Controlling the Charge State and Redox Properties of Supported Polyoxometalates via Soft Landing of Mass Selected Ions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gunaratne, Kalupathirannehelage Don D.; Johnson, Grant E.; Andersen, Amity

2014-12-04

We investigate the controlled deposition of Keggin polyoxometalate (POM) anions, PMo12O403- and PMo12O402-, onto different self-assembled monolayer (SAM) surfaces via soft landing of mass-selected ions. Utilizing in situ infrared reflection absorption spectroscopy (IRRAS), ex situ cyclic voltammetry (CV) and electronic structure calculations, we examine the structure and charge retention of supported multiply-charged POM anions and characterize the redox properties of the modified surfaces. SAMs of alkylthiol (HSAM), perfluorinated alkylthiol (FSAM), and alkylthiol terminated with NH3+ functional groups (NH3+SAM) are chosen as model substrates for soft landing to examine the factors which influence the immobilization and charge retention of multiply chargedmore » anionic molecules. The distribution of charge states of POMs on different SAM surfaces are determined by comparing the IRRAS spectra with vibrational spectra calculated using density functional theory (DFT). In contrast to the results obtained previously for multiply charged cations, soft landed anions are found to retain charge on all three SAM surfaces. This charge retention is attributed to the substantial electron binding energy of the POM anions. Investigation of redox properties by CV reveals that, while surfaces prepared by soft landing exhibit similar features to those prepared by adsorption of POM from solution, the soft landed POM2- has a pronounced shift in oxidation potential compared to POM3- for one of the redox couples. These results demonstrate that ion soft landing is uniquely suited for precisely controlled preparation of substrates with specific electronic and chemical properties that cannot be achieved using conventional deposition techniques.« less

Dynamics of spider glue adhesion: effect of surface energy and contact area

NASA Astrophysics Data System (ADS)

Amarpuri, Gaurav; Chen, Yizhou; Blackledge, Todd; Dhinojwala, Ali

Spider glue is a unique biological adhesive which is humidity responsive such that the adhesion continues to increase upto 100% relative humidity (RH) for some species. This is unlike synthetic adhesives that significantly drop in adhesion with an increase in humidity. However, most of adhesion data reported in literature have used clean hydrophilic glass substrate, unlike the hydrophobic, and charged insect cuticle surface that adheres to spider glue in nature. Previously, we have reported that the spider glue viscosity changes over five orders of magnitude with humidity. Here, we vary the surface energy and surface charge of the substrate to test the change in Larnioides cornutus spider glue adhesion with humidity. We find that an increase in both surface energy and surface charge density increases the droplet spreading and there exists an optimum droplet contact area where adhesion is maximized. Moreover, spider glue droplets act as reusable adhesive for low energy hydrophobic surface at the optimum humidity. These results explain why certain prey are caught more efficiently by spiders in their habitat. The mechanism by which spider species tune its glue adhesion for local prey capture can inspire new generation smart adhesives.

Nanowell-Trapped Charged Ligand-Bearing Nanoparticle Surfaces – A Novel Method of Enhancing Flow-Resistant Cell Adhesion

PubMed Central

Tran, Phat L.; Gamboa, Jessica R.; McCracken, Katherine E.; Riley, Mark R.

2014-01-01

Assuring cell adhesion to an underlying biomaterial surface is vital in implant device design and tissue engineering, particularly under circumstances where cells are subjected to potential detachment from overriding fluid flow. Cell-substrate adhesion is a highly regulated process involving the interplay of mechanical properties, surface topographic features, electrostatic charge, and biochemical mechanisms. At the nanoscale level the physical properties of the underlying substrate are of particular importance in cell adhesion. Conventionally, natural, pro-adhesive, and often thrombogenic, protein biomaterials are frequently utilized to facilitate adhesion. In the present study nanofabrication techniques are utilized to enhance the biological functionality of a synthetic polymer surface, polymethymethacrylate, with respect to cell adhesion. Specifically we examine the effect on cell adhesion of combining: 1. optimized surface texturing, 2. electrostatic charge and 3. cell adhesive ligands, uniquely assembled on the substrata surface, as an ensemble of nanoparticles trapped in nanowells. Our results reveal that the ensemble strategy leads to enhanced, more than simply additive, endothelial cell adhesion under both static and flow conditions. This strategy may be of particular utility for enhancing flow-resistant endothelialization of blood-contacting surfaces of cardiovascular devices subjected to flow-mediated shear. PMID:23225491

Protein Corona Composition of Superparamagnetic Iron Oxide Nanoparticles with Various Physico-Chemical Properties and Coatings

NASA Astrophysics Data System (ADS)

Sakulkhu, Usawadee; Mahmoudi, Morteza; Maurizi, Lionel; Salaklang, Jatuporn; Hofmann, Heinrich

2014-05-01

Because of their biocompatibility and unique magnetic properties, superparamagnetic iron oxide nanoparticles NPs (SPIONs) are recognized as some of the most prominent agents for theranostic applications. Thus, understanding the interaction of SPIONs with biological systems is important for their safe design and efficient applications. In this study, SPIONs were coated with 2 different polymers: polyvinyl alcohol polymer (PVA) and dextran. The obtained NPs with different surface charges (positive, neutral, and negative) were used as a model study of the effect of surface charges and surface polymer materials on protein adsorption using a magnetic separator. We found that the PVA-coated SPIONs with negative and neutral surface charge adsorbed more serum proteins than the dextran-coated SPIONs, which resulted in higher blood circulation time for PVA-coated NPs than the dextran-coated ones. Highly abundant proteins such as serum albumin, serotransferrin, prothrombin, alpha-fetoprotein, and kininogen-1 were commonly found on both PVA- and dextran-coated SPIONs. By increasing the ionic strength, soft- and hard-corona proteins were observed on 3 types of PVA-SPIONs. However, the tightly bound proteins were observed only on negatively charged PVA-coated SPIONs after the strong protein elution.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yafyasov, A. M., E-mail: yafyasov@gmail.com; Bogevolnov, V. B.; Ryumtsev, E. I.

A semiconductor—organic-insulator system with spatially distributed charge is created with a uniquely low density of fast surface states (N{sub ss}) at the interface. A system with N{sub ss} ≈ 5 × 10{sup 10} cm{sup –2} is obtained for the example of n-Ge and the physical characteristics of the interface are measured for this system with liquid and metal field electrodes. For a system with an organic insulator, the range of variation of the surface potential from enrichment of the space-charge region of the semiconductor to the inversion state is first obtained without changing the mechanism of interaction between the adsorbedmore » layer and the semiconductor surface. The effect of enhanced polarization of the space-charge region of the semiconductor occurs due to a change in the spatial structure of mobile charge in the organic dielectric layer. The system developed in the study opens up technological opportunities for the formation of a new generation of electronic devices based on organic film structures and for experimental modeling of the electronic properties of biological membranes.« less

Fluorescent Nanocrystals Reveal Regulated Portals of Entry into and Between the Cells of Hydra

PubMed Central

Tortiglione, Claudia; Quarta, Alessandra; Malvindi, Maria Ada; Tino, Angela; Pellegrino, Teresa

2009-01-01

Initially viewed as innovative carriers for biomedical applications, with unique photophysical properties and great versatility to be decorated at their surface with suitable molecules, nanoparticles can also play active roles in mediating biological effects, suggesting the need to deeply investigate the mechanisms underlying cell-nanoparticle interaction and to identify the molecular players. Here we show that the cell uptake of fluorescent CdSe/CdS quantum rods (QRs) by Hydra vulgaris, a simple model organism at the base of metazoan evolution, can be tuned by modifying nanoparticle surface charge. At acidic pH, amino-PEG coated QRs, showing positive surface charge, are actively internalized by tentacle and body ectodermal cells, while negatively charged nanoparticles are not uptaken. In order to identify the molecular factors underlying QR uptake at acidic pH, we provide functional evidence of annexins involvement and explain the QR uptake as the combined result of QR positive charge and annexin membrane insertion. Moreover, tracking QR labelled cells during development and regeneration allowed us to uncover novel intercellular trafficking and cell dynamics underlying the remarkable plasticity of this ancient organism. PMID:19888325

Study of digital charge coupled devices

NASA Technical Reports Server (NTRS)

Wilson, D. D.; Young, V. F.

1980-01-01

Charge coupled devices represent unique usage of the metal oxide semiconductor concept. These devices can sample an AC signal at the input, transfer charge proportional to this signal through the CCD shift register and then provide an output of the same frequency and shape as the input. The delay time between input and output is controlled by the CCD operating frequency and the number of stages in the shift resistor. This work is a reliability evaluation of the buried channel and surface channel CCD technologies. The constructions are analyzed, failure modes are described, and test results are reported.

Unique Three-Dimensional InP Nanopore Arrays for Improved Photoelectrochemical Hydrogen Production.

PubMed

Li, Qiang; Zheng, Maojun; Ma, Liguo; Zhong, Miao; Zhu, Changqing; Zhang, Bin; Wang, Faze; Song, Jingnan; Ma, Li; Shen, Wenzhong

2016-08-31

Ordered three-dimensional (3D) nanostructure arrays hold promise for high-performance energy harvesting and storage devices. Here, we report the fabrication of InP nanopore arrays (NPs) in unique 3D architectures with excellent light trapping characteristic and large surface areas for use as highly active photoelectrodes in photoelectrochemical (PEC) hydrogen evolution devices. The ordered 3D NPs were scalably synthesized by a facile two-step etching process of (1) anodic etching of InP in neutral 3 M NaCl electrolytes to realize nanoporous structures and (2) wet chemical etching in HCl/H3PO4 (volume ratio of 1:3) solutions for removing the remaining top irregular layer. Importantly, we demonstrated that the use of neutral electrolyte of NaCl instead of other solutions, such as HCl, in anodic etching of InP can significantly passivate the surface states of 3D NPs. As a result, the maximum photoconversion efficiency obtained with ∼15.7 μm thick 3D NPs was 0.95%, which was 7.3 and 1.4 times higher than that of planar and 2D NPs. Electrochemical impedance spectroscopy and photoluminescence analyses further clarified that the improved PEC performance was attributed to the enhanced charge transfer across 3D NPs/electrolyte interfaces, the improved charge separation at 3D NPs/electrolyte junction, and the increased PEC active surface areas with our unique 3D NP arrays.

Ligand and coactivator identity determines the requirement of the charge clamp for coactivation of the peroxisome proliferator-activated receptor gamma.

PubMed

Wu, Yifei; Chin, William W; Wang, Yong; Burris, Thomas P

2003-03-07

The activation function 2 (AF-2)-dependent recruitment of coactivator is essential for gene activation by nuclear receptors. We show that the peroxisome proliferator-activated receptor gamma (PPARgamma) (NR1C3) coactivator-1 (PGC-1) requires both the intact AF-2 domain of PPARgamma and the LXXLL domain of PGC-1 for ligand-dependent and ligand-independent interaction and coactivation. Although the AF-2 domain of PPARgamma is absolutely required for PGC-1-mediated coactivation, this coactivator displayed a unique lack of requirement for the charge clamp of the ligand-binding domain of the receptor that is thought to be essential for LXXLL motif recognition. The mutation of a single serine residue adjacent to the core LXXLL motif of PGC-1 led to restoration of the typical charge clamp requirement. Thus, the unique structural features of the PGC-1 LXXLL motif appear to mediate an atypical mode of interaction with PPARgamma. Unexpectedly, we discovered that various ligands display variability in terms of their requirement for the charge clamp of PPARgamma for coactivation by PGC-1. This ligand-selective variable requirement for the charge clamp was coactivator-specific. Thus, distinct structural determinants, which may be unique for a particular ligand, are utilized by the receptor to recognize the coactivator. Our data suggest that even subtle differences in ligand structure are perceived by the receptor and translated into a unique display of the coactivator-binding surface of the ligand-binding domain, allowing for differential recognition of coactivators that may underlie distinct pharmacological profiles observed for ligands of a particular nuclear receptor.

New Techniques to Evaluate the Incendiary Behavior of Insulators

NASA Technical Reports Server (NTRS)

Buhler, Charles; Calle, Carlos; Clements, Sid; Trigwell, Steve; Ritz, Mindy

2008-01-01

New techniques for evaluating the incendiary behavior of insulators is presented. The onset of incendive brush discharges in air is evaluated using standard spark probe techniques for the case simulating approaches of an electrically grounded sphere to a charged insulator in the presence of a flammable atmosphere. However, this standard technique is unsuitable for the case of brush discharges that may occur during the charging-separation process for two insulator materials. We present experimental techniques to evaluate this hazard in the presence of a flammable atmosphere which is ideally suited to measure the incendiary nature of micro-discharges upon separation, a measurement never before performed. Other measurement techniques unique to this study include; surface potential measurements of insulators before, during and after contact and separation, as well as methods to verify fieldmeter calibrations using a charge insulator surface opposed to standard high voltage plates. Key words: Kapton polyimide film, incendiary discharges, brush discharges, contact and frictional electrification, ignition hazards, insulators, contact angle, surface potential measurements.

Reduced graphene oxide wrapped Ag nanostructures for enhanced SERS activity

NASA Astrophysics Data System (ADS)

Nair, Anju K.; Kala, M. S.; Thomas, Sabu; Kalarikkal, Nandakumar

2018-04-01

Graphene - metal nanoparticle hybrids have received great attention due to their unique electronic properties, large specific surface area, very high conductivity and more charge transfer. Thus, it is extremely advantages to develop a simple and efficient process to disperse metal nanostructures over the surface of graphene sheets. Herein, we report a hydrothermal assisted strategy for developing reduced graphene oxide /Ag nanomorphotypes (cube, wire) for surface enhanced Raman scattering (SERS) applications, considering the advantages of synergistic effect of graphene and plasmonic properties of Ag nanomorphotypes.

Extracting dielectric fixed charge density on highly doped crystalline-silicon surfaces using photoconductance measurements

NASA Astrophysics Data System (ADS)

To, A.; Hoex, B.

2017-11-01

A novel method for the extraction of fixed interface charge, Qf, and the surface recombination parameters, Sn0 and Sp0, from the injection-level dependent effective minority carrier lifetime measurements is presented. Unlike conventional capacitance-voltage measurements, this technique can be applied to highly doped surfaces provided the surface carrier concentration transitions into strong depletion or inversion with increased carrier injection. By simulating the injection level dependent Auger-corrected inverse lifetime curve of symmetrically passivated and diffused samples after sequential annealing and corona charging, it was revealed that Qf, Sn0, and Sp0 have unique signatures. Therefore, these important electronic parameters, in some instances, can independently be resolved. Furthermore, it was shown that this non-linear lifetime behaviour is exhibited on both p-type and n-type diffused inverted surfaces, by demonstrating the approach with phosphorous diffused n+pn+ structures and boron diffused p+np+ structures passivated with aluminium oxide (AlOx) and silicon nitride, respectively (SiNx). The results show that the approximation of a mid-gap Shockley-Read-Hall defect level with equal capture cross sections is able to, in the samples studied in this work, reproduce the observed injection level dependent lifetime behaviour.

Charging and Discharging of Lichtenberg Electrets

NASA Astrophysics Data System (ADS)

Wood, Monika

The research presented here describes a unique way to deposit a large amount of charge onto the surface of a thin dielectric sheet to create a Lichtenberg electret that can be discharged elsewhere to form spectacular Lichtenberg figures. This study examines how the amount of charge deposited onto the surface, the geometry of the probes, and the type of material used can all impact the formation of the Lichtenberg figures. Photographs of the Lichtenberg figures were taken and used to determine the voltage, current, and energy released during each discharge. It was found that a single discharge can release 0.49 J of energy in 1.24 micros for a Lichtenberg figure that covers approximately 500 cm. 2. Lichtenberg figures can be used to characterize high-voltage surgeson power lines, to diagnose lightning strike victims, to analyze electrical breakdown of insulating materials, for artistic purposes, and for similar applications where pulsed capacitors are commonly used.

Operando Positron Annihilation Gamma Spectrometer (OPAGS)

NASA Astrophysics Data System (ADS)

Satyal, S.; Shastry, K.; Mukherjee, S.; Weiss, A. H.

2009-03-01

Surface properties measured under UHV conditions cannot be extended to surfaces interacting with gases under realistic pressures due to surface reconstruction and other strong perturbations of the surface. Surface probing techniques require UHV conditions to perform efficiently and avoid data loss due to scattering of outgoing particles. This poster describes the design of an Operando Positron Annihilation Gamma Spectrometer (OPAGS) currently under construction at the University of Texas at Arlington. The new system will be capable of obtaining surface and defect specific chemical and charge state information from surfaces under realistic pressures. Differential pumping will be used to maintain the sample in a gas environment while the rest of the beam is under UHV. Elemental content of the surface interacting with the gas environment will be determined from the Doppler broadened gamma spectra. This system will also include a time of flight (TOF) Auger spectrometer which correlates with the results of the Doppler measurements at lower pressures. By employing the unique capabilities of OPAGS together with those of the TOF PAES spectroscopy the charge transfer mechanisms at the surface in catalytic systems can be understood.

On the application potential of gold nanoparticles in nanoelectronics and biomedicine.

PubMed

Homberger, Melanie; Simon, Ulrich

2010-03-28

Ligand-stabilized gold nanoparticles (AuNPs) are of high interest to research dedicated to future technologies such as nanoelectronics or biomedical applications. This research interest arises from the unique size-dependent properties such as surface plasmon resonance or Coulomb charging effects. It is shown here how the unique properties of individual AuNPs and AuNP assemblies can be used to create new functional materials for applications in a technical or biological environment. While the term technical environment focuses on the potential use of AuNPs as subunits in nanoelectronic devices, the term biological environment addresses issues of toxicity and novel concepts of controlling biomolecular reactions on the surface of AuNPs.

Experimental and modeling study on charge storage/transfer mechanism of graphene-based supercapacitors

NASA Astrophysics Data System (ADS)

Ban, Shuai; Jing, Xie; Zhou, Hongjun; Zhang, Lei; Zhang, Jiujun

2014-12-01

A symmetrical graphene-based supercapacitor is constructed for studying the charge-transfer mechanism within the graphene-based electrodes using both experiment measurements and molecular simulation. The in-house synthesized graphene is characterized by XRD, SEM and BET measurements for morphology and surface area. It is observed that the electric capacity of graphene electrode can be reduced by both high internal resistance and limited mass transfer. Computer modeling is conducted at the molecular level to characterize the diffusion behavior of electrolyte ions to the interior of electrode with emphasis on the unique 2D confinement imposed by graphene layers. Although graphene powder poses a moderate internal surface of 400 m2 g-1, the capacitance performance of graphene electrode can be as good as that of commercial activated carbon which has an overwhelming surface area of 1700 m2 g-1. An explanation to this abnormal correlation is that graphene material has an intrinsic capability of adaptively reorganizing its microporous structure in response to intercalation of ions and immergence of electrolyte solvent. The accessible surface of graphene is believed to be dramatically enlarged for ion adsorption during the charging process of capacitor.

Supported Silver Nanoparticle and Near-Interface Solution Dynamics in a Deep Eutectic Solvent

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hammons, Joshua A.; Ustarroz, Jon; Muselle, Thibault

2016-01-28

Type III deep eutectic solvents (DES) have attracted significant interest as both environmentally friendly and functional solvents that are, in some ways, advantageous to traditional aqueous systems. While these solvents continue to produce remarkable thin films and nanoparticle assemblies, their interactions with metallic surfaces are complex and difficult to manipulate. In this study, the near-surface region (2–600 nm) of a carbon surface is investigated immediately following silver nanoparticle nucleation and growth. This is accomplished, in situ, using a novel grazing transmission small-angle X-ray scattering approach with simultaneous voltammetry and electrochemical impedance spectroscopy. With this physical and electrochemical approach, the timemore » evolution of three distinct surface interaction phenomena is observed: aggregation and coalescence of Ag nanoparticles, multilayer perturbations induced by nonaggregated Ag nanoparticles, and a stepwise transport of dissolved Ag species from the carbon surface. The multilayer perturbations contain charge-separated regions of positively charged choline-ethylene and negatively charged Ag and Cl species. Both aggregation-coalescence and the stepwise decrease in Ag precursor near the surface are observed to be very slow (~2 h) processes, as both ion and particle transport are significantly impeded in a DES as compared to aqueous electrolytes. Finally, altogether, this study shows how the unique chemistry of the DES changes near the surface and in the presence of nanoparticles that adsorb the constituent species.« less

Fabrication of Periodic Gold Nanocup Arrays Using Colloidal Lithography

DOE Office of Scientific and Technical Information (OSTI.GOV)

DeVetter, Brent M.; Bernacki, Bruce E.; Bennett, Wendy D.

Within recent years, the field of plasmonics has exploded as researchers have demonstrated exciting applications related to chemical and optical sensing in combination with new nanofabrication techniques. A plasmon is a quantum of charge density oscillation that lends nanoscale metals such as gold and silver unique optical properties. In particular, gold and silver nanoparticles exhibit localized surface plasmon resonances—collective charge density oscillations on the surface of the nanoparticle—in the visible spectrum. Here, we focus on the fabrication of periodic arrays of anisotropic plasmonic nanostructures. These half-shell (or nanocup) structures can exhibit additional unique light-bending and polarization dependent optical properties thatmore » simple isotropic nanostructures cannot. Researchers are interested in the fabrication of periodic arrays of nanocups for a wide variety of applications such as low-cost optical devices, surface-enhanced Raman scattering, and tamper indication. We present a scalable technique based on colloidal lithography in which it is possible to easily fabricate large periodic arrays of nanocups using spin-coating and self-assembled commercially available polymeric nanospheres. Electron microscopy and optical spectroscopy from the visible to near-IR was performed to confirm successful nanocup fabrication. We conclude with a demonstration of the transfer of nanocups to a flexible, conformal adhesive film.« less

Investigation of protein selectivity in multimodal chromatography using in silico designed Fab fragment variants.

PubMed

Karkov, Hanne Sophie; Krogh, Berit Olsen; Woo, James; Parimal, Siddharth; Ahmadian, Haleh; Cramer, Steven M

2015-11-01

In this study, a unique set of antibody Fab fragments was designed in silico and produced to examine the relationship between protein surface properties and selectivity in multimodal chromatographic systems. We hypothesized that multimodal ligands containing both hydrophobic and charged moieties would interact strongly with protein surface regions where charged groups and hydrophobic patches were in close spatial proximity. Protein surface property characterization tools were employed to identify the potential multimodal ligand binding regions on the Fab fragment of a humanized antibody and to evaluate the impact of mutations on surface charge and hydrophobicity. Twenty Fab variants were generated by site-directed mutagenesis, recombinant expression, and affinity purification. Column gradient experiments were carried out with the Fab variants in multimodal, cation-exchange, and hydrophobic interaction chromatographic systems. The results clearly indicated that selectivity in the multimodal system was different from the other chromatographic modes examined. Column retention data for the reduced charge Fab variants identified a binding site comprising light chain CDR1 as the main electrostatic interaction site for the multimodal and cation-exchange ligands. Furthermore, the multimodal ligand binding was enhanced by additional hydrophobic contributions as evident from the results obtained with hydrophobic Fab variants. The use of in silico protein surface property analyses combined with molecular biology techniques, protein expression, and chromatographic evaluations represents a previously undescribed and powerful approach for investigating multimodal selectivity with complex biomolecules. © 2015 Wiley Periodicals, Inc.

Low-dimensional carbon and MXene-based electrochemical capacitor electrodes.

PubMed

Yoon, Yeoheung; Lee, Keunsik; Lee, Hyoyoung

2016-04-29

Due to their unique structure and outstanding intrinsic physical properties such as extraordinarily high electrical conductivity, large surface area, and various chemical functionalities, low-dimension-based materials exhibit great potential for application in electrochemical capacitors (ECs). The electrical properties of electrochemical capacitors are determined by the electrode materials. Because energy charge storage is a surface process, the surface properties of the electrode materials greatly influence the electrochemical performance of the cell. Recently, graphene, a single layer of sp(2)-bonded carbon atoms arrayed into two-dimensional carbon nanomaterial, has attracted wide interest as an electrode material for electrochemical capacitor applications due to its unique properties, including a high electrical conductivity and large surface area. Several low-dimensional materials with large surface areas and high conductivity such as onion-like carbons (OLCs), carbide-derived carbons (CDCs), carbon nanotubes (CNTs), graphene, metal hydroxide, transition metal dichalcogenides (TMDs), and most recently MXene, have been developed for electrochemical capacitors. Therefore, it is useful to understand the current issues of low-dimensional materials and their device applications.

Coarse-graining, Electrostatics and pH effects in phospholipid systems

NASA Astrophysics Data System (ADS)

Travesset, Alex; Vangaveti, Sweta

2010-03-01

We introduce a minimal free energy describing the interaction of charged groups and counterions including both classical electrostatic and specific interactions. The predictions of the model are compared against the standard model for describing ions next to charged interfaces, consisting of Poisson-Boltzmann theory with additional constants describing ion binding, which are specific to the counterion and the interfacial charge (``chemical binding''). It is shown that the ``chemical'' model can be appropriately described by an underlying ``physical'' model over several decades in concentration, but the extracted binding constants are not uniquely defined, as they differ depending on the particular observable quantity being studied. It is also shown that electrostatic correlations for divalent (or higher valence) ions enhance the surface charge by increasing deprotonation, an effect not properly accounted within chemical models. The model is applied to the charged phospholipids phosphatidylserine, Phosphatidc acid and Phosphoinositides and implications for different biological processes are discussed.

Electronic structure and surface properties of MgB2(0001) upon oxygen adsorption

NASA Astrophysics Data System (ADS)

Kim, Chang-Eun; Ray, Keith G.; Bahr, David F.; Lordi, Vincenzo

2018-05-01

We use density-functional theory to investigate the bulk and surface properties of MgB2. The unique bonding structure of MgB2 is investigated by Bader's atoms-in-molecules, charge density difference, and occupancy projected band structure analyses. Oxygen adsorption on the charge-depleted surfaces of MgB2 is studied by a surface potential energy mapping method, reporting a complete map including low-symmetry binding sites. The B-terminated MgB2(0001) demonstrates reconstruction of the graphenelike B layer, and the reconstructed geometry exposes a threefold site of the subsurface Mg, making it accessible from the surface. Detailed reconstruction mechanisms are studied by simulated annealing method based on ab initio molecular dynamics and nudged elastic band calculations. The surface clustering of B atoms significantly modifies the B 2 p states to occupy low energy valence states. The present paper emphasizes that a thorough understanding of the surface phase may explain an apparent inconsistency in the experimental surface characterization of MgB2. Furthermore, these results suggest that the surface passivation can be an important technical challenge when it comes to development of a superconducting device using MgB2.

Manipulating semiconductor colloidal stability through doping.

PubMed

Fleharty, Mark E; van Swol, Frank; Petsev, Dimiter N

2014-10-10

The interface between a doped semiconductor material and electrolyte solution is of considerable fundamental interest, and is relevant to systems of practical importance. Both adjacent domains contain mobile charges, which respond to potential variations. This is exploited to design electronic and optoelectronic sensors, and other enabling semiconductor colloidal materials. We show that the charge mobility in both phases leads to a new type of interaction between semiconductor colloids suspended in aqueous electrolyte solutions. This interaction is due to the electrostatic response of the semiconductor interior to disturbances in the external field upon the approach of two particles. The electrostatic repulsion between two charged colloids is reduced from the one governed by the charged groups present at the particles surfaces. This type of interaction is unique to semiconductor particles and may have a substantial effect on the suspension dynamics and stability.

Using DNA-labelled nano- and microparticles to track particle transport in the environment

NASA Astrophysics Data System (ADS)

McNew, Coy; Wang, Chaozi; Dahlke, Helen; Lyon, Steve; Walter, Todd

2017-04-01

By utilizing bio-molecular nanotechnology developed for nano-medicines and drug delivery, we are able to produce DNA-labelled nano- and microparticle tracers for use in a myriad of environmental systems. The use of custom sequenced DNA allows for the fabrication of an enormous number of uniquely labelled tracers with identical transport properties (approximately 1.61 x 1060 unique sequences), each independently quantifiable, that can be applied simultaneously in any hydrologic system. By controlling the fabrication procedure to produce particles of custom size and charge, we are able to tag each size-charge combination uniquely in order to directly probe the effect of these variables on the transport properties of the particles. Here we present our methods for fabrication, extraction, and analysis of the DNA nano- and microparticle tracers, along with results from several successful applications of the tracers, including transport and retention analysis at the lab, continuum, and field scales. To date, our DNA-labelled nano- and microparticle tracers have proved useful in surface and subsurface water applications, soil retention, and even subglacial flow pathways. The range of potential applications continue to prove nearly limitless.

Investigating local degradation and thermal stability of charged nickel-based cathode materials through real-time electron microscopy.

PubMed

Hwang, Sooyeon; Kim, Seung Min; Bak, Seong-Min; Cho, Byung-Won; Chung, Kyung Yoon; Lee, Jeong Yong; Chang, Wonyoung; Stach, Eric A

2014-09-10

In this work, we take advantage of in situ transmission electron microscopy (TEM) to investigate thermally induced decomposition of the surface of Li(x)Ni(0.8)Co(0.15)Al(0.05)O2 (NCA) cathode materials that have been subjected to different states of charge (SOC). While uncharged NCA is stable up to 400 °C, significant changes occur in charged NCA with increasing temperature. These include the development of surface porosity and changes in the oxygen K-edge electron energy loss spectra, with pre-edge peaks shifting to higher energy losses. These changes are closely related to O2 gas released from the structure, as well as to phase changes of NCA from the layered structure to the disordered spinel structure, and finally to the rock-salt structure. Although the temperatures where these changes initiate depend strongly on the state of charge, there also exist significant variations among particles with the same state of charge. Notably, when NCA is charged to x = 0.33 (the charge state that is the practical upper limit voltage in most applications), the surfaces of some particles undergo morphological and oxygen K-edge changes even at temperatures below 100 °C, a temperature that electronic devices containing lithium ion batteries (LIB) can possibly see during normal operation. Those particles that experience these changes are likely to be extremely unstable and may trigger thermal runaway at much lower temperatures than would be usually expected. These results demonstrate that in situ heating experiments are a unique tool not only to study the general thermal behavior of cathode materials but also to explore particle-to-particle variations, which are sometimes of critical importance in understanding the performance of the overall system.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gürel, Hikmet Hakan, E-mail: hhakan.gurel@kocaeli.edu.tr; Salmankurt, Bahadır

Graphene as a 2D material has unique chemical and electronic properties. Because of its unique physical, chemical, and electronic properties, its interesting shape and size make it a promising nanomaterial in many biological applications. However, the lower water-solubility and the irreversible aggregation due to the strong π-π stacking hinder the wide application of graphene nanosheets in biomedical field. Thus, graphene oxide (GO), one derivative of graphene, has been used more frequently in the biological system owing to its relatively higher water solubility and biocompatibility. Recently, it has been demonstrated that nanomaterials with different functional groups on the surface can bemore » used to bind the drug molecules with high affinity. GO has different functional groups such as H, OH and O on its surface; it can be a potential candidate as a drug carrier. The interactions of biomolecules and graphene like structures are long-ranged and very weak. Development of new techniques is very desirable for design of bioelectronics sensors and devices. In this work, we present first-principles spin polarized calculations within density functional theory to calculate effects of charging on DNA/RNA nucleobases on graphene oxide. It is shown that how modify structural and electronic properties of nucleobases on graphene oxide by applied charging.« less

Finite-element 3D simulation tools for high-current relativistic electron beams

NASA Astrophysics Data System (ADS)

Humphries, Stanley; Ekdahl, Carl

2002-08-01

The DARHT second-axis injector is a challenge for computer simulations. Electrons are subject to strong beam-generated forces. The fields are fully three-dimensional and accurate calculations at surfaces are critical. We describe methods applied in OmniTrak, a 3D finite-element code suite that can address DARHT and the full range of charged-particle devices. The system handles mesh generation, electrostatics, magnetostatics and self-consistent particle orbits. The MetaMesh program generates meshes of conformal hexahedrons to fit any user geometry. The code has the unique ability to create structured conformal meshes with cubic logic. Organized meshes offer advantages in speed and memory utilization in the orbit and field solutions. OmniTrak is a versatile charged-particle code that handles 3D electric and magnetic field solutions on independent meshes. The program can update both 3D field solutions from the calculated beam space-charge and current-density. We shall describe numerical methods for orbit tracking on a hexahedron mesh. Topics include: 1) identification of elements along the particle trajectory, 2) fast searches and adaptive field calculations, 3) interpolation methods to terminate orbits on material surfaces, 4) automatic particle generation on multiple emission surfaces to model space-charge-limited emission and field emission, 5) flexible Child law algorithms, 6) implementation of the dual potential model for 3D magnetostatics, and 7) assignment of charge and current from model particle orbits for self-consistent fields.

Analysis of Surface Electric Field Measurements from an Array of Electric Field Mills

NASA Astrophysics Data System (ADS)

Lucas, G.; Thayer, J. P.; Deierling, W.

2016-12-01

Kennedy Space Center (KSC) has operated an distributed array of over 30 electric field mills over the past 18 years, providing a unique data set of surface electric field measurements over a very long timespan. In addition to the electric field instruments there are many meteorological towers around KSC that monitor the local meteorological conditions. Utilizing these datasets we have investigated and found unique spatial and temporal signatures in the electric field data that are attributed to local meteorological effects and the global electric circuit. The local and global scale influences on the atmospheric electric field will be discussed including the generation of space charge from the ocean surf, local cloud cover, and a local enhancement in the electric field that is seen at sunrise.

Modeling of protein-anion exchange resin interaction for the human growth hormone charge variants.

PubMed

Lapelosa, Mauro; Patapoff, Thomas W; Zarraga, Isidro E

2015-12-01

Modeling ion exchange chromatography (IEC) behavior has generated significant interest because of the wide use of IEC as an analytical technique as well as a preparative protein purification process; indeed there is a need for better understanding of what drives the unique behavior of protein charge variants. We hypothesize that a complex protein molecule, which contains both hydrophobic and charged moieties, would interact strongly with an in silico designed resin through charged electrostatic patches on the surface of the protein. In the present work, variants of recombinant human growth hormone that mimic naturally-occurring deamidation products were produced and characterized in silico. The study included these four variants: rhGH, N149D, N152D, and N149D/N152D. Poisson-Boltzmann calculations were used to determine surface electrostatic potential. Metropolis Monte Carlo simulations were carried out with the resulting variants to simulate IEC systems, examining the free energy of the interaction of the protein with an in silico anion exchange column represented by polylysine polypeptide. The results show that the charge variants have different average binding energies and the free energy of interaction can be used to predict the retention time for the different variants. Copyright © 2015 Elsevier B.V. All rights reserved.

Enhanced Raman Scattering on In-plane Anisotropic Layered Materials

DOE PAGES

Liang, Liangbo; Meunier, Vincent; Sumpter, Bobby G.; ...

2015-11-19

Surface-enhanced Raman scattering (SERS) on two-dimensional (2D) layered materials has provided a unique platform to study the chemical mechanism (CM) of the enhancement due to its natural separation from electromagnetic enhancement. The CM stems from the basic charge interactions between the substrate and molecules. Despite the extensive studies of the energy alignment between 2D materials and molecules, an understanding of how the electronic properties of the substrate are explicitly involved in the charge interaction is still unclear. Lately, a new group of 2D layered materials with anisotropic structure, including orthorhombic black phosphorus (BP) and triclinic rhenium disulphide (ReS2), has attractedmore » great interest due to their unique anisotropic electrical and optical properties. Herein, we report a unique anisotropic Raman enhancement on few-layered BP and ReS2 using copper phthalocyanine (CuPc) molecules as a Raman probe, which is absent on isotropic graphene and h-BN. According to detailed Raman tensor analysis and density functional theory calculations, anisotropic charge interactions due to the anisotropic carrier mobilities of the 2D materials are responsible for the angular dependence of the Raman enhancement. Our findings not only provide new insights into the CM process in SERS, but also open up new avenues for the exploration and application of the electronic properties of anisotropic 2D layered materials.« less

Electrospray Charging of Minerals: Surface Chemistry and Applications to High-Velocity Microparticle Impacts

NASA Astrophysics Data System (ADS)

Daly, T.; Call, S.; Austin, D. E.

2010-12-01

Electrospray is a soft ionization technique commonly used to charge large biomolecules; it has, however, also been applied to inorganic compounds. We are extending this technique to mineral microparticles. Electrospray-charged mineral microparticles are interesting in the context of surface science because surface chemistry dictates where and how charge carriers can bond to mineral surfaces. In addition, using electrospray to charge mineral particles allows these particles to be electrostatically accelerated as projectiles in high- and hyper-velocity impacts. Since current techniques for producing high- and hyper-velocity microparticle impacts are largely limited to metal or metal-coated projectiles, using minerals as projectiles is a significant innovation. Electrospray involves three steps: creation of charged droplets containing solute/particles, evaporation and bifurcation of droplets, and desolvation of the solute/particles. An acidified solution is slowly pumped through a needle in a strong DC field, which causes the solution to break into tiny, charged droplets laden with protons. Solvent evaporates from the electrosprayed droplets as they move through the electric field toward a grounded plate, causing the charge on the droplet to increase relative to its mass. When the electrosprayed droplet’s charge becomes such that the droplet is no longer stable, it bifurcates, and each of the resulting droplets carries some of the original droplet’s charge. Evaporation and bifurcation continues until the solute particle is completely desolvated. The result is a protonated solute molecule or particle. We built an instrument that electrosprays particles into vacuum and measures them using an image charge detector. Mineral microparticles were prepared by grinding natural mineral samples to ~2 µm diameter. These microparticles are then added to a 4:1 methanol:water solution to create a 0.005% w/v suspension. The suspension is electrosprayed into vacuum, where the charge detector measures the electrosprayed mineral particles’ speed and charge. Quartz microparticles have been successfully electrosprayed. Variation in quartz microparticles’ charge as a function of pH is being evaluated. In addition, we are studying how to completely desolvate electrosprayed mineral particles. Desolvation is not trivial and often requires more than the passive passage of the droplets from the needle to the grounded plate and into vacuum. We are testing two desolvation methods: a heated beam tube and a heated capillary. Preliminary data suggests we have achieved complete desolvation with a hot beam tube. Although quartz’s surface chemistry is rather unique, successful electrospray of quartz microparticles strongly suggests that other minerals may also be electrosprayed. We are preparing olivine samples for electrospray. In addition, an instrument that creates high-velocity microparticle impacts using electrospray-charged mineral microparticles is being developed. This instrument will not only permit minerals to be used as projectiles, but also allows direction characterization of chemical speciation occurring during microparticle impacts.

Extended hierarchical solvent perturbations from curved surfaces of mesoporous silica particles in a deep eutectic solvent.

PubMed

Hammons, Joshua A; Zhang, Fan; Ilavsky, Jan

2018-06-15

Many applications of deep eutectic solvents (DES) rely on exploitation of their unique yet complex liquid structures. Due to the ionic nature of the DES components, their diffuse structures are perturbed in the presence of a charged surface. We hypothesize that it is possible to perturb the bulk DES structure far (>100 nm) from a curved, charged surface with mesoscopic dimensions. We performed in situ, synchrotron-based ultra-small angle X-ray scattering (USAXS) experiments to study the solvent distribution near the surface of charged mesoporous silica particles (MPS) (≈0.5 µm in diameter) suspended in both water and a common type of DES (1:2 choline Cl-:ethylene glycol). A careful USAXS analysis reveals that the perturbation of electron density distribution within the DES extends ≈1 μm beyond the particle surface, and that this perturbation can be manipulated by the addition of salt ions (AgCl). The concentration of the pore-filling fluid is greatly reduced in the DES. Notably, we extracted the real-space structures of these fluctuations from the USAXS data using a simulated annealing approach that does not require a priori knowledge about the scattering form factor, and can be generalized to a wide range of complex small-angle scattering problems. Copyright © 2018 Elsevier Inc. All rights reserved.

High reduction of interfacial charge recombination in colloidal quantum dot solar cells by metal oxide surface passivation.

PubMed

Chang, Jin; Kuga, Yuki; Mora-Seró, Iván; Toyoda, Taro; Ogomi, Yuhei; Hayase, Shuzi; Bisquert, Juan; Shen, Qing

2015-03-12

Bulk heterojunction (BHJ) solar cells based on colloidal QDs and metal oxide nanowires (NWs) possess unique and outstanding advantages in enhancing light harvesting and charge collection in comparison to planar architectures. However, the high surface area of the NW structure often brings about a large amount of recombination (especially interfacial recombination) and limits the open-circuit voltage in BHJ solar cells. This problem is solved here by passivating the surface of the metal oxide component in PbS colloidal quantum dot solar cells (CQDSCs). By coating thin TiO2 layers onto ZnO-NW surfaces, the open-circuit voltage and power conversion efficiency have been improved by over 40% in PbS CQDSCs. Characterization by transient photovoltage decay and impedance spectroscopy indicated that the interfacial recombination was significantly reduced by the surface passivation strategy. An efficiency as high as 6.13% was achieved through the passivation approach and optimization for the length of the ZnO-NW arrays (device active area: 16 mm2). All solar cells were tested in air, and exhibited excellent air storage stability (without any performance decline over more than 130 days). This work highlights the significance of metal oxide passivation in achieving high performance BHJ solar cells. The charge recombination mechanism uncovered in this work could shed light on the further improvement of PbS CQDSCs and/or other types of solar cells.

Influence of the electron-cation interaction on electron mobility in dye-sensitized ZnO and TiO2 nanocrystals: a study using ultrafast terahertz spectroscopy.

PubMed

Nemec, H; Rochford, J; Taratula, O; Galoppini, E; Kuzel, P; Polívka, T; Yartsev, A; Sundström, V

2010-05-14

Charge transport and recombination in nanostructured semiconductors are poorly understood key processes in dye-sensitized solar cells. We have employed time-resolved spectroscopies in the terahertz and visible spectral regions supplemented with Monte Carlo simulations to obtain unique information on these processes. Our results show that charge transport in the active solar cell material can be very different from that in nonsensitized semiconductors, due to strong electrostatic interaction between injected electrons and dye cations at the surface of the semiconductor nanoparticle. For ZnO, this leads to formation of an electron-cation complex which causes fast charge recombination and dramatically decreases the electron mobility even after the dissociation of the complex. Sensitized TiO2 does not suffer from this problem due to its high permittivity efficiently screening the charges.

Impact of speciation on the electron charge transfer properties of nanodiamond drug carriers

NASA Astrophysics Data System (ADS)

Sun, Baichuan; Barnard, Amanda S.

2016-07-01

Unpassivated diamond nanoparticles (bucky-diamonds) exhibit a unique surface reconstruction involving graphitization of certain crystal facets, giving rise to hybrid core-shell particles containing both aromatic and aliphatic carbon. Considerable effort is directed toward eliminating the aromatic shell, but persistent graphitization of subsequent subsurface-layers makes perdurable purification a challenge. In this study we use some simple statistical methods, in combination with electronic structure simulations, to predict the impact of different fractions of aromatic and aliphatic carbon on the charge transfer properties of the ensembles of bucky-diamonds. By predicting quality factors for a variety of cases, we find that perfect purification is not necessary to preserve selectivity, and there is a clear motivation for purifying samples to improve the sensitivity of charge transfer reactions. This may prove useful in designing drug delivery systems where the release of (selected) drugs needs to be sensitive to specific conditions at the point of delivery.Unpassivated diamond nanoparticles (bucky-diamonds) exhibit a unique surface reconstruction involving graphitization of certain crystal facets, giving rise to hybrid core-shell particles containing both aromatic and aliphatic carbon. Considerable effort is directed toward eliminating the aromatic shell, but persistent graphitization of subsequent subsurface-layers makes perdurable purification a challenge. In this study we use some simple statistical methods, in combination with electronic structure simulations, to predict the impact of different fractions of aromatic and aliphatic carbon on the charge transfer properties of the ensembles of bucky-diamonds. By predicting quality factors for a variety of cases, we find that perfect purification is not necessary to preserve selectivity, and there is a clear motivation for purifying samples to improve the sensitivity of charge transfer reactions. This may prove useful in designing drug delivery systems where the release of (selected) drugs needs to be sensitive to specific conditions at the point of delivery. Electronic supplementary information (ESI) available. See DOI: 10.1039/c6nr03068h

Effects of ion concentration on thermally-chargeable double-layer supercapacitors

NASA Astrophysics Data System (ADS)

Lim, Hyuck; Lu, Weiyi; Chen, Xi; Qiao, Yu

2013-11-01

The concept of thermally-chargeable supercapacitor was discussed and validated experimentally. As two double-layer supercapacitor-type devices were placed at different temperatures and connected, due to the thermal dependence of surface charge structures, the electrode potentials became different, and thermal energy could be harvested and stored as electric energy. The important effect of ion concentration was investigated. The results were quite different from the prediction of conventional surface theory, which should be attributed to the unique behaviors of the ions confined in the nanoporous electrodes.

Effects of ion concentration on thermally-chargeable double-layer supercapacitors.

PubMed

Lim, Hyuck; Lu, Weiyi; Chen, Xi; Qiao, Yu

2013-11-22

The concept of thermally-chargeable supercapacitor was discussed and validated experimentally. As two double-layer supercapacitor-type devices were placed at different temperatures and connected, due to the thermal dependence of surface charge structures, the electrode potentials became different, and thermal energy could be harvested and stored as electric energy. The important effect of ion concentration was investigated. The results were quite different from the prediction of conventional surface theory, which should be attributed to the unique behaviors of the ions confined in the nanoporous electrodes.

XPS/NEXAFS spectroscopic and conductance studies of glycine on AlGaN/GaN transistor devices

NASA Astrophysics Data System (ADS)

Myers, Matthew; Khir, Farah Liyana Muhammad; Home, Michael A.; Mennell, Christopher; Gillbanks, Jeremy; Tadich, Anton; Baker, Murray V.; Nener, Brett D.; Parish, Giacinta

2018-03-01

We report on a study using a combination of XPS/NEXAFS and conductivity measurements to develop a fundamental understanding of how dipolar molecules interact with the heterostructure device surface and affect the device conductivity of AlGaN/GaN heterostructure-based transistors. In such structures, which are increasingly being investigated for chemical and biological sensing, a 2-dimensional electron gas spontaneously forms at the layer interface that is sensitive to the charge characteristics of the exposed surface. Glycine, chosen for this study because it is the simplest of the amino acids and is known to form a zwitterionic configuration when stabilized through intermolecular interactions, was evaporated under ultra-high vacuum conditions onto the device surface and subsequently both XPS/NEXAFS and conductivity measurements were conducted. NEXAFS spectra show a preferential orientation for the Glycine molecules on the surface and evidence for both neutral and zwitterionic species on the surface. In situ conductivity measurements suggest that the negatively charged carboxylate group is closest to the surface. These results are a unique and pivotal contribution to the previous and at times conflicting literature on the zwitterionic nature of Glycine.

Visible-light-driven photoelectrochemical and photocatalytic performances of Cr-doped SrTiO3/TiO2 heterostructured nanotube arrays.

PubMed

Jiao, Zhengbo; Chen, Tao; Xiong, Jinyan; Wang, Teng; Lu, Gongxuan; Ye, Jinhua; Bi, Yingpu

2013-01-01

Well-aligned TiO2 nanotube arrays have become of increasing significance because of their unique highly ordered array structure, high specific surface area, unidirectional charge transfer and transportation features. However, their poor visible light utilization as well as the high recombination rate of photoexcited electron-hole pairs greatly limited their practical applications. Herein, we demonstrate the fabrication of visible-light-responsive heterostructured Cr-doped SrTiO3/TiO2 nanotube arrays by a simple hydrothermal method, which facilitate efficient charge separation and thus improve the photoelectrochemical as well as photocatalytic performances.

Crystal structure of class III chitinase from pomegranate provides the insight into its metal storage capacity.

PubMed

Masuda, Taro; Zhao, Guanghua; Mikami, Bunzo

2015-01-01

Chitinase hydrolyzes the β-1,4-glycosidic bond in chitin. In higher plants, this enzyme has been regarded as a pathogenesis-related protein. Recently, we identified a class III chitinase, which functions as a calcium storage protein in pomegranate (Punica granatum) seed (PSC, pomegranate seed chitinase). Here, we solved a crystal structure of PSC at 1.6 Å resolution. Although its overall structure, including the structure of catalytic site and non-proline cis-peptides, was closely similar to those of other class III chitinases, PSC had some unique structural characteristics. First, there were some metal-binding sites with coordinated water molecules on the surface of PSC. Second, many unconserved aspartate residues were present in the PSC sequence which rendered the surface of PSC negatively charged. This acidic electrostatic property is in contrast to that of hevamine, well-characterized plant class III chitinase, which has rather a positively charged surface. Thus, the crystal structure provides a clue for metal association property of PSC.

Observation of Internal Photoinduced Electron and Hole Separation in Hybrid Two-Dimentional Perovskite Films.

PubMed

Liu, Junxue; Leng, Jing; Wu, Kaifeng; Zhang, Jun; Jin, Shengye

2017-02-01

Two-dimensional (2D) organolead halide perovskites are promising for various optoelectronic applications. Here we report a unique spontaneous charge (electron/hole) separation property in multilayered (BA) 2 (MA) n-1 Pb n I 3n+1 (BA = CH 3 (CH 2 ) 3 NH 3 + , MA = CH 3 NH 3 + ) 2D perovskite films by studying the charge carrier dynamics using ultrafast transient absorption and photoluminescence spectroscopy. Surprisingly, the 2D perovskite films, although nominally prepared as "n = 4", are found to be mixture of multiple perovskite phases, with n = 2, 3, 4 and ≈ ∞, that naturally align in the order of n along the direction perpendicular to the substrate. Driven by the band alignment between 2D perovskites phases, we observe consecutive photoinduced electron transfer from small-n to large-n phases and hole transfer in the opposite direction on hundreds of picoseconds inside the 2D film of ∼358 nm thickness. This internal charge transfer efficiently separates electrons and holes to the upper and bottom surfaces of the films, which is a unique property beneficial for applications in photovoltaics and other optoelectronics devices.

Electrostatic correlations at the Stern layer: Physics or chemistry?

NASA Astrophysics Data System (ADS)

Travesset, A.; Vangaveti, S.

2009-11-01

We introduce a minimal free energy describing the interaction of charged groups and counterions including both classical electrostatic and specific interactions. The predictions of the model are compared against the standard model for describing ions next to charged interfaces, consisting of Poisson-Boltzmann theory with additional constants describing ion binding, which are specific to the counterion and the interfacial charge ("chemical binding"). It is shown that the "chemical" model can be appropriately described by an underlying "physical" model over several decades in concentration, but the extracted binding constants are not uniquely defined, as they differ depending on the particular observable quantity being studied. It is also shown that electrostatic correlations for divalent (or higher valence) ions enhance the surface charge by increasing deprotonation, an effect not properly accounted within chemical models. The charged phospholipid phosphatidylserine is analyzed as a concrete example with good agreement with experimental results. We conclude with a detailed discussion on the limitations of chemical or physical models for describing the rich phenomenology of charged interfaces in aqueous media and its relevance to different systems with a particular emphasis on phospholipids.

Measurement of clay surface areas by polyvinylpyrrolidone (PVP) sorption and its use for quantifying illite and smectite abundance

USGS Publications Warehouse

Blum, A.E.; Eberl, D.D.

2004-01-01

A new method has been developed for quantifying smectite abundance by sorbing polyvinylpyrrolidone (PVP) on smectite particles dispersed in aqueous solution. The sorption density of PVP-55K on a wide range of smectites, illites and kaolinites is ~0.99 mg/m2, which corresponds to ~0.72 g of PVP-55K per gram of montmorillonite. Polyvinylpyrrolidone sorption on smectites is independent of layer charge and solution pH. PVP sorption on SiO2, Fe2O3 and ZnO normalized to the BET surface area is similar to the sorption densities on smectites. γ-Al2O3, amorphous Al(OH)3 and gibbsite have no PVP sorption over a wide range of pH, and sorption of PVP by organics is minimal. The insensitivity of PVP sorption densities to mineral layer charge, solution pH and mineral surface charge indicates that PVP sorption is not localized at charged sites, but is controlled by more broadly distributed sorption mechanisms such as Van der Waals’ interactions and/or hydrogen bonding. Smectites have very large surface areas when dispersed as single unit-cell-thick particles (~725 m2/g) and usually dominate the total surface areas of natural samples in which smectites are present. In this case, smectite abundance is directly proportional to PVP sorption. In some cases, however, the accurate quantification of smectite abundance by PVP sorption may require minor corrections for PVP uptake by other phases, principally illite and kaolinite. Quantitative XRD can be combined with PVP uptake measurements to uniquely determine the smectite concentration in such samples.

Hysteresis in Carbon Nanotube Transistors: Measurement and Analysis of Trap Density, Energy Level, and Spatial Distribution.

PubMed

Park, Rebecca Sejung; Shulaker, Max Marcel; Hills, Gage; Suriyasena Liyanage, Luckshitha; Lee, Seunghyun; Tang, Alvin; Mitra, Subhasish; Wong, H-S Philip

2016-04-26

We present a measurement technique, which we call the Pulsed Time-Domain Measurement, for characterizing hysteresis in carbon nanotube field-effect transistors, and demonstrate its applicability for a broad range of 1D and 2D nanomaterials beyond carbon nanotubes. The Pulsed Time-Domain Measurement enables the quantification (density, energy level, and spatial distribution) of charged traps responsible for hysteresis. A physics-based model of the charge trapping process for a carbon nanotube field-effect transistor is presented and experimentally validated using the Pulsed Time-Domain Measurement. Leveraging this model, we discover a source of traps (surface traps) unique to devices with low-dimensional channels such as carbon nanotubes and nanowires (beyond interface traps which exist in today's silicon field-effect transistors). The different charge trapping mechanisms for interface traps and surface traps are studied based on their temperature dependencies. Through these advances, we are able to quantify the interface trap density for carbon nanotube field-effect transistors (∼3 × 10(13) cm(-2) eV(-1) near midgap), and compare this against a range of previously studied dielectric/semiconductor interfaces.

Characterization of the unique function of a reduced amide bond in a cytolytic peptide that acts on phospholipid membranes.

PubMed Central

Oh, J E; Lee, K H

2000-01-01

The incorporation of a reduced amide bond, psi(CH(2)NH), into peptide results in an increase in the net positive charge and the perturbation of alpha-helical structure. By using this characteristic of the reduced amide bond, we designed and synthesized novel pseudopeptides containing reduced amide bonds, which had a great selectivity between bacterial and mammalian cells. A structure-activity relationship study on pseudopeptides indicated that the decrease in alpha-helicity and the increase in net positive charge in the backbone, caused by the incorporation of a reduced amide bond into the peptide, both contributed to an improvement in the selectivity between lipid membranes with various surface charges. However, activity results in vitro indicated that a perturbation of alpha-helical structure rather than an increase in net positive charge in the backbone is more important in the selectivity between bacterial and mammalian cells. The present result revealed that the backbone of membrane-active peptides were important not only in maintaining the secondary structure for the interactions with lipid membranes but also in direct interactions with lipid membranes. The present study showed the unique function of a reduced amide bond in cytolytic peptides and a direction for developing novel anti-bacterial agents from cytolytic peptides that act on the lipid membrane of micro-organisms. PMID:11104671

Proliferative activity of elastin-like-peptides depends on charge and phase transition.

PubMed

Yuan, Yuan; Koria, Piyush

2016-03-01

Elastin-like-peptides (ELPs) are stimulus-responsive protein-based polymers and are attractive biomaterials due to their biocompatibility and unique properties. This study shows that in addition to their physical properties, ELPs have biological activities that are conducive to tissue regeneration. Specifically, we found that ELPs induce fibroblast proliferation via cell surface heparan sulfate proteoglycans (HSPG). Furthermore, our data suggests that ELP based materials with differential proliferative potential can be designed by controlling the interaction of ELPs with HSPGs by incorporating either hydrophobic or positively charged residues within the ELP sequence. Fibroblast proliferation is important for granulation tissue formation which is important in chronic wounds as well as in healing of other tissues. The customizable biological activity of ELPs coupled with their unique physical properties will enable us to design novel, sustainable and cost effective therapies for different tissue regeneration applications. © 2015 Wiley Periodicals, Inc. J Biomed Mater Res Part A: 104A: 697-706, 2016. © 2015 Wiley Periodicals, Inc.

