In this study, we explore the influence of bromide anions concentration on the surface chemistry of colloidal gold nanoparticles synthesized via pulsed laser ablation in liquids (PLAL). Using X-ray photoelectron spectroscopy (XPS) in a controlled environment, by probing a beam of free-standing gold nanoparticles, we quantitatively characterize the surface composition of the nanoparticles, revealing that bromide adsorption significantly contributes to surface oxidation independently of counterion type and pH for alkaline solution. Additionally, our findings demonstrate the adjustability of halogen coverage post-synthesis, offering a versatile method for controlling nanoparticle properties.

The performance of time-resolved photoelectron spectroscopy for the study of subpicosecond dynamics of laser-heated solids is often limited by space charge effects. The consequent shift and distortion of the photoelectron spectrum induced by electrons emitted by the ultrashort pump pulse is studied here using a fully coherent approach based on experimental measurements and space charge calculations. The temporal dynamics of the valence band of a copper sample is recorded before and after an 800 nm laser pump excitation at a fluence of 750 mJ/cm2. The probe pulse is produced using a laboratory-based high-harmonics source delivering 25 fs pulses up to 100 eV photon energy. We extract the laser-heating contribution by comparing these measurements with space charge calculations based on particle-in-cell simulations of the pump and probe electron clouds mutual interaction on their way to the detector. The deduced picosecond dynamics associated to the electronic density of states shift is attributed to lattice changes with the help of hydrodynamic simulations including the two-temperature model.

Pulsed laser ablation in liquid (PLAL) is a powerful method for producing nanoparticle colloids with a long-term stability despite the absence of stabilizing organic agents. The colloid stability involves different reactivities and chemical equilibria with complex ionic-specific effects at the nanoparticle/solvent interface which must be strongly influenced by their chemical composition. In this work, the surface composition of PLAL-produced gold nanoparticles in alkaline and saline (NaBr) water is investigated by X-ray photoelectron spectroscopy on free-flying nanoparticles, exempt from any substrate or radiation damage artifact. The Au 4f photoelectron spectra with a depth profiling investigation are used to evaluate the degree of nanoparticle surface oxidation. In alkaline water, the results preclude any surface oxidation contrary to the case of nanoparticles produced in NaBr solution. In addition, the analysis of Br 3d core-level photoelectron spectra agrees with a clear signature of Br on the nanoparticle surface, which is confirmed by a specific valence band feature. This experimental study is supported by DFT calculations, evaluating the energy balance of halide adsorption on different configurations of gold surfaces including oxidation or adsorbed salts.

Surface chemistry of gold nanoparticles produced by laser ablation in liquids has been investigated using synchrotron radiation and the X-ray Photoelectron Spectroscopy technique. Thanks to the recorded core-level and valence spectra, combined with a detailed analysis based on Bayesian statistical methods, the oxide presence and its proportion on the nanoparticle surface have been determined.

Synopsis Ion-ion collisions between slow (kev/u) and fast (MeV/u) ions play an important role in for example astrophysical or inertial fusion plasmas as well as in ion-matter interaction. In this regime the energy transfer is maximum, as all primary electronic processes reach their maximum. At the same time up to today no reliable experimental data exists while being difficult to treat accurately by theory. We present the current status and performance of the low energy beam-line of the FISIC experiment which aims at filling in the blanks in this regime.

We present the Aurore platform for ultrafast sciences. This platform is based on a unique 20 W, 1 kHz, 26 fs Ti:sapphire laser system designed for reliable operation and high intensity temporal contrast. The specific design ensures the high stability in terms of pulse duration, energy, and beam pointing necessary for extended experimental campaigns. The laser supplies 5 different beamlines, all dedicated to a specific field: attosecond science (Aurore 1), ultrafast phase transitions in solids (Aurore 2 and 3), ultrafast luminescence in solids (Aurore 4), and femtochemistry (Aurore 5). The technical specifications of these five beamlines are described in detail, and examples of the recent results are given.

