4f sublattice. The strength of the inter-atomic exchange coupling which depends on composition, determines the efficiency of the angular momentum flow from the Gd 4f spin towards the lattice. Our results are in qualitative agreements with the predictions of the microscopic three temperatures model for ferrimagnetic alloys., 8 pages, 6 figures

International audience; In Cu(In,Ga)Se 2 (CIGS) thin-film solar cells, laterally inhomogeneous distributions of point defects may induce electrostatic potential fluctuations and thus reduce the open-circuit voltage (V oc). In the present work, we investigate possible origins of fluctuating potentials and estimate the amplitude of fluctuations and V oc losses in solar cells with various [Ga] in the CIGS absorber, with different buffer layers and with different durations of an RbF postdeposition treatment (PDT). Electron-beam-induced current measurements were employed to study the local difference in the width of the space-charge region (w SCR). It is shown that the amplitude of fluctuations in the w SCR depends significantly on the choice of buffer system and on the duration of the RbF PDT. In addition, energy-dispersive X-ray spectroscopy and cat-hodoluminescence measurements reveal that band-gap fluctuations do not have substantial impact on the device performance. Finally, some of the investigated cells were exposed to light soaking, which was found to be a means to reduce the detected electrostatic potential fluctuations and also to increase the effective electron diffusion length in the CIGS absorber for a part of the investigated cells.

Current state-of-the-art Cu2ZnSn(S,Se)(4) kesterite solar cells are limited by low open-circuit voltages (V-OC). In order to evaluate to what extent the substitution of Sn by Ge is able to result in higher V oc values, this article focuses on Cu2ZnGeSe4 "CZGSe" devices. To reveal their full potential, different strategies are explored that, in particular, aim at the optimization of the CZGSe/buffer heterojunction. Here, employing hard X-ray photoelectron spectroscopy, it is evidenced that only a combination of different surface treatments is able to remove all detrimental secondary phases. Further improvements are achieved by establishing a solar cell heat treatment in air. A systematic study of the impact of different annealing temperatures and durations determines the best heat treatment parameters to be 60 min at 200 degrees C. Also, Zn(O,S,OH) as a more transparent alternative to the heavy-metal compound CdS buffer layer has been realized. Combining all of the strategies, solar cells with 8.5 and 7.5% total area efficiency have been prepared, which is a record for Sn-free kesterite solar cells and any kesterite solar cell with a Zn(O,S,OH) buffer, respectively. Beyond these records, this work clearly confirms the emerging trend that Ge-for-Sn substitution is a successful strategy to improve the V-OC of kesterite solar cells. This project has received funding from the European Union's Horizon 2020 Research and Innovation Program under grant agreement no. 640868. Choubrac, L (corresponding author), Univ Nantes, UMR6502, CNRS, Inst Mat Jean Rouxel IMN, F-44300 Nantes, France; Helmholtz Zentrum Berlin Mat & Energie GmbH, Dept Struct & Dynam Energy Mat, D-14109 Berlin, Germany. leo.choubrac@helmholtz-berlin.de

Epitaxial strain is a useful handle to engineer the physical properties of perovskite oxide materials. Here, we apply it to orthorhombic chromites that are a family of antiferromagnets showing fruitful functionalities as well as strong spin–lattice coupling via antisymmetric exchange interaction along Cr–O–Cr bonds. Using pulsed laser deposition, we grow YCrO3 thin films on various substrates imposing strain levels in the range from −1.8% to +0.3%. The films are stoichiometric with a 3+ valence for Cr both within the films and at their surface. They display an antiferromagnetic spin order below their Néel temperature, which we show can be strongly tuned by epitaxial strain with a slope of −8.54 K/%. A dimensionless figure of merit (defined as the slope normalized by the Néel temperature of bulk) is determined to be 6.1, which is larger than that of other perovskites, such as manganites (5.5), ferrites (2.3), or nickelates (4.6). Density functional theory simulations bring insight into the role of Cr–O bond lengths and oxygen octahedral rotations on the observed behavior. Our results shed light on orthorhombic chromites that may offer an energy-efficient piezo-spintronic operation.

Quantum error mitigation has been proposed as a means to combat unwanted and unavoidable errors in near-term quantum computing using no or few additional quantum resources, in contrast to fault-tolerant schemes that come along with heavy overheads. Error mitigation has been successfully applied to reduce noise in near-term applications. In this work, however, we identify strong limitations to the degree to which quantum noise can be effectively `undone' for larger system sizes. We set up a framework that rigorously captures large classes of error mitigation schemes in use today. The core of our argument combines fundamental limits of statistical inference with a construction of families of random circuits that are highly sensitive to noise. We show that even at poly log log n depth, a super-polynomial number of samples is needed in the worst case to estimate the expectation values of noiseless observables, the principal task of error mitigation. Notably, our construction implies that scrambling due to noise can kick in at exponentially smaller depths than previously thought. They also impact other near-term applications, constraining kernel estimation in quantum machine learning, causing an earlier emergence of noise-induced barren plateaus in variational quantum algorithms and ruling out exponential quantum speed-ups in estimating expectation values in the presence of noise or preparing the ground state of a Hamiltonian., Comment: 37 pages, 4 figures, substantially rewritten and edited

International audience; Here we introduce a versatile stereolithographic route to produce three different kinds of Si-containing thermosets that yield high performance ceramics upon thermal treatment. Our approach is based on a fast and inexpensive thiol-ene free radical addition that can be applied for different classes of preceramic polymers with carbon-carbon double bonds. Due to the rapidity and efficiency of the thiol-ene click reactions, this additive manufacturing process can be effectively carried out using conventional light sources on benchtop printers. Through light initiated cross-linking, the liquid preceramic polymers transform into stable infusible thermosets that preserve their shape during the polymer-to-ceramic transformation. Through pyrolysis the thermosets transform into glassy ceramics with uniform shrinkage and high density. The obtained ceramic structures are nearly fully dense, have smooth surfaces, and are free from macroscopic voids and defects. A fabricated SiOC honeycomb was shown to exhibit a significantly higher compressive strength to weight ratio in comparison to other porous ceramics.

