Abstract Plasmonic systems convert light into electrical charges and heat, mediating catalytic transformations. However, there is ongoing controversy regarding the involvement of hot carriers in process. In this study, we demonstrate direct utilisation plasmon electrons hydrogen evolution reaction with visible light. We intentionally assemble a plasmonic nanohybrid system comprising NiO/Au/[Co(1,10-Phenanthrolin-5-amine) 2 (H O) ], which unstable at water thermolysis temperatures. This...

An array of surface science measurements has revealed novel water adsorption behavior at the Fe(3)O(4)(001) surface. Following room temperature exposure to water, a low coverage hydrogen atoms is observed, with no associated hydroxyl group. Mild annealing hydrogenated leads desorption via abstraction oxygen atoms, leading reduction These results point an irreversible splitting molecule. The observed phenomena are discussed in context recent DFT calculations (Mulakaluri, N.; Pentcheva, R.;...

We present a Scanning Tunneling Microscopy (STM) investigation of gold deposited at the magnetite Fe3O4(001) surface room temperature. This forms reconstruction with (\surd2\times\surd2)R45{\deg} symmetry, where pairs Fe and neighboring O ions are slightly displaced laterally, forming undulating rows 'narrow' 'wide' adsorption sites. At fractional monolayer coverages, single Au adatoms adsorb exclusively narrow sites, no significant sintering up to annealing temperatures 400 {\deg}C. The...

A combination of Photoemission, Atomic Force and Scanning Tunneling Microscopy/Spectroscopy measurements shows that excess electrons in TiO2 anatase (101) surface are trapped at step edges. Consequently, steps act as preferred adsorption sites for O2. In Density Functional Theory calculations localize clean edges, this tendency is enhanced by O vacancies hydroxylation. The results show the importance defects wide-ranging applications titania.

Reduced terminations of the Fe${}_{3}$O${}_{4}$(001) surface were studied using scanning tunneling microscopy, x-ray photoelectron spectroscopy (XPS), and density functional theory (DFT). Fe atoms, deposited onto thermodynamically stable, distorted B-layer termination at room temperature (RT), occupy one two available tetrahedrally coordinated sites per ($\sqrt{2}\ifmmode\times\else\texttimes\fi{}\sqrt{2}$)$R$45\ifmmode^\circ\else\textdegree\fi{} unit cell. Further RT deposition results in...

The high specific activity and cost-effectiveness of single-atom catalysts (SACs) hold great promise for numerous catalytic chemistries. In hydrogenation reactions, the mechanisms critical steps such as hydrogen activation spillover are far from understood. Here, we employ a combination scanning tunneling microscopy density functional theory to demonstrate that on model SAC comprised single Pd atoms Fe3O4(001), H2 dissociates heterolytically between surface oxygen. efficient allows...

A new endstation to perform operando chemical analysis at solid-liquid interfaces by means of ambient pressure x-ray photoelectron spectroscopy (APXPS) is presented. The located the Swiss Light Source and can be attached soft in situ beamline (X07DB) for solid-gas type experiments a tender (PHOENIX I) interface experiments. setup consists three interconnected ultrahigh vacuum chambers: one sample preparation using surface science techniques, chamber APXPS experiments, an entry-lock transfer...

Antimony selenide (Sb2Se3) is an auspicious material for solar energy conversion that has seen rapid improvement over the past ten years, but photovoltage deficit remains a challenge. Here, simple and low-temperature treatments of p-n heterojunction interface Sb2Se3/TiO2-based photocathodes photoelectrochemical water splitting were explored to address this The FTO/Ti/Au/Sb2Se3 (substrate configuration) stack was treated with (NH4)2S as etching solution, followed by CuCl2 treatment prior...

The atomic-scale mechanisms underlying the growth of Ag on (√2×√2)R45°-Fe3O4(001) surface were studied using scanning tunneling microscopy and density functional theory based calculations. For coverages up to 0.5 ML, adatoms populate exclusively; agglomeration into nanoparticles occurs only with lifting reconstruction at 720 K. Above clusters nucleate spontaneously grow expense surrounding material mild annealing. This unusual behavior results from a kinetic barrier associated (√2×√2)R45°...

While loading of cocatalysts is one the most widely investigated strategies to promote efficiency photoelectrodes, understanding their functionality remains controversial. We established new hybrid molecular photoanodes with cobalt-based cubane on hematite as a model system. Photoelectrochemical and rate law analyses revealed an interesting transition {Co(II)4O4}-type cocatalysts. Their role changed from predominant hole reservoirs catalytic centers upon modulation applied bias. Kinetic...

Carbon contamination is a notorious issue that has an enormous influence on surface science experiments, especially in near-atmospheric conditions. While it often mentioned publications when affecting experiment’s results, more rarely analyzed detail. We performed ambient-pressure x-ray photoelectron spectroscopy experiments toward examining the build-up of adventitious carbon species (both inorganic and hydrocarbons) clean well-prepared using large-scale (50 × 10 mm2) rutile TiO2(110)...