Mini-LENS: developing a charged-current approach to measuring CNO and pp solar neutrinos

NASA Astrophysics Data System (ADS)

Vogelaar, R. Bruce

2014-03-01

The Low-Energy Neutrino Spectroscopy (LENS) experiment is based on neutrino detection via a charged-current interaction with 115In and offers the ability to cleanly observe both pp and CNO neutrinos. In contrast, elastic-scattering detectors, such as Borexino and SNO + suffer from virtually inseparable backgrounds. Thus, LENS might be uniquely positioned to resolve the solar metallicity question via measurement of the CNO neutrino flux, as well as test the predicted equivalence of solar luminosity as measured by photons versus neutrinos The mini-LENS program is testing the performance of the optically-segmented 3D lattice geometry unique to LENS. This first-of-a-kind lattice design is also suited for a range of other applications where high segmentation and large light collection are required (eg: sterile neutrinos with sources, double beta decay, and surface detection of reactor neutrinos). The current status and recent design changes of miniLENS at KURF will be presented. funded by NSF: 1001394.

LETS: Lunar Environments Test System

NASA Technical Reports Server (NTRS)

Vaughn, Jason A.; Schneider, Todd; Craven, Paul; Norwood, Joey

2008-01-01

The Environmental Effects Branch (EM50) at the Marshall Space Flight Center has developed a unique capability within the agency, namely the Lunar Environment Test System (LETS). LETS is a cryo-pumped vacuum chamber facility capable of high vacuum (10-7 Torr). LETS is a cylindrical chamber, 30 in. (0.8 m) diameter by 48 in. (1.2 m) long thermally controlled vacuum system. The chamber is equipped with a full array of radiation sources including vacuum ultraviolet, electron, and proton radiation. The unique feature of LETS is that it contains a large lunar simulant bed (18 in. x 40 in. x 6 in.) holding 75 kg of JSC-1a simulant while operating at a vacuum of 10-7 Torr. This facility allows three applications: 1) to study the charging, levitation and migration of dust particles, 2) to simulate the radiation environment on the lunar surface, and 3) to electrically charge the lunar simulant enhancing the attraction and adhesion of dust particles to test articles more closely simulating the lunar surface dust environment. LETS has numerous diagnostic instruments including TREK electrostatic probes, residual gas analyzer (RGA), temperature controlled quartz crystal microbalance (TQCM), and particle imaging velocimeter (PIV). Finally, LETS uses continuous Labview data acquisition for computer monitoring and system control.

Experimental Investigation of Charging Properties of Interstellar Type Silica Dust Grains by Secondary Electron Emissions

NASA Technical Reports Server (NTRS)

Tankosic, D.; Abbas, M. M.

2013-01-01

The dust charging by electron impact is an important dust charging processes in astrophysical and planetary environments. Incident low energy electrons are reflected or stick to the grains charging the dust grains negatively. At sufficiently high energies electrons penetrate the grains, leading to excitation and emission of electrons referred to as secondary electron emission (SEE). Available classical theoretical models for calculations of SEE yields are generally applicable for neutral, planar, or bulk surfaces. These models, however, are not valid for calculations of the electron impact charging properties of electrostatically charged micron/submicron-size dust grains in astrophysical environments. Rigorous quantum mechanical models are not yet available, and the SEE yields have to be determined experimentally for development of more accurate models for charging of individual dust grains. At the present time, very limited experimental data are available for charging of individual micron-size dust grains, particularly for low energy electron impact. The experimental results on individual, positively charged, micron-size lunar dust grains levitated carried out by us in a unique facility at NASA-MSFC, based on an electrodynamic balance, indicate that the SEE by electron impact is a complex process. The electron impact may lead to charging or discharging of dust grains depending upon the grain size, surface potential, electron energy, electron flux, grain composition, and configuration (Abbas et al, 2010, 2012). In this paper, we discuss SEE charging properties of individual micron-size silica microspheres that are believed to be analogs of a class of interstellar dust grains. The measurements indicate charging of the 0.2m silica particles when exposed to 25 eV electron beams and discharging when exposed to higher energy electron beams. Relatively large size silica particles (5.2-6.82m) generally discharge to lower equilibrium potentials at both electron energies. These measurements conducted on silica microspheres are qualitatively similar in nature to our previous SEE measurements on lunar Apollo missions dust samples.

Ions, metabolites, and cells: Water as a reporter of surface conditions during bacterial growth.

PubMed

Jarisz, Tasha A; Lane, Sarah; Gozdzialski, Lea; Hore, Dennis K

2018-06-14

Surface-specific nonlinear vibrational spectroscopy, combined with bulk solution measurements and imaging, is used to study the surface conditions during the growth of E. coli. As a result of the silica high surface charge density, the water structure at the silica-aqueous interface is known to be especially sensitive to pH and ionic strength, and surface concentration profiles develop that can be appreciably different from the bulk solution conditions. We illustrate that, in the presence of growing cells, a unique surface micro-environment is established as a result of metabolites accumulating on the silica surface. Even in the subsequent absence of the cells, this surface layer works to reduce the interfacial ionic strength as revealed by the enhanced signal from surface water molecules. In the presence of growing cells, an additional boost in surface water signal is attributed to a local pH that is higher than that of the bulk solution.

Ions, metabolites, and cells: Water as a reporter of surface conditions during bacterial growth

NASA Astrophysics Data System (ADS)

Jarisz, Tasha A.; Lane, Sarah; Gozdzialski, Lea; Hore, Dennis K.

2018-06-01

Surface-specific nonlinear vibrational spectroscopy, combined with bulk solution measurements and imaging, is used to study the surface conditions during the growth of E. coli. As a result of the silica high surface charge density, the water structure at the silica-aqueous interface is known to be especially sensitive to pH and ionic strength, and surface concentration profiles develop that can be appreciably different from the bulk solution conditions. We illustrate that, in the presence of growing cells, a unique surface micro-environment is established as a result of metabolites accumulating on the silica surface. Even in the subsequent absence of the cells, this surface layer works to reduce the interfacial ionic strength as revealed by the enhanced signal from surface water molecules. In the presence of growing cells, an additional boost in surface water signal is attributed to a local pH that is higher than that of the bulk solution.

Temporal Characteristics of Electron Flux Events at Geosynchronous Orbit

NASA Astrophysics Data System (ADS)

Olson, D. K.; Larsen, B.; Henderson, M. G.

2017-12-01

Geosynchronous satellites such as the LANL-GEO fleet are exposed to hazardous conditions when they encounter regions of hot, intense plasma such as that from the plasma sheet. These conditions can lead to the build-up of charge on the surface of a spacecraft, with undesired, and often dangerous, side effects. Observation of electron flux levels at geosynchronous orbit (GEO) with multiple satellites provides a unique view of plasma sheet access to that region. Flux "events", or periods when fluxes are elevated continuously above the LANL-GEO spacecraft charging threshold, can be characterized by duration in two dimensions: a spatial dimension of local time, describing the duration of an event from the perspective of a single spacecraft, and a temporal dimension describing the duration in time in which high energy plasma sheet particles have access to geosynchronous orbit. We examine the statistical properties of the temporal duration of 8 keV electron flux events at geosynchronous orbit over a twelve-year period. These results, coupled with the spatial duration characteristics, provide the key information needed to formulate a statistical model for forecasting the electron flux conditions at GEO that are correlated with LANL-GEO surface charging. Forecasting models are an essential component to understanding space weather and mitigating the dangers of surface charging on our satellites. We also examine the correlation of flux event durations with solar wind parameters and geomagnetic indices, identifying the data needed to improve upon a statistical forecasting model

Unveiling Surface Redox Charge Storage of Interacting Two-Dimensional Hetero-Nanosheets in Hierarchical Architectures

DOE PAGES

Mahmood, Qasim; Bak, Seong-Min; Kim, Min G.; ...

2015-03-03

Two-dimensional (2D) heteronanosheets are currently the focus of intense study due to the unique properties that emerge from the interplay between two low-dimensional nanomaterials with different properties. However, the properties and new phenomena based on the two 2D heteronanosheets interacting in a 3D hierarchical architecture have yet to be explored. Here, we unveil the surface redox charge storage mechanism of surface-exposed WS2 nanosheets assembled in a 3D hierarchical heterostructure using in situ synchrotron X-ray absorption and Raman spectroscopic methods. The surface dominating redox charge storage of WS2 is manifested in a highly reversible and ultrafast capacitive fashion due to themore » interaction of heteronanosheets and the 3D connectivity of the hierarchical structure. In contrast, compositionally identical 2D WS2 structures fail to provide a fast and high capacitance with different modes of lattice vibration. The distinctive surface capacitive behavior of 3D hierarchically structured heteronanosheets is associated with rapid proton accommodation into the in-plane W–S lattice (with the softening of the E2g bands), the reversible redox transition of the surface-exposed intralayers residing in the electrochemically active 1T phase of WS2 (with the reversible change in the interatomic distance and peak intensity of W–W bonds), and the change in the oxidation state during the proton insertion/deinsertion process. This proposed mechanism agrees with the dramatic improvement in the capacitive performance of the two heteronanosheets coupled in the hierarchical structure.« less

First principles investigation of heterogeneous catalysis on metal oxide surfaces

NASA Astrophysics Data System (ADS)

Ghoussoub, Mireille

Metal oxides possess unique electronic and structural properties that render them highly favourable for applications in heterogeneous catalysis. In this study, computational atomistic modelling based on Density Functional Theory was used to investigate the reduction of carbon dioxide over hydroxylated indium oxide nanoparticles, as well at the activation of methane over oxygen-covered bimetallic surfaces. The first study employed metadynamics-biased ab initio molecular dynamics to obtain the free energy surface of the various reaction steps at finite temperature. In the second study, the nudged elastic band method was used to probe the C-H activation mechanisms for different surface configurations. In both cases, activation energies, reaction energies, transition state structures, and charge analysis results are used to explain the underlying mechanistic pathways.

Surface Pb nanoparticle aggregation, coalescence and differential capacitance in a deep eutectic solvent using a simultaneous sample-rotated small angle x-ray scattering and electrochemical methods approach [Surface Pb nanoparticle aggregation, coalescence and differential capacitance in a deep eutectic solvent using a simultaneous grazing transmission small angle x-ray scattering and electrochemical methods approach

DOE PAGES

Hammons, Joshua A.; Ilavsky, Jan

2017-01-18

Nanoparticle electrodeposition is a simple and scalable approach to synthesizing supported nanoparticles. Used with a deep eutectic solvent (DES), surface nanoparticles can be assembled and exhibit unique surface charge separation when the DES is adsorbed on the nanoparticle surface. Key to understanding and controlling the assembly and the capacitance is a thorough understanding of surface particle mobility and charge screening, which requires an in-situ approach. In this study, Pb particle formation, size, shape and capacitance are resolved in a 1:2 choline Cl –: urea deep eutectic solvent whilst sweeping the cell potential in the range: 0.2 V to –1.2 Vmore » (vs. Ag/AgCl). These system parameters were resolved using a complementary suite of sample-rotated small angle X-ray scattering (SR-SAXS) and electrochemical impedance spectroscopy (EIS), which are presented and discussed in detail. This approach is able to show that both particle and ion transport are impeded in the DES, as aggregation occurs over the course of 6 minutes, and dissolved Pb ions accumulate and remain near the surface after a nucleation pulse is applied. The DES-Pb interactions strongly depend on the cell potential as evidenced by the specific differential capacitance of the Pb deposit, which has a maximum value of 2.5 +/– 0.5 F g –1 at –1.0 V vs. Ag/AgCl. Together, the SR-SAXS-EIS approach is able to characterize the unique nanoparticle capacitance, mobility and ion mobility in a DES and can be used to study a wide range of nanoparticle deposition systems in-situ.« less

Surface Pb nanoparticle aggregation, coalescence and differential capacitance in a deep eutectic solvent using a simultaneous sample-rotated small angle x-ray scattering and electrochemical methods approach [Surface Pb nanoparticle aggregation, coalescence and differential capacitance in a deep eutectic solvent using a simultaneous grazing transmission small angle x-ray scattering and electrochemical methods approach

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hammons, Joshua A.; Ilavsky, Jan

Nanoparticle electrodeposition is a simple and scalable approach to synthesizing supported nanoparticles. Used with a deep eutectic solvent (DES), surface nanoparticles can be assembled and exhibit unique surface charge separation when the DES is adsorbed on the nanoparticle surface. Key to understanding and controlling the assembly and the capacitance is a thorough understanding of surface particle mobility and charge screening, which requires an in-situ approach. In this study, Pb particle formation, size, shape and capacitance are resolved in a 1:2 choline Cl –: urea deep eutectic solvent whilst sweeping the cell potential in the range: 0.2 V to –1.2 Vmore » (vs. Ag/AgCl). These system parameters were resolved using a complementary suite of sample-rotated small angle X-ray scattering (SR-SAXS) and electrochemical impedance spectroscopy (EIS), which are presented and discussed in detail. This approach is able to show that both particle and ion transport are impeded in the DES, as aggregation occurs over the course of 6 minutes, and dissolved Pb ions accumulate and remain near the surface after a nucleation pulse is applied. The DES-Pb interactions strongly depend on the cell potential as evidenced by the specific differential capacitance of the Pb deposit, which has a maximum value of 2.5 +/– 0.5 F g –1 at –1.0 V vs. Ag/AgCl. Together, the SR-SAXS-EIS approach is able to characterize the unique nanoparticle capacitance, mobility and ion mobility in a DES and can be used to study a wide range of nanoparticle deposition systems in-situ.« less

Study of solids by use of nonthermalized positrons

NASA Astrophysics Data System (ADS)

Nielsen, Bent; Lynn, K. G.; Chen, Yen-C.

1986-10-01

We have measured the energy distribution of positrons reemitted from the surfaces of solids after being implanted at low energy. It is shown that this provides a unique possibility to study energy losses of a charged particle down to near-thermal energy. Such measurements are used to estimate the positron thermalization time in Al. A dramatic change in this energy distribution was observed after oxidation of the Al surface. We attribute this to the band gap of the oxide. Trapping of epithermal positrons with a remarkably high cross section was observed for both Al and Cu.

Chemically directing d-block heterometallics to nanocrystal surfaces as molecular beacons of surface structure

DOE PAGES

Rosen, Evelyn L.; Gilmore, Keith; Sawvel, April M.; ...

2015-07-28

Our understanding of structure and bonding in nanoscale materials is incomplete without knowledge of their surface structure. Needed are better surveying capabilities responsive not only to different atoms at the surface, but also their respective coordination environments. We report here that d-block organometallics, when placed at nanocrystal surfaces through heterometallic bonds, serve as molecular beacons broadcasting local surface structure in atomic detail. This unique ability stems from their elemental specificity and the sensitivity of their d-orbital level alignment to local coordination environment, which can be assessed spectroscopically. Re-surfacing cadmium and lead chalcogenide nanocrystals with iron- or ruthenium-based molecular beacons ismore » readily accomplished with trimethylsilylated cyclopentadienyl metal carbonyls. For PbSe nanocrystals with iron-based beacons, we show how core-level X-ray spectroscopies and DFT calculations enrich our understanding of both charge and atomic reorganization at the surface when beacons are bound.« less

Photoelectrodes based on 2D opals assembled from Cu-delafossite double-shelled microspheres for an enhanced photoelectrochemical response.

PubMed

Oh, Yunjung; Yang, Wooseok; Tan, Jeiwan; Lee, Hyungsoo; Park, Jaemin; Moon, Jooho

2018-02-22

Although a unique light-harvesting property was recently demonstrated in a photocathode based on 2-dimensional (2D) opals of CuFeO 2 -shelled SiO 2 microspheres, the performance of a monolayer of ultra-thin CuFeO 2 -shelled microspheres is limited by ineffective charge separation. Herein, we propose an innovative design rule, in which an inner CuFeO 2 /outer CuAlO 2 double-shelled heterojunction is formed on each partially etched microsphere to obtain a hexagonally assembled 2D opal photoelectrode. Our Cu-delafossite double-shelled photocathode shows a dramatically improved charge separation capability, with a 9-fold increase in the photocurrent compared to that of the single-shelled counterpart. Electrochemical impedance spectroscopy clearly confirms the reduced charge transport/transfer resistance associated with the Cu-delafossite double-shelled photocathode, while surface photovoltage spectra reveal enhanced polarization of the photogenerated carrier, indicating improved charge separation capability with the aid of the heterojunction. Our finding sheds light on the importance of heterojunction interfaces in achieving optimal charge separation in opal architectures as well as the inner-shell/electrolyte interface to expedite charge separation/transport.

A Nonmetal Plasmonic Z-Scheme Photocatalyst with UV- to NIR-Driven Photocatalytic Protons Reduction.

PubMed

Zhang, Zhenyi; Huang, Jindou; Fang, Yurui; Zhang, Mingyi; Liu, Kuichao; Dong, Bin

2017-05-01

Ultrabroad-spectrum absorption and highly efficient generation of available charge carriers are two essential requirements for promising semiconductor-based photocatalysts, towards achieving the ultimate goal of solar-to-fuel conversion. Here, a fascinating nonmetal plasmonic Z-scheme photocatalyst with the W 18 O 49 /g-C 3 N 4 heterostructure is reported, which can effectively harvest photon energies spanning from the UV to the nearinfrared region and simultaneously possesses improved charge-carrier dynamics to boost the generation of long-lived active electrons for the photocatalytic reduction of protons into H 2 . By combining with theoretical simulations, a unique synergistic photocatalysis effect between the semiconductive Z-scheme charge-carrier separation and metal-like localized-surface-plasmon-resonance-induced "hot electrons" injection process is demonstrated within this binary heterostructure. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Time-resolved energy transduction in a quantum capacitor

PubMed Central

Jung, Woojin; Cho, Doohee; Kim, Min-Kook; Choi, Hyoung Joon; Lyo, In-Whan

2011-01-01

The capability to deposit charge and energy quantum-by-quantum into a specific atomic site could lead to many previously unidentified applications. Here we report on the quantum capacitor formed by a strongly localized field possessing such capability. We investigated the charging dynamics of such a capacitor by using the unique scanning tunneling microscopy that combines nanosecond temporal and subangstrom spatial resolutions, and by using Si(001) as the electrode as well as the detector for excitations produced by the charging transitions. We show that sudden switching of a localized field induces a transiently empty quantum dot at the surface and that the dot acts as a tunable excitation source with subangstrom site selectivity. The timescale in the deexcitation of the dot suggests the formation of long-lived, excited states. Our study illustrates that a quantum capacitor has serious implications not only for the bottom-up nanotechnology but also for future switching devices. PMID:21817067

Optimization of power and energy densities in supercapacitors

NASA Astrophysics Data System (ADS)

Robinson, David B.

Supercapacitors use nanoporous electrodes to store large amounts of charge on their high surface areas, and use the ions in electrolytes to carry charge into the pores. Their high power density makes them a potentially useful complement to batteries. However, ion transport through long, narrow channels still limits power and efficiency in these devices. Proper design can mitigate this. Current collector geometry must also be considered once this is done. Here, De Levie's model for porous electrodes is applied to quantitatively predict device performance and to propose optimal device designs for given specifications. Effects unique to nanoscale pores are considered, including that pores may not have enough salt to fully charge. Supercapacitors are of value for electric vehicles, portable electronics, and power conditioning in electrical grids with distributed renewable sources, and that value will increase as new device fabrication methods are developed and proper design accommodates those improvements. Example design outlines for vehicle applications are proposed and compared.

Epithelial Microvilli Establish an Electrostatic Barrier to Microbial Adhesion

PubMed Central

Bennett, Kaila M.; Walker, Sharon L.

2014-01-01

Microvilli are membrane extensions on the apical surface of polarized epithelia, such as intestinal enterocytes and tubule and duct epithelia. One notable exception in mucosal epithelia is M cells, which are specialized for capturing luminal microbial particles; M cells display a unique apical membrane lacking microvilli. Based on studies of M cell uptake under different ionic conditions, we hypothesized that microvilli may augment the mucosal barrier by providing an increased surface charge density from the increased membrane surface and associated glycoproteins. Thus, electrostatic charges may repel microbes from epithelial cells bearing microvilli, while M cells are more susceptible to microbial adhesion. To test the role of microvilli in bacterial adhesion and uptake, we developed polarized intestinal epithelial cells with reduced microvilli (“microvillus-minus,” or MVM) but retaining normal tight junctions. When tested for interactions with microbial particles in suspension, MVM cells showed greatly enhanced adhesion and uptake of particles compared to microvillus-positive cells. This preference showed a linear relationship to bacterial surface charge, suggesting that microvilli resist binding of microbes by using electrostatic repulsion. Moreover, this predicts that pathogen modification of electrostatic forces may contribute directly to virulence. Accordingly, the effacement effector protein Tir from enterohemorrhagic Escherichia coli O157:H7 expressed in epithelial cells induced a loss of microvilli with consequent enhanced microbial binding. These results provide a new context for microvillus function in the host-pathogen relationship, based on electrostatic interactions. PMID:24778113

Bulk-Induced 1/f Noise at the Surface of Three-Dimensional Topological Insulators.

PubMed

Bhattacharyya, Semonti; Banerjee, Mitali; Nhalil, Hariharan; Islam, Saurav; Dasgupta, Chandan; Elizabeth, Suja; Ghosh, Arindam

2015-12-22

Slow intrinsic fluctuations of resistance, also known as the flicker noise or 1/f-noise, in the surface transport of strong topological insulators (TIs) is a poorly understood phenomenon. Here, we have systematically explored the 1/f-noise in field-effect transistors (FET) of mechanically exfoliated Bi1.6Sb0.4Te2Se TI films when transport occurs predominantly via the surface states. We find that the slow kinetics of the charge disorder within the bulk of the TI induces mobility fluctuations at the surface, providing a new source of intrinsic 1/f-noise that is unique to bulk TI systems. At small channel thickness, the noise magnitude can be extremely small, corresponding to the phenomenological Hooge parameter γH as low as ≈10(-4), but it increases rapidly when channel thickness exceeds ∼1 μm. From the temperature (T)-dependence of noise, which displayed sharp peaks at characteristic values of T, we identified generation-recombination processes from interband transitions within the TI bulk as the dominant source of the mobility fluctuations in surface transport. Our experiment not only establishes an intrinsic microscopic origin of noise in TI surface channels, but also reveals a unique spectroscopic information on the impurity bands that can be useful in bulk TI systems in general.

Mass spectrometry of acoustically levitated droplets.

PubMed

Westphall, Michael S; Jorabchi, Kaveh; Smith, Lloyd M

2008-08-01

Containerless sample handling techniques such as acoustic levitation offer potential advantages for mass spectrometry, by eliminating surfaces where undesired adsorption/desorption processes can occur. In addition, they provide a unique opportunity to study fundamental aspects of the ionization process as well as phenomena occurring at the air-droplet interface. Realizing these advantages is contingent, however, upon being able to effectively interface levitated droplets with a mass spectrometer, a challenging task that is addressed in this report. We have employed a newly developed charge and matrix-assisted laser desorption/ionization (CALDI) technique to obtain mass spectra from a 5-microL acoustically levitated droplet containing peptides and an ionic matrix. A four-ring electrostatic lens is used in conjunction with a corona needle to produce bursts of corona ions and to direct those ions toward the droplet, resulting in droplet charging. Analyte ions are produced from the droplet by a 337-nm laser pulse and detected by an atmospheric sampling mass spectrometer. The ion generation and extraction cycle is repeated at 20 Hz, the maximum operating frequency of the laser employed. It is shown in delayed ion extraction experiments that both positive and negative ions are produced, behavior similar to that observed for atmospheric pressure matrix-assisted laser absorption/ionization. No ion signal is observed in the absence of droplet charging. It is likely, although not yet proven, that the role of the droplet charging is to increase the strength of the electric field at the surface of the droplet, reducing charge recombination after ion desorption.

C@SiNW/TiO2 Core-Shell Nanoarrays with Sandwiched Carbon Passivation Layer as High Efficiency Photoelectrode for Water Splitting

PubMed Central

Devarapalli, Rami Reddy; Debgupta, Joyashish; Pillai, Vijayamohanan K.; Shelke, Manjusha V.

2014-01-01

One-dimensional heterostructure nanoarrays are efficiently promising as high performance electrodes for photo electrochemical (PEC) water splitting applications, wherein it is highly desirable for the electrode to have a broad light absorption, efficient charge separation and redox properties as well as defect free surface with high area suitable for fast interfacial charge transfer. We present highly active and unique photoelectrode for solar H2 production, consisting of silicon nanowires (SiNWs)/TiO2 core-shell structures. SiNWs are passivated to reduce defect sites and protected against oxidation in air or water by forming very thin carbon layer sandwiched between SiNW and TiO2 surfaces. This carbon layer decreases recombination rates and also enhances the interfacial charge transfer between the silicon and TiO2. A systematic investigation of the role of SiNW length and TiO2 thickness on photocurrent reveals enhanced photocurrent density up to 5.97 mA/cm2 at 1.0 V vs.NHE by using C@SiNW/TiO2 nanoarrays with photo electrochemical efficiency of 1.17%. PMID:24810865

Characterization of charged polymer self-assemblies by multidetector thermal field-flow fractionation in aqueous mobile phases.

PubMed

Greyling, Guilaume; Pasch, Harald

2018-01-12

Charged block copolymer self-assemblies, such as charged micelles, have attracted much attention as versatile drug delivery systems due to their readily tunable characteristics such as size and surface charge. However, current column-based analytical techniques are not suitable to fractionate and comprehensively characterize charged micelles in terms of size, molar mass, chemical composition and morphology. Multidetector thermal field-flow fractionation (ThFFF) is shown to be a unique characterization platform that can be used to characterize charged micelles in terms of size, molar mass, chemical composition and morphology in aqueous mobile phases with various ionic strengths and pH. This is demonstrated by the characterization of poly(methacrylic acid)-b-poly(methyl methacrylate) self-assemblies in high pH buffers as well as the characterization of cationic poly(2-vinyl pyridine)-b-polystyrene and poly(4-vinyl pyridine)-b-polystyrene self-assemblies in low pH buffers. Moreover, it is shown that ThFFF is capable of separating charged micelles according to the corona composition. These investigations prove convincingly that ThFFF is broadly applicable to the comprehensive characterization of amphiphilic self-assemblies even when aqueous mobile phases are used. Copyright © 2017 Elsevier B.V. All rights reserved.

Cubic mesoporous Ag@CN: a high performance humidity sensor.

PubMed

Tomer, Vijay K; Thangaraj, Nishanthi; Gahlot, Sweta; Kailasam, Kamalakannan

2016-12-01

The fabrication of highly responsive, rapid response/recovery and durable relative humidity (%RH) sensors that can precisely monitor humidity levels still remains a considerable challenge for realizing the next generation humidity sensing applications. Herein, we report a remarkably sensitive and rapid %RH sensor having a reversible response using a nanocasting route for synthesizing mesoporous g-CN (commonly known as g-C 3 N 4 ). The 3D replicated cubic mesostructure provides a high surface area thereby increasing the adsorption, transmission of charge carriers and desorption of water molecules across the sensor surfaces. Owing to its unique structure, the mesoporous g-CN functionalized with well dispersed catalytic Ag nanoparticles exhibits excellent sensitivity in the 11-98% RH range while retaining high stability, negligible hysteresis and superior real time %RH detection performances. Compared to conventional resistive sensors based on metal oxides, a rapid response time (3 s) and recovery time (1.4 s) were observed in the 11-98% RH range. Such impressive features originate from the planar morphology of g-CN as well as unique physical affinity and favourable electronic band positions of this material that facilitate water adsorption and charge transportation. Mesoporous g-CN with Ag nanoparticles is demonstrated to provide an effective strategy in designing high performance %RH sensors and show great promise for utilization of mesoporous 2D layered materials in the Internet of Things and next generation humidity sensing applications.

DNA-labeled micro- and nanoparticles: a new approach to study contaminant transport in the subsurface

NASA Astrophysics Data System (ADS)

McNew, C.; Wang, C.; Kocis, T. N.; Murphy, N. P.; Dahlke, H. E.

2017-12-01

Though our understanding of contaminant behavior in the subsurface has improved, our ability to measure and predict complex contaminant transport pathways at hillslope to watershed scales is still lacking. By utilizing bio-molecular nanotechnology developed for nano-medicines and drug delivery, we are able to produce DNA-labeled micro- and nanoparticles for use in a myriad of environmental systems. Control of the fabrication procedure allows us to produce particles of custom size, charge, and surface functionality to mimic the transport properties of the particulate contaminant or colloid of interest. The use of custom sequenced DNA allows for the fabrication of an enormous number of unique particle labels (approximately 1.61 x 1060 unique sequences) and the ability to discern between varied spatial and temporal applications, or the transport effect of varied particle size, charge, or surface properties. To date, this technology has been utilized to study contaminant transport from lab to field scales, including surface and open channel flow applications, transport in porous media, soil retention, and even subglacial flow pathways. Here, we present the technology for production and detection of the DNA-labeled particles along with the results from a current hillslope study at the Sierra Foothills Research and Extension Center (SFREC). This field study utilizes spatial and temporal variations in DNA-labeled particle applications to identify subsurface pollutant transport pathways through the four distinct soil horizons present at the SFREC site. Results from this and previous studies highlight the tremendous potential of the DNA-labeled particle technology for studying contaminant transport through the subsurface.

Protein sensing by nanofluidic crystal and its signal enhancement

PubMed Central

Sang, Jianming; Du, Hongtan; Wang, Wei; Chu, Ming; Wang, Yuedan; Li, Haichao; Alice Zhang, Haixia; Wu, Wengang; Li, Zhihong

2013-01-01

Nanofluidics has a unique property that ionic conductance across a nanometer-sized confined space is strongly affected by the space surface charge density, which can be utilized to construct electrical read-out biosensor. Based on this principle, this work demonstrated a novel protein sensor along with a sandwich signal enhancement approach. Nanoparticles with designed aptamer onside are assembled in a suspended micropore to form a 3-dimensional network of nanometer-sized interstices, named as nanofluidic crystal hereafter, as the basic sensing unit. Proteins captured by aptamers will change the surface charge density of nanoparticles and thereby can be detected by monitoring the ionic conductance across this nanofluidic crystal. Another aptamer can further enlarge the variations of the surface charge density by forming a sandwich structure (capturing aptamer/protein/signal enhancement aptamer) and the read-out conductance as well. The preliminary experimental results indicated that human α-thrombin was successfully detected by the corresponding aptamer modified nanofluidic crystal with the limit of detection of 5 nM (0.18 μg/ml) and the read-out signal was enhanced up to 3 folds by using another thrombin aptamer. Being easy to graft probe, facile and low-cost to prepare the nano-device, and having an electrical read-out, the present nanofluidic crystal scheme is a promising and universal strategy for protein sensing. PMID:24404017

Nanoporous membranes with electrochemically switchable, chemically stabilized ionic selectivity

NASA Astrophysics Data System (ADS)

Small, Leo J.; Wheeler, David R.; Spoerke, Erik D.

2015-10-01

Nanopore size, shape, and surface charge all play important roles in regulating ionic transport through nanoporous membranes. The ability to control these parameters in situ provides a means to create ion transport systems tunable in real time. Here, we present a new strategy to address this challenge, utilizing three unique electrochemically switchable chemistries to manipulate the terminal functional group and control the resulting surface charge throughout ensembles of gold plated nanopores in ion-tracked polycarbonate membranes 3 cm2 in area. We demonstrate the diazonium mediated surface functionalization with (1) nitrophenyl chemistry, (2) quinone chemistry, and (3) previously unreported trimethyl lock chemistry. Unlike other works, these chemistries are chemically stabilized, eliminating the need for a continuously applied gate voltage to maintain a given state and retain ionic selectivity. The effect of surface functionalization and nanopore geometry on selective ion transport through these functionalized membranes is characterized in aqueous solutions of sodium chloride at pH = 5.7. The nitrophenyl surface allows for ionic selectivity to be irreversibly switched in situ from cation-selective to anion-selective upon reduction to an aminophenyl surface. The quinone-terminated surface enables reversible changes between no ionic selectivity and a slight cationic selectivity. Alternatively, the trimethyl lock allows ionic selectivity to be reversibly switched by up to a factor of 8, approaching ideal selectivity, as a carboxylic acid group is electrochemically revealed or hidden. By varying the pore shape from cylindrical to conical, it is demonstrated that a controllable directionality can be imparted to the ionic selectivity. Combining control of nanopore geometry with stable, switchable chemistries facilitates superior control of molecular transport across the membrane, enabling tunable ion transport systems.Nanopore size, shape, and surface charge all play important roles in regulating ionic transport through nanoporous membranes. The ability to control these parameters in situ provides a means to create ion transport systems tunable in real time. Here, we present a new strategy to address this challenge, utilizing three unique electrochemically switchable chemistries to manipulate the terminal functional group and control the resulting surface charge throughout ensembles of gold plated nanopores in ion-tracked polycarbonate membranes 3 cm2 in area. We demonstrate the diazonium mediated surface functionalization with (1) nitrophenyl chemistry, (2) quinone chemistry, and (3) previously unreported trimethyl lock chemistry. Unlike other works, these chemistries are chemically stabilized, eliminating the need for a continuously applied gate voltage to maintain a given state and retain ionic selectivity. The effect of surface functionalization and nanopore geometry on selective ion transport through these functionalized membranes is characterized in aqueous solutions of sodium chloride at pH = 5.7. The nitrophenyl surface allows for ionic selectivity to be irreversibly switched in situ from cation-selective to anion-selective upon reduction to an aminophenyl surface. The quinone-terminated surface enables reversible changes between no ionic selectivity and a slight cationic selectivity. Alternatively, the trimethyl lock allows ionic selectivity to be reversibly switched by up to a factor of 8, approaching ideal selectivity, as a carboxylic acid group is electrochemically revealed or hidden. By varying the pore shape from cylindrical to conical, it is demonstrated that a controllable directionality can be imparted to the ionic selectivity. Combining control of nanopore geometry with stable, switchable chemistries facilitates superior control of molecular transport across the membrane, enabling tunable ion transport systems. Electronic supplementary information (ESI) available: Experimental procedures, synthesis, and characterization of molecules 1, 2 and 3. Explanation of the electrochemical method for approximating nanopore diameter. Additional XPS spectra. See DOI: 10.1039/C5NR02939B

Initial Efforts in Characterizing Radiation and Plasma Effects on Space Assets: Bridging the Space Environment, Engineering and User Community

NASA Astrophysics Data System (ADS)

Zheng, Y.; Ganushkina, N. Y.; Guild, T. B.; Jiggens, P.; Jun, I.; Mazur, J. E.; Meier, M. M.; Minow, J. I.; Pitchford, D. A.; O'Brien, T. P., III; Shprits, Y.; Tobiska, W. K.; Xapsos, M.; Rastaetter, L.; Jordanova, V. K.; Kellerman, A. C.; Fok, M. C. H.

2017-12-01

The Community Coordinated Modeling Center (CCMC) has been leading the community-wide model validation projects for many years. Such effort has been broadened and extended via the newly-launched International Forum for Space Weather Modeling Capabilities Assessment (https://ccmc.gsfc.nasa.gov/assessment/), Its objective is to track space weather models' progress and performance over time, which is critically needed in space weather operations. The Radiation and Plasma Effects Working Team is working on one of the many focused evaluation topics and deals with five different subtopics: Surface Charging from 10s eV to 40 keV electrons, Internal Charging due to energetic electrons from hundreds keV to several MeVs. Single Event Effects from solar energetic particles (SEPs) and galactic cosmic rays (GCRs) (several MeV to TeVs), Total Dose due to accumulation of doses from electrons (>100 KeV) and protons (> 1 MeV) in a broad energy range, and Radiation Effects from SEPs and GCRs at aviation altitudes. A unique aspect of the Radiation and Plasma Effects focus area is that it bridges the space environments, engineering and user community. This presentation will summarize the working team's progress in metrics discussion/definition and the CCMC web interface/tools to facilitate the validation efforts. As an example, tools in the areas of surface charging/internal charging will be demoed.

A rigorous and simpler method of image charges

NASA Astrophysics Data System (ADS)

Ladera, C. L.; Donoso, G.

2016-07-01

The method of image charges relies on the proven uniqueness of the solution of the Laplace differential equation for an electrostatic potential which satisfies some specified boundary conditions. Granted by that uniqueness, the method of images is rightly described as nothing but shrewdly guessing which and where image charges are to be placed to solve the given electrostatics problem. Here we present an alternative image charges method that is based not on guessing but on rigorous and simpler theoretical grounds, namely the constant potential inside any conductor and the application of powerful geometric symmetries. The aforementioned required uniqueness and, more importantly, guessing are therefore both altogether dispensed with. Our two new theoretical fundaments also allow the image charges method to be introduced in earlier physics courses for engineering and sciences students, instead of its present and usual introduction in electromagnetic theory courses that demand familiarity with the Laplace differential equation and its boundary conditions.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tomizawa, Shinya

We show a uniqueness theorem for Kaluza-Klein black holes in the bosonic sector of five-dimensional minimal supergravity. More precisely, under the assumptions of the existence of two commuting axial isometries and a nondegenerate connected event horizon of the cross-section topology S{sup 3}, or lens space, we prove that a stationary charged rotating Kaluza-Klein black hole in five-dimensional minimal supergravity is uniquely characterized by its mass, two independent angular momenta, electric charge, magnetic flux, and nut charge, provided that there exists neither a nut nor a bolt (a bubble) in the domain of outer communication. We also show that under themore » assumptions of the same symmetry, same asymptotics, and the horizon cross section of S{sup 1}xS{sup 2}, a black ring within the same theory--if it exists--is uniquely determined by its dipole charge and rod intervals besides the charges and magnetic flux.« less

Fast and efficient charge breeding of the Californium rare isotope breeder upgrade electron beam ion source

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ostroumov, P. N.; Barcikowski, A.; Dickerson, C. A.

The Electron Beam Ion Source (EBIS), developed to breed CARIBU radioactive beams at ATLAS, is being tested off-line. A unique property of the EBIS is a combination of short breeding times, high repetition rates and a large acceptance. Overall, we have implemented many innovative features during the design and construction of the CARIBU EBIS as compared to the existing EBIS breeders. The offline charge breeding tests are being performed using a surface ionization source that produces singly-charged cesium ions. The main goal of the off-line commissioning is to demonstrate stable operation of the EBIS at a 10 Hz repetition ratemore » and a breeding efficiency into single charge state higher than 15%. These goals have been successfully achieved and exceeded. We have measured (20±0.7)% breeding efficiency into the single charge state of 28+ cesium ions with the breeding time of 28 ms. In general, the current CARIBU EBIS operational parameters can provide charge breeding of any ions in the full mass range of periodic table with high efficiency, short breeding times and sufficiently low charge-to-mass ratio, 1/6.3 for the heaviest masses, for further acceleration in ATLAS. In this paper we discuss the parameters of the EBIS and the charge breeding results in a pulsed injection mode with repetition rates up to 10 Hz.« less

Clathrin to Lipid Raft-Endocytosis via Controlled Surface Chemistry and Efficient Perinuclear Targeting of Nanoparticle.

PubMed

Chakraborty, Atanu; Jana, Nikhil R

2015-09-17

Nanoparticle interacts with live cells depending on their surface chemistry, enters into cell via endocytosis, and is commonly trafficked to an endosome/lysozome that restricts subcellular targeting options. Here we show that nanoparticle surface chemistry can be tuned to alter their cell uptake mechanism and subcellular trafficking. Quantum dot based nanoprobes of 20-30 nm hydrodynamic diameters have been synthesized with tunable surface charge (between +15 mV to -25 mV) and lipophilicity to influence their cellular uptake processes and subcellular trafficking. It is observed that cationic nanoprobe electrostatically interacts with cell membrane and enters into cell via clathrin-mediated endocytosis. At lower surface charge (between +10 mV to -10 mV), the electrostatic interaction with cell membrane becomes weaker, and additional lipid raft endocytosis is initiated. If a lipophilic functional group is introduced on a weakly anionic nanoparticle surface, the uptake mechanism shifts to predominant lipid raft-mediated endocytosis. In particular, the zwitterionic-lipophilic nanoprobe has the unique advantage as it weakly interacts with anionic cell membrane, migrates toward lipid rafts for interaction through lipophilic functional group, and induces lipid raft-mediated endocytosis. While predominate or partial clathrin-mediated entry traffics most of the nanoprobes to lysozome, predominate lipid raft-mediated entry traffics them to perinuclear region, particularly to the Golgi apparatus. This finding would guide in designing appropriate nanoprobe for subcellular targeting and delivery.

Probing lipid membrane electrostatics

NASA Astrophysics Data System (ADS)

Yang, Yi

The electrostatic properties of lipid bilayer membranes play a significant role in many biological processes. Atomic force microscopy (AFM) is highly sensitive to membrane surface potential in electrolyte solutions. With fully characterized probe tips, AFM can perform quantitative electrostatic analysis of lipid membranes. Electrostatic interactions between Silicon nitride probes and supported zwitterionic dioleoylphosphatidylcholine (DOPC) bilayer with a variable fraction of anionic dioleoylphosphatidylserine (DOPS) were measured by AFM. Classical Gouy-Chapman theory was used to model the membrane electrostatics. The nonlinear Poisson-Boltzmann equation was numerically solved with finite element method to provide the potential distribution around the AFM tips. Theoretical tip-sample electrostatic interactions were calculated with the surface integral of both Maxwell and osmotic stress tensors on tip surface. The measured forces were interpreted with theoretical forces and the resulting surface charge densities of the membrane surfaces were in quantitative agreement with the Gouy-Chapman-Stern model of membrane charge regulation. It was demonstrated that the AFM can quantitatively detect membrane surface potential at a separation of several screening lengths, and that the AFM probe only perturbs the membrane surface potential by <2%. One important application of this technique is to estimate the dipole density of lipid membrane. Electrostatic analysis of DOPC lipid bilayers with the AFM reveals a repulsive force between the negatively charged probe tips and the zwitterionic lipid bilayers. This unexpected interaction has been analyzed quantitatively to reveal that the repulsion is due to a weak external field created by the internai membrane dipole moment. The analysis yields a dipole moment of 1.5 Debye per lipid with a dipole potential of +275 mV for supported DOPC membranes. This new ability to quantitatively measure the membrane dipole density in a noninvasive manner will be useful in identifying the biological effects of the dipole potential. Finally, heterogeneous model membranes were studied with fluid electric force microscopy (FEFM). Electrostatic mapping was demonstrated with 50 nm resolution. The capabilities of quantitative electrostatic measurement and lateral charge density mapping make AFM a unique and powerful probe of membrane electrostatics.

Hybrid supercapacitor-battery materials for fast electrochemical charge storage

PubMed Central

Vlad, A.; Singh, N.; Rolland, J.; Melinte, S.; Ajayan, P. M.; Gohy, J.-F.

2014-01-01

High energy and high power electrochemical energy storage devices rely on different fundamental working principles - bulk vs. surface ion diffusion and electron conduction. Meeting both characteristics within a single or a pair of materials has been under intense investigations yet, severely hindered by intrinsic materials limitations. Here, we provide a solution to this issue and present an approach to design high energy and high power battery electrodes by hybridizing a nitroxide-polymer redox supercapacitor (PTMA) with a Li-ion battery material (LiFePO4). The PTMA constituent dominates the hybrid battery charge process and postpones the LiFePO4 voltage rise by virtue of its ultra-fast electrochemical response and higher working potential. We detail on a unique sequential charging mechanism in the hybrid electrode: PTMA undergoes oxidation to form high-potential redox species, which subsequently relax and charge the LiFePO4 by an internal charge transfer process. A rate capability equivalent to full battery recharge in less than 5 minutes is demonstrated. As a result of hybrid's components synergy, enhanced power and energy density as well as superior cycling stability are obtained, otherwise difficult to achieve from separate constituents. PMID:24603843

Method for imaging informational biological molecules on a semiconductor substrate

NASA Technical Reports Server (NTRS)

Coles, L. Stephen (Inventor)

1994-01-01

Imaging biological molecules such as DNA at rates several times faster than conventional imaging techniques is carried out using a patterned silicon wafer having nano-machined grooves which hold individual molecular strands and periodically spaced unique bar codes permitting repeatably locating all images. The strands are coaxed into the grooves preferably using gravity and pulsed electric fields which induce electric charge attraction to the molecular strands in the bottom surfaces of the grooves. Differential imaging removes substrate artifacts.

Surface charge accumulation of solid insulator under nanosecond pulse in vacuum: 3D distribution features and mechanism

NASA Astrophysics Data System (ADS)

Qi, Bo; Gao, Chunjia; Sun, Zelai; Li, Chengrong

2017-11-01

Surface charge accumulation can incur changes in electric field distribution, involved in the electron propagation process, and result in a significant decrease in the surface flashover voltage. The existing 2D surface charge measurement fails to meet the actual needs in real engineering applications that usually adopt the 45° conical frustum insulators. The present research developed a novel 3D measurement platform to capture surface charge distribution on solid insulation under nanosecond pulse in a vacuum. The results indicate that all surface charges are positive under a positive pulse and negative under a negative pulse. Surface charges tend to accumulate more near the upper electrode. Surface charge density increases significantly with the increase in pulse counts and amplitudes. Accumulation of surface charge results in a certain decrease of flashover voltage. Taking consideration of the secondary electron emission for the surface charge accumulation, four materials were obtained to demonstrate the effects on surface charge. Combining the effect incurred by secondary electron emission and the weighty action taken by surface charge accumulation on the flashover phenomena, the discharge mechanism along the insulator surface under nanosecond pulse voltage was proposed.

Amorphous Metal Polysulfides: Electrode Materials with Unique Insertion/Extraction Reactions.

PubMed

Sakuda, Atsushi; Ohara, Koji; Fukuda, Katsutoshi; Nakanishi, Koji; Kawaguchi, Tomoya; Arai, Hajime; Uchimoto, Yoshiharu; Ohta, Toshiaki; Matsubara, Eiichiro; Ogumi, Zempachi; Okumura, Toyoki; Kobayashi, Hironori; Kageyama, Hiroyuki; Shikano, Masahiro; Sakaebe, Hikari; Takeuchi, Tomonari

2017-07-05

A unique charge/discharge mechanism of amorphous TiS 4 is reported. Amorphous transition metal polysulfide electrodes exhibit anomalous charge/discharge performance and should have a unique charge/discharge mechanism: neither the typical intercalation/deintercalation mechanism nor the conversion-type one, but a mixture of the two. Analyzing the mechanism of such electrodes has been a challenge because fewer tools are available to examine the "amorphous" structure. It is revealed that the electrode undergoes two distinct structural changes: (i) the deformation and formation of S-S disulfide bonds and (ii) changes in the coordination number of titanium. These structural changes proceed continuously and concertedly for Li insertion/extraction. The results of this study provide a novel and unique model of amorphous electrode materials with significantly larger capacities.

Ultrafast adsorption and selective desorption of aqueous aromatic dyes by graphene sheets modified by graphene quantum dots

NASA Astrophysics Data System (ADS)

Ying, Yulong; He, Peng; Ding, Guqiao; Peng, Xinsheng

2016-06-01

Graphene modified by graphene quantum dots (GQDs) has been employed to remove toxic organic dyes. An excellent removal capacity (497 mg g-1) and record-breaking adsorption rate (475 mg g-1 min-1 at 20 °C) were demonstrated for Rhodamine B. The enhancement in performance by nearly a factor of three compared to that of graphene was ascribed to the greatly increased accessible surface area of graphene in aqueous solution as well as the increase in surface charges with the modification with GQDs. Besides, this unique adsorption behavior of the modified graphene was expanded to other typical toxic aqueous aromatic dyes such as Evans Blue, Methyl Orange, Malachite Green and Rose Bengal. What is more, a unique desorption behavior of dyes was first observed when employing different solvents, which enabled the GQD-modified graphene to be exploited for selective extraction of dyes and recycling of the adsorbent. The adsorption and desorption mechanism were further investigated. Combining high removal capacity, rapid adsorption kinetics, good recyclability and unique selective desorption, GQD-modified graphene has potential applications in both water purification and separation of aromatic dyes.

Measurements of charge distributions of the fragments in the low energy fission reaction

NASA Astrophysics Data System (ADS)

Wang, Taofeng; Han, Hongyin; Meng, Qinghua; Wang, Liming; Zhu, Liping; Xia, Haihong

2013-01-01

The measurement for charge distributions of fragments in spontaneous fission 252Cf has been performed by using a unique style of detector setup consisting of a typical grid ionization chamber and a ΔΕ-Ε particle telescope, in which a thin grid ionization chamber served as the ΔΕ-section and the E-section was an Au-Si surface barrier detector. The typical physical quantities of fragments, such as mass number and kinetic energies as well as the deposition in the gas ΔΕ detector and E detector were derived from the coincident measurement data. The charge distributions of the light fragments for the fixed mass number A2* and total kinetic energy (TKE) were obtained by the least-squares fits for the response functions of the ΔΕ detector with multi-Gaussian functions representing the different elements. The results of the charge distributions for some typical fragments are shown in this article which indicates that this detection setup has the charge distribution capability of Ζ:ΔΖ>40:1. The experimental method developed in this work for determining the charge distributions of fragments is expected to be employed in the neutron induced fissions of 232Th and 238U or other low energy fission reactions.

Ultrathin two-dimensional MnO2/graphene hybrid nanostructures for high-performance, flexible planar supercapacitors.

PubMed

Peng, Lele; Peng, Xu; Liu, Borui; Wu, Changzheng; Xie, Yi; Yu, Guihua

2013-05-08

Planar supercapacitors have recently attracted much attention owing to their unique and advantageous design for 2D nanomaterials based energy storage devices. However, improving the electrochemical performance of planar supercapacitors still remains a great challenge. Here we report for the first time a novel, high-performance in-plane supercapacitor based on hybrid nanostructures of quasi-2D ultrathin MnO2/graphene nanosheets. Specifically, the planar structures based on the δ-MnO2 nanosheets integrated on graphene sheets not only introduce more electrochemically active surfaces for absorption/desorption of electrolyte ions, but also bring additional interfaces at the hybridized interlayer areas to facilitate charge transport during charging/discharging processes. The unique structural design for planar supercapacitors enables great performance enhancements compared to graphene-only devices, exhibiting high specific capacitances of 267 F/g at current density of 0.2 A/g and 208 F/g at 10 A/g and excellent rate capability and cycling stability with capacitance retention of 92% after 7000 charge/discharge cycles. Moreover, the high planar malleability of planar supercapacitors makes possible superior flexibility and robust cyclability, yielding capacitance retention over 90% after 1000 times of folding/unfolding. Ultrathin 2D nanomaterials represent a promising material platform to realize highly flexible planar energy storage devices as the power back-ups for stretchable/flexible electronic devices.

A unique mid-sequence linker used to multimerize the lipid-phosphatidylserine (PS) binding peptide-peptoid hybrid PPS1.

PubMed

Shukla, Satya Prakash; Manarang, Joseph C; Udugamasooriya, D Gomika

2017-09-08

Ligand multimerizations enhance the binding affinity towards cell surface biomarkers through their avidity effects. Typical linkers connect individual monomeric ligand moieties from one end (e.g., C- or N-terminus of a peptide) and exclusively target protein receptors. The lipid phosphatidylserine (PS) is normally present on the cytoplasmic side of the eukaryotic cell membrane, but in tumors and tumor endothelial cells, this negatively charged PS flips to the outer layer. We recently reported a PS binding peptide-peptoid hybrid (PPS1) that has distinct positively charged and hydrophobic residue-containing regions. The PPS1 monomer is inactive, and upon C-terminal dimerization (PPS1D1), it triggers cytotoxicity. In the current study, a unique series of PPS1 multimeric derivatives were synthesized by switching the linker from the C-terminus to an internal position. The unimportant fourth residue (N-lys) from the C-terminus was utilized to build the linker. The synthesis strategy was developed employing variations of (I) the linker size, (II) the number of positively charged residues, and (III) the number of hydrophobic regions. Cytotoxicity of these new derivatives on HCC4017 lung cancer cells showed that a minimum of two hydrophobic regions was important to retain the activity and that the shortest linker length was optimal for activity. Copyright © 2017 Elsevier Masson SAS. All rights reserved.

Animated molecular dynamics simulations of hydrated caesium-smectite interlayers

PubMed Central

Sutton, Rebecca; Sposito, Garrison

2002-01-01

Computer animation of center of mass coordinates obtained from 800 ps molecular dynamics simulations of Cs-smectite hydrates (1/3 and 2/3 water monolayers) provided information concerning the structure and dynamics of the interlayer region that could not be obtained through traditional simulation analysis methods. Cs+ formed inner sphere complexes with the mineral surface, and could be seen to jump from one attracting location near a layer charge site to the next, while water molecules were observed to migrate from the hydration shell of one ion to that of another. Neighboring ions maintained a partial hydration shell by sharing water molecules, such that a single water molecule hydrated two ions simultaneously for hundreds of picoseconds. Cs-montmorillonite hydrates featured the largest extent of this sharing interaction, because interlayer ions were able to inhabit positions near surface cavities as well as at their edges, close to oxygen triads. The greater positional freedom of Cs+ within the montmorillonite interlayer, a result of structural hydroxyl orientation and low tetrahedral charge, promoted the optimization of distances between cations and water molecules required for water sharing. Preference of Cs+ for locations near oxygen triads was observed within interlayer beidellite and hectorite. Water molecules also could be seen to interact directly with the mineral surface, entering its surface cavities to approach attracting charge sites and structural hydroxyls. With increasing water content, water molecules exhibited increased frequency and duration of both cavity habitation and water sharing interactions. Competition between Cs+ and water molecules for surface sites was evident. These important cooperative and competitive features of interlayer molecular behavior were uniquely revealed by animation of an otherwise highly complex simulation output.

DNA surface hybridization regimes

PubMed Central

Gong, Ping; Levicky, Rastislav

2008-01-01

Surface hybridization reactions, in which sequence-specific recognition occurs between immobilized and solution nucleic acids, are routinely carried out to quantify and interpret genomic information. Although hybridization is fairly well understood in bulk solution, the greater complexity of an interfacial environment presents new challenges to a fundamental understanding, and hence application, of these assays. At a surface, molecular interactions are amplified by the two-dimensional nature of the immobilized layer, which focuses the nucleic acid charge and concentration to levels not encountered in solution, and which impacts the hybridization behavior in unique ways. This study finds that, at low ionic strengths, an electrostatic balance between the concentration of immobilized oligonucleotide charge and solution ionic strength governs the onset of hybridization. As ionic strength increases, the importance of electrostatics diminishes and the hybridization behavior becomes more complex. Suppression of hybridization affinity constants relative to solution values, and their weakened dependence on the concentration of DNA counterions, indicate that the immobilized strands form complexes that compete with hybridization to analyte strands. Moreover, an unusual regime is observed in which the surface coverage of immobilized oligonucleotides does not significantly influence the hybridization behavior, despite physical closeness and hence compulsory interactions between sites. These results are interpreted and summarized in a diagram of hybridization regimes that maps specific behaviors to experimental ranges of ionic strength and probe coverage. PMID:18381819

An Ideal Electrode Material, 3D Surface-Microporous Graphene for Supercapacitors with Ultrahigh Areal Capacitance

DOE PAGES

Chang, Liang; Stacchiola, Dario J.; Hu, Yun Hang

2017-07-03

The efficient charge accumulation of an ideal supercapacitor electrode requires abundant micropores and its fast electrolyte-ions transport prefers meso/macropores. But, current electrode materials cannot meet both requirements, resulting in poor performance. We creatively constructed three-dimensional cabbage-coral-like graphene as an ideal electrode material, in which meso/macro channels are formed by graphene walls and rich micropores are incorporated in the surface layer of the graphene walls. The unique 3D graphene material can achieve a high gravimetric capacitance of 200 F/g with aqueous electrolyte, 3 times larger than that of commercially used activated carbon (70.8 F/g). Furthermore, it can reach an ultrahigh arealmore » capacitance of 1.28 F/cm 2 and excellent rate capability (83.5% from 0.5 to 10 A/g) as well as high cycling stability (86.2% retention after 5000 cycles). The excellent electric double-layer performance of the 3D graphene electrode can be attributed to the fast electrolyte ion transport in the meso/macro channels and the rapid and reversible charge adsorption with negligible transport distance in the surface micropores.« less

An Ideal Electrode Material, 3D Surface-Microporous Graphene for Supercapacitors with Ultrahigh Areal Capacitance

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chang, Liang; Stacchiola, Dario J.; Hu, Yun Hang

The efficient charge accumulation of an ideal supercapacitor electrode requires abundant micropores and its fast electrolyte-ions transport prefers meso/macropores. But, current electrode materials cannot meet both requirements, resulting in poor performance. We creatively constructed three-dimensional cabbage-coral-like graphene as an ideal electrode material, in which meso/macro channels are formed by graphene walls and rich micropores are incorporated in the surface layer of the graphene walls. The unique 3D graphene material can achieve a high gravimetric capacitance of 200 F/g with aqueous electrolyte, 3 times larger than that of commercially used activated carbon (70.8 F/g). Furthermore, it can reach an ultrahigh arealmore » capacitance of 1.28 F/cm 2 and excellent rate capability (83.5% from 0.5 to 10 A/g) as well as high cycling stability (86.2% retention after 5000 cycles). The excellent electric double-layer performance of the 3D graphene electrode can be attributed to the fast electrolyte ion transport in the meso/macro channels and the rapid and reversible charge adsorption with negligible transport distance in the surface micropores.« less

Coexistent three-component and two-component Weyl phonons in TiS, ZrSe, and HfTe

NASA Astrophysics Data System (ADS)

Li, Jiangxu; Xie, Qing; Ullah, Sami; Li, Ronghan; Ma, Hui; Li, Dianzhong; Li, Yiyi; Chen, Xing-Qiu

2018-02-01

In analogy to various fermions of electrons in topological semimetals, topological mechanical states with two types of bosons, Dirac and Weyl bosons, were reported in some macroscopic systems of kHz frequency, and those with a type of doubly-Weyl phonons in atomic vibrational framework of THz frequency of solid crystals were recently predicted. Here, through first-principles calculations, we have reported that the phonon spectra of the WC-type TiS, ZrSe, and HfTe commonly host the unique triply degenerate nodal points (TDNPs) and single two-component Weyl points (WPs) in THz frequency. Quasiparticle excitations near TDNPs of phonons are three-component bosons, beyond the conventional and known classifications of Dirac, Weyl, and doubly-Weyl phonons. Moreover, we have found that both TiS and ZrSe have five pairs of type-I Weyl phonons and a pair of type-II Weyl phonons, whereas HfTe only has four pairs of type-I Weyl phonons. They carry nonzero topological charges. On the (10 1 ¯0 ) crystal surfaces, we observe topological protected surface arc states connecting two WPs with opposite charges, which host modes that propagate nearly in one direction on the surface.