International audience; Since many decades nickel yttria-stabilized zirconia cermet (Ni/YSZ) has been the most frequently used fuel electrode material for high temperature solid oxide cells (SOCs). However, in recent years there has been considerable effort to improve the Ni/YSZ performance through surface engineering. In this work, we report a simple strategy to apply nanosized un-doped (CeOx) and Ni-doped (NiCeOy) ceria particles into porous Ni/YSZ cermet electrodes via infiltration from hexane solution. Detailed characterization of the particles in their solution revealed differences in the ease of agglomeration, with NiCeOy nanoparticles being better dispersed and thus forming smaller aggregates. This property is critical for the effectiveness of the solution in filling the pores of Ni/YSZ cermet and the consequent ceria deposition. In particular, morphological and microstructural characterization reveals that NiCeOy nanoparticles decorate uniformly the pores of Ni/YSZ backbone, deep up to the interface with the electrolyte. More importantly, this can be done with relatively high ceria loading per infiltration/co-firing step. Electrochemical tests demonstrate that infiltrated Ni/YSZ fuel electrodes have improved I-V performance in CO2 electrolysis as compared to pristine Ni/YSZ. Synchrotron-based operando NAP-XPS experiments using both soft and tender X-rays revealed the formation of an ultrathin Ni-Ce3+ layer on the electrode surface, which can rationalize the ameliorated CO2 electrolysis performance.

International audience; We report an element-and time-resolved investigation of femtosecond laser induced ultrafast dynamics of the Co 3d and Dy 4f spins in a ferrimagnetic Co80Dy20 alloy as a function of the temperature. We observe that the Co characteristic demagnetization time (τCo) remains nearly constant (~0.2 ps) on increasing the temperature. Conversely, the Dy characteristic demagnetization time (τDy) decreases from ~1 ps to ~0.4 ps with the rise of temperature. Comparing our experimental data with literature shows that τCo and τDy are independent of the alloy composition or the demagnetization amplitude and that τDy scales with the relative temperature T* = TCurie-T.

Structural dynamics 8(3), 034305 (1-9) (2021). doi:10.1063/4.0000109, During the last two decades, a variety of models have been developed to explain the ultrafast quenching of magnetization following femtosecond optical excitation. These models can be classified into two broad categories, relying either on a local or a non-local transfer of angular momentum. The acquisition of the magnetic depth profiles with femtosecond resolution, using time-resolved x-ray resonant magnetic reflectivity, can distinguish local and non-local effects. Here, we demonstrate the feasibility of this technique in a pump–probe geometry using a custom-built reflectometer at the FLASH2 free-electron laser (FEL). Although FLASH2 is limited to the production of photons with a fundamental wavelength of 4 nm (≃310 eV), we were able to probe close to the Fe $L_3$ edge (706.8 eV) of a magnetic thin film employing the third harmonic of the FEL. Our approach allows us to extract structural and magnetic asymmetry signals revealing two dynamics on different time scales which underpin a non-homogeneous loss of magnetization and a significant dilation of 2 Å of the layer thickness followed by oscillations. Future analysis of the data will pave the way to a full quantitative description of the transient magnetic depth profile combining femtosecond with nanometer resolution, which will provide further insight into the microscopic mechanisms underlying ultrafast demagnetization, Published by AIP Publishing LLC, Melville, NY

The metallic and semiconducting character of a large family of organic materials based on the electron donor molecule tetrathiafulvalene (TTF) is rooted in the partial oxidation (charge transfer or mixed valency) of TTF derivatives leading to partially filled molecular orbital-based electronic bands. The intrinsic structure of such complexes, with segregated donor and acceptor molecular chains or planes, leads to anisotropic electronic properties (quasi one-dimensional or two-dimensional) and morphology (needle-like or platelet-like crystals). Recently, such materials have been synthesized as nanoparticles by intentionally frustrating the intrinsic anisotropic growth. X-ray photoemission spectroscopy (XPS) has emerged as a valuable technique to characterize the transfer of charge due to its ability to discriminate the different chemical environments or electronic configurations manifested by chemical shifts of core level lines in high-resolution spectra. Since the photoemission process is inherently fast (well below the femtosecond time scale), dynamic processes can be efficiently explored. We determine here the fingerprint of partial oxidation on the photoemission lines of nanoparticles of selected TTF-based conductors., This research was supported by the Spanish Ministry of Economy and Competitiveness (MINECO) under Contract No. PGC2018-095032-B-100. The ICN2 is funded by the CERCA program/Generalitat de Catalunya. The ICN2 is supported by the Severo Ochoa program of MINECO (Grant SEV-2017-0706). The research leading to these results received funding from the European Community’s Seventh Framework Program (FP7/2007-2013) under grant agreement no. 226716. We also acknowledge support through the BESSY IA-SFS program (BESSY-ID.09.2.90190).

International audience; We have deposited WS2 thin films on Si, SiO2/Si, and sapphire substrates by reactive sputtering from a WS2 target in an Ar/H2S atmosphere. We demonstrate that it is possible to deposit (001)-textured tungsten sulfide films that are thicker than 100 nm. However, the sputtered films are slightly substoichiometric with a composition of WS1.94. Films were deposited at different processing pressures (0.67 Pa–6.67 Pa), substrate temperatures (up to 700 °C) and relative amounts of H2S (0%–100%) in the gas mixture. Structure, morphology, composition, and resistivity of the films were investigated for the different processing conditions. Results from X-ray diffraction show that best crystallization was achieved for the highest substrate temperatures and processing pressures. We show that the addition of H2S may help obtaining fully stoichiometric films and reduce the risk of losing the (001) texture for thicker films. The challenges of obtaining an epitaxial and fully stoichiometric film are pointed out and suggestions on how to modify the process parameters in order to obtain films with even higher quality are presented.

