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Dependence of interface energetics and kinetics on catalyst loading in a photoelectrochemical system
Solar hydrogen production by the photoelectrochemical method promises a means to store solar energy. While it is generally understood that the process is highly sensitive to the nature of the interface between the semiconductor and the electrolyte, a detailed understanding of this interface is still missing. For instance, few prior studies have established a clear relationship between the interface energetics and the catalyst loading amount. Here we aim to study this relationship on a prototypical Si-based photoelectrochemical system. Two types of interfaces were examined, one with GaN nanowires as a protection layer and one without. It was found that when GaN was present, higher Pt loading (> 0.1 μg/cm 2 ) led to not only better water reduction (and, hence, hydrogen evolution) kinetics but also more favorable interface energetics for greater photovoltages. In the absence of the protection layer, by stark contrast, increased Pt loading exhibited no measurable influence on the interface energetics, and the main difference was observed only in the hydrogen evolution kinetics. Furthermore, the study sheds new light on the importance of interface engineering for further improvement of photoelectrochemical systems, especially concerning the role of catalysts and protection layers.
Simulations and Analysis of the Reshocked Inclined Interface Richtmyer–Meshkov Instability for Linear and Nonlinear Interface Perturbations
A computational study of the Richtmyer–Meshkov instability (RMI) is presented for an inclined interface perturbation in support of experiments being performed at the Texas A&M shock tube facility. The study is comprised of 2D, viscous, diffusive, compressible simulations performed using the arbitrary Lagrange Eulerian code, ARES, developed at Lawrence Livermore National Laboratory. These simulations were performed to late times after reshock with two initial interface perturbations, in the linear and nonlinear regimes each, prescribed by the interface inclination angle. The interaction of the interface with the reshock wave produced a complex 2D set of compressible wave interactions including expansion waves, which also interacted with the interface. Distinct differences in the interface growth rates prior to reshock were found in previous work. The current work provides in-depth analysis of the vorticity and enstrophy fields to elucidate the physics of reshock for the inclined interface RMI. After reshock, the two cases exhibit some similarities in integral measurements despite their disparate initial conditions but also show different vorticity decay trends, power law decay for the nonlinear and linear decay for the linear perturbation case.
Hidden Interface Driven Exchange Coupling in Oxide Heterostructures
A variety of emergent phenomena have been enabled by interface engineering in complex oxides. The existence of an intrinsic interfacial layer has often been found at oxide heterointerfaces. However, the role of such an interlayerin controlling functionalities is not fully explored. Here, we report the control of the exchange bias (EB) in single-phase manganite thin films with nominallyuniform chemical composition across the interfaces. The sign of EB depends on the magnitude of the cooling field. A pinned layer, confirmed by polarized neutron reflectometry, provides the source of unidirectional anisotropy. The origin of the exchange bias coupling is discussed in terms of magnetic interactions between the interfacial ferromagnetically reduced layer and the bulk ferromagnetic region. The sign of EB is related to the frustration of antiferromagnetic coupling between the ferromagnetic region and the pinned layer. Our results shed new light on using oxide interfaces to design functional spintronic devices.
A method for site-specific and cryogenic specimen fabrication of liquid/solid interfaces for atom probe tomography
A site-specific, cryogenic, focused ion beam (FIB) method is presented for the preparation of atom probe tomography (APT) specimens from a frozen liquid/solid interface. As a practical example, the interface between water and a corroded boroaluminosilicate glass has been characterized by APT for the first time. The water/glass interface is preserved throughout specimen preparation by plunge freezing the corroding glass particles with the corrosion solution into slush nitrogen. Site-specific specimen preparation is enabled through a new approach to extract and mount a small volume of material using a cryogenically cooled FIB stage and micromanipulator. The prepared APT specimens are subsequently transferred from the FIB to APT under cryogenic and high-vacuum conditions using a novel FIB/APT transfer shuttle and home-built environmental transfer hub attached to the APT system. Particular focus is given to the technical methods for specimen fabrication under cryogenic conditions. Persistent challenges are discussed in addition to future opportunities for this new specimen preparation method.
New Insights into Secondary Organic Aerosol Formation at the Air–Liquid Interface
Air-liquid interfacial processing of volatile organic compound oxidation has been suggested as an important source of secondary organic aerosols. However, owing to the lack of techniques for in situ air-liquid interface analysis, the detailed interfacial mechanism remains speculative. To obviate this, the analysis of air-liquid interfacial reactions and the dynamics of glyoxal oxidation as a model volatile organic compound using in situ liquid synchrotron-based vacuum ultraviolet single photon ionization mass spectrometry enabled by the system for analysis at the liquid vacuum interface microreactor is reported. This approach allows for determination of reaction intermediates and oxidation products including polymers and oligomers at the air-liquid interface by mass spectral analysis and appearance energy measurements. Furthermore, an expanded reaction mechanism of photooxidation free radical induced reactions as a source of aqueous secondary organic aerosol formation is proposed based on these new results, suggesting that single photon ionization could be applied to provide unique insights into interfacial chemistry changing the earth atmospheric composition.
