Charge carrier dynamics and photocatalytic activity of {111} and {100} faceted AgPO particles.

Silver orthophosphate is a highly promising visible light photocatalyst with high quantum yield for solar driven water oxidation. Recently, the performance of this material has been further enhanced using facet-controlled synthesis. The tetrahedral particles with {111} exposed facets demonstrate higher photocatalytic performance than the cubic particles with {100} exposed facets.

Mechanistic insight into carbon-carbon bond formation on cobalt under simulated Fischer-Tropsch synthesis conditions.

Facile C-C bond formation is essential to the formation of long hydrocarbon chains in Fischer-Tropsch synthesis. Various chain growth mechanisms have been proposed previously, but spectroscopic identification of surface intermediates involved in C-C bond formation is scarce. We here show that the high CO coverage typical of Fischer-Tropsch synthesis affects the reaction pathways of CH adsorbates on a Co(0001) model catalyst and promote C-C bond formation.

MANTIS: A real-time quantitative multispectral imaging system for fusion plasmas.

This work presents a novel, real-time capable, 10-channel Multispectral Advanced Narrowband Tokamak Imaging System installed on the TCV tokamak, MANTIS. Software and hardware requirements are presented together with the complete system architecture. The image quality of the system is assessed with emphasis on effects resulting from the narrowband interference filters.

Ultrafast Dynamics of Nonequilibrium Organic Exciton-Polariton Condensates.

Exciton-polariton condensation in organic materials, arising from the coupling of Frenkel excitons to the electromagnetic field in cavities, is a phenomenon resulting in low-threshold coherent light emission among other fascinating properties. The exact mechanisms leading to the thermalization of organic exciton-polaritons toward condensation are not yet understood, partly due to the complexity of organic molecules and partly to the canonical microcavities used in condensation studies, which limit broadband studies. Here, we exploit an entirely different cavity design, i.

Observation of Nanoparticle Exsolution from Perovskite Oxides: From Atomic Scale Mechanistic Insight to Nanostructure Tailoring.

Understanding and controlling the formation of nanoparticles at the surface of functional oxide supports is critical for tuning activity and stability for catalytic and energy conversion applications. Here, we use a latest generation environmental transmission electron microscope to follow the exsolution of individual nanoparticles at the surface of perovskite oxides, with ultrahigh spatial and temporal resolution. Qualitative and quantitative analysis of the data reveals the atomic scale processes that underpin the formation of the socketed, strain-inducing interface that confers exsolved particles their exceptional stability and reactivity.

Tunable plasmonic HfN nanoparticles and arrays.

We present the fabrication of tunable plasmonic hafnium nitride (HfN) nanoparticles. HfN is a metallic refractory material with the potential of supporting plasmon resonances in the visible range, similar to silver and gold, but with the additional benefits of high melting point, chemical stability, and mechanical hardness. However, the preparation of HfN nanoparticles and the experimental demonstration of their plasmonic potential are still in their infancy.

Solar Hydrogen Generation from Ambient Humidity Using Functionalized Porous Photoanodes.

Solar hydrogen is a promising sustainable energy vector, and steady progress has been made in the development of photoelectrochemical (PEC) cells. Most research in this field has focused on using acidic or alkaline liquid electrolytes for ionic transfer. However, the performance is limited by (i) scattering of light and blocking of catalytic sites by gas bubbles and (ii) mass transport limitations.

Electrochemistry of Sputtered Hematite Photoanodes: A Comparison of Metallic DC versus Reactive RF Sputtering.

The water splitting activity of hematite is sensitive to the film processing parameters due to limiting factors such as a short hole diffusion length, slow oxygen evolution kinetics, and poor light absorptivity. In this work, we use direct current (DC) magnetron sputtering as a fast and cost-effective route to deposit metallic iron thin films, which are annealed in air to obtain well-adhering hematite thin films on F:SnO-coated glass substrates. These films are compared to annealed hematite films, which are deposited by reactive radio frequency (RF) magnetron sputtering, which is usually used for depositing metal oxide thin films, but displays an order of magnitude lower deposition rate.

Super-resolution Mapping of Enhanced Emission by Collective Plasmonic Resonances.

Plasmonic particle arrays have remarkable optical properties originating from their collective behavior, which results in resonances with narrow line widths and enhanced electric fields extending far into the surrounding medium. Such resonances can be exploited for applications in strong light-matter coupling, sensing, light harvesting, nonlinear nanophotonics, lasing, and solid-state lighting. However, as the lattice constants associated with plasmonic particle arrays are on the order of their resonance wavelengths, mapping the interaction between point dipoles and plasmonic particle arrays cannot be done with diffraction-limited methods.

High and intermediate temperature sodium-sulfur batteries for energy storage: development, challenges and perspectives.

In view of the burgeoning demand for energy storage stemming largely from the growing renewable energy sector, the prospects of high (>300 °C), intermediate (100-200 °C) and room temperature (25-60 °C) battery systems are encouraging. Metal sulfur batteries are an attractive choice since the sulfur cathode is abundant and offers an extremely high theoretical capacity of 1672 mA h g upon complete discharge. Sodium also has high natural abundance and a respectable electrochemical reduction potential (-2.

Why does NiOOH cocatalyst increase the oxygen evolution activity of α-FeO?

Nickel oxyhydroxide (NiOOH) is known to increase the oxygen evolution reaction (OER) performance of hematite (FeO) photoanodes. In recent experimental studies, it has been reported that the increased OER activity is related to the activation of the hematite (α-FeO) surface by NiOOH rather than the activity of NiOOH itself. In this study, we investigate the reason behind the higher activity and the low overpotentials for NiOOH-FeO photoanodes using first principles calculations.

Nonlinear Emission of Molecular Ensembles Strongly Coupled to Plasmonic Lattices with Structural Imperfections.

We demonstrate nonlinear emission from molecular layers strongly coupled to extended light fields in arrays of plasmonic nanoparticles in the presence of structural imperfections. Hybrid light-matter states, known as plasmon-exciton polaritons (PEPs), are formed by the strong coupling of Frenkel excitons in molecules to surface lattice resonances. These resonances result from the radiative coupling of localized surface plasmon polaritons in silver nanoparticles enhanced by diffraction on the array.

Quantifying Photothermal and Hot Charge Carrier Effects in Plasmon-Driven Nanoparticle Syntheses.

The excitation of localized surface plasmon resonances in Au and Ag colloids can be used to drive the synthesis of complex nanostructures, such as anisotropic prisms, bipyramids, and core@shell nanoparticles. Yet, after two decades of research, it is challenging to paint a complete picture of the mechanisms driving such light-induced chemical transformations. In particular, whereas the injection of hot charge carriers from the metal nanoparticles is usually proposed as the dominant mechanism, the contribution of plasmon-induced heating can often not be neglected.

Enhanced electrochemical water oxidation: the impact of nanoclusters and nanocavities.

The structures of transition metal surfaces and metal oxides are commonly believed to have a significant effect on the catalytic reactions. Density functional theory calculations are therefore used in this study to investigate the oxygen evolution reaction (OER) over nanostructured, i.e.

Secondary Electron Emission Materials for Transmission Dynodes in Novel Photomultipliers: A Review.

Secondary electron emission materials are reviewed with the aim of providing guidelines for the future development of novel transmission dynodes. Materials with reflection secondary electron yield higher than three and transmission secondary electron yield higher than one are tabulated for easy reference. Generations of transmission dynodes are listed in the order of the invention time with a special focus on the most recent atomic-layer-deposition synthesized transmission dynodes.

Multi-chromatic silicon nanocrystals.

Silicon nanocrystals (SiNCs) have great potential to become environmental friendly alternatives to heavy-metal containing nanocrystals for applications including medical imaging, lighting and displays. SiNCs exhibit excellent photostability, non-toxicity and abundant resources, but their often reported inefficient and spectrally limited light emission seriously impair their applications. Here we demonstrate a new method that converts SiNCs into an efficient and robust multi-chromatic phosphor.

High-Efficiency Nanowire Solar Cells with Omnidirectionally Enhanced Absorption Due to Self-Aligned Indium-Tin-Oxide Mie Scatterers.

Photovoltaic cells based on arrays of semiconductor nanowires promise efficiencies comparable or even better than their planar counterparts with much less material. One reason for the high efficiencies is their large absorption cross section, but until recently the photocurrent has been limited to less than 70% of the theoretical maximum. Here we enhance the absorption in indium phosphide (InP) nanowire solar cells by employing broadband forward scattering of self-aligned nanoparticles on top of the transparent top contact layer.

Layer-by-Layer Assembled Films of Perylene Diimide- and Squaraine-Containing Metal-Organic Framework-like Materials: Solar Energy Capture and Directional Energy Transfer.

We demonstrate that thin films of metal-organic framework (MOF)-like materials, containing two perylenediimides (PDICl4, PDIOPh2) and a squaraine dye (S1), can be fabricated by layer-by-layer assembly (LbL). Interestingly, these LbL films absorb across the visible light region (400-750 nm) and facilitate directional energy transfer. Due to the high spectral overlap and oriented transition dipole moments of the donor (PDICl4 and PDIOPh2) and acceptor (S1) components, directional long-range energy transfer from the bluest to reddest absorber was successfully demonstrated in the multicomponent MOF-like films.

Analysis of temporal evolution of quantum dot surface chemistry by surface-enhanced Raman scattering.

Temporal evolution of surface chemistry during oxidation of silicon quantum dot (Si-QD) surfaces were probed using surface-enhanced Raman scattering (SERS). A monolayer of hydrogen and chlorine terminated plasma-synthesized Si-QDs were spin-coated on silver oxide thin films. A clearly enhanced signal of surface modes, including Si-Clx and Si-Hx modes were observed from as-synthesized Si-QDs as a result of the plasmonic enhancement of the Raman signal at Si-QD/silver oxide interface.

Effect of ionic strength on intra-protein electron transfer reactions: The case study of charge recombination within the bacterial reaction center.

It is a common believe that intra-protein electron transfer (ET) involving reactants and products that are overall electroneutral are not influenced by the ions of the surrounding solution. The results presented here show an electrostatic coupling between the ionic atmosphere surrounding a membrane protein (the reaction center (RC) from the photosynthetic bacterium Rhodobacter sphaeroides) and two very different intra-protein ET processes taking place within it. Specifically we have studied the effect of salt concentration on: i) the kinetics of the charge recombination between the reduced primary quinone acceptor QA(-) and the primary photoxidized donor P(+); ii) the thermodynamic equilibrium (QA(-)↔QB(-)) for the ET between QA(-) and the secondary quinone acceptor QB.

Modeling and Simulations in Photoelectrochemical Water Oxidation: From Single Level to Multiscale Modeling.

This review summarizes recent developments, challenges, and strategies in the field of modeling and simulations of photoelectrochemical (PEC) water oxidation. We focus on water splitting by metal-oxide semiconductors and discuss topics such as theoretical calculations of light absorption, band gap/band edge, charge transport, and electrochemical reactions at the electrode-electrolyte interface. In particular, we review the mechanisms of the oxygen evolution reaction, strategies to lower overpotential, and computational methods applied to PEC systems with particular focus on multiscale modeling.

Reconstructing solute-induced phase transformations within individual nanocrystals.

Strain and defects can significantly impact the performance of functional nanomaterials. This effect is well exemplified by energy storage systems, in which structural changes such as volume expansion and defect generation govern the phase transformations associated with charging and discharging. The rational design of next-generation storage materials therefore depends crucially on understanding the correlation between the structure of individual nanoparticles and their solute uptake and release.

Phase-locking of magnetic islands diagnosed by ECE-imaging.

Millimeter-wave imaging diagnostics identify phase-locking and the satisfaction of 3-wave coupling selection criteria among multiple magnetic island chains by providing a localized, internal measurement of the 2D power spectral density, S(ω, kpol). In high-confinement tokamak discharges, these interactions impact both plasma rotation and tearing stability. Nonlinear coupling among neoclassical tearing modes of different n-number, with islands not satisfying the poloidal mode number selection criterion ⟨m, m('), m - m(')⟩, contributes to a reduction in core rotation and flow shear in the vicinity of the modes.