Metal-chelate dye-controlled organization of Cd32S14(SPh)40(4-) nanoclusters into three-dimensional molecular and covalent open architecture.

PubMed

Zheng, Nanfeng; Lu, Haiwei; Bu, Xianhui; Feng, Pingyun

2006-04-12

Chalcogenide II-VI nanoclusters are usually prepared as isolated clusters and have defied numerous efforts to join them into covalent open-framework architecture with conventional templating methods such as protonated amines or inorganic cations commonly used to direct the formation of porous frameworks. Herein, we report the first templated synthesis of II-VI covalent superlattices from large II-VI tetrahedral clusters (i.e., [Cd32S14(SPh)38]2-). Our method takes advantage of low charge density of metal-chelate dyes that is a unique match with three-dimensional II-VI semiconductor frameworks in charge density, surface hydrophilicity-hydrophobicity, and spatial organization. In addition, metal-chelate dyes also serve to tune the optical properties of resulting dye semiconductor composite materials.

Reborn quadrant anode image sensor

NASA Astrophysics Data System (ADS)

Prokazov, Yury; Turbin, Evgeny; Vitali, Marco; Herzog, Andreas; Michaelis, Bernd; Zuschratter, Werner; Kemnitz, Klaus

2009-06-01

We describe a position sensitive photon counting microchannel plate based detector with an improved quadrant anode (QA) readout system. The technique relies on a combination of the four planar elements pattern and an additional fifth electrode. The charge cloud induced by single particle detection is split between the electrodes. The measured charge values uniquely define the position of the initial event. QA has been first published in 1976 by Lampton and Malina. This anode configuration was undeservedly forgotten and its potential has been hardly underestimated. The presented approach extends the operating spatial range to the whole sensitive area of the microchannel plate surface and demonstrates good linearity over the field of view. Therefore, the novel image sensor results in spatial resolution better then 50 μm and count rates up to one million events per second.

Quantification of surface charge density and its effect on boundary slip.

PubMed

Jing, Dalei; Bhushan, Bharat

2013-06-11

Reduction of fluid drag is important in the micro-/nanofluidic systems. Surface charge and boundary slip can affect the fluid drag, and surface charge is also believed to affect boundary slip. The quantification of surface charge and boundary slip at a solid-liquid interface has been widely studied, but there is a lack of understanding of the effect of surface charge on boundary slip. In this paper, the surface charge density of borosilicate glass and octadecyltrichlorosilane (OTS) surfaces immersed in saline solutions with two ionic concentrations and deionized (DI) water with different pH values and electric field values is quantified by fitting experimental atomic force microscopy (AFM) electrostatic force data using a theoretical model relating the surface charge density and electrostatic force. Results show that pH and electric field can affect the surface charge density of glass and OTS surfaces immersed in saline solutions and DI water. The mechanisms of the effect of pH and electric field on the surface charge density are discussed. The slip length of the OTS surface immersed in saline solutions with two ionic concentrations and DI water with different pH values and electric field values is measured, and their effects on the slip length are analyzed from the point of surface charge. Results show that a larger absolute value of surface charge density leads to a smaller slip length for the OTS surface.

Amphiphilic Cyclodextrin Derivatives for Targeted Drug Delivery to Tumors.

PubMed

Erdogar, Nazlı; Varan, Gamze; Bilensoy, Erem

2017-01-01

Villiers has extensively studied cyclodextrins, a family of macrocyclic oligosaccharides linked by α-1,4 glycosidic bonds, in different fields since their discovery in 1891. The unique structure enabling inclusion complexation for natural cyclodextrins and cyclodextrin derivatives make them attractive for novel drug delivery systems. Cyclodextrins can be modified with long aliphatic chains to render an amphiphilic property and these different amphiphilic cyclodextrins are able to form nanoparticles without surfactants. In the literature, several different amphiphilic cyclodextrins are reported and applied to drug delivery and targeting especially to tumors. Specificly, folateconjugated amphiphilic cyclodextrin derivatives are used for active tumor targeting of poorly water soluble drugs and improve the efficacy and safety of therapeutic agents. On the other hand, effect of positive surface charge has also been under research in the recent years. Polycationic amphiphilic cyclodextrins have shown promise towards forming small complexes with negatively charged molecules such as drugs or plasmid DNA. Polycationic amphiphilic cyclodextrins enhance interaction with cell membrane due to their net positive surface charge. The scope of this review is to describe potential uses and pharmaceutical applications of tumor-targeted amphiphilic cyclodextrins, with focus on folate-conjugated cyclodextrin derivatives and polycationic cyclodextrin derivatives both studied by our group at Hacettepe University. Copyright© Bentham Science Publishers; For any queries, please email at epub@benthamscience.org.

An equivalent body surface charge model representing three-dimensional bioelectrical activity

NASA Technical Reports Server (NTRS)

He, B.; Chernyak, Y. B.; Cohen, R. J.

1995-01-01

A new surface-source model has been developed to account for the bioelectrical potential on the body surface. A single-layer surface-charge model on the body surface has been developed to equivalently represent bioelectrical sources inside the body. The boundary conditions on the body surface are discussed in relation to the surface-charge in a half-space conductive medium. The equivalent body surface-charge is shown to be proportional to the normal component of the electric field on the body surface just outside the body. The spatial resolution of the equivalent surface-charge distribution appears intermediate between those of the body surface potential distribution and the body surface Laplacian distribution. An analytic relationship between the equivalent surface-charge and the surface Laplacian of the potential was found for a half-space conductive medium. The effects of finite spatial sampling and noise on the reconstruction of the equivalent surface-charge were evaluated by computer simulations. It was found through computer simulations that the reconstruction of the equivalent body surface-charge from the body surface Laplacian distribution is very stable against noise and finite spatial sampling. The present results suggest that the equivalent body surface-charge model may provide an additional insight to our understanding of bioelectric phenomena.

Fabrication of highly ordered polyaniline nanocone on pristine graphene for high-performance supercapacitor electrodes

NASA Astrophysics Data System (ADS)

Song, Ningning; Wang, Wucong; Wu, Yue; Xiao, Ding; Zhao, Yaping

2018-04-01

The hybrids of pristine graphene with polyaniline were synthesized by in situ polymerizations for making a high-performance supercapacitor. The formed high-ordered PANI nanocones were vertically aligned on the graphene sheets. The length of the PANI nanocones increased with the concentration of aniline monomer. The specific capacitance of the hybrids electrode in the three-electrode system was measured as high as 481 F/g at a current density of 0.1 A/g, and its stability remained 87% after constant charge-discharge 10000 cycles at a current density of 1 A/g. This outstanding performance is attributed to the coupling effects of the pristine graphene and the hierarchical structure of the PANI possessing high specific surface area. The unique structure of the PANI provided more charge transmission pathways and fast charge-transfer speed of electrons to the pristine graphene because of its large specific area exposed to the electrolyte. The hybrid is expected to have potential applications in supercapacitor electrodes.

Open and closed loop manipulation of charged microchiplets in an electric field

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lu, J. P., E-mail: jplu@parc.com; Thompson, J. D.; Whiting, G. L.

We demonstrate the ability to orient, position, and transport microchips (“chiplets”) with electric fields. In an open-loop approach, modified four phase traveling wave potential patterns manipulate chiplets in a dielectric solution using dynamic template agitation techniques. Repeatable parallel assembly of chiplets is demonstrated to a positional accuracy of 6.5 μm using electrodes of 200 μm pitch. Chiplets with dipole surface charge patterns are used to show that orientation can be controlled by adding unique charge patterns on the chiplets. Chip path routing is also demonstrated. With a closed-loop control system approach using video feedback, dielectric, and electrophoretic forces are used to achievemore » positioning accuracy of better than 1 μm with 1 mm pitch driving electrodes. These chip assembly techniques have the potential to enable future printer systems where inputs are electronic chiplets and the output is a functional electronic system.« less

Upconversion-Triggered Charge Separation in Polymer Semiconductors.

PubMed

Jang, Yu Jin; Kim, Eunah; Ahn, Seonghyeon; Chung, Kyungwha; Kim, Jihyeon; Kim, Heejun; Wang, Huan; Lee, Jiseok; Kim, Dong-Wook; Kim, Dong Ha

2017-01-19

Upconversion is a unique optical property that is driven by a sequential photon pumping and generation of higher energy photons in a consecutive manner. The efficiency improvement in photovoltaic devices can be achieved when upconverters are integrated since upconverters contribute to the generation of extra photons. Despite numerous experimental studies confirming the relationship, fundamental explanations for a real contribution of upconversion to photovoltaic efficiency are still in demand. In this respect, we suggest a new approach to visualize the upconversion event in terms of surface photovoltage (SPV) by virtue of Kelvin probe force microscopy (KPFM). One of the most conventional polymer semiconductors, poly(3-hexyl thiophene) (P3HT), is employed as a sensitizer to generate charge carriers by upconverted light. KPFM measurements reveal that the light upconversion enabled the formation of charge carriers in P3HT, resulting in large SPV of -54.9 mV. It confirms that the energy transfer from upconverters to P3HT can positively impact the device performance in organic solar cells (OSCs).

Low energy positrons as probes of reconstructed semiconductor surfaces.

NASA Astrophysics Data System (ADS)

Fazleev, Nail G.; Weiss, Alex H.

2007-03-01

Positron probes of semiconductor surfaces that play a fundamental role in modern science and technology are capable to non-destructively provide information that is both unique to the probe and complimentary to that extracted using other more standard techniques. We discuss recent progress in studies of the reconstructed Si(100), Si(111), Ge(100), and Ge(111) surfaces, clean and exposed to hydrogen and oxygen, using a surface characterization technique, Positron-Annihilation-Induced Auger-Electron Spectroscopy (PAES). Experimental PAES results are analyzed by performing first-principles calculations of positron surface states and annihilation probabilities of surface-trapped positrons with relevant core electrons for the reconstructed surfaces, taking into account discrete lattice effects, the electronic reorganization due to bonding, and charge redistribution effects at the surface. Effects of the hydrogen and oxygen adsorption on semiconductor surfaces on localization of positron surface state wave functions and annihilation characteristics are also analyzed. Theoretical calculations confirm that PAES intensities, which are proportional to annihilation probabilities of the surface trapped positrons that results in a core hole, are sensitive to the crystal face, surface structure and elemental content of the semiconductors.

Reversible Adhesion with Polyelectrolyte Brushes Tailored via the Uptake and Release of Trivalent Lanthanum Ions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Farina, Robert; Laugel, Nicolas; Yu, Jing

Applications of end-tethered polyelectrolyte “brushes” to modify solid surfaces have been developed and studied for their colloidal stabilization and high lubrication properties. Current efforts have expanded into biological realms and stimuli-responsive materials. Our work explores responsive and reversible aspects of polyelectrolyte brush behavior when polyelectrolyte chains interact with oppositely charged multivalent ions and complexes, which act as counterions. There is a significant void in the polyelectrolyte literature regarding interactions with multivalent species. This paper demonstrates that interactions between solid surfaces bearing negatively charged polyelectrolyte brushes are highly sensitive to the presence of trivalent lanthanum, La3+. Lanthanum cations have unique interactionsmore » with polyelectrolyte chains, in part due to their small size and hydration radius which results in a high local charge density. Using La3+ in conjunction with the surface forces apparatus (SFA), adhesion has been observed to reversibly appear and disappear upon the uptake and release, respectively, of these multivalent cations acting as counterions. In media of fixed ionic strength set by monovalent sodium salt, at I0 = 0.003 M and I0 = 0.3 M, the sign of the interaction forces between overlapping brushes changes from repulsive to attractive when La3+ concentrations reach 0.1 mol % of the total ion concentration. These results are also shown to be generally consistent with, but subtlety different from, previous polyelectrolyte brush experiments using trivalent ruthenium hexamine in the role of the multivalent counterion.« less

MAPs/bFGF-PLGA microsphere composite-coated titanium surfaces promote increased adhesion and proliferation of fibroblasts.

PubMed

Wang, Zhongshan; Wu, Guofeng; Bai, Shizhu; Feng, Zhihong; Dong, Yan; Zhou, Jian; Qin, Haiyan; Zhao, Yimin

2014-06-01

Infection and epithelial downgrowth are two major problems with maxillofacial transcutaneous implants, and both are mainly due to lack of stable closure of soft tissues at transcutaneous sites. Fibroblasts have been shown to play a key role in the formation of biological seals. In this work, titanium (Ti) model surfaces were coated with mussel adhesive proteins (MAPs) utilizing its unique adhesion ability on diverse inorganic and organic surfaces in wet environments. Prepared basic fibroblast growth factor (bFGF)-poly(lactic-co-glycolic acid) (PLGA) microspheres can be easily synthesized and combined onto MAPs-coated Ti surfaces, due to the negative surface charges of microspheres in aqueous solution, which is in contrast to the positive charges of MAPs. Titanium model surfaces were divided into three groups. Group A: MAPs/bFGF-PLGA microspheres composite-coated Ti surfaces. Group B: MAPs-coated Ti surfaces. Group C: uncoated Ti surfaces. The effects of coated Ti surfaces on adhesion of fibroblasts, cytoskeletal organization, proliferation, and extracellular matrix (ECM)-related gene expressions were examined. The results revealed increased adhesion (P < 0.05), enhanced actin cytoskeletal organization, and up-regulated ECM-related gene expressions in groups A and B compared with group C. Increased proliferation of fibroblasts during five days of incubation was observed in group A compared with groups B and C (P < 0.05). Collectively, the results from this in vitro study demonstrated that MAPs/bFGF-PLGA microspheres composite-coated Ti surfaces had the ability to increase fibroblast functionality. In addition, MAPs/bFGF-PLGA microsphere composite-coated Ti surfaces should be studied further as a method of promoting formation of stable biological seals around transcutaneous sites.

Experimental and DFT studies of gold nanoparticles supported on MgO(111) nano-sheets and their catalytic activity.

PubMed

Li, Zhi; Ciobanu, Cristian V; Hu, Juncheng; Palomares-Báez, Juan-Pedro; Rodríguez-López, José-Luis; Richards, Ryan

2011-02-21

A wet chemical preparation of MgO with the (111) facet as the primary surface has recently been reported and with alternating layers of oxygen anions and magnesium cations, this material shows unique chemical and physical properties. The potential to utilize the MgO(111) surface for the immobilization of metal particles is intriguing because the surface itself offers a very different environment for the metal particle with an all oxygen interface, as opposed to the typical (100) facet that possesses alternating oxygen anion and magnesium cation sites on the surface. Gold nanoparticles have demonstrated a broad range of interesting catalytic properties, but are often susceptible to aggregation at high temperatures and are very sensitive to substrate effects. Here, we investigate gold-supported on MgO(111) nanosheets as a catalyst system for the aerobic oxidation of benzyl alcohol. Gold nanoparticles deposited on MgO(111) show an increased level of activity in the solvent-free benzyl alcohol aerobic oxidation as compared to gold nanoparticles deposited on a typical MgO aerogel. TEM studies reveal that the gold nanoparticles have a hemispherical shape while sitting on the main surface of MgO(111) nanosheets, with a large Au-MgO interface. Given that the gold nanoparticles deposited on the two types of MgO have similar size, and that the two types of unmodified MgO show almost the same activities in the blank reaction, we infer that the high activity of Au/MgO(111) is due to the properties of the (111) support and/or those of the gold-support interface. To understand the binding of Au on low-index MgO surfaces and the charge distribution at the surface of the support, we have performed density functional theory (DFT) calculations on all low-index MgO substrates (with and without gold), using a model Au(10) cluster. Due to similar lattice constants of Au(111) and MgO(111) planes, the Au cluster retains its structural integrity and binds strongly on MgO(111) with either oxygen or magnesium termination. Furthermore, we have found that for the (001) and (110) substrates the charges of the ions in the top surface layer have similar values as in bulk MgO, but that on (111) surfaces these charges are significantly different. This difference in surface charge determines the direction of the electronic transfer upon adsorption of gold, such transfer occurring so as to restore the bulk MgO charge values. Using the results from theoretical calculations, we provide an explanation of our observations of increased catalytic activity in the case of the Au/MgO(111) system.

Mass Spectrometry of Acoustically Levitated Droplets

PubMed Central

Westphall, Michael S.; Jorabchi, Kaveh; Smith, Lloyd M.

2008-01-01

Containerless sample handling techniques such as acoustic levitation offer potential advantages for mass spectrometry, by eliminating surfaces where undesired adsorption/desorption processes can occur. In addition, they provide a unique opportunity to study fundamental aspects of the ionization process as well as phenomena occurring at the air–droplet interface. Realizing these advantages is contingent, however, upon being able to effectively interface levitated droplets with a mass spectrometer, a challenging task that is addressed in this report. We have employed a newly developed charge and matrix-assisted laser desorption/ionization (CALDI) technique to obtain mass spectra from a 5-μL acoustically levitated droplet containing peptides and an ionic matrix. A four-ring electrostatic lens is used in conjunction with a corona needle to produce bursts of corona ions and to direct those ions toward the droplet, resulting in droplet charging. Analyte ions are produced from the droplet by a 337-nm laser pulse and detected by an atmospheric sampling mass spectrometer. The ion generation and extraction cycle is repeated at 20 Hz, the maximum operating frequency of the laser employed. It is shown in delayed ion extraction experiments that both positive and negative ions are produced, behavior similar to that observed for atmospheric pressure matrix-assisted laser absorption/ionization. No ion signal is observed in the absence of droplet charging. It is likely, although not yet proven, that the role of the droplet charging is to increase the strength of the electric field at the surface of the droplet, reducing chargere combination after ion desorption. PMID:18582090

Fast and efficient charge breeding of the Californium rare isotope breeder upgrade electron beam ion source

DOE PAGES

Ostroumov, P. N.; Barcikowski, A.; Dickerson, C. A.; ...

2015-08-28

The Electron Beam Ion Source (EBIS), developed to breed Californium Rare Isotope Breeder Upgrade (CARIBU) radioactive beams at Argonne Tandem Linac Accelerator System (ATLAS), is being tested off-line. A unique property of the EBIS is a combination of short breeding times, high repetition rates, and a large acceptance. Overall, we have implemented many innovative features during the design and construction of the CARIBU EBIS as compared to the existing EBIS breeders. The off-line charge breeding tests are being performed using a surface ionization source that produces singly charged cesium ions. The main goal of the off-line commissioning is to demonstratemore » stable operation of the EBIS at a 10 Hz repetition rate and a breeding efficiency into single charge state higher than 15%. These goals have been successfully achieved and exceeded. We have measured (20% ± 0.7%) breeding efficiency into the single charge state of 28+ cesium ions with the breeding time of 28 ms. In general, the current CARIBU EBIS operational parameters can provide charge breeding of any ions in the full mass range of periodic table with high efficiency, short breeding times, and sufficiently low charge-to-mass ratio, 1/6.3 for the heaviest masses, for further acceleration in ATLAS. In this study, we discuss the parameters of the EBIS and the charge breeding results in a pulsed injection mode with repetition rates up to 10 Hz.« less

Charge properties and bacterial contact-killing of hyperbranched polyurea-polyethyleneimine coatings with various degrees of alkylation

NASA Astrophysics Data System (ADS)

Roest, Steven; van der Mei, Henny C.; Loontjens, Ton J. A.; Busscher, Henk J.

2015-11-01

Coatings of immobilized-quaternary-ammonium-ions (QUAT) uniquely kill adhering bacteria upon contact. QUAT-coatings require a minimal cationic-charge surface density for effective contact-killing of adhering bacteria of around 1014 cm-2. Quaternization of nitrogen is generally achieved through alkylation. Here, we investigate the contribution of additional alkylation with methyl-iodide to the cationic-charge density of hexyl-bromide alkylated, hyperbranched polyurea-polyethyleneimine coatings measuring charge density with fluorescein staining. X-ray-photoelectron-spectroscopy was used to determine the at.% alkylated-nitrogen. Also streaming potentials, water contact-angles and bacterial contact-killing were measured. Cationic-charge density increased with methyl-iodide alkylation times up to 18 h, accompanied by an increase in the at.% alkylated-nitrogen. Zeta-potentials became more negative upon alkylation as a result of shielding of cationiccharges by hydrophobic alkyl-chains. Contact-killing of Gram-positive Staphylococci only occurred when the cationic-charge density exceeded 1016 cm-2 and was carried by alkylated-nitrogen (electron-binding energy 401.3 eV). Gram-negative Escherichia coli was not killed upon contact with the coatings. There with this study reveals that cationic-charge density is neither appropriate nor sufficient to determine the ability of QUAT-coatings to kill adhering bacteria. Alternatively, the at.% of alkylated-nitrogen at 401.3 eV is proposed, as it reflects both cationic-charge and its carrier. The at.% N401.3 eV should be above 0.45 at.% for Gram-positive bacterial contact-killing.

Fast and efficient charge breeding of the Californium rare isotope breeder upgrade electron beam ion source

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ostroumov, P. N.; Barcikowski, A.; Dickerson, C. A.

The Electron Beam Ion Source (EBIS), developed to breed Californium Rare Isotope Breeder Upgrade (CARIBU) radioactive beams at Argonne Tandem Linac Accelerator System (ATLAS), is being tested off-line. A unique property of the EBIS is a combination of short breeding times, high repetition rates, and a large acceptance. Overall, we have implemented many innovative features during the design and construction of the CARIBU EBIS as compared to the existing EBIS breeders. The off-line charge breeding tests are being performed using a surface ionization source that produces singly charged cesium ions. The main goal of the off-line commissioning is to demonstratemore » stable operation of the EBIS at a 10 Hz repetition rate and a breeding efficiency into single charge state higher than 15%. These goals have been successfully achieved and exceeded. We have measured (20% ± 0.7%) breeding efficiency into the single charge state of 28+ cesium ions with the breeding time of 28 ms. In general, the current CARIBU EBIS operational parameters can provide charge breeding of any ions in the full mass range of periodic table with high efficiency, short breeding times, and sufficiently low charge-to-mass ratio, 1/6.3 for the heaviest masses, for further acceleration in ATLAS. In this study, we discuss the parameters of the EBIS and the charge breeding results in a pulsed injection mode with repetition rates up to 10 Hz.« less

Fast and efficient charge breeding of the Californium rare isotope breeder upgrade electron beam ion source

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ostroumov, P. N., E-mail: ostroumov@anl.gov; Barcikowski, A.; Dickerson, C. A.

The Electron Beam Ion Source (EBIS), developed to breed Californium Rare Isotope Breeder Upgrade (CARIBU) radioactive beams at Argonne Tandem Linac Accelerator System (ATLAS), is being tested off-line. A unique property of the EBIS is a combination of short breeding times, high repetition rates, and a large acceptance. Overall, we have implemented many innovative features during the design and construction of the CARIBU EBIS as compared to the existing EBIS breeders. The off-line charge breeding tests are being performed using a surface ionization source that produces singly charged cesium ions. The main goal of the off-line commissioning is to demonstratemore » stable operation of the EBIS at a 10 Hz repetition rate and a breeding efficiency into single charge state higher than 15%. These goals have been successfully achieved and exceeded. We have measured (20% ± 0.7%) breeding efficiency into the single charge state of 28+ cesium ions with the breeding time of 28 ms. In general, the current CARIBU EBIS operational parameters can provide charge breeding of any ions in the full mass range of periodic table with high efficiency, short breeding times, and sufficiently low charge-to-mass ratio, 1/6.3 for the heaviest masses, for further acceleration in ATLAS. In this paper, we discuss the parameters of the EBIS and the charge breeding results in a pulsed injection mode with repetition rates up to 10 Hz.« less

Nanoscale surface modification of Li-rich layered oxides for high-capacity cathodes in Li-ion batteries

NASA Astrophysics Data System (ADS)

Lan, Xiwei; Xin, Yue; Wang, Libin; Hu, Xianluo

2018-03-01

Li-rich layered oxides (LLOs) have been developed as a high-capacity cathode material for Li-ion batteries, but the structural complexity and unique initial charging behavior lead to several problems including large initial capacity loss, capacity and voltage fading, poor cyclability, and inferior rate capability. Since the surface conditions are critical to electrochemical performance and the drawbacks, nanoscale surface modification for improving LLO's properties is a general strategy. This review mainly summarizes the surface modification of LLOs and classifies them into three types of surface pre-treatment, surface gradient doping, and surface coating. Surface pre-treatment usually introduces removal of Li2O for lower irreversible capacity while surface doping is aimed to stabilize the structure during electrochemical cycling. Surface coating layers with different properties, protective layers to suppress the interface side reaction, coating layers related to structural transformation, and electronic/ionic conductive layers for better rate capability, can avoid the shortcomings of LLOs. In addition to surface modification for performance enhancement, other strategies can also be investigated to achieve high-performance LLO-based cathode materials.

Upregulation of BMSCs Osteogenesis by Positively-Charged Tertiary Amines on Polymeric Implants via Charge/iNOS Signaling Pathway

PubMed Central

Zhang, Wei; Liu, Na; Shi, Haigang; Liu, Jun; Shi, Lianxin; Zhang, Bo; Wang, Huaiyu; Ji, Junhui; Chu, Paul K.

2015-01-01

Positively-charged surfaces on implants have a similar potential to upregulate osteogenesis of bone marrow-derived mesenchymal stem cells (BMSCs) as electromagnetic therapy approved for bone regeneration. Generally, their osteogenesis functions are generally considered to stem from the charge-induced adhesion of extracellular matrix (ECM) proteins without exploring the underlying surface charge/cell signaling molecule pathways. Herein, a positively-charged surface with controllable tertiary amines is produced on a polymer implant by plasma surface modification. In addition to inhibiting the TNF-α expression, the positively-charged surface with tertiary amines exhibits excellent cytocompatibility as well as remarkably upregulated osteogenesis-related gene/protein expressions and calcification of the contacted BMSCs. Stimulated by the charged surface, these BMSCs display high iNOS expressions among the three NOS isoforms. Meanwhile, downregulation of the iNOS by L-Can or siRNA inhibit osteogenic differentiation in the BMSCs. These findings suggest that a positively-charged surface with tertiary amines induces osteogenesis of BMSCs via the surface charge/iNOS signaling pathway in addition to elevated ECM protein adhesion. Therefore, creating a positively-charged surface with tertiary amines is a promising approach to promote osseointegration with bone tissues. PMID:25791957

Synthesis of the RGO/Al2O3 core-shell nanocomposite flakes and characterization of their unique electrostatic properties using zeta potential measurements

NASA Astrophysics Data System (ADS)

Jastrzębska, A. M.; Karcz, J.; Letmanowski, R.; Zabost, D.; Ciecierska, E.; Zdunek, J.; Karwowska, E.; Siekierski, M.; Olszyna, A.; Kunicki, A.

2016-01-01

The aim of this study was to describe the influence of the modification of electrostatic properties of RGO/Al2O3 core-shell nanocomposite flakes. The amount of crystalline form of aluminum oxide was very small. It existed mostly in amorphous phase in the form of covalently bonded to GO surface. The morphological, structural and physicochemical investigations results showed that spherical Al2O3 nanoparticles (ca. 41 nm) in gamma phase completely covered the surface of curly-shaped RGO flakes and acted as a spreader between individual flakes. The high BET specific surface area of the analyzed composite (119.71 m2/g) together with very low open porosity (0.479 cm3/g) indicated that RGO/Al2O3 nanocomposite flakes showed low tendency to agglomeration. The zeta potential curves obtained for RGO/Al2O3 core-shell nanocomposite flakes were differing from curves obtained for GO and Al2O3 suspensions in distilled water and neutral environment. The specific electrostatic properties of the core-shell system of RGO/Al2O3 flakes had an influence on its surface charge (zeta potential) which was measured by applying an external electric field. The FTIR and Raman investigations results also confirmed that the Cdbnd O species were not taking part in the surface amphoteric reactions resulting in the formation of electrostatic surface charge.

Modulation of protein stability and aggregation properties by surface charge engineering.

PubMed

Raghunathan, Govindan; Sokalingam, Sriram; Soundrarajan, Nagasundarapandian; Madan, Bharat; Munussami, Ganapathiraman; Lee, Sun-Gu

2013-09-01

An attempt to alter protein surface charges through traditional protein engineering approaches often affects the native protein structure significantly and induces misfolding. This limitation is a major hindrance in modulating protein properties through surface charge variations. In this study, as a strategy to overcome such a limitation, we attempted to co-introduce stabilizing mutations that can neutralize the destabilizing effect of protein surface charge variation. Two sets of rational mutations were designed; one to increase the number of surface charged amino acids and the other to decrease the number of surface charged amino acids by mutating surface polar uncharged amino acids and charged amino acids, respectively. These two sets of mutations were introduced into Green Fluorescent Protein (GFP) together with or without stabilizing mutations. The co-introduction of stabilizing mutations along with mutations for surface charge modification allowed us to obtain functionally active protein variants (s-GFP(+15-17) and s-GFP(+5-6)). When the protein properties such as fluorescent activity, folding rate and kinetic stability were assessed, we found the possibility that the protein stability can be modulated independently of activity and folding by engineering protein surface charges. The aggregation properties of GFP could also be altered through the surface charge engineering.

Molecular simulation study of feruloyl esterase adsorption on charged surfaces: effects of surface charge density and ionic strength.

PubMed

Liu, Jie; Peng, Chunwang; Yu, Gaobo; Zhou, Jian

2015-10-06

The surrounding conditions, such as surface charge density and ionic strength, play an important role in enzyme adsorption. The adsorption of a nonmodular type-A feruloyl esterase from Aspergillus niger (AnFaeA) on charged surfaces was investigated by parallel tempering Monte Carlo (PTMC) and all-atom molecular dynamics (AAMD) simulations at different surface charge densities (±0.05 and ±0.16 C·m(-2)) and ionic strengths (0.007 and 0.154 M). The adsorption energy, orientation, and conformational changes were analyzed. Simulation results show that whether AnFaeA can adsorb onto a charged surface is mainly controlled by electrostatic interactions between AnFaeA and the charged surface. The electrostatic interactions between AnFaeA and charged surfaces are weakened when the ionic strength increases. The positively charged surface at low surface charge density and high ionic strength conditions can maximize the utilization of the immobilized AnFaeA. The counterion layer plays a key role in the adsorption of AnFaeA on the negatively charged COOH-SAM. The native conformation of AnFaeA is well preserved under all of these conditions. The results of this work can be used for the controlled immobilization of AnFaeA.

Mechanism of the dielectric enhancement in polymer-alumina nano-particle composites

NASA Astrophysics Data System (ADS)

Jacob, Rebecca; Jacob, Anne Pavitra; Mainwaring, David E.

2009-09-01

Polymer-alumina nano-composites with enhanced dielectric properties as a possibility to enable the miniaturization of devices have been reported. The enhancement of dielectric properties was found to be unique to the polymer. In the present work, the mechanism of the dielectric enhancement is established by performing ab initio molecular orbital calculations in order to study the molecular interactions in the interfacial region between the alumina-nano-particle surface and the polymer medium. The calculations predict the existence of strong electrostatic attraction between the positive charge on the aluminium of the alumina clusters and the negative charge of the oxygens of the polymer at the polymer-nano-particle interface resulting in an increase in the dipole moment and the polarization of the system leading to enhanced dielectric properties. The oxygen thus plays a dual role by involving in covalent bonding with the polymer chain and electrostatic bonding interactions with the alumina nano-particles. The unique structure of the polymer provides the highly electronegative oxygens, as carbonyl groups or ether linkages in conjugation with aromatic rings in an extended polymer chain system, facilitating this type of bonding at the interface.

Crystal step edges can trap electrons on the surfaces of n-type organic semiconductors.

PubMed

He, Tao; Wu, Yanfei; D'Avino, Gabriele; Schmidt, Elliot; Stolte, Matthias; Cornil, Jérôme; Beljonne, David; Ruden, P Paul; Würthner, Frank; Frisbie, C Daniel

2018-05-30

Understanding relationships between microstructure and electrical transport is an important goal for the materials science of organic semiconductors. Combining high-resolution surface potential mapping by scanning Kelvin probe microscopy (SKPM) with systematic field effect transport measurements, we show that step edges can trap electrons on the surfaces of single crystal organic semiconductors. n-type organic semiconductor crystals exhibiting positive step edge surface potentials display threshold voltages that increase and carrier mobilities that decrease with increasing step density, characteristic of trapping, whereas crystals that do not have positive step edge surface potentials do not have strongly step density dependent transport. A device model and microelectrostatics calculations suggest that trapping can be intrinsic to step edges for crystals of molecules with polar substituents. The results provide a unique example of a specific microstructure-charge trapping relationship and highlight the utility of surface potential imaging in combination with transport measurements as a productive strategy for uncovering microscopic structure-property relationships in organic semiconductors.

Effect of Surface Hydration on Antifouling Properties of Mixed Charged Polymers.

PubMed

Leng, Chuan; Huang, Hao; Zhang, Kexin; Hung, Hsiang-Chieh; Xu, Yao; Li, Yaoxin; Jiang, Shaoyi; Chen, Zhan

2018-05-07

Interfacial water structure on a polymer surface in water (or surface hydration) is related to the antifouling activity of the polymer. Zwitterionic polymer materials exhibit excellent antifouling activity due to their strong surface hydration. It was proposed to replace zwitterionic polymers using mixed charged polymers because it is much easier to prepare mixed charged polymer samples with much lower costs. In this study, using sum frequency generation (SFG) vibrational spectroscopy, we investigated interfacial water structures on mixed charged polymer surfaces in water, and how such structures change while exposing to salt solutions and protein solutions. The 1:1 mixed charged polymer exhibits excellent antifouling property while other mixed charged polymers with different ratios of the positive/negative charges do not. It was found that on the 1:1 mixed charged polymer surface, SFG water signal is dominated by the contribution of the strongly hydrogen bonded water molecules, indicating strong hydration of the polymer surface. The responses of the 1:1 mixed charged polymer surface to salt solutions are similar to those of zwitterionic polymers. Interestingly, exposure to high concentrations of salt solutions leads to stronger hydration of the 1:1 mixed charged polymer surface after replacing the salt solution with water. Protein molecules do not substantially perturb the interfacial water structure on the 1:1 mixed charged polymer surface and do not adsorb to the surface, showing that this mixed charged polymer is an excellent antifouling material.

Effects of Discrete Charge Clustering in Simulations of Charged Interfaces.

PubMed

Grime, John M A; Khan, Malek O

2010-10-12

A system of counterions between charged surfaces is investigated, with the surfaces represented by uniform charged planes and three different arrangements of discrete surface charges - an equispaced grid and two different clustered arrangements. The behaviors of a series of systems with identical net surface charge density are examined, with particular emphasis placed on the long ranged corrections via the method of "charged slabs" and the effects of the simulation cell size. Marked differences are observed in counterion distributions and the osmotic pressure dependent on the particular representation of the charged surfaces; the uniformly charged surfaces and equispaced grids of discrete charge behave in a broadly similar manner, but the clustered systems display a pronounced decrease in osmotic pressure as the simulation size is increased. The influence of the long ranged correction is shown to be minimal for all but the very smallest of system sizes.

Photogenerated carriers transport behaviors in L-cysteine capped ZnSe core-shell quantum dots

NASA Astrophysics Data System (ADS)

Shan, Qingsong; Li, Kuiying; Xue, Zhenjie; Lin, Yingying; Yin, Hua; Zhu, Ruiping

2016-02-01

The photoexcited carrier transport behavior of zinc selenide (ZnSe) quantum dots (QDs) with core-shell structure is studied because of their unique photoelectronic characteristics. The surface photovoltaic (SPV) properties of self-assembled ZnSe/ZnS/L-Cys core-shell QDs were probed via electric field induced surface photovoltage and transient photovoltage (TPV) measurements supplemented by Fourier transform infrared, laser Raman, absorption, and photoluminescence spectroscopies. The ZnSe QDs displayed p-type SPV characteristics with a broader stronger SPV response over the whole ultraviolet-to-near-infrared range compared with those of other core-shell QDs in the same group. The relationship between the SPV phase value of the QDs and external bias was revealed in their SPV phase spectrum. The wide transient photovoltage response region from 3.3 × 10-8 to 2 × 10-3 s was closely related to the long diffusion distance of photoexcited free charge carriers in the interfacial space-charge region of the QDs. The strong SPV response corresponding to the ZnSe core mainly originated from an obvious quantum tunneling effect in the QDs.

Ultrathin nanoporous membranes for insulator-based dielectrophoresis.

PubMed

Mukaibo, Hitomi; Wang, Tonghui; Perez-Gonzalez, Victor H; Getpreecharsawas, Jirachai; Wurzer, Jack; Lapizco-Encinas, Blanca H; McGrath, James L

2018-06-08

Insulator-based dielectrophoresis (iDEP) is a simple, scalable mechanism that can be used for directly manipulating particle trajectories in pore-based filtration and separation processes. However, iDEP manipulation of nanoparticles presents unique challenges as the dielectrophoretic force [Formula: see text] exerted on the nanoparticles can easily be overshadowed by opposing kinetic forces. In this study, a molecularly thin, SiN-based nanoporous membrane (NPN) is explored as a breakthrough technology that enhances [Formula: see text] By numerically assessing the gradient of the electric field square [Formula: see text]-a common measure for [Formula: see text] magnitude-it was found that the unique geometrical features of NPN (pore tapering, sharp pore corner and ultrathin thickness) act in favor of intensifying the overall [Formula: see text] A comparative study indicated that [Formula: see text] generated in NPN are four orders of magnitude larger than track-etched polycarbonate membranes with comparable pore size. The stronger [Formula: see text] suggests that iDEP can be conducted under lower voltage bias with NPN: reducing joule heating concerns and enabling solutions to have higher ionic strength. Enabling higher ionic strength solutions may also extend the opportunities of iDEP applications under physiologically relevant conditions. This study also highlights the effects of [Formula: see text] induced by the ion accumulation along charged surfaces (electric-double layer (EDL)). EDL-based [Formula: see text] exists along the entire charged surface, including locations where geometry-based iDEP is negligible. The high surface-to-volume ratio of NPN offers a unique platform for exploiting such EDL-based DEP systems. The EDL-based [Formula: see text] was also found to offset the geometry-based [Formula: see text] but this effect was easily circumvented by reducing the EDL thickness (e.g. increasing the ionic strength from 0.1 to 100 mM). The results from this study imply the potential application of iDEP as a direct, in-operando antifouling mechanism for ultrafiltration technology, and also as an active tuning mechanism to control the cut-off size limit for continuous selectivity of nanomembrane-based separations.

Using of Quantum Dots in Biology and Medicine.

PubMed

Pleskova, Svetlana; Mikheeva, Elza; Gornostaeva, Ekaterina

2018-01-01

Quantum dots are nanoparticles, which due to their unique physical and chemical (first of all optical) properties, are promising in biology and medicine. There are many ways for quantum dots synthesis, both in the form of nanoislands self-forming on the surfaces, which can be used as single-photon emitters in electronics for storing information, and in the form of colloidal quantum dots for diagnostic and therapeutic purposes in living systems. The paper describes the main methods of quantum dots synthesis and summarizes medical and biological ways of their use. The main emphasis is laid on the ways of quantum dots surface modification. Influence of the size and form of nanoparticles, charge on the surfaces of quantum dots, and cover type on the efficiency of internalization by cells and cell compartments is shown. The main mechanisms of penetration are considered.

Studies of Surface Charging of Polymers by Indirect Triboelectrification

NASA Astrophysics Data System (ADS)

Mantovani, James; Calle, Carlos; Groop, Ellen; Buehler, Martin

2001-03-01

Charge is known to develop on the surface of an insulating polymer by frictional charging through direct physical contact with another material. We will present results of recent triboelectrification studies of polymer surfaces that utilized an indirect method of frictional charging. This method first involves placing a grounded thin metal foil in stationary contact over the polymer surface. The exposed metal foil is then rubbed with the surface of the material that generates the triboelectric charge. Data is presented for five types of polymers: fiberglass/epoxy, polycarbonate (Lexan), polytetraflouroethylene (Teflon), Rulon J, and polymethylmethacrylate (PMMA, Lucite). The amount of charge that develops on an insulator's surface is measured using the MECA Electrometer, which was developed jointly by NASA Kennedy Space Center and the Jet Propulsion Laboratory to study the electrostatic properties of soil on the surface of Mars. Even though the insulator's surface is electrically shielded from the rubbing material by the grounded metal foil, charge measurements obtained by the MECA Electrometer after the metal foil is separated from the insulator's surface reveal that the insulator's surface does accumulate charge by indirect frictional charging. A possible explanation of the observations will be presented based on a simple contact barrier model.

Current-voltage characteristics influenced by the nanochannel diameter and surface charge density in a fluidic field-effect-transistor.

PubMed

Singh, Kunwar Pal; Guo, Chunlei

2017-06-21

The nanochannel diameter and surface charge density have a significant impact on current-voltage characteristics in a nanofluidic transistor. We have simulated the effect of the channel diameter and surface charge density on current-voltage characteristics of a fluidic nanochannel with positive surface charge on its walls and a gate electrode on its surface. Anion depletion/enrichment leads to a decrease/increase in ion current with gate potential. The ion current tends to increase linearly with gate potential for narrow channels at high surface charge densities and narrow channels are more effective to control the ion current at high surface charge densities. The current-voltage characteristics are highly nonlinear for wide channels at low surface charge densities and they show different regions of current change with gate potential. The ion current decreases with gate potential after attaining a peak value for wide channels at low values of surface charge densities. At low surface charge densities, the ion current can be controlled by a narrow range of gate potentials for wide channels. The current change with source drain voltage shows ohmic, limiting and overlimiting regions.

Effective Electrostatic Interactions Between Two Overall Neutral Surfaces with Quenched Charge Heterogeneity Over Atomic Length Scale

NASA Astrophysics Data System (ADS)

Zhou, S.

2017-12-01

Using Monte Carlo results as a reference, a classical density functional theory ( CDFT) is shown to reliably predict the forces between two heterogeneously charged surfaces immersed in an electrolyte solution, whereas the Poisson-Boltzmann ( PB) theory is demonstrated to deteriorate obviously for the same system even if the system parameters considered fall within the validity range of the PB theory in the homogeneously charged surfaces. By applying the tested CDFT, we study the effective electrostatic potential of mean force ( EPMF) between two face-face planar and hard surfaces of zero net charge on which positive and negative charges are separated and considered to present as discontinuous spots on the inside edges of the two surfaces. Main conclusions are summarized as follows: (i) strength of the EPMF in the surface charge separation case is very sensitively and positively correlated with the surface charge separation level and valency of the salt ion. Particularly, the charge separation level and the salt ion valency have a synergistic effect, which makes high limit of the EPMF strength in the surface charge separation case significantly go beyond that of the ideal homogeneously charged surface counterpart at average surface charge density similar to the average surface positive or negative charge density in the charge separation case. (ii) The surface charge distribution patterns mainly influence sign of the EPMF: symmetrical and asymmetrical patterns induce repulsive and attractive (at small distances) EPMF, respectively; but with low valency salt ions and low charge separation level the opposite may be the case. With simultaneous presence of both higher valency cation and anion, the EPMF can be repulsive at intermediate distances for asymmetrical patterns. (iii) Salt ion size has a significant impact, which makes the EPMF tend to become more and more repulsive with the ion diameter regardless of the surface charge distribution patterns and the valency of the salt ion; whereas if the 1:1 type electrolyte and the symmetrical patterns are considered, then the opposite may be the case. All of these findings can be explained self-consistently from several perspectives: an excess adsorption of the salt ions (induced by the surface charge separation) serving to raise the osmotic pressure between the plates, configuration fine-tuning in the thinner ion adsorption layer driven by the energy decrease principle, direct Coulombic interactions operating between charged objects on the two face-to-face plates involved, and net charge strength in the ion adsorption layer responsible for the net electrostatic repulsion.

Rectification of nanopores at surfaces

PubMed Central

Sa, Niya

2011-01-01

At the nanoscale, methods to measure surface charge can prove challenging. Herein we describe a general method to report surface charge through the measurement of ion current rectification of a nanopipette brought in close proximity to a charged substrate. This method is able to discriminate between charged cationic and anionic substrates when the nanopipette is brought within distances from ten to hundreds of nanometers from the surface. Further studies of the pH dependence on the observed rectification support a surface-induced mechanism and demonstrate the ability to further discriminate between cationic and nominally uncharged surfaces. This method could find application in measurement and mapping of heterogeneous surface charges and is particularly attractive for future biological measurements, where noninvasive, noncontact probing of surface charge will prove valuable. PMID:21675734

Production of thick uniform-coating films containing rectorite on nanofibers through the use of an automated coating machine.

PubMed

Wu, Yang; Li, Xueyong; Shi, Xiaowen; Zhan, Yingfei; Tu, Hu; Du, Yumin; Deng, Hongbing; Jiang, Linbin

2017-01-01

When an efficient automated coating machine is used to process layer-by-layer (LBL) deposited nanofibrous mats, it causes an obvious planar effect on the surface of the mats, which can be eliminated through ultimate immersion. During this process, chitosan (CS) - rectorite (REC) intercalated composite films are built on the surface of cellulose acetate (CA) nanofibrous mats by a coating machine. Then, the immersion process is utilized to allow positively charged CS or CS-REC intercalated composites to uniformly assemble on the surface of negatively charged CA nanofibers. An investigation into the morphology of the resultant scaffolds confirms that the uniquely small pore size, high specific surface area and typically three-dimensional (3D) structure of nanofibrous mats remain present. The results of Fourier transform infrared (FT-IR) and X-ray photoelectron spectroscopy (XPS) indicate that it is feasible to assemble nanofibrous mats using a coating machine. The intercalated structure of CS-REC is confirmed by the results of small-angle X-ray diffraction (SAXRD) and wide-angle X-ray diffraction (WAXRD). The results of the cell experiment and antibacterial test demonstrate that the addition of REC not only has little impact on the cytocompatibility of the mats but also enhances their ability to inhibit bacteria. Copyright © 2016 Elsevier B.V. All rights reserved.

The electrokinetic behavior of calcium oxalate monohydrate in macromolecular solutions

NASA Technical Reports Server (NTRS)

Curreri, P. A.; Onoda, G. Y., Jr.; Finlayson, B.

1988-01-01

Electrophoretic mobilities were measured for calcium oxalate monohydrate (COM) in solutions containing macromolecules. Two mucopolysaccharides (sodium heparin and chrondroitin sulfate) and two proteins (positively charged lysozyme and negatively charged bovine serum albumin) were studied as adsorbates. The effects of pH, calcium oxalate surface charge (varied by calcium or oxalate ion activity), and citrate concentration were investigated. All four macromolecules showed evidence for chemical adsorption. The macromolecule concentrations needed for reversing the surface charge indicated that the mucopopolysacchrides have greater affinity for the COM surface than the proteins. The amount of proteins that can chemically adsorb appears to be limited to approximately one monomolecular layer. When the surface charge is high, an insufficient number of proteins can chemically adsorb to neutralize or reverse the surface charge. The remaining surface charge is balanced by proteins held near the surface by longer range electrostatic forces only. Citrate ions at high concentrations appear to compete effectively with the negative protein for surface sites but show no evidence for competing with the positively charged protein.

14 CFR 1215.113 - User charges.

Code of Federal Regulations, 2013 CFR

2013-01-01

... 14 Aeronautics and Space 5 2013-01-01 2013-01-01 false User charges. 1215.113 Section 1215.113 Aeronautics and Space NATIONAL AERONAUTICS AND SPACE ADMINISTRATION TRACKING AND DATA RELAY SATELLITE SYSTEM... shall reimburse NASA the sum of the charges for standard and mission-unique services. Charges will be...

Protein adsorption at charged surfaces: the role of electrostatic interactions and interfacial charge regulation.

PubMed

Hartvig, Rune A; van de Weert, Marco; Østergaard, Jesper; Jorgensen, Lene; Jensen, Henrik

2011-03-15

The understanding of protein adsorption at charged surfaces is important for a wide range of scientific disciplines including surface engineering, separation sciences and pharmaceutical sciences. Compared to chemical entities having a permanent charge, the adsorption of small ampholytes and proteins is more complicated as the pH near a charged surface can be significantly different from the value in bulk solution. In this work, we have developed a phenomenological adsorption model which takes into account the combined role of interfacial ion distribution, interfacial charge regulation of amino acids in the proximity of the surface, electroneutrality, and mass balance. The model is straightforward to apply to a given set of experimental conditions as most model parameters are obtained from bulk properties and therefore easy to estimate or are directly measurable. The model provides a detailed understanding of the importance of surface charge on adsorption and in particular of how changes in surface charge, concentration, and surface area may affect adsorption behavior. The model is successfully used to explain the experimental adsorption behavior of the two model proteins lysozyme and α-lactalbumin. It is demonstrated that it is possible to predict the pH and surface charge dependent adsorption behavior from experimental or theoretical estimates of a preferred orientation of a protein at a solid charged interface.

The Charging Events in Contact-Separation Electrification.

PubMed

Musa, Umar G; Cezan, S Doruk; Baytekin, Bilge; Baytekin, H Tarik

2018-02-06

Contact electrification (CE)-charging of surfaces that are contacted and separated, is a common phenomenon, however it is not completely understood yet. Recent studies using surface imaging techniques and chemical analysis revealed a 'spatial' bipolar distribution of charges at the nano dimension, which made a paradigm shift in the field. However, such analyses can only provide information about the charges that remained on the surface after the separation, providing limited information about the actual course of the CE event. Tapping common polymers and metal surfaces to each other and detecting the electrical potential produced on these surfaces 'in-situ' in individual events of contact and separation, we show that, charges are generated and transferred between the surfaces in both events; the measured potential is bipolar in contact and unipolar in separation. We show, the 'contact-charges' on the surfaces are indeed the net charges that results after the separation process, and a large contribution to tribocharge harvesting comes, in fact, from the electrostatic induction resulting from the generated CE charges. Our results refine the mechanism of CE providing information for rethinking the conventional ranking of materials' charging abilities, charge harvesting, and charge prevention.

Charged particle detectors with active detector surface for partial energy deposition of the charged particles and related methods

DOEpatents

Gerts, David W; Bean, Robert S; Metcalf, Richard R

2013-02-19

A radiation detector is disclosed. The radiation detector comprises an active detector surface configured to generate charge carriers in response to charged particles associated with incident radiation. The active detector surface is further configured with a sufficient thickness for a partial energy deposition of the charged particles to occur and permit the charged particles to pass through the active detector surface. The radiation detector further comprises a plurality of voltage leads coupled to the active detector surface. The plurality of voltage leads is configured to couple to a voltage source to generate a voltage drop across the active detector surface and to separate the charge carriers into a plurality of electrons and holes for detection. The active detector surface may comprise one or more graphene layers. Timing data between active detector surfaces may be used to determine energy of the incident radiation. Other apparatuses and methods are disclosed herein.

Adsorption of a cationic dye molecule on polystyrene microspheres in colloids: effect of surface charge and composition probed by second harmonic generation.

PubMed

Eckenrode, Heather M; Jen, Shih-Hui; Han, Jun; Yeh, An-Gong; Dai, Hai-Lung

2005-03-17

Nonlinear optical probe, second harmonic generation (SHG), of the adsorption of the dye molecule malachite green (MG), in cationic form at pH < or = 5, on polystyrene microspheres in aqueous solution is used to study the effect of surface charge and composition on molecular adsorption. Three types of polystyrene microspheres with different surface composition are investigated: (1) a sulfate terminated, anionic surface, (2) a neutral surface without any functional group termination, and (3) an amine terminated, cationic surface. The cationic dye was found to adsorb at all three surfaces, regardless of surface charge. The adsorption free energies, DeltaG's, measured for the three surfaces are -12.67, -12.39, and -10.46 kcal/mol, respectively, with the trend as expected from the charge interactions. The adsorption density on the anionic surface, where attractive charge-charge interaction dominates, is determined by the surface negative charge density. The adsorption densities on the neutral and cationic surfaces are on the other hand higher, perhaps as a result of a balance between minimizing repulsive charge interaction and maximizing attractive molecule-substrate and intermolecular interactions. The relative strength of the SH intensity per molecule, in combination of a model calculation, reveals that the C(2) axis of the MG molecule is nearly perpendicular to the surface on the anionic surface and tilts away from the surface norm when the surface is neutral and further away when cationic. Changing the pH of the solution may alter the surface charge and subsequently affect the adsorption configuration and SH intensity.

Electronic Disorder in Organic Semiconducting Films Observed with Kelvin Probe Force Microscopy

NASA Astrophysics Data System (ADS)

Hoffman, Benjamin Carl

This work is a study into electronic disorder within organic semiconducting (OSC) films from a scan-probe perspective. Organic electronics are an exciting technology poised for use in next generation devices with unique applications such as transparent displays and ultrathin flexible solar cells. Understanding and mapping electronic disorder in OSC has a high degree of relevance towards recognizing the properties of charge trapping that hinders transport and diminishes device performance. Evidence of surface potential inhomogeneity is identified by using Kelvin probe force microscopy (KPFM) to measure the contact potential difference (CPD) between probe and sample. OSC films are grown via organic molecular beam deposition (OMBD) to create well-ordered crystals with precise control of nominal thickness. Further research methods involve the study of diffraction peaks from grazing-incidence wide-angle x-ray scattering (GIWAXS) for crystallographic analysis as well as use of a probe station for transfer characteristics of fabricated thin film transistors. Initial research into this subject involved thin films of the novel organic molecule 2,8- diflouro-5,11-bis(triethylsilylethynyl)-anthradithiophene (diF-TES-ADT) that were grown on silicon substrates with a native oxide layer and analyzed with GIWAXS and KPFM. The crystallography of the films is that of a uniform (001) orientation. Variations in surface potential in diF-TES-ADT crystallites are observed to be unique from variations in the substrate. Nevertheless, surface potential variations in thick films are influenced by chemical passivation of the substrate and so the source of CPD variations are assigned to be intrinsic defects. Chemical treatment and processing methods control the growth kinetics which are linked to charge traps locally distorting the surface potential in OSC films. To continue the research into identifying charge trapping in ultra-thin films, 1.5 monolayer thick films of alpha-sexithiophene (6T) were grown on silicon substrates with a thick oxide layer to compare the surface potential of the first monolayer with that of the bilayer. The temperature of the substrate during film growth was varied and found to influence the interlayer surface potential contrast. Higher temperature samples have a bilayer with CPD above that of the monolayer, while lower temperature samples have a bilayer with CPD below that of the monolayer. GIWAXS data collected shows that the lower temperature sample has no observed out-of-plane order which we identify as the source of interlayer trapping formed between the first and second monolayers of the 6T films. The final project into the specifics of disorder involves using ultrathin films of 6T in an operational transistor with grounded source-drain electrodes to study the influence of gate bias on surface potential. Using the mean and standard deviation of CPD for a series of gate biases, the trap density of states (DOS) is calculated directly while allowing for the quantification of spatial variations. CPD histograms from the series of images illustrate the screening of deep traps as the transistor is turned on. While in the 'off' regime the images are electrostatic, after transitioning to the 'on' state the images show instability after threshold voltage. This dynamic 'on' state offers a unique view of shallow trap states being filled and then thermally released.

