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At least 145 records · Page 8

Erratum to: Soft- and reactive landing of ions onto surfaces: concepts and applications

Soft- and reactive landing of mass-selected ions is gaining attention as a promising approach for the precisely-controlled preparation of materials on surfaces that are not amenable to deposition using conventional methods. A broad range of ionization sources and mass filters are available that make ion soft-landing a versatile tool for surface modification using beams of hyperthermal (<100?eV) ions. The ability to select the mass-to-charge ratio of the ion, its kinetic energy and charge state, along with precise control of the size, shape, and position of the ion beam on the deposition target distinguishes ion soft landing from other surface modification techniques. Soft- and reactive landing have been used to prepare interfaces for practical applications as well as precisely-defined model surfaces for fundamental investigations in chemistry, physics, and materials science. For instance, soft- and reactive landing have been applied to study the surface chemistry of ions isolated in the gas-phase, prepare arrays of proteins for high-throughput biological screening, produce novel carbon-based and polymer materials, enrich the secondary structure of peptides and the chirality of organic molecules, immobilize electrochemically-active proteins and organometallics on electrodes, create thin films of complex molecules, and immobilize catalytically active organometallics as well as ligated metal clusters. In addition, soft landing has enabled investigation of the size-dependent behavior of bare metal clusters in the critical subnanometer size regime where chemical and physical properties do not scale predictably with size. The morphology, aggregation, and immobilization of larger bare metal nanoparticles, which are directly relevant to the design of catalysts as well as improved memory and electronic devices, have also been studied using ion soft landing. This review article begins in section 1 with a brief introduction to the existing applications of ion soft- and reactive landing. Section 2 provides an overview of the ionization sources and mass filters that have been used to date for soft landing of mass-selected ions. A discussion of the competing processes that occur during ion deposition as well as the types of ions and surfaces that have been investigated follows in section 3. Section 4 discusses the physical phenomena that occur during and after ion soft landing, including retention and reduction of ionic charge along with factors that impact the efficiency of ion deposition. The influence of soft landing on the secondary structure and biological activity of complex ions is addressed in section 5. Lastly, an overview of the structure and mobility as well as the catalytic, optical, magnetic, and redox properties of bare ionic clusters and nanoparticles deposited onto surfaces is presented in section 6. © 2015 Wiley Periodicals, Inc. Mass Spec Rev 35:439–479, 2016.

Johnson, Grant E.↗

The ion-gas-neutral interactions with surfaces-2 (IGNIS-2) facility for the study of plasma–material interactions

The Ion-Gas-Neutral Interactions with Surfaces-2 (IGNIS-2) surface science facility has been designed at the Pennsylvania State University with the specific purpose of enabling experiments to study plasma–material interactions. This in situ surface modification and characterization facility consists of multiple reconfigurable substations that are connected through a central transfer chamber. This fully connected vacuum system ensures that the physical and chemical properties of samples are not altered between surface modification and analysis. The modification techniques in IGNIS-2 include a low-energy (<300 eV), high-flux (up to 1016 cm−2 s−1) broad-beam ion source, a liquid metal dropper, a lithium injection system, an RF sputter source, and an evaporator. Its characterization techniques include charged particle-based techniques, such as low-energy ion scattering (enabled by two <5 keV ion sources) and x-ray photoelectron spectroscopy, and photon and light-based techniques, such as x-ray fluorescence, multi-beam optical stress sensors, and optical cameras. All of these techniques can be utilized up to mTorr pressures, allowing both in situ and in operando studies to be conducted. Results are presented on lithium wetting experiments of argon-irradiated tungsten-based composites, surface stress measurements of tungsten films during deuterium ion irradiation, and temperature-programmed desorption of deuterium-irradiated graphite to demonstrate the in situ capabilities of this new facility.

Instruments & Instrumentation↗

Probing Cellular Activity Via Charge‐Sensitive Quantum Nanoprobes

Nitrogen‐vacancy (NV) based quantum sensors hold great potential for real‐time single‐cell sensing with far‐reaching applications in fundamental biology and medical diagnostics. Although highly sensitive, the mapping of quantum measurements onto cellular physiological states has remained an exceptional challenge. Here, we introduce a novel quantum sensing modality capable of detecting changes in cellular activity. Our approach is based on the detection of environment‐induced charge depletion within an individual particle that, owing to a previously unaccounted transverse dipole term, induces systematic shifts in the zero‐field splitting (ZFS). Importantly, these charge‐induced shifts serve as a reliable indicator for lipopolysaccharide (LPS)‐mediated inflammatory response in macrophages. Furthermore, we demonstrate that surface modification of our diamond nanoprobes effectively suppresses these environment‐induced ZFS shifts, providing an important tool for differentiating electrostatic shifts caused by the environment from other unrelated effects, such as temperature variations. Notably, this surface modification also leads to significant reductions in particle‐induced toxicity and inflammation. Our findings shed light on systematic drifts and sensitivity limits of NV spectroscopy in a biological environment with ramifications for the critical discussion surrounding single‐cell thermogenesis. Notably, this work establishes the foundation for a novel sensing modality capable of probing complex cellular processes through straightforward physical measurements.

