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Advanced structured packing geometries fabricated with 3D printing were used for absorber CO 2 capture with a liquid solvent. Compared to conventional packing, they had greatly enhanced (90–140%) effective surface areas and comparable hydrodynamics.
The structure of the surface layer of a heterogeneous solid body (xenolite) before and after friction is studied by infrared and Raman spectroscopy. Before friction, the layer contained hornblende and pyroxene crystals. The friction resulted in partial transformation of pyroxenes into hornblende and the latter was transformed into montmorillonite clay. The xenolite surface is covered with a ~60-nm-thick layer of water.
Nested wrinkle structures, hierarchical surface wrinkles of different periodicities of sub-μm and tens-μm, have been fabricated on a siloxane-photomonomer hybrid film via a photo-induced surface polymerization of acrylamide. The formation mechanism of the nested wrinkle structures is examined based on a time-dependent structure observation and chemical composition analyses. In-situ observation of the evolving surface structure showed that sub-μm scale wrinkles first formed, subsequently the tens-μm scale ones did. In-situ FT-IR analysis indicated that the nested wrinkles formation took place along with the development of siloxane network of under layer. A cross sectional observation of the film revealed that the film was composed of three layers. FT-IR spectra of the film revealed that the surface and interior layers were polyacrylamide rich layer and siloxane-polymer rich layer, respectively. The intermediate layer formed as a diffusion layer by migration of acrylamide from interior to the surface. These three layers have different chemical compositions and therefore different mechanical characteristics, which allows the wrinkle formation. Shrinkage of siloxane-polymer interior layers, as a result of polycondensation of siloxane network, induced mechanical instabilities at interlayers, to form the nested wrinkle structures.
An analysis of the gaseous component in protoplanetary disks can inform us about their thermal and physical structure, chemical composition, and kinematic properties, all of which are crucial for understanding various processes within the disks. By exploiting the asymmetry of the line emission, or via line profile analysis, we can locate the emitting surfaces. Here, we present the emission surfaces of the exoALMA sources in 12 CO J = 3–2, 13 CO J = 3–2, and CS J = 7–6. We find that 12 CO traces the upper disk atmosphere, with mean $\langle$ z/r $\rangle$ values of ≈0.28, while 13 CO and CS trace lower regions of the disk with mean $\langle$ z/r $\rangle$ values of ≈0.16 and ≈0.18, respectively. We find that 12 CO $\langle$ z/r $\rangle$ and the disk mass are positively correlated with each other; this relationship offers a straightforward way to infer the disk mass. We derive 2D r – z temperature distributions of the disks. Additionally, we search for substructure in the surfaces and radial intensity profiles; we find evidence of localized substructure in the emission surfaces and peak intensity profiles of nearly every disk, with this substructure often being coincident between molecular tracers, intensity profiles, and kinematic perturbations. Four disks display evidence of potential photodesorption, implying that this effect may be common even in low far-ultraviolet star-forming regions. For most disks, we find that the physical and thermal structure is more complex than analytical models can account for, highlighting a need for more theoretical work and a better understanding of the role of projection effects on our observations.
In the recently discovered topological crystalline insulators SnTe and Pb 1–x Sn x (Te, Se), crystal symmetry and electronic topology intertwine to create topological surface states with many interesting features including Lifshitz transition, Van-Hove singularity, and fermion mass generation. These surface states are protected by mirror symmetry with respect to the (110) plane. In this work we present a comprehensive study of the effects of different mirror-symmetry-breaking perturbations on the (001) surface band structure. Pristine (001) surface states have four branches of Dirac fermions at low energy. We show that ferroelectric-type structural distortion generates a mass and gaps out some or all of these Dirac points, while strain shifts Dirac points in the Brillouin zone. An in-plane magnetic field leaves the surface state gapless, but introduces asymmetry between Dirac points. Finally, an out-of-plane magnetic field leads to discrete Landau levels. We show that the Landau level spectrum has an unusual pattern of degeneracy and interesting features due to the unique underlying band structure. Furthermore this suggests that Landau level spectroscopy can detect and distinguish between different mechanisms of symmetry breaking in topological crystalline insulators.