Laser interaction with solids is routinely used for functionalizing materials' surfaces. In most cases, the generation of patterns/structures is the key feature to endow materials with specific properties like hardening, superhydrophobicity, plasmonic color-enhancement, or dedicated functions like anti-counterfeiting tags. A way to generate random patterns, by means of generation of wrinkles on surfaces resulting from laser melting of amorphous Ge-based chalcogenide thin films, is presented. These patterns, similar to fingerprints, are modulations of the surface height by a few tens of nanometers with a sub-micrometer periodicity. It is shown that the patterns' spatial frequency depends on the melted layer thickness, which can be tuned by varying the impinging laser fluence. The randomness of these patterns makes them an excellent candidate for the generation of physical unclonable function tags (PUF-tags) for anti-counterfeiting applications. Two specific ways are tested to identify the obtained PUF-tag: cross-correlation procedure or using a neural network. In both cases, it is demonstrated that the PUF-tag can be compared to a reference image (PUF-key) and identified with a high recognition ratio on most real application conditions. This paves the way to straightforward non-deterministic PUF-tag generation dedicated to small sensitive parts such as, for example, electronic devices/components, jewelry, or watchmak.

Synopsis This work aims to study laser-induced lattice dynamics when there is strong electron-lattice temperature non-equilibrium for which the material properties are poorly known. The proposed experimental technique is time-resolved photoelectron spectroscopy (Tr-PES). The main challenges of such technique are the superposition of pump and probe spectra and the distortion of the probe spectra due to the interaction with pump-induced electrons, called space charge effect (SCE). We strongly reduced this effect by tuning the 100eV XUV beamline we have developed, enabling us to investigate Copper samples.

“Pop-art” like patterns resulting from the interaction of a single laser pulse focused on a-Ge based chalcogenide thin film capped with a SiN layer are presented by Jérôme Gaudin and co-workers. These nondeterministic surface patterns, described in article number 2003032, are wrinkles with a height of less than 100 nm and sub-micrometer periodicity, which depends on the impinging laser fluence. Application as physical unclonable functions is demonstrated using a fast recognition algorithm.

D. Schury1, A. Kumar1, A. Méry2, J.M. Ramillon2, L. Adoui2, J.-Y. Chesnel2, A. Lévy1, S. Macé1, C. Prigent1, J. Rangama2, P. Rousseau2, S. Steydli1, M. Trassinelli1, D. Vernhet1, A. Gumberidze3, Th. Stöhlker3,4,5, A. Bräuning-Demian3, C. Hahn4, U. Spillmann3 and E. Lamour1 1. Institut des Nanosciences de Paris, UMR CNRS 7588, Sorbonne Université, 4 Place Jussieu, 75005 Paris, France 2. CIMAP,CEA/CNRS/ENSICAEN/Université de Caen Basse-Normandie, Boulevard Henri Becquerel, 14070 Caen, France 3. GSI Helmholtzzentrum für Schwerionenforschung, Planckstr. 1, 64291 Darmstadt, Germany 4. Friedrich-Schiller-Universität Jena, Max-Wien-Platz 1, 07743 Jena, Germany 5. Helmholtz-Institut Jena, Fröbelstieg 3, 07743 Jena, Germany

The performance of a newly built omega type electrostatic analyzer designed to act as an in-line charge-state purification system for ions in the kiloelectronvolt energy range is reported. The analyzer consists of a set of four consecutive electrostatic 140° concentric cylindrical electrodes enclosed by Matsuda electrodes. This setup was recently tested and validated using O5+, Ar9+, and Xe20+ ion beams at an energy of 14 qkeV at the ARIBE facility. A resolving power of 10.5 and a transmission of 100% of the desired charge state are measured allowing a good purification of incoming ion beams with charge states up to 10+ and a fairly good purification for charge states at least up to 20+. In comparison with other in-line solutions such as the Wien filter, our system has the advantage of being purely electrostatic and therefore lacking common drawbacks as, for example, hysteresis.

The surface chemistry of gold nanoparticles produced by the pulsed laser ablation in liquids method is investigated by X-ray photoelectron spectroscopy (XPS). The presence of surface oxide expected on these systems is investigated using synchrotron radiation in conditions close to their original state in solvent but free from substrate or solvent effects which could affect the interpretation of spectroscopic observations. For that purpose we performed the experiment on a controlled free-standing nanoparticle beam produced by combination of an atomizer and an aerodynamic lens system. These results are compared with those obtained by the standard situation of deposited nanoparticles on silicon substrate. An accurate analysis based on Bayesian statistics concludes that the existence of oxide in the free-standing conditions cannot be solely confirmed by the recorded core-level 4f spectra. If present, our data indicate an upper limit of 2.15 ± 0.68% of oxide. However, a higher credence to the hypothesis of its existence is brought by the structureless valence profile of the free-standing beam. Moreover, the cross-comparison with the deposited nanoparticles case clearly evidences an important misleading substrate effect. Experiment with free-standing nanoparticles is then demonstrated to be the right way to further investigate oxidation states on Au nanoparticles.

The chemical and geometrical structure of freestanding carbon dots (Cdots) prepared from the pyrolysis of N-hydroxysuccinimide (NHS) have been characterized using X-ray photoelectron spectroscopy (XPS). An aerodynamic lens system was used to generate a sufficient particle density of monodispersed Cdots for XPS studies at the PLEIADES beamline at the SOLEIL synchrotron facility. Varying the X-ray excitation energy between 315 and 755 eV allows probing of the Cdots from the surface toward their core, owing to the kinetic energy dependence of the photoelectron inelastic mean free path. The C 1s, O 1s, and N 1s core-levels were recorded with high-spectral resolution to identify their main chemical components and branching ratios. While high resolution transmission electron microscopy (HRTEM) reveals a defective graphitic core, the C is spectrum evidence two main peaks similar to those measured from the solid NHS. Their relative abundance as a function of the probing depth is strongly related to the chemical composition of the ligand shell that does not vary substantially over the first 3.4 nm. Combining the depth-resolved XPS and HRTEM studies, it was concluded that the Cdots possess a graphitic core surrounded by a relatively homogeneous shell of at least 3.4 nm thickness with a composition similar to that of the solid NHS.

We have investigated the formation, evolution, and late-time propagation of a laser-generated cylindrical blast wave (BW). The whole blast wave evolution over timescales of several nanoseconds was reconstructed experimentally (via temporally resolved interferometric measurements) and via hydrodynamic simulations that included modeling of nonlocal electron transport and radiation diffusion. Comparison between the experimental results and the simulations indicates that the early expansion phase is characterised by nonlocal electron heat transport causing energy spread on times shorter than the typical timescales for hydrodynamic expansion. Nonlocal electron transport ionizes the gas ahead of the plasma front and gives rise to a smooth radial density gradient. At later times, once the shock is launched and the BW is formed, radiation results in reduced shock velocity compared to the adiabatic case. These investigations provide a suitable and effective platform to benchmark the inclusion of kinetic and radiative effects in fluid modeling of the plasma dynamics over timescales that may be inaccessible to fully kinetic simulations.

Magnetic refrigeration based on the magnetocaloric effect at room temperature is one of the most attractive alternatives to the current gas compression/expansion method routinely employed. Nevertheless, in giant magnetocaloric materials, optimal refrigeration is restricted to the narrow temperature window of the phase transition (T-c). In this work, we present the possibility of varying this transition temperature in the same giant magnetocaloric material by ion irradiation. We demonstrate that the transition temperature of iron rhodium thin films can be tuned by the bombardment of ions of Ne5+ with varying fluences up to 10(14) ions cm(-2), leading to optimal refrigeration over a large 270-380 K temperature window. The T-c modification is found to be due to the ion-induced disorder and to the density of new pointlike defects. The variation of the phase transition temperature with the number of incident ions opens new perspectives in the conception of devices using giant magnetocaloric materials.

Synopsis By varying different irradiation conditions, we investigate the reduction of the thermal hysteresis in magnetocaloric thin films induced by impact of slow ions. This suppression looks connected to the total deposited energy by the ions and not to the number of implanted ions. This hypothesis is reinforced by magnetic-force microscope measurements that display local changes induced by clusters of irradiation defects.

The Fast Ion - Slow Ion Collisions (FISIC) project consists of a crossed-beam arrangement to study ion-ion collisions in the intermediate velocity regime. For the low energy channel, ion trajectory simulations has been used to develop a complete beam line that includes a new Omega type purification system located just before the collision point and a charge state analyzer after interaction.

Investigations of the complex behavior of the magnetization of manganese arsenide thin films due to defects induced by irradiation of slow heavy ions are presented. In addition to the thermal hysteresis suppression already highlighted in Trassinelli et al (2014 Appl. Phys. Lett. 104 081906), we report here on new local magnetic features recorded by a magnetic force microscope at different temperatures close to the characteristic sample phase transition. Complementary measurements of the global magnetization in different conditions (applied magnetic field and temperatures) enable the film characterization to be completed. The obtained results suggest that the ion bombardment produces regions where the local mechanical constraints are significantly different from the average, promoting the local presence of magneto-structural phases far from the equilibrium. These regions could be responsible for the thermal hysteresis suppression previously reported, irradiation-induced defects acting as seeds in the phase transition.