band bending↗

Electron beam induced damage in ITO coated Kapton

Data for the stability of thin conductive indium tin oxide films on 0.003 inch thick Kapton substrates during exposure of the surface to electron beams are reported. The electron beam energy was 3 keV and the diameter was about 0.8 mm. Thermal effects and surface modifications are considered. For primary current greater than 0.6 microamperes, an obvious dark discoloration with diameter approximately that of the beam was produced. The structure of the discolored region was studied with the scanning electron microscope, and the findings are stated. Surface modifications were explored by AES, obtaining spectra and secondary emission coefficient as a function of time for different beam intensities. In all cases beam exposure results in a decrease of the secondary yield but because of thermal effects this change, as well as composition changes, cannot be directly interpreted in terms of electron beam dosage.

Krainsky, I.↗

Preparing large area of thermochromic nanocomposite films for smart window application

The challenges posed by high building energy bill necessitate proactive implementation of energy-efficient strategies to minimize the uses of both electricity and heating gas and promote the use of free solar energy sources. "Smart" window films/glass, leveraging thermochromic vanadium dioxide (VO 2 ), offer an adaptive approach to harness solar energy, significantly reducing the thermal load of buildings. This is achieved by reflecting the infrared portion of the solar spectrum through a phase transition in the monoclinic M-phase (M) of VO 2 induced by heating. In this study, a scalable continuous flow synthesis process invented by Argonne was employed to explore a wide parameter space, targeting the controlled synthesis of monoclinic VO 2 (M) nanoparticles with well-controlled sizes and morphologies. Additionally, a doping strategy and surface modifications were utilized for high-throughput tuning of the metal-to-insulator transition temperature. Strategies to enhance the solar modulation properties of VO 2 nanoparticles in polymer films were investigated through (i) morphological transformation from spherical to nanorod structures, (ii) surface modification with low refractive index ligands, and (iii) incorporation of additional thermochromic materials for improved solar energy modulation and aesthetically appealing colors in smart films. Furthermore, the study outlines scaling-up synthesis methods for VO 2 nanoparticles in a continuous flow reactor using hydrazine monohydrate. This comprehensive investigation provides valuable insights into the upscaling synthesis and design of advanced VO 2 /polymer composite smart window films with enhanced functionality, solar energy modulation and visible light transmittance, driving the technology a step close for industrial application.

14 SOLAR ENERGY↗

Experimental study of crystallization fouling by calcium carbonate: Effects of surface structure and material

We report mitigation of crystallization fouling on heat transfer surface is crucial for developing highly efficient desalination techniques, because the tenacious and porous crystal layer can drastically deteriorate system efficiency. Surface modification is a potential approach to decrease scale formation and promote crystal removal, but some of the mechanisms between crystallization and substrate properties are still not fully understood. In this study, we use dual-angle microscopic visualization and image processing to quantify three-dimensional crystallization behavior and analyze the impact of surface structure and material. The transition of crystal size and distance with roughness and wettability are identified from statistical analysis. The determination of crystal porosity and effective thermal conductivity is enabled by visualized geometry and measured deposition mass. This study shed lights on potential strategies of surface modification to mitigate scaling in desalination by enhancing scale removal and localizing crystal growth.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Status and directions of modified tribological surfaces by ion processes

An overview is presented of recent advances in modifying contacting surfaces in motion by the various ion assisted surface coating/modification processes to reduce and control tribological failures. The ion assisted coating processes and the surface modification processes offer the greatest potential to custom tailor and optimize the tribological performance. Hard, wear resistant and low shear coatings deposited by the ion assisted processes are discussed. Primarily the recent advances of sputtered MoS2 ion plated Au, Ag, Pb lubricating films and sputtered and ion plated hard, wear resistant TiN, HfN, TiC films are described in terms of structural property performance interrelationships which lead to improved adhesion, cohesion, nucleation, morphological growth, density, film thickness as determined by structural and chemical characterization and frictional and wear behavior. Also, the recent tribological advances using the surface modification processes such as ion implantation, ion beam mixing is discussed with emphasis on the development of lubricous high temperature ceramic surfaces.