Amorphous oxide thin films grown by thermal atomic layer deposition (ALD) typically contain high impurity concentrations of hydrogen, which affects both chemistry and structure thereby the functional properties, such as barrier properties in, for example, microelectronic photovoltaic devices. This study discloses effect H incorporation in amorphous Al 2 O 3 ALD on local chemical binding states Al, H, well density stoichiometry, a combined analytical approach using elastic recoil detection...

Graphene-like materials can be viewed as promising storage media for hydrogen they are lightweight, durable, and scalable. For practical use, doping is required to overcome the kinetic limitations diffusion recombination on surfaces due rehybridization of atoms. We studied synthesis nitrogen-doped graphene Ru(0001) by chemical vapor deposition (CVD) pyridine N-doping through ion irradiation. Using combination scanning tunneling microscopy (STM), x-ray photoelectron spectroscopy, density...

A detailed analysis of the N(1s) and C(1s) X-Ray Photoelectron Spectroscopy (XPS) is made, where measured XPS compared with theoretical Sudden Approximation (SA) intensities Binding Energies (BEs). There remarkably good agreement between predictions XPS; in particular, different full width at half maximum values for BEs are explained terms unresolved C atoms pyridine. This work demonstrates that combination theory measurements can extract relevant to molecular electronic structure. The used...

Antiphase domain boundaries (APDBs) in the $(\sqrt{2}\ifmmode\times\else\texttimes\fi{}\sqrt{2})R{45}^{\ensuremath{\circ}}$ reconstruction of Fe${}_{3}$O${}_{4}$(001) surface were investigated using scanning tunneling microscopy (STM) and density functional theory [(DFT) + $U$] calculations. The equilibrium structure APDBs is interpreted terms distorted $B$-layer model for which a lattice distortion couples to charge order subsurface layers. are observed after prolonged annealing at 700...

The interaction of water with oxide surfaces is great interest for both fundamental science and applications. We present a combined theoretical (density functional theory (DFT)) experimental (scanning tunneling microscopy (STM) photoemission spectroscopy (PES)) study the two-dimensional titania overlayer that terminates SrTiO3(110)-(4 × 1) surface consists TiO4 tetrahedra. STM core-level valence band PES show H2O neither adsorbs nor dissociates on stoichiometric at room temperature, whereas...

Carboxylic acids bind to titanium dioxide (TiO2) dissociatively, forming surface superstructures that give rise a (2 × 1) pattern detected by low-energy electron diffraction. Exposing this system water, however, leads loss of the highly ordered structure. The formate-covered was investigated combination diffraction and spectroscopy techniques, together with static dynamic ab initio simulations, conclusion equilibrium exists between adsorbed formic acid water molecules. This process is an...

Cuprous oxide ([Formula: see text]) is a promising material for photoelectrochemical energy conversion due to its small direct band gap, high absorbance, and Earth-abundant constituents. High efficiencies require transport of photoexcited charges the interface without loss. We studied electron dynamics in [Formula: text](111) by time-resolved two-photon photoemission different surface defect densities order elucidate influence on charge carrier transport. On pristine bulk terminated surface,...

Using time-lapsed ambient-pressure X-ray photoelectron spectroscopy, we investigate the thermal oxidation of single-crystalline Ir(100) films toward rutile IrO2(110) in situ. We initially observe formation a carbon-free surface covered with complete monolayer oxygen, based on binding energies Ir 4f and O 1s core level peaks. During rather long induction period nearly constant oxygen coverage, work function changes continuously as sensed by gas phase signal. The sudden rapid IrO2 thickness...

Combining electrochemical measurements with in situ and ex photoelectron spectroscopy simulations to detect the formation of cobalt oxyhydroxide during oxygen evolution reaction.

Abstract The thermal oxidation of Ru(0001) has been extensively studied in the surface science community to determine pathway towards ruthenium dioxide (RuO 2 (110)), improving knowledge chemistry. Using time-lapsed ambient-pressure x-ray photoelectron spectroscopy (APXPS), we investigate single-crystalline films toward rutile RuO (110) situ . APXPS spectra were continuously collected while exposed a fixed O partial pressure 10 −2 mbar and sample temperature was increased stepwise from room...

The interaction of CO with the Fe3O4(001)-(√2 × √2)R45° surface was studied using temperature-programmed desorption (TPD), scanning tunneling microscopy (STM), and X-ray photoelectron spectroscopy (XPS), latter both under ultrahigh vacuum (UHV) conditions in pressures up to 1 mbar. In general, CO–Fe3O4 is found be weak. strongest adsorption occurs at defects, leading small TPD peaks 115, 130, 190 K. Desorption from regular two distinct regimes. For coverages molecules per (√2 unit cell,...

Deposition of two-dimensional (2D) materials onto catalyst surfaces is known to alter the adsorption energies active sites due nanoconfinement effect. Traditionally, these 2D heterostructures were prepared by depositing a material pristine metallic surface. Preparing well-defined monolayers, instead, on metal-oxide challenging, although it possible via O2 intercalation oxidizing metal substrate underneath. Several studies demonstrate this intercalative behavior covers, however, without...