NASA charging analyzer program: A computer tool that can evaluate electrostatic contamination

NASA Technical Reports Server (NTRS)

Stevens, N. J.; Roche, J. C.; Mandell, M. J.

1978-01-01

A computer code, the NASA Charging Analyzer Program (NASCAP), was developed to study the surface charging of bodies subjected to geomagnetic substorm conditions. This program will treat the material properties of a surface in a self-consistent manner and calculate the electric fields in space due to the surface charge. Trajectories of charged particles in this electric field can be computed to determine if these particles enhance surface contamination. A preliminary model of the Spacecraft Charging At The High Altitudes (SCATHA) satellite was developed in the NASCAP code and subjected to a geomagnetic substorm environment to investigate the possibility of electrostatic contamination. The results indicate that differential voltages will exist between the spacecraft ground surfaces and the insulator surfaces. The electric fields from this differential charging can enhance the contamination of spacecraft surfaces.

Adhesion of osteoblasts to a nanorough titanium implant surface

PubMed Central

Gongadze, Ekaterina; Kabaso, Doron; Bauer, Sebastian; Slivnik, Tomaž; Schmuki, Patrik; van Rienen, Ursula; Iglič, Aleš

2011-01-01

This work considers the adhesion of cells to a nanorough titanium implant surface with sharp edges. The basic assumption was that the attraction between the negatively charged titanium surface and a negatively charged osteoblast is mediated by charged proteins with a distinctive quadrupolar internal charge distribution. Similarly, cation-mediated attraction between fibronectin molecules and the titanium surface is expected to be more efficient for a high surface charge density, resulting in facilitated integrin mediated osteoblast adhesion. We suggest that osteoblasts are most strongly bound along the sharp convex edges or spikes of nanorough titanium surfaces where the magnitude of the negative surface charge density is the highest. It is therefore plausible that nanorough regions of titanium surfaces with sharp edges and spikes promote the adhesion of osteoblasts. PMID:21931478

Structure-function analysis of rotavirus NSP2 octamer by using a novel complementation system.

PubMed

Taraporewala, Zenobia F; Jiang, Xiaofang; Vasquez-Del Carpio, Rodrigo; Jayaram, Hariharan; Prasad, B V Venkataram; Patton, John T

2006-08-01

Viral inclusion bodies, or viroplasms, that form in rotavirus-infected cells direct replication and packaging of the segmented double-stranded RNA (dsRNA) genome. NSP2, one of two rotavirus proteins needed for viroplasm assembly, possesses NTPase, RNA-binding, and helix-unwinding activities. NSP2 of the rotavirus group causing endemic infantile diarrhea (group A) was shown to self-assemble into large doughnut-shaped octamers with circumferential grooves and deep clefts containing nucleotide-binding histidine triad (HIT)-like motifs. Here, we demonstrate that NSP2 of group C rotavirus, a group that fails to reassort with group A viruses, retains the unique architecture of the group A octamer but differs in surface charge distribution. By using an NSP2-dependent complementation system, we show that the HIT-dependent NTPase activity of NSP2 is necessary for dsRNA synthesis, but not for viroplasm formation. The complementation system also showed that despite the retention of the octamer structure and the HIT-like fold, group C NSP2 failed to rescue replication and viroplasm formation in NSP2-deficient cells infected with group A rotavirus. The distinct differences in the surface charges on the Bristol and SA11 NSP2 octamers suggest that charge complementarity of the viroplasm-forming proteins guides the specificity of viroplasm formation and, possibly, reassortment restriction between rotavirus groups.

Effects of image charges, interfacial charge discreteness, and surface roughness on the zeta potential of spherical electric double layers.

PubMed

Gan, Zecheng; Xing, Xiangjun; Xu, Zhenli

2012-07-21

We investigate the effects of image charges, interfacial charge discreteness, and surface roughness on spherical electric double layer structures in electrolyte solutions with divalent counterions in the setting of the primitive model. By using Monte Carlo simulations and the image charge method, the zeta potential profile and the integrated charge distribution function are computed for varying surface charge strengths and salt concentrations. Systematic comparisons were carried out between three distinct models for interfacial charges: (1) SURF1 with uniform surface charges, (2) SURF2 with discrete point charges on the interface, and (3) SURF3 with discrete interfacial charges and finite excluded volume. By comparing the integrated charge distribution function and the zeta potential profile, we argue that the potential at the distance of one ion diameter from the macroion surface is a suitable location to define the zeta potential. In SURF2 model, we find that image charge effects strongly enhance charge inversion for monovalent interfacial charges, and strongly suppress charge inversion for multivalent interfacial charges. For SURF3, the image charge effect becomes much smaller. Finally, with image charges in action, we find that excluded volumes (in SURF3) suppress charge inversion for monovalent interfacial charges and enhance charge inversion for multivalent interfacial charges. Overall, our results demonstrate that all these aspects, i.e., image charges, interfacial charge discreteness, their excluding volumes, have significant impacts on zeta potentials of electric double layers.

On the physics of both surface overcharging and charge reversal at heterophase interfaces.

PubMed

Wang, Zhi-Yong; Zhang, Pengli; Ma, Zengwei

2018-02-07

The conventional paradigm for characterizing surface overcharging and charge reversal is based on the so-called Stern layer, in which surface dissociation reaction and specific chemical adsorption are assumed to take place. In this article, a series of Monte Carlo simulations have been applied to obtain useful insights into the underlying physics responsible for these two kinds of anomalous phenomena at the interface of two dielectrics, with special emphasis on the case of divalent counterions that are more relevant in natural and biological environments. At a weakly charged surface, it is found that independent of the type of surface charge distribution and the dielectric response of the solution, the overcharging event is universally driven by the ion size-asymmetric effect. Exceptionally, the overcharging still persists when the surface is highly charged but is only restricted to the case of discrete surface charge in a relatively low dielectric medium. As compared to the adsorption onto the homogeneously smeared charge surface that has the same average affinity for counterions, on the other hand, charge reversal under the action of a dielectric response can be substantially enhanced in the discrete surface charge representation due to strong association of counterions with interfacial groups, and the degree of enhancement depends in a nontrivial way on the reduction of the medium dielectric constant and the steric effects of finite ion size. Rather interestingly, the charge reversal is of high relevance to the overcharging of interfaces because the overwhelming interfacial association forces the coions closer to the surface due to their smaller size than the counterions. Upon the addition of a monovalent salt to the solution, the interfacial association with divalent counterions makes surface overcharging and charge reversal widely unaffected, in contrast to the prevailing notion that screening of surface charge of a homogeneous nature is determined by the competitive effects between size-exclusion effects and energetic contributions. Overall, the present work highlights that the complex interplay between the electrostatic and steric interactions should be coupled to the realistic character of surface charge to establish a faithful description of the overcharging and charge reversal at heterophase interfaces.

Montmorillonite-lipid hybrid carriers for ionizable and neutral poorly water-soluble drugs: Formulation, characterization and in vitro lipolysis studies.

PubMed

Dening, Tahnee J; Rao, Shasha; Thomas, Nicky; Prestidge, Clive A

2017-06-30

Lipid-based formulations (LBFs) are a popular strategy for enhancing the gastrointestinal solubilization and absorption of poorly water-soluble drugs. In light of this, montmorillonite-lipid hybrid (MLH) particles, composed of medium-chain triglycerides, lecithin and montmorillonite clay platelets, have been developed as a novel solid-state LBF. Owing to the unique charge properties of montmorillonite, whereby the clay platelet surfaces carry a permanent negative charge and the platelet edges carry a pH-dependent charge, three model poorly water-soluble drugs with different charge properties; blonanserin (weak base, pKa 7.7), ibuprofen (weak acid, pKa 4.5) and fenofibrate (neutral), were formulated as MLH particles and their performance during biorelevant in vitro lipolysis at pH 7.5 was investigated. For blonanserin, drug solubilization during in vitro lipolysis was significantly reduced 3.4-fold and 3.2-fold for MLH particles in comparison to a control lipid solution and silica-lipid hybrid (SLH) particles, respectively. It was hypothesized that strong electrostatic interactions between the anionic montmorillonite platelet surfaces and cationic blonanserin molecules were responsible for the inferior performance of MLH particles. In contrast, no significant influence on drug solubilization was observed for ibuprofen- and fenofibrate-loaded MLH particles. The results of the current study indicate that whilst MLH particles are a promising novel formulation strategy for poorly water-soluble drugs, drug ionization tendency and the potential for drug-clay interactions must be taken into consideration to ensure an appropriate performance. Copyright © 2017 Elsevier B.V. All rights reserved.

A method for unique identification of relativistic /greater than 0.5/ magnetic monopoles with a fast film Cerenkov detector

NASA Technical Reports Server (NTRS)

Pinsky, L. S.; Hagstrom, R.

1975-01-01

A magnetic monopole traversing a dielectric medium at a velocity greater than the phase velocity of light in that medium, will give rise to Cerenkov radiation with the electric field tangent to the cone generated by the photon wave propagation vector, and the magnetic field normal to that surface. This is the opposite polarization to that encountered with an electric charge. It is proposed that either by inserting a linearly polarizing layer between the radiator and the photographic emulsion, or by selecting a linearly polarizing material as the radiator, one could directly observe the field polarization by examining the photographic image and thus uniquely identify a magnetic monopole. The ability of the detector is further enhanced by the index of refraction dependence of the Cerenkov output from a magnetic monopole.

Nanopipette delivery: influence of surface charge.

PubMed

Shi, Wenqing; Sa, Niya; Thakar, Rahul; Baker, Lane A

2015-07-21

In this report, transport through a nanopipette is studied and the interplay between current rectification and ion delivery for small pipettes is examined. First, surface charge dependence of concentration polarization effects in a quartz nanopipette was investigated. Electrical characterization was performed through current-potential (I-V) measurements. In addition, fluorescein (an anionic fluorescent probe) was utilized to optically map ion enrichment and ion depletion in the nanopipette tip. Bare nanopipettes and polyethylenimine (PEI)-modified nanopipettes were examined. Results confirm that concentration polarization is a surface charge dependent phenomenon and delivery can be controlled through modification of surface charge. The relationship between concentration polarization effects and voltage-driven delivery of charged electroactive species was investigated with a carbon ring/nanopore electrode fabricated from pyrolyzed parylene C (PPC). Factors such as surface charge polarity of the nanopipette, electrolyte pH, and electrolyte concentration were investigated. Results indicate that with modification of surface charge, additional control over delivery of charged species can be achieved.

Mutual promotion of electrochemical-localized surface plasmon resonance on nanochip for sensitive sialic acid detection.

PubMed

Li, Shuang; Liu, Jinglong; Lu, Yanli; Zhu, Long; Li, Candong; Hu, Lijiang; Li, Jun; Jiang, Jing; Low, Szeshin; Liu, Qingjun

2018-06-01

Localized surface plasmon resonance (LSPR) induced charge separation were concentrated on the metal nanoparticles surface, which made it sensitive to the surface refractive index changes during optical sensing. Similarly, electrochemical detection was based on the electron transformation on the electrode surface. Herein, we fabricated a nanochip by decorating a nanocone-array substrate with gold nanoparticles and silver nanoparticles for dynamic electro-optical spectroscopy. Mercaptophenyl boronic acid (MPBA) was immobilized firmly on the nanochip by the metal-S bond for sensitive sialic acid sensing. Owing to the high stability of gold nanoparticles and the high sensitivity of silver nanoparticles, the nanochip showed good performance in LSPR detection with rich and high responses. Besides, the nanochip also showed sensitive electrical signals during electrochemical detection due to the excitation of the energetic charges from the nanoparticles surface to the reaction system. The dynamic electro-optical spectroscopy was based on a unique combination of LSPR and linear sweep voltammetry (LSV). On the one hand, electrochemical signals activated the electrons on the nanochip to promote the propagation and resonance of surface plasmon. On the other hand, LSPR concentrated the electrons on the nanochip surface, which made the electrons easily driven to enhance the current in electrochemical detection. Results showed that mutual promotion of electrochemical-LSPR on nanochip covered a linear dynamic range from 0.05 mM to 5 mM on selective sialic acid detection with a low detection limit of 17 μM. The synchronous amplification of the electro-optical response during electrochemical-LSPR, opened up a new perspective for efficient and sensitive biochemical detection. Copyright © 2018 Elsevier B.V. All rights reserved.

Polarization-induced surface charges in hydroxyapatite ceramics

NASA Astrophysics Data System (ADS)

Horiuchi, N.; Nakaguki, S.; Wada, N.; Nozaki, K.; Nakamura, M.; Nagai, A.; Katayama, K.; Yamashita, K.

2014-07-01

Calcium hydroxyapatite (HAp; Ca10(PO4)6(OH)2) is a well-known biomaterial that is the main inorganic component of bones and teeth. Control over the surface charge on HAp would be a key advance in the development of the material for tissue engineering. We demonstrate here that surface charge can be induced by an electrical poling process using the Kelvin method. Positive and negative charges were induced on the HAp surface in response to the applied electric field in the poling process. The surface charging is attributed to dipole polarization that is homogeneously distributed in HAp. Additionally, the surface charging is considered to originate from the organization of OH- ions into a polar phase in the structure.

Poisson-Boltzmann theory of the charge-induced adsorption of semi-flexible polyelectrolytes.

PubMed

Ubbink, Job; Khokhlov, Alexei R

2004-03-15

A model is suggested for the structure of an adsorbed layer of a highly charged semi-flexible polyelectrolyte on a weakly charged surface of opposite charge sign. The adsorbed phase is thin, owing to the effective reversal of the charge sign of the surface upon adsorption, and ordered, owing to the high surface density of polyelectrolyte strands caused by the generally strong binding between polyelectrolyte and surface. The Poisson-Boltzmann equation for the electrostatic interaction between the array of adsorbed polyelectrolytes and the charged surface is solved for a cylindrical geometry, both numerically, using a finite element method, and analytically within the weak curvature limit under the assumption of excess monovalent salt. For small separations, repulsive surface polarization and counterion osmotic pressure effects dominate over the electrostatic attraction and the resulting electrostatic interaction curve shows a minimum at nonzero separations on the Angstrom scale. The equilibrium density of the adsorbed phase is obtained by minimizing the total free energy under the condition of equality of chemical potential and osmotic pressure of the polyelectrolyte in solution and in the adsorbed phase. For a wide range of ionic conditions and charge densities of the charged surface, the interstrand separation as predicted by the Poisson-Boltzmann model and the analytical theory closely agree. For low to moderate charge densities of the adsorbing surface, the interstrand spacing decreases as a function of the charge density of the charged surface. Above about 0.1 M excess monovalent salt, it is only weakly dependent on the ionic strength. At high charge densities of the adsorbing surface, the interstrand spacing increases with increasing ionic strength, in line with the experiments by Fang and Yang [J. Phys. Chem. B 101, 441 (1997)]. (c) 2004 American Institute of Physics.

Method for Estimating the Charge Density Distribution on a Dielectric Surface.

PubMed

Nakashima, Takuya; Suhara, Hiroyuki; Murata, Hidekazu; Shimoyama, Hiroshi

2017-06-01

High-quality color output from digital photocopiers and laser printers is in strong demand, motivating attempts to achieve fine dot reproducibility and stability. The resolution of a digital photocopier depends on the charge density distribution on the organic photoconductor surface; however, directly measuring the charge density distribution is impossible. In this study, we propose a new electron optical instrument that can rapidly measure the electrostatic latent image on an organic photoconductor surface, which is a dielectric surface, as well as a novel method to quantitatively estimate the charge density distribution on a dielectric surface by combining experimental data obtained from the apparatus via a computer simulation. In the computer simulation, an improved three-dimensional boundary charge density method (BCM) is used for electric field analysis in the vicinity of the dielectric material with a charge density distribution. This method enables us to estimate the profile and quantity of the charge density distribution on a dielectric surface with a resolution of the order of microns. Furthermore, the surface potential on the dielectric surface can be immediately calculated using the obtained charge density. This method enables the relation between the charge pattern on the organic photoconductor surface and toner particle behavior to be studied; an understanding regarding the same may lead to the development of a new generation of higher resolution photocopiers.

Lunar Surface Charging during Solar Energetic Particle Events

NASA Astrophysics Data System (ADS)

Halekas, Jasper S.; Delory, G. T.; Mewaldt, R. A.; Lin, R. P.; Fillingim, M. O.; Brain, D. A.; Lee, C. O.; Stubbs, T. J.; Farrell, W. M.; Hudson, M. K.

2006-09-01

The surface of the Moon, not protected by any substantial atmosphere, is directly exposed to the impact of both solar UV and solar wind plasma and energetic particles. This creates a complex lunar electrostatic environment, with the surface typically charging slightly positive in sunlight, and negative in shadow. Observations from the Apollo era and theoretical considerations strongly suggest that surface charging leads to dust electrification and transport, posing a potentially significant hazard for exploration. The most significant charging effects should occur when the Moon is exposed to high-temperature plasmas like those encountered in the terrestrial plasmasheet or in solar storms. We now present evidence for kilovolt-scale negative charging of the shadowed lunar surface during solar energetic particle (SEP) events, utilizing data from the Lunar Prospector Electron Reflectometer (LP ER). We find that SEP events are associated with the most extreme lunar surface charging observed during the LP mission - rivaled only by previously reported charging during traversals of the terrestrial plasmasheet. The largest charging event observed by LP is a 4 kV negative surface potential (as compared to typical values of V) during a SEP event in May 1998. We characterize lunar surface charging during several SEP events, and compare to energetic particle measurements from ACE, Wind, and SOHO in order to determine the relationship between SEP events and extreme lunar surface charging. Space weather events are already considered by NASA to be a significant hazard to lunar exploration, due to high-energy ionizing radiation. Our observations demonstrate that plasma interactions with the lunar surface during SEP events, causing extreme surface charging and potentially significant dust electrification and transport, represent an additional hazard associated with space weather.

Potentiometric Titrations for Measuring the Capacitance of Colloidal Photodoped ZnO Nanocrystals.

PubMed

Brozek, Carl K; Hartstein, Kimberly H; Gamelin, Daniel R

2016-08-24

Colloidal semiconductor nanocrystals offer a unique opportunity to bridge molecular and bulk semiconductor redox phenomena. Here, potentiometric titration is demonstrated as a method for quantifying the Fermi levels and charging potentials of free-standing colloidal n-type ZnO nanocrystals possessing between 0 and 20 conduction-band electrons per nanocrystal, corresponding to carrier densities between 0 and 1.2 × 10(20) cm(-3). Potentiometric titration of colloidal semiconductor nanocrystals has not been described previously, and little precedent exists for analogous potentiometric titration of any soluble reductants involving so many electrons. Linear changes in Fermi level vs charge-carrier density are observed for each ensemble of nanocrystals, with slopes that depend on the nanocrystal size. Analysis indicates that the ensemble nanocrystal capacitance is governed by classical surface electrical double layers, showing no evidence of quantum contributions. Systematic shifts in the Fermi level are also observed with specific changes in the identity of the charge-compensating countercation. As a simple and contactless alternative to more common thin-film-based voltammetric techniques, potentiometric titration offers a powerful new approach for quantifying the redox properties of colloidal semiconductor nanocrystals.

Charge-Spot Model for Electrostatic Forces in Simulation of Fine Particulates

NASA Technical Reports Server (NTRS)

Walton, Otis R.; Johnson, Scott M.

2010-01-01

The charge-spot technique for modeling the static electric forces acting between charged fine particles entails treating electric charges on individual particles as small sets of discrete point charges, located near their surfaces. This is in contrast to existing models, which assume a single charge per particle. The charge-spot technique more accurately describes the forces, torques, and moments that act on triboelectrically charged particles, especially image-charge forces acting near conducting surfaces. The discrete element method (DEM) simulation uses a truncation range to limit the number of near-neighbor charge spots via a shifted and truncated potential Coulomb interaction. The model can be readily adapted to account for induced dipoles in uncharged particles (and thus dielectrophoretic forces) by allowing two charge spots of opposite signs to be created in response to an external electric field. To account for virtual overlap during contacts, the model can be set to automatically scale down the effective charge in proportion to the amount of virtual overlap of the charge spots. This can be accomplished by mimicking the behavior of two real overlapping spherical charge clouds, or with other approximate forms. The charge-spot method much more closely resembles real non-uniform surface charge distributions that result from tribocharging than simpler approaches, which just assign a single total charge to a particle. With the charge-spot model, a single particle may have a zero net charge, but still have both positive and negative charge spots, which could produce substantial forces on the particle when it is close to other charges, when it is in an external electric field, or when near a conducting surface. Since the charge-spot model can contain any number of charges per particle, can be used with only one or two charge spots per particle for simulating charging from solar wind bombardment, or with several charge spots for simulating triboelectric charging. Adhesive image-charge forces acting on charged particles touching conducting surfaces can be up to 50 times stronger if the charge is located in discrete spots on the particle surface instead of being distributed uniformly over the surface of the particle, as is assumed by most other models. Besides being useful in modeling particulates in space and distant objects, this modeling technique is useful for electrophotography (used in copiers) and in simulating the effects of static charge in the pulmonary delivery of fine dry powders.

Atomistic and molecular effects in electric double layers at high surface charges

DOE PAGES

Templeton, Jeremy Alan; Lee, Jonathan; Mani, Ali

2015-06-16

Here, the Poisson–Boltzmann theory for electrolytes near a charged surface is known to be invalid due to unaccounted physics associated with high ion concentration regimes. In order to investigate this regime, fluids density functional theory (f-DFT) and molecular dynamics (MD) simulations were used to determine electric surface potential as a function of surface charge. Based on these detailed computations, for electrolytes with nonpolar solvent, the surface potential is shown to depend quadratically on the surface charge in the high charge limit. We demonstrate that modified Poisson–Boltzmann theories can model this limit if they are augmented with atomic packing densities providedmore » by MD. However, when the solvent is a highly polar molecule water an intermediate regime is identified in which a constant capacitance is realized. Simulation results demonstrate the mechanism underlying this regime, and for the salt water system studied here, it persists throughout the range of physically realistic surface charge densities so the potential’s quadratic surface charge dependence is not obtained.« less

Surface charge mapping with a nanopipette.

PubMed

McKelvey, Kim; Kinnear, Sophie L; Perry, David; Momotenko, Dmitry; Unwin, Patrick R

2014-10-01

Nanopipettes are emerging as simple but powerful tools for probing chemistry at the nanoscale. In this contribution the use of nanopipettes for simultaneous surface charge mapping and topographical imaging is demonstrated, using a scanning ion conductance microscopy (SICM) format. When a nanopipette is positioned close to a surface in electrolyte solution, the direct ion current (DC), driven by an applied bias between a quasi-reference counter electrode (QRCE) in the nanopipette and a second QRCE in the bulk solution, is sensitive to surface charge. The charge sensitivity arises because the diffuse double layers at the nanopipette and the surface interact, creating a perm-selective region which becomes increasingly significant at low ionic strengths (10 mM 1:1 aqueous electrolyte herein). This leads to a polarity-dependent ion current and surface-induced rectification as the bias is varied. Using distance-modulated SICM, which induces an alternating ion current component (AC) by periodically modulating the distance between the nanopipette and the surface, the effect of surface charge on the DC and AC is explored and rationalized. The impact of surface charge on the AC phase (with respect to the driving sinusoidal signal) is highlighted in particular; this quantity shows a shift that is highly sensitive to interfacial charge and provides the basis for visualizing charge simultaneously with topography. The studies herein highlight the use of nanopipettes for functional imaging with applications from cell biology to materials characterization where understanding surface charge is of key importance. They also provide a framework for the design of SICM experiments, which may be convoluted by topographical and surface charge effects, especially for small nanopipettes.

In Situ Synthesis of Vertical Standing Nanosized NiO Encapsulated in Graphene as Electrodes for High-Performance Supercapacitors.

PubMed

Lin, Jinghuang; Jia, Henan; Liang, Haoyan; Chen, Shulin; Cai, Yifei; Qi, Junlei; Qu, Chaoqun; Cao, Jian; Fei, Weidong; Feng, Jicai

2018-03-01

NiO is a promising electrode material for supercapacitors. Herein, the novel vertically standing nanosized NiO encapsulated in graphene layers (G@NiO) are rationally designed and synthesized as nanosheet arrays. This unique vertical standing structure of G@NiO nanosheet arrays can enlarge the accessible surface area with electrolytes, and has the benefits of short ion diffusion path and good charge transport. Further, an interconnected graphene conductive network acts as binder to encapsulate the nanosized NiO particles as core-shell structure, which can promote the charge transport and maintain the structural stability. Consequently, the optimized G@NiO hybrid electrodes exhibit a remarkably enhanced specific capacity up to 1073 C g -1 and excellent cycling stability. This study provides a facial strategy to design and construct high-performance metal oxides for energy storage.

Super-Resolution Optical Fluctuation Bio-Imaging with Dual-Color Carbon Nanodots.

PubMed

Chizhik, Anna M; Stein, Simon; Dekaliuk, Mariia O; Battle, Christopher; Li, Weixing; Huss, Anja; Platen, Mitja; Schaap, Iwan A T; Gregor, Ingo; Demchenko, Alexander P; Schmidt, Christoph F; Enderlein, Jörg; Chizhik, Alexey I

2016-01-13

Success in super-resolution imaging relies on a proper choice of fluorescent probes. Here, we suggest novel easily produced and biocompatible nanoparticles-carbon nanodots-for super-resolution optical fluctuation bioimaging (SOFI). The particles revealed an intrinsic dual-color fluorescence, which corresponds to two subpopulations of particles of different electric charges. The neutral nanoparticles localize to cellular nuclei suggesting their potential use as an inexpensive, easily produced nucleus-specific label. The single particle study revealed that the carbon nanodots possess a unique hybrid combination of fluorescence properties exhibiting characteristics of both dye molecules and semiconductor nanocrystals. The results suggest that charge trapping and redistribution on the surface of the particles triggers their transitions between emissive and dark states. These findings open up new possibilities for the utilization of carbon nanodots in the various super-resolution microscopy methods based on stochastic optical switching.

Theoretical Insights into a CO Dimerization Mechanism in CO2 Electroreduction.

PubMed

Montoya, Joseph H; Shi, Chuan; Chan, Karen; Nørskov, Jens K

2015-06-04

In this work, we present DFT simulations that demonstrate the ability of Cu to catalyze CO dimerization in CO2 and CO electroreduction. We describe a previously unreported CO dimer configuration that is uniquely stabilized by a charged water layer on both Cu(111) and Cu(100). Without this charged water layer at the metal surface, the formation of the CO dimer is prohibitively endergonic. Our calculations also demonstrate that dimerization should have a lower activation barrier on Cu(100) than Cu(111), which, along with a more exergonic adsorption energy and a corresponding higher coverage of *CO, is consistent with experimental observations that Cu(100) has a high activity for C-C coupling at low overpotentials. We also demonstrate that this effect is present with cations other than H(+), a finding that is consistent with the experimentally observed pH independence of C2 formation on Cu.

High resolution printing of charge

DOEpatents

Rogers, John; Park, Jang-Ung

2015-06-16

Provided are methods of printing a pattern of charge on a substrate surface, such as by electrohydrodynamic (e-jet) printing. The methods relate to providing a nozzle containing a printable fluid, providing a substrate having a substrate surface and generating from the nozzle an ejected printable fluid containing net charge. The ejected printable fluid containing net charge is directed to the substrate surface, wherein the net charge does not substantially degrade and the net charge retained on the substrate surface. Also provided are functional devices made by any of the disclosed methods.

Photoelectric charging of partially sunlit dielectric surfaces in space

NASA Technical Reports Server (NTRS)

De, B. R.; Criswell, D. R.

1977-01-01

Sunlight-shadow effects may substantially alter the charging situation for a dielectric surface. The sunlight-shadow boundary tends to be the site of intense multipole electric fields. Charges on a sunlit dielectric surface have a finite effective mobility. The charge distribution tends to resemble that on a conducting surface. A boundary between a conducting and a dielectric surface may not represent a conductivity discontinuity when this boundary is sunlit; charges may migrate at a nontrivial rate across the boundary. A contracting or expanding sunlit area may experience a supercharging.

Effect of the surface charge discretization on electric double layers: a Monte Carlo simulation study.

PubMed

Madurga, Sergio; Martín-Molina, Alberto; Vilaseca, Eudald; Mas, Francesc; Quesada-Pérez, Manuel

2007-06-21

The structure of the electric double layer in contact with discrete and continuously charged planar surfaces is studied within the framework of the primitive model through Monte Carlo simulations. Three different discretization models are considered together with the case of uniform distribution. The effect of discreteness is analyzed in terms of charge density profiles. For point surface groups, a complete equivalence with the situation of uniformly distributed charge is found if profiles are exclusively analyzed as a function of the distance to the charged surface. However, some differences are observed moving parallel to the surface. Significant discrepancies with approaches that do not account for discreteness are reported if charge sites of finite size placed on the surface are considered.

Luminescent systems based on the isolation of conjugated PI systems and edge charge compensation with polar molecules on a charged nanostructured surface

DOEpatents

Ivanov, Ilia N.; Puretzky, Alexander A.; Zhao, Bin; Geohegan, David B.; Styers-Barnett, David J.; Hu, Hui

2014-07-15

A photoluminescent or electroluminescent system and method of making a non-luminescent nanostructured material into such a luminescent system is presented. The method of preparing the luminescent system, generally, comprises the steps of modifying the surface of a nanostructured material to create isolated regions to act as luminescent centers and to create a charge imbalance on the surface; applying more than one polar molecule to the charged surface of the nanostructured material; and orienting the polar molecules to compensate for the charge imbalance on the surface of the nanostructured material. The compensation of the surface charge imbalance by the polar molecules allows the isolated regions to exhibit luminescence.

Proximity charge sensing for semiconductor detectors

DOEpatents

Luke, Paul N; Tindall, Craig S; Amman, Mark

2013-10-08

A non-contact charge sensor includes a semiconductor detector having a first surface and an opposing second surface. The detector includes a high resistivity electrode layer on the first surface and a low resistivity electrode on the high resistivity electrode layer. A portion of the low resistivity first surface electrode is deleted to expose the high resistivity electrode layer in a portion of the area. A low resistivity electrode layer is disposed on the second surface of the semiconductor detector. A voltage applied between the first surface low resistivity electrode and the second surface low resistivity electrode causes a free charge to drift toward the first or second surface according to a polarity of the free charge and the voltage. A charge sensitive preamplifier coupled to a non-contact electrode disposed at a distance from the exposed high resistivity electrode layer outputs a signal in response to movement of free charge within the detector.

Close-in Blast Waves from Spherical Charges*

NASA Astrophysics Data System (ADS)

Howard, William; Kuhl, Allen

2011-06-01

We study the close-in blast waves created by the detonation of spherical high explosives (HE) charges, via numerical simulations with our Arbitrary-Lagrange-Eulerian (ALE3D) code. We used a finely-resolved, fixed Eulerian 2-D mesh (200 μm per cell) to capture the detonation of the charge, the blast wave propagation in air, and the reflection of the blast wave from an ideal surface. The thermodynamic properties of the detonation products and air were specified by the Cheetah code. A programmed-burn model was used to detonate the charge at a rate based on measured detonation velocities. The results were analyzed to evaluate the: (i) free air pressure-range curves: Δps (R) , (ii) free air impulse curves, (iii) reflected pressure-range curves, and (iv) reflected impulse-range curves. A variety of explosives were studied. Conclusions are: (i) close-in (R < 10 cm /g 1 / 3) , each explosive had its own (unique) blast wave (e.g., Δps (R , HE) ~ a /Rn , where n is different for each explosive); (ii) these close-in blast waves do not scale with the ``Heat of Detonation'' of the explosive (because close-in, there is not enough time to fully couple the chemical energy to the air via piston work); (iii) instead they are related to the detonation conditions inside the charge. Scaling laws will be proposed for such close-in blast waves.

Ultrafast Exciton Dissociation and Long-Lived Charge Separation in a Photovoltaic Pentacene-MoS2 van der Waals Heterojunction.

PubMed

Bettis Homan, Stephanie; Sangwan, Vinod K; Balla, Itamar; Bergeron, Hadallia; Weiss, Emily A; Hersam, Mark C

2017-01-11

van der Waals heterojunctions between two-dimensional (2D) layered materials and nanomaterials of different dimensions present unique opportunities for gate-tunable optoelectronic devices. Mixed-dimensional p-n heterojunction diodes, such as p-type pentacene (0D) and n-type monolayer MoS 2 (2D), are especially interesting for photovoltaic applications where the absorption cross-section and charge transfer processes can be tailored by rational selection from the vast library of organic molecules and 2D materials. Here, we study the kinetics of excited carriers in pentacene-MoS 2 p-n type-II heterojunctions by transient absorption spectroscopy. These measurements show that the dissociation of MoS 2 excitons occurs by hole transfer to pentacene on the time scale of 6.7 ps. In addition, the charge-separated state lives for 5.1 ns, up to an order of magnitude longer than the recombination lifetimes from previously reported 2D material heterojunctions. By studying the fractional amplitudes of the MoS 2 decay processes, the hole transfer yield from MoS 2 to pentacene is found to be ∼50%, with the remaining holes undergoing trapping due to surface defects. Overall, the ultrafast charge transfer and long-lived charge-separated state in pentacene-MoS 2 p-n heterojunctions suggest significant promise for mixed-dimensional van der Waals heterostructures in photovoltaics, photodetectors, and related optoelectronic technologies.

Probing the Surface Charge on the Basal Planes of Kaolinite Particles with High-Resolution Atomic Force Microscopy

PubMed Central

2017-01-01

High-resolution atomic force microscopy is used to map the surface charge on the basal planes of kaolinite nanoparticles in an ambient solution of variable pH and NaCl or CaCl2 concentration. Using DLVO theory with charge regulation, we determine from the measured force–distance curves the surface charge distribution on both the silica-like and the gibbsite-like basal plane of the kaolinite particles. We observe that both basal planes do carry charge that varies with pH and salt concentration. The silica facet was found to be negatively charged at pH 4 and above, whereas the gibbsite facet is positively charged at pH below 7 and negatively charged at pH above 7. Investigations in CaCl2 at pH 6 show that the surface charge on the gibbsite facet increases for concentration up to 10 mM CaCl2 and starts to decrease upon further increasing the salt concentration to 50 mM. The increase of surface charge at low concentration is explained by Ca2+ ion adsorption, while Cl– adsorption at higher CaCl2 concentrations partially neutralizes the surface charge. Atomic resolution imaging and density functional theory calculations corroborate these observations. They show that hydrated Ca2+ ions can spontaneously adsorb on the gibbsite facet of the kaolinite particle and form ordered surface structures, while at higher concentrations Cl– ions will co-adsorb, thereby changing the observed ordered surface structure. PMID:29140711

Probing the Surface Charge on the Basal Planes of Kaolinite Particles with High-Resolution Atomic Force Microscopy.

PubMed

Kumar, N; Andersson, M P; van den Ende, D; Mugele, F; Siretanu, I

2017-12-19

High-resolution atomic force microscopy is used to map the surface charge on the basal planes of kaolinite nanoparticles in an ambient solution of variable pH and NaCl or CaCl 2 concentration. Using DLVO theory with charge regulation, we determine from the measured force-distance curves the surface charge distribution on both the silica-like and the gibbsite-like basal plane of the kaolinite particles. We observe that both basal planes do carry charge that varies with pH and salt concentration. The silica facet was found to be negatively charged at pH 4 and above, whereas the gibbsite facet is positively charged at pH below 7 and negatively charged at pH above 7. Investigations in CaCl 2 at pH 6 show that the surface charge on the gibbsite facet increases for concentration up to 10 mM CaCl 2 and starts to decrease upon further increasing the salt concentration to 50 mM. The increase of surface charge at low concentration is explained by Ca 2+ ion adsorption, while Cl - adsorption at higher CaCl 2 concentrations partially neutralizes the surface charge. Atomic resolution imaging and density functional theory calculations corroborate these observations. They show that hydrated Ca 2+ ions can spontaneously adsorb on the gibbsite facet of the kaolinite particle and form ordered surface structures, while at higher concentrations Cl - ions will co-adsorb, thereby changing the observed ordered surface structure.

The crystal structure of Haloferax volcanii proliferating cell nuclear antigen reveals unique surface charge characteristics due to halophilic adaptation

PubMed Central

Winter, Jody A; Christofi, Panayiotis; Morroll, Shaun; Bunting, Karen A

2009-01-01

Background The high intracellular salt concentration required to maintain a halophilic lifestyle poses challenges to haloarchaeal proteins that must stay soluble, stable and functional in this extreme environment. Proliferating cell nuclear antigen (PCNA) is a fundamental protein involved in maintaining genome integrity, with roles in both DNA replication and repair. To investigate the halophilic adaptation of such a key protein we have crystallised and solved the structure of Haloferax volcanii PCNA (HvPCNA) to a resolution of 2.0 Å. Results The overall architecture of HvPCNA is very similar to other known PCNAs, which are highly structurally conserved. Three commonly observed adaptations in halophilic proteins are higher surface acidity, bound ions and increased numbers of intermolecular ion pairs (in oligomeric proteins). HvPCNA possesses the former two adaptations but not the latter, despite functioning as a homotrimer. Strikingly, the positive surface charge considered key to PCNA's role as a sliding clamp is dramatically reduced in the halophilic protein. Instead, bound cations within the solvation shell of HvPCNA may permit sliding along negatively charged DNA by reducing electrostatic repulsion effects. Conclusion The extent to which individual proteins adapt to halophilic conditions varies, presumably due to their diverse characteristics and roles within the cell. The number of ion pairs observed in the HvPCNA monomer-monomer interface was unexpectedly low. This may reflect the fact that the trimer is intrinsically stable over a wide range of salt concentrations and therefore additional modifications for trimer maintenance in high salt conditions are not required. Halophilic proteins frequently bind anions and cations and in HvPCNA cation binding may compensate for the remarkable reduction in positive charge in the pore region, to facilitate functional interactions with DNA. In this way, HvPCNA may harness its environment as opposed to simply surviving in extreme halophilic conditions. PMID:19698123

Electronically shielded solid state charged particle detector

DOEpatents

Balmer, D.K.; Haverty, T.W.; Nordin, C.W.; Tyree, W.H.

1996-08-20

An electronically shielded solid state charged particle detector system having enhanced radio frequency interference immunity includes a detector housing with a detector entrance opening for receiving the charged particles. A charged particle detector having an active surface is disposed within the housing. The active surface faces toward the detector entrance opening for providing electrical signals representative of the received charged particles when the received charged particles are applied to the active surface. A conductive layer is disposed upon the active surface. In a preferred embodiment, a nonconductive layer is disposed between the conductive layer and the active surface. The conductive layer is electrically coupled to the detector housing to provide a substantially continuous conductive electrical shield surrounding the active surface. The inner surface of the detector housing is supplemented with a radio frequency absorbing material such as ferrite. 1 fig.

Electronically shielded solid state charged particle detector

DOEpatents

Balmer, David K.; Haverty, Thomas W.; Nordin, Carl W.; Tyree, William H.

1996-08-20

An electronically shielded solid state charged particle detector system having enhanced radio frequency interference immunity includes a detector housing with a detector entrance opening for receiving the charged particles. A charged particle detector having an active surface is disposed within the housing. The active surface faces toward the detector entrance opening for providing electrical signals representative of the received charged particles when the received charged particles are applied to the active surface. A conductive layer is disposed upon the active surface. In a preferred embodiment, a nonconductive layer is disposed between the conductive layer and the active surface. The conductive layer is electrically coupled to the detector housing to provide a substantially continuous conductive electrical shield surrounding the active surface. The inner surface of the detector housing is supplemented with a radio frequency absorbing material such as ferrite.

pH-activatable nanoparticles for tumor-specific drug delivery

NASA Astrophysics Data System (ADS)

Liu, Karen C.

To address the need for a tumor-specific drug delivery system that can achieve both prolonged circulation and cellular retention at the tumor site, nanocomplexes of Zwitterionic Chitosan (ZWC) and Polyamidoamine (PAMAM) generation 5 were designed. Polyamidoamine (PAMAM) dendrimers have been widely explored as carriers of therapeutics and imaging agents, however, amine-terminated PAMAM dendrimers are rarely utilized in systemic applications due to its cytotoxicity and risk of opsonization, caused by its cationic charge. Such undesirable effects may be mitigated by shielding the PAMAM dendrimer surface with polymers that reduce the charges. However, this shielding may also interfere with PAMAM dendrimers' ability to interact with target cells, thus reducing cellular uptake and overall efficacy of the delivery system. ZWC, a new chitosan derivative, has a unique pH-sensitive charge profile and can shield the cationic surface of PAMAM dendrimers and block adsorption of serum proteins to allow for prolonged circulation. The hypothesis of this approach is that ZWC is anionic and able to coat PAMAM in neutral pH but becomes positive in the acidic tumor microenvironment, revealing the polycationic drug carrier. We expect that ZWC will provide (i) stealth coating for PAMAM drug carrier during circulation (pH 7.4) and (ii) be removed from the PAMAM drug carrier at acidic pH (pH ~6.3), allowing for cellular interaction. The cationic charge of PAMAM has been demonstrated to facilitate uptake and drug delivery to tumor cells via interactions with the negatively charged cell surface. Stable electrostatic complexes of ZWC and PAMAM dendrimers were formed at pH 7.4, as demonstrated by fluorescence spectroscopy and transmission electron microscopy. The presence of ZWC coating protected red blood cells and fibroblast cells from hemolytic and cytotoxic activities of PAMAM dendrimers, respectively. Confocal microscopy showed that the protective effect of ZWC disappeared at low pH as the complex dissociated due to the charge conversion of ZWC, allowing PAMAM dendrimers to enter cells. These results demonstrate that ZWC is able to provide a surface coverage of PAMAM dendrimers in a pH-dependent manner and, thus, enhance the utility of PAMAM dendrimers as a drug carrier to solid tumors with acidifying microenvironment. Paclitaxel, curcumin, and camptothecin were evaluated as model drugs for use in ZWC(PAMAM) drug carrier based on bioactivity against SKOV-3 ovarian cancer cells and drug loading and release. Stability of nanocarriers in circulation is a requirement for successful tumor-specific drug release. Strategies to improve the stability of ZWC(PAMAM) NPs were also explored and evaluated.

Strong coupling electrostatics for randomly charged surfaces: antifragility and effective interactions.

PubMed

Ghodrat, Malihe; Naji, Ali; Komaie-Moghaddam, Haniyeh; Podgornik, Rudolf

2015-05-07

We study the effective interaction mediated by strongly coupled Coulomb fluids between dielectric surfaces carrying quenched, random monopolar charges with equal mean and variance, both when the Coulomb fluid consists only of mobile multivalent counterions and when it consists of an asymmetric ionic mixture containing multivalent and monovalent (salt) ions in equilibrium with an aqueous bulk reservoir. We analyze the consequences that follow from the interplay between surface charge disorder, dielectric and salt image effects, and the strong electrostatic coupling that results from multivalent counterions on the distribution of these ions and the effective interaction pressure they mediate between the surfaces. In a dielectrically homogeneous system, we show that the multivalent counterions are attracted towards the surfaces with a singular, disorder-induced potential that diverges logarithmically on approach to the surfaces, creating a singular but integrable counterion density profile that exhibits an algebraic divergence at the surfaces with an exponent that depends on the surface charge (disorder) variance. This effect drives the system towards a state of lower thermal 'disorder', one that can be described by a renormalized temperature, exhibiting thus a remarkable antifragility. In the presence of an interfacial dielectric discontinuity, the singular behavior of counterion density at the surfaces is removed but multivalent counterions are still accumulated much more strongly close to randomly charged surfaces as compared with uniformly charged ones. The interaction pressure acting on the surfaces displays in general a highly non-monotonic behavior as a function of the inter-surface separation with a prominent regime of attraction at small to intermediate separations. This attraction is caused directly by the combined effects from charge disorder and strong coupling electrostatics of multivalent counterions, which dominate the surface-surface repulsion due to the (equal) mean charges on the two surfaces and the osmotic pressure of monovalent ions residing between them. These effects can be quite significant even with a small degree of surface charge disorder relative to the mean surface charge. The strong coupling, disorder-induced attraction is typically much stronger than the van der Waals interaction between the surfaces, especially within a range of several nanometers for the inter-surface separation, where such effects are predicted to be most pronounced.

Effect of surface material on electrostatic charging of houseflies (Musca domestica L).

PubMed

McGonigle, Daniel F; Jackson, Chris W

2002-04-01

Houseflies (Musca domestica L) accumulated electrostatic charges when walking over clean, uncharged dielectric surfaces. The charges elicited on a walking housefly by a range of materials were quantified, allowing a triboelectric series to be determined relative to M domestica. This ranged from surfaces that charged individuals positively, e.g. Correx (corrugated polypropylene) [.1 (+/- 4.2)pC], to those that applied a negative charge, e.g. clear cast acrylic [-14.9 (+/- 2.9)pC]. Maximum positive and negative charges accumulated by individual M domestica were +73 and -27 pC. Replicate measurements on the same fly and surface showed little variation. Variation between individuals was not related to sex and was not consistent between surfaces. Different materials charged M domestica significantly differently and individual flies had significantly different charging properties. Variation in temperature between 21.3 degrees C and 24.7 degrees C and humidity between 24% and 41% RH significantly affected charge accumulated by M domestica on some surfaces, although further experimentation is needed to confirm this. The implications of this work are discussed in relation to insect trap design and pollination biology.

Characterization of Colloidal Quantum Dot Ligand Exchange by X-ray Photoelectron Spectroscopy

NASA Astrophysics Data System (ADS)

Atewologun, Ayomide; Ge, Wangyao; Stiff-Roberts, Adrienne D.

2013-05-01

Colloidal quantum dots (CQDs) are chemically synthesized semiconductor nanoparticles with size-dependent wavelength tunability. Chemical synthesis of CQDs involves the attachment of long organic surface ligands to prevent aggregation; however, these ligands also impede charge transport. Therefore, it is beneficial to exchange longer surface ligands for shorter ones for optoelectronic devices. Typical characterization techniques used to analyze surface ligand exchange include Fourier-transform infrared spectroscopy, x-ray diffraction, transmission electron microscopy, and nuclear magnetic resonance spectroscopy, yet these techniques do not provide a simultaneously direct, quantitative, and sensitive method for evaluating surface ligands on CQDs. In contrast, x-ray photoelectron spectroscopy (XPS) can provide nanoscale sensitivity for quantitative analysis of CQD surface ligand exchange. A unique aspect of this work is that a fingerprint is identified for shorter surface ligands by resolving the regional XPS spectrum corresponding to different types of carbon bonds. In addition, a deposition technique known as resonant infrared matrix-assisted pulsed laser evaporation is used to improve the CQD film uniformity such that stronger XPS signals are obtained, enabling more accurate analysis of the ligand exchange process.

Oil Contact Angles in a Water-Decane-Silicon Dioxide System: Effects of Surface Charge

NASA Astrophysics Data System (ADS)

Xu, Shijing; Wang, Jingyao; Wu, Jiazhong; Liu, Qingjie; Sun, Chengzhen; Bai, Bofeng

2018-04-01

Oil wettability in the water-oil-rock systems is very sensitive to the evolution of surface charges on the rock surfaces induced by the adsorption of ions and other chemical agents in water flooding. Through a set of large-scale molecular dynamics simulations, we reveal the effects of surface charge on the oil contact angles in an ideal water-decane-silicon dioxide system. The results show that the contact angles of oil nano-droplets have a great dependence on the surface charges. As the surface charge density exceeds a critical value of 0.992 e/nm2, the contact angle reaches up to 78.8° and the water-wet state is very apparent. The variation of contact angles can be confirmed from the number density distributions of oil molecules. With increasing the surface charge density, the adsorption of oil molecules weakens and the contact areas between nano-droplets and silicon dioxide surface are reduced. In addition, the number density distributions, RDF distributions, and molecular orientations indicate that the oil molecules are adsorbed on the silicon dioxide surface layer-by-layer with an orientation parallel to the surface. However, the layered structure of oil molecules near the silicon dioxide surface becomes more and more obscure at higher surface charge densities.

Oil Contact Angles in a Water-Decane-Silicon Dioxide System: Effects of Surface Charge.

PubMed

Xu, Shijing; Wang, Jingyao; Wu, Jiazhong; Liu, Qingjie; Sun, Chengzhen; Bai, Bofeng

2018-04-19

Oil wettability in the water-oil-rock systems is very sensitive to the evolution of surface charges on the rock surfaces induced by the adsorption of ions and other chemical agents in water flooding. Through a set of large-scale molecular dynamics simulations, we reveal the effects of surface charge on the oil contact angles in an ideal water-decane-silicon dioxide system. The results show that the contact angles of oil nano-droplets have a great dependence on the surface charges. As the surface charge density exceeds a critical value of 0.992 e/nm 2 , the contact angle reaches up to 78.8° and the water-wet state is very apparent. The variation of contact angles can be confirmed from the number density distributions of oil molecules. With increasing the surface charge density, the adsorption of oil molecules weakens and the contact areas between nano-droplets and silicon dioxide surface are reduced. In addition, the number density distributions, RDF distributions, and molecular orientations indicate that the oil molecules are adsorbed on the silicon dioxide surface layer-by-layer with an orientation parallel to the surface. However, the layered structure of oil molecules near the silicon dioxide surface becomes more and more obscure at higher surface charge densities.

Critical Dipole Length for the Wetting Transition Due to Collective Water-dipoles Interactions

PubMed Central

Wang, Chunlei; Zhou, Bo; Tu, Yusong; Duan, Manyi; Xiu, Peng; Li, Jingye; Fang, Haiping

2012-01-01

The wetting behavior of water on the solid surfaces is fundamental to various physical, chemical and biological processes. Conventionally, the surface with charges or charge dipoles is hydrophilic, whereas the non-polar surface is hydrophobic though some exceptions were recently reported. Using molecular dynamics simulations, we show that there is a critical length of the charge dipoles on the solid surface. The solid surface still exhibited hydrophobic behavior when the dipole length was less than the critical value, indicating that the water molecules on the solid surface seemed not “feel” attractive interactions from the charge dipoles on the solid surface. Those unexpected observations result from the collective interactions between the water molecules and charge dipoles on the solid surface, where the steric exclusion effect between water molecules greatly reduces the water-dipole interactions. Remarkably, the steric exclusion effect is also important for surfaces with charge dipole lengths greater than this critical length. PMID:22496954

Reinvestigating the surface and bulk electronic properties of Cd3As2

NASA Astrophysics Data System (ADS)

Roth, S.; Lee, H.; Sterzi, A.; Zacchigna, M.; Politano, A.; Sankar, R.; Chou, F. C.; Di Santo, G.; Petaccia, L.; Yazyev, O. V.; Crepaldi, A.

2018-04-01

Cd3As2 is widely considered among the few materials realizing the three-dimensional (3D) Dirac semimetal phase. Linearly dispersing states, responsible for the ultrahigh charge mobility, have been reported by several angle-resolved photoelectron spectroscopy (ARPES) investigations. However, in spite of the general agreement between these studies, some details are at odds. From scanning tunneling microscopy and optical experiments under magnetic field, a puzzling scenario emerges in which multiple states show linear dispersion at different energy scales. Here, we solve this apparent controversy by reinvestigating the electronic properties of the (112) surface of Cd3As2 by combining ARPES and theoretical calculations. We disentangle the presence of massive and massless metallic bulk and surface states, characterized by different symmetries. Our systematic experimental and theoretical study clarifies the complex band dispersion of Cd3As2 by extending the simplistic 3D Dirac semimetal model to account for multiple bulk and surface states crossing the Fermi level, and thus contributing to the unique material transport properties.

Polyelectrolyte adsorption onto like-charged surfaces mediated by trivalent counterions: A Monte Carlo simulation study

NASA Astrophysics Data System (ADS)

Luque-Caballero, Germán; Martín-Molina, Alberto; Quesada-Pérez, Manuel

2014-05-01

Both experiments and theory have evidenced that multivalent cations can mediate the interaction between negatively charged polyelectrolytes and like-charged objects, such as anionic lipoplexes (DNA-cation-anionic liposome complexes). In this paper, we use Monte Carlo simulations to study the electrostatic interaction responsible for the trivalent-counterion-mediated adsorption of polyelectrolytes onto a like-charged planar surface. The evaluation of the Helmholtz free energy allows us to characterize both the magnitude and the range of the interaction as a function of the polyelectrolyte charge, surface charge density, [3:1] electrolyte concentration, and cation size. Both polyelectrolyte and surface charge favor the adsorption. It should be stressed, however, that the adsorption will be negligible if the surface charge density does not exceed a threshold value. The effect of the [3:1] electrolyte concentration has also been analyzed. In certain range of concentrations, the counterion-mediated attraction seems to be independent of this parameter, whereas very high concentrations of salt weaken the adsorption. If the trivalent cation diameter is doubled the adsorption moderates due to the excluded volume effects. The analysis of the integrated charge density and ionic distributions suggests that a delicate balance between charge inversion and screening effects governs the polyelectrolyte adsorption onto like-charged surfaces mediated by trivalent cations.

Charge renormalization and inversion of a highly charged lipid bilayer: effects of dielectric discontinuities and charge correlations.

PubMed

Taheri-Araghi, Sattar; Ha, Bae-Yeun

2005-08-01

We reexamine the problem of charge renormalization and inversion of a highly charged surface of a low dielectric constant immersed in ionic solutions. To be specific, we consider an asymmetrically charged lipid bilayer, in which only one layer is negatively charged. In particular, we study how dielectric discontinuities and charge correlations (among lipid charges and condensed counterions) influence the effective charge of the surface. When counterions are monovalent (e.g., Na+), our mean-field approach implies that dielectric discontinuities can enhance counterion condensation. A simple scaling picture shows how the effects of dielectric discontinuities and surface-charge distributions are intertwined: Dielectric discontinuities diminish condensation if the backbone charge is uniformly smeared out while counterions are localized in space; they can, however, enhance condensation when the backbone charge is discrete. In the presence of asymmetric salts such as CaCl2 , we find that the correlation effect, treated at the Gaussian level, is more pronounced when the surface has a lower dielectric constant, inverting the sign of the charge at a smaller value of Ca2+ concentration.

Ion association at discretely-charged dielectric interfaces: Giant charge inversion [Dielectric response controlled ion association at physically heterogeneous surfaces: Giant charge reversal

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Zhi -Yong; Wu, Jianzhong

2017-07-11

Giant charge reversal has been identified for the first time by Monte Carlo simulation for a discretely charged surface in contact with a trivalent electrolyte solution. It takes place regardless of the surface charge density under study and the monovalent salt. In stark contrast to earlier predictions based on the 2-dimensional Wigner crystal model to describe strong correlation of counterions at the macroion surface, we find that giant charge reversal reflects an intricate interplay of ionic volume effects, electrostatic correlations, surface charge heterogeneity, and the dielectric response of the confined fluids. While the novel phenomenon is yet to be confirmedmore » with experiment, the simulation results appear in excellent agreement with a wide range of existing observations in the subregime of charge inversion. Lastly, our findings may have far-reaching implications to understanding complex electrochemical phenomena entailing ionic fluids under dielectric confinements.« less

Triboelectric, Corona, and Induction Charging of Insulators as a Function of Pressure

NASA Technical Reports Server (NTRS)

Hogue, Michael D.; Mucciolo, Eduardo R.; Calle, Carlos I.

2006-01-01

Theoretical and experimental research has been performed that shows that the surface charge on an insulator after triboelectric charging with another insulator is rapidly dissipated with lowered atmospheric pressure. This pressure discharge is consistent with surface ions being evaporated off the surface once their vapor pressure is attained. In this paper we will report on the results of three different charging techniques (triboelectric, corona, and induction) performed on selected polymers with varying atmospheric pressure. This data will show that ion exchange between the polymer samples is the mechanism responsible for most of the surface charge on the polymer surfaces.

Material properties that predict preservative uptake for silicone hydrogel contact lenses.

PubMed

Green, J Angelo; Phillips, K Scott; Hitchins, Victoria M; Lucas, Anne D; Shoff, Megan E; Hutter, Joseph C; Rorer, Eva M; Eydelman, Malvina B

2012-11-01

To assess material properties that affect preservative uptake by silicone hydrogel lenses. We evaluated the water content (using differential scanning calorimetry), effective pore size (using probe penetration), and preservative uptake (using high-performance liquid chromatography with spectrophotometric detection) of silicone and conventional hydrogel soft contact lenses. Lenses grouped similarly based on freezable water content as they did based on total water content. Evaluation of the effective pore size highlighted potential differences between the surface-treated and non-surface-treated materials. The water content of the lens materials and ionic charge are associated with the degree of preservative uptake. The current grouping system for testing contact lens-solution interactions separates all silicone hydrogels from conventional hydrogel contact lenses. However, not all silicone hydrogel lenses interact similarly with the same contact lens solution. Based upon the results of our research, we propose that the same material characteristics used to group conventional hydrogel lenses, water content and ionic charge, can also be used to predict uptake of hydrophilic preservatives for silicone hydrogel lenses. In addition, the hydrophobicity of silicone hydrogel contact lenses, although not investigated here, is a unique contact lens material property that should be evaluated for the uptake of relatively hydrophobic preservatives and tear components.