Spalvins, Talivaldis↗

Clicking the Surface of Poly[1-(trimethylsilyl)propyne] (PTMSP) via a Thiol–Ene Reaction: Unexpected CO 2 /N 2 Permeability

The surface modification of poly[1-(trimethylsilyl)- propyne] (PTMSP) film via a thiol-ene click reaction with sodium 3-mercapto-1-propanesulfonate has yielded membranes having a CO 2 permeance as high as 530 GPU with a CO 2 /N 2 selectivity of 21. This level of performance, together with the simplicity of this surface modification, indicates that such materials could become viable alternatives to some of the most enticing membrane materials that are currently being explored for the practical capture of CO 2 from flue gas.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Bifunctional Asymmetric Fabric with Tailored Thermal Conduction and Radiation for Personal Cooling and Warming

Personal thermal management is emerging as a promising strategy to provide thermal comfort for the human body while conserving energy. By improving control over the heat dissipating from the human body, personal thermal management can provide effective personal cooling and warming. Here, we propose a facile surface modification approach to tailor the thermal conduction and radiation properties based on commercially available fabrics, to realize better management of the whole heat transport pathway from the human body to the ambient. Additionally, a bifunctional asymmetric fabric (BAF) offering both a cooling and a warming effect is demonstrated. Due to the advantages of roughness asymmetry and surface modification, the BAF demonstrates an effective cooling effect through enhanced heat conduction and radiation in the cooling mode; in the warming mode, heat dissipation along both routes is reduced for personal warming. As a result, a 4.6 °C skin temperature difference is measured between the cooling and warming BAF modes, indicating that the thermal comfort zone of the human body can be enlarged with one piece of BAF clothing. We expect this work to present new insights for the design of personal thermal management textiles as well as a novel solution for the facile modification of available fabrics for both personal cooling and warming.

42 ENGINEERING↗

Surface coating by mechanofusion modulates bulk charging pathways and battery performance of Ni-rich layered cathodes

Ni-rich layered oxides as high-capacity battery cathodes suffer from degradation at high voltages. Here, we utilize a dry surface modification method, mechanofusion (MF), to achieve enhanced battery stability. The simplicity, high yield, and flexibility make it cost-effective and highly attractive for processing at the industrial scale. The underlying mechanisms responsible for performance improvement are unveiled by a systematic study combining multiple probes, e.g., 3D nano-tomography, spectroscopic imaging, in situ synchrotron diffraction, and finite element analysis (FEA). MF affects the bulk crystallography by introducing partially disordered structure, microstrain, and local lattice variation. Furthermore, the crack initiation and propagation pattern during delithiation are regulated and the overall mechanical fracture is reduced after such surface coating. We validate that MF can alter the bulk charging pathways. Such a synergic effect between surface modification and bulk charge distribution is fundamentally important for designing next-generation battery cathode materials.

25 ENERGY STORAGE↗

Surface property modification of silicon

The main emphasis of this work has been to determine the wear rate of silicon in fluid environments and the parameters that influence wear. Three tests were carried out on single crystal Czochralski silicon wafers: circular and linear multiple-scratch tests in fluids by a pyramidal diamond simulated fixed-particle abrasion; microhardness and three-point bend tests were used to determine the hardness and fracture toughness of abraded silicon and the extent of damage induced by abrasion. The wear rate of (100) and (111) n and p-type single crystal Cz silicon abraded by a pyramidal diamond in ethanol, methanol, acetone and de-ionized water was determined by measuring the cross-sectional areas of grooves of the circular and linear multiple-scratch tests. The wear rate depends on the loads on the diamond and is highest for ethanol and lowest for de-ionized water. The surface morphology of the grooves showed lateral and median cracks as well as a plastically deformed region. The hardness and fracture toughness are critical parameters that influence the wear rate. Microhardness tests were conducted to determine the hardness as influenced by fluids. Median cracks and the damage zone surrounding the indentations were also related to the fluid properties.