Accelerated Cu2O Reduction by Single Pt Atoms at the Metal-Oxide Interface§
The reducibility of metal oxides, when serving as the catalyst support or the active sites themselves, plays an important role in heterogeneous catalytic reactions. Here we present an integrated experimental and theoretical study that reveals how the addition of small amounts of atomically dispersed Pt at the metal/oxide interface dramatically enhances the reducibility of a Cu2O thin film by H2. X-ray photoelectron spectroscopy (XPS) and temperature-programmed desorption (TPD) results reveal that upon oxidation, a PtCu single-atom alloy (SAA) surface is covered by a thin Cu2O film and is therefore unable to dissociate H2. Despite this, in situ studies using ambient pressure (AP) XPS reveal that the presence of a small amount of Pt under the oxide layer can, at the single-atom limit, promote the reduction of Cu2O by H2 at room temperature. We build two density functional theory based surface models to better understand these experimental findings: A Cu2O/Cu(111)-like surface oxide layer, known as the ‘29’ oxide, in which Pt is alloyed into the Cu(111) surface as well as a PtCu SAA. Our calculations suggest that the increased activity is due to the presence of atomically dispersed Pt under the surface oxide layer, which weakens the Cu-O bonds in its immediate vicinity, thus making the interface between subsurface Pt and the surface oxide a nucleation site for the formation of metallic Cu. This initial step in the reduction process results in the presence of surface Pt atoms surrounded by metallic Cu patches, and the Pt atoms become active in H2 dissociation, which consequently accelerates the reduction of the oxide layer. This work demonstrates how isolated Pt atoms at the metal/oxide interface of a Cu-based catalyst accelerate the reduction of the oxide and, therefore, helps maintain the active, reduced state of the catalyst under reaction conditions, as is required for the synthesis of methanol from CO2 hydrogenation.
PHIL Interface Design for Use With a Voltage-Regulated Amplifier
Power hardware-in-the-loop (PHIL) has emerged as a leading strategy to thoroughly assess the impact of proprietary inverter controls on a specific power system. The development of a PHIL test bed typically involves an inverter under test, a power amplifier, controllable DC supply, and a digital real-time simulator (DRTS) to simulate the power system under study. As a result of PHIL nonidealities, a form of digital compensation within the DRTS is used, which is commonly referred to as a PHIL interface. Many existing methods use legacy power amplifiers that do not contain internal voltage regulation. These existing interface methods are based around a voltage regulator within the DRTS and do not consider the interaction with the controls in newer amplifiers. In this study, a three-step approach of PHIL interface development for modern power amplifiers with built-in voltage regulation is introduced and is validated in hardware with a 30-kW grid-following inverter.
Discovering Reactant Supply Pathways at Electrode/PEM Reaction Interfaces Via a Tailored Interface-Visible Characterization Cell
In situ and micro-scale visualization of electrochemical reactions and multiphase transports on the interface of porous transport electrode (PTE) materials and solid polymer electrolyte (SPE) has been one of the greatest challenges for electrochemical energy conversion devices, such as proton exchange membrane electrolyzer cells (PEMECs), CO 2 reduction electrolyzers, PEM fuel cells, etc. Here, an interface-visible characterization cell (IV-CC) is developed to in situ visualize micro-scaled and rapid electrochemical reactions and transports in PTE/SPE interfaces. Taking the PEMEC of a green hydrogen generator as a study case, the unanticipated local gas blockage, micro water droplets, and their evolution processes are successfully visualized on PTE/PEM interfaces in a practical PEMEC device, indicating the existence of unconventional reactant supply pathways in PEMs. Further comprehensive results reveal that PEM water supplies to reaction interfaces are significantly impacted with current densities. Here these results provide critical insights about the reaction interface optimization and mass transport enhancement in various electrochemical energy conversion devices.
Accurate gradient approximation for complex interface problems in 3D by an improved coupling interface method
Most elliptic interface solvers become complicated for complex interface problems at those “exceptional points” where there are not enough neighboring interior points for high order interpolation. Such complication increases especially in three dimensions. Usually, the solvers are thus reduced to low order accuracy. In this paper, we classify these exceptional points and propose two recipes to maintain order of accuracy there, aiming at improving the previous coupling interface method [26]. Yet the idea is also applicable to other interface solvers. The main idea is to have at least first order approximations for second order derivatives at those exceptional points. Recipe 1 is to use the finite difference approximation for the second order derivatives at a nearby interior grid point, whenever this is possible. Recipe 2 is to flip domain signatures and introduce a ghost state so that a second-order method can be applied. This ghost state is a smooth extension of the solution at the exceptional point from the other side of the interface. The original state is recovered by a post-processing using nearby states and jump conditions. The choice of recipes is determined by a classification scheme of the exceptional points. The method renders the solution and its gradient uniformly second-order accurate in the entire computed domain. Numerical examples are provided to illustrate the second order accuracy of the presently proposed method in approximating the gradients of the original states for some complex interfaces which we had tested previous in two and three dimensions, and a real molecule ( (1D63)) which is double-helix shape and composed of hundreds of atoms.