Molecular sensing using monolayer floating gate, fully depleted SOI MOSFET acting as an exponential transducer.

PubMed

Takulapalli, Bharath R

2010-02-23

Field-effect transistor-based chemical sensors fall into two broad categories based on the principle of signal transduction-chemiresistor or Schottky-type devices and MOSFET or inversion-type devices. In this paper, we report a new inversion-type device concept-fully depleted exponentially coupled (FDEC) sensor, using molecular monolayer floating gate fully depleted silicon on insulator (SOI) MOSFET. Molecular binding at the chemical-sensitive surface lowers the threshold voltage of the device inversion channel due to a unique capacitive charge-coupling mechanism involving interface defect states, causing an exponential increase in the inversion channel current. This response of the device is in opposite direction when compared to typical MOSFET-type sensors, wherein inversion current decreases in a conventional n-channel sensor device upon addition of negative charge to the chemical-sensitive device surface. The new sensor architecture enables ultrahigh sensitivity along with extraordinary selectivity. We propose the new sensor concept with the aid of analytical equations and present results from our experiments in liquid phase and gas phase to demonstrate the new principle of signal transduction. We present data from numerical simulations to further support our theory.

Modulating the fixed charge density in silicon nitride films while monitoring the surface recombination velocity by photoluminescence imaging

NASA Astrophysics Data System (ADS)

Bazilchuk, Molly; Haug, Halvard; Marstein, Erik Stensrud

2015-04-01

Several important semiconductor devices such as solar cells and photodetectors may be fabricated based on surface inversion layer junctions induced by fixed charge in a dielectric layer. Inversion layer junctions can easily be fabricated by depositing layers with a high density of fixed charge on a semiconducting substrate. Increasing the fixed charge improves such devices; for instance, the efficiency of a solar cell can be substantially increased by reducing the surface recombination velocity, which is a function of the fixed charge density. Methods for increasing the charge density are therefore of interest. In this work, the fixed charge density in silicon nitride layers deposited by plasma enhanced chemical vapor deposition is increased to very high values above 1 × 1013 cm-2 after the application of an external voltage to a gate electrode. The effect of the fixed charge density on the surface recombination velocity was experimentally observed using the combination of capacitance-voltage characterization and photoluminescence imaging, showing a significant reduction in the surface recombination velocity for increasing charge density. The surface recombination velocity vs. charge density data was analyzed using a numerical device model, which indicated the presence of a sub-surface damage region formed during deposition of the layers. Finally, we have demonstrated that the aluminum electrodes used for charge injection may be chemically removed in phosphoric acid without loss of the underlying charge. The injected charge was shown to be stable for a prolonged time period, leading us to propose charge injection in silicon nitride films by application of soaking voltage as a viable method for fabricating inversion layer devices.

Theoretical investigation of stabilities and optical properties of Si12C12 clusters

NASA Astrophysics Data System (ADS)

Duan, Xiaofeng F.; Burggraf, Larry W.

2015-01-01

By sorting through hundreds of globally stable Si12C12 isomers using a potential surface search and using simulated annealing, we have identified low-energy structures. Unlike isomers knit together by Si-C bonds, the lowest energy isomers have segregated carbon and silicon regions that maximize stronger C-C bonding. Positing that charge separation between the carbon and silicon regions would produce interesting optical absorption in these cluster molecules, we used time-dependent density functional theory to compare the calculated optical properties of four isomers representing structural classes having different types of silicon and carbon segregation regions. Absorptions involving charge transfer between segregated carbon and silicon regions produce lower excitation energies than do structures having alternating Si-C bonding for which frontier orbital charge transfer is exclusively from separated carbon atoms to silicon atoms. The most stable Si12C12 isomer at temperatures below 1100 K is unique as regards its high symmetry and large optical oscillator strength in the visible blue. Its high-energy and low-energy visible transitions (1.15 eV and 2.56 eV) are nearly pure one-electron silicon-to-carbon transitions, while an intermediate energy transition (1.28 eV) is a nearly pure carbon-to-silicon one-electron charge transfer.

Passive Plasma Contact Mechanisms for Small-Scale Spacecraft

NASA Astrophysics Data System (ADS)

McTernan, Jesse K.

Small-scale spacecraft represent a paradigm shift in how entities such as academia, industry, engineering firms, and the scientific community operate in space. However, although the paradigm shift produces unique opportunities to build satellites in unique ways for novel missions, there are also significant challenges that must be addressed. This research addresses two of the challenges associated with small-scale spacecraft: 1) the miniaturization of spacecraft and associated instrumentation and 2) the need to transport charge across the spacecraft-environment boundary. As spacecraft decrease in size, constraints on the size, weight, and power of on-board instrumentation increase--potentially limiting the instrument's functionality or ability to integrate with the spacecraft. These constraints drive research into mechanisms or techniques that use little or no power and efficiently utilize existing resources. One limited resource on small-scale spacecraft is outer surface area, which is often covered with solar panels to meet tight power budgets. This same surface area could also be needed for passive neutralization of spacecraft charging. This research explores the use of a transparent, conductive layer on the solar cell coverglass that is electrically connected to spacecraft ground potential. This dual-purpose material facilitates the use of outer surfaces for both energy harvesting of solar photons as well as passive ion collection. Mission capabilities such as in-situ plasma measurements that were previously infeasible on small-scale platforms become feasible with the use of indium tin oxide-coated solar panel coverglass. We developed test facilities that simulate the space environment in low Earth orbit to test the dual-purpose material and the various application of this approach. Particularly, this research is in support of two upcoming missions: OSIRIS-3U, by Penn State's Student Space Programs Lab, and MiTEE, by the University of Michigan. The purpose of OSIRIS-3U is to investigate the effects of space weather on the ionosphere. The spacecraft will use a pulsed Langmuir probe, an instrument now enabled on small-scale spacecraft through the techniques outlined in this research.

Effects of charge design features on parameters of acoustic and seismic waves and cratering, for SMR chemical surface explosions

NASA Astrophysics Data System (ADS)

Gitterman, Y.

2012-04-01

A series of experimental on-surface shots was designed and conducted by the Geophysical Institute of Israel at Sayarim Military Range (SMR) in Negev desert, including two large calibration explosions: about 82 tons of strong IMI explosives in August 2009, and about 100 tons of ANFO explosives in January 2011. It was a collaborative effort between Israel, CTBTO, USA and several European countries, with the main goal to provide fully controlled ground truth (GT0) infrasound sources in different weather/wind conditions, for calibration of IMS infrasound stations in Europe, Middle East and Asia. Strong boosters and the upward charge detonation scheme were applied to provide a reduced energy release to the ground and an enlarged energy radiation to the atmosphere, producing enhanced infrasound signals, for better observation at far-regional stations. The following observations and results indicate on the required explosives energy partition for this charge design: 1) crater size and local seismic (duration) magnitudes were found smaller than expected for these large surface explosions; 2) small test shots of the same charge (1 ton) conducted at SMR with different detonation directions showed clearly lower seismic amplitudes/energy and smaller crater size for the upward detonation; 3) many infrasound stations at local and regional distances showed higher than expected peak amplitudes, even after application of a wind-correction procedure. For the large-scale explosions, high-pressure gauges were deployed at 100-600 m to record air-blast properties, evaluate the efficiency of the charge design and energy generation, and provide a reliable estimation of the charge yield. Empirical relations for air-blast parameters - peak pressure, impulse and the Secondary Shock (SS) time delay - depending on distance, were developed and analyzed. The parameters, scaled by the cubic root of estimated TNT equivalent charges, were found consistent for all analyzed explosions, except of SS time delays clearly separated for the shot of IMI explosives (characterized by much higher detonation velocity than ANFO). Additionally acoustic records at close distances from WSMR explosions Distant Image (2440 tons of ANFO) and Minor Uncle (2725 tons of ANFO) were used to extend the charge and distance range for the SS delay scaled relationship, that showed consistency with SMR ANFO shots. The developed specific charge design contributed to the success of this unique dual Sayarim explosion experiment, providing the strongest GT0 sources since the establishment of the IMS network, that demonstrated clearly the most favorable westward/ eastward infrasound propagation up to 3400/6250 km according to appropriate summer/winter weather pattern and stratospheric wind directions, respectively, and thus verified empirically common models of infrasound propagation in the atmosphere. The research was supported by the CTBTO, Vienna, and the Israel Ministry of Immigrant Absorption.

Electric Double-Layer Interaction between Dissimilar Charge-Conserved Conducting Plates.

PubMed

Chan, Derek Y C

2015-09-15

Small metallic particles used in forming nanostructured to impart novel optical, catalytic, or tribo-rheological can be modeled as conducting particles with equipotential surfaces that carry a net surface charge. The value of the surface potential will vary with the separation between interacting particles, and in the absence of charge-transfer or electrochemical reactions across the particle surface, the total charge of each particle must also remain constant. These two physical conditions require the electrostatic boundary condition for metallic nanoparticles to satisfy an equipotential whole-of-particle charge conservation constraint that has not been studied previously. This constraint gives rise to a global charge conserved constant potential boundary condition that results in multibody effects in the electric double-layer interaction that are either absent or are very small in the familiar constant potential or constant charge or surface electrochemical equilibrium condition.

Bacterial attachment to RO membranes surface-modified by concentration-polarization-enhanced graft polymerization.

PubMed

Bernstein, Roy; Belfer, Sofia; Freger, Viatcheslav

2011-07-15

Concentration polarization-enhanced radical graft polymerization, a facile surface modification technique, was examined as an approach to reduce bacterial deposition onto RO membranes and thus contribute to mitigation of biofouling. For this purpose an RO membrane ESPA-1 was surface-grafted with a zwitterionic and negatively and positively charged monomers. The low monomer concentrations and low degrees of grafting employed in modifications moderately reduced flux (by 20-40%) and did not affect salt rejection, yet produced substantial changes in surface chemistry, charge and hydrophilicity. The propensity to bacterial attachment of original and modified membranes was assessed using bacterial deposition tests carried out in a parallel plate flow setup using a fluorescent strain of Pseudomonas fluorescens. Compared to unmodified ESPA-1 the deposition (mass transfer) coefficient was significantly increased for modification with the positively charged monomer. On the other hand, a substantial reduction in bacterial deposition rates was observed for membranes modified with zwitterionic monomer and, still more, with very hydrophilic negatively charged monomers. This trend is well explained by the effects of surface charge (as measured by ζ-potential) and hydrophilicity (contact angle). It also well correlated with force distance measurements by AFM using surrogate spherical probes with a negative surface charge mimicking the bacterial surface. The positively charged surface showed a strong hysteresis with a large adhesion force, which was weaker for unmodified ESPA-1 and still weaker for zwitterionic surface, while negatively charged surface showed a long-range repulsion and negligible hysteresis. These results demonstrate the potential of using the proposed surface- modification approach for varying surface characteristics, charge and hydrophilicity, and thus minimizing bacterial deposition and potentially reducing propensity biofouling.

Improved electrochemical properties of morphology-controlled titania/titanate nanostructures prepared by in-situ hydrothermal surface modification of self-source Ti substrate for high-performance supercapacitors.

PubMed

Banerjee, Arghya Narayan; Anitha, V C; Joo, Sang W

2017-10-16

Ti substrate surface is modified into two-dimensional (2D) TiO 2 nanoplatelet or one-dimensional (1D) nanorod/nanofiber (or a mixture of both) structure in a controlled manner via a simple KOH-based hydrothermal technique. Depending on the KOH concentration, different types of TiO 2 nanostructures (2D platelets, 1D nanorods/nanofibers and a 2D+1D mixed sample) are fabricated directly onto the Ti substrate surface. The novelty of this technique is the in-situ modification of the self-source Ti surface into titania nanostructures, and its direct use as the electrochemical microelectrode without any modifications. This leads to considerable improvement in the interfacial properties between metallic Ti and semiconducting TiO 2 . Since interfacial states/defects have profound effect on charge transport properties of electronic/electrochemical devices, therefore this near-defect-free interfacial property of Ti-TiO 2 microelectrode has shown high supercapacitive performances for superior charge-storage devices. Additionally, by hydrothermally tuning the morphology of titania nanostructures, the electrochemical properties of the electrodes are also tuned. A Ti-TiO 2 electrode comprising of a mixture of 2D-platelet+1D-nanorod structure reveals very high specific capacitance values (~7.4 mF.cm -2 ) due to the unique mixed morphology which manifests higher active sites (hence, higher utilization of the active materials) in terms of greater roughness at the 2D-platelet structures and higher surface-to-volume-ratio in the 1D-nanorod structures.

CO 2 Adsorption on Anatase TiO 2 (101) Surfaces in the Presence of Subnanometer Ag/Pt Clusters: Implications for CO 2 Photoreduction

DOE PAGES

Yang, Chi-Ta; Wood, Brandon C.; Bhethanabotla, Venkat R.; ...

2014-10-20

We show how CO 2 adsorption on perfect and reduced anatase TiO 2 (101) surfaces can be substantially modified by the presence of surface Ag and Pt octamer clusters, using density functional theory calculations. Furthermore, we found that adsorption was affected even at sites where the adsorbate was not in direct contact with the octamer, which we attributed to charge donation to CO 2 from the Ag/Pt-modified surface, as well as an electrostatic competition between attractive (Ti–O) and repulsive (Ti–C) interactions. Additionally, TiO 2-supported Pt octamers offer key advantages that could be leveraged for CO 2 photoreduction, including providing additionalmore » stable adsorption sites for bent CO 2 species and facilitating charge transfer to aid in CO 2– anion formation. Electronic structure analysis suggests these factors arise primarily from the hybridization of the bonding molecular orbitals of CO 2 with d orbitals of the Pt atoms. Our results show that, for adsorption on TiO 2-supported Pt octamers, the O–C–O bending and C–O asymmetric stretching frequencies can be used as reliable indicators of the presence of the CO 2– anion intermediate as well as to distinguish unique adsorption geometries or sites. Finally, we suggest a possible pathway for subsequent CO 2 dissociation to CO at the surface of a reduced anatase TiO 2 (101)-supported Pt octamer, which has a computed energy barrier of 1.01 eV.« less

Surface-induced dissociation: a unique tool for studying energetics and kinetics of the gas-phase fragmentation of large ions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Laskin, Julia

2015-01-01

Surface-induced dissociation (SID) is valuable tool for investigating activation and dissociation of large ions in tandem mass spectrometry. This account summarizes key findings from studies of the energetics and mechanisms of complex ion dissociation, in which SID experiments were combined with Rice-Ramsperger-Kassel-Marcus (RRKM) modeling of the experimental data. These studies used time- and collision-energy-resolved SID experiments and SID combined with resonant ejection of selected fragment ions on a specially designed Fourier transform ion cyclotron resonance mass spectrometer (FT-ICR MS). Fast ion activation by collision with a surface combined with the long and variable timescale of a FT-ICR MS is perfectlymore » suited for studying the energetics and dynamics of complex ion dissociation in the gas phase. Modeling of time- and collision-energy-resolved SID enables accurate determination of energy and entropy effects in the dissociation process. It has been demonstrated that entropy effects play an important role in determining the dissociation rates of both covalent and non-covalent bonds in large gaseous ions. SID studies have provided important insights on the competition between charge-directed and charge-remote fragmentation in even-electron peptide ions and the role of charge and radical site on the energetics of the dissociation of odd-electron peptide ions. Furthermore, this work examined factors that affect the strength of non-covalent binding, as well as the competition between covalent and non-covalent bond cleavages and between proton and electron transfer in model systems. Finally, SID studies have been used to understand the factors affecting nucleation and growth of clusters in solution and the gas phase.« less

Charging of moving surfaces by corona discharges sustained in air

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Jun-Chieh, E-mail: junchwan@umich.edu; Kushner, Mark J., E-mail: mjkush@umich.edu; Zhang, Daihua, E-mail: dhzhang@tju.edu.cn

Atmospheric pressure corona discharges are used in electrophotographic (EP) printing technologies for charging imaging surfaces such as photoconductors. A typical corona discharge consists of a wire (or wire array) biased with a few hundred volts of dc plus a few kV of ac voltage. An electric discharge is produced around the corona wire from which electrons drift towards and charge the underlying dielectric surface. The surface charging reduces the voltage drop across the gap between the corona wire and the dielectric surface, which then terminates the discharge, as in a dielectric barrier discharge. In printing applications, this underlying surface ismore » continuously moving throughout the charging process. For example, previously charged surfaces, which had reduced the local electric field and terminated the local discharge, are translated out of the field of view and are replaced with uncharged surface. The uncharged surface produces a rebound in the electric field in the vicinity of the corona wire which in turn results in re-ignition of the discharge. The discharge, so reignited, is then asymmetric. We found that in the idealized corona charging system we investigated, a negatively dc biased corona blade with a dielectric covered ground electrode, the discharge is initially sustained by electron impact ionization from the bulk plasma and then dominated by ionization from sheath accelerated secondary electrons. Depending on the speed of the underlying surface, the periodic re-ignition of the discharge can produce an oscillatory charging pattern on the moving surface.« less

Adsorption of insulin peptide on charged single-walled carbon nanotubes: significant role of ordered water molecules.

PubMed

Shen, Jia-Wei; Wu, Tao; Wang, Qi; Kang, Yu; Chen, Xin

2009-06-02

Ordered hydration shells: The more ordered hydration shells outside the charged CNT surfaces prevent more compact adsorption of the peptide in the charged CNT systems [picture: see text], but peptide binding strengths on the charged CNT surfaces are stronger due to the electrostatic interaction.Studies of adsorption dynamics and stability for peptides/proteins on single-walled carbon nanotubes (SWNTs) are of great importance for a better understanding of the properties and nature of nanotube-based biosystems. Herein, the dynamics and mechanism of the adsorption of the insulin chain B peptide on different charged SWNTs are investigated by explicit solvent molecular dynamics simulations. The results show that all types of surfaces effectively attract the model peptide. Water molecules play a significant role in peptide adsorption on the surfaces of charged carbon nanotubes (CNTs). Compared to peptide adsorption on neutral CNT surfaces, the more ordered hydration shells outside the tube prevent more compact adsorption of the peptide in charged CNT systems. This shield effect leads to a smaller conformational change and van der Waals interaction between the peptide and surfaces, but peptide binding strengths on charged CNT surfaces are stronger than those on the neutral CNT surface due to the strong electrostatic interaction. The result of these simulations implies the possibility of improving the binding strength of peptides/proteins on CNT surfaces, as well as keeping the integrity of the peptide/protein conformation in peptide/protein-CNT complexes by charging the CNTs.

Effect of surface charge density on the affinity of oxide nanoparticles for the vapor-water interface.

PubMed

Brown, Matthew A; Duyckaerts, Nicolas; Redondo, Amaia Beloqui; Jordan, Inga; Nolting, Frithjof; Kleibert, Armin; Ammann, Markus; Wörner, Hans Jakob; van Bokhoven, Jeroen A; Abbas, Zareen

2013-04-23

Using in-situ X-ray photoelectron spectroscopy at the vapor-water interface, the affinity of nanometer-sized silica colloids to adsorb at the interface is shown to depend on colloid surface charge density. In aqueous suspensions at pH 10 corrected Debye-Hückel theory for surface complexation calculations predict that smaller silica colloids have increased negative surface charge density that originates from enhanced screening of deprotonated silanol groups (≡Si-O(-)) by counterions in the condensed ion layer. The increased negative surface charge density results in an electrostatic repulsion from the vapor-water interface that is seen to a lesser extent for larger particles that have a reduced charge density in the XPS measurements. We compare the results and interpretation of the in-situ XPS and corrected Debye-Hückel theory for surface complexation calculations with traditional surface tension measurements. Our results show that controlling the surface charge density of colloid particles can regulate their adsorption to the interface between two dielectrics.

The effect of surface charge, negative and bipolar ionization on the deposition of airborne bacteria.

PubMed

Meschke, S; Smith, B D; Yost, M; Miksch, R R; Gefter, P; Gehlke, S; Halpin, H A

2009-04-01

A series of experiments were conducted to evaluate the effect of surface charge and air ionization on the deposition of airborne bacteria. The interaction between surface electrostatic potential and the deposition of airborne bacteria in an indoor environment was investigated using settle plates charged with electric potentials of 0, +/-2.5kV and +/-5kV. Results showed that bacterial deposition on the plates increased proportionally with increased potential to over twice the gravitational sedimentation rate at +5kV. Experiments were repeated under similar conditions in the presence of either negative or bipolar air ionization. Bipolar air ionization resulted in reduction of bacterial deposition onto the charged surfaces to levels nearly equal to gravitational sedimentation. In contrast, diffusion charging appears to have occurred during negative air ionization, resulting in an even greater deposition onto the oppositely charged surface than observed without ionization. Static charges on fomitic surfaces may attract bacteria resulting in deposition in excess of that expected by gravitational sedimentation or simple diffusion. Implementation of bipolar ionization may result in reduction of bacterial deposition. Fomitic surfaces are important vehicles for the transmission of infectious organisms. This study has demonstrated a simple strategy for minimizing charge related deposition of bacteria on surfaces.

14 CFR § 1215.113 - User charges.

Code of Federal Regulations, 2014 CFR

2014-01-01

... 14 Aeronautics and Space 5 2014-01-01 2014-01-01 false User charges. § 1215.113 Section § 1215.113 Aeronautics and Space NATIONAL AERONAUTICS AND SPACE ADMINISTRATION TRACKING AND DATA RELAY.... (a) The user shall reimburse NASA the sum of the charges for standard and mission-unique services...

The role of electrostatic charge in the adhesion of spherical particles onto planar surfaces in atmospheric systems

DOE PAGES

Kweon, Hyojin; Yiacoumi, Sotira Z.; Tsouris, Costas

2015-06-19

In this study, the influence of electrostatic charge on the adhesive force between spherical particles and planar surfaces in atmospheric systems was studied using atomic force microscopy. Electrical bias was applied to modify the surface charge, and it was found that application of a stronger positive bias to a particle induces a stronger total adhesive force. The sensitivity of the system to changes in the bias depended on the surface charge density. For larger-size particles, the contribution of the electrostatic force decreased, and the capillary force became the major contributor to the total adhesive force. The influence of water adsorptionmore » on the total adhesive force and, specifically, on the contribution of the electrostatic force depended on the hydrophobicity of interacting surfaces. For a hydrophilic surface, water adsorption either attenuated the surface charge or screened the effect of surface potential. An excessive amount of adsorbed water provided a path to surface charge leakage, which might cancel out the electrostatic force, leading to a reduction in the adhesive force. Theoretically calculated forces were comparable with measured adhesive forces except for mica which has a highly localized surface potential. The results of this study provide information on the behavior of charged colloidal particles in atmospheric systems.« less

Altering surface charge nonuniformity on individual colloidal particles.

PubMed

Feick, Jason D; Chukwumah, Nkiru; Noel, Alexandra E; Velegol, Darrell

2004-04-13

Charge nonuniformity (sigmazeta) was altered on individual polystyrene latex particles and measured using the novel experimental technique of rotational electrophoresis. It has recently been shown that unaltered sulfated latices often have significant charge nonuniformity (sigmazeta = 100 mV) on individual particles. Here it is shown that anionic polyelectrolytes and surfactants reduce the native charge nonuniformity on negatively charged particles by 80% (sigmazeta = 20 mV), even while leaving the average surface charge density almost unchanged. Reduction of charge uniformity occurs as large domains of nonuniformity are minimized, giving a more random distribution of charge on individual particle surfaces. Targeted reduction of charge nonuniformity opens new opportunities for the dispersion of nanoparticles and the oriented assembly of particles.

Lateral Charge Transport in Silicon Nanomembranes

NASA Astrophysics Data System (ADS)

Hu, Weiwei

Silicon nanomembranes, also called SiNMs, Si thin sheets or films, are a great platform to study surface sciences, since the bulk is diminished and the surface-to-volume ratio is large. In a single crystalline material, atoms on the surface experience different forces, electric fields, thermodynamic surroundings, etc., than those within the bulk. Therefore, unique structural, mechanical, electronic, optical, and many other properties associated with surfaces overweigh bulk effects; novel phenomena emerge. In particular, electronic features of Si are of significance due to the extensive use of Si in integrated circuit devices and biochemical sensor technologies. As a result, especially with the size of transistors quickly decreasing nowadays, the exploration of electronic characteristics of Si surfaces become much more significant. This is also interesting as a topic within the area of fundamental surface science. Silicon-on-insulator (SOI) provides a new structure for studying charge transport in the SiNM, which is monocrystalline and sits on top of the SOI wafer. I use SOI based SiNMs with two surface orientations: Si (001) and Si (111). The former is pervasive in industrial applications while the latter has interesting metallic surface states when 7x7 reconstruction occurs on a clean surface. My goal is to measure/infer the sheet conductance in the true surface layer with different surface situations, and to further investigate the surface band structure and how carriers distribute and move accordingly. The biggest challenge is to eliminate interferences, e.g., bulk effects. The following are two solutions. 1) The thickness of the used SiNMs spans 40 nm to 500 nm, with a nominal doping level of 1015 cm -3 in our experiment. A straightforward calculation of areal dopant density indicates that charge carriers from the extrinsic doping are 1˜2 orders of magnitude fewer than the trap states at the interface between the buried oxide in SOI and the top SiNM, meaning that moderate doping is irrelevant and the SiNM acts like an intrinsic one. 2) The back gate that is applied to the measured sample is an innovative design among myriad analogous studies. It enables the tuning of the Fermi level (EF) throughout the SiNMs and makes it possible for a membrane to reach its most depleted status, thus efficiently removing the bulk conduction path. The four-probe van der Pauw measurements of film conductance are taken inside an ultrahigh vacuum chamber, where the surface condition remains stable and controllable. On Si (111) 7x7 surfaces, we find from the independence of conductance on membrane thickness that we are measuring the surface transport only. The sheet conductance is high, as it is on the microS/□scale, which supports the 7x7 surface having metallicity in lateral charge transport, a point which has been debated extensively. Nevertheless, weak semiconductor behavior is still present. For hydrogenated Si (001), which is obtained after hydrogen fluoric acid (HF) treatment, surface Fermi level is found around mid-bandgap based on temperature dependent measurements. No surface Fermi level pinning to closely below the conduction band minimum exists in my HF treated Si (001) NMs.

Mechanism of the free charge carrier generation in the dielectric breakdown

NASA Astrophysics Data System (ADS)

Rahim, N. A. A.; Ranom, R.; Zainuddin, H.

2017-12-01

Many studies have been conducted to investigate the effect of environmental, mechanical and electrical stresses on insulator. However, studies on physical process of discharge phenomenon, leading to the breakdown of the insulator surface are lacking and difficult to comprehend. Therefore, this paper analysed charge carrier generation mechanism that can cause free charge carrier generation, leading toward surface discharge development. Besides, this paper developed a model of surface discharge based on the charge generation mechanism on the outdoor insulator. Nernst’s Planck theory was used in order to model the behaviour of the charge carriers while Poisson’s equation was used to determine the distribution of electric field on insulator surface. In the modelling of surface discharge on the outdoor insulator, electric field dependent molecular ionization was used as the charge generation mechanism. A mathematical model of the surface discharge was solved using method of line technique (MOL). The result from the mathematical model showed that the behaviour of net space charge density was correlated with the electric field distribution.

Structural characterization of a unique marine animal family 7 cellobiohydrolase suggests a mechanism of cellulase salt tolerance.

PubMed

Kern, Marcelo; McGeehan, John E; Streeter, Simon D; Martin, Richard N A; Besser, Katrin; Elias, Luisa; Eborall, Will; Malyon, Graham P; Payne, Christina M; Himmel, Michael E; Schnorr, Kirk; Beckham, Gregg T; Cragg, Simon M; Bruce, Neil C; McQueen-Mason, Simon J

2013-06-18

Nature uses a diversity of glycoside hydrolase (GH) enzymes to convert polysaccharides to sugars. As lignocellulosic biomass deconstruction for biofuel production remains costly, natural GH diversity offers a starting point for developing industrial enzymes, and fungal GH family 7 (GH7) cellobiohydrolases, in particular, provide significant hydrolytic potential in industrial mixtures. Recently, GH7 enzymes have been found in other kingdoms of life besides fungi, including in animals and protists. Here, we describe the in vivo spatial expression distribution, properties, and structure of a unique endogenous GH7 cellulase from an animal, the marine wood borer Limnoria quadripunctata (LqCel7B). RT-quantitative PCR and Western blot studies show that LqCel7B is expressed in the hepatopancreas and secreted into the gut for wood degradation. We produced recombinant LqCel7B, with which we demonstrate that LqCel7B is a cellobiohydrolase and obtained four high-resolution crystal structures. Based on a crystallographic and computational comparison of LqCel7B to the well-characterized Hypocrea jecorina GH7 cellobiohydrolase, LqCel7B exhibits an extended substrate-binding motif at the tunnel entrance, which may aid in substrate acquisition and processivity. Interestingly, LqCel7B exhibits striking surface charges relative to fungal GH7 enzymes, which likely results from evolution in marine environments. We demonstrate that LqCel7B stability and activity remain unchanged, or increase at high salt concentration, and that the L. quadripunctata GH mixture generally contains cellulolytic enzymes with highly acidic surface charge compared with enzymes derived from terrestrial microbes. Overall, this study suggests that marine cellulases offer significant potential for utilization in high-solids industrial biomass conversion processes.

Structural characterization of a unique marine animal family 7 cellobiohydrolase suggests a mechanism of cellulase salt tolerance

PubMed Central

Kern, Marcelo; McGeehan, John E.; Streeter, Simon D.; Martin, Richard N. A.; Besser, Katrin; Elias, Luisa; Eborall, Will; Malyon, Graham P.; Payne, Christina M.; Himmel, Michael E.; Schnorr, Kirk; Beckham, Gregg T.; Cragg, Simon M.; Bruce, Neil C.; McQueen-Mason, Simon J.

2013-01-01

Nature uses a diversity of glycoside hydrolase (GH) enzymes to convert polysaccharides to sugars. As lignocellulosic biomass deconstruction for biofuel production remains costly, natural GH diversity offers a starting point for developing industrial enzymes, and fungal GH family 7 (GH7) cellobiohydrolases, in particular, provide significant hydrolytic potential in industrial mixtures. Recently, GH7 enzymes have been found in other kingdoms of life besides fungi, including in animals and protists. Here, we describe the in vivo spatial expression distribution, properties, and structure of a unique endogenous GH7 cellulase from an animal, the marine wood borer Limnoria quadripunctata (LqCel7B). RT-quantitative PCR and Western blot studies show that LqCel7B is expressed in the hepatopancreas and secreted into the gut for wood degradation. We produced recombinant LqCel7B, with which we demonstrate that LqCel7B is a cellobiohydrolase and obtained four high-resolution crystal structures. Based on a crystallographic and computational comparison of LqCel7B to the well-characterized Hypocrea jecorina GH7 cellobiohydrolase, LqCel7B exhibits an extended substrate-binding motif at the tunnel entrance, which may aid in substrate acquisition and processivity. Interestingly, LqCel7B exhibits striking surface charges relative to fungal GH7 enzymes, which likely results from evolution in marine environments. We demonstrate that LqCel7B stability and activity remain unchanged, or increase at high salt concentration, and that the L. quadripunctata GH mixture generally contains cellulolytic enzymes with highly acidic surface charge compared with enzymes derived from terrestrial microbes. Overall, this study suggests that marine cellulases offer significant potential for utilization in high-solids industrial biomass conversion processes. PMID:23733951

Collisional charging of individual submillimeter particles: Using ultrasonic levitation to initiate and track charge transfer

NASA Astrophysics Data System (ADS)

Lee, Victor; James, Nicole M.; Waitukaitis, Scott R.; Jaeger, Heinrich M.

2018-03-01

Electrostatic charging of insulating fine particles can be responsible for numerous phenomena ranging from lightning in volcanic plumes to dust explosions. However, even basic aspects of how fine particles become charged are still unclear. Studying particle charging is challenging because it usually involves the complexities associated with many-particle collisions. To address these issues, we introduce a method based on acoustic levitation, which makes it possible to initiate sequences of repeated collisions of a single submillimeter particle with a flat plate, and to precisely measure the particle charge in situ after each collision. We show that collisional charge transfer between insulators is dependent on the hydrophobicity of the contacting surfaces. We use glass, which we modify by attaching nonpolar molecules to the particle, the plate, or both. We find that hydrophilic surfaces develop significant positive charges after contacting hydrophobic surfaces. Moreover, we demonstrate that charging between a hydrophilic and a hydrophobic surface is suppressed in an acidic environment and enhanced in a basic one. Application of an electric field during each collision is found to modify the charge transfer, again depending on surface hydrophobicity. We discuss these results within the context of contact charging due to ion transfer, and we show that they lend strong support to O H- ions as the charge carriers.

Label-free specific detection of femtomolar cardiac troponin using an integrated nanoslit array fluidic diode.

PubMed

Liu, Yifan; Yobas, Levent

2014-12-10

We demonstrate here for the first time the utility of an integrated nanofluidic diode for detecting and quantifying physiologically relevant macromolecules. Troponin T, a key human cardiac protein biomarker, was selectively and rapidly detected free of labels for concentrations down to 10 fg/mL (∼ 0.3 fM) in buffer as well as 10 pg/mL (∼ 300 fM) in untreated human serum. This ultrasensitive detection arises from monolithic integration of a unique nanofluidic diode structure that is highly robust and amenable to site-specific surface modification. The structure features a planar nanoslit array where each nanoslit is defined at a nominal width of 70 nm over a micrometer-scale silicon trench without the use of high-resolution patterning techniques. Through vapor deposition, a glass layer is placed at a nonuniform thickness, tapering the trench profile upward and contributing to the triangular nanoslit structure. This asymmetric profile is essential for ionic current rectification noted here at various pH values, ionic strengths, and captured target species, which modulate the surface-charge density within the sensitive region of the nanoslit. The nanoslit, unlike nanopores, offers only 1D confinement, which appears to be adequate for reasonable rectification. The measurements are found in quantitative agreement with the diode simulations for the first time based on a pH- and salt-dependent surface-charge model.

Structural Insights into the Unusually Strong ATPase Activity of the AAA Domain of the Caenorhabditis elegans Fidgetin-like 1 (FIGL-1) Protein*

PubMed Central

Peng, Wentao; Lin, Zhijie; Li, Weirong; Lu, Jing; Shen, Yuequan; Wang, Chunguang

2013-01-01

The FIGL-1 (fidgetin like-1) protein is a homolog of fidgetin, a protein whose mutation leads to multiple developmental defects. The FIGL-1 protein contains an AAA (ATPase associated with various activities) domain and belongs to the AAA superfamily. However, the biological functions and developmental implications of this protein remain unknown. Here, we show that the AAA domain of the Caenorhabditis elegans FIGL-1 protein (CeFIGL-1-AAA), in clear contrast to homologous AAA domains, has an unusually high ATPase activity and forms a hexamer in solution. By determining the crystal structure of CeFIGL-1-AAA, we found that the loop linking helices α9 and α10 folds into the short helix α9a, which has an acidic surface and interacts with a positively charged surface of the neighboring subunit. Disruption of this charge interaction by mutagenesis diminishes both the ATPase activity and oligomerization capacity of the protein. Interestingly, the acidic residues in helix α9a of CeFIGL-1-AAA are not conserved in other homologous AAA domains that have relatively low ATPase activities. These results demonstrate that the sequence of CeFIGL-1-AAA has adapted to establish an intersubunit charge interaction, which contributes to its strong oligomerization and ATPase activity. These unique properties of CeFIGL-1-AAA distinguish it from other homologous proteins, suggesting that CeFIGL-1 may have a distinct biological function. PMID:23979136

Structural insights into the unusually strong ATPase activity of the AAA domain of the Caenorhabditis elegans fidgetin-like 1 (FIGL-1) protein.

PubMed

Peng, Wentao; Lin, Zhijie; Li, Weirong; Lu, Jing; Shen, Yuequan; Wang, Chunguang

2013-10-11

The FIGL-1 (fidgetin like-1) protein is a homolog of fidgetin, a protein whose mutation leads to multiple developmental defects. The FIGL-1 protein contains an AAA (ATPase associated with various activities) domain and belongs to the AAA superfamily. However, the biological functions and developmental implications of this protein remain unknown. Here, we show that the AAA domain of the Caenorhabditis elegans FIGL-1 protein (CeFIGL-1-AAA), in clear contrast to homologous AAA domains, has an unusually high ATPase activity and forms a hexamer in solution. By determining the crystal structure of CeFIGL-1-AAA, we found that the loop linking helices α9 and α10 folds into the short helix α9a, which has an acidic surface and interacts with a positively charged surface of the neighboring subunit. Disruption of this charge interaction by mutagenesis diminishes both the ATPase activity and oligomerization capacity of the protein. Interestingly, the acidic residues in helix α9a of CeFIGL-1-AAA are not conserved in other homologous AAA domains that have relatively low ATPase activities. These results demonstrate that the sequence of CeFIGL-1-AAA has adapted to establish an intersubunit charge interaction, which contributes to its strong oligomerization and ATPase activity. These unique properties of CeFIGL-1-AAA distinguish it from other homologous proteins, suggesting that CeFIGL-1 may have a distinct biological function.

A Combined Model of Charging of the Surface and Bulk of a Dielectric Target by Electrons with the Energies 10-30 keV

NASA Astrophysics Data System (ADS)

Zykov, V. M.; Neiman, D. A.

2018-04-01

A physico-mathematical model of the processes of radiation-induced charging of dielectric materials with open surfaces, irradiated with monoenergetic electrons in the energy range 10-30 keV, is described. The model takes into account the relationship between the processes of surface and bulk charging for the given conditions of the experimental design, which accounts for the effect of anomalously long charging of dielectrics after the incident energy of primary electrons during charging is reduced to below the second critical energy for the secondary electronic emission coefficient. The initial fast phase of charging a high-resistivity dielectric material (Al2O3) is investigated. It is shown that as the incident electron energy is approaching the second critical energy during charging, the secondary electronic emission is partially suppressed due to negative charging of the open surface of the dielectric and formation of a near-surface inversion electrical field retarding the electronic emission yield.

Ion association at discretely-charged dielectric interfaces: Giant charge inversion

NASA Astrophysics Data System (ADS)

Wang, Zhi-Yong; Wu, Jianzhong

2017-07-01

Giant charge reversal has been identified for the first time by Monte Carlo simulation for a discretely charged surface in contact with a trivalent electrolyte solution. It takes place regardless of the surface charge density under study and the monovalent salt. In stark contrast to earlier predictions based on the 2-dimensional Wigner crystal model to describe strong correlation of counterions at the macroion surface, we find that giant charge reversal reflects an intricate interplay of ionic volume effects, electrostatic correlations, surface charge heterogeneity, and the dielectric response of the confined fluids. While the novel phenomenon is yet to be confirmed with experiment, the simulation results appear in excellent agreement with a wide range of existing observations in the subregime of charge inversion. Our findings may have far-reaching implications to understanding complex electrochemical phenomena entailing ionic fluids under dielectric confinements.

VARIABLE CHARGE SOILS: MINERALOGY AND CHEMISTRY

DOE Office of Scientific and Technical Information (OSTI.GOV)

Van Ranst, Eric; Qafoku, Nikolla; Noble, Andrew

2016-09-19

Soils rich in particles with amphoteric surface properties in the Oxisols, Ultisols, Alfisols, Spodosols and Andisols orders (1) are considered to be variable charge soils (2) (Table 1). The term “variable charge” is used to describe organic and inorganic soil constituents with reactive surface groups whose charge varies with pH and ionic concentration and composition of the soil solution. Such groups are the surface carboxyl, phenolic and amino functional groups of organic materials in soils, and surface hydroxyl groups of Fe and Al oxides, allophane and imogolite. The hydroxyl surface groups are also present on edges of some phyllosilicate mineralsmore » such as kaolinite, mica, and hydroxyl-interlayered vermiculite. The variable charge is developed on the surface groups as a result of adsorption or desorption of ions that are constituents of the solid phase, i.e., H+, and the adsorption or desorption of solid-unlike ions that are not constituents of the solid phase. Highly weathered soils and subsoils (e.g., Oxisols and some Ultisols, Alfisols and Andisols) may undergo isoelectric weathering and reach a “zero net charge” stage during their development. They usually have a slightly acidic to acidic soil solution pH, which is close to either the point of zero net charge (PZNC) (3) or the point of zero salt effect (PZSE) (3). They are characterized by high abundances of minerals with a point of zero net proton charge (PZNPC) (3) at neutral and slightly basic pHs; the most important being Fe and Al oxides and allophane. Under acidic conditions, the surfaces of these minerals are net positively charged. In contrast, the surfaces of permanent charge phyllosilicates are negatively charged regardless of ambient conditions. Variable charge soils therefore, are heterogeneous charge systems.« less

Water organization between oppositely charged surfaces: Implications for protein sliding along DNA a)

NASA Astrophysics Data System (ADS)

Marcovitz, Amir; Naftaly, Aviv; Levy, Yaakov

2015-02-01

Water molecules are abundant in protein-DNA interfaces, especially in their nonspecific complexes. In this study, we investigated the organization and energetics of the interfacial water by simplifying the geometries of the proteins and the DNA to represent them as two equally and oppositely charged planar surfaces immersed in water. We found that the potential of mean force for bringing the two parallel surfaces into close proximity comprises energetic barriers whose properties strongly depend on the charge density of the surfaces. We demonstrated how the organization of the water molecules into discretized layers and the corresponding energetic barriers to dehydration can be modulated by the charge density on the surfaces, salt, and the structure of the surfaces. The 1-2 layers of ordered water are tightly bound to the charged surfaces representing the nonspecific protein-DNA complex. This suggests that water might mediate one-dimensional diffusion of proteins along DNA (sliding) by screening attractive electrostatic interactions between the positively charged molecular surface on the protein and the negatively charged DNA backbone and, in doing so, reduce intermolecular friction in a manner that smoothens the energetic landscape for sliding, and facilitates the 1D diffusion of the protein.

Characterizing the effects of regolith surface roughness on photoemission from surfaces in space

NASA Astrophysics Data System (ADS)

Dove, A.; Horanyi, M.; Wang, X.

2017-12-01

Surfaces of airless bodies and spacecraft in space are exposed to a variety of charging environments. A balance of currents due to plasma bombardment, photoemission, electron and ion emission and collection, and secondary electron emission determines the surface's charge. Photoelectron emission is the dominant charging process on sunlit surfaces in the inner solar system due to the intense solar UV radiation. This can result in a net positive surface potential, with a cloud of photoelectrons immediately above the surface, called the photoelectron sheath. Conversely, the unlit side of the body will charge negatively due the collection of the fast-moving solar wind electrons. The interaction of charged dust grains with these positively and negatively charged surfaces, and within the photoelectron and plasma sheaths may explain the occurrence of dust lofting, levitation and transport above the lunar surface. The surface potential of exposed objects is also dependent on the material properties of their surfaces. Composition and particle size primarily affect the quantum efficiency of photoelectron generation; however, surface roughness can also control the charging process. In order to characterize these effects, we have conducted laboratory experiments to examine the role of surface roughness in generating photoelectrons in dedicated laboratory experiments using solid and dusty surfaces of the same composition (CeO2), and initial comparisons with JSC-1 lunar simulant. Using Langmuir probe measurements, we explore the measured potentials above insulating surfaces exposed to UV and an electric field, and we show that the photoemission current from a dusty surface is largely reduced due to its higher surface roughness, which causes a significant fraction of the emitted photoelectrons to be re-absorbed within the surface. We will discuss these results in context of similar situations on planetary surfaces.

Space and surface charge behavior analysis of charge-eliminated polymer films

DOE Office of Scientific and Technical Information (OSTI.GOV)

Oda, Tetsuji; Takashima, Kazunori; Ichiyama, Shinichiro

1995-12-31

Charge behavior of corona-charged or charge eliminated polymer films being dipped in the city water were studied. They were polytetrafluoroethylene (PTFE teflon{trademark}), polypropylene (PP), low density or high density polyethylene (LDPE or HDPE) thin films which are as grown (native) or plasma-processed. The plasma processing at low pressure was tested as antistatic processing. Charge elimination was done by being dipped in alcohol or city water. TSDC analysis and surface charge profile measurement were done for both charged and charge eliminated polymer films. Surface charge density of plasma processed polymer films just after corona charging is roughly the same as thatmore » of an original film. There is little difference between surface charge density profile of a native film and that of a plasma processed film. A large hetero current peak of TSDC was observed at room temperature for a processed film. It was found that the hetero peak disappears after charge elimination process. A pressure pulse wave method by using a pulse-driven piezoelectric PVDF polymer film as a piezoelectric actuator was newly developed to observe real space charge distribution. A little difference of internal space charge distribution between the plasma processed film and the native one after corona charging is found.« less

Ordered adsorption of coagulation factor XII on negatively charged polymer surfaces probed by sum frequency generation vibrational spectroscopy.

PubMed

Chen, Xiaoyun; Wang, Jie; Paszti, Zoltan; Wang, Fulin; Schrauben, Joel N; Tarabara, Volodymyr V; Schmaier, Alvin H; Chen, Zhan

2007-05-01

Electrostatic interactions between negatively charged polymer surfaces and factor XII (FXII), a blood coagulation factor, were investigated by sum frequency generation (SFG) vibrational spectroscopy, supplemented by several analytical techniques including attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR), quartz crystal microbalance (QCM), zeta-potential measurement, and chromogenic assay. A series of sulfonated polystyrenes (sPS) with different sulfonation levels were synthesized as model surfaces with different surface charge densities. SFG spectra collected from FXII adsorbed onto PS and sPS surfaces with different surface charge densities showed remarkable differences in spectral features and especially in spectral intensity. Chromogenic assay experiments showed that highly charged sPS surfaces induced FXII autoactivation. ATR-FTIR and QCM results indicated that adsorption amounts on the PS and sPS surfaces were similar even though the surface charge densities were different. No significant conformational change was observed from FXII adsorbed onto surfaces studied. Using theoretical calculations, the possible contribution from the third-order nonlinear optical effect induced by the surface electric field was evaluated, and it was found to be unable to yield the SFG signal enhancement observed. Therefore it was concluded that the adsorbed FXII orientation and ordering were the main reasons for the remarkable SFG amide I signal increase on sPS surfaces. These investigations indicate that negatively charged surfaces facilitate or induce FXII autoactivation on the molecular level by imposing specific orientation and ordering on the adsorbed protein molecules.

Colloidal lithography with electrochemical nickel deposition as a unique method for improved silver decorated nanocavities in SERS applications

NASA Astrophysics Data System (ADS)

Petruš, Ondrej; Oriňak, Andrej; Oriňaková, Renáta; Orságová Králová, Zuzana; Múdra, Erika; Kupková, Miriam; Kovaľ, Karol

2017-11-01

Two types of metallised nanocavities (single and hybrid) were fabricated by colloid lithography followed by electrochemical deposition of Ni and subsequently Ag layers. Introductory Ni deposition step iniciates more homogenous decoration of nanocavities with Ag nanoparticles. Silver nanocavity decoration has been so performed with lower nucleation rate and with Ag nanoparticles homogeinity increase. By this, two step Ni and Ag deposition trough polystyrene nanospheres (100, 300, 500, 700, 900 nm), the various Ag surfaces were obtained. Ni layer formation in the first step of deposition enabled more precise controlling of Ag film deposition and thus final Ag surface morphology. Prepared substrates were tested as active surfaces in SERS application. The best SERS signal enhancement was observed at 500 nm Ag nanocavities with normalised thickness Ni layer ∼0.5. Enhancement factor has been established at value 1.078 × 1010; time stability was determined within 13 weeks; charge distribution at nanocavity Ag surfaces as well as reflection spectra were calculated by FDTD method. Newly prepared nanocavity surface can be applied in SERS analysis, predominantly.

Polymorphism and metal-induced structural transformation in 5,5'-bis(4-pyridyl)(2,2'-bispyrimidine) adlayers on Au(111).

PubMed

Hötger, Diana; Carro, Pilar; Gutzler, Rico; Wurster, Benjamin; Chandrasekar, Rajadurai; Klyatskaya, Svetlana; Ruben, Mario; Salvarezza, Roberto C; Kern, Klaus; Grumelli, Doris

2018-05-31

Metal-organic coordination networks self-assembled on surfaces have emerged as functional low-dimensional architectures with potential applications ranging from the fabrication of functional nanodevices to electrocatalysis. Among them, bis-pyridyl-bispyrimidine (PBP) and Fe-PBP on noble metal surfaces appear as interesting systems in revealing the details of the molecular self-assembly and the effect of metal incorporation on the organic network arrangement. Herein, we report a combined STM, XPS, and DFT study revealing polymorphism in bis-pyridyl-bispyrimidine adsorbed adlayers on the reconstructed Au(111) surface. The polymorphic structures are converted by the addition of Fe adatoms into one unique Fe-PBP surface structure. DFT calculations show that while all PBP phases exhibit a similar thermodynamic stability, metal incorporation selects the PBP structure that maximizes the number of metal-N close contacts. Charge transfer from the Fe adatoms to the Au substrate and N-Fe interactions stabilize the Fe-PBP adlayer. The increased thermodynamic stability of the metal-stabilized structure leads to its sole expression on the surface.

Influence of non-adherent yeast cells on electrical characteristics of diamond-based field-effect transistors

NASA Astrophysics Data System (ADS)

Procházka, Václav; Cifra, Michal; Kulha, Pavel; Ižák, Tibor; Rezek, Bohuslav; Kromka, Alexander

2017-02-01

Diamond thin films provide unique features as substrates for cell cultures and as bio-electronic sensors. Here we employ solution-gated field effect transistors (SGFET) based on nanocrystalline diamond thin films with H-terminated surface which exhibits the sub-surface p-type conductive channel. We study an influence of yeast cells (Saccharomyces cerevisiae) on electrical characteristics of the diamond SGFETs. Two different cell culture solutions (sucrose and yeast peptone dextrose-YPD) are used, with and without the cells. We have found that transfer characteristics of the SGFETs exhibit a negative shift of the gate voltage by -26 mV and -42 mV for sucrose and YPD with cells in comparison to blank solutions without the cells. This effect is attributed to a local pH change in close vicinity of the H-terminated diamond surface due to metabolic processes of the yeast cells. The pH sensitivity of the diamond-based SGFETs, the role of cell and protein adhesion on the gate surface and the role of negative surface charge of yeast cells on the SGFETs electrical characteristics are discussed as well.

Photosystem I assembly on chemically tailored SAM/ Au substrates for bio-hybrid device fabrication

NASA Astrophysics Data System (ADS)

Mukherjee, Dibyendu; Khomami, Bamin

2011-03-01

Photosystem I (PS I), a supra-molecular protein complex and a biological photodiode responsible for driving natural photosynthesis mechanism, charge separates upon exposure to light. Effective use of the photo-electrochemical activities of PS I for future bio-hybrid electronic devices requires controlled attachment of these proteins onto organic/ inorganic substrates. Our results indicate that various experimental parameters alter the surface topography of PS I deposited from colloidal aqueous buffer suspensions onto OH-terminated alkanethiolate SAM /Au substrates, thereby resulting in complex columnar structures that affect the electron capture pathway of PS I. Specifically, solution phase characterizations indicate that specific detergents used for PS I stabilization in buffer solutions drive the unique colloidal chemistry to tune protein-protein interactions and prevent aggregation, thereby allowing us to tailor the morphology of surface immobilized PS I. We present surface topographical, adsorption, and electrochemical characterizations of PSI /SAM/Au substrates to elucidate protein-surface attachment dynamics and its effect on the photo-activated electronic activities of surface immobilized PS I. Sustainable Energy Education and Research Center (SEERC).

Experimental and Theoretical Investigations of Glass Surface Charging Phenomena

NASA Astrophysics Data System (ADS)

Agnello, Gabriel

Charging behavior of multi-component display-type (i.e. low alkali) glass surfaces has been studied using a combination of experimental and theoretical methods. Data obtained by way of a Rolling Sphere Test (RST), streaming/zeta potential and surface energy measurements from commercially available display glass surfaces (Corning EAGLE XGRTM and Lotus(TM) XT) suggest that charge accumulation is highly dependent on surface treatment (chemical and/or physical modification) and measurement environment, presumably through reactionary mechanisms at the surface with atmospheric moisture. It has been hypothesized that water dissociation, along with the corresponding hydroxylation of the glass surface, are important processes related to charging in glass-metal contact systems. Classical Molecular Dynamics (MD) simulations, in conjunction with various laboratory based measurements (RST, a newly developed ElectroStatic Gauge (ESG) and Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS)) on simpler Calcium AluminoSilicate (CAS) glass surfaces were used to further explore these phenomena. Analysis of simulated high-silica content (≥50%) (CAS) glass structures suggest that controlled variation of bulk chemistry can directly affect surface defect concentrations, such as non-bridging oxygen (NBO), which can be suitable high-energy sites for hydrolysis-type reactions to occur. Calculated NBO surface concentrations correlate well with charge based measurements on laboratory fabricated CAS surfaces. The data suggest that a directional/polar shift in contact-charge transfer occurs at low silica content (≤50%) where the highest concentrations of NBOs are observed. Surface charging sensitivity with respect to NBO concentration decreases as the relative humidity of the measurement environment increases; which should be expected as the highly reactive sites are progressively covered by liquid water layers. DRIFTS analysis of CAS powders expand on this analysis showing a gradual increase in molecular water absorption at the surface in samples containing ≥60% silica, and an abrupt decrease in those with ≤60% silica. This behavior is very likely related to the aforementioned charge polarity shift (negative (-) to positive (+)) in low silica containing glasses, leading to the conclusion that structural defect mediated charge accumulation and/or transfer are likely to be important mechanisms related to the contact charging of glass surfaces.

Structural characteristics of alkaline phosphatase from the moderately halophilic bacterium Halomonas sp. 593

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arai, Shigeki; Yonezawa, Yasushi; Ishibashi, Matsujiro

2014-03-01

In order to clarify the structural basis of the halophilic characteristics of an alkaline phosphatase derived from the moderate halophile Halomonas sp. 593 (HaAP), the tertiary structure of HaAP was determined to 2.1 Å resolution by X-ray crystallography. The structural properties of surface negative charge and core hydrophobicity were shown to be intermediate between those characteristic of halophiles and non-halophiles, and may explain the unique functional adaptation to a wide range of salt concentrations. Alkaline phosphatase (AP) from the moderate halophilic bacterium Halomonas sp. 593 (HaAP) catalyzes the hydrolysis of phosphomonoesters over a wide salt-concentration range (1–4 M NaCl). Inmore » order to clarify the structural basis of its halophilic characteristics and its wide-range adaptation to salt concentration, the tertiary structure of HaAP was determined by X-ray crystallography to 2.1 Å resolution. The unit cell of HaAP contained one dimer unit corresponding to the biological unit. The monomer structure of HaAP contains a domain comprised of an 11-stranded β-sheet core with 19 surrounding α-helices similar to those of APs from other species, and a unique ‘crown’ domain containing an extended ‘arm’ structure that participates in formation of a hydrophobic cluster at the entrance to the substrate-binding site. The HaAP structure also displays a unique distribution of negatively charged residues and hydrophobic residues in comparison to other known AP structures. AP from Vibrio sp. G15-21 (VAP; a slight halophile) has the highest similarity in sequence (70.0% identity) and structure (C{sup α} r.m.s.d. of 0.82 Å for the monomer) to HaAP. The surface of the HaAP dimer is substantially more acidic than that of the VAP dimer (144 exposed Asp/Glu residues versus 114, respectively), and thus may enable the solubility of HaAP under high-salt conditions. Conversely, the monomer unit of HaAP formed a substantially larger hydrophobic interior comprising 329 C atoms from completely buried residues, whereas that of VAP comprised 264 C atoms, which may maintain the stability of HaAP under low-salt conditions. These characteristics of HaAP may be responsible for its unique functional adaptation permitting activity over a wide range of salt concentrations.« less

Direct measurement of sub-Debye-length attraction between oppositely charged surfaces.