Ambient-pressure Kelvin probe and photoelectron yield spectroscopy methods were employed to investigate the impact of the KF and RbF postdeposition treatments (KF-PDT, RbF-PDT) on the electronic features of Cu(In,Ga)Se2 (CIGSe) thin films and the CdS/CIGSe interface in a CdS thickness series that has been sequentially prepared during the chemical bath deposition (CBD) process depending on the deposition time. We observe distinct features correlated to the CBD-CdS growth stages. In particular, we find that after an initial CBD etching stage, the valence band maximum (VBM) of the CIGSe surface is significantly shifted (by 180-620 mV) toward the Fermi level. However, VBM positions at the surface of the CIGSe are still much below the VBM of the CIGSe bulk. The CIGSe surface band gap is found to depend on the type of postdeposition treatment, showing values between 1.46 and 1.58 eV, characteristic for a copper-poor CIGSe surface composition. At the CdS/CIGSe interface, the lowest VBM discontinuity is observed for the RbF-PDT sample. At this interface, a thin layer with a graded band gap is found. We also find that K and Rb act as compensating acceptors in the CdS layer. Detailed energy band diagrams of the CdS/CIGSe heterostructures are proposed.

International audience; The magnetic and structural properties of Hf0.75Ta0.25Fe2 have been investigated under the duplicate conditions, i.e., high magnetic fields and high pressures, by combining magnetization measurements up to 26 T, neutron powder diffraction experiments up to 14.5 T, and angle dispersive synchrotron x-ray diffraction up to 10 GPa. The intermetallic compound Hf0.75Ta0.25Fe2 exhibits an antiferromagnetic (AFM) ground state below the Néel temperature TN = 342 K. In the AFM structure, the Fe-6h magnetic moments (1.02 μΒ at 2 K) align along the c axis while Fe atoms at 2a sites are not magnetically ordered. We further show that the AFM ground state gets transformed into a ferromagnetic (FM) state via a field-induced metamagnetic phase transition. Magnetic-field dependent neutron diffractograms demonstrate that FM phase sets in with a change of the easy magnetization direction from axial to basal-plane and an extremely anisotropic lattice expansion. The unit cell expands drastically in the basal plane upon increasing the applied magnetic field, while its dimension along c-axis shrinks slightly; resulting in a huge positive volume magnetostriction ΔV/V = 0.78%. The application of hydrostatic pressure leads to the continuous decrease of the cell parameters. The shrinkage of the hexagonal cell is anisotropic with a larger compression along the six-fold symmetry axis c. A bulk modulus of K0 = 247 GPa has been deduced from the pressure-volume relationship.

Using ultrafast x-ray diffraction, we directly monitor the lattice dynamics induced by femtosecond laser pulses in nanoscale thin films of bismuth iron garnet in external magnetic fields ${H}_{\mathrm{ext}}$. We control the ultrafast laser-induced lattice strain amplitude by changing the laser pulse helicity. The strength of ${H}_{\mathrm{ext}}$ is used as an external parameter to switch the helicity dependence on and off, respectively. Based on magneto-optical spectroscopic measurements, we explain these phenomena by magnetic circular dichroism. Our findings highlight an important approach for ultrafast manipulation of lattice strain in magnetic materials, in particular insulators, and open exciting perspectives towards ultrafast control of lattice strain and heat-induced magnetization switching and spin waves in bismuth substituted iron garnets using the polarization of light.

International audience; In this paper, we investigate the magnetic, optical, and lattice responses of a Pt/Cu/Bi 1 Y 2 Fe 5 O 12 /Gd 3 Ga 5 O 12 heterostructure to femtosecond laser excitation of the opaque Pt/Cu metallic bilayer. The electronic excitation generates coherent and incoherent phonons, which trigger high-frequency standing spin waves (SWs) in the dielectric Bi 1 Y 2 Fe 5 O 12 layer via a phonon-induced change of magnetic anisotropy. We find that the incoherent phonons (heat) can induce a fast (1000 ps) decrease of the magnetic order by different spin-phonon interaction scenarios. These results open perspectives for generating high-frequency SWs in buried magnetic garnets.

International audience; Several emerging battery technologies are currently on endeavour to take a share of the dominant position taken by Li-ion batteries in the field of energy storage. Among them, sodium-based batteries offer a combination of attractive properties i.e., low cost, sustainable precursors and secure raw material supplies. Na-based batteries include related battery concepts, such as Na-ion, all solid-state Na batteries, Na/O2 and Na/S, that differ in key components and in redox chemistry, and therefore result in separate challenges and metrics. Na-ion batteries represent an attractive solution which is almost ready to challenge Li-ion technology in certain applications; the other cell concepts represent a more disruptive innovation, with a higher performance gain, provided that major hurdles are overcome. The present review aims at highlighting the most promising materials in the field of Na-based batteries and challenges needed to be addressed to make this technology industrially appealing, by providing an in-depth analysis of performance metrics from recent literature. To this end, half-cell reported metrics have been extrapolated to full cell level for the more mature Na-ion technology to provide a fair comparison with existing technologies.

International audience; The development of tailorable and biocompatible three-dimensional (3D) substrates or molecular networks that reliably mimic the extracellular matrix (ECM) and influence cell behavior and growth in vitro is of increasing interest for cell-based applications in the field of tissue engineering and regenerative medicine. In this context, we present a novel coiled coilbased peptide that self-assembles into a 3D-$\alpha$-helical fibril network and functions as a selfsupporting hydrogel. By functionalizing distinct coiled-coil peptides with cellular binding motifs (RGD) or carbohydrate ligands (mannose), and by utilizing the multivalency and modularity of coiled-coil assemblies, tailored artificial ECMs are obtained. Fibrillar network and ligand density, as well as ligand composition can readily be adjusted by changes in water content or peptide concentrations, respectively. Mesoscopic structure of these networks was assessed by rheology and small-angle neutron scattering experiments. Initial cell viability studies using NIH/3T3 cells showed comparable or even superior cell viability using the presented artificial ECMs, compared to commercially available 3D-cell culture scaffold Matrigel®. The herein reported approach presents a reliable (low batch-to-batch variation) and modular pathway towards biocompatible and tailored artificial ECMs.