Danyluk, S.↗

Tuning electrochemical and transport processes to achieve extreme performance and efficiency in solid oxide cells

Solid oxide cells (SOCs) have important applications as fuel cells and electrolyzers. The application for storage of renewable electricity is also becoming increasingly relevant; however, it is difficult to meet stringent area-specific resistance (ASR) and long-term stability targets needed to achieve required efficiency and cost. Here we show a new SOC that utilizes a very thin Gd-doped ceria (GDC)/yttria-stabilized zirconia (YSZ) bi-layer electrolyte, Ni–YSZ cell support with enhanced porosity, and electrode surface modification using PrO x and GDC nanocatalysts to achieve unprecedented low ASR values < 0.1 Ω cm 2 , fuel cell power density ~3 W cm –2 , and electrolysis current density ~4 A cm –2 at 800 °C. Besides this exceptionally high performance, fuel cell and electrolysis life tests suggest very promising stability in fuel cell and steam electrolysis modes. Furthermore, electrochemical impedance spectroscopy analysis done using a novel impedance subtraction method shows how rate-limiting electrode processes are impacted by the new SOC materials and design.

25 ENERGY STORAGE↗

Functional Surface Coating to Enhance the Stability of LiNi 0.6 Mn 0.2 Co 0.2 O 2

Parasitic reactions are responsible for continuous performance loss during the normal operation and storage of lithium-ion batteries, particularly for those using nickel-rich cathode materials. Among many contributors, residual Li 2 CO 3 on the surface of nickel-rich cathodes plays a detrimental role in promoting parasitic reactions, and hence accelerates the performance loss of those cathode materials. In this work, a wet impregnation process was utilized to convert the detrimental Li 2 CO 3 and LiOH impurities into a beneficial functional surface coating comprising phosphates. Specifically, hydro-phosphates were used as the functional surface modification agents to mitigate the detrimental effect of surface residuals. The best electrochemical performance was achieved by modifying LiNi 0.6 Mn 0.2 Co 0.2 O 2 with a diluted dihydro-phosphate solution (pKa = 7.2), while the metal cation had a negligible impact on the electrochemical performance. This work provides a cheap and simple method for enabling the high performance of nickel-rich cathodes.

25 ENERGY STORAGE↗

The tectonic and volcanic history of Mercury as inferred from studies of scarps, ridges, troughs, and other lineaments

Tectonic and volcanic modification of the Mercurian surface is discussed, and nine landform classes are defined. An evolutionary chronology, based on reported interpretations of scarp, ridge, trough, and other lineament features, is presented, and the roles (in chronological order) of accretion and differentiation, tidal spindown, plains volcanism, heavy bombardment, cooling/contraction, Caloris impact, intense surface modification, basin subsidence, local plains volcanism, isostatic basin uplift, and light cratering are considered. The observational data were obtained by Mariner 10.

Dzurisin, D.↗

Surface property modification of semiconductors by fluid absorption

The University of Illinois at Chicago program to develop an understanding of the basic mechanisms of deformation during the lubricated cutting of silicon is discussed. Also described is the development of a nondestructive measurement technique for residual stress in a silicon sheet.

Danyluk, S.↗

Variable-Energy Ion Beams For Modification Of Surfaces

Beam of low-energy negative oxygen ions used to grow layer of silicon dioxide on silicon. Beam unique both in purity, contains no molecular oxygen or other charged species, and in low energy, which is insufficient to damage silicon by physically displacing atoms. Low-energy growth accomplished with help of ion-beam apparatus. Directs electrons into crosswise stream of gas, generating stream of negative ions. Pair of charged plates separates ions from accompanying electrons and diverts ion beam to target - silicon substrate. Diameter of beam at target 0.5 to 0.75 cm. Promises useful device to study oxidation of semiconductors and, in certain applications, to replace conventional oxidation processes.

Chutjian, Ara↗

Synthesis, Characterization, Topographical Modification, and Surface Properties of Copoly(Imide Siloxane)s

Novel copoly(imide siloxane)s were synthesized from commercially available aminopropyl terminated siloxane oligomers, aromatic dianhydrides, and diamines. This synthetic approach produced copolymers with well-defined siloxane blocks linked with imide units in a random fashion. The copoly(amide acid)s were characterized by solution viscosity and subsequently used to cast thin films followed by thermal imidization in an inert atmosphere. Thin films were characterized using contact angle goniometry, attenuated total reflection Fourier transform infrared spectroscopy, confocal and optical microscopy, and tensile testing. Adhesion of micronsized particles was determined quantitatively using a sonication device. The polydimethylsiloxane (PDMS) moieties lowered the copolymer surface energy due to migration of siloxane moieties to the film s surface, resulting in a notable reduction in particle adhesion. A further reduction in particle adhesion was achieved by introducing topographical features on a scale of several to tens of microns by a laser ablation technique.

Wohl, Christopher J.↗