PubMed

Kampf, Nir; Ben-Yaakov, Dan; Andelman, David; Safran, S A; Klein, Jacob

2009-09-11

Using a surface force balance with fast video analysis, we have measured directly the attractive forces between oppositely charged solid surfaces (charge densities sigma(+), sigma(-)) across water over the entire range of interaction, in particular, at surface separations D below the Debye screening length lambda(S). At very low salt concentration we find a long-ranged attraction between the surfaces (onset ca. 100 nm), whose variation at D

Mapping surface charge density of lipid bilayers by quantitative surface conductivity microscopy

PubMed Central

Klausen, Lasse Hyldgaard; Fuhs, Thomas; Dong, Mingdong

2016-01-01

Local surface charge density of lipid membranes influences membrane–protein interactions leading to distinct functions in all living cells, and it is a vital parameter in understanding membrane-binding mechanisms, liposome design and drug delivery. Despite the significance, no method has so far been capable of mapping surface charge densities under physiologically relevant conditions. Here, we use a scanning nanopipette setup (scanning ion-conductance microscope) combined with a novel algorithm to investigate the surface conductivity near supported lipid bilayers, and we present a new approach, quantitative surface conductivity microscopy (QSCM), capable of mapping surface charge density with high-quantitative precision and nanoscale resolution. The method is validated through an extensive theoretical analysis of the ionic current at the nanopipette tip, and we demonstrate the capacity of QSCM by mapping the surface charge density of model cationic, anionic and zwitterionic lipids with results accurately matching theoretical values. PMID:27561322

Mapping surface charge density of lipid bilayers by quantitative surface conductivity microscopy

NASA Astrophysics Data System (ADS)

Klausen, Lasse Hyldgaard; Fuhs, Thomas; Dong, Mingdong

2016-08-01

Local surface charge density of lipid membranes influences membrane-protein interactions leading to distinct functions in all living cells, and it is a vital parameter in understanding membrane-binding mechanisms, liposome design and drug delivery. Despite the significance, no method has so far been capable of mapping surface charge densities under physiologically relevant conditions. Here, we use a scanning nanopipette setup (scanning ion-conductance microscope) combined with a novel algorithm to investigate the surface conductivity near supported lipid bilayers, and we present a new approach, quantitative surface conductivity microscopy (QSCM), capable of mapping surface charge density with high-quantitative precision and nanoscale resolution. The method is validated through an extensive theoretical analysis of the ionic current at the nanopipette tip, and we demonstrate the capacity of QSCM by mapping the surface charge density of model cationic, anionic and zwitterionic lipids with results accurately matching theoretical values.

Mapping surface charge density of lipid bilayers by quantitative surface conductivity microscopy.

PubMed

Klausen, Lasse Hyldgaard; Fuhs, Thomas; Dong, Mingdong

2016-08-26

Local surface charge density of lipid membranes influences membrane-protein interactions leading to distinct functions in all living cells, and it is a vital parameter in understanding membrane-binding mechanisms, liposome design and drug delivery. Despite the significance, no method has so far been capable of mapping surface charge densities under physiologically relevant conditions. Here, we use a scanning nanopipette setup (scanning ion-conductance microscope) combined with a novel algorithm to investigate the surface conductivity near supported lipid bilayers, and we present a new approach, quantitative surface conductivity microscopy (QSCM), capable of mapping surface charge density with high-quantitative precision and nanoscale resolution. The method is validated through an extensive theoretical analysis of the ionic current at the nanopipette tip, and we demonstrate the capacity of QSCM by mapping the surface charge density of model cationic, anionic and zwitterionic lipids with results accurately matching theoretical values.

Surface charges for gravity and electromagnetism in the first order formalism

NASA Astrophysics Data System (ADS)

Frodden, Ernesto; Hidalgo, Diego

2018-02-01

A new derivation of surface charges for 3  +  1 gravity coupled to electromagnetism is obtained. Gravity theory is written in the tetrad-connection variables. The general derivation starts from the Lagrangian, and uses the covariant symplectic formalism in the language of forms. For gauge theories, surface charges disentangle physical from gauge symmetries through the use of Noether identities and the exactness symmetry condition. The surface charges are quasilocal, explicitly coordinate independent, gauge invariant and background independent. For a black hole family solution, the surface charge conservation implies the first law of black hole mechanics. As a check, we show the first law for an electrically charged, rotating black hole with an asymptotically constant curvature (the Kerr–Newman (anti-)de Sitter family). The charges, including the would-be mass term appearing in the first law, are quasilocal. No reference to the asymptotic structure of the spacetime nor the boundary conditions is required and therefore topological terms do not play a rôle. Finally, surface charge formulae for Lovelock gravity coupled to electromagnetism are exhibited, generalizing the one derived in a recent work by Barnich et al Proc. Workshop ‘ About Various Kinds of Interactions’ in honour of Philippe Spindel (4–5 June 2015, Mons, Belgium) C15-06-04 (2016 (arXiv:1611.01777 [gr-qc])). The two different symplectic methods to define surface charges are compared and shown equivalent.

Direct Observation of Charge Transfer at a MgO(111) Surface

NASA Astrophysics Data System (ADS)

Subramanian, A.; Marks, L. D.; Warschkow, O.; Ellis, D. E.

2004-01-01

Transmission electron diffraction (TED) combined with direct methods have been used to study the √(3)×√(3)R30° reconstruction on the polar (111) surface of MgO and refine the valence charge distribution. The surface is nonstoichiometric and is terminated by a single magnesium atom. A charge-compensating electron hole is localized in the next oxygen layer and there is a nominal charge transfer from the oxygen atoms to the top magnesium atom. The partial charges that we obtain for the surface atoms are in reasonable agreement with empirical bond-valence estimations.

The surface charge of trypanosomatids.

PubMed

Souto-Padrón, Thaïs

2002-12-01

The surface charge of trypanosomatids was evaluated by means of the binding of cationic particles, as visualized by electron microscopy and by direct measurements of the electrophoretic mobility of cells. The results obtained indicate that most of the trypanosomatids exhibit a negatively charged surface whose value is species specific and varies according to the developmental stages. Sialic acids associated with glycoproteins, glycolipids and phosphate groups are the major components responsible for the net negative surface charge of the trypanosomatids.

Miniaturized ultrafine particle sizer and monitor

NASA Technical Reports Server (NTRS)

Qi, Chaolong (Inventor); Chen, Da-Ren (Inventor)

2011-01-01

An apparatus for measuring particle size distribution includes a charging device and a precipitator. The charging device includes a corona that generates charged ions in response to a first applied voltage, and a charger body that generates a low energy electrical field in response to a second applied voltage in order to channel the charged ions out of the charging device. The corona tip and the charger body are arranged relative to each other to direct a flow of particles through the low energy electrical field in a direction parallel to a direction in which the charged ions are channeled out of the charging device. The precipitator receives the plurality of particles from the charging device, and includes a disk having a top surface and an opposite bottom surface, wherein a predetermined voltage is applied to the top surface and the bottom surface to precipitate the plurality of particles.

Final Technical Report for the Energy Frontier Research Center Understanding Charge Separation and Transfer at Interfaces in Energy Materials (EFRC:CST)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vanden Bout, David A.

2015-09-14

Our EFRC was founded with the vision of creating a broadly collaborative and synergistic program that would lead to major breakthroughs in the molecular-level understanding of the critical interfacial charge separation and charge transfer (CST) processes that underpin the function of candidate materials for organic photovoltaic (OPV) and electrical-energy-storage (EES) applications. Research in these energy contexts shares an imposing challenge: How can we understand charge separation and transfer mechanisms in the presence of immense materials complexity that spans multiple length scales? To address this challenge, our 50-member Center undertook a total of 28 coordinated research projects aimed at unraveling themore » CST mechanisms that occur at interfaces in these nanostructured materials. This rigorous multi-year study of CST interfaces has greatly illuminated our understanding of early-timescale processes (e.g., exciton generation and dissociation dynamics at OPV heterojunctions; control of Li+-ion charging kinetics by surface chemistry) occurring in the immediate vicinity of interfaces. Program outcomes included: training of 72 graduate student and postdoctoral energy researchers at 5 institutions and spanning 7 academic disciplines in science and engineering; publication of 94 peer-reviewed journal articles; and dissemination of research outcomes via 340 conference, poster and other presentations. Major scientific outcomes included: implementation of a hierarchical strategy for understanding the electronic communication mechanisms and ultimate fate of charge carriers in bulk heterojunction OPV materials; systematic investigation of ion-coupled electron transfer processes in model Li-ion battery electrode/electrolyte systems; and the development and implementation of 14 unique technologies and instrumentation capabilities to aid in probing sub-ensemble charge separation and transfer mechanisms.« less

Method of adhesion between an oxide layer and a metal layer

DOEpatents

Jennison, Dwight R.; Bogicevic, Alexander; Kelber, Jeffry A.; Chambers, Scott A.

2004-09-14

A method of controlling the wetting characteristics and increasing the adhesion between a metal and an oxide layer. By introducing a negatively-charged species to the surface of an oxide layer, layer-by-layer growth of metal deposited onto the oxide surface is promoted, increasing the adhesion strength of the metal-oxide interface. The negatively-charged species can either be deposited onto the oxide surface or a compound can be deposited that dissociates on, or reacts with, the surface to form the negatively-charged species. The deposited metal adatoms can thereby bond laterally to the negatively-charged species as well as vertically to the oxide surface as well as react with the negatively charged species, be oxidized, and incorporated on or into the surface of the oxide.

Anion-π Catalysis on Fullerenes.

PubMed

López-Andarias, Javier; Frontera, Antonio; Matile, Stefan

2017-09-27

Anion-π interactions on fullerenes are about as poorly explored as the use of fullerenes in catalysis. However, strong exchange-correlation contributions and the localized π holes on their surface promise unique selectivities. To elaborate on this promise, tertiary amines are attached nearby. Dependent on their positioning, the resulting stabilization of anionic transition states on fullerenes is shown to accelerate disfavored enolate addition and exo Diels-Alder reactions enantioselectively. The found selectivities are consistent with computational simulations, particularly concerning the discrimination of differently planarized and charge-delocalized enolate tautomers by anion-π interactions. Enolate-π interactions on fullerenes are much shorter than standard π-π interactions and anion-π interactions on planar surfaces, and alternative cation-π interactions are not observed. These findings open new perspectives with regard to anion-π interactions in general and the use of carbon allotropes in catalysis.

Contributions of oxygen vacancies and titanium interstitials to band-gap states of reduced titania

NASA Astrophysics Data System (ADS)

Li, Jingfeng; Lazzari, Rémi; Chenot, Stéphane; Jupille, Jacques

2018-01-01

The spectroscopic fingerprints of the point defects of titanium dioxide remain highly controversial. Seemingly indisputable experiments lead to conflicting conclusions in which oxygen vacancies and titanium interstitials are alternately referred to as the primary origin of the Ti 3 d band-gap states. We report on experiments performed by electron energy loss spectroscopy whose key is the direct annealing of only the very surface of rutile TiO2(110 ) crystals and the simultaneous measurement of its temperature via the Bose-Einstein loss/gain ratio. By surface preparations involving reactions with oxygen and water vapor, in particular, under electron irradiation, vacancy- and interstitial-related band-gap states are singled out. Off-specular measurements reveal that both types of defects contribute to a unique charge distribution that peaks in subsurface layers with a common dispersive behavior.

Communication: Ion mobility of the radical cation dimers: (Naphthalene)2+• and naphthalene+•-benzene: Evidence for stacked sandwich and T-shape structures

NASA Astrophysics Data System (ADS)

Platt, Sean P.; Attah, Isaac K.; Aziz, Saadullah; El-Shall, M. Samy

2015-05-01

Dimer radical cations of aromatic and polycyclic aromatic molecules are good model systems for a fundamental understanding of photoconductivity and ferromagnetism in organic materials which depend on the degree of charge delocalization. The structures of the dimer radical cations are difficult to determine theoretically since the potential energy surface is often very flat with multiple shallow minima representing two major classes of isomers adopting the stacked parallel or the T-shape structure. We present experimental results, based on mass-selected ion mobility measurements, on the gas phase structures of the naphthalene+ṡ ṡ naphthalene homodimer and the naphthalene+ṡ ṡ benzene heterodimer radical cations at different temperatures. Ion mobility studies reveal a persistence of the stacked parallel structure of the naphthalene+ṡ ṡ naphthalene homodimer in the temperature range 230-300 K. On the other hand, the results reveal that the naphthalene+ṡ ṡ benzene heterodimer is able to exhibit both the stacked parallel and T-shape structural isomers depending on the experimental conditions. Exploitation of the unique structural motifs among charged homo- and heteroaromatic-aromatic interactions may lead to new opportunities for molecular design and recognition involving charged aromatic systems.

Method and system for treating an interior surface of a workpiece using a charged particle beam

DOEpatents

Swenson, David Richard

2007-05-23

A method and system of treating an interior surface on an internal cavity of a workpiece using a charged particle beam. A beam deflector surface of a beam deflector is placed within the internal cavity of the workpiece and is used to redirect the charged particle beam toward the interior surface to treat the interior surface.

Band gap modulation of graphene by metal substrate: A first principles study

NASA Astrophysics Data System (ADS)

Sahoo, Mihir Ranjan; Sahu, Sivabrata; Kushwaha, Anoop Kumar; Nayak, S. K.

2018-04-01

Due to high in-plane charge carrier mobility with high electron velocity and long spin diffusion length, graphene guarantees as a completely unique material for devices with various applications. Unaffected 2pz orbitals of carbon atoms in graphene can be highly influenced by substrates and leads to tuning in electronic properties. We report here a density functional calculation of graphene monolayer based on metallic substrate like nickel surfaces. Band-gap of graphene near K points opens due to interactions between 2pz and d-orbitals of nickel atoms and the gap modulation can be done with the increasing number of layers of substrates.

Metal oxide nanosensors using polymeric membranes, enzymes and antibody receptors as ion and molecular recognition elements.

PubMed

Willander, Magnus; Khun, Kimleang; Ibupoto, Zafar Hussain

2014-05-16

The concept of recognition and biofunctionality has attracted increasing interest in the fields of chemistry and material sciences. Advances in the field of nanotechnology for the synthesis of desired metal oxide nanostructures have provided a solid platform for the integration of nanoelectronic devices. These nanoelectronics-based devices have the ability to recognize molecular species of living organisms, and they have created the possibility for advanced chemical sensing functionalities with low limits of detection in the nanomolar range. In this review, various metal oxides, such as ZnO-, CuO-, and NiO-based nanosensors, are described using different methods (receptors) of functionalization for molecular and ion recognition. These functionalized metal oxide surfaces with a specific receptor involve either a complex formation between the receptor and the analyte or an electrostatic interaction during the chemical sensing of analytes. Metal oxide nanostructures are considered revolutionary nanomaterials that have a specific surface for the immobilization of biomolecules with much needed orientation, good conformation and enhanced biological activity which further improve the sensing properties of nanosensors. Metal oxide nanostructures are associated with certain unique optical, electrical and molecular characteristics in addition to unique functionalities and surface charge features which shows attractive platforms for interfacing biorecognition elements with effective transducing properties for signal amplification. There is a great opportunity in the near future for metal oxide nanostructure-based miniaturization and the development of engineering sensor devices.

Determination of molecular configuration by debye length modulation.

PubMed

Vacic, Aleksandar; Criscione, Jason M; Rajan, Nitin K; Stern, Eric; Fahmy, Tarek M; Reed, Mark A

2011-09-07

Silicon nanowire field effect transistors (FETs) have emerged as ultrasensitive, label-free biodetectors that operate by sensing bound surface charge. However, the ionic strength of the environment (i.e., the Debye length of the solution) dictates the effective magnitude of the surface charge. Here, we show that control of the Debye length determines the spatial extent of sensed bound surface charge on the sensor. We apply this technique to different methods of antibody immobilization, demonstrating different effective distances of induced charge from the sensor surface.

Mapping the surface charge distribution of amyloid fibril

NASA Astrophysics Data System (ADS)

Lee, Gyudo; Lee, Wonseok; Lee, Hyungbeen; Woo Lee, Sang; Sung Yoon, Dae; Eom, Kilho; Kwon, Taeyun

2012-07-01

It is of high importance to measure and map the surface charge distribution of amyloids, since electrostatic interaction between amyloidogenic proteins and biomolecules plays a vital role in amyloidogenesis. In this work, we have measured and mapped the surface charge distributions of amyloids (i.e., β-lactoglobulin fibril) using Kelvin probe force microscopy. It is shown that the surface charge distribution is highly dependent on the conformation of amyloids (e.g., the helical pitch of amyloid fibrils) as well as the pH of a solvent.

Charging Characteristics of an Insulating Hollow Cylinder in Vacuum

NASA Astrophysics Data System (ADS)

Yamamoto, Osamu; Hayashi, Hirotaka; Wadahama, Toshihiko; Takeda, Daisuke; Hamada, Shoji; Ohsawa, Yasuharu

This paper deals with charging characteristics of the inner surface of an insulating hollow cylinder in vacuum. We conducted measurements of electric field strength near the triple points on cathode by using an electrostatic probe. Also we conducted a computer simulation of charging based on the Secondary Electron Emission Avalanche (SEEA) mechanism. These results are compared with those obtained previously for solid cylinders. As a result, we have clarified that hollow cylinders acquire surface charge which is larger than that of solid cylinders. We have also found that charge controlling effect by roughening the inner surface, which have been proved effective to depress charging on the surface of solid cylinders in our previous studies, is limited for hollow cylinders.

Relating Silica Scaling in Reverse Osmosis to Membrane Surface Properties.

PubMed

Tong, Tiezheng; Zhao, Song; Boo, Chanhee; Hashmi, Sara M; Elimelech, Menachem

2017-04-18

We investigated the relationship between membrane surface properties and silica scaling in reverse osmosis (RO). The effects of membrane hydrophilicity, free energy for heterogeneous nucleation, and surface charge on silica scaling were examined by comparing thin-film composite polyamide membranes grafted with a variety of polymers. Results show that the rate of silica scaling was independent of both membrane hydrophilicity and free energy for heterogeneous nucleation. In contrast, membrane surface charge demonstrated a strong correlation with the extent of silica scaling (R 2 > 0.95, p < 0.001). Positively charged membranes significantly facilitated silica scaling, whereas a more negative membrane surface charge led to reduced scaling. This observation suggests that deposition of negatively charged silica species on the membrane surface plays a critical role in silica scale formation. Our findings provide fundamental insights into the mechanisms governing silica scaling in reverse osmosis and highlight the potential of membrane surface modification as a strategy to reduce silica scaling.

Self-Assembled α-Fe2O3 mesocrystals/graphene nanohybrid for enhanced electrochemical capacitors.

PubMed

Yang, Shuhua; Song, Xuefeng; Zhang, Peng; Sun, Jing; Gao, Lian

2014-06-12

Self-assembled α-Fe2O3 mesocrystals/graphene nanohybrids have been successfully synthesized and have a unique mesocrystal porous structure, a large specific surface area, and high conductivity. Mesocrystal structures have recently attracted unparalleled attention owing to their promising application in energy storage as electrochemical capacitors. However, mesocrystal/graphene nanohybrids and their growth mechanism have not been clearly investigated. Here we show a facile fabrication of short rod-like α-Fe2O3 mesocrystals/graphene nanohybrids by self-assembly of FeOOH nanorods as the primary building blocks on graphene under hydrothermal conditions, accompanied and promoted by concomitant phase transition from FeOOH to α-Fe2O3. A systematic study of the formation mechanism is also presented. The galvanostatic charge/discharge curve shows a superior specific capacitance of the as-prepared α-Fe2O3 mesocrystals/graphene nanohybrid (based on total mass of active materials), which is 306.9 F g(-1) at 3 A g(-1) in the aqueous electrolyte under voltage ranges of up to 1 V. The nanohybrid with unique sufficient porous structure and high electrical conductivity allows for effective ion and charge transport in the whole electrode. Even at a high discharge current density of 10 A g(-1), the enhanced ion and charge transport still yields a higher capacitance (98.2 F g(-1)), exhibiting enhanced rate capability. The α-Fe2O3 mesocrystal/graphene nanohybrid electrode also demonstrates excellent cyclic performance, which is superior to previously reported graphene-based hematite electrode, suggesting it is highly stable as an electrochemical capacitor. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Molecular dynamics investigation of the ionic liquid/enzyme interface: application to engineering enzyme surface charge.

PubMed

Burney, Patrick R; Nordwald, Erik M; Hickman, Katie; Kaar, Joel L; Pfaendtner, Jim

2015-04-01

Molecular simulations of the enzymes Candida rugosa lipase and Bos taurus α-chymotrypsin in aqueous ionic liquids 1-butyl-3-methylimidazolium chloride and 1-ethyl-3-methylimidazolium ethyl sulfate were used to study the change in enzyme-solvent interactions induced by modification of the enzyme surface charge. The enzymes were altered by randomly mutating lysine surface residues to glutamate, effectively decreasing the net surface charge by two for each mutation. These mutations resemble succinylation of the enzyme by chemical modification, which has been shown to enhance the stability of both enzymes in ILs. After establishing that the enzymes were stable on the simulated time scales, we focused the analysis on the organization of the ionic liquid substituents about the enzyme surface. Calculated solvent charge densities show that for both enzymes and in both solvents that changing positively charged residues to negative charge does indeed increase the charge density of the solvent near the enzyme surface. The radial distribution of IL constituents with respect to the enzyme reveals decreased interactions with the anion are prevalent in the modified systems when compared to the wild type, which is largely accompanied by an increase in cation contact. Additionally, the radial dependence of the charge density and ion distribution indicates that the effect of altering enzyme charge is confined to short range (≤1 nm) ordering of the IL. Ultimately, these results, which are consistent with that from prior experiments, provide molecular insight into the effect of enzyme surface charge on enzyme stability in ILs. © 2015 Wiley Periodicals, Inc.

Competitive Adsorption and Ordered Packing of Counterions near Highly Charged Surfaces: From Mean-Field Theory to Monte Carlo Simulations

PubMed Central

Wen, Jiayi; Zhou, Shenggao; Xu, Zhenli; Li, Bo

2013-01-01

Competitive adsorption of counterions of multiple species to charged surfaces is studied by a size-effect included mean-field theory and Monte Carlo (MC) simulations. The mean-field electrostatic free-energy functional of ionic concentrations, constrained by Poisson’s equation, is numerically minimized by an augmented Lagrangian multiplier method. Unrestricted primitive models and canonical ensemble MC simulations with the Metropolis criterion are used to predict the ionic distributions around a charged surface. It is found that, for a low surface charge density, the adsorption of ions with a higher valence is preferable, agreeing with existing studies. For a highly charged surface, both of the mean-field theory and MC simulations demonstrate that the counterions bind tightly around the charged surface, resulting in a stratification of counterions of different species. The competition between mixed entropy and electrostatic energetics leads to a compromise that the ionic species with a higher valence-to-volume ratio has a larger probability to form the first layer of stratification. In particular, the MC simulations confirm the crucial role of ionic valence-to-volume ratios in the competitive adsorption to charged surfaces that had been previously predicted by the mean-field theory. The charge inversion for ionic systems with salt is predicted by the MC simulations but not by the mean-field theory. This work provides a better understanding of competitive adsorption of counterions to charged surfaces and calls for further studies on the ionic size effect with application to large-scale biomolecular modeling. PMID:22680474

Competitive adsorption and ordered packing of counterions near highly charged surfaces: From mean-field theory to Monte Carlo simulations.

PubMed

Wen, Jiayi; Zhou, Shenggao; Xu, Zhenli; Li, Bo

2012-04-01

Competitive adsorption of counterions of multiple species to charged surfaces is studied by a size-effect-included mean-field theory and Monte Carlo (MC) simulations. The mean-field electrostatic free-energy functional of ionic concentrations, constrained by Poisson's equation, is numerically minimized by an augmented Lagrangian multiplier method. Unrestricted primitive models and canonical ensemble MC simulations with the Metropolis criterion are used to predict the ionic distributions around a charged surface. It is found that, for a low surface charge density, the adsorption of ions with a higher valence is preferable, agreeing with existing studies. For a highly charged surface, both the mean-field theory and the MC simulations demonstrate that the counterions bind tightly around the charged surface, resulting in a stratification of counterions of different species. The competition between mixed entropy and electrostatic energetics leads to a compromise that the ionic species with a higher valence-to-volume ratio has a larger probability to form the first layer of stratification. In particular, the MC simulations confirm the crucial role of ionic valence-to-volume ratios in the competitive adsorption to charged surfaces that had been previously predicted by the mean-field theory. The charge inversion for ionic systems with salt is predicted by the MC simulations but not by the mean-field theory. This work provides a better understanding of competitive adsorption of counterions to charged surfaces and calls for further studies on the ionic size effect with application to large-scale biomolecular modeling.

Battery Power Management in Heavy-duty HEVs based on the Estimated Critical Surface Charge

DTIC Science & Technology

2011-03-01

health prospects without any penalty on fuel efficiency. Keywords: Lithium - ion battery ; power management; critical surface charge; Lithium-ion...fuel efficiency. 15. SUBJECT TERMS Lithium - ion battery ; power management; critical surface charge; Lithium-ion concentration; estimation; extended...Di Domenico, D., Fiengo, G., and Stefanopoulou, A. (2008) ’ Lithium - ion battery state of charge estimation with a kalman filter based on a

Aggregation and charging of sulfate and amidine latex particles in the presence of oxyanions.

PubMed

Sugimoto, Takuya; Cao, Tianchi; Szilagyi, Istvan; Borkovec, Michal; Trefalt, Gregor

2018-08-15

Electrophoretic mobility and time resolved light scattering are used to measure the effect on charging and aggregation of amidine and sulfate latex particles of different oxyanions namely, phosphate, arsenate, sulfate, and selenate. In the case of negatively charged sulfate latex particles oxyanions represent the coions, while they represent counterions in the case of the positively charged amidine latex. Repulsive interaction between the sulfate latex surface and the coions results in weak ion specific effects on the charging and aggregation. On the other hand the interaction of oxyanions with the amidine latex surface is highly specific. The monovalent dihydrogen phosphate ion strongly adsorbs to the positively charged surface and reverses the charge of the particle. This charge reversal leads also to the restabilization of the amidine latex suspension at the intermediate phosphate concentrations. In the case of dihydrogen arsenate the adsorption to amidine latex surface is weaker and no charge reversal and restabilization occurs. Similar differences are seen between the sulfate and selenate analogues, where selenate adsorbs more strongly to the surface as compared to the sulfate ion and invokes charge reversal. The present results indicate that ion specificity is much more pronounced in the case of counterions. Copyright © 2018 Elsevier Inc. All rights reserved.

Scalable 2D Mesoporous Silicon Nanosheets for High-Performance Lithium-Ion Battery Anode.

PubMed

Chen, Song; Chen, Zhuo; Xu, Xingyan; Cao, Chuanbao; Xia, Min; Luo, Yunjun

2018-03-01

Constructing unique mesoporous 2D Si nanostructures to shorten the lithium-ion diffusion pathway, facilitate interfacial charge transfer, and enlarge the electrode-electrolyte interface offers exciting opportunities in future high-performance lithium-ion batteries. However, simultaneous realization of 2D and mesoporous structures for Si material is quite difficult due to its non-van der Waals structure. Here, the coexistence of both mesoporous and 2D ultrathin nanosheets in the Si anodes and considerably high surface area (381.6 m 2 g -1 ) are successfully achieved by a scalable and cost-efficient method. After being encapsulated with the homogeneous carbon layer, the Si/C nanocomposite anodes achieve outstanding reversible capacity, high cycle stability, and excellent rate capability. In particular, the reversible capacity reaches 1072.2 mA h g -1 at 4 A g -1 even after 500 cycles. The obvious enhancements can be attributed to the synergistic effect between the unique 2D mesoporous nanostructure and carbon capsulation. Furthermore, full-cell evaluations indicate that the unique Si/C nanostructures have a great potential in the next-generation lithium-ion battery. These findings not only greatly improve the electrochemical performances of Si anode, but also shine some light on designing the unique nanomaterials for various energy devices. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Role of protein surface charge in monellin sweetness.

PubMed

Xue, Wei-Feng; Szczepankiewicz, Olga; Thulin, Eva; Linse, Sara; Carey, Jannette

2009-03-01

A small number of proteins have the unusual property of tasting intensely sweet. Despite many studies aimed at identifying their sweet taste determinants, the molecular basis of protein sweetness is not fully understood. Recent mutational studies of monellin have implicated positively charged residues in sweetness. In the present work, the effect of overall net charge was investigated using the complementary approach of negative charge alterations. Multiple substitutions of Asp/Asn and Glu/Gln residues radically altered the surface charge of single-chain monellin by removing six negative charges or adding four negative charges. Biophysical characterization using circular dichroism, fluorescence, and two-dimensional NMR demonstrates that the native fold of monellin is preserved in the variant proteins under physiological solution conditions although their stability toward chemical denaturation is altered. A human taste test was employed to determine the sweetness detection threshold of the variants. Removal of negative charges preserves monellin sweetness, whereas added negative charge has a large negative impact on sweetness. Meta-analysis of published charge variants of monellin and other sweet proteins reveals a general trend toward increasing sweetness with increasing positive net charge. Structural mapping of monellin variants identifies a hydrophobic surface predicted to face the receptor where introduced positive or negative charge reduces sweetness, and a polar surface where charges modulate long-range electrostatic complementarity.

Fibronectin module FN(III)9 adsorption at contrasting solid model surfaces studied by atomistic molecular dynamics.

PubMed

Kubiak-Ossowska, Karina; Mulheran, Paul A; Nowak, Wieslaw

2014-08-21

The mechanism of human fibronectin adhesion synergy region (known as integrin binding region) in repeat 9 (FN(III)9) domain adsorption at pH 7 onto various and contrasting model surfaces has been studied using atomistic molecular dynamics simulations. We use an ionic model to mimic mica surface charge density but without a long-range electric field above the surface, a silica model with a long-range electric field similar to that found experimentally, and an Au {111} model with no partial charges or electric field. A detailed description of the adsorption processes and the contrasts between the various model surfaces is provided. In the case of our model silica surface with a long-range electrostatic field, the adsorption is rapid and primarily driven by electrostatics. Because it is negatively charged (-1e), FN(III)9 readily adsorbs to a positively charged surface. However, due to its partial charge distribution, FN(III)9 can also adsorb to the negatively charged mica model because of the absence of a long-range repulsive electric field. The protein dipole moment dictates its contrasting orientation at these surfaces, and the anchoring residues have opposite charges to the surface. Adsorption on the model Au {111} surface is possible, but less specific, and various protein regions might be involved in the interactions with the surface. Despite strongly influencing the protein mobility, adsorption at these model surfaces does not require wholesale FN(III)9 conformational changes, which suggests that the biological activity of the adsorbed protein might be preserved.

Suppression of surface charge accumulation on Al{sub 2}O{sub 3}-filled epoxy resin insulator under dc voltage by direct fluorination

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Boya; Zhang, Guixin, E-mail: guixin@mail.tsinghua.edu.cn; Li, Chuanyang

2015-12-15

Surface charge accumulation on insulators under high dc voltage is a major factor that may lead to the reduction of insulation levels in gas insulated devices. In this paper, disc insulators made of Al{sub 2}O{sub 3}-filled epoxy resin were surface fluorinated using a F{sub 2}/N{sub 2} mixture (12.5% F{sub 2}) at 50 °C and 0.1 MPa for different durations of 15 min, 30 min and 60 min. A dc voltage was applied to the insulator for 30 min and the charge density on its surface was measured by an electrostatic probe. The results revealed significant lower surface charge densities on themore » fluorinated insulators in comparison with the original one. Surface conductivity measurements indicated a higher surface conductivity by over three orders of magnitude after fluorination, which would allow the charges to transfer along the surface and thus may suppress their accumulation. Further, attenuated total reflection infrared analysis and surface morphology observations of the samples revealed that the introduction of fluoride groups altered the surface physicochemical properties. These structure changes, especially the physical defects reduced the depth of charge traps in the surface layer, which was verified by the measurement of energy distributions of the electron and hole traps based on the isothermal current theory. The results in this paper demonstrate that fluorination can be a promising and effective method to suppress surface charge accumulation on epoxy insulators in gas insulated devices.« less

Charge heterogeneity of surfaces: mapping and effects on surface forces.

PubMed

Drelich, Jaroslaw; Wang, Yu U

2011-07-11

The DLVO theory treats the total interaction force between two surfaces in a liquid medium as an arithmetic sum of two components: Lifshitz-van der Waals and electric double layer forces. Despite the success of the DLVO model developed for homogeneous surfaces, a vast majority of surfaces of particles and materials in technological systems are of a heterogeneous nature with a mosaic structure composed of microscopic and sub-microscopic domains of different surface characteristics. In such systems, the heterogeneity of the surface can be more important than the average surface character. Attractions can be stronger, by orders of magnitude, than would be expected from the classical mean-field DLVO model when area-averaged surface charge or potential is employed. Heterogeneity also introduces anisotropy of interactions into colloidal systems, vastly ignored in the past. To detect surface heterogeneities, analytical tools which provide accurate and spatially resolved information about material surface chemistry and potential - particularly at microscopic and sub-microscopic resolutions - are needed. Atomic force microscopy (AFM) offers the opportunity to locally probe not only changes in material surface characteristic but also charges of heterogeneous surfaces through measurements of force-distance curves in electrolyte solutions. Both diffuse-layer charge densities and potentials can be calculated by fitting the experimental data with a DLVO theoretical model. The surface charge characteristics of the heterogeneous substrate as recorded by AFM allow the charge variation to be mapped. Based on the obtained information, computer modeling and simulation can be performed to study the interactions among an ensemble of heterogeneous particles and their collective motions. In this paper, the diffuse-layer charge mapping by the AFM technique is briefly reviewed, and a new Diffuse Interface Field Approach to colloid modeling and simulation is briefly discussed. Copyright © 2011 Elsevier B.V. All rights reserved.

The impact of nano-coating on surface charge accumulation of epoxy resin insulator: characteristic and mechanism

NASA Astrophysics Data System (ADS)

Qi, Bo; Gao, Chunjia; Lv, Yuzhen; Li, Chengrong; Tu, Youping; Xiong, Jun

2018-06-01

The flashover phenomenon of the insulator is the main cause for insulating failure of GIS/GIL, and one of the most critical impacting factors is the accumulation of surface charge. The common methods to restrain the surface charge accumulation are reviewed in this paper. Through the reasonable comparison and analysis of these methods, nano-coatings for the insulator were selected as a way to restrain the surface charge accumulation. Based on this, six nano-coated epoxy resin samples with different concentrations of P25-TiO2 nanoparticles were produced. A high precision 3D surface charge measurement system was developed in this paper with a spatial resolution of 4.0 mm2 and a charge resolution of 0.01 µC (m2 · mV)‑1. The experimental results for the epoxy resin sample showed that with the concentration of nanoparticles of the coating material increasing, the surface charge density tended to first decrease and then increase. In the sample coated with 0.5% concentration of nanoparticles, the suppression effect is the optimum, leading to a 63.8% reduction of charge density under DC voltage. The application test for actual nano-coated GIS/GIL basin insulator indicated that the maximum suppression degree for the charge density under DC voltage could reach 48.3%, while it could reach 22.2% for switching impulse voltage and 12.5% for AC context. The control mechanism of nano-coatings on charge accumulation was proposed based on the analysis for surface morphology features and traps characteristics; the shallow traps dominate in the migration of charges while the deep traps operate on the charge accumulation. With the concentration of nanoparticles in nano-coating material mounting up, the density of shallow traps continuously increases, while for deep traps, it first decreases and then increases. For the sample with 0.5% concentration of nanoparticles coated, the competition between shallow traps and deep traps comes to the most balanced state, producing the most significant suppression impact on surface charge accumulation.

Secondary Structures of Ubiquitin Ions Soft-Landed onto Self-Assembled Monolayer Surfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hu, Qichi; Laskin, Julia

2016-06-09

The secondary structures of multiply charged ubiquitin ions soft-landed onto self-assembled monolayer (SAM) surfaces were studied using in situ infrared reflection-absorption spectroscopy (IRRAS). Two charge states of ubiquitin, 5+ and 13+, were mass selected separately from a mixture of different charge states produced by electrospray ionization (ESI). The low 5+ charge state represents a native-like folded state of ubiquitin, while the high 13+ charge state assumes an extended, almost linear conformation. Each of the two charge states was soft-landed onto a CH 3- and COOH-terminated SAM of alkylthiols on gold (HSAM and COOH-SAM). HSAM is a hydrophobic surface known tomore » stabilize helical conformations of soft-landed protonated peptides, whereas COOH-SAM is a hydrophilic surface that preferentially stabilizes β-sheet conformations. IRRAS spectra of the soft-landed ubiquitin ions were acquired as a function of time during and after ion soft-landing. Similar to smaller peptide ions, helical conformations of ubiquitin are found to be more abundant on HSAM, while the relative abundance of β-sheet conformations increases on COOH-SAM. The initial charge state of ubiquitin also has a pronounced effect on its conformation on the surface. Specifically, on both surfaces, a higher relative abundance of helical conformations and lower relative abundance of β-sheet conformations is observed for the 13+ charge state compared to the 5+ charge state. Time-resolved experiments indicate that the α-helical band in the spectrum of the 13+ charge state slowly increases with time on the HSAM surface and decreases in the spectrum of the 13+ charge state on COOH-SAM. These results further support the preference of the hydrophobic HSAM surface toward helical conformations and demonstrate that soft-landed protein ions may undergo slow conformational changes during and after deposition.« less

Evolution of LiFePO4 thin films interphase with electrolyte

NASA Astrophysics Data System (ADS)

Dupré, N.; Cuisinier, M.; Zheng, Y.; Fernandez, V.; Hamon, J.; Hirayama, M.; Kanno, R.; Guyomard, D.

2018-04-01

Many parameters may control the growth and the characteristics of the interphase, such as surface structure and morphology, structural defects, grain boundaries, surface reactions, etc. However, polycrystalline surfaces contain these parameters simultaneously, resulting in a quite complicated system to study. Working with model electrode surfaces using crystallographically oriented crystalline thin films appears as a novel and unique approach to understand contributions of preferential orientation and rugosity of the surface. In order to rebuild the interphase architecture along electrochemical cycling, LiFePO4 epitaxial films offering ideal 2D (100) interfaces are here investigated through the use of non-destructive depth profiling by Angular Resolved X-ray Photoelectron Spectroscopy (ARXPS). The composition and structure of the interphase is then monitored upon cycling for samples stopped at the end of charge and discharge for various numbers of cycles, and discussed in the light of combined XPS and X-ray reflectivity (XRR) measurements. Such an approach allows describing the interphase evolution on a specific model LiFePO4 crystallographic orientation and helps understanding the nature and evolution of the LiFePO4/electrolyte interphase forming on the surface of LiFePO4 poly-crystalline powder.

Optical second harmonic spectroscopy of silicon-adsorbate surfaces and silicon nanocrystals

NASA Astrophysics Data System (ADS)

Downer, Michael

2002-03-01

Second harmonic generation (SHG) provides a surface-specific, noninvasive probe of adsorbates. However, microscopic first-principles theory of adsorbate-specific spectroscopic SHG responses has proven elusive. Here we present experimental SHG spectra for six well-characterized, technologically important Si(001) surfaces in ultrahigh vacuum (UHV): clean Si(001)-2x1 and Si(001) terminated with hydrogen (H), [1] germanium (Ge), Ge and H, [2] boron (B) and B and H. [3] Each adsorbate (combination) alters SHG uniquely. Our microscopic theories based on ab initio pseudopotential or semi-empirical tight-binding (SETB) methods then explain observed trends, and predict new features in unexplored spectral regions. [3,4] Charge transfer among surface bonds is found to govern SHG spectroscopy of surface-adsorbate systems strongly. New results on SHG from Si nanocrystals embedded in SiO2 will also be presented. [5] SHG is sensitive to Si/SiO2 interface states, electrostatic charge on the nanocrystals, and macroscopic particle density gradients. Finally, a new frequency-domain interferometric second-harmonic (FDISH) spectroscopic technique to measure simultaneously the intensity and phase of SH radiation over a broad spectral range without laser tuning will be described. [6] 1. J. Dadap et al., Phys. Rev. B 56, 13367 (1997). 2. P. Parkinson et al., Appl. Phys. B 68, 641 (1999). 3. D. Lim et al., Phys. Rev. Lett. 84, 3406 (2000); Appl. Phys. Lett. 77, 181 (2000). 4. V. Gavrilenko et al., Phys. Rev. B 63, 1653 (2001); M. C. Downer et al., Surf. Interface Anal. 31, 966 (2001); M. C. Downer et al., phys. stat. sol. (a), in press (2001). 5. Y. Jiang et al., Appl. Phys. Lett. 78, 766 (2001). 6. P. T. Wilson et al., Opt. Lett. 24, 496 (1999).

Ionic liquids behave as dilute electrolyte solutions

PubMed Central

Gebbie, Matthew A.; Valtiner, Markus; Banquy, Xavier; Fox, Eric T.; Henderson, Wesley A.; Israelachvili, Jacob N.

2013-01-01

We combine direct surface force measurements with thermodynamic arguments to demonstrate that pure ionic liquids are expected to behave as dilute weak electrolyte solutions, with typical effective dissociated ion concentrations of less than 0.1% at room temperature. We performed equilibrium force–distance measurements across the common ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide ([C4mim][NTf2]) using a surface forces apparatus with in situ electrochemical control and quantitatively modeled these measurements using the van der Waals and electrostatic double-layer forces of the Derjaguin–Landau–Verwey–Overbeek theory with an additive repulsive steric (entropic) ion–surface binding force. Our results indicate that ionic liquids screen charged surfaces through the formation of both bound (Stern) and diffuse electric double layers, where the diffuse double layer is comprised of effectively dissociated ionic liquid ions. Additionally, we used the energetics of thermally dissociating ions in a dielectric medium to quantitatively predict the equilibrium for the effective dissociation reaction of [C4mim][NTf2] ions, in excellent agreement with the measured Debye length. Our results clearly demonstrate that, outside of the bound double layer, most of the ions in [C4mim][NTf2] are not effectively dissociated and thus do not contribute to electrostatic screening. We also provide a general, molecular-scale framework for designing ionic liquids with significantly increased dissociated charge densities via judiciously balancing ion pair interactions with bulk dielectric properties. Our results clear up several inconsistencies that have hampered scientific progress in this important area and guide the rational design of unique, high–free-ion density ionic liquids and ionic liquid blends. PMID:23716690

The study of surface wetting, nanobubbles and boundary slip with an applied voltage: A review

PubMed Central

Pan, Yunlu; Zhao, Xuezeng

2014-01-01

Summary The drag of fluid flow at the solid–liquid interface in the micro/nanoscale is an important issue in micro/nanofluidic systems. Drag depends on the surface wetting, nanobubbles, surface charge and boundary slip. Some researchers have focused on the relationship between these interface properties. In this review, the influence of an applied voltage on the surface wettability, nanobubbles, surface charge density and slip length are discussed. The contact angle (CA) and contact angle hysteresis (CAH) of a droplet of deionized (DI) water on a hydrophobic polystyrene (PS) surface were measured with applied direct current (DC) and alternating current (AC) voltages. The nanobubbles in DI water and three kinds of saline solution on a PS surface were imaged when a voltage was applied. The influence of the surface charge density on the nanobubbles was analyzed. Then the slip length and the electrostatic force on the probe were measured on an octadecyltrichlorosilane (OTS) surface with applied voltage. The influence of the surface charge on the boundary slip and drag of fluid flow has been discussed. Finally, the influence of the applied voltage on the surface wetting, nanobubbles, surface charge, boundary slip and the drag of liquid flow are summarized. With a smaller surface charge density which could be achieved by applying a voltage on the surface, larger and fewer nanobubbles, a larger slip length and a smaller drag of liquid flow could be found. PMID:25161839

The study of surface wetting, nanobubbles and boundary slip with an applied voltage: A review.

PubMed

Pan, Yunlu; Bhushan, Bharat; Zhao, Xuezeng

2014-01-01

The drag of fluid flow at the solid-liquid interface in the micro/nanoscale is an important issue in micro/nanofluidic systems. Drag depends on the surface wetting, nanobubbles, surface charge and boundary slip. Some researchers have focused on the relationship between these interface properties. In this review, the influence of an applied voltage on the surface wettability, nanobubbles, surface charge density and slip length are discussed. The contact angle (CA) and contact angle hysteresis (CAH) of a droplet of deionized (DI) water on a hydrophobic polystyrene (PS) surface were measured with applied direct current (DC) and alternating current (AC) voltages. The nanobubbles in DI water and three kinds of saline solution on a PS surface were imaged when a voltage was applied. The influence of the surface charge density on the nanobubbles was analyzed. Then the slip length and the electrostatic force on the probe were measured on an octadecyltrichlorosilane (OTS) surface with applied voltage. The influence of the surface charge on the boundary slip and drag of fluid flow has been discussed. Finally, the influence of the applied voltage on the surface wetting, nanobubbles, surface charge, boundary slip and the drag of liquid flow are summarized. With a smaller surface charge density which could be achieved by applying a voltage on the surface, larger and fewer nanobubbles, a larger slip length and a smaller drag of liquid flow could be found.

Full-Particle Simulations on Electrostatic Plasma Environment near Lunar Vertical Holes

NASA Astrophysics Data System (ADS)

Miyake, Y.; Nishino, M. N.

2015-12-01

The Kaguya satellite and the Lunar Reconnaissance Orbiter have observed a number of vertical holes on the terrestrial Moon [Haruyama et al., GRL, 2009; Robinson et al., PSS, 2012], which have spatial scales of tens of meters and are possible lava tube skylights. The hole structure has recently received particular attention, because the structure gives an important clue to the complex volcanic history of the Moon. The holes also have high potential as locations for constructing future lunar bases, because of fewer extra-lunar rays/particles and micrometeorites reaching the hole bottoms. In this sense, these holes are not only interesting in selenology, but are also significant from the viewpoint of electrostatic environments. The subject can also be an interesting resource of research in comparative planetary science, because hole structures have been found in other solar system bodies such as the Mars. The lunar dayside electrostatic environment is governed by electrodynamic interactions among the solar wind plasma, photoelectrons, and the charged lunar surface, providing topologically complex boundaries to the plasma. We use the three-dimensional, massively-parallelized, particle-in-cell simulation code EMSES [Miyake and Usui, POP, 2009] to simulate the near-hole plasma environment on the Moon [Miyake and Nishino, Icarus, 2015]. We took into account the solar wind plasma downflow, photoelectron emission from the sunlit part of the lunar surface, and plasma charge deposition on the surface. The simulation domain consists of 400×400×2000 grid points and contains about 25 billion plasma macro-particles. Thus, we need to use supercomputers for the simulations. The vertical wall of the hole introduces a new boundary for both photo and solar wind electrons. The current balance condition established at a hole bottom is altered by the limited solar wind electron penetration into the hole and complex photoelectron current paths inside the hole. The self-consistent modeling not only reproduces intense differential charging between sunlit and shadowed surfaces, but also reveals the potential difference between sunlit surfaces inside and outside the hole. The results demonstrate the uniqueness of the near-hole plasma environment as well as provide useful knowledge for future landing missions.

Profiling charge complementarity and selectivity for binding at the protein surface.

PubMed

Sulea, Traian; Purisima, Enrico O

2003-05-01

A novel analysis and representation of the protein surface in terms of electrostatic binding complementarity and selectivity is presented. The charge optimization methodology is applied in a probe-based approach that simulates the binding process to the target protein. The molecular surface is color coded according to calculated optimal charge or according to charge selectivity, i.e., the binding cost of deviating from the optimal charge. The optimal charge profile depends on both the protein shape and charge distribution whereas the charge selectivity profile depends only on protein shape. High selectivity is concentrated in well-shaped concave pockets, whereas solvent-exposed convex regions are not charge selective. This suggests the synergy of charge and shape selectivity hot spots toward molecular selection and recognition, as well as the asymmetry of charge selectivity at the binding interface of biomolecular systems. The charge complementarity and selectivity profiles map relevant electrostatic properties in a readily interpretable way and encode information that is quite different from that visualized in the standard electrostatic potential map of unbound proteins.

Structural morphology of crystals with the barite (BaSO 4) structure: A revision and extension

NASA Astrophysics Data System (ADS)

Hartman, P.; Strom, C. S.

1989-09-01

The structural morphology of crystals with the barite (BaSO 4) structure (sulphates, chromates, perchlorates, permanganates and tetrafluoroborates) has been determined with the use of computer programs. Uniquely defined F forms are {002}, {210}, {211}, {020} and {201}. Two different F slices were found for {101} and {200}, 33 for {011}. Attachment energies and specific surface energies have been calculated for an electrostatic point charge model as a function of the charge distribution in the anion. On this basis it is concluded that {101} behaves as an F form, {200} as an S form and {011} as a K form. The theoretical growth form shows {210}, {101} and {002} as main forms. A comparison is made with habits of natural and synthetic crystals. Experiments on KCIO 4 show that {011} appears at high supersaturations (>38; ;20%). It is shown that a broken bond model provides relative attachment energies that are higher by a factor of about three.

Understanding the Unique Properties of Organometal Trihalide Perovskite with Single Crystals

NASA Astrophysics Data System (ADS)

Huang, Jinsong

Organometal Trihalide Perovskite has been discovered to be all-round optoelectronic materials many types of electronic devices. The understanding of this family of materials is however limited yet due to the complicated grain structures in polycrystalline films which are generally used in most of the devices. In this contribution, I will present our recent progress in understanding the fundamental properties, including optoelectronic properties and electromechanical properties, using the high quality organometal trihalide perovskite single crystals. I will report the crystallographic orientation dependent charge transport and collection, surface and bulk charge recombination process, and direction measuring of carrier diffusion length using the lasing induced photocurrent scanning. The polarity of the organometal trihalide perovskite crystals will also be examined. We thank financial support from SunShot Initiative at Department of Energy under Award DE-EE0006709, and from National Science Foundation Grant DMR-1505535 and Grant DMR-1420645, and from Office of Naval Research under Award N00014-15-1-2713.

Controllable construction of flower-like FeS/Fe2O3 composite for lithium storage

NASA Astrophysics Data System (ADS)

Wang, Jie; He, Huan; Wu, Zexing; Liang, Jianing; Han, Lili; Xin, Huolin L.; Guo, Xuyun; Zhu, Ye; Wang, Deli

2018-07-01

Transitions metal sulfides/oxides have been considered as promising anode candidates for next generation lithium-ion batteries (LIBs) due to high theoretical capacities. However, the large volume change during lithiation/delithiation process and poor electronic conductivity often result in a poor charging/discharging performance. Herein, we design a flower-like FeS/Fe2O3 composite via a simple "solvothermal-oxidation" method, in which the Fe2O3 is most distributed on the surface of the flower. The unique porous structure and synergistic effect between FeS and Fe2O3 not only accommodate the large volume expansion, but also facilitate Li ion and electron transport. The Fe2O3 shell effectively reduce the dissolution of Li2Sx during discharge/charge process. When serving as the anode material in lithium ion battery, FeS/Fe2O3 exhibits superior specific capacity, rate capacity and cycling stability compared with pure FeS and Fe2O3.

Bivalence Mn5O8 with hydroxylated interphase for high-voltage aqueous sodium-ion storage

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shan, Xiaoqiang; Charles, Daniel S.; Lei, Yinkai

Aqueous electrochemical energy storage devices have attracted significant attention owing to their high safety, low cost, and environmental friendliness. However, their applications have been limited by a narrow potential window (~1.23 V), beyond which the hydrogen and oxygen evolution reactions occur. Here, we report the formation of layered Mn 5O 8 pseudocapacitor electrode material with a well ordered hydroxylated interphase. A symmetric full cell using such electrodes demonstrates a stable potential window of 3.0 V in an aqueous electrolyte, as well as high energy and power performance, nearly 100% coulombic efficiency and 85% energy efficiency after 25,000 charge-discharge cycles. Furthermore,more » the interplay between hydroxylated interphase on the surface and the unique bivalence structure of Mn 5O 8 suppresses the gas evolution reactions, offers a two-electron charge transfer via Mn 2+/Mn 4+ redox couple, and provides facile pathway for Na-ion transport via intra-/inter-layer defects of Mn 5O 8.« less

Bivalence Mn5O8 with hydroxylated interphase for high-voltage aqueous sodium-ion storage

DOE PAGES

Shan, Xiaoqiang; Charles, Daniel S.; Lei, Yinkai; ...

2016-11-15

Aqueous electrochemical energy storage devices have attracted significant attention owing to their high safety, low cost, and environmental friendliness. However, their applications have been limited by a narrow potential window (~1.23 V), beyond which the hydrogen and oxygen evolution reactions occur. Here, we report the formation of layered Mn 5O 8 pseudocapacitor electrode material with a well ordered hydroxylated interphase. A symmetric full cell using such electrodes demonstrates a stable potential window of 3.0 V in an aqueous electrolyte, as well as high energy and power performance, nearly 100% coulombic efficiency and 85% energy efficiency after 25,000 charge-discharge cycles. Furthermore,more » the interplay between hydroxylated interphase on the surface and the unique bivalence structure of Mn 5O 8 suppresses the gas evolution reactions, offers a two-electron charge transfer via Mn 2+/Mn 4+ redox couple, and provides facile pathway for Na-ion transport via intra-/inter-layer defects of Mn 5O 8.« less

Estimates of Sputter Yields of Solar-Wind Heavy Ions of Lunar Regolith Materials

NASA Technical Reports Server (NTRS)

Barghouty, Abdulmasser F.; Adams, James H., Jr.

2008-01-01

At energies of approximately 1 keV/amu, solar-wind protons and heavy ions interact with the lunar surface materials via a number of microscopic interactions that include sputtering. Solar-wind induced sputtering is a main mechanism by which the composition of the topmost layers of the lunar surface can change, dynamically and preferentially. This work concentrates on sputtering induced by solar-wind heavy ions. Sputtering associated with slow (speeds the electrons speed in its first Bohr orbit) and highly charged ions are known to include both kinetic and potential sputtering. Potential sputtering enjoys some unique characteristics that makes it of special interest to lunar science and exploration. Unlike the yield from kinetic sputtering where simulation and approximation schemes exist, the yield from potential sputtering is not as easy to estimate. This work will present a preliminary numerical scheme designed to estimate potential sputtering yields from reactions relevant to this aspect of solar-wind lunar-surface coupling.

The perturbation energy: A missing key to understand the “nobleness” of bulk gold

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alcántara Ortigoza, Marisol, E-mail: Marisol.AlcantaraOrtigoza@ucf.edu; Stolbov, Sergey, E-mail: Sergey.Stolbov@ucf.edu

2015-05-21

The nobleness of gold surfaces has been appreciated since long before the beginning of recorded history. Yet, the origin of this phenomenon remains open because the so far existing explanations either incorrectly imply that silver should be the noblest metal or would fail to predict the dissolution of Au in aqua regia. Here, based on our analyses of oxygen adsorption, we advance that bulk gold’s unique resistance to oxidation is traced to the large energy cost associated with the perturbation its surfaces undergo upon adsorption of highly electronegative species. This fact is related to the almost totally filled d-band ofmore » Au and relativistic effects, but does not imply that the strength of the adsorbate-Au bond is weak. The magnitude of the structural and charge-density perturbation energy upon adsorption of atomic oxygen—which is largest for Au—is assessed from first-principles calculations and confirmed via a multiple regression analysis of the binding energy of oxygen on metal surfaces.« less

Wrinkled substrate and Indium Tin Oxide-free transparent electrode making organic solar cells thinner in active layer

NASA Astrophysics Data System (ADS)

Liu, Kong; Lu, Shudi; Yue, Shizhong; Ren, Kuankuan; Azam, Muhammad; Tan, Furui; Wang, Zhijie; Qu, Shengchun; Wang, Zhanguo

2016-11-01

To enable organic solar cells with a competent charge transport efficiency, reducing the thickness of active layer without sacrificing light absorption efficiency turns out to be of high feasibility. Herein, organic solar cells on wrinkled metal surface are designed. The purposely wrinkled Al/Au film with a smooth surface provides a unique scaffold for constructing thin organic photovoltaic devices by avoiding pinholes and defects around sharp edges in conventional nanostructures. The corresponding surface light trapping effect enables the thin active layer (PTB7-Th:PC71BM) with a high absorption efficiency. With the innovative MoO3/Ag/ZnS film as the top transparent electrode, the resulting Indium Tin Oxide-free wrinkled devices show a power conversion efficiency as 7.57% (50 nm active layer), higher than the planner counterparts. Thus, this paper provides a new methodology to improve the performance of organic solar cells by balancing the mutual restraint factors to a high level.

A New Kinetic Simulation Model with Self-Consistent Calculation of Regolith Layer Charging for Moon-Plasma Interactions

NASA Astrophysics Data System (ADS)

Han, D.; Wang, J.