International audience; Unusual adsorption phenomena, such as breathing and negative gas adsorption (NGA), are rare and challenge our thermodynamic understanding of adsorption in deformable porous solids. In particular, NGA appears to break the rules of thermodynamics in these materials by exhibiting a spontaneous release of gas accompanying an increase in pressure. This anomaly relies on long-lived metastable states. A fundamental understanding of this process is desperately required for the discovery of new materials with this exotic property. Interestingly, NGA was initially observed upon adsorption of methane at relatively low temperature, close to the respective standard boiling point of the adsorptive, and no NGA was observed at elevated temperatures. In this contribution, we present an extensive investigation of adsorption of an array of gases at various temperatures on DUT-49, a material which features an NGA transition. Experiments, featuring a wide range of gases and vapors at temperatures ranging from 21–308 K, were used to identify for each guest a critical temperature range in which NGA can be detected. The experimental results were complemented by molecular simulations that help to rationalize the absence of NGA at elevated temperatures, and the non-monotonic behavior present upon temperature decrease. Furthermore, this in-depth analysis highlights the crucial thermodynamic and kinetic conditions for NGA, which are unique to each guest and potentially other solids with similar effects. We expect this exploration to provide detailed guidelines for experimentally discovering NGA and related “rule breaking” phenomena in novel and already known materials, and provide the conditions required for the application of this effect, for example as pressure amplifying materials.

International audience; EXAFS analysis of pure elements, binary and ternary equiatomic refractory alloys within the Nb-Zr-Ti-Hf-Ta system is performed at the Nb and Zr K-edges to analyze the evolution of the chemical local environment and the lattice distortion. A good mixing of the elements is found at the atomic scale. For some compounds, a distribution of distances between the central atom and its neighbors suggests a distortion of the structure. Finally, analysis of the Debye-Waller parameters show some correlation with the lattice distortion parameter δ², and allows to quantify experimentally the static disorder in medium entropy alloys.

In this contribution, the dynamics of a proton-coupled electron-transfer (PCET) process for nitrogen-doped graphene oxide (NGO) model systems is studied. The real-time electron dynamics of the over...

Robustness to disorder - the defining property of any topological state - has been mostly tested in low-disorder translationally-invariant materials systems where the protecting underlying symmetry, such as time reversal, is preserved. The ultimate disorder limits to topological protection are still unknown, however, a number of theories predict that even in the amorphous state a quantized conductance might yet reemerge. Here we report a directly detected robust spin response in structurally disordered thin films of the topological material Sb2Te3 free of extrinsic magnetic dopants, which we controllably tune from a strong (amorphous) to a weak crystalline) disorder state. The magnetic signal onsets at a surprisingly high temperature (~ 200 K) and eventually ceases within the crystalline state. We demonstrate that in a strongly disordered state disorder-induced spin correlations dominate the transport of charge - they engender a spin memory phenomenon, generated by the nonequilibrium charge currents controlled by localized spins. The negative magnetoresistance (MR) in the extensive spin-memory phase space is isotropic. Within the crystalline state, it transitions into a positive MR corresponding to the weak antilocalization (WAL) quantum interference effect, with a 2D scaling characteristic of the topological state. Our findings demonstrate that these nonequilibrium currents set a disorder threshold to the topological state; they lay out a path to tunable spin-dependent charge transport and point to new possibilities of spin control by disorder engineering of topological materials

International audience; Layered Ruddlesden–Popper (RP) lanthanide nickelates, Lnn+1NinO3n+1 (Ln = La, Pr and Nd; n = 1, 2 and 3), are considered potential cathode materials in solid oxide fuel cells. In this study, the thermal evolution of the structure, oxygen nonstoichiometry, electrical conductivity and oxygen transport properties of La2NiO4+δ, Nd2NiO4+δ, La3Ni2O7−δ, La4Ni3O10−δ, Pr4Ni3O10−δ and Nd4Ni3O10−δ are investigated. Phase transitions involving a disruption of the cooperative tilting of the perovskite layers in the low-temperature structure thereby transforming it to a more symmetric structure are observed in several of the materials upon heating in air. Pr4Ni3O10−δ and Nd4Ni3O10−δ show no phase transition from room temperature up to 1000 °C. High density ceramics (>96%) are obtained after sintering at 1300 °C and (for n = 2 and n = 3 members) post-sintering annealing at reduced temperatures. Data for the electrical conductivity measurements on these specimens indicate itinerant behaviour of the charge carriers in the RP nickelates. The increase in p-type conductivity with the order n of the RP phase is interpreted as arising from the concomitant increase in the formal valence of Ni. The observations can be interpreted in terms of a simple energy band scheme, showing that electron holes are formed in the σx2−y2↑ band upon increasing the oxidation state of Ni. Electrical conductivity relaxation measurements reveal remarkable similarities between the surface exchange coefficients (kchem) of the different RP phases despite the differences in the order parameter n and the nature of the lanthanide ion. Calculation of the oxygen self-diffusion coefficients (Ds) from the experimental values of the chemical diffusion coefficients (Dchem), using the corresponding data of oxygen non-stoichiometry from thermogravimetry measurements, shows that these are strongly determined by the order parameter n. The value of Ds decreases almost one order of magnitude on going from the n = 1 members La2NiO4+δ and Nd2NiO4+δ to the n = 2 member La3Ni2O7−δ, and again one order of magnitude on going to the n = 3 members La4Ni3O10−δ, Pr4Ni3O10−δ and Nd4Ni3O10−δ. The results confirm that oxygen-ion transport in the investigated RP nickelates predominantly occurs via an interstitialcy mechanism within the rock-salt layer of the structures.