The “quenching” technique was used to investigate the initial stage of the formation of a terracestep nanostructure on the R-cut surface of sapphire crystal upon high-temperature annealing in air. The morphological features of the formation of A- and R-sapphire planes are experimentally shown in dependence on the misorientation direction and qualitatively interpreted with allowance for the surface energy density for the main sapphire faces. The possibilities of forming AlN layers on the R-sapphire surface with a terrace-step nanostructure under thermochemical effect and high-temperature substrate annealing in a mixture of nitrogen and reducing gases are considered.
Extended surface Pt or Pt-M (M = Ni or Co) catalysts are a viable alternative to supported nanoparticle catalysts for the oxygen reduction reaction (ORR) at the cathode in proton exchange membrane fuel cells (PEMFCs). The activity and durability of these catalysts in membrane electrode assemblies (MEAs) are greatly dependent on the surface and bulk properties of the catalyst material, integration with ionomer, and the three-dimensional structure of the electrode, necessitating extensive characterization of the catalyst in the electrode at multiple scales. In this work, extended surface PtNi nanowire-based electrocatalysts derived by spontaneous galvanic displacement, and post-treated to obtain high specific and mass activities, are characterized by X-ray spectroscopies to assess catalyst composition and to determine the extent of Pt-Ni alloying. Transmission X-ray microscopy (TXM) is used to generate two- and three-dimensional images of catalyst layers with varied compositions within the electrode to show the distribution of nanowires and to study Ni dissolution and redeposition within the electrode. These techniques are complemented by electron microscopy, which is used to confirm leaching of nickel from the nanowires and its redeposition within the electrode. This process is shown to have detrimental effect on the MEA performance, which can be at least in part recovered by soaking electrodes in acid. The combination of these techniques provides unprecedented detail of the evolution of the nanowire-based extended surface catalyst and electrode structure guiding the targeted design of high performance electrodes based on this class of materials.
Surface-enhanced Raman scattering (SERS) intensity of two-dimensional (2D) materials critically depends on the resonant conditions and factors such as the substrate interferences and molecule adsorption fluctuations, making comprehensive investigation, understanding, and optimization of 2D materials-assisted SERS challenging. Here, in this work, the wavelength-dependent SERS of van der Waals structures of 2D materials is systematically investigated, focusing on the intrinsic frequency-dependent Raman tensors by first-principles method while ruling out other extrinsic factors in experiments. Distinct enhancement profiles are found for different 2D materials, among which MoS2 and graphene exhibit remarkably strong and broadband enhancement effects. For stacked multilayers and heterostructures of 2D materials, the calculated SERS addresses the significance of the first contact monolayer effect. Based on the above theory, the van der Waals sandwich structures are proposed and investigated as the SERS substrates, verifying a further significantly enhanced SERS performance. This resonant first-principles study demonstrates a comprehensive and analytical way to explore and promote the SERS of van der Waals structures.
Local optimization of adsorption systems inherently involves different scales: within the substrate, within the molecule, and between the molecule and the substrate. In this work, we show how the explicit modeling of different characteristics of the bonds in these systems improves the performance of machine learning methods for optimization. Furthermore, we introduce an anisotropic kernel in the Gaussian process regression framework that guides the search for the local minimum, and we show its overall good performance across different types of atomic systems. The method shows a speed-up of up to a factor of two compared with the fastest standard optimization methods on adsorption systems. Additionally, we show that a limited memory approach is not only beneficial in terms of overall computational resources but can also result in a further reduction of energy and force calculations.
Bulk Cr 2 O 3 is an antiferromagnetic (AFM) oxide that exhibits the magnetoelectric effect at room temperature, with neither spontaneous magnetization nor net electric polarization. These physical properties stem from a subtle competition between exchange and crystal field interactions. In this article, we exploit the symmetry breaking at the surface of Cr 2 O 3 nanoparticles for unbalancing this delicate physical equilibrium. The emerging weak ferromagnetic signal we observe persists up to near room temperature (≈ 270 K) at which the antiferromagnetic order disappears. In addition, an exchange-bias effect, that rapidly decreases on heating from low temperature up to 30 K, is resistant to thermal disorder above 200 K. In conclusion, our findings point to the possible formation of an entangled core/shell magnetic structure, where pinned uncompensated spins at the shell are randomly distributed in a low-temperature spin-glass ordering, with low net magnetic moment and an ordering temperature governed by the AFM Néel temperature.
