Exploring the formation of gold/silver nanoalloys with gas-phase synthesis and machine-learning assisted simulations.

While nanoalloys are of paramount scientific and practical interest, the main processes leading to their formation are still poorly understood. Key structural features in the alloy systems, including the crystal phase, chemical ordering, and morphology, are challenging to control at the nanoscale, making it difficult to extend their use to industrial applications. In this contribution, we focus on the gold/silver system that has two of the most prevalent noble metals and combine experiments with simulations to uncover the formation mechanisms at the atomic level. Nanoparticles were produced using a state-of-the-art inert-gas aggregation source and analyzed using transmission electron microscopy and energy-dispersive X-ray spectroscopy. Machine-learning-assisted molecular dynamics simulations were employed to model the crystallization process from liquid droplets to nanocrystals. Our study finds a preponderance of nanoparticles with five-fold symmetric morphology, including icosahedra and decahedra which is consistent with previous results on mono-metallic nanoparticles. However, we observed that gold atoms, rather than silver atoms, segregate at the surface of the obtained nanoparticles for all the considered alloy compositions. These segregation tendencies are in contrast to previous studies and have consequences on the crystallization dynamics and the subsequent crystal ordering. We finally showed that the underpinning of this surprising segregation dynamics is due to charge transfer and electrostatic interactions rather than surface energy considerations.

Tuning photovoltaic response in Bi2FeCrO6 films by ferroelectric poling.

Ferroelectric materials are interesting candidates for future photovoltaic applications due to their potential to overcome the fundamental limits of conventional single bandgap semiconductor-based solar cells. Although a more efficient charge separation and above bandgap photovoltages are advantageous in these materials, tailoring their photovoltaic response using ferroelectric functionalities remains puzzling. Here we address this issue by reporting a clear hysteretic character of the photovoltaic effect as a function of electric field and its dependence on the poling history. Furthermore, we obtain insight into light induced nonequilibrium charge carrier dynamics in Bi2FeCrO6 films involving not only charge generation, but also recombination processes. At the ferroelectric remanence, light is able to electrically depolarize the films with remanent and transient effects as evidenced by electrical and piezoresponse force microscopy (PFM) measurements. The hysteretic nature of the photovoltaic response and its nonlinear character at larger light intensities can be used to optimize the photovoltaic performance of future ferroelectric-based solar cells.

Towards sensitive, high-throughput, biomolecular assays based on fluorescence lifetime.

Time-resolved fluorescence detection for robust sensing of biomolecular interactions is developed by implementing time-correlated single photon counting in high-throughput conditions. Droplet microfluidics is used as a promising platform for the very fast handling of low-volume samples. We illustrate the potential of this very sensitive and cost-effective technology in the context of an enzymatic activity assay based on fluorescently-labeled biomolecules. Fluorescence lifetime detection by time-correlated single photon counting is shown to enable reliable discrimination between positive and negative control samples at a throughput as high as several hundred samples per second.

High-throughput time-correlated single photon counting.

We demonstrate time-correlated single photon counting (TCSPC) in microfluidic droplets under high-throughput conditions. We discuss the fundamental limitations in the photon acquisition rate imposed by the single photon detection technique and show that it does not preclude accurate fluorescence lifetime (FLT) measurements at a droplet throughput exceeding 1 kHz with remarkable sensitivity. This work paves the way for the implementation of innovative biomolecular interaction assays relying on the FLT detection of nanosecond-lived fluorophores for high-throughput biotechnological applications, including high-throughput screening or cell sorting potentially allowed by droplet microfluidics or other fast sample handling facilities.

Raman scattering of magnetoelectric gallium ferrite thin films.

Gallium ferrite, Ga(2-x)Fe(x)O(3) (GFO), is a promising magnetoelectric material as it exhibits both magnetic and electric orders close to room temperature. Here, we report a temperature-dependent investigation of GFO thin films with x = 1.0 and 1.4 by using Raman scattering. Our investigation suggests the absence of a structural phase transition of both films in the investigated 90-500 K temperature range, which is similar to earlier observations on bulk samples. We note, however, the occurrence of weak anomalies in the temperature-dependent band position of some phonons, which we attribute to spin-phonon coupling as the anomalies occur close to the Néel temperature of the materials.

Influence of free surface, unsteadiness and viscous effects on oar blade hydrodynamic loads.

Flow around a rowing blade is a very complex phenomenon, involving unsteady three-dimensional flow with violent motion of the free surface. However, in the literature, forces acting on blades are modelled using extreme and dubious simplifications. The aim of the present study was to evaluate the influence of free surface and unsteadiness (two physical characteristics that are commonly neglected when modelling loads on blades) as well as viscous effects. In fact, quasi-static approaches are often used, with no influence of the free surface effects. To conduct this study, computational fluid dynamics is used, supported by experimental results performed with a dedicated device reproducing a simplified rowing stroke in the towing tank. Comparisons show that both free surface flow and unsteadiness must be considered to capture the whole physics of the phenomenon accurately. In contrast, the viscous effects have a very limited influence.