openaire: EC/H2020/721065/EU//CREATE Various bifunctional metal-oxide composites have recently been proposed as advanced hydrogen oxidation reaction (HOR) electrocatalysts for anion-exchange membrane fuel cells (AEMFCs). It is postulated that metal and oxide are active sites for the adsorption of hydrogen/proton and hydroxide ions, respectively. Of particular interest are the so-called buried interfaces. To investigate processes governing activity and stability at such interfaces, we prepare model Pd and Pt electrocatalysts which are fully covered by thin CeOx films. We investigate how oxide thickness influences HOR activity and dissolution stability of the electrocatalysts. It is found that materials behave very differently and that only Pd exhibits an enhanced HOR activity, while both oxide-protected metals are more stable toward dissolution. A 10-fold decrease in dissolution and 15-fold increase in HOR exchange current density are demonstrated for the optimized Pd/CeOx composites in comparison to pure Pd. We assess the mechanism of the electrocatalytic improvement as well as the role of the protective oxide films in such systems through advanced electrochemical and physical analysis. It is highlighted that a uniform, semipermeable oxide layer with a maximized electrocatalyst-oxide interface is crucial to form HOR catalysts with improved activity and stability.

Framework materials at the molecular level, such as metal–organic frameworks (MOF), were recently found to exhibit exotic and counterintuitive micromechanical properties. Stimulated by host–guest interactions, these so-called soft porous crystals can display counterintuitive adsorption phenomena such as negative gas adsorption (NGA). NGA materials are bistable frameworks where the occurrence of a metastable overloaded state leads to pressure amplification upon a sudden framework contraction. How can we control activation barriers and energetics via functionalization of the molecular building blocks that dictate the frameworks' mechanical response? In this work we tune the elastic and inelastic properties of building blocks at the molecular level and analyze the mechanical response of the resulting frameworks. From a set of 11 frameworks, we demonstrate that widening of the backbone increases stiffness, while elongation of the building blocks results in a decrease in critical yield stress of buckling. We further functionalize the backbone by incorporation of sp3 hybridized carbon atoms to soften the molecular building blocks, or stiffen them with sp2 and sp carbons. Computational modeling shows how these modifications of the building blocks tune the activation barriers within the energy landscape of the guest-free bistable frameworks. Only frameworks with free energy barriers in the range of 800 to 1100 kJ mol−1 per unit cell, and moderate yield stress of 0.6 to 1.2 nN for single ligand buckling, exhibit adsorption-induced contraction and negative gas adsorption. Advanced experimental in situ methodologies give detailed insights into the structural transitions and the adsorption behavior. The new framework DUT-160 shows the highest magnitude of NGA ever observed for nitrogen adsorption at 77 K. Our computational and experimental analysis of the energetics and mechanical response functions of porous frameworks is an important step towards tuning activation barriers in dynamic framework materials and provides critical design principles for molecular building blocks leading to pressure amplifying materials., We characterise the elastic properties of molecular building blocks and how they impact the mechanical properties of soft porous crystals.

International audience; When the spatial dimensions of metallic heterostructures shrink below the mean free path of its conduction electrons, the transport of electrons and hence the transport of thermal energy by electrons continuously changes from diffusive to ballistic. Electron-phonon coupling sets the mean free path to the nanoscale and the time for equilibration of electron and lattice temperatures to the picosecond range. A particularly intriguing situation occurs in trilayer heterostructures combining metals with very different electron-phonon coupling strength: Heat energy deposited in few atomic layers of Pt is transported into a nanometric Ni film, which is heated more than the Cu film through which the heat is released. Femtosecond pump-probe experiments with hard X-ray pulses provide a layer-specific probe of the heat energy. A purely diffusive two-temperature model with increased thermal conductivity of hot electrons excellently reproduces the observed signals from all three layers. At the time when the Ni lattice is maximally heated, no significant heat has entered the Cu lattice. This phenomenon would be enhanced in thinner layers where ballistic transport dominates. In this context it is shown that purely diffusive transport can lead to a linear time-to-length dependence that must not be misinterpreted as ballistic transport.

Bismuth vanadate (BiVO4) has surface states that give rise to defect levels that mediate electron-hole recombination. In order to minimize the inefficiencies, an ultrathin Al overlayer was deposited on the BiVO4electrodes. A 54 % improvement on the photocurrent density was obtained using the Al-modified BiVO4electrode, accompanied by a 15 % increase in stability over 7.5 h of continuous irradiation. Moreover, surface capacitance measurements showed that the Al overlayer was indeed passivating the surface states. We also shed light on the deposition of an Al overlayer on the surface of BiVO4, by investigating the process on model BiVO4powders. This study presents useful, previously unreported information about the surface chemistry of BiVO4based on experimental methods and gives unique insights on the characterization of the BiVO4surface. The existence of surface reactive sites on BiVO4was confirmed and quantified (1.5 reactive sites/nm2) via chemical titration

Two-pulse laser excitation of FePt nanolayers distinguishes ultrafast stresses of magnetic excitations from the Poisson effect., Invar-behavior occurring in many magnetic materials has long been of interest to materials science. Here, we show not only invar behavior of a continuous film of FePt but also even negative thermal expansion of FePt nanograins upon equilibrium heating. Yet, both samples exhibit pronounced transient expansion upon laser heating in femtosecond x-ray diffraction experiments. We show that the granular microstructure is essential to support the contractive out-of-plane stresses originating from in-plane expansion via the Poisson effect that add to the uniaxial contractive stress driven by spin disorder. We prove the spin contribution by saturating the magnetic excitations with a first laser pulse and then detecting the purely expansive response to a second pulse. The contractive spin stress is reestablished on the same 100-ps time scale that we observe for the recovery of the ferromagnetic order. Finite-element modeling of the mechanical response of FePt nanosystems confirms the morphology dependence of the dynamics.