2015-12-01

The moon-plasma interactions and the resulting surface charging have been subjects of extensive recent investigations. While many particle-in-cell (PIC) based simulation models have been developed, all existing PIC simulation models treat the surface of the Moon as a boundary condition to the plasma flow. In such models, the surface of the Moon is typically limited to simple geometry configurations, the surface floating potential is calculated from a simplified current balance condition, and the electric field inside the regolith layer cannot be resolved. This paper presents a new full particle PIC model to simulate local scale plasma flow and surface charging. A major feature of this new model is that the surface is treated as an "interface" between two mediums rather than a boundary, and the simulation domain includes not only the plasma but also the regolith layer and the bedrock underneath it. There are no limitations on the surface shape. An immersed-finite-element field solver is applied which calculates the regolith surface floating potential and the electric field inside the regolith layer directly from local charge deposition. The material property of the regolith layer is also explicitly included in simulation. This new model is capable of providing a self-consistent solution to the plasma flow field, lunar surface charging, the electric field inside the regolith layer and the bedrock for realistic surface terrain. This new model is applied to simulate lunar surface-plasma interactions and surface charging under various ambient plasma conditions. The focus is on the lunar terminator region, where the combined effects from the low sun elevation angle and the localized plasma wake generated by plasma flow over a rugged terrain can generate strongly differentially charged surfaces and complex dust dynamics. We discuss the effects of the regolith properties and regolith layer charging on the plasma flow field, dust levitation, and dust transport.

Acceleration of osteogenesis by using barium titanate piezoelectric ceramic as an implant material

NASA Astrophysics Data System (ADS)

Furuya, K.; Morita, Y.; Tanaka, K.; Katayama, T.; Nakamachi, E.

2011-04-01

As bone has piezoelectric properties, it is expected that activity of bone cells and bone formation can be accelerated by applying piezoelectric ceramics to implants. Since lead ions, included in ordinary piezoelectric ceramics, are harmful, a barium titanate (BTO) ceramic, which is a lead-free piezoelectric ceramic, was used in this study. The purpose of this study was to investigate piezoelectric effects of surface charge of BTO on cell differentiation under dynamic loading in vitro. Rat bone marrow cells seeded on surfaces of BTO ceramics were cultured in culture medium supplemented with dexamethasone, β-glycerophosphate and ascorbic acid while a dynamic load was applied to the BTO ceramics. After 10 days of cultivation, the cell layer and synthesized matrix on the BTO surfaces were scraped off, and then DNA content, alkaline phosphtase (ALP) activity and calcium content were measured, to evaluate osteogenic differentiation. ALP activity on the charged BTO surface was slightly higher than that on the non-charged BTO surface. The amount of calcium on the charged BTO surface was also higher than that on the non-charged BTO surface. These results showed that the electric charged BTO surface accelerated osteogenesis.

Adsorption of hydrophobin on different self-assembled monolayers: the role of the hydrophobic dipole and the electric dipole.

PubMed

Peng, Chunwang; Liu, Jie; Zhao, Daohui; Zhou, Jian

2014-09-30

In this work, the adsorptions of hydrophobin (HFBI) on four different self-assembled monolayers (SAMs) (i.e., CH3-SAM, OH-SAM, COOH-SAM, and NH2-SAM) were investigated by parallel tempering Monte Carlo and molecular dynamics simulations. Simulation results indicate that the orientation of HFBI adsorbed on neutral surfaces is dominated by a hydrophobic dipole. HFBI adsorbs on the hydrophobic CH3-SAM through its hydrophobic patch and adopts a nearly vertical hydrophobic dipole relative to the surface, while it is nearly horizontal when adsorbed on the hydrophilic OH-SAM. For charged SAM surfaces, HFBI adopts a nearly vertical electric dipole relative to the surface. HFBI has the narrowest orientation distribution on the CH3-SAM, and thus can form an ordered monolayer and reverse the wettability of the surface. For HFBI adsorption on charged SAMs, the adsorption strength weakens as the surface charge density increases. Compared with those on other SAMs, a larger area of the hydrophobic patch is exposed to the solution when HFBI adsorbs on the NH2-SAM. This leads to an increase of the hydrophobicity of the surface, which is consistent with the experimental results. The binding of HFBI to the CH3-SAM is mainly through hydrophobic interactions, while it is mediated through a hydration water layer near the surface for the OH-SAM. For the charged SAM surfaces, the adsorption is mainly induced by electrostatic interactions between the charged surfaces and the oppositely charged residues. The effect of a hydrophobic dipole on protein adsorption onto hydrophobic surfaces is similar to that of an electric dipole for charged surfaces. Therefore, the hydrophobic dipole may be applied to predict the probable orientations of protein adsorbed on hydrophobic surfaces.

Precision Blasting Techniques For Avalanche Control

NASA Astrophysics Data System (ADS)

Powell, Kevin M.

Experimental firings sponsored by the Center For Snow Science at Alta, Utah have demonstrated the potential of a unique prototype shaped charge device designed to stimulate snow pack and ice. These studies, conducted against stable snow pack, demonstrated a fourfold increase in crater volume yield and introduced a novel application of Shock Tube technology to facilitate position control, detonation and dud recovery of manually deployed charges. The extraordinary penetration capability of the shaped charge mechanism has been exploited in many non-military applications to meet a wide range of rapidpiercing and/or cutting requirements. The broader exploitation of the potential of the shaped charge mechanism has nevertheless remained confined to defence based applications. In the studies reported in this paper, the inimitable ability of the shaped charge mechanism to project shock energy, or a liner material, into a highly focussed energetic stream has been applied uniquely to the stimulation of snow pack. Recent research and development work, conducted within the UK, has resulted in the integration of shaped charge technology into a common Avalauncher and hand charge device. The potential of the common charge configuration and spooled Shock Tube fire and control system to improve the safety and cost effectiveness of explosives used in avalanche control operations was successfully demonstrated at Alta in March 2001. Future programmes of study will include focussed shock/blast mechanisms for suspended wire traverse techniques, application of the shaped charge mechanism to helibombing, and the desig n and development of non-fragmenting shaped charge ammunition formilitary artillery gun systems.

Phosphorus solubility of agricultural soils: a surface charge and phosphorus-31 NMR speciation study

USDA-ARS?s Scientific Manuscript database

We investigated ten soils from six states in United States to determine the relationship between potentiometric titration derived soil surface charge and Phosphorus-31 (P) nuclear magnetic resonance (NMR) speciation with the concentration of water-extractable P (WEP). The surface charge value at the...

Charge gradient microscopy

DOEpatents

Roelofs, Andreas; Hong, Seungbum

2018-02-06

A method for rapid imaging of a material specimen includes positioning a tip to contact the material specimen, and applying a force to a surface of the material specimen via the tip. In addition, the method includes moving the tip across the surface of the material specimen while removing electrical charge therefrom, generating a signal produced by contact between the tip and the surface, and detecting, based on the data, the removed electrical charge induced through the tip during movement of the tip across the surface. The method further includes measuring the detected electrical charge.

Variable Charge Soils: Mineralogy and Chemistry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Qafoku, Nik; Van Ranst, Eric; Noble, Andrew

2003-11-01

Soils rich in particles with amphoteric surface properties in the Oxisols, Ultisols, Alfisols, Spodosols and Andisols orders (1) are considered variable charge soils (2). The term “variable charge” is used to describe organic and inorganic soil constituents with reactive surface groups whose charge varies with pH, ionic concentration and composition of the soil solution. Such groups are the surface carboxyl, phenolic and amino functional groups of organic materials in soils, and surface hydroxyl groups of Fe and Al oxides, allophane and imogolite. The hydroxyl surface groups are also present on edges of some phyllosilicate minerals such as kaolinite, mica, andmore » hydroxyl-interlayered vermiculite. The variable charge is developed on the surface groups as a result of adsorption or desorption of ions that are constituents of the solid phase, i.e., H+, and the adsorption or desorption of solid-unlike ions that are not constituents of the solid. Highly weathered soils usually undergo isoeletric weathering and reach a “zero net charge” stage during their development. They have a slightly acidic to acidic soil solution pH, which is close to either point of zero net charge (PZNC) (3) or point of zero salt effect (PZSE) (3). They are characterized by high abundances of minerals with a point of zero net proton charge (PZNPC) (3) at neutral and slightly basic pHs; the most important being Fe and Al oxides and allophane. Under acidic conditions, the surfaces of these minerals are net positively charged. In contrast, the surfaces of permanent charge phyllosilicates are negatively charged regardless of ambient conditions. Variable charge soils therefore, are heterogeneous charge systems. The coexistence and interactions of oppositely charged surfaces or particles confers a different pattern of physical and chemical behavior on the soil, relatively to a homogeneously charged system of temperate regions. In some variable charge soils (Oxisols and some Ultisols developed on ferromagnesian-rich parent materials) the surfaces of phyllosilicates are coated to a lesser or greater extent by amorphous or crystalline, oppositely charged nanoparticles of Fe and Al oxides. These coatings exhibit a high reactive surface area and help cementing larger particles with one another. As a result of these electrostatic interactions, stable microaggregates that are difficult to disperse are formed in variable charge soils. Most of highly weathered soils have reached the “advanced stage” of Jackson-Sherman weathering sequence that is characterized by the removal of Na, K, Ca, Mg, and Fe(II), the presence of Fe and Al polymers, and very dilute soil solutions with an ionic strength (IS) of less than 1 mmol L-1. The inter-penetration or overlapping of the diffuse double layers on oppositely charged surfaces may occur in these dilute systems. These diffuse layer interactions may affect the magnitude of the effective charge, i.e., the counter-ion charge (4). In addition, salt adsorption, which is defined as the simultaneous adsorption in equivalent amounts of the cation and anion of an electrolyte with no net release of other ions into the soil solution, appears to be a common phenomenon in these soils. They act as cation- and anion-exchangers and as salt-sorbers. The magnitude of salt adsorption depends strongly on initial IS in the soil solution and the presence in appreciable amounts of oppositely charged surfaces. Among the authors that have made illustrious contributions towards a better understanding of these fascinating soil systems are S. Matson, R.K. Schofield, van Olphen, M.E. Sumner, G.W. Thomas, G.P. Gillman, G. Uehara, B.K.G. Theng, K. Wada, N.J. Barrow, J.W. Bowden, R.J. Hunter and G. Sposito. This entry is mainly based on publications by these authors.« less

Effect of Surfaces on Amyloid Fibril Formation

PubMed Central

Moores, Bradley; Drolle, Elizabeth; Attwood, Simon J.; Simons, Janet; Leonenko, Zoya

2011-01-01

Using atomic force microscopy (AFM) we investigated the interaction of amyloid beta (Aβ) (1–42) peptide with chemically modified surfaces in order to better understand the mechanism of amyloid toxicity, which involves interaction of amyloid with cell membrane surfaces. We compared the structure and density of Aβ fibrils on positively and negatively charged as well as hydrophobic chemically-modified surfaces at physiologically relevant conditions. We report that due to the complex distribution of charge and hydrophobicity amyloid oligomers bind to all types of surfaces investigated (CH3, COOH, and NH2) although the charge and hydrophobicity of surfaces affected the structure and size of amyloid deposits as well as surface coverage. Hydrophobic surfaces promote formation of spherical amorphous clusters, while charged surfaces promote protofibril formation. We used the nonlinear Poisson-Boltzmann equation (PBE) approach to analyze the electrostatic interactions of amyloid monomers and oligomers with modified surfaces to complement our AFM data. PMID:22016789

Parallel tempering Monte Carlo simulations of lysozyme orientation on charged surfaces

NASA Astrophysics Data System (ADS)

Xie, Yun; Zhou, Jian; Jiang, Shaoyi

2010-02-01

In this work, the parallel tempering Monte Carlo (PTMC) algorithm is applied to accurately and efficiently identify the global-minimum-energy orientation of a protein adsorbed on a surface in a single simulation. When applying the PTMC method to simulate lysozyme orientation on charged surfaces, it is found that lysozyme could easily be adsorbed on negatively charged surfaces with "side-on" and "back-on" orientations. When driven by dominant electrostatic interactions, lysozyme tends to be adsorbed on negatively charged surfaces with the side-on orientation for which the active site of lysozyme faces sideways. The side-on orientation agrees well with the experimental results where the adsorbed orientation of lysozyme is determined by electrostatic interactions. As the contribution from van der Waals interactions gradually dominates, the back-on orientation becomes the preferred one. For this orientation, the active site of lysozyme faces outward, which conforms to the experimental results where the orientation of adsorbed lysozyme is co-determined by electrostatic interactions and van der Waals interactions. It is also found that despite of its net positive charge, lysozyme could be adsorbed on positively charged surfaces with both "end-on" and back-on orientations owing to the nonuniform charge distribution over lysozyme surface and the screening effect from ions in solution. The PTMC simulation method provides a way to determine the preferred orientation of proteins on surfaces for biosensor and biomaterial applications.

Effect of electrical polarization of hydroxyapatite ceramics on new bone formation.

PubMed

Itoh, S; Nakamura, S; Kobayashi, T; Shinomiya, K; Yamashita, K; Itoh, S

2006-03-01

Large surface charges can be induced on hydroxyapatite (HAp) ceramics by proton transport polarization, but this does not affect beta-tricalcium phosphate (TCP) because of its low polarizability. We wished to examine differences in osteogenic cell activity and new bone growth between positively or negatively surface-charged HAp and HAp/TCP plates using a calvarial bone defect model. In the first group of rats, test pieces were placed with their positively charged surfaces face down on the dura mater. In the second group, test pieces were placed with their negatively charged surfaces face down on the dura mater. A third group received noncharged test pieces. Histological examination, including enzymatic staining for osteoblasts and osteoclasts, was carried out. While no bone formation was observed at the pericranium, direct bone formation on the cranial bone debris and new bone growth expanded from the margins of the sites of injury to bridge across both the positively and negatively charged surfaces of HAp and HAp/TCP plates occurred. Electrical polarization of implanted plates, including positive charge, led to enhanced osteoblast activity, though decreased osteoclast activity was seen on the positively charged plate surface. Thus, polarization of HAp ceramics may modulate new bone formation and resorption.

PALS and SPM/EFM investigation of charged nanoporous electret films

NASA Astrophysics Data System (ADS)

Chiang, Dar-Ming; Liu, Wen-Liang; Chen, Jen-Luan; Susuki, Ryoichi

2005-08-01

The electret properties of nanoporous Teflon-FEP films, fabricated by the super-critical fluids method and charged by the corona method at room temperature, are investigated. PALS and SAXS are applied first to examine the charge characteristics of a free volume of electret materials. The topography and surface charges of electret materials are determined by scanning probe microscopy and electric field microscopy, respectively. The experimental results reveal that the interior surface areas of the pores of the electret materials influence the retention and stability of charge. Initial and aged surface charge was increased by factors of two and ten, with and without nanoporous Teflon-FEP films, respectively.

Targeting the lymphatics using dendritic polymers (dendrimers).

PubMed

Kaminskas, Lisa M; Porter, Christopher J H

2011-09-10

Dendrimers are unique biomaterials that are constructed by the stepwise addition of layers (generations) of polymer around a central core. They can be constructed with a range of molecular weights and have a polyfunctional surface that facilitates the attachment of drugs and pharmacokinetic modifiers such PEG or targeting moieties. These properties have led to considerable interest in the development of dendrimers for a range of biomedical applications. After subcutaneous administration, larger dendrimers in particular (> 8 nm), preferentially drain from the injection site into the peripheral lymphatic capillaries and therefore have potential as lymphatic imaging agents for magnetic resonance and optical fluorescence lymphangiography and as vectors for drug-targeting to lymphatic sites of disease progression. In general, lymphatic targeting of dendrimers is enhanced by increasing size although ultimately larger constructs may be incompletely absorbed from the injection site. Increasing hydrophilicity and reducing surface charge enhances drainage from subcutaneous injection sites, but the reverse is true of uptake into lymph nodes where charge and hydrophobicity promote retention. Larger hydrophilic dendrimers are also capable of extravasation from the systemic circulation, absorption into the lymphatic system and recirculation into the blood. Lymphatic recirculation may therefore be a characteristic of PEGylated dendrimers with long systemic circulation times. Copyright © 2011 Elsevier B.V. All rights reserved.

Solar Wind Access to Lunar Polar Craters: Feedback Between Surface Charging and Plasma Expansion

NASA Technical Reports Server (NTRS)

Zimmerman, M. I.; Farrell, W. M.; Stubbs, T. J.; Halekas, J. S.; Jackson, T. L.

2011-01-01

Determining the plasma environment within permanently shadowed lunar craters is critical to understanding local processes such as surface charging, electrostatic dust transport, volatile sequestration, and space weathering. In order to investigate the nature of this plasma environment, the first two-dimensional kinetic simulations of solar wind expansion into a lunar crater with a self-consistent plasma-surface interaction have been undertaken. The present results reveal how the plasma expansion into a crater couples with the electrically-charged lunar surface to produce a quasi-steady wake structure. In particular, there is a negative feedback between surface charging and ambipolar wake potential that allows an equilibrium to be achieved, with secondary electron emission strongly moderating the process. A range of secondary electron yields is explored, and two distinct limits are highlighted in which either surface charging or ambipoiar expansion is responsible for determining the overall wake structure.

Microelectrophoretic study of calcium oxalate monohydrate in macromolecular solutions

NASA Technical Reports Server (NTRS)

Curreri, P. A.; Onoda, G. Y., Jr.; Finlayson, B.

1987-01-01

Electrophoretic mobilities were measured for calcium oxalate monohydrate (COM) in solutions containing macromolecules. Two mucopolysaccharides (sodium heparin and chondroitin sulfate) and two proteins (positively charged lysozyme and negatively charged bovine serum albumin) were studied as adsorbates. The effects of pH, calcium oxalate surface charge (varied by calcium or oxalate ion activity), and citrate concentration were investigated. All four macromolecules showed evidence for adsorption. The macromolecule concentrations needed for reversing the surface charge indicated that the mucopolysaccharides have greater affinity for the COM surface than the proteins. Citrate ions at high concentrations appear to compete effectively with the negative protein for surface sites but show no evidence for competing with the positively charged protein.

Structural charge site influence on the interlayer hydration of expandable three-sheet clay minerals

USGS Publications Warehouse

Kerns, Raymond L.; Mankin, Charles J.

1968-01-01

Previous investigations have demonstrated the influences of interlayer cation composition, relative humidity, temperature, and magnitude of interlayer surface charge on the interlayer hydration of montmorillonites and vermiculites. It has been suggested that the sites of layer charge deficiencies may also have an influence upon the amount of hydration that can take place in the interlayers of expandable clay minerals. If the interlayer cation-to-layer bonds are considered as ideally electrostatic, the magnitude of the forces resisting expansion may be expressed as a form of Coulomb's law. If this effect is significant, expandable structures in which the charge-deficiency sites are predominantly in the tetrahedral sheet should have less pronounced swelling properties than should structures possessing charge deficiencies located primarily in the octahedral sheet.Three samples that differed in location of layer charge sites were selected for study. An important selection criterion was a non-correlation between tetrahedral charge sites and high surface-charge density, and between octahedral charge sites and low surface-charge density.The effects of differences in interlayer cation composition were eliminated by saturating portions of each sample with the same cations. Equilibrium (001) d values at controlled constant humidities were used as a measure of the relative degree of interlayer hydration.Although no correlation could be made between the degree of interlayer hydration and total surface-charge density, the investigation does not eliminate total surface-charge density as being significant to the swelling properties of three-sheet clay-mineral structures. The results do indicate a correlation between more intense expandability and predominance of charge deficiencies in the octahedral sheet. Conversely, less intense swelling behavior is associated with predominantly tetrahedral charge deficiencies.

The role of surface charge on the uptake and biocompatibility of hydroxyapatite nanoparticles with osteoblast cells

PubMed Central

Chen, Liang; Mccrate, Joseph M.; Lee, James C-M.; Li, Hao

2011-01-01

The objective of this study is to evaluate the effect of hydroxyapatite (HAP) nanoparticles with different surface charges on the cellular uptake behavior and in vitro cell viability and proliferation of MC3T3-E1 cell lines (osteoblast). The nanoparticles surface charge was varied by the surface modification with two carboxylic acids: 12-aminododecanoic acid (positive) and dodecanedioic acid (negative). The untreated HAP nanoparticles and dodecanoic acid modified HAP nanoparticles (neutral) were used as the control. X-ray diffraction (XRD) revealed that surface modifications by the three carboxylic acids did not change the crystal structure of HAP nanoparticles; Fourier transform infrared spectroscopy (FTIR) confirmed the adsorption and binding of the carboxylic acids on HAP nanoparticle surface; and zeta potential measurement confirmed that the chemicals successfully modified the surface charge of HAP nanoparticles in water based solution. Transmission electron microscopy (TEM) images showed that positively charged, negatively charged and untreated HAP nanoparticles, with similar size and shape, all penetrated into the cells and cells had more uptake of HAP nanoparticles with positive charge compared to those with negative charge, which might be attributed to the attractive or repulsive interaction between the negatively charged cell membrane and positively/negatively charged HAP nanoparticles. The neutral HAP nanoparticles could not penetrate cell membrane due to the larger size. MTT assay and LDH assay results indicated that as compared with the polystyrene control, greater cell viability and cell proliferation were measured on MC3T3-E1 cells treated with the three kinds of the HAP nanoparticles (neutral, positive, and untreated), among which positively charged HAP nanoparticles shows strongest improvement for cell viability and cell proliferation. In summary, the surface charge of HAP nanoparticles can be modified to influence the cellular uptake of HAP nanoparticles and the different uptake also influence the behavior of cells. These in-vitro results may also provide useful information for investigations of HAP nanoparticles applications in the gene delivery and intracellular drug delivery. PMID:21289408

Charge Retention by Monodisperse Gold Clusters on Surfaces Prepared Using Soft Landing of Mass Selected Ions

NASA Astrophysics Data System (ADS)

Johnson, Grant; Priest, Thomas; Laskin, Julia

2012-02-01

Monodisperse gold clusters have been prepared on surfaces in different charge states through soft landing of mass-selected ions. Gold clusters were synthesized in methanol solution by reduction of a gold precursor with a weak reducing agent in the presence of a diphosphine capping ligand. Electrospray ionization was used to introduce the clusters into the gas-phase and mass-selection was employed to isolate a single ionic cluster species which was delivered to surfaces at well controlled kinetic energies. Using in-situ time of flight secondary ion mass spectrometry (SIMS) it is demonstrated that the cluster retains its 3+ charge state when soft landed onto the surface of a fluorinated self assembled monolayer on gold. In contrast, when deposited onto carboxylic acid terminated and conventional alkyl thiol surfaces on gold the clusters exhibit larger relative abundances of the 2+ and 1+ charge states, respectively. The kinetics of charge reduction on the surface have been investigated using in-situ Fourier Transform Ion Cyclotron Resonance SIMS. It is shown that an extremely slow interfacial charge reduction occurs on the fluorinated monolayer surface while an almost instantaneous neutralization takes place on the surface of the alkyl thiol monolayer. Our results demonstrate that the size and charge state of small gold clusters on surfaces, both of which exert a dramatic influence on their chemical and physical properties, may be tuned through soft landing of mass-selected ions onto selected substrates.

Studies of oxidation and thermal reduction of the Cu(100) surface using a slow positron beam

NASA Astrophysics Data System (ADS)

Maddox, W. B.; Fazleev, N. G.; Nadesalingam, M. P.; Weiss, A. H.

2007-10-01

Positron probes of surfaces of oxides that play a fundamental role in modern science and technology are capable to non-destructively provide information that is both unique to the probe and complimentary to that extracted using other more standard techniques. We discuss recent progress in studies of oxidation and thermal reduction of the Cu(100) surface using positron-annihilation-induced Auger-electron spectroscopy (PAES). PAES measurements show a large increase in the intensity of the Cu M2,3VV Auger peak as the sample is subjected to a series of isochronal anneals in vacuum up to annealing temperature 300 C. The intensity then decreases monotonically as the annealing temperature is increased to 600 C. Experimental PAES results are analyzed by performing calculations of positron surface states and annihilation probabilities of surface-trapped positrons with relevant core electrons taking into account the charge redistribution at the surface and surface reconstruction. The effects of oxygen adsorption and defects on localization of the positron surface state wave function and positron annihilation characteristics are also analyzed. Possible explanations are provided for the observed behavior of the intensity of the positron annihilation induced Cu M2,3VV Auger peak with changes of the annealing temperature.

A Spacecraft Charging Capability for SXTF.

DTIC Science & Technology

1979-01-17

surfaces can charge up. ’Iiiis differential charging of satellite surfaces can cause vacutum sparks , and dielectric breakdowns, and wi 11 effect the S...times required to reach steady charge state in the spacecraft internal dielectrics upon electron irradiation. In space , typical times (order of magni...WORDS (Continue on reverse side it necessary end Identify by block nunmber) Spacecraft charging Dielectric breakdown SGEMP Electron accelerators

Precise control of surface electrostatic forces on polymer brush layers with opposite charges for resistance to protein adsorption.

PubMed

Sakata, Sho; Inoue, Yuuki; Ishihara, Kazuhiko

2016-10-01

Various molecular interaction forces are generated during protein adsorption process on material surfaces. Thus, it is necessary to control them to suppress protein adsorption and the subsequent cell and tissue responses. A series of binary copolymer brush layers were prepared via surface-initiated atom transfer radical polymerization, by mixing the cationic monomer unit and anionic monomer unit randomly in various ratios. Surface characterization revealed that the constructed copolymer brush layers exhibited an uniform super-hydrophilic nature and different surface potentials. The strength of the electrostatic interaction forces operating on these mixed-charge copolymer brush surfaces was evaluated quantitatively using force-versus-distance (f-d) curve measurements by atomic force microscopy (AFM) and probes modified by negatively charged carboxyl groups or positively charged amino groups. The electrostatic interaction forces were determined based on the charge ratios of the copolymer brush layers. Notably, the surface containing equivalent cationic/anionic monomer units hardly interacted with both the charged groups. Furthermore, the protein adsorption force and the protein adsorption mass on these surfaces were examined by AFM f-d curve measurement and surface plasmon resonance measurement, respectively. To clarify the influence of the electrostatic interaction on the protein adsorption behavior on the surface, three kinds of proteins having negative, positive, and relatively neutral net charges under physiological conditions were used in this study. We quantitatively demonstrated that the amount of adsorbed proteins on the surfaces would have a strong correlation with the strength of surface-protein interaction forces, and that the strength of surface-protein interaction forces would be determined from the combination between the properties of the electrostatic interaction forces on the surfaces and the charge properties of the proteins. Especially, the copolymer brush surface composed of equivalent cationic/anionic monomer units exhibited no significant interaction forces, and dramatically suppressed the adsorption of proteins regardless of their charge properties. We conclude that the established methodology could elucidate relationship between the protein adsorption behavior and molecular interaction, especially the electrostatic interaction forces, and demonstrated that the suppression of the electrostatic interactions with the ionic functional groups would be important for the development of new polymeric biomaterials with a high repellency of protein adsorption. Copyright © 2016 Elsevier Ltd. All rights reserved.

The role of interfacial water layer in atmospherically relevant charge separation

NASA Astrophysics Data System (ADS)

Bhattacharyya, Indrani

Charge separation at interfaces is important in various atmospheric processes, such as thunderstorms, lightning, and sand storms. It also plays a key role in several industrial processes, including ink-jet printing and electrostatic separation. Surprisingly, little is known about the underlying physics of these charging phenomena. Since thin films of water are ubiquitous, they may play a role in these charge separation processes. This talk will focus on the experimental investigation of the role of a water adlayer in interfacial charging, with relevance to meteorologically important phenomena, such as atmospheric charging due to wave actions on oceans and sand storms. An ocean wave generates thousands of bubbles, which upon bursting produce numerous large jet droplets and small film droplets that are charged. In the 1960s, Blanchard showed that the jet droplets are positively charged. However, the charge on the film droplets was not known. We designed an experiment to exclusively measure the charge on film droplets generated by bubble bursting on pure water and aqueous salt solution surfaces. We measured their charge to be negative and proposed a model where a slight excess of hydroxide ions in the interfacial water layer is responsible for generating these negatively charged droplets. The findings from this research led to a better understanding of the ionic disposition at the air-water interface. Sand particles in a wind-blown sand layer, or 'saltation' layer, become charged due to collisions, so much so, that it can cause lightning. Silica, being hydrophilic, is coated with a water layer even under low-humidity conditions. To investigate the importance of this water adlayer in charging the silica surfaces, we performed experiments to measure the charge on silica surfaces due to contact and collision processes. In case of contact charging, the maximum charge separation occurred at an optimum relative humidity. On the contrary, in collisional charging process, no humidity effect was observed. We proposed an ion transfer mechanism in case of contact charging. However, an electron transfer mechanism explained the collisional charging process. The effects of temperature, surface roughness, and chemical nature of surface were also studied for both contact and collisional charging processes.

Polyelectrolytes tethered to a free surface

NASA Astrophysics Data System (ADS)

Dubreuil, F.; Guenoun, P.

Several attempts have been already carried out in order to tether charged chains by an end at a free fluctuating surface. We review here most of these attempts and focus on how close the physics of charged brushes can be investigated by such an approach. We first describe results about films of charged-neutral diblock copolymers spread at the surface of water. Results can be mostly rationalized in terms of charged brushes although additional structurations and fluctuations of the interface can be observed. The latter deformations are also observed when adsorbed layers of charged-neutral diblock copolymers are considered. At last, we examine how free suspended films of charged-neutral diblock copolymers can be viewed as two opposing charged brushes, both in terms of thickness and pressure.

Probing charge transfer in a novel class of luminescent perovskite-based heterostructures composed of quantum dots bound to RE-activated CaTiO 3 phosphors

DOE PAGES

Crystal S. Lewis; Wong, Stanislaus S.; Liu, Haiqing; ...

2016-01-04

We report on the synthesis and structural characterization of novel semiconducting heterostructures composed of cadmium selenide (CdSe) quantum dots (QDs) attached onto the surfaces of novel high-surface area, porous rare-earth-ion doped alkaline earth titanate micron-scale spherical motifs, i.e. both Eu-doped and Pr-doped CaTiO 3, composed of constituent, component nanoparticles. These unique metal oxide perovskite building blocks were created by a multi-pronged synthetic strategy involving molten salt and hydrothermal protocols. Subsequently, optical characterization of these heterostructures indicated a clear behavioral dependence of charge transfer in these systems upon a number of parameters such as the nature of the dopant, the reactionmore » temperature, and particle size. Specifically, 2.7 nm diameter ligand-functionalized CdSe QDs were anchored onto sub-micron sized CaTiO 3-based spherical assemblies, prepared by molten salt protocols. We found that both the Pr- and Eu-doped CaTiO 3 displayed pronounced PL emissions, with maximum intensities observed using optimized lanthanide concentrations of 0.2 mol% and 6 mol%, respectively. Analogous experiments were performed on Eu-doped BaTiO 3 and SrTiO 3 motifs, but CaTiO 3 still performed as the most effective host material amongst the three perovskite systems tested. Furthermore, the ligand-capped CdSe QD-doped CaTiO 3 heterostructures exhibited effective charge transfer between the two individual constituent nanoscale components, an assertion corroborated by the corresponding quenching of their measured PL signals.« less

From two-dimensional graphene oxide to three-dimensional honeycomb-like Ni3S2@graphene oxide composite: insight into structure and electrocatalytic properties

NASA Astrophysics Data System (ADS)

Wei, Xinting; Li, Yueqiang; Xu, Wenli; Zhang, Kaixuan; Yin, Jie; Shi, Shaozhen; Wei, Jiazhen; Di, Fangfang; Guo, Junxue; Wang, Can; Chu, Chaofan; Sui, Ning; Chen, Baoli; Zhang, Yingtian; Hao, Hongguo; Zhang, Xianxi; Zhao, Jinsheng; Zhou, Huawei; Wang, Shuhao

2017-12-01

Three-dimensional (3D) graphene composites have drawn increasing attention in energy storage/conversion applications due to their unique structures and properties. Herein, we synthesized 3D honeycomb-like Ni3S2@graphene oxide composite (3D honeycomb-like Ni3S2@GO) by a one-pot hydrothermal method. We found that positive charges of Ni2+ and negative charges of NO_{3^{- in Ni(NO3)2 induced a transformation of graphene oxide with smooth surface into graphene oxide with wrinkled surface (w-GO). The w-GO in the mixing solution of Ni(NO3)2/thioacetamide/H2O evolved into 3D honeycomb-like Ni3S2@GO in solvothermal process. The GO effectively inhibited the aggregation of Ni3S2 nanoparticles. Photoelectrochemical cells based on 3D Ni3S2@GO synthesized at 60 mM l-1 Ni(NO3)2 exhibited the best energy conversion efficiency. 3D Ni3S2@GO had smaller charge transfer resistance and larger exchange current density than pure Ni3S2 for iodine reduction reaction. The cyclic stability of 3D honeycomb-like Ni3S2@GO was good in the iodine electrolyte. Results are of great interest for fundamental research and practical applications of 3D GO and its composites in solar water-splitting, artificial photoelectrochemical cells, electrocatalysts and Li-S or Na-S batteries.}}

Depletion region surface effects in electron beam induced current measurements.

PubMed

Haney, Paul M; Yoon, Heayoung P; Gaury, Benoit; Zhitenev, Nikolai B

2016-09-07

Electron beam induced current (EBIC) is a powerful characterization technique which offers the high spatial resolution needed to study polycrystalline solar cells. Current models of EBIC assume that excitations in the p - n junction depletion region result in perfect charge collection efficiency. However we find that in CdTe and Si samples prepared by focused ion beam (FIB) milling, there is a reduced and nonuniform EBIC lineshape for excitations in the depletion region. Motivated by this, we present a model of the EBIC response for excitations in the depletion region which includes the effects of surface recombination from both charge-neutral and charged surfaces. For neutral surfaces we present a simple analytical formula which describes the numerical data well, while the charged surface response depends qualitatively on the location of the surface Fermi level relative to the bulk Fermi level. We find the experimental data on FIB-prepared Si solar cells is most consistent with a charged surface, and discuss the implications for EBIC experiments on polycrystalline materials.

Significance of surface charge and shell material of superparamagnetic iron oxide nanoparticle (SPION) based core/shell nanoparticles on the composition of the protein corona.

PubMed

Sakulkhu, Usawadee; Mahmoudi, Morteza; Maurizi, Lionel; Coullerez, Geraldine; Hofmann-Amtenbrink, Margarethe; Vries, Marcel; Motazacker, Mahdi; Rezaee, Farhad; Hofmann, Heinrich

2015-02-01

As nanoparticles (NPs) are increasingly used in many applications their safety and efficient applications in nanomedicine have become concerns. Protein coronas on nanomaterials' surfaces can influence how the cell "recognizes" nanoparticles, as well as the in vitro and in vivo NPs' behaviors. The SuperParamagnetic Iron Oxide Nanoparticle (SPION) is one of the most prominent agents because of its superparamagnetic properties, which is useful for separation applications. To mimic surface properties of different types of NPs, a core-shell SPION library was prepared by coating with different surfaces: polyvinyl alcohol polymer (PVA) (positive, neutral and negative), SiO2 (positive and negative), titanium dioxide and metal gold. The SPIONs with different surfaces were incubated at a fixed serum : nanoparticle surface ratio, magnetically trapped and washed. The tightly bound proteins were quantified and identified. The surface charge has a great impact on protein adsorption, especially on PVA and silica where proteins preferred binding to the neutral and positively charged surfaces. The importance of surface material on protein adsorption was also revealed by preferential binding on TiO2 and gold coated SPION, even negatively charged. There is no correlation between the protein net charge and the nanoparticle surface charge on protein binding, nor direct correlation between the serum proteins' concentration and the proteins detected in the coronas.

Laser-Assisted Field Evaporation and Three-Dimensional Atom-by-Atom Mapping of Diamond Isotopic Homojunctions.

PubMed

Mukherjee, Samik; Watanabe, Hideyuki; Isheim, Dieter; Seidman, David N; Moutanabbir, Oussama

2016-02-10

It addition to its high evaporation field, diamond is also known for its limited photoabsorption, strong covalent bonding, and wide bandgap. These characteristics have been thought for long to also complicate the field evaporation of diamond and make its control hardly achievable on the atomistic-level. Herein, we demonstrate that the unique behavior of nanoscale diamond and its interaction with pulsed laser lead to a controlled field evaporation thus enabling three-dimensional atom-by-atom mapping of diamond (12)C/(13)C homojunctions. We also show that one key element in this process is to operate the pulsed laser at high energy without letting the dc bias increase out of bounds for diamond nanotip to withstand. Herein, the role of the dc bias in evaporation of diamond is essentially to generate free charge carriers within the nanotip via impact ionization. The mobile free charges screen the internal electric field, eventually creating a hole rich surface where the pulsed laser is effectively absorbed leading to an increase in the nanotip surface temperature. The effect of this temperature on the uncertainty in the time-of-flight of an ion, the diffusion of atoms on the surface of the nanotip, is also discussed. In addition to paving the way toward a precise manipulation of isotopes in diamond-based nanoscale and quantum structures, this result also elucidates some of the basic properties of dielectric nanostructures under high electric field.

Metal-organic frameworks for lithium ion batteries and supercapacitors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ke, Fu-Sheng; Wu, Yu-Shan; Deng, Hexiang, E-mail: hdeng@whu.edu.cn

2015-03-15

Porous materials have been widely used in batteries and supercapacitors attribute to their large internal surface area (usually 100–1000 m{sup 2} g{sup −1}) and porosity that can favor the electrochemical reaction, interfacial charge transport, and provide short diffusion paths for ions. As a new type of porous crystalline materials, metal-organic frameworks (MOFs) have received huge attention in the past decade due to their unique properties, i.e. huge surface area (up to 7000 m{sup 2} g{sup −1}), high porosity, low density, controllable structure and tunable pore size. A wide range of applications including gas separation, storage, catalysis, and drug delivery benefitmore » from the recent fast development of MOFs. However, their potential in electrochemical energy storage has not been fully revealed. Herein, the present mini review appraises recent and significant development of MOFs and MOF-derived materials for rechargeable lithium ion batteries and supercapacitors, to give a glimpse into these potential applications of MOFs. - Graphical abstract: MOFs with large surface area and high porosity can offer more reaction sites and charge carriers diffusion path. Thus MOFs are used as cathode, anode, electrolyte, matrix and precursor materials for lithium ion battery, and also as electrode and precursor materials for supercapacitors. - Highlights: • MOFs have potential in electrochemical area due to their high porosity and diversity. • We summarized and compared works on MOFs for lithium ion battery and supercapacitor. • We pointed out critical challenges and provided possible solutions for future study.« less

Determination of the surface charge density and temperature dependence of purple membrane by electric force microscopy.

PubMed

Du, Huiwen; Li, Denghua; Wang, Yibing; Wang, Chenxuan; Zhang, Dongdong; Yang, Yan-lian; Wang, Chen

2013-08-29

We report here the measurement of the temperature-dependent surface charge density of purple membrane (PM) by using electrostatic force microscopy (EFM). The surface charge density was measured to be 3.4 × 10(5) e/cm(2) at room temperature and reaches the minimum at around 52 °C. The initial decrease of the surface charge density could be attributed to the reduced dipole alignment because of the thermally induced protein mobility in PM. The increase of charge density at higher temperature could be ascribed to the weakened interaction between proteins and the lipids, which leads to the exposure of the charged amino acids. This work could be a benefit to the direct assessment of the structural stability and electric properties of biological membranes at the nanoscale.

Surface-Charge-Based Micro-Models--A Solid Foundation for Learning about Direct Current Circuits

ERIC Educational Resources Information Center

Hirvonen, P. E.

2007-01-01

This study explores how the use of a surface-charge-based instructional approach affects introductory university level students' understanding of direct current (dc) circuits. The introduced teaching intervention includes electrostatics, surface-charge-based micro-models that explain the existence of an electric field inside the current-carrying…

Utilities Power Change: Engaging Commercial Customers in Workplace Charging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lommele, Stephen; Dafoe, Wendy

As stewards of an electric grid that is available almost anywhere people park, utilities that support workplace charging are uniquely positioned to help their commercial customers be a part of the rapidly expanding network of charging infrastructure. Utilities understand the distinctive challenges of their customers, have access to technical information about electrical infrastructure, and have deep experience modeling and managing demand for electricity. This case study highlights the experiences of two utilities with workplace charging programs.

Modulating interactions between ligand-coated nanoparticles and phase-separated lipid bilayers by varying the ligand density and the surface charge.

PubMed

Chen, Xiaojie; Tieleman, D Peter; Liang, Qing

2018-02-01

The interactions between nanoparticles and lipid bilayers are critical in applications of nanoparticles in nanomedicine, cell imaging, toxicology, and elsewhere. Here, we investigate the interactions between nanoparticles coated with neutral and/or charged ligands and phase-separated lipid bilayers using coarse-grained molecular dynamics simulation. Both penetration and adsorption processes as well as the final distribution of the nanoparticles can be readily modulated by varying the ligand density and the surface charge of the nanoparticles. Completely hydrophobic (neutral) nanoparticles with larger size initially preferentially penetrate into the liquid-disordered region of the lipid bilayer and finally transfer into the liquid-ordered region; partially hydrophilic nanoparticles with low or moderate surface charge tend to either distribute in the liquid-disordered region or be adsorbed on the surface of the lipid bilayer, while strongly hydrophilic nanoparticles with high surface charge always reside on the surface of the lipid bilayer. Interactions of the nanoparticles with the lipid bilayers are affected by the surface charge of nanoparticles, hydrophobic mismatch, bending of the ligands, and the packing state of the lipids. Insight in these factors can be used to improve the efficiency of designing nanoparticles for specific applications.

Modulation of Silica Nanoparticle Uptake into Human Osteoblast Cells by Variation of the Ratio of Amino and Sulfonate Surface Groups: Effects of Serum

PubMed Central

2015-01-01

To study the importance of the surface charge for cellular uptake of silica nanoparticles (NPs), we synthesized five different single- or multifunctionalized fluorescent silica NPs (FFSNPs) by introducing various ratios of amino and sulfonate groups into their surface. The zeta potential values of these FFSNPs were customized from highly positive to highly negative, while other physicochemical properties remained almost constant. Irrespective of the original surface charge, serum proteins adsorbed onto the surface, neutralized the zeta potential values, and prevented the aggregation of the tailor-made FFSNPs. Depending on the surface charge and on the absence or presence of serum, two opposite trends were found concerning the cellular uptake of FFSNPs. In the absence of serum, positively charged NPs were more strongly accumulated by human osteoblast (HOB) cells than negatively charged NPs. In contrast, in serum-containing medium, anionic FFSNPs were internalized by HOB cells more strongly, despite the similar size and surface charge of all types of protein-covered FFSNPs. Thus, at physiological condition, when the presence of proteins is inevitable, sulfonate-functionalized silica NPs are the favorite choice to achieve a desired high rate of NP internalization. PMID:26030456

Increasing binding density of yeast cells by control of surface charge with allylamine grafting to ion modified polymer surfaces.

PubMed

Tran, Clara T H; Kondyurin, Alexey; Chrzanowski, Wojciech; Bilek, Marcela M M; McKenzie, David R

2014-10-01

Plasma immersion ion implantation (PIII) treatment of polymers creates a biointerface capable of direct covalent immobilization of biomolecules. The immobilization of protein molecules is achieved by covalent bonds formed between embedded radicals on the treated surface and amino acid side chains and cells can be immobilized through cell-wall proteins. The attachment density of negatively charged entities on a PIII treated surface is inhibited by its negative surface charge at neutral pH. To reduce the negative charge of PIII treated surfaces in phosphate buffer (pH 7.4, 11mM), we develop an effective approach of grafting allylamine monomers onto the treated surface. The results reveal reactions between allylamine and radicals on the PIII treated surface. One of these triggers polymerization, increasing the number of amine groups grafted. As a consequence, the PIII treated polystyrene surface after allylamine exposure becomes more hydrophobic and less negatively charged in phosphate buffer. Using yeast cells as an example, we have shown a significant improvement (6-15 times) of cell density immobilized on the PIII treated surface after exposure to allylamine. Copyright © 2014 Elsevier B.V. All rights reserved.

The Electrical Structure of Discharges Modified by Electron Beams

NASA Astrophysics Data System (ADS)

Haas, F. A.; Braithwaite, N. St. J.

1997-10-01

Injection of an electron beam into a low pressure plasma modifies both the electrical structure and the distributions of charged particle energies. The electrical structure is investigated here in a one-dimensional model by representing the discharge as two collisionless sheaths with a monenergetic electron beam, linked by a quasi-neutral collisional region. The latter is modelled by fluid equations in which the beam current decreases with position. Since the electrodes are connected by an external conductor this implies through Kirchoff's laws that the thermal electron current must correspondingly increase with position. Given the boundary conditions and beam input at the first electrode then the rest of the system is uniquely described. The model reveals the dependence of the sheath potentials at the emitting and absorbing surfaces on the beam current. The model is relevant to externally injected beams and to electron beams originating from secondary processes on surfaces exposed to the plasma.

Lessons Learned in Thermal Coatings from the DSCOVR Mission

NASA Technical Reports Server (NTRS)

Abraham, Nithin S.

2015-01-01

Finding solutions to thermal coating issues on the Deep Space Climate Observatory (DSCOVR) mission was a very challenging and unique endeavor. As a passive thermal control system, coatings provide the desired thermal, optical, and electrical charging properties, while surviving a harsh space environment. DSCOVR mission hardware was repurposed from the late 1990s satellite known as Triana. As a satellite that was shelved for over a decade, the coating surfaces consequently degraded with age, and became fairly outdated. Although the mission successfully launched in February 2015, there were unfamiliar observations and unanticipated issues with the coating surfaces during the revival phases of the project. For example, the thermal coatings on DSCOVR experienced particulate contamination and resistivity requirement problems, among other issues. While finding solutions to these issues, valuable lessons were learned in thermal coatings that may provide great insight to future spaceflight missions in similar situations.

Two-Dimensional Titanium Carbide (MXene) as Surface-Enhanced Raman Scattering Substrate

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sarycheva, Asia; Makaryan, Taron; Maleski, Kathleen

Here, noble metal (gold or silver) nanoparticles or patterned films are typically used as substrates for surface-enhanced Raman spectroscopy (SERS). Two-dimensional (2D) carbides and nitrides (MXenes) exhibit unique electronic and optical properties, including metallic conductivity and plasmon resonance in the visible or near-infrared range, making them promising candidates for a wide variety of applications. Herein, we show that 2D titanium carbide, Ti 3C 2T x, enhances Raman signal from organic dyes on a substrate and in solution. As a proof of concept, MXene SERS substrates were manufactured by spray-coating and used to detect several common dyes, with calculated enhancement factorsmore » reaching ~10 6. Titanium carbide MXene demonstrates SERS effect in aqueous colloidal solutions, suggesting the potential for biomedical or environmental applications, where MXene can selectively enhance positively charged molecules.« less

Gold-Based Magneto/Optical Nanostructures: Challenges for In Vivo Applications in Cancer Diagnostics and Therapy.

PubMed

Melancon, Marites; Lu, Wei; Li, Chun

2009-06-01

Nanoparticles with gold shell and iron core have unique optical and magnetic properties which can be utilized for simultaneous detection and treatment strategies. Several nanoparticles have been synthesized and shown to mediate a variety of potential applications in biomedicine, including cancer molecular optical and magnetic resonance imaging, controlled drug delivery, and photothermal ablation therapy. However, to be effective, these nanoparticles must be delivered efficiently into their targets. In this review, we will provide an updated summary of the gold-shelled magnetic nanoparticles that have been synthesized, methods for characterization, and their potential for cancer diagnosis and treatment. We will also discuss the biological barriers that need to be overcome for the effective delivery of these nanoparticles. The desired nanoparticle characteristics needed to evade these biological barriers were also explained. Hopefully, this review will help researchers in designing nanoparticles by carefully choosing the optimum size, shape, surface charge, and surface coating.

Bioinspired ion-transport properties of solid-state single nanochannels and their applications in sensing.

PubMed

Tian, Ye; Wen, Liping; Hou, Xu; Hou, Guanglei; Jiang, Lei

2012-07-16

Biological ion channels are able to control ion-transport processes precisely because of their intriguing properties, such as selectivity, rectification, and gating. Learning from nature, scientists have developed a promising system--solid-state single nanochannels--to mimic biological ion-transport properties. These nanochannels have many impressive properties, such as excess surface charge, making them selective; the ability to be produced or modified asymmetrically, endowing them with rectification; and chemical reactivity of the inner surface, imparting them with desired gating properties. Based on these unique characteristics, solid-state single nanochannels have been explored in various applications, such as sensing. In this context, we summarize recent developments of bioinspired solid-state single nanochannels with ion-transport properties that resemble their biological counterparts, including selectivity, rectification, and gating; their applications in sensing are also introduced briefly. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Numerical modelling of needle-grid electrodes for negative surface corona charging system

NASA Astrophysics Data System (ADS)

Zhuang, Y.; Chen, G.; Rotaru, M.

2011-08-01

Surface potential decay measurement is a simple and low cost tool to examine electrical properties of insulation materials. During the corona charging stage, a needle-grid electrodes system is often used to achieve uniform charge distribution on the surface of the sample. In this paper, a model using COMSOL Multiphysics has been developed to simulate the gas discharge. A well-known hydrodynamic drift-diffusion model was used. The model consists of a set of continuity equations accounting for the movement, generation and loss of charge carriers (electrons, positive and negative ions) coupled with Poisson's equation to take into account the effect of space and surface charges on the electric field. Four models with the grid electrode in different positions and several mesh sizes are compared with a model that only has the needle electrode. The results for impulse current and surface charge density on the sample clearly show the effect of the extra grid electrode with various positions.

Behavior of micro-particles in monolith ceramic membrane filtration with pre-coagulation.

PubMed

Yonekawa, H; Tomita, Y; Watanabe, Y

2004-01-01

This paper is intended to clarify the characteristics unique to monolith ceramic membranes with pre-coagulation by referring to the behavior of micro-particles. Flow analysis and experiments have proved that monolith ceramic membranes show a unique flow pattern in the channels within the element, causing extremely rapid flocculation in the channel during dead-end filtration. It was assumed that charge-neutralized micro-particles concentrated near the membrane surface grow in size due to flocculation, and as a result, coarse micro-particles were taken up by the shearing force to flow out. As the dead end points of flow in all the channels are located near the end of the channels with higher filterability, most of the flocculated coarse particles are formed to a columnar cake intensively at the dead end point. Therefore cake layer forming on the membrane other than around the dead end point is alleviated. This behavior of particle flocculation and cake formation at the dead end point within the channels are unique characteristics of monolith ceramic membranes. This is why all monolith ceramic membrane water purification systems operating in Japan do not have pretreatment equipment for flocculation and sedimentation.

Protein interactions with layers of TiO2 nanotube and nanopore arrays: Morphology and surface charge influence.

PubMed

Kulkarni, Mukta; Mazare, Anca; Park, Jung; Gongadze, Ekaterina; Killian, Manuela Sonja; Kralj, Slavko; von der Mark, Klaus; Iglič, Aleš; Schmuki, Patrik

2016-11-01

In the present work we investigate the key factors involved in the interaction of small-sized charged proteins with TiO 2 nanostructures, i.e. albumin (negatively charged), histone (positively charged). We examine anodic nanotubes with specific morphology (simultaneous control over diameter and length, e.g. diameter - 15, 50 or 100nm, length - 250nm up to 10μm) and nanopores. The nanostructures surface area has a direct influence on the amount of bound protein, nonetheless the protein physical properties as electric charge and size (in relation to nanotopography and biomaterial's electric charge) are crucial too. The highest quantity of adsorbed protein is registered for histone, for 100nm diameter nanotubes (10μm length) while higher values are registered for 15nm diameter nanotubes when normalizing protein adsorption to nanostructures' surface unit area (evaluated from dye desorption measurements) - consistent with theoretical considerations. The proteins presence on the nanostructures is evaluated by XPS and ToF-SIMS; additionally, we qualitatively assess their presence along the nanostructures length by ToF-SIMS depth profiles, with decreasing concentration towards the bottom. Surface nanostructuring of titanium biomedical devices with TiO 2 nanotubes was shown to significantly influence the adhesion, proliferation and differentiation of mesenchymal stem cells (and other cells too). A high level of control over the nanoscale topography and over the surface area of such 1D nanostructures enables a direct influence on protein adhesion. Herein, we investigate and show how the nanostructure morphology (nanotube diameter and length) influences the interactions with small-sized charged proteins, using as model proteins bovine serum albumin (negatively charged) and histone (positively charged). We show that the protein charge strongly influences their adhesion to the TiO 2 nanostructures. Protein adhesion is quantified by ELISA measurements and determination of the nanostructures' total surface area. We use a quantitative surface charge model to describe charge interactions and obtain an increased magnitude of the surface charge density at the top edges of the nanotubes. In addition, we track the proteins presence on and inside the nanostructures. We believe that these aspects are crucial for applications where the incorporation of active molecules such as proteins, drugs, growth factors, etc., into nanotubes is desired. Copyright © 2016 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Dust Grain Charge above the Lunar terminator

NASA Astrophysics Data System (ADS)

Vaverka, Jakub; Richterova, Ivana; Nemecek, Zdenek; Safrankova, Jana; Pavlu, Jiri; Vysinka, Marek

Interaction of a lunar surface with the solar wind and magnetosphere leads to its charging by several processes as photoemission, a collection of primary particles, and secondary electron emission. Nevertheless, charging of the lunar surface is complicated by a shielding of solar light and solar wind ions by hills, craters, and boulders that can locally influence the surface potential. Moreover, a presence of a plasma wake can strongly affect this potential at the night side of the Moon. A typical surface potential varies from slightly positive (dayside) to negative values of the order of several hundred volts (night side). An electric field above the charged surface can lead to a levitation of dust grains as it has been observed by several spacecraft and by astronauts during Apollo missions. Although charging and transport of dust grains above the lunar surface are in the center of interest for many years, these phenomena are not still completely understood. We present calculation of an equilibrium potential of dust grains above the lunar surface. We focus on a terminator area during the Earth’s plasma sheet crossing. We use the secondary electron emission model for dust grains which takes into account an influence of the grain size, material, and surface roughness and findings from laboratory experiments with charging of lunar dust simulants by an electron beam.

Profiling Charge Complementarity and Selectivity for Binding at the Protein Surface

PubMed Central

Sulea, Traian; Purisima, Enrico O.

2003-01-01

A novel analysis and representation of the protein surface in terms of electrostatic binding complementarity and selectivity is presented. The charge optimization methodology is applied in a probe-based approach that simulates the binding process to the target protein. The molecular surface is color coded according to calculated optimal charge or according to charge selectivity, i.e., the binding cost of deviating from the optimal charge. The optimal charge profile depends on both the protein shape and charge distribution whereas the charge selectivity profile depends only on protein shape. High selectivity is concentrated in well-shaped concave pockets, whereas solvent-exposed convex regions are not charge selective. This suggests the synergy of charge and shape selectivity hot spots toward molecular selection and recognition, as well as the asymmetry of charge selectivity at the binding interface of biomolecular systems. The charge complementarity and selectivity profiles map relevant electrostatic properties in a readily interpretable way and encode information that is quite different from that visualized in the standard electrostatic potential map of unbound proteins. PMID:12719221

Chlorhexidine possesses unique cytotoxic actions in rat thymic lymphocytes: Its relation with electrochemical property of membranes.

PubMed

Nonami, Kayo; Saitoh, Shohei; Nishimura-Danjobara, Yumiko; Ishida, Shiro; Oyama, Yasuo

2016-12-01

Chlorhexidine (CHX) is an antibacterial agent used in various types of pharmaceutical products. Therefore, CHX is easily found around us. Owing to its positive charge, the electrochemical property of cell membranes was assumed to be a key point of cytotoxic action of CHX. Depolarization of membranes attenuated the cytotoxic action of CHX in rat thymic lymphocytes. CHX interfered with annexin V binding to membranes. Manipulations to induce exposure of phosphatidylserine on the outer membrane surface augmented the cytotoxic action of CHX, indicating that changes in the electrochemical property of membranes affected the cytotoxic action of CHX. Hence, CHX might kill cells physiologically undergoing apoptosis, resulting instead in necrotic cell death. However, the threshold CHX concentration in this in vitro study was slightly higher than blood CHX concentrations observed clinically. Therefore, these results may support the safety of CHX use although CHX possesses unique cytotoxic actions described in this study. Copyright © 2016 Elsevier B.V. All rights reserved.

Acentric 2-D ensembles of D-br-A electron-transfer chromophores via vectorial orientation within amphiphilic n-helix bundle peptides for photovoltaic device applications.

PubMed

Koo, Jaseung; Park, Jaehong; Tronin, Andrey; Zhang, Ruili; Krishnan, Venkata; Strzalka, Joseph; Kuzmenko, Ivan; Fry, H Christopher; Therien, Michael J; Blasie, J Kent

2012-02-14

We show that simply designed amphiphilic 4-helix bundle peptides can be utilized to vectorially orient a linearly extended donor-bridge-acceptor (D-br-A) electron transfer (ET) chromophore within its core. The bundle's interior is shown to provide a unique solvation environment for the D-br-A assembly not accessible in conventional solvents and thereby control the magnitudes of both light-induced ET and thermal charge recombination rate constants. The amphiphilicity of the bundle's exterior was employed to vectorially orient the peptide-chromophore complex at a liquid-gas interface, and its ends were tailored for subsequent covalent attachment to an inorganic surface, via a "directed assembly" approach. Structural data, combined with evaluation of the excited state dynamics exhibited by these peptide-chromophore complexes, demonstrate that densely packed, acentrically ordered 2-D monolayer ensembles of such complexes at high in-plane chromophore densities approaching 1/200 Å(2) offer unique potential as active layers in binary heterojunction photovoltaic devices.

Vacuum Potentials for the Two Only Permanent Free Particles, Proton and Electron. Pair Productions

NASA Astrophysics Data System (ADS)

Zheng-Johansson, J. X.

2012-02-01

The two only species of isolatable, smallest, or unit charges +e and -e present in nature interact with the universal vacuum in a polarisable dielectric representation through two uniquely defined vacuum potential functions. All of the non-composite subatomic particles containing one-unit charges, +e or -e, are therefore formed in terms of the IED model of the respective charges, of zero rest masses, oscillating in either of the two unique vacuum potential fields, together with the radiation waves of their own charges. In this paper we give a first principles treatment of the dynamics of charge in a dielectric vacuum, based on which, combined with solutions for the radiation waves obtained previously, we subsequently derive the vacuum potential function for a given charge q, which we show to be quadratic and consist each of quantised potential levels, giving therefore rise to quantised characteristic oscillation frequencies of the charge and accordingly quantised, sharply-defined masses of the IED particles. By further combining with relevant experimental properties as input information, we determine the IED particles built from the charges +e, -e at their first excited states in the respective vacuum potential wells to be the proton and the electron, the observationally two only stable (permanently lived) and "free" particles containing one-unit charges. Their antiparticles as produced in pair productions can be accordingly determined. The characteristics of all of the other more energetic single-charged non-composite subatomic particles can also be recognised. We finally discuss the energy condition for pair production, which requires two successive energy supplies to (1) first disintegrate the bound pair of vaculeon charges +e, -e composing a vacuuon of the vacuum and (2) impart masses to the disintegrated charges.

Deionization and desalination using electrostatic ion pumping

DOEpatents

Bourcier, William L.; Aines, Roger D.; Haslam, Jeffery J.; Schaldach, Charlene M.; O& #x27; Brien, Kevin C.; Cussler, Edward

2013-06-11

The present invention provides a new method and apparatus/system for purifying ionic solutions, such as, for example, desalinating water, using engineered charged surfaces to sorb ions from such solutions. Surface charge is applied externally, and is synchronized with oscillatory fluid movements between substantially parallel charged plates. Ions are held in place during fluid movement in one direction (because they are held in the electrical double layer), and released for transport during fluid movement in the opposite direction by removing the applied electric field. In this way the ions, such as salt, are "ratcheted" across the charged surface from the feed side to the concentrate side. The process itself is very simple and involves only pumps, charged surfaces, and manifolds for fluid collection.

Deionization and desalination using electrostatic ion pumping

DOEpatents

Bourcier, William L [Livermore, CA; Aines, Roger D [Livermore, CA; Haslam, Jeffery J [Livermore, CA; Schaldach, Charlene M [Pleasanton, CA; O'Brien, Kevin C [San Ramon, CA; Cussler, Edward [Edina, MN

2011-07-19

The present invention provides a new method and apparatus/system for purifying ionic solutions, such as, for example, desalinating water, using engineered charged surfaces to sorb ions from such solutions. Surface charge is applied externally, and is synchronized with oscillatory fluid movements between substantially parallel charged plates. Ions are held in place during fluid movement in one direction (because they are held in the electrical double layer), and released for transport during fluid movement in the opposite direction by removing the applied electric field. In this way the ions, such as salt, are "ratcheted" across the charged surface from the feed side to the concentrate side. The process itself is very simple and involves only pumps, charged surfaces, and manifolds for fluid collection.

A switchable polymer layer: Chain folding in end-charged polymer brushes

NASA Astrophysics Data System (ADS)

Heine, David; Wu, David T.

2001-03-01

We use a self-consistent field approximation to model the configurations of end-charged homopolymer and block copolymer brushes in response to an external electric field due to charges on the grafting surface. By varying the charge density on the grafting surface, we can cause the chains either to extend outward, greatly increasing the brush height, or to loop back to the grafting surface. We show that such a copolymer brush can present one block at the exposed surface in the extended state and present the other block in the retracted state. This occurs for both a solvated brush and a dry brush. We also compare these results to those of a modified Alexander-de Gennes model for the end-charged homopolymer brush.

Complexation of ferric oxide particles with pectins of different charge density.

PubMed

Milkova, Viktoria; Kamburova, Kamelia; Petkanchin, Ivana; Radeva, Tsetska

2008-09-02

The effect of polyelectrolyte charge density on the electrical properties and stability of suspensions of oppositely charged oxide particles is followed by means of electro-optics and electrophoresis. Variations in the electro-optical effect and the electrophoretic mobility are examined at conditions where fully ionized pectins of different charge density adsorb onto particles with ionizable surfaces. The charge neutralization point coincides with the maximum of particle aggregation in all suspensions. We find that the concentration of polyelectrolyte, needed to neutralize the particle charge, decreases with increasing charge density of the pectin. The most highly charged pectin presents an exception to this order, which is explained with a reduction of the effective charge density of this pectin due to condensation of counterions. The presence of condensed counterions, remaining bound to the pectin during its adsorption on the particle surface, is proved by investigation of the frequency behavior of the electro-optical effect at charge reversal of the particle surface.

Kinetics of optically excited charge carriers at the GaN surface: Influence of catalytic Pt nanostructures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Winnerl, Andrea, E-mail: andrea.winnerl@wsi.tum.de; Pereira, Rui N.; Stutzmann, Martin

2015-10-21

In this work, we use GaN with different deposited Pt nanostructures as a controllable model system to investigate the kinetics of photo-generated charge carriers in hybrid photocatalysts. We combine conductance and contact potential difference measurements to investigate the influence of Pt on the processes involved in the capture and decay of photo-generated charge carriers at and close to the GaN surface. We found that in the presence of Pt nanostructures the photo-excitation processes are similar to those found in Pt free GaN. However, in GaN with Pt nanostructures, photo-generated holes are preferentially trapped in surface states of the GaN coveredmore » with Pt and/or in electronic states of the Pt and lead to an accumulation of positive charge there, whereas negative charge is accumulated in localized states in a shallow defect band of the GaN covered with Pt. This preferential accumulation of photo-generated electrons close to the surface is responsible for a dramatic acceleration of the turn-off charge transfer kinetics and a stronger dependence of the surface photovoltage on light intensity when compared to a Pt free GaN surface. Our study shows that in hybrid photocatalysts, the metal nanostructures induce a spatially inhomogeneous surface band bending of the semiconductor that promotes a lateral drift of photogenerated charges towards the catalytic nanostructures.« less

Mediating electrostatic binding of 1-butyl-3-methylimidazolium chloride to enzyme surfaces improves conformational stability.

PubMed

Nordwald, Erik M; Kaar, Joel L

2013-08-01

We have recently developed a general approach to improve the utility of enzymes in ionic liquids (ILs) via tuning of the ratio of enzyme-containing positive to negative surface charges. In this work, the impact of enzyme surface charge ratio on the biophysical interaction of 1-butyl-3-methylimidazolium chloride ([BMIM][Cl]) with chymotrypsin and lipase was investigated to understand this approach at the molecular level. Results of fluorescence quenching assays indicated that the extent of binding of the [BMIM] cation decreased (7- and 3.5-fold for chymotrypsin and lipase, respectively) as a function of increasing ratio of positive to negative surface charges. Conformational stability assays further showed a close correlation between thermodynamic stabilization and enzyme surface charge ratio as well as [BMIM] binding. As evidence of this correlation, succinylation and acetylation resulted in the stabilization of chymotrypsin in 10% (v/v) [BMIM][Cl] by 17.0 and 6.6 kJ/mol, respectively, while cationization destabilized chymotrypsin by 3.6 kJ/mol. Combined, these results indicate that altering the surface charge ratio mediates the organization of IL molecules, namely, [BMIM] and [Cl], around the enzymes. Preferential exclusion of [Cl], in particular, via lowering of the ratio of positive to negative surface charges, correlated with increased enzyme stability. Accordingly, these results more broadly provide insight into the mechanism of stabilization in ILs via charge modification.

Effect of Atomic Oxygen Exposure on Surface Resistivity Change of Spacecraft Insulator Material

NASA Astrophysics Data System (ADS)

Mundari, Noor Danish Ahrar; Khan, Arifur Rahman; Chiga, Masaru; Okumura, Teppei; Masui, Hirokazu; Iwata, Minoru; Toyoda, Kazuhiro; Cho, Mengu

Spacecraft surface charging can lead to arcing and a loss of electricity generation capability in solar panels or even loss of a satellite. The charging problem may be further aggravated by atomic oxygen (AO) exposure in Low Earth orbits, which modifies the surface of materials like polyimide, Teflon, anti-reflective coatings, cover glass etc, used on satellite surfaces, affecting materials properties, such as resistivity, secondary electron emissivity and photo emission, which govern the charging behavior. These properties are crucial input parameters for spacecraft charging analysis. To study the AO exposure effect on charging governing properties, an atomic oxygen exposure facility based on laser detonation of oxygen was built. The facility produces AO with a peak velocity value around 10-12km/s and a higher flux than that existing in orbit. After exposing the polyimide test material to the equivalent of 10 years of AO fluence at an altitude of 700-800 km, surface charging properties like surface resistivity and volume resistivity were measured. The measurement was performed in a vacuum using the charge storage decay method at room temperature, which is considered the most appropriate for measuring resistivity for space applications. The results show that the surface resistivity increases and the volume resistivity remains almost the same for the AO exposure fluence of 5.4×1018 atoms cm-2.

Surface charge sensing by altering the phase transition in VO2

NASA Astrophysics Data System (ADS)

Kumar, S.; Esfandyarpour, R.; Davis, R.; Nishi, Y.

2014-08-01

Detection of surface charges has various applications in medicine, electronics, biotechnology, etc. The source of surface charge induction may range from simple charge-polarized molecules like water to complicated proteins. It was recently discovered that surface charge accumulation can alter the temperature at which VO2 undergoes a Mott transition. Here, we deposited polar molecules onto the surface of two-terminal thin-film VO2 lateral devices and monitored the joule-heating-driven Mott transition, or conductance switching. We observed that the power required to induce the conductance switching reduced upon treatment with polar molecules and, using in-situ blackbody-emission direct measurement of local temperature, we show that this reduction in power was accompanied by reduction in the Mott transition temperature. Further evidence suggested that this effect has specificity to the nature of the species used to induce surface charges. Using x-ray absorption spectroscopy, we also show that there is no detectable change in oxidation state of vanadium or structural phase in the bulk of the 40 nm VO2 thin-film even as the phase transition temperature is reduced by up to 20 K by the polar molecules. The ability to alter the phase transition parameters by depositing polar molecules suggests a potential application in sensing surface charges of different origins and this set of results also highlights interesting aspects of the phase transition in VO2.

Through thick and thin: tuning the threshold voltage in organic field-effect transistors.

PubMed

Martínez Hardigree, Josué F; Katz, Howard E

2014-04-15

Organic semiconductors (OSCs) constitute a class of organic materials containing densely packed, overlapping conjugated molecular moieties that enable charge carrier transport. Their unique optical, electrical, and magnetic properties have been investigated for use in next-generation electronic devices, from roll-up displays and radiofrequency identification (RFID) to biological sensors. The organic field-effect transistor (OFET) is the key active element for many of these applications, but the high values, poor definition, and long-term instability of the threshold voltage (V(T)) in OFETs remain barriers to realization of their full potential because the power and control circuitry necessary to compensate for overvoltages and drifting set points decrease OFET practicality. The drifting phenomenon has been widely observed and generally termed "bias stress." Research on the mechanisms responsible for this poor V(T) control has revealed a strong dependence on the physical order and chemical makeup of the interfaces between OSCs and adjacent materials in the OFET architecture. In this Account, we review the state of the art for tuning OFET performance via chemical designs and physical processes that manipulate V(T). This parameter gets to the heart of OFET operation, as it determines the voltage regimes where OFETs are either ON or OFF, the basis for the logical function of the devices. One obvious way to decrease the magnitude and variability of V(T) is to work with thinner and higher permittivity gate dielectrics. From the perspective of interfacial engineering, we evaluate various methods that we and others have developed, from electrostatic poling of gate dielectrics to molecular design of substituted alkyl chains. Corona charging of dielectric surfaces, a method for charging the surface of an insulating material using a constant high-voltage field, is a brute force means of shifting the effective gate voltage applied to a gate dielectric. A gentler and more direct method is to apply surface voltage to dielectric interfaces by direct contact or postprocess biasing; these methods could also be adapted for high throughput printing sequences. Dielectric hydrophobicity is an important chemical property determining the stability of the surface charges. Functional organic monolayers applied to dielectrics, using the surface attachment chemistry made available from "self-assembled" monolayer chemistry, provide local electric fields without any biasing process at all. To the extent that the monolayer molecules can be printed, these are also suitable for high throughput processes. Finally, we briefly consider V(T) control in the context of device integration and reliability, such as the role of contact resistance in affecting this parameter.

Atomistic Molecular Dynamics Simulations of Charged Latex Particle Surfaces in Aqueous Solution.

PubMed

Li, Zifeng; Van Dyk, Antony K; Fitzwater, Susan J; Fichthorn, Kristen A; Milner, Scott T

2016-01-19

Charged particles in aqueous suspension form an electrical double layer at their surfaces, which plays a key role in suspension properties. For example, binder particles in latex paint remain suspended in the can because of repulsive forces between overlapping double layers. Existing models of the double layer assume sharp interfaces bearing fixed uniform charge, and so cannot describe aqueous binder particle surfaces, which are soft and diffuse, and bear mobile charge from ionic surfactants as well as grafted multivalent oligomers. To treat this industrially important system, we use atomistic molecular dynamics simulations to investigate a structurally realistic model of commercial binder particle surfaces, informed by extensive characterization of particle synthesis and surface properties. We determine the interfacial profiles of polymer, water, bound and free ions, from which the charge density and electrostatic potential can be calculated. We extend the traditional definitions of the inner and outer Helmholtz planes to our diffuse interfaces. Beyond the Stern layer, the simulated electrostatic potential is well described by the Poisson-Boltzmann equation. The potential at the outer Helmholtz plane compares well to the experimental zeta potential. We compare particle surfaces bearing two types of charge groups, ionic surfactant and multivalent oligomers, with and without added salt. Although the bare charge density of a surface bearing multivalent oligomers is much higher than that of a surfactant-bearing surface at realistic coverage, greater counterion condensation leads to similar zeta potentials for the two systems.

Host-guest chemistry of dendrimer-drug complexes. 2. Effects of molecular properties of guests and surface functionalities of dendrimers.

PubMed

Hu, Jingjing; Cheng, Yiyun; Wu, Qinglin; Zhao, Libo; Xu, Tongwen

2009-08-06

The host-guest chemistry of dendrimer-drug complexes is investigated by NMR techniques, including (1)H NMR and 2D-NOESY studies. The effects of molecular properties of drug molecules (protonation ability and spatial steric hindrance of charged groups) and surface functionalities of dendrimers (positively charged amine groups and negatively charged carboxylate groups) on the host-guest interactions are discussed. Different interaction mechanisms between dendrimers and drug molecules are proposed on the basis of NMR results. Primary amine- and secondary amine-containing drugs preferentially bind to negatively charged dendrimers by strong electrostatic interactions, whereas tertiary amine and quaternary ammonium-containing drugs have weak binding ability with dendrimers due to relatively low protonation ability of the tertiary amine group and serious steric hindrance of the quaternary ammonium group. Positively charged drugs locate only on the surface of negatively charged dendrimers, whereas negatively charged drugs locate both on the surface and in the interior cavities of positively charged dendrimers. The host-guest chemistry of dendrimer-drug complexes is promising for the development of new drug delivery systems.

Effect of surface charge alteration on stability of L-asparaginase II from Escherichia sp.

PubMed

Vidya, Jalaja; Ushasree, Mrudula Vasudevan; Pandey, Ashok

2014-03-05

Escherichia coli L-asparaginases have great significance in the treatment of leukemia. Consequently, there is considerable interest in engineering this enzyme for improving its stability. In this work, the effect of surface charge on the stability of the enzyme l-asparaginase II was studied by site-directed mutagenesis of the cloned ansB gene from Escherichia sp. Replacement of two positively charged residues (K139 and K207) on the surface loops with neutral and reverse charges resulted in altered thermo stability in designed variants. Neutral charge substitutions (K139A and K207A) retained greater tolerance and stability followed by negative charge substitutions (K139D and K207D) compared to control mutant K139R and wild enzyme. From the results, it was concluded that the optimization of surface charge contributed much to the thermal properties of proteins without affecting the structure. Copyright © 2013 Elsevier Inc. All rights reserved.

Analysis of microscopic parameters of surface charging in polymer caused by defocused electron beam irradiation.

PubMed

Liu, Jing; Zhang, Hai-Bo

2014-12-01

The relationship between microscopic parameters and polymer charging caused by defocused electron beam irradiation is investigated using a dynamic scattering-transport model. The dynamic charging process of an irradiated polymer using a defocused 30 keV electron beam is conducted. In this study, the space charge distribution with a 30 keV non-penetrating e-beam is negative and supported by some existing experimental data. The internal potential is negative, but relatively high near the surface, and it decreases to a maximum negative value at z=6 μm and finally tend to 0 at the bottom of film. The leakage current and the surface potential behave similarly, and the secondary electron and leakage currents follow the charging equilibrium condition. The surface potential decreases with increasing beam current density, trap concentration, capture cross section, film thickness and electron-hole recombination rate, but with decreasing electron mobility and electron energy. The total charge density increases with increasing beam current density, trap concentration, capture cross section, film thickness and electron-hole recombination rate, but with decreasing electron mobility and electron energy. This study shows a comprehensive analysis of microscopic factors of surface charging characteristics in an electron-based surface microscopy and analysis. Copyright © 2014 Elsevier Ltd. All rights reserved.

The role of surface charge density in cationic liposome-promoted dendritic cell maturation and vaccine-induced immune responses

NASA Astrophysics Data System (ADS)

Ma, Yifan; Zhuang, Yan; Xie, Xiaofang; Wang, Ce; Wang, Fei; Zhou, Dongmei; Zeng, Jianqiang; Cai, Lintao

2011-05-01

Cationic liposomes have emerged as a novel adjuvant and antigen delivery system to enhance vaccine efficacy. However, the role of surface charge density in cationic liposome-regulated immune responses has not yet been elucidated. In the present study, we prepared a series of DOTAP/DOPC cationic liposomes with different surface densities by incorporating varying amounts of DOPC (a neutral lipid) into DOTAP (a cationic lipid). The results showed that DOTAP/DOPC cationic liposome-regulated immune responses relied on the surface charge density, and might occur through ROS signaling. The liposomes with a relatively high charge density, such as DOTAP/DOPC 5 : 0 and 4 : 1 liposomes, potently enhanced dendritic cell maturation, ROS generaion, antigen uptake, as well as the production of OVA-specific IgG2a and IFN-γ. In contrast, low-charge liposomes, such as DOTAP/DOPC 1 : 4 liposome, failed to promote immune responses even at high concentrations, confirming that the immunoregulatory effect of cationic liposomes is mostly attributable to their surface charge density. Moreover, the DOTAP/DOPC 1 : 4 liposome suppressed anti-OVA antibody responses in vivo. Overall, maintaining an appropriate surface charge is crucial for optimizing the adjuvant effect of cationic liposomes and enhancing the efficacy of liposome-based vaccines.

Charge reversal at a planar boundary between two dielectrics.

PubMed

Wang, Zhi-Yong

2016-01-01

Despite the ubiquitous character and relevance of the electric double layer in the entire realm of interface and colloid science, very little is known of the effect that surface heterogeneity exerts on the underlying mechanisms of ion adsorption. Herein, computer simulations offer a perspective that, in sharp contrast to the homogeneously charged surface, discrete groups promote multivalent counterion binding, leading to charge reversal but possibly having not a sign change of the electrophoretic mobility. Counterintuitively, the introduction of dielectric images yields a significantly greater accumulation of counterions, which further facilitates the magnitude of charge reversal. The reported results are very sensitive to both the degree of ion hydration and the representation of surface charges. Our findings shed light on the mechanism for charge reversal over a broad range of coupling regimes operating the adsorption of counterions through surface group bridging attraction with their own images and provide opportunities for experimental studies and theoretical development.

Charge reversal at a planar boundary between two dielectrics

NASA Astrophysics Data System (ADS)

Wang, Zhi-Yong

2016-01-01

Despite the ubiquitous character and relevance of the electric double layer in the entire realm of interface and colloid science, very little is known of the effect that surface heterogeneity exerts on the underlying mechanisms of ion adsorption. Herein, computer simulations offer a perspective that, in sharp contrast to the homogeneously charged surface, discrete groups promote multivalent counterion binding, leading to charge reversal but possibly having not a sign change of the electrophoretic mobility. Counterintuitively, the introduction of dielectric images yields a significantly greater accumulation of counterions, which further facilitates the magnitude of charge reversal. The reported results are very sensitive to both the degree of ion hydration and the representation of surface charges. Our findings shed light on the mechanism for charge reversal over a broad range of coupling regimes operating the adsorption of counterions through surface group bridging attraction with their own images and provide opportunities for experimental studies and theoretical development.

Electrostatic thin film chemical and biological sensor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Prelas, Mark A.; Ghosh, Tushar K.; Tompson, Jr., Robert V.

A chemical and biological agent sensor includes an electrostatic thin film supported by a substrate. The film includes an electrostatic charged surface to attract predetermined biological and chemical agents of interest. A charge collector associated with said electrostatic thin film collects charge associated with surface defects in the electrostatic film induced by the predetermined biological and chemical agents of interest. A preferred sensing system includes a charge based deep level transient spectroscopy system to read out charges from the film and match responses to data sets regarding the agents of interest. A method for sensing biological and chemical agents includesmore » providing a thin sensing film having a predetermined electrostatic charge. The film is exposed to an environment suspected of containing the biological and chemical agents. Quantum surface effects on the film are measured. Biological and/or chemical agents can be detected, identified and quantified based on the measured quantum surface effects.« less

Biochemical Study of Anti-Inflammatory Proteins vCCI and vMIP-II

DTIC Science & Technology

2014-07-17

protein ), where we showed that vCCI is able to bind so many different chemokines due to its general negatively charged surface , allowing it to bind...sample of these competition curves. Our conclusion from the data in Table 1 and Figure 1 is that the negatively charged surface of vCCI allows it to...Similar to our mutagenesis results, the overall data indicate that vCCI uses a negatively charged surface to bind positive charges on the chemokine

SPM observation of nano-dots induced by slow highly charged ions

NASA Astrophysics Data System (ADS)

Nakamura, Nobuyuki; Terada, Masashi; Nakai, Yoichi; Kanai, Yasuyuki; Ohtani, Shunsuke; Komaki, Ken-ichiro; Yamazaki, Yasunori

2005-05-01

We have observed nano-dots on a highly oriented pyrolytic graphite (HOPG) surface produced by highly charged ion impacts with a scanning probe microscope. In order to clarify the role of potential and kinetic energies in surface modification, we have measured the kinetic energy and incident ion charge dependences of the dot size. The results showed that the potential energy or the incident ion charge has strong influence on the surface modification rather than the kinetic energy.

Direct evidence and enhancement of surface plasmon resonance effect on Ag-loaded TiO2 nanotube arrays for photocatalytic CO2 reduction

NASA Astrophysics Data System (ADS)

Low, Jingxiang; Qiu, Shuoqi; Xu, Difa; Jiang, Chuanjia; Cheng, Bei

2018-03-01

Surface plasmon resonance (SPR) effect has been utilized in many solar conversion applications because of its ability to convert visible photons into "hot electron" energy. However, the direct evidence and enhancement of this unique effect are still great challenges, limiting its practical applications. Here we present the direct evidence and enhancement of SPR effect using TiO2 nanotube arrays (TNTAs) loaded with Ag nanoparticles (NPs) as a proof-of-concept example. Particularly, electrochemical deposition method is applied to deposit Ag NPs into the inner space of TNTAs for enhancing SPR effect of Ag NPs, as demonstrated by Raman and light absorption spectroscopies. This enhanced SPR effect is because multi-scattered light within TNTAs can be effectively utilized by Ag NPs in the inner space of TNTAs. Moreover, combining synchronous-illumination X-ray photoelectron and electrochemical impedance spectroscopy characterization, we confirm that the SPR effect of Ag NPs can enhance photocatalytic performance of TNTAs mainly from two aspects: (i) injection of "hot electrons" from Ag NPs to TNTAs and (ii) acceleration of charge carrier migration on the TNTAs through a unique near field effect. The direct evidence and enhancement of SPR effect open new perspectives in design of functional plasmonic nanomaterials with high solar conversion efficiency.

Two-Dimensional Nanomaterials for Biomedical Applications: Emerging Trends and Future Prospects.

PubMed

Chimene, David; Alge, Daniel L; Gaharwar, Akhilesh K

2015-12-02

Two-dimensional (2D) nanomaterials are ultrathin nanomaterials with a high degree of anisotropy and chemical functionality. Research on 2D nanomaterials is still in its infancy, with the majority of research focusing on elucidating unique material characteristics and few reports focusing on biomedical applications of 2D nanomaterials. Nevertheless, recent rapid advances in 2D nanomaterials have raised important and exciting questions about their interactions with biological moieties. 2D nanoparticles such as carbon-based 2D materials, silicate clays, transition metal dichalcogenides (TMDs), and transition metal oxides (TMOs) provide enhanced physical, chemical, and biological functionality owing to their uniform shapes, high surface-to-volume ratios, and surface charge. Here, we focus on state-of-the-art biomedical applications of 2D nanomaterials as well as recent developments that are shaping this emerging field. Specifically, we describe the unique characteristics that make 2D nanoparticles so valuable, as well as the biocompatibility framework that has been investigated so far. Finally, to both capture the growing trend of 2D nanomaterials for biomedical applications and to identify promising new research directions, we provide a critical evaluation of potential applications of recently developed 2D nanomaterials. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Charge-coupled device image sensor study

NASA Technical Reports Server (NTRS)

1973-01-01

The design specifications and predicted performance characteristics of a Charge-Coupled Device Area Imager and a Charge-Coupled Device Linear Imager are presented. The Imagers recommended are intended for use in space-borne imaging systems and therefore would meet the requirements for the intended application. A unique overlapping metal electrode structure and a buried channel structure are described. Reasons for the particular imager designs are discussed.

Electrostatic dust transport on the surfaces of airless bodies

NASA Astrophysics Data System (ADS)

Wang, X.; Schwan, J.; Hsu, H. W.; Horanyi, M.

2015-12-01

The surfaces of airless bodies are charged due to the exposure to solar wind plasma and UV radiation. Dust particles on the regolith of these surfaces can become charged, and may move and even get lofted due to electrostatic force. Electrostatic dust transport has been a long-standing problem that may be related to many observed phenomena on the surfaces of airless planetary bodies, including the lunar horizon glow, the dust ponds on asteroid Eros, the spokes in Saturn's rings, and more recently, the collection of dust particles ejected off Comet 67P, observed by Rosetta. In order to resolve these puzzles, a handful of laboratory experiments have been performed in the past and demonstrated that dust indeed moves and lifts from surfaces exposed to plasma. However, the exact mechanisms for the mobilization of dust particles still remain a mystery. Current charging models, including the so-called "shared charge model" and the charge fluctuation theory, will be discussed. It is found that neither of these models can explain the results from either laboratory experiments or in-situ observations. Recently, single dust trajectories were captured with our new dust experiments, enabling novel micro-scale investigations. The particles' initial launch speeds and size distributions are analyzed, and a new so-called "patched charge model" is proposed to explain our findings. We identify the role of plasma micro-cavities that are formed in-between neighboring dust particles. The emitted secondary or photo- electrons are proposed to be absorbed inside the micro-cavities, resulting in significant charge accumulation on the exposed patches of the surfaces of neighboring particles. The resulting enhanced Coulomb force (repulsion) between particles is likely the dominant force to mobilize and lift them off the surface. The role of other properties, including surface morphology, cohesion and photoelectron charging, will also be discussed.

A review on preparation of silver nano-particles

NASA Astrophysics Data System (ADS)

Haider, Adawiya J.; Haider, Mohammad J.; Mehde, Mohammad S.

2018-05-01

The term "nano particle" (NP) refers to particle diameter in nanometers in size. Nanoparticles contain a small number of constituent atoms or molecules that differ from the properties inherent in their bulk counterparts, found in various forms such as spherical, triangular, cubic, pentagonal, rod-shaped, shells, elliptical and so on. In this chapter, it has been presented the theoretical concepts of the preparation of AgNPS as powders and collide nanoparticles, techniques of preparation with their characterization (morphology, sign charge and potential value, particle distribution ….etc.). Also, included unique properties of AgNPS that are different from those of their bulk materials like: High surface area to volume ratio effects Quantization of electronic and vibration properties.

Lunar Radio Telescopes: A Staged Approach for Lunar Science, Heliophysics, Astrobiology, Cosmology, and Exploration

NASA Technical Reports Server (NTRS)

Lazio, Joseph; Bowman, Judd D.; Burns, Jack O.; Farrell, W. M.; Jones, D. L.; Kasper, J. C.; MacDowall, R. J.; Stewart, K. P.; Weiler, K.

2012-01-01

Observations with radio telescopes address key problems in cosmology, astrobiology, heliophysics, and planetary science including the first light in the Universe (Cosmic Dawn), magnetic fields of extrasolar planets, particle acceleration mechanisms, and the lunar ionosphere. The Moon is a unique science platform because it allows access to radio frequencies that do not penetrate the Earth's ionosphere and because its far side is shielded from intense terrestrial emissions. The instrument packages and infrastructure needed for radio telescopes can be transported and deployed as part of Exploration activities, and the resulting science measurements may inform Exploration (e.g., measurements of lunar surface charging). An illustrative roadmap for the staged deployment of lunar radio telescopes

Scalable synthesis and energy applications of defect engineeered nano materials

NASA Astrophysics Data System (ADS)

Karakaya, Mehmet

Nanomaterials and nanotechnologies have attracted a great deal of attention in a few decades due to their novel physical properties such as, high aspect ratio, surface morphology, impurities, etc. which lead to unique chemical, optical and electronic properties. The awareness of importance of nanomaterials has motivated researchers to develop nanomaterial growth techniques to further control nanostructures properties such as, size, surface morphology, etc. that may alter their fundamental behavior. Carbon nanotubes (CNTs) are one of the most promising materials with their rigidity, strength, elasticity and electric conductivity for future applications. Despite their excellent properties explored by the abundant research works, there is big challenge to introduce them into the macroscopic world for practical applications. This thesis first gives a brief overview of the CNTs, it will then go on mechanical and oil absorption properties of macro-scale CNT assemblies, then following CNT energy storage applications and finally fundamental studies of defect introduced graphene systems. Chapter Two focuses on helically coiled carbon nanotube (HCNT) foams in compression. Similarly to other foams, HCNT foams exhibit preconditioning effects in response to cyclic loading; however, their fundamental deformation mechanisms are unique. Bulk HCNT foams exhibit super-compressibility and recover more than 90% of large compressive strains (up to 80%). When subjected to striker impacts, HCNT foams mitigate impact stresses more effectively compared to other CNT foams comprised of non-helical CNTs (~50% improvement). The unique mechanical properties we revealed demonstrate that the HCNT foams are ideally suited for applications in packaging, impact protection, and vibration mitigation. The third chapter describes a simple method for the scalable synthesis of three-dimensional, elastic, and recyclable multi-walled carbon nanotube (MWCNT) based light weight bucky-aerogels (BAGs) that are capable of efficiently absorbing non-polar solvents and separating oil-in-water emulsions. Furthermore, BAGs exhibit resilience to impact by recovering more than 70% of the deformation. The energy dissipated by BAGs at 80% compressive strain is in the order of 500 kJm-3, which is nearly 50 times more than the energy dissipated by commercial foams with similar densities. In the forth chapter, we demonstrate the synthesis of high-surface area, polymer-modified carbon nanotube (or helically coiled carbon nanotube (HCNT)) "paper" electrodes for high-power, high-energy density supercapacitors using simple fabrication methods. The use of conductive, high surface area carbon nanomaterials allows for the utilization of low-cost, non-conductive polymers containing reversible redox groups with higher charge capacity, such as sulfonated lignin. Compared to electrodes containing only helically coiled carbon nanotubes (80 Fg-1), paper electrodes fabricated with redox polymers show an increase in electrode capacitance to over 600 Fg -1 along with an increase in charge capacity from 20 mA hrg -1 to 80 mA hrg-1. Chapter Five presents a scalable roll-to-roll (R2R) spray coating process for synthesizing randomly oriented multi-walled carbon nanotubes electrodes on Al foils. The coin and jellyroll type supercapacitors comprised such electrodes yield high power densities (~700 mW/cm3) and energy densities (1 mW h/cm3) on par with Li-ion thin film batteries. These devices exhibit excellent cycle stability with no loss in performance over more than a thousand cycles. In the sixth chapter, we have indicated a methodology for both increasing and decreasing the electrochemical capacitance of Few Layer Graphene based nano-graphites through a combination of argon and hydrogen-based plasma processing. In addition to the utility for charge storage, our work contributes to understanding and controlling the charge storage characteristics. In the final chapter, we have investigated a nitrogen-doped graphene. We demonstrate through Raman spectroscopy, nonlinear optical and ultrafast spectroscopy, and density functional theory that the graphitic dopant configuration is stable in graphene and does not significantly alter electron--electron or electron--phonon scattering, that is otherwise present in doped graphene, by preserving the crystal coherence length (La)..

Influence of charge and flexibility on smectic phase formation in filamentous virus suspensions

NASA Astrophysics Data System (ADS)

Purdy, Kirstin R.; Fraden, Seth

2007-07-01

We present experimental measurements of the cholesteric-smectic phase transition of suspensions of charged semiflexible rods as a function of rod flexibility and surface charge. The rod particles consist of the bacteriophage M13 and closely related mutants, which are structurally identical to M13, but vary either in contour length and therefore ratio of persistence length to contour length, or surface charge. Surface charge is altered in two ways; by changing solution pH and by comparing M13 with fd virus, a virus which differs from M13 only by the substitution of a single charged amino acid for a neutral one per viral coat protein. Phase diagrams are measured as a function of particle length, particle charge, and ionic strength. The experimental results are compared with existing theoretical predictions for the phase behavior of flexible rods and charged rods.

Influence of radioactivity on surface charging and aggregation kinetics of particles in the atmosphere.

PubMed

Kim, Yong-Ha; Yiacoumi, Sotira; Lee, Ida; McFarlane, Joanna; Tsouris, Costas

2014-01-01

Radioactivity can influence surface interactions, but its effects on particle aggregation kinetics have not been included in transport modeling of radioactive particles. In this research, experimental and theoretical studies have been performed to investigate the influence of radioactivity on surface charging and aggregation kinetics of radioactive particles in the atmosphere. Radioactivity-induced charging mechanisms have been investigated at the microscopic level, and heterogeneous surface potential caused by radioactivity is reported. The radioactivity-induced surface charging is highly influenced by several parameters, such as rate and type of radioactive decay. A population balance model, including interparticle forces, has been employed to study the effects of radioactivity on particle aggregation kinetics in air. It has been found that radioactivity can hinder aggregation of particles because of similar surface charging caused by the decay process. Experimental and theoretical studies provide useful insights into the understanding of transport characteristics of radioactive particles emitted from severe nuclear events, such as the recent accident of Fukushima or deliberate explosions of radiological devices.

The role of charged surface residues in the binding ability of small hubs in protein-protein interaction networks

PubMed Central

Patil, Ashwini; Nakamura, Haruki

2007-01-01

Hubs are highly connected proteins in a protein-protein interaction network. Previous work has implicated disordered domains and high surface charge as the properties significant in the ability of hubs to bind multiple proteins. While conformational flexibility of disordered domains plays an important role in the binding ability of large hubs, high surface charge is the dominant property in small hubs. In this study, we further investigate the role of the high surface charge in the binding ability of small hubs in the absence of disordered domains. Using multipole expansion, we find that the charges are highly distributed over the hub surfaces. Residue enrichment studies show that the charged residues in hubs are more prevalent on the exposed surface, with the exception of Arg, which is predominantly found at the interface, as compared to non-hubs. This suggests that the charged residues act primarily from the exposed surface rather than the interface to affect the binding ability of small hubs. They do this through (i) enhanced intra-molecular electrostatic interactions to lower the desolvation penalty, (ii) indirect long – range intermolecular interactions with charged residues on the partner proteins for better complementarity and electrostatic steering, and (iii) increased solubility for enhanced diffusion-controlled rate of binding. Along with Arg, we also find a high prevalence of polar residues Tyr, Gln and His and the hydrophobic residue Met at the interfaces of hubs, all of which have the ability to form multiple types of interactions, indicating that the interfaces of hubs are optimized to participate in multiple interactions. PMID:27857564

The role of charged surface residues in the binding ability of small hubs in protein-protein interaction networks.

PubMed

Patil, Ashwini; Nakamura, Haruki

2007-01-01

Hubs are highly connected proteins in a protein-protein interaction network. Previous work has implicated disordered domains and high surface charge as the properties significant in the ability of hubs to bind multiple proteins. While conformational flexibility of disordered domains plays an important role in the binding ability of large hubs, high surface charge is the dominant property in small hubs. In this study, we further investigate the role of the high surface charge in the binding ability of small hubs in the absence of disordered domains. Using multipole expansion, we find that the charges are highly distributed over the hub surfaces. Residue enrichment studies show that the charged residues in hubs are more prevalent on the exposed surface, with the exception of Arg, which is predominantly found at the interface, as compared to non-hubs. This suggests that the charged residues act primarily from the exposed surface rather than the interface to affect the binding ability of small hubs. They do this through (i) enhanced intra-molecular electrostatic interactions to lower the desolvation penalty, (ii) indirect long - range intermolecular interactions with charged residues on the partner proteins for better complementarity and electrostatic steering, and (iii) increased solubility for enhanced diffusion-controlled rate of binding. Along with Arg, we also find a high prevalence of polar residues Tyr, Gln and His and the hydrophobic residue Met at the interfaces of hubs, all of which have the ability to form multiple types of interactions, indicating that the interfaces of hubs are optimized to participate in multiple interactions.

The effect of charging rate on the graphite electrode of commercial lithium-ion cells: A post-mortem study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Somerville, L.; Bareno, J.; Trask, S.

Increased charging rates negatively affect the lifetime of lithium-ion cells by increasing cell resistance and reducing capacity. This work is a post-mortem study of 18650 cells subjected to charge rates of 0.7-, 2-, 4-, and 6-C. For cells charged at 0.7-C to 4-C, this performance degradation is primarily related to surface film thickness with no observable change in surface film chemical composition. However, at charge rates of 6-C, the chemical composition of the surface film changes significantly, suggesting that this change is the reason for the sharper increase in cell resistance compared to the lower charge rates. In addition, wemore » found that surface film formation was not uniform across the electrode. Surface film was thicker and chemically different along the central band of the electrode “jelly roll”. This result is most likely attributable to an increase in temperature that results from non-uniform electrode wetting during manufacture. As a result, this non-uniform change further resulted in active material delamination from the current collector owing to chemical changes to the binder for the cell charged at 6-C.« less

The effect of charging rate on the graphite electrode of commercial lithium-ion cells: A post-mortem study

DOE PAGES

Somerville, L.; Bareno, J.; Trask, S.; ...

2016-10-22

Increased charging rates negatively affect the lifetime of lithium-ion cells by increasing cell resistance and reducing capacity. This work is a post-mortem study of 18650 cells subjected to charge rates of 0.7-, 2-, 4-, and 6-C. For cells charged at 0.7-C to 4-C, this performance degradation is primarily related to surface film thickness with no observable change in surface film chemical composition. However, at charge rates of 6-C, the chemical composition of the surface film changes significantly, suggesting that this change is the reason for the sharper increase in cell resistance compared to the lower charge rates. In addition, wemore » found that surface film formation was not uniform across the electrode. Surface film was thicker and chemically different along the central band of the electrode “jelly roll”. This result is most likely attributable to an increase in temperature that results from non-uniform electrode wetting during manufacture. As a result, this non-uniform change further resulted in active material delamination from the current collector owing to chemical changes to the binder for the cell charged at 6-C.« less

Geoelectrical Monitoring of Ammonium Sorption Processes in a Biochar Filtration System

NASA Astrophysics Data System (ADS)

Wang, S. L.; Osei, C.; Rabinovich, A.; Ntarlagiannis, D.; Rouff, A.

2017-12-01

With the rise of modern agriculture, nutrient pollution has become an increasingly important environmental concern. A common problem is excess nitrogen which agricultural livestock farms often generate in the form of ammonium (NH4+). This highly soluble ion is easily transported through runoff and leaching, leading to water supply contamination and soil fertility decline. Biochar is the carbon-rich product of thermal decomposition of biomass in an oxygen-free environment. It is primarily used as a soil enhancer with other applications currently under research. Biochar's unique characteristics such as high surface area, high sorption capacity and long term biological and chemical stability make it a prime candidate for environmental applications such as contaminant regulation and waste effluent treatment. The spectral induced polarization (SIP) method is an established geoelectrical method that has been increasingly used in environmental investigations. SIP is unique among geophysical methods because it is sensitive not only to the bulk properties of the medium under investigation but also to the interfacial properties (e.g., mineral-fluid). The unique properties that make biochar attractive for environmental use are associated with surface properties (e.g., surface area, surface charge, presence of functional groups) that are expected to have a profound effect on SIP signals. This study presents early results on the use of the SIP method to monitor ammonium recycling of swine wastewater in a biochar filtration system. SIP measurements were taken continuously as biochar-packed columns were first injected with an ammonium wastewater solution (sorption phase) and then an ammonium-free solution (desorption phase). Geochemical monitoring showed that outflow ammonium concentration decreased during the sorption phase and increased during the desorption phase. The collected SIP data appear to be in agreement with the geochemical monitoring, providing a temporally continuous record of changes on the waste fluid and biochar surface. The results suggest that biochar successfully sorbs and releases ammonium and that the SIP method is sensitive these sorption processes. Further research is required for the quantitative interpretation of the SIP signals, including the signal source mechanism.

[Sorption of microorganisms by fiber materials].

PubMed

Nikovskaia, G N; Gordienko, A S; Globa, L I

1986-01-01

Candida guilliermondii and Escherichia coli cells were adsorbed on glass and basalt fibres with a similar specific surface, but with a different charge. The quantity of adsorbed microorganisms did not depend on the type and charge of a fibre surface. However, cells were adsorbed faster and more firmly on positively charged and uncharged fibres than on negatively charged fibres.

A fluorescent imaging technique for quantifying spray deposits on plant leaves

USDA-ARS?s Scientific Manuscript database

Because of the unique characteristics of electrostatically-charged sprays, use of traditional methods to quantify deposition from these sprays has been challenging. A new fluorescent imaging technique was developed to quantify spray deposits from electrostatically-charged sprays on natural plant lea...

Metal Oxide Nanosensors Using Polymeric Membranes, Enzymes and Antibody Receptors as Ion and Molecular Recognition Elements

PubMed Central

Willander, Magnus; Khun, Kimleang; Ibupoto, Zafar Hussain

2014-01-01

The concept of recognition and biofunctionality has attracted increasing interest in the fields of chemistry and material sciences. Advances in the field of nanotechnology for the synthesis of desired metal oxide nanostructures have provided a solid platform for the integration of nanoelectronic devices. These nanoelectronics-based devices have the ability to recognize molecular species of living organisms, and they have created the possibility for advanced chemical sensing functionalities with low limits of detection in the nanomolar range. In this review, various metal oxides, such as ZnO-, CuO-, and NiO-based nanosensors, are described using different methods (receptors) of functionalization for molecular and ion recognition. These functionalized metal oxide surfaces with a specific receptor involve either a complex formation between the receptor and the analyte or an electrostatic interaction during the chemical sensing of analytes. Metal oxide nanostructures are considered revolutionary nanomaterials that have a specific surface for the immobilization of biomolecules with much needed orientation, good conformation and enhanced biological activity which further improve the sensing properties of nanosensors. Metal oxide nanostructures are associated with certain unique optical, electrical and molecular characteristics in addition to unique functionalities and surface charge features which shows attractive platforms for interfacing biorecognition elements with effective transducing properties for signal amplification. There is a great opportunity in the near future for metal oxide nanostructure-based miniaturization and the development of engineering sensor devices. PMID:24841244

Charge collection kinetics on ferroelectric polymer surface using charge gradient microscopy

DOE PAGES

Choi, Yoon-Young; Tong, Sheng; Ducharme, Stephen P.; ...

2016-05-03

Here, a charge gradient microscopy (CGM) probe was used to collect surface screening charges on poly(vinylidene fluoride-trifluoroethylene) [P(VDF-TrFE)] thin films. These charges are naturally formed on unscreened ferroelectric domains in ambient condition. The CGM data were used to map the local electric current originating from the collected surface charges on the poled ferroelectric domains in the P(VDF-TrFE) thin films. Both the direction and amount of the collected current were controlled by changing the polarity and area of the poled domains. The endurance of charge collection by rubbing the CGM tip on the polymer film was limited to 20 scan cycles,more » after which the current reduced to almost zero. This degradation was attributed to the increase of the chemical bonding strength between the external screening charges and the polarization charges. Once this degradation mechanism is mitigated, the CGM technique can be applied to efficient energy harvesting devices using polymer ferroelectrics.« less

Surface Assisted Transient Displacement Charge Technique. II. Effect of Gases on Photoinduced Charge Transfer in Self-Assembled Monolayers

PubMed Central

Krasnoslobodtsev, Alexey V.; Smirnov, Sergei N.

2008-01-01

Surface assisted photoinduced transient displacement charge (SPTDC) technique was used to study charge transfer in self-assembled monolayers of 7-diethylaminocoumarin covalently linked to oxide surface in atmosphere of different gases. The dipole signal was found to be opposite to that in solution and dependent on the nature of gas and its pressure. The results were explained by collision-induced relaxation that impedes uninhibited tilting of molecules onto the surface. Collisions with paramagnetic oxygen induce intersystem crossing to long-lived triplet dipolar states of coumarin with the rate close to the half of that for the collision rate. PMID:16956285

Role of Surface Charge Density in Nanoparticle-templated Assembly of Bromovirus Protein Cages

PubMed Central

Daniel, Marie-Christine; Tsvetkova, Irina B.; Quinkert, Zachary T.; Murali, Ayaluru; De, Mrinmoy; Rotello, Vincent M.; Kao, C. Cheng; Dragnea, Bogdan

2010-01-01

Self-assembling icosahedral protein cages have potencially useful physical and chemical characteristics for a variety of nanotechnology applications, ranging from therapeutic or diagnostic vectors to building blocks for hierarchical materials. For application-specific functional control of protein cage assemblies, a deeper understanding of the interaction between the protein cage and its payload is necessary. Protein-cage encapsulated nanoparticles, with their well-defined surface chemistry, allow for systematic control over key parameters of encapsulation such as the surface charge, hydrophobicity, and size. Independent control over these variables allows experimental testing of different assembly mechanism models. Previous studies done with Brome mosaic virus capsids and negatively-charged gold nanoparticles indicated that the result of the self-assembly process depends on the diameter of the particle. However, in these experiments, the surface-ligand density was maintained at saturation levels, while the total charge and the radius of curvature remained coupled variables, making the interpretation of the observed dependence on the core size difficult. The current work furnishes evidence of a critical surface charge density for assembly through an analysis aimed at decoupling the surface charge the core size. PMID:20575505

In Vitro Biocompatibility of Si Alloyed Multi-Principal Element Carbide Coatings

PubMed Central

Vladescu, Alina; Titorencu, Irina; Dekhtyar, Yuri; Jinga, Victor; Pruna, Vasile; Balaceanu, Mihai; Dinu, Mihaela; Pana, Iulian; Vendina, Viktorija

2016-01-01

In the current study, we have examined the possibility to improve the biocompatibility of the (TiZrNbTaHf)C through replacement of either Ti or Ta by Si. The coatings were deposited on Si and 316L stainless steel substrates by magnetron sputtering in an Ar+CH4 mixed atmosphere and were examined for elemental composition, chemical bonds, surface topography, surface electrical charge and biocompatible characteristics. The net surface charge was evaluated at nano and macroscopic scale by measuring the electrical potential and work function, respectively. The biocompatible tests comprised determination of cell viability and cell attachment to the coated surface. The deposited coatings had C/(metal+Si) ratios close to unity, while a mixture of metallic carbide, free-carbon and oxidized species formed on the film surface. The coatings’ surfaces were smooth and no influence of surface roughness on electrical charge or biocompatibility was found. The biocompatible characteristics correlated well with the electrical potential/work function, suggesting a significant role of surface charge in improving biocompatibility, particularly cell attachment to coating's surface. Replacement of either Ti or Ta by Si in the (TiZrNbTaHf)C coating led to an enhanced surface electrical charge, as well as to superior biocompatible properties, with best results for the (TiZrNbSiHf)C coating. PMID:27571361

Chemical Modification of Semiconductor Surfaces for Molecular Electronics.

PubMed

Vilan, Ayelet; Cahen, David

2017-03-08

Inserting molecular monolayers within metal/semiconductor interfaces provides one of the most powerful expressions of how minute chemical modifications can affect electronic devices. This topic also has direct importance for technology as it can help improve the efficiency of a variety of electronic devices such as solar cells, LEDs, sensors, and possible future bioelectronic ones. The review covers the main aspects of using chemistry to control the various aspects of interface electrostatics, such as passivation of interface states and alignment of energy levels by intrinsic molecular polarization, as well as charge rearrangement with the adjacent metal and semiconducting contacts. One of the greatest merits of molecular monolayers is their capability to form excellent thin dielectrics, yielding rich and unique current-voltage characteristics for transport across metal/molecular monolayer/semiconductor interfaces. We explain the interplay between the monolayer as tunneling barrier on the one hand, and the electrostatic barrier within the semiconductor, due to its space-charge region, on the other hand, as well as how different monolayer chemistries control each of these barriers. Practical tools to experimentally identify these two barriers and distinguish between them are given, followed by a short look to the future. This review is accompanied by another one, concerning the formation of large-area molecular junctions and charge transport that is dominated solely by molecules.

Enhanced flashover strength in polyethylene nanodielectrics by secondary electron emission modification

NASA Astrophysics Data System (ADS)

Wang, Weiwang; Li, Shengtao; Min, Daomin

2016-04-01

This work studies the correlation between secondary electron emission (SEE) characteristics and impulse surface flashover in polyethylene nanodielectrics both theoretically and experimentally, and illustrates the enhancement of flashover voltage in low-density polyethylene (LDPE) through incorporating Al2O3 nanoparticles. SEE characteristics play key roles in surface charging and gas desorption during surface flashover. This work demonstrates that the presence of Al2O3 nanoparticles decreases the SEE coefficient of LDPE and enhances the impact energy at the equilibrium state of surface charging. These changes can be explained by the increase of surface roughness and of surface ionization energy, and the strong interaction between nanoparticles and the polymer dielectric matrix. The surface charge and flashover voltage are calculated according to the secondary electron emission avalanche (SEEA) model, which reveals that the positive surface charges are reduced near the cathode triple point, while the presence of more nanoparticles in high loading samples enhances the gas desorption. Consequently, the surface flashover performance of LDPE/Al2O3 nanodielectrics is improved.

High-T C superconductivity in Cs3C60 compounds governed by local Cs-C60 Coulomb interactions

NASA Astrophysics Data System (ADS)

Harshman, Dale R.; Fiory, Anthony T.

2017-04-01

Unique among alkali-doped A 3C60 fullerene compounds, the A15 and fcc forms of Cs3C60 exhibit superconducting states varying under hydrostatic pressure with highest transition temperatures at T\\text{C}\\text{meas}   =  38.3 and 35.2 K, respectively. Herein it is argued that these two compounds under pressure represent the optimal materials of the A 3C60 family, and that the C60-associated superconductivity is mediated through Coulombic interactions with charges on the alkalis. A derivation of the interlayer Coulombic pairing model of high-T C superconductivity employing non-planar geometry is introduced, generalizing the picture of two interacting layers to an interaction between charge reservoirs located on the C60 and alkali ions. The optimal transition temperature follows the algebraic expression, T C0  =  (12.474 nm2 K)/ℓζ, where ℓ relates to the mean spacing between interacting surface charges on the C60 and ζ is the average radial distance between the C60 surface and the neighboring Cs ions. Values of T C0 for the measured cation stoichiometries of Cs3-x C60 with x  ≈  0 are found to be 38.19 and 36.88 K for the A15 and fcc forms, respectively, with the dichotomy in transition temperature reflecting the larger ζ and structural disorder in the fcc form. In the A15 form, modeled interacting charges and Coulomb potential e2/ζ are shown to agree quantitatively with findings from nuclear-spin relaxation and mid-infrared optical conductivity. In the fcc form, suppression of T\\text{C}\\text{meas} below T C0 is ascribed to native structural disorder. Phononic effects in conjunction with Coulombic pairing are discussed.

Coverage Dependent Charge Reduction of Cationic Gold Clusters on Surfaces Prepared Using Soft Landing of Mass-selected Ions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, Grant E.; Priest, Thomas A.; Laskin, Julia

2012-11-29

The ionic charge state of monodisperse cationic gold clusters on surfaces may be controlled by selecting the coverage of mass-selected ions soft landed onto a substrate. Polydisperse diphosphine-capped gold clusters were synthesized in solution by reduction of chloro(triphenylphosphine)gold(I) with borane tert-butylamine in the presence of 1,3-bis(diphenylphosphino)propane. The polydisperse gold clusters were introduced into the gas phase by electrospray ionization and mass selection was employed to select a multiply charged cationic cluster species (Au11L53+, m/z = 1409, L = 1,3-bis(diphenylphosphino)propane) which was delivered to the surfaces of four different self-assembled monolayers on gold (SAMs) at coverages of 1011 and 1012 clusters/mm2.more » Employing the spatial profiling capabilities of in-situ time-of-flight secondary ion mass spectrometry (TOF-SIMS) it is shown that, in addition to the chemical functionality of the monolayer (as demonstrated previously: ACS Nano, 2012, 6, 573) the coverage of cationic gold clusters on the surface may be used to control the distribution of ionic charge states of the soft-landed multiply charged clusters. In the case of a 1H,1H,2H,2H-perfluorodecanethiol SAM (FSAM) almost complete retention of charge by the deposited Au11L53+ clusters was observed at a lower coverage of 1011 clusters/mm2. In contrast, at a higher coverage of 1012 clusters/mm2, pronounced reduction of charge to Au11L52+ and Au11L5+ was observed on the FSAM. When soft landed onto 16- and 11-mercaptohexadecanoic acid surfaces on gold (16,11-COOH-SAMs), the mass-selected Au11L53+ clusters exhibited partial reduction of charge to Au11L52+ at lower coverage and additional reduction of charge to both Au11L52+ and Au11L5+ at higher coverage. The reduction of charge was found to be more pronounced on the surface of the shorter (thinner) C11 than the longer (thicker) C16-COOH-SAM. On the surface of the 1-dodecanethiol (HSAM) monolayer, the most abundant charge state was found to be Au11L52+ at lower coverage and Au11L5+ at higher coverage, respectively. A coverage-dependent electron tunneling mechanism is proposed to account for the observed reduction of charge of mass-selected multiply charged gold clusters soft landed on SAMs. The results demonstrate that one of the critical parameters that influence the chemical and physical properties of supported metal clusters, ionic charge state, may be controlled by selecting the coverage of charged species soft landed onto surfaces.« less

Effects of O 2 and N 2/H 2 plasma treatments on the neuronal cell growth on single-walled carbon nanotube paper scaffolds

NASA Astrophysics Data System (ADS)

Yoon, Ok Ja; Lee, Hyun Jung; Jang, Yeong Mi; Kim, Hyun Woo; Lee, Won Bok; Kim, Sung Su; Lee, Nae-Eung

2011-08-01

The O 2 and N 2/H 2 plasma treatments of single-walled carbon nanotube (SWCNT) