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Electrolyte layering at the calcite(104)-water interface indicated by Rb + - and Se(VI) K-edge resonant interface diffraction
Calcite–water interface reactions are of major importance in various environmental settings as well as in industrial applications. Here we present resonant interface diffraction results on the calcite(104)–aqueous solution interface, measured in solutions containing either 10 mmol L -1 RbCl or 0.5 mmol L -1 Se(VI). Results indicate that Rb + ions enter the surface adsorbed water layers and adsorb at the calcite(104)–water interface in an inner-sphere fashion. A detailed analysis based on specular and off-specular resonant interface diffraction data reveals three distinct Rb + adsorption species: one 1.2 Å above the surface, the second associated with surface adsorbed water molecules 3.2 Å above the surface, and the third adsorbed in an outer-sphere fashion 5.6 Å above the surface. A peak in resonant amplitude between L = 1.5 and L = 3.0 is interpreted as signal from a layered electrolyte structure. The presence of a layered electrolyte structure seems to be confirmed by data measured in the presence of Se(VI).
Patterned surface anchoring of nematic droplets at miscible liquid–liquid interfaces
We report on the internal configurations of droplets of nematic liquid crystals (LCs; 10–50 μm-in-diameter; comprised of 4-cyano-4'-pentylbiphenyl and 4-(3-acryloyloxypropyloxy)benzoic acid 2-methyl-1,4-phenylene ester) sedimented from aqueous solutions of sodium dodecyl sulfate (SDS) onto interfaces formed with pure glycerol. We observed a family of internal LC droplet configurations and topological defects consistent with a remarkably abrupt transition from homeotropic (perpendicular) to tangential anchoring on the surface of the LC droplets in the interfacial environment. Calculations of the interdiffusion of water and glycerol at the aqueous–glycerol interface revealed the thickness of the diffuse interfacial region of the two miscible liquids to be small (0.2–0.5 μm) compared to the diameters of the LC droplets on the experimental time-scale (15–120 minutes), leading us to hypothesize that the patterned surface anchoring was induced by gradients in concentration of SDS and glycerol across the diameter of the LC droplets in the interfacial region. This hypothesis received additional support from experiments in which the time of sedimentation of the LC droplets onto the interface was systematically increased and the droplets were photo-polymerized to preserve their configurations: the configurations of the LC droplets were consistent with a time-dependent decrease in the fraction of the surface area of each droplet exhibiting homeotropic anchoring. Specifically, LC droplets with <10% surface area with tangential anchoring exhibited a bulk point defect within the LC droplet, whereas droplets with >10% surface area with tangential anchoring exhibited a boojum defect within the tangential region and a disclination loop separated the regions with tangential and homeotropic anchoring. The topological charge of these LC droplet configurations was found to be consistent with the geometrical theorems of Poincaré and Gauss and also well-described by computer simulations performed by minimization of a Landau–de Gennes free energy. Additional experimental observations (e.g., formation of “Janus-like” particles with one hemisphere exhibiting tangential anchoring and the other perpendicular anchoring) and simulations (e.g., a size-dependent set of LC droplet configurations with <10% surface area exhibiting tangential anchoring) support our general conclusion that placement of LC droplets into miscible liquid–liquid interfacial environments with compositional gradients can lead to a rich set of LC droplet configurations with symmetries and optical characteristics that are not encountered in LC droplet systems in homogeneous, bulk environments. Finally, our results also reveal that translocation of LC droplets across liquid–liquid interfaces can define new transition pathways that connect distinct configurations of LC droplets.