Concomitant with the rapid development of quantum technologies, challenging demands arise concerning the certification and characterization of devices. The promises of the field can only be achieved if stringent levels of precision of components can be reached and their functioning guaranteed. This review provides a brief overview of the known characterization methods of certification, benchmarking, and tomographic recovery of quantum states and processes, as well as their applications in quantum computing, simulation, and communication., Comment: 10 pages, 1 figure, 5 text boxes, 1 table, invited review for Nature Reviews, v2 extended and updated

International audience; Interparticle Coulombic Decay (ICD) is an efficient energy transfer process between two weakly interacting systems. ICD was recently proposed as the underlying fundamental mechanism for technological purposes based on quantum dot nanostructures, such as wavelength-sensitive detectors. Via ICD, an excited donor quantum dot releases its excess energy by ionizing a neighbouring acceptor dot. Here, we demonstrate that the presence of a third (ICD inactive) quantum dot can serve as a bridge between the two dots, which is shown to result in an enhancement of the efficiency of the ICD-mediated energy transfer. Furthermore, our results show that this enhancement is found to be robust against the change of the characteristics of the bridge quantum dot and particularly the depth and size. On the other hand, its relative position with respect to the donor and acceptor dots is found to foster the ICD when it is located in between the two dots. Our findings provide new insights for the development of ICD-based nanostructure technologies and particularly for rational design of three coupled quantum dots. 2

International audience; We investigated the Fe-Fe 2 Ti eutectic microstructure obtained by Direct Energy Deposition (DED) with a hypereutectic composition of Fe-17.6 at.% Ti. Ultrafine lamellar spacings as low as 200 nm were achieved, features which otherwise can only be obtained in thin specimens, e.g. by suction casting. However, at interlayer boundaries (ILBs) a globular morphology of the primary Fe 2 Ti phase is observed with halos of the Fe phase. For the given DED conditions the crystalline structure is thus discontinuous across the ILBs. Both 2D and 3D analysis methods were used to quantify the microstructure, including high resolution synchrotron holographic X-ray computed tomography (HXCT). The generic behaviour of eutectic systems under conditions that qualitatively correspond to those of laser additive manufacturing was explored by phase-field modelling for selected nucleation scenarios and alloy compositions spanning from eutectic to hyper-eutectic. While providing valuable insights into microstructure formation, the simulations point out the need to further deepen our understanding about melting under additive manufacturing conditions in order to implement suitable nucleation and / or free growth models. The simulations also show that globular ILBs can be prevented when using exactly eutectic alloy compositions.

This work reports on developments in the field of wide band gap Cu2ZnXY4 (with X = Sn, Si or Ge, and Y = S, Se) kesterite thin film solar cells. An overview on recent developments and the current understanding of wide band gap kesterite absorber layers, alternative buffer layers, and suitable transparent back contacts is presented. Cu2ZnGe(S,Se)(4) absorbers with absorber band gaps up to 1.7 eV have been successfully developed and integrated into solar cells. Combining a CdS buffer layer prepared by an optimized chemical bath deposition process with a 1.36 eV band gap absorber resulted in a record Cu2ZnGeSe4 cell efficiency of 7.6%, while the highest open-circuit voltage of 730 mV could be obtained for a 1.54 eV band gap absorber and a Zn(O,S) buffer layer. Employing InZnOx or TiO2 protective top layers on SnO2:In transparent back contacts yields 85-90% of the solar cell performance of reference cells (with Mo back contact). These advances show the potential as well as the challenges of wide band gap kesterites for future applications in high-efficiency and low-cost tandem photovoltaic devices. This project has received funding from the European Union's Horizon 2020 Research and Innovation Program under grant agreement No. 640868. The synchrotron radiation experiments were performed at the SPring-8 beamline BL15XU with the approval of the NIMS Synchrotron X-ray Station (Proposals 2016A4600, 2016B4601, and 2017A4600) and at BESSY II with the approval of HZB. B. Vermang has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Programme (grant agreement no. 715027).

International audience; Laser-driven non-local electron dynamics in ultrathin magnetic samples on a sub-10 nm length scale is a key process in ultrafast magnetism. However, the experimental access has been challenging due to the nanoscopic and femtosecond nature of such transport processes. Here, we present a scattering-based experiment relying on a laser-induced electro-and magneto-optical grating in a Co/Pd ferromagnetic multilayer as a new technique to investigate non-local magnetization dynamics on nanometer length and femtosecond timescales. We induce a spatially modulated excitation pattern using tailored Al near-field masks with varying periodicities on a nanometer length scale and measure the first four diffraction orders in an x-ray scattering experiment with magnetic circular dichroism contrast at the free-electron laser facility FERMI, Trieste. The design of the periodic excitation mask leads to a strongly enhanced and characteristic transient scattering response allowing for sub-wavelength in-plane sensitivity for magnetic structures. In conjunction with scattering simulations, the experiment allows us to infer that a potential ultrafast lateral expansion of the initially excited regions of the magnetic film mediated by hot-electron transport and spin transport remains confined to below three nanometers.

International audience; Optical excitation of spin-ordered rare earth metals triggers a complex response of the crystal lattice since expansive stresses from electron and phonon excitations compete with a contractive stress induced by spin disorder. Using ultrafast x-ray diffraction experiments, we study the layer specific strain response of a dysprosium film within a metallic heterostructure upon femtosecond laser-excitation. The elastic and diffusive transport of energy to an adjacent, non-excited detection layer clearly separates the contributions of strain pulses and thermal excitations in the time domain. We find that energy transfer processes to magnetic excitations significantly modify the observed conventional bipolar strain wave into a unipolar pulse. By modeling the spin system as a saturable energy reservoir that generates substantial contractive stress on ultrafast timescales, we can reproduce the observed strain response and estimate the time- and space dependent magnetic stress. The saturation of the magnetic stress contribution yields a non-monotonous total stress within the nanolayer, which leads to unconventional picosecond strain pulses.

24th International Symposium on Metastable, Amorphous and Nanostructured Materials (ISMANAM), San Sebastian, SPAIN, JUN 18-23, 2017; The effect of impurities, Sr additions and cooling rate on the microstructural evolution of high-purity Al-10Si-0.3Fe and corresponding impure commercial alloys is examined by optical microscopy and in situ by X-ray synchrotron 3D tomography. At fast cooling rate (similar to 470 K min(-1)) the presence of impurities decreases the growth rate of primary Al dendrites and enables formation of the beta phase. Besides a modification of the eutectic Si, the addition of Sr prevents the formation of the beta phase and increases the growth rate of Al dendrites. A low cooling rate (similar to 1 K min(-1)) leads to the formation of alpha, gamma, delta and beta intermetallic phases. In all four alloys, the dominant phase is the delta phase, regardless of commercial impurities or the Sr level. Intermetallic phases formed during slow cooling rates are much coarser than those formed during fast cooling and they have different morphologies. Our results suggest that the velocity of growth and the final morphology and size of the intermetallic phases are mainly determined by diffusional processes which in turn are controlled by the cooling rate. (c) 2018 Elsevier B.V. All rights reserved.

Made available in DSpace on 2022-04-29T08:39:59Z (GMT). No. of bitstreams: 0 Previous issue date: 2022-02-14 The domain switching dynamics in a relaxor ferroelectric lanthanum-modified lead zirconate titanate thin film with 12 mol. % La was investigated by time-resolved x-ray diffraction. While most frequently epitaxial thin films are investigated, the present work reports results on a polycrystalline thin film. Asymmetric butterfly loops of the strain as a function of the applied electric field evidenced a built-in electric field oriented toward the thin film-substrate interface. The piezoelectric coefficient d33 (in the film reference frame) diminishes with the increasing frequency of an applied AC electric field. From the strain transient during the application of positive-up negative-down voltage pulse sequences with frequencies of up to 100 kHz, characteristic times of the order of 100-200 ns were determined for these relaxor ferroelectric thin films. While switching times ranging from the picosecond to the millisecond range are reported in the literature for different materials, these characteristic switching times are comparable to epitaxial lead zirconate titanate thin films of various compositions despite the polycrystallinity of the present thin film. However, the evidenced built-in electric field significantly influences the switching behavior for different polarities. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH Wilhelm-Conrad Röntgen Campus BESSY II, Albert-Einstein-Straße 15 Aix Marseille Univ Univ Toulon CNRS IM2NP UMR 7334 Synchrotron SOLEIL L'Orme des Merisiers, Saint-Aubin - BP 48, Gif-sur-Yvette Institute Functional Oxides for Energy-Efficient Information Technology Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Hahn-Meitner-Platz 1 Freie Universität Berlin Physical Chemistry, Arnimallee 22 Department of Physics and Chemistry School of Natural Sciences and Engineering São Paulo State University (UNESP), Ilha Solteira, SP Department of Physics and Chemistry School of Natural Sciences and Engineering São Paulo State University (UNESP), Ilha Solteira, SP

We study the correlations length of the charge-charge pair correlations in concentrated electrolyte solutions by means of all-atom, explicit-solvent molecular dynamics simulations. We investigate LiCl and NaI in water, which constitute highly soluble, prototypical salts for experiments, as well as two more complex, molecular electrolyte systems of lithium bis(trifluoromethane)sulfonimide (LiTFSI), commonly employed in electrochemical storage systems, in water and in an organic solvent mixture of dimethoxyethane (DME) and dioxolane (DOL). Our simulations support the recent experimental observations as well as theoretical predictions of a non-monotonic behavior of the correlation length with increasing salt concentration. We observe a Debye-Hückel like regime at low concentration, followed by a minimum reached when d/λD = 1, where λD is the Debye correlation length and d the effective ionic diameter, and an increasing correlation length with salt concentration in very concentrated electrolytes. As in the experiments, we find that the screening length in the concentrated regime follows a universal scaling law as a function d/λD for all studied salts. However, the scaling exponent is significantly lower than the experimentally measured one, and lies in the range of the theoretical predictions based on much simpler electrolyte models.

Chalcopyrite solar cells achieve efficiencies above 23%. The latest improvements are due to post-deposition treatments (PDT) with heavy alkalis. This study provides a comprehensive description of the effect of PDT on the chemical and electronic structure of surface and bulk of Cu(In,Ga)Se-2. Chemical changes at the surface appear similar, independent of absorber or alkali. However, the effect on the surface electronic structure differs with absorber or type of treatment, although the improvement of the solar cell efficiency is the same. Thus, changes at the surface cannot be the only effect of the PDT treatment. The main effect of PDT with heavy alkalis concerns bulk recombination. The reduction in bulk recombination goes along with a reduced density of electronic tail states. Improvements in open-circuit voltage appear together with reduced band bending at grain boundaries. Heavy alkalis accumulate at grain boundaries and are not detected in the grains. This behavior is understood by the energetics of the formation of single-phase Cu-alkali compounds. Thus, the efficiency improvement with heavy alkali PDT can be attributed to reduced band bending at grain boundaries, which reduces tail states and nonradiative recombination and is caused by accumulation of heavy alkalis at grain boundaries. This work was supported by the European Union's Horizon 2020 research and innovation program under grant agreement no. 641004 (Sharc25) and by the Swiss State Secretariat for Education, Research and Innovation (SERI) under contract number 15.0158. Siebentritt, S (reprint author), Univ Luxembourg, Lab Photovolta, Phys & Mat Sci Res Unit, 41 Rue Brill, L-4422 Belvaux, Luxembourg. susanne.siebentritt@uni.lu

The incorporation of terminal alkynes into the chemical structure of persistent organic perchlorotriphenylmethyl (PTM) radicals provides new chemical tools to expand their potential applications. In this work, this is demonstrated by the chemical functionalization of two types of substrates, hydrogenated SiO2-free silicon (Si–H) and gold, and, by exploiting the click chemistry, scarcely used with organic radicals, to synthesise multifunctional systems. On one hand, the one-step functionalization of Si–H allows a light-triggered capacitance switch to be successfully achieved under electrochemical conditions. On the other hand, the click reaction between the alkyne-terminated PTM radical and a ferrocene azide derivative, used here as a model azide system, leads to a multistate electrochemical switch. The successful post-surface modification makes the self-assembled monolayers reported here an appealing platform to synthesise multifunctional systems grafted on surfaces., S. Ababou-Girard and C. Meriadec (Institut de Physique de Rennes, UMR6251, France) are fully acknowledged for XPS measurements on the Si–H surfaces. Dr Vega Lloveras and Amable Bernab´e are acknowledged for the EPR and MALDI-ToF measurements, respectively. We also would like to thank Thomas Chass´e for allowing us to access the photoelectron laboratory at the University of Tubingen, Hilmar Adler for ¨ technical support, and Helmholtz-Zentrum Berlin (HZB) for providing beamtime at BESSY II. This work was funded by the Spanish Ministry project FANCYCTQ2016-80030-R, the Generalitat de Catalunya (2017SGR918) and the Spanish Ministry of Economy and Competitiveness, through the “Severo Ochoa” Programme for Centers of Excellence in R&D (SEV-2015-0496), the CSIC with the i-Link+ 2018 (Ref. LINKA20128) and CIBERBBN. J. A. de S. is enrolled in the Materials Science PhD program of UAB. J.A. de S. thanks the Spanish Ministry for the FPI fellowship. Financial support from the German Research Foundation (DFG) under the contract CA852/11-1 and from Helmholtz-Zentrum Berlin is gratefully acknowledged.

Halogenation of conjugated molecules represents a powerful approach to tune the electronic structure of molecular thin films through inductive effects and long-range intermolecular electrostatic interactions. The mixing of halogenated molecules with their pristine counterparts has recently proven successful in altering the blend’s energy levels to adjust the open-circuit voltage of organic solar cells by the mixing ratio. Here, we show that the prevailing rationale for this effect is not equally valid for different molecular orientations. We provide a comprehensive experimental and theoretical analysis of the prototypical blend formed by pentacene and perfluoropentacene to relate structure with electronic properties. We find a mixed-stack structural motif in standing and lying orientations depending on the substrate nature. In the standing orientation, the ionization potential lies in between the values of the pure components, in line with the established picture of averaged molecular quadrupole moments. For the lying orientation, however, we experimentally observe an ionization potential lower than both pristine values, which seems at odds with this simple rationale. Electrostatic simulations based on the knowledge of the atomistic structure of the films capture the complex experimental scenario for both orientations. In particular, the ultralow ionization potential of films formed by lying molecules is identified as a signature of the monolayer structure, where quadrupolar interactions are responsible for a difference of ca. 0.4 eV in the highest occupied molecular orbital energy as compared to thicker films with the same molecular orientation.

This paper quantifies the lattice expansion of an insulator upon two photon excitation. The ultrafast x-ray diffraction experiments measure a clean quadratic dependence of the strain on the laser fluency and prove that the pulse intensity is the relevant quantity, as the signal is anti-proportional to the pulse duration. The investigated material Bi:YIG is the standard material for magnonics, where ultrashort laser-pulses can create spin-waves via various mechanisms, including strain modulation of the anisotropy

We review some of the recent efforts in devising and engineering bosonic qubits for superconducting devices, with emphasis on the Gottesman-Kitaev-Preskill (GKP) qubit. We present some new results on decoding repeated GKP error correction using finitely-squeezed GKP ancilla qubits, exhibiting differences with previously studied stochastic error models. We discuss circuit-QED ways to realize CZ gates between GKP qubits and we discuss different scenario's for using GKP and regular qubits as building blocks in a scalable superconducting surface code architecture., 54 pages; 18 Figs; 3 Appendices; invited topical review for Quantum Science & Technology. v2 has a few corrections and some additional references. v3 has a few additional corrections and references

International audience; Magnetization, magnetic torque, neutron diffraction and NMR experiments are used to map out the H−T phase diagram of the prototypical quasi-two-dimensional ferro-antiferromagnet Pb2VO(PO4)2 in magnetic fields up to 27 T. When the field is applied perpendicular to the axis of magnetic anisotropy, a new magnetic state emerges through a discontinuous transition and persists in a narrow field range just below saturation. The measured NMR spectra suggest a complex and possibly incommensurate magnetic order in that regime.

Zinc oxide (ZnO) thin films grown on glass substrates are prepared by means of the Ion Layer Gas Reaction process. The XRD pattern revealed that the ZnO lattice parameters decrease continuously, with the increasing of the film thickness, indicating a continuous variation in the compressive strain. The influence of the thickness on the optical, morphological and structural properties of deposited ZnO thin films was investigated. The UV–Vis absorption spectra of deposited thin films were shown to exhibit a blue-shift, resulting in an increase in the optical band gap from 3.13 eV to 3.24 eV. Structural parameters such as crystallite size, lattice parameters, Zn–O bond length, and residual stress have been determined, and the compressive strain (tensile stress) is found to increase with the increasing of spray time and in turn deposited thin film thickness. The PL spectra of deposited ZnO films, show stronger PL intensity with increasing deposited thin film thickness, which confirm the influence of deposited film thickness on the recombination process of charge carriers and thus on its optical properties. These results, were confirmed by the photo-electrochemical experiments. In addition, a wettability alteration and shift from hydrophobic to hydrophilic surface is observed under UV light exposure, which shows that structural defects and surface morphology of deposited thin films were also demonstrated to have a direct impact on deposited films’ optical properties. Furthermore, to further confirm these experimental optical results, theoretical first principle calculations were conducted. In addition, a wettability alteration and shift from hydrophobic to hydrophilic surface is observed under UV light exposure.