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The local environment of metal-oxide supported single-atom catalysts plays a decisive role in the surface reactivity and related catalytic properties. The study of such systems is complicated by the presence of point defects on the surface, which are often associated with the localization of excess charge in the form of polarons. This can affect the stability, the electronic configuration, and the local geometry of the adsorbed adatoms. In this work, through the use of density functional theory and surface-sensitive experiments, we study the adsorption of Rh1, Pt1, and Au1 metals on the reduced TiO2(110) surface, a prototypical polaronic material. A systematic analysis of the adsorption configurations and oxidation states of the adsorbed metals reveals different types of couplings between adsorbates and polarons. As confirmed by scanning tunneling microscopy measurements, the favored Pt1 and Au1 adsorption at oxygen vacancy sites is associated with a strong electronic charge transfer from polaronic states to adatom orbitals, which results in a reduction of the adsorbed metal. In contrast, the Rh1 adatoms interact weakly with the excess charge, which leaves the polarons largely unaffected. Our results show that an accurate understanding of the properties of single-atom catalysts on oxide surfaces requires a careful account of the interplay between adatoms, vacancy sites, and polarons.

Motile bacteria detect ambient chemical gradients and control their locomotion via conserved chemotaxis signaling networks, enabling cells to locate nutrients, potential hosts and other important biological niches. The sensory apparatus of the chemotaxis pathway is an array of core-signaling units (CSU) composed of transmembrane chemoreceptors, the histidine kinase CheA and an adaptor protein CheW. Although chemotaxis pathways represent the best understood signaling systems, a detailed mechanistic understanding of signal transduction has been hindered by the lack of a complete structural picture of the CSU and extended array. In this study, we present the structure of the complete CSU from phage E-gene lysedE. colicells, determined using cryo-electron tomography and sub-tomogram averaging to 12 Å resolution. Using AlphaFold2, we further predict the atomic structures of the CSU’s constituent proteins as well as key protein-protein interfaces, enabling the assembly an all-atom CSU model, which we conformationally refine using our cryoET map. Molecular dynamics simulations of the resulting model provide new insight into the periplasmic organization of the complex, including novel interactions between neighboring receptor ligand binding domains. Our results further elucidate previously unresolved interactions between individual CheA domains, including an anti-parallel P1 dimer and non-productive binding mode between P1 and P4, enhancing our understanding of the structural mechanisms underlying CheA signaling and regulation.

Oxide-supported single-atom catalysts are commonly modelled as a metal atom substituting surface cation sites in a low-index surface. Adatoms with dangling bonds will inevitably coordinate molecules from the gas phase, and adsorbates such as water can affect both stability and catalytic activity. Here, we use scanning tunneling microscopy (STM), noncontact atomic force microscopy (ncAFM), and x-ray photoelectron spectroscopy (XPS) to show that high densities of single Rh adatoms are stabilized on alpha-Fe2O3(1-102) in the presence of 2x10^(-8) mbar of water at room temperature, in marked contrast to the rapid sintering observed under UHV conditions. Annealing to 50 {\deg}C in UHV desorbs all water from the substrate leaving only the OH groups coordinated to Rh, and high-resolution ncAFM images provide a direct view into the internal structure. We provide direct evidence of the importance of OH ligands in the stability of single atoms, and argue that their presence should be assumed when modelling SAC systems.

In isotropic environments, an Escherichia coli cell exhibits coordinated rotational switching of its flagellar motors, produced by fluctuations in the intracellular concentration of phosphorylated CheY (CheY-P) emanating from chemoreceptor signaling arrays. In this study, we show that these CheY-P fluctuations arise through modifications of chemoreceptors by two sensory adaptation enzymes: the methyltransferase CheR and the methylesterase CheB. A cell containing CheR, CheB, and the serine chemoreceptor Tsr exhibited motor synchrony, whereas a cell lacking CheR and CheB or containing enzymatically inactive forms did not. Tsr variants with different combinations of methylation-mimicking Q residues at the adaptation sites also failed to show coordinated motor switching in cells lacking CheR and CheB. Cells containing CheR, CheB, and Tsr [NDND], a variant in which the adaptation site residues are not substrates for CheR or CheB modifications, also lacked motor synchrony. TsrΔNWETF, which lacks a C-terminal pentapeptide-binding site for CheR and CheB, and the ribose-galactose receptor Trg, which natively lacks this motif, failed to produce coordinated motor switching, despite the presence of CheR and CheB. However, addition of the NWETF sequence to Trg enabled Trg-NWETF to produce motor synchrony, as the sole receptor type in cells containing CheR and CheB. Finally, CheBc, the catalytic domain of CheB, supported motor coordination in combination with CheR and Tsr. These results indicate that the coordination of motor switching requires CheR/CheB-mediated changes in receptor modification state. We conclude that the opposing receptor substrate-site preferences of CheR and CheB produce spontaneous blinking of the chemoreceptor array’s output activity. IMPORTANCE Under steady-state conditions with no external stimuli, an Escherichia coli cell coordinately switches the rotational direction of its flagellar motors. Here, we demonstrate that the CheR and CheB enzymes of the chemoreceptor sensory adaptation system mediate this coordination. Stochastic fluctuations in receptor adaptation states trigger changes in signal output from the receptor array, and this array blinking generates fluctuations in CheY-P concentration that coordinate directional switching of the flagellar motors. Thus, in the absence of chemoeffector gradients, the sensory adaptation system controls run-tumble swimming of the cell, its optimal foraging strategy.

Dynamic properties of allosteric complexes are crucial for cellular information processing. However, direct observations of allosteric switches have been limited to compact molecular assemblies. Here, we reportin vivoFRET measurements of spontaneous discrete-level fluctuations in the activity of theEscherichia colichemosensory array — an extensive membrane-associated assembly comprising thousands of molecules. Finite-size scaling analysis of the temporal statistics by a two-dimensional conformational spread model revealed nearest-neighbor coupling strengths within 3% of the Ising second-order phase transition, indicating that chemosensory arrays are poised at criticality. Our analysis yields estimates for the intrinsic timescale of conformational changes (~ 10 ms) of allosteric units, and identifies near-critical tuning as a design principle for balancing the inherent tradeoff between response amplitude and response speed in higher-order signaling assemblies.One-setence summaryIn vivomeasurements of protein signaling array fluctuations reveal an allosteric system poised at criticality.

Polarizable materials attract attention in catalysis because they have a free parameter for tuning chemical reactivity. Their surfaces entangle the dielectric polarization with surface polarity, excess charge, and orbital hybridization. How this affects individual adsorbed molecules is shown for the incipient ferroelectric perovskite KTaO

The spatial distribution and magnitude of snowfall resulting from cloud seeding with silver iodide (AgI) is closely linked to atmospheric conditions, seeding operations, and dynamical, thermodynamical, and microphysical processes. Here, microphysical processes leading to ice and snow production are analyzed in orographic clouds for three cloud-seeding events, each with light or no natural precipitation and well-defined, traceable seeding lines. Airborne and ground-based radar observations are linked to in situ cloud and precipitation measurements to determine the spatiotemporal evolution of ice initiation, particle growth, and snow fallout in seeded clouds. These processes and surface snow amounts are explored as particle plumes evolve from varying amounts of AgI released, and within changing environmental conditions, including changes in liquid water content (LWC) along and downwind of the seeding track, wind speed, and shear. More AgI did not necessarily produce more liquid equivalent snowfall (LESnow). The greatest amount of LESnow, largest area covered by snowfall, and highest peak snowfall produced through seeding occurred on the day with the largest and most widespread occurrence of supercooled drizzle, highest wind shear, and greater LWC along and downwind of the seeding track. The day with the least supercooled drizzle and the lowest LWC downwind of the seeding track produced the smallest amount of LESnow through seeding. The stronger the wind was, the farther away the snowfall occurred from the seeding track.

The chemotaxis machinery of

The chemotaxis machinery of Escherichia coli has served as a model for exploring the molecular signaling mechanisms of transmembrane chemoreceptors known as methyl-accepting chemotaxis proteins (MCPs). Yet, fundamental questions about signal transmission through MCP molecules remain unanswered. Our work with the E. coli serine chemoreceptor Tsr has developed in vivo reporters that distinguish kinase-OFF and kinase-ON structures in the cytoplasmic methylation helix (MH) cap, which receives stimulus signals from an adjoining, membrane-proximal histidine kinase, adenylyl cyclases, MCPs, and phosphatases (HAMP) domain. The cytoplasmic helices of the Tsr homodimer interact mainly through packing interactions of hydrophobic residues at a and d heptad positions. We investigated the in vivo crosslinking properties of Tsr molecules bearing cysteine replacements at functionally tolerant g heptad positions in the N-terminal and C-terminal cap helices. Upon treatment of cells with bismaleimidoethane (BMOE), a bifunctional thiol-reagent, Tsr-G273C/Q504C readily formed a doubly crosslinked product in the presence of serine but not in its absence. Moreover, a serine stimulus combined with BMOE treatment during in vivo Förster resonance energy transfer–based kinase assays locked Tsr-G273C/Q504C in kinase-OFF output. An OFF-shifting lesion in MH1 (D269P) promoted the formation of the doubly crosslinked species in the absence of serine, whereas an ON-shifting lesion (G268P) suppressed the formation of the doubly crosslinked species. Tsr-G273C/Q504C also showed output-dependent crosslinking patterns in combination with ON-shifting and OFF-shifting adaptational modifications. Our results are consistent with a helix breathing-axial rotation-bundle repacking signaling mechanism and imply that in vivo crosslinking tools could serve to probe helix-packing transitions and their output consequences in other regions of the receptor molecule.

Modeling single-atom reactivity Noble metals often perform best for demanding reactions such as oxygen reduction, an effect often explained by the position of their d-band. One way to minimize the cost of noble metals is to disperse them as single atoms. To model the reactivity of supported single atoms, Hulva et al. evaporated different transition metals such as nickel, silver, and iridium on an Fe 3 O 4 (001) support. Single atoms adsorbed in the same twofold site between underlying rows of surface iron atoms. In studies of CO adsorption as a proxy for reactivity, the d-band was strongly affected by the charge transfer to the support and CO-induced structural changes. These effects can weaken the adsorption energy compared with the expected values based on electronic structure alone. Science , this issue p. 375

Heterogeneous catalysts based on subnanometer metal clusters often exhibit strongly size-dependent properties, and the addition or removal of a single atom can make all the difference. Identifying the most active species and deciphering the reaction mechanism is extremely difficult, however, because it is often not clear how the catalyst evolves in operando. Here, we use a combination of atomically resolved scanning probe microscopies, spectroscopic techniques, and density functional theory (DFT)-based calculations to study CO oxidation by a model Pt/Fe

Difficulties associated with the integration of liquids into a UHV environment make surface-science style studies of mineral dissolution particularly challenging. Recently, we developed a novel experimental setup for the UHV-compatible dosing of ultrapure liquid water, and studied its interaction with TiO2 and Fe3O4 surfaces. Here, we describe a simple approach to vary the pH through the partial pressure of CO2 (pCO2) in the surrounding vacuum chamber, and use this to study how these surfaces react to an acidic solution. The TiO2(110) surface is unaffected by the acidic solution, except for a small amount of carbonaceous contamination. The Fe3O4(001)-(rt2 x rt2)R45 surface begins to dissolve at a pH 4.0-3.9 (pCO2 = 0.8-1 bar) and, although it is significantly roughened, the atomic-scale structure of the Fe3O4(001) surface layer remains visible in scanning tunneling microscopy (STM) images. X-ray photoelectron spectroscopy (XPS) reveals that the surface is chemically reduced, and contains a significant accumulation of bicarbonate (HCO3-) species. These observations are consistent with Fe(II) being extracted by bicarbonate ions, leading to dissolved iron bicarbonate complexes (Fe(HCO3)2), which precipitate onto the surface when the water evaporates.

Hematite (α-Fe2O3) is one of the most investigated anode materials for photoelectrochemical water splitting. Its efficiency improves by doping with Ti, but the underlying mechanisms are not understood. One hurdle is separating the influence of doping on conductivity, surface states, and morphology, which all affect performance. To address this complexity, one needs well-defined model systems. We build such a model system by growing single-crystalline, atomically flat Ti-doped α-Fe2O3(1102) films by pulsed laser deposition (PLD). We characterize their surfaces, combining in situ scanning tunneling microscopy (STM) with density functional theory (DFT), and reveal how dilute Ti impurities modify the atomic-scale structure of the surface as a function of the oxygen chemical potential and Ti content. Ti preferentially substitutes subsurface Fe and causes a local restructuring of the topmost surface layers. Based on the experimental quantification of Ti-induced surface modifications and the structural model we have established, we propose a strategy that can be used to separate the effects of Ti-induced modifications to the surface atomic and electronic structures and bulk conductivity on the reactivity of Ti-doped hematite.

Cloud seeding has been used as one water management strategy to overcome the increasing demand for water despite decades of inconclusive results on the efficacy of cloud seeding. In this study snowfall accumulation from glaciogenic cloud seeding is quantified based on snow gauge and radar observations from three days in January 2017, when orographic clouds in the absent of natural precipitation were seeded with silver iodide (AgI) in the Payette basin of Idaho during the Seeded and Natural Orographic Wintertime Clouds: The Idaho Experiment (SNOWIE). On each day, a seeding aircraft equipped with AgI flares flew back and forth on a straight-line flight track producing a zig-zag pattern representing two to eight lines of clouds visible through enhancements in radar reflectivity. As these seeding lines started to form precipitation, they passed over several snow gauges and through the radar observational domain. For the three cases presented here, precipitation gauges measured increases between 0.05-0.3 mm as precipitation generated by cloud seeding pass over the instruments. A variety of relationships between radar reflectivity factor and liquid equivalent snowfall rate were used to quantify snowfall within the radar observation domain. For the three cases, snowfall occurred within the radar observational domain between 25 -160 min producing a total amount of water generated by cloud seeding ranging from 123,220 to 339,540 m3 using the best-match Ze-S relationship. Uncertainties in radar reflectivity estimated snowfall are provided by considering not only the best-match Ze-S relationship but also an ensemble of Ze-S relationships based on the range of coefficients published from previous studies and then examining the percentile of snowfall estimates based on all of the Ze-S relationships within the ensemble. Considering the interquartile range and 5th/95th percentiles, uncertainties in total amount of water generated by cloud seeding can range between 20-45% compared to the best-math estimates. These results provide new insights towards understanding how cloud seeding impacts precipitation and its distribution across a region.

The Escherichia coli chemoreceptor array is a supramolecular assembly that enables cells to respond to extracellular cues dynamically and with great precision and sensitivity. In the array, transmembrane receptors organized as trimers of dimers are connected at their cytoplasmic tips by hexameric rings of alternating subunits of the kinase CheA and the scaffolding protein CheW (CheA-CheW rings). Interactions of CheW molecules with the members of receptor trimers not directly bound to CheA-CheW rings may lead to the formation of hexameric CheW rings in the chemoreceptor array. Here, we detected such CheW rings with a cellular cysteine-directed cross-linking assay and explored the requirements for their formation and their participation in array assembly. We found that CheW ring formation varied with cellular CheW abundance, depended on the presence of receptors capable of a trimer-of-dimers arrangement, and did not require CheA. Cross-linking studies of a CheA~CheW fusion protein incapable of forming homomeric CheW oligomers demonstrated that CheW rings were not essential for the assembly of CheA-containing arrays. Förster resonance energy transfer (FRET)–based kinase assays of arrays containing variable amounts of CheW rings revealed that CheW rings enhanced the cooperativity and the sensitivity of the responses to attractants. We propose that six-membered CheW rings provide the additional interconnectivity required for optimal signaling and gradient tracking performance by chemosensory arrays.

Polarizable materials attract attention in catalysis because they have a free parameter for tuning chemical reactivity. Their surfaces entangle the dielectric polarization with surface polarity, excess charge, and orbital hybridization. How this affects individual adsorbed molecules is shown for the incipient ferroelectric perovskite KTaO 3 . This intrinsically polar material cleaves along (001) into KO- and TaO 2 -terminated surface domains. At TaO 2 terraces, the polarity-compensating excess electrons form a two-dimensional electron gas and can also localize by coupling to ferroelectric distortions. TaO 2 terraces host two distinct types of CO molecules, adsorbed at equivalent lattice sites but charged differently as seen in atomic force microscopy/scanning tunneling microscopy. Temperature-programmed desorption shows substantially stronger binding of the charged CO; in density functional theory calculations, the excess charge favors a bipolaronic configuration coupled to the CO. These results pinpoint how adsorption states couple to ferroelectric polarization.

Oxygen exchange at oxide/liquid and oxide/gas interfaces is important in technology and environmental studies, as it is closely linked to both catalytic activity and material degradation. The atomic-scale details are mostly unknown, however, and are often ascribed to poorly defined defects in the crystal lattice. Here we show that even thermodynamically stable, well-ordered surfaces can be surprisingly reactive. Specifically, we show that all the 3-fold coordinated lattice oxygen atoms on a defect-free single-crystalline “r-cut” (\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$1\bar{1}02$$\end{document}11¯02) surface of hematite (α-Fe2O3) are exchanged with oxygen from surrounding water vapor within minutes at temperatures below 70 °C, while the atomic-scale surface structure is unperturbed by the process. A similar behavior is observed after liquid-water exposure, but the experimental data clearly show most of the exchange happens during desorption of the final monolayer, not during immersion. Density functional theory computations show that the exchange can happen during on-surface diffusion, where the cost of the lattice oxygen extraction is compensated by the stability of an HO-HOH-OH complex. Such insights into lattice oxygen stability are highly relevant for many research fields ranging from catalysis and hydrogen production to geochemistry and paleoclimatology., Knowing how individual water molecules interact with surfaces is crucial for understanding surface and interface phenomena. Here, the authors show how local water-water interactions enable an unforeseen and surprisingly rapid mechanism of atom exchange between a common mineral and its surroundings.

International audience; This report describes the final results of the fourth phase of IEA TCP Wind Task 29. The project period of this fourth phase was from January 1 st 2018 until December 31 st 2020. It was the follow-up of three former IEA Task 29 phases (often denoted as Mexnext-I to Mexnext-III). In all phases wind turbine aerodynamic models were validated and improved with detailed aerodynamic measurements. In these detailed aerodynamic experiments pressure distributions at different locations along the rotor blades are measured anyhow where measurements of e.g. inflow velocities and boundary layer transition are very nice to know. The first three phases were mainly built around wind tunnel measurements on a small scale wind turbine with rotor diameter of 4.5 meter from the (New) Mexico project but the present phase was built around field measurements from the DanAero experiment.This DanAero experiment was carried out at atmospheric field conditions on a 2MW turbine by Danish Technical University DTU and 4 industrial partners (LM Glassfiber, Siemens WindPower, Vestas and Dong Energy) in 2 periods from 2007 until 2010 and from 2010 until 2013. Amongst others surface pressures and inflow velocities were measured at four sections along a blade and a row of surface flush mounted microphones was installed at the outer part ofthe blade. In IEA Task29 Phase IV the DanAero data were made available to the IEA Task 29 participants which enabled a detailed analysis in a collaborative action. Amongst others a critical scrutinising of data took place with subsequent further improvement of measurement quality. Moreover the measurements were used as validation material for the many design models which are available in the consortium. A wide variety of models could be considered ranging from high fidelity (but time consuming) CFD to lower fidelity but efficient engineering models. Intermediate methods (e.g. free wake methods) were applied as well. Several calculational rounds were carried out where calculations were compared with measurements. Amongst others a case was defined at simple steady and axi-symmetric conditions close to a measurement case with little shear and little yaw but also measurement cases at high yaw and high shear were simulated. Moreover the level of detail from the DanAero experiment allowed an in-depth analysis of several wind turbine aerodynamic aspects, e.g. Aerodynamic response to turbulent inflow; Sheared inflow; 2D/3D aerodynamics;Aeroelastic effectsTransition characteristics in realistic flow conditions;Acoustics. The project was carried out by a consortium which consisted of research groups and industries from 9 different countries China: Chinese Wind Energy Association, CWEA Denmark: Technical University of Denmark, DTU, Siemens-Gamesa Renewable Energy France: IFPEn, LHEEA lab - Centrale Nantes/CNRS, ONERA, EDFGermany: ForWind/Fraunhofer IWES, Kiel University of Applied Sciences, University of Stuttgart, WindNovation, Enercon Deutsches Zentrum für Luft- und Raumfahrt e.V., DLR University of Applied Sciences EmdenItaly: PoliMi, RSE, CNR - INMNetherlands: TNO Energy Transition (formerly ECN, Operating Agent), Delft University of Technology, TUDelft, DNV-GL Suzlon Blade Technology, SBT, CWI, LM and University of Twente, UTwenteItaly: PoliMi, RSE, CNR - INMSweden: Uppsala University, Campus GotlandSwitzerland: UAS RapperswilUSA: National Renewable Energy Laboratory, NREL

This paper reviews research conducted over the last six decades to understand and quantify the efficacy of wintertime orographic cloud seeding to increase winter snowpack and water supplies within a mountain basin. The fundamental hypothesis underlying cloud seeding as a method to enhance precipitation from wintertime orographic cloud systems is that a cloud’s natural precipitation efficiency can be enhanced by converting supercooled water to ice upstream and over a mountain range in such a manner that newly created ice particles can grow and fall to the ground as additional snow on a specified target area. The review summarizes the results of physical, statistical, and modeling studies aimed at evaluating this underlying hypothesis, with a focus on results from more recent experiments that take advantage of modern instrumentation and advanced computation capabilities. Recent advances in assessment and operations are also reviewed, and recommendations for future experiments, based on the successes and failures of experiments of the past, are given.

Motile Escherichia coli cells use chemoreceptor signaling arrays to track chemical gradients with exquisite precision. Highly conserved residues in the cytoplasmic hairpin tip of chemoreceptor molecules promote assembly of trimer-based signaling complexes and modulate the activity of their CheA kinase partners. To explore hairpin tip output states in the serine receptor Tsr, we characterized the signaling consequences of amino acid replacements at the salt-bridge residue pair E385-R388. All mutant receptors assembled trimers and signaling complexes, but most failed to support serine chemotaxis in soft agar assays. Small side-chain replacements at either residue produced OFF- or ON-shifted outputs that responded to serine stimuli in wild-type fashion, suggesting that these receptors, like the wild-type, operate as two-state signaling devices. Larger aliphatic or aromatic side chains caused slow or partial kinase control responses that proved dependent on the connections between core signaling units that promote array cooperativity. In a mutant lacking one of two key adapter-kinase contacts (interface 2), those mutant receptors exhibited more wild-type behaviors. Lastly, mutant receptors with charged amino acid replacements assembled signaling complexes that were locked in kinase-ON (E385K|R) or kinase-OFF (R388D|E) output. The hairpin tips of mutant receptors with these more aberrant signaling properties probably have nonnative structures or dynamic behaviors. Our results suggest that chemoeffector stimuli and adaptational modifications influence the cooperative connections between core signaling units. This array remodeling process may involve activity-dependent changes in the relative strengths of interface 1 and 2 interactions between the CheW and CheA.P5 components of receptor core signaling complexes.

The high specific activity and cost-effectiveness of single-atom catalysts (SACs) hold great promise for numerous catalytic chemistries. In hydrogenation reactions, the mechanisms of critical steps...

The transport of H adatoms across oxide supports plays an important role in many catalytic reactions. We investigate the dynamics of H/Fe3O4(001) between 295 and 382 K. By scanning tunneling microscopy at frame rates of up to 19.6 fps, we observe the thermally activated switching of H between two O atoms on neighboring Fe rows. This switching rate changes in proximity to a defect, explained by density functional theory as a distortion in the Fe-O lattice shortening the diffusion path. Quantitative analysis yields an apparent activation barrier of 0.94 +/- 0.07 eV on a pristine surface. The present work highlights the importance of local techniques in the study of atomic-scale dynamics at defective surfaces such as oxide supports.

We studied how nickel doping affects water adsorption at the Fe3O4(001) surface to understand the enhanced performance of spinel ferrites for the water-gas shift and oxygen evolution reactions. Two different configurations were prepared: 2-fold-coordinated Ni adatoms on top of the surface and Ni atoms incorporated into the octahedral sites of the support. Using temperature-programmed desorption, X-ray photoemission spectroscopy, and scanning tunneling microscopy, we show that water is adsorbed and dissociated on the nickel adatoms at room temperature, resulting in Ni–OH species and surface hydroxyl groups. Nickel atoms incorporated into the support do not directly adsorb water but modify the electronic properties of the surface Fe, and water adsorbed on these sites has similar characteristics as that of water adsorbed on intrinsic surface defects. In both cases, the presence of Ni significantly alters the growth of the first water monolayer on Fe3O4(001).

The interaction of water with the most prominent surfaces of Fe3O4, (001) and (111), is directly compared using a combination of temperature-programmed desorption, temperature-programmed low energy electron diffraction (TP LEED), and scanning probe microscopies. Adsorption on the (√2 × √2)R45°-reconstructed surface of Fe3O4(001) is strongly influenced by the surface reconstruction, which remains intact at all coverages. Close to the completion of the first monolayer, however, the ad-layer adopts a longer-range (2 × 2) superstructure. This finding is discussed in the context of a similar (2 × 2) superstructure recently observed on the (111) facet, which exists over a significantly larger range of temperatures and coverages. In both cases, the long-range order is evidence that water–water interactions exert a significant influence on the structure already prior to the nucleation of the second layer. We conclude that the stability differences stem from the smaller unit cell on the (111) surface, and the ability of water to more easily form stable hexagonal ice-like structures on the hexagonal substrate.

The oxygen evolution reaction (OER) is thought to occur via a four-step mechanism with *O, *OH, and *OOH as adsorbed intermediates. Linear scaling of the *OH and **OOH adsorption energies is proposed to limit the oxides’ efficiency as OER catalysts, but the use of simple descriptors to screen candidate materials neglects potentially important water–water interactions. Here, we use a combination of temperature-programmed desorption (TPD), X-ray photoemission spectroscopy (XPS), noncontact atomic force microscopy (nc-AFM), and density functional theory (DFT)-based computations to show that highly stable HO–H2O dimer species form at the (1102) facet of hematite; a promising anode material for photoelectrochemical water splitting. The UHV-based results are complemented by measurements following exposure to liquid water and are consistent with prior X-ray scattering results. The presence of strongly bound water agglomerates is generally not taken into account in OER reaction schemes but may play a role in det...

The Seeded and Natural Orographic Wintertime Clouds: The Idaho Experiment (SNOWIE) project aims to study the impacts of cloud seeding on winter orographic clouds. The field campaign took place in Idaho between 7 January and 17 March 2017 and employed a comprehensive suite of instrumentation, including ground-based radars and airborne sensors, to collect in situ and remotely sensed data in and around clouds containing supercooled liquid water before and after seeding with silver iodide aerosol particles. The seeding material was released primarily by an aircraft. It was hypothesized that the dispersal of the seeding material from aircraft would produce zigzag lines of silver iodide as it dispersed downwind. In several cases, unambiguous zigzag lines of reflectivity were detected by radar, and in situ measurements within these lines have been examined to determine the microphysical response of the cloud to seeding. The measurements from SNOWIE aim to address long-standing questions about the efficacy of cloud seeding, starting with documenting the physical chain of events following seeding. The data will also be used to evaluate and improve computer modeling parameterizations, including a new cloud-seeding parameterization designed to further evaluate and quantify the impacts of cloud seeding.

Iron oxides (FeOx) are among the most common support materials utilized in single atom catalysis. The support is nominally Fe2O3, but strongly reductive treatments are usually applied to activate the as-synthesized catalyst prior to use. Here, we study Rh adsorption and incorporation on the (1-102) surface of hematite ({\alpha}-Fe2O3), which switches from a stoichiometric (1x1) termination to a reduced (2x1) reconstruction in reducing conditions. Rh atoms form clusters at room temperature on both surface terminations, but Rh atoms incorporate into the support lattice as isolated atoms upon annealing above 400 {\deg}C. Under mildly oxidizing conditions, the incorporation process is so strongly favoured that even large Rh clusters containing hundreds of atoms dissolve into the surface. Based on a combination of low energy ion scattering and scanning tunnelling microscopy data, as well as density functional theory, we conclude that the Rh atoms are stabilized in the immediate subsurface, rather than the surface layer.