Hydrogen evolution activity tuning via two-dimensional electron accumulation at buried interfaces
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Rate Theory of Ion Pairing at the Water Liquid-Vapor Interface: A Case of Sodium Iodide
Studies of ion pairing at interfaces have been intensified recently because of their importance in many chemical reactive phenomena such as ion–ion interactions that are affected by interfaces and their influence on kinetic processes. In this study, we performed simulations to examine the thermodynamics and kinetics of small polarizable sodium iodide ions in the bulk and near the water liquid–vapor interface. Using classical transition state theory, we calculated the dissociation rates, and corrected them with transmission coefficients obtained from the reactive flux formalism and Grote-Hynes theory. Our results show that in addition to affecting the free energy of ions in solution, the interfacial environments significantly influence the kinetics of ion pairing. Results on the relaxation time obtained using the reactive flux formalism and Grote-Hynes theory present an unequivocal picture that the interface suppresses ion dissociation. The effects of the use of molecular models on the ion interactions as well as the ion-pair configurations at the interface also are quantified and discussed. Acknowledgments This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. The calculations were carried out using computer resources provided by the Office of Basic Energy Sciences.
The Shifted Interface Method: A flexible approach to embedded interface computations
We propose a new embedded finite element method to simulate partial differential equations over domains with internal interfaces. Our approach belongs to the family of surrogate/approximate interface methods and relies on the idea of shifting the location and value of jump interface conditions. This choice has the goal of preserving optimal convergence rates while avoiding small cut cells and related problematic issues, typical of traditional embedded methods. The proposed approach is accurate, robust, efficient, and simple to implement. We apply this concept to internal interface computations in the context of the mixed Poisson problem, also known as the Darcy flow problem. An extensive set of numerical tests is provided to demonstrate the performance of the proposed approach.
Interface- and discontinuity-aware numerical schemes for plasma 3-T radiation diffusion in two and three dimensions
A set of numerical schemes is developed for two- and three-dimensional time-dependent 3-T radiation diffusion equations in systems involving multi-materials. To resolve sub-cell structure, interface reconstruction is implemented within any cell that has more than one material. Therefore, the system of 3-T radiation diffusion equations is solved on two- and three-dimensional polyhedral meshes. The focus of the development is on the fully coupling between radiation and material, the treatment of nonlinearity in the equations, i.e., in the diffusion terms and source terms, treatment of the discontinuity across cell interfaces in material properties, the formulations for both transient and steady states, the property for large time steps, and second order accuracy in both space and time. The discontinuity of material properties between different materials is correctly treated based on the governing physics principle for general polyhedral meshes and full nonlinearity. The treatment is exact for arbitrarily strong discontinuity. The scheme is fully nonlinear for the full nonlinearity in the 3-T diffusion equations. Three temperatures are fully coupled and are updated simultaneously. The scheme is general in two and three dimensions on general polyhedral meshes. The features of the scheme are demonstrated through numerical examples for transient problems and steady states. The effects of some simplifications of numerical schemes are also shown through numerical examples, such as linearization, simple average of diffusion coefficient, and approximate treatment for the coupling between radiation and material.
Quantifying Photocurrent Loss of a Single Particle–Particle Interface in Nanostructured Photoelectrodes
Particle–particle interfaces are ubiquitous in nanostructured photoelectrodes and photovoltaics, which are important devices for solar energy conversion. Furthermore, these interfaces are expected to cause performance losses in these devices, but how much loss they would incur is poorly defined. Here we use a subparticle photoelectrochemical current measurement, in combination with specific photoelectrode configurations, to quantify the current losses from single particle–particle interfaces formed between individual TiO 2 nanorods operating as photoanodes in aqueous electrolytes. We find that a single interface leads to ~20% photocurrent loss (i.e., ~80% retention of the original current). Such quantitative, first-of-its-kind, information provides a metric for guiding the optimization and design of nanostructured photoelectrodes and photovoltaics.
Investigation of Thermal Interface Materials Using Phase-Sensitive Transient Thermoreflectance Technique: Preprint
With increasing power density in electronics packages/modules, thermal resistances at multiple interfaces are a bottleneck to efficient heat removal from the package. In this work, the performance of thermal interface materials such as grease, thermoplastic adhesives and diffusion-bonded interfaces are characterized using the phase-sensitive transient thermoreflectance technique. A multi-layer heat conduction model was constructed and theoretical solutions were derived to obtain the relation between phase lag and the thermal/physical properties. This technique enables simultaneous extraction of the contact resistance and bulk thermal conductivity of the TIMs. With the measurements, the bulk thermal conductivity of Dow TC-5022 thermal grease (70 to 75 um bondline thickness) was 3 to 5 W/(m-K) and the contact resistance was 5 to 10 mm2-K/W. For the Btech thermoplastic material (45 to 80 μm bondline thickness), the bulk thermal conductivity was 20 to 50 W/(m-K) and the contact resistance was 2 to 5 mm2-K/W. Measurements were also conducted to quantify the thermal performance of diffusion-bonded interface for power electronics applications. Results with the diffusion-bonded sample showed that the interfacial thermal resistance is more than one order of magnitude lower than those of traditional TIMs, suggesting potential pathways to efficient thermal management.
Band-Gap Engineering at a Semiconductor-Crystalline Oxide Interface
The epitaxial growth of crystalline oxides on semiconductors provides a pathway to introduce new functionalities to semiconductor devices. Key to electrically coupling crystalline oxides with semiconductors to realize functional behavior is controlling the manner in which their bands align at interfaces. Here we apply principles of band gap engineering traditionally used at heterojunctions between conventional semiconductors to control the band offset between a single crystalline oxide and a semiconductor. Reactive molecular beam epitaxy is used to realize atomically abrupt and structurally coherent interfaces between SrZr x Ti 1-x O 3 and Ge, in which the band gap of the former is enhanced with Zr content x. We present structural, electrical and photoemission characterization of SrZr x Ti 1-x O 3 3-Ge heterojunctions for x = 0.2 to 0.75 and demonstrate the band offset can be tuned from type-II to type-I. The type-I band offset provides a platform to integrate the dielectric, ferroelectric and ferromagnetic functionalities of oxides with semiconducting devices.
Interface PINNs (I-PINNs): A physics-informed neural networks framework for interface problems
Here, we present a novel physics-informed neural networks (PINNs) framework for modeling interface problems, termed Interface PINNs (I-PINNs). I-PINNs uses different neural networks for any two subdomains separated by a sharp interface such that the neural networks differ only through their activation functions while the other parameters remain identical. The performance of I-PINNs, conventional PINNs, and other existing domain-decomposition PINNs methods such as extended PINNs (XPINNs) and multi-domain PINN (M-PINN) is compared through several one-dimensional, two-dimensional, and three-dimensional benchmark elliptic interface problems. The results demonstrate that I-PINNs provides a root-mean-square-error accuracy, at least two orders of magnitude better than conventional PINNs and XPINNs at approximately one-tenth of the computational cost of conventional PINNs and half the cost of XPINNs. Additionally, while I-PINNs and M-PINN provide comparable accuracies, M-PINN is found to be approximately 50% more expensive.
Quantum Confinement and Decoherence Effect on Excited Electron Transfer at the Semiconductor–Molecule Interface: A First-Principles Dynamics Study
Excited electron dynamics at the semiconductor–molecule interface play a vital role in many solar energy conversion applications and beyond. First-principles dynamics simulation is used to study how excited electron dynamics in a type-II semiconductor–molecule interface is affected when the surface of a bulk semiconductor is replaced with that of a quantum dot. In particular, the interface between the hydrogen-terminated silicon(111) surface and a simple organic molecule is investigated. Quantum confinement was found to significantly slow down the excited electron relaxation and the interfacial transfer of the excited electron. Additionally, the role of decoherence was examined. The decoherence affects the dynamics much more significantly for the interface with the quantum dot, while the bulk surface case is affected only marginally by it. Finally, compared to the excited electron relaxation within the quantum dot, the decoherence effect was found to slow down the interfacial transfer from the quantum dot to the molecule by more than an order of magnitude, exhibiting a significant quantum Zeno effect.
Effect of Functional and Electron Correlation on the Structure and Spectroscopy of the Al 2 O 3 (001)–H 2 O Interface
Oxide–water interfaces are ubiquitous, with many applications in industry and the environment, yet there is a great deal of controversy over their properties and microscopic structure. This controversy stems, in part, from the unique H-bond networks formed at different surface terminations and mineral compositions. Density functional theory simulations of these interfaces require an accurate description of both the oxide mineral and water in diverse H-bond environments. Thus, herein we simulate the Al 2 O 3 (001)–H 2 O interface using the PBE, PBE-TS, RPBE, SCAN, and HSE06-TS functionals to determine how calculated interfacial properties depend on the choice of functional. We find that the structure of the first few layers of water at the surface is determined by electron correlation in a way that cannot be approximated using semiemipirical van der Waals corrections. Of the functionals investigated, we find that SCAN yields the most accurate interfacial structure, dynamics, and sum frequency generation spectrum. Furthermore, SCAN leads to a reduction in the order of the 2D H-bond network of water at the alumina surface predicted by GGA functionals, leading to a significant decrease in the anisotropy of the diffusion coefficient at the surface. We emphasize the importance of using a functional which accurately describes electron correlation for more complex oxides, such as transition-metal oxides, where electron correlation may play an even greater role in determining the structure and dynamics of the oxide–water interface.
Pathways for Electron Transfer at MgO–Water Interfaces from Ab Initio Molecular Dynamics
The nature of electron transfer across metal oxide–water interfaces depends significantly on the band gap of the oxide and its band edge energies relative to the potentials of relevant aqueous redox couples. Here we focus on the water interface with MgO, a prototypical wide band gap oxide whose conduction band edge is close in energy to that of water. We investigate the behavior of an excess electron at and out of equilibrium near the interface using ab initio molecular dynamics based on hybrid density functional theory. Our simulations show that under equilibrium conditions the excess electron (donated by an Al impurity in MgO) localizes to a midgap defect state comparable in energy and shape to a hydrated electron in bulk water. To characterize the electron transfer from the conduction band of MgO to interfacial product states, we dope near-equilibrium configurations of the pristine MgO–water system with Al and run short trajectories of these instantaneously out-of-equilibrium systems. Here we observe two distinct products associated with the excess electron: a surface-localized electron (e surf –) and an aqueous hydrogen radical (H • ). The H • pathway exhibits a much higher activation barrier despite being more exoergic, making e surf – the kinetic product. Our characterization of the pathways on the basis of Marcus theory is consistent with the poor observed utility of MgO for water radiolysis. Moreover, we anticipate that the computational framework employed here will be broadly applicable to assessing electron transfer mechanisms at aqueous, photocatalytic interfaces.
Passivation of In{sub 0.53}Ga{sub 0.47}As/ZrO{sub 2} interfaces by AlN atomic layer deposition process
Reducing defects at III-V/high-k interfaces is essential for optimizing devices built on these materials. Here, the role of an interfacial AlN process at In{sub 0.53}Ga{sub 0.47}As/ZrO{sub 2} interfaces is investigated by hard x-ray photoelectron spectroscopy (HAXPES) and capacitance/voltage (C-V) measurements. C-V measurements show a significant reduction in the density of interface traps with the interfacial AlN process and a capping TiN layer. To elucidate the specific role of the AlN process, blanket films with various deposition processes are compared. The AlN process alone (without subsequent dielectric deposition) reduces InGaAs oxide levels below the HAXPES detection limit, even though the AlN is ultimately found to be oxidized into AlO{sub x} with only trace N incorporation, yet AlN passivation provides a lower D{sub it} (density of interface traps) when compared with an H{sub 2}O-based Al{sub 2}O{sub 3} deposition. The AlN process does not passivate against re-oxidation of the InGaAs during an O{sub 3} based ZrO{sub 2} deposition process, but it does provide passivation against As-As development during subsequent TiN deposition. The role of chemical defects in the C-V characteristics is also discussed.
Intermixing at the absorber-buffer layer interface in thin-film solar cells: The electronic effects of point defects in Cu(In,Ga)(Se,S){sub 2} and Cu{sub 2}ZnSn(Se,S){sub 4} devices
We investigate point defects in the buffer layers CdS and ZnS that may arise from intermixing with Cu(In,Ga)(S,Se){sub 2} (CIGS) or Cu{sub 2}ZnSn(S,Se){sub 4} (CZTS) absorber layers in thin-film photovoltaics. Using hybrid functional calculations, we characterize the electrical and optical behavior of Cu, In, Ga, Se, Sn, Zn, Na, and K impurities in the buffer. We find that In and Ga substituted on the cation site act as shallow donors in CdS and tend to enhance the prevailing n-type conductivity at the interface facilitated by Cd incorporation in CIGS, whereas they are deep donors in ZnS and will be less effective dopants. Substitutional In and Ga can favorably form complexes with cation vacancies (A-centers) which may contribute to the “red kink” effect observed in some CIGS-based devices. For CZTS absorbers, we find that Zn and Sn defects substituting on the buffer cation site are electrically inactive in n-type buffers and will not supplement the donor doping at the interface as in CIGS/CdS or ZnS devices. Sn may also preferentially incorporate on the S site as a deep acceptor in n-type ZnS, which suggests possible concerns with absorber-related interfacial compensation in CZTS devices with ZnS-derived buffers. Cu, Na, and K impurities are found to all have the same qualitative behavior, most favorably acting as compensating acceptors when substituting on the cation site. Our results suggest one beneficial role of K and Na incorporation in CIGS or CZTS devices is the partial passivation of vacancy-related centers in CdS and ZnS buffers, rendering them less effective interfacial hole traps and recombination centers.
Charge separation at nanoscale interfaces: Energy-level alignment including two-quasiparticle interactions
The universal and fundamental criteria for charge separation at interfaces involving nanoscale materials are investigated. In addition to the single-quasiparticle excitation, all the two-quasiparticle effects including exciton binding, Coulomb stabilization, and exciton transfer are considered, which play critical roles on nanoscale interfaces for optoelectronic applications. We propose a scheme allowing adding these two-quasiparticle interactions on top of the single-quasiparticle energy level alignment for determining and illuminating charge separation at nanoscale interfaces. Employing the many-body perturbation theory based on Green's functions, we quantitatively demonstrate that neglecting or simplifying these crucial two-quasiparticle interactions using less accurate methods is likely to predict qualitatively incorrect charge separation behaviors at nanoscale interfaces where quantum confinement dominates.
Ternary superlattice boosting interface-stabilized magnetic chirality
In cobalt-nickel multilayers grown on iridium surfaces, magnetic homo-chirality can be stabilized by Dzyaloshinskii-Moriya interactions (DMI) at the interface with the substrate. When thickness of the multilayers is increased beyond threshold values, then non-chiral bulk properties exceed interface contributions and this type of chirality vanishes. Here, we use spin-polarized low energy electron microscopy to measure these thickness thresholds, and we determine estimates of the strength of the DMI from the measurements. Even though the same 5d heavy metal is used as a substrate, a remarkably large variation is found between the two 3d magnets: our results indicate that the strength of the DMI at Co/Ir interfaces is three times larger than at Ni/Ir interfaces. We show how this finding provides ways to extend interfacial-DMI stabilization of domain wall chirality to 3d/5d/3d ternary multilayers such as [Ni/Ir/Co]{sub n}. Such strategies may extend chirality-control to larger film thickness and a wider range of substrates, which may be useful for designing new spintronics devices.