Since the initial discovery of colloidal lead halide perovskite nanocrystals, there has been significant interest placed on these semiconductors because of their remarkable optoelectronic properties, including very high photoluminescence quantum yields, narrow size- and composition-tunable emission over a wide color gamut, defect tolerance, and suppressed blinking. These material attributes have made them attractive components for next-generation solar cells, light emitting diodes, low-threshold lasers, single photon emitters, and X-ray scintillators. While a great deal of research has gone into the various applications of colloidal lead halide perovskite nanocrystals, comparatively little work has focused on the fundamental surface chemistry of these materials. While the surface chemistry of colloidal semiconductor nanocrystals is generally affected by their particle morphology, surface stoichiometry, and organic ligands that contribute to the first coordination sphere of their surface atoms, these attributes are markedly different in lead halide perovskite nanocrystals because of their ionicity. Herein, emerging work on the surface chemistry of lead halide perovskite nanocrystals is highlighted, with a particular focus placed on the most-studied composition of CsPbBr 3 . We begin with an in-depth exploration of the native surface chemistry of as-prepared, 0-D cuboidal CsPbBr 3 nanocrystals, including an atomistic description of their surface termini, vacancies, and ionic bonding with ligands. We then proceed to discuss various post-synthetic surface treatments that have been developed to increase the photoluminescence quantum yields and stability of CsPbBr 3 nanocrystals, including the use of tetraalkylammonium bromides, metal bromides, zwitterions, and phosphonic acids, and how these various ligands are known to bind to the nanocrystal surface. To underscore the effect of post-synthetic surface treatments on the application of these materials, we focus on lead halide perovskite nanocrystal-based light emitting diodes, and the positive effect of various surface treatments on external quantum efficiencies. We also discuss the current state-of-the-art in the surface chemistry of 1-D nanowires and 2-D nanoplatelets of CsPbBr 3 , which are more quantum confined than the corresponding cuboidal nanocrystals but also generally possess a higher defect density because of their increased surface area-to-volume ratios.
Solid state synthesis and physical mechanisms of electrical conductivity variation in polycrystalline, strontium doped indium oxide In{sub 2}O{sub 3}:(SrO){sub x} were investigated for materials with different doping levels at different temperatures (T = 20–300 °C) and ambient atmosphere content including humidity and low pressure. Gas sensing ability of these compounds as well as the sample resistance appeared to increase by 4 and 8 orders of the magnitude, respectively, with the doping level increase from zero up to x = 10%. The conductance variation due to doping is explained by two mechanisms: acceptor-like electrical activity of Sr as a point defect and appearance of an additional phase of SrIn{sub 2}O{sub 4}. An unusual property of high level (x = 10%) doped samples is a possibility of extraordinarily large and fast oxygen exchange with ambient atmosphere at not very high temperatures (100–200 °C). This peculiarity is explained by friable structure of crystallite surface. Friable structure provides relatively fast transition of samples from high to low resistive state at the expense of high conductance of the near surface layer of the grains. Microscopic study of the electro-diffusion process at the surface of oxygen deficient samples allowed estimation of the diffusion coefficient of oxygen vacancies in the friable surface layer at room temperature as 3 × 10{sup −13} cm{sup 2}/s, which is by one order of the magnitude smaller than that known for amorphous indium oxide films.
Specific features of the structure formation in rapidly quenched high-cobalt alloy coatings formed by plasma sputtering have been investigated. The structural state of the investigated coatings has been identified by the X-ray diffraction technique. The sequence and kinetics of structural transformations occurring in the specified time-temperature heating regimes have been examined using differential thermal analysis. It has been established that heat generation and crystallization temperature depend on the conditions of formation of bulk amorphous coatings.
The ligand-nanocrystal boundaries of colloidal quantum dots (QDs) mediate the primary energy and electron transfer processes that underpin photochemical and photocatalytic transformations at their surfaces. We use mid-infrared transient absorption spectroscopy to reveal the influence that ligand structure and bonding to nanocrystal surfaces have on the changes of the excited state surface chemistry of this boundary in PbS QDs and the corresponding impact on charge transfer processes between nanocrystals. We demonstrate that oleate ligands undergo marked changes in their bonding to surfaces in the excitonic excited states of the nanocrystals, indicating that oleate passivated PbS surfaces undergo significant structural changes following photoexcitation. These changes can impact the surface mobility of the ligands and the ability of redox shuttles to approach the nanocrystal surfaces to undergo charge transfer in photocatalytic reactions. In contrast, markedly different transient vibrational features are observed in iodide/mercaptoproprionic acid passivated PbS QD films that result from charge transfer between neighboring nanocrystals and localization of holes at the nanocrystal surfaces near MPA ligands. This ability to distinguish the influence that excitonic excited states vs charge transfer processes have on the surface chemistry of the ligand-nanocrystal boundary lays the groundwork for exploration of how this boundary can be understood and controlled for the design of nanocrystalline materials tailored for specific applications in solar energy harvesting and photocatalytic reactions.
We study the physics of steady detonation wave propagation in a two-dimensional circular arc via a Detonation Shock Dynamics (DSD) surface evolution model. The dependence of the surface angular speed and surface spatial structure on the inner arc radius ( $R_{i}$ ), the arc thickness ( $R_{e}-R_{i}$ , where $R_{e}$ is the outer arc radius) and the degree of confinement on the inner and outer arc is examined. We first analyse the results for a linear $D_{n}$ – $\unicode[STIX]{x1D705}$ model, in which the normal surface velocity $D_{n}=D_{CJ}(1-B\unicode[STIX]{x1D705})$ , where $D_{CJ}$ is the planar Chapman–Jouguet velocity, $\unicode[STIX]{x1D705}$ is the total surface curvature and $B$ is a length scale representative of a reaction zone thickness. An asymptotic analysis assuming the ratio $B/R_{i}\ll 1$ is conducted for this model and reveals a complex surface structure as a function of the radial variation from the inner to the outer arc. For sufficiently thin arcs, where $(R_{e}-R_{i})/R_{i}=O(B/R_{i})$ , the angular speed of the surface depends on the inner arc radius, the arc thickness and the inner and outer arc confinement. For thicker arcs, where $(R_{e}-R_{i})/R_{i}=O(1)$ , the angular speed does not depend on the outer arc radius or the outer arc confinement to the order calculated. It is found that the leading-order angular speed depends only on $D_{CJ}$ and $R_{i}$ , and corresponds to a Huygens limit (zero curvature) propagation model where $D_{n}=D_{CJ}$ , assuming a constant angular speed and perfect confinement on the inner arc surface. Having the normal surface speed depend on curvature requires the insertion of a boundary layer structure near the inner arc surface. This is driven by an increase in the magnitude of the surface wave curvature as the inner arc surface is approached that is needed to meet the confinement condition on the inner arc surface. For weak inner arc confinement, the surface wave spatial variation with the radial coordinate is described by a triple-deck structure. The first-order correction to the angular speed brings in a dependence on the surface curvature through the parameter $B$ , while the influence of the inner arc confinement on the angular velocity only appears in the second-order correction. For stronger inner arc confinement, the surface wave structure is described by a two-layer solution, where the effect of the confinement on the angular speed is promoted to the first-order correction. We also compare the steady-state arc solution for a PBX 9502 DSD model to an experimental two-dimensional arc geometry validation test.
The surface reconstruction on the (110) surface of LnScO 3 (Ln=Gd,Tb,Dy) has been investigated using x-ray photoelectron spectroscopy, atomic force microscopy, and transmission electron diffraction coupled with higher-level density-functional theory methods. The experimental techniques generate constraints on the surface chemistry and structure that are used to inform the theoretical comparison of a number of potential surface structures. The resulting structure is then compared to experimental aberration-corrected transmission electron microscopy results using multislice simulation. The surfaces of both single-crystalline substrates and hydrosauna synthesized nanoparticles exhibit a Sc-rich double layer with a Sc 3 O 4 termination.
Ab initio calculations show that a cleanly cleaved nonpolar surface of considered nonmagnetic insulating metal oxides always has a band gap. If the bulk valence band edge has mainly oxygen 2p character while the bulk conduction band edge has mainly metal d character, then there is no in-the-band-gap surface state. A simple procedure to identify the polarity of a given arbitrary surface is presented.