Carrier lifetimes and interface recombination velocities in CdTe/Mg{sub x}Cd{sub 1−x}Te double heterostructures with different Mg compositions grown by molecular beam epitaxy
The interface recombination velocities of CdTe/Mg{sub x}Cd{sub 1−x}Te double heterostructure (DH) samples with different CdTe layer thicknesses and Mg compositions are studied using time-resolved photoluminescence measurements. A lowest interface recombination velocity of 30 ± 10 cm/s has been measured for the CdTe/Mg{sub 0.46}Cd{sub 0.54}Te interface, and a longest carrier lifetime of 0.83 μs has been observed for the studied DHs. These values are very close to the best reported numbers for GaAs/AlGaAs DHs. The impact of carrier escape through thermionic emission over the MgCdTe barrier on the recombination process in the DHs is also studied.
Quasi-two-dimensional electron gas at the interface of γ-Al{sub 2}O{sub 3}/SrTiO{sub 3} heterostructures grown by atomic layer deposition
We report the formation of a quasi-two-dimensional electron gas (2-DEG) at the interface of γ-Al{sub 2}O{sub 3}/TiO{sub 2}-terminated SrTiO{sub 3} (STO) grown by atomic layer deposition (ALD). The ALD growth of Al{sub 2}O{sub 3} on STO(001) single crystal substrates was performed at temperatures in the range of 200–345 °C. Trimethylaluminum and water were used as co-reactants. In situ reflection high energy electron diffraction, ex situ x-ray diffraction, and ex situ cross-sectional transmission electron microscopy were used to determine the crystallinity of the Al{sub 2}O{sub 3} films. As-deposited Al{sub 2}O{sub 3} films grown above 300 °C were crystalline with the γ-Al{sub 2}O{sub 3} phase. In situ x-ray photoelectron spectroscopy was used to characterize the Al{sub 2}O{sub 3}/STO interface, indicating that a Ti{sup 3+} feature in the Ti 2p spectrum of STO was formed after 2–3 ALD cycles of Al{sub 2}O{sub 3} at 345 °C and even after the exposure to trimethylaluminum alone at 300 and 345 °C. The interface quasi-2-DEG is metallic and exhibits mobility values of ∼4 and 3000 cm{sup 2} V{sup −1} s{sup −1} at room temperature and 15 K, respectively. The interfacial conductivity depended on the thickness of the Al{sub 2}O{sub 3} layer. The Ti{sup 3+} signal originated from the near-interfacial region and vanished after annealing in an oxygen environment.
The effect of atomic structure on interface spin-polarization of half-metallic spin valves: Co{sub 2}MnSi/Ag epitaxial interfaces
Using density functional theory calculations motivated by aberration-corrected electron microscopy, we show how the atomic structure of a fully epitaxial Co{sub 2}MnSi/Ag interfaces controls the local spin-polarization. The calculations show clear difference in spin-polarization at Fermi level between the two main types: bulk-like terminated Co/Ag and Mn-Si/Ag interfaces. Co/Ag interface spin-polarization switches sign from positive to negative, while in the case of Mn-Si/Ag, it is still positive but reduced. Cross-sectional atomic structure analysis of Co{sub 2}MnSi/Ag interface, part of a spin-valve device, shows that the interface is determined by an additional layer of either Co or Mn. The presence of an additional Mn layer induces weak inverse spin-polarisation (−7%), while additional Co layer makes the interface region strongly inversely spin-polarized (−73%). In addition, we show that Ag diffusion from the spacer into the Co{sub 2}MnSi electrode does not have a significant effect on the overall Co{sub 2}MnSi /Ag performance.
Electronic and magnetic phenomena at the interface of LaAlO3 and Ru doped SrTiO3
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Ab Initio Study of Energetics, Charge Transfer, and Atomic Structures of FCC Fe/NbC Interfaces with and Without N Doping: From Coherent to Semi-coherent Interfaces
Nitrogen is added to stainless steels to improve their toughness and corrosion resistance. However, it is not well understood how nitrogen may impact the precipitate/matrix interfacial properties. In this work, we consider the (FCC) Fe (001)/NbC (001) interface as a model system to study how interfacial structure, energy, and electron charge are affected by nitrogen using DFT calculations. We compare the structures and energetics of coherent and semi-coherent interfaces by including the elastic contribution component. It is found that nitrogen does not have a significant effect on either the interfacial energy or the atomic arrangement near the interface region. A highly intricate bonding feature is revealed near heterophase interfaces between alloy elements, in which metallic and covalent features are present together with charge transfer. Additionally, the work on determining accurate interfacial energies is at the core of all quantitative precipitation modeling efforts (in particular, in the XMAT Program). In turn, nucleation, growth/dissolution, and coarsening of precipitates contribute critically to the material’s ability to withstand creep, creep fatigue, and other detrimental processes reducing its service life. It is for this reason that developing quantitative understanding of interfaces and their energetics in materials is so important for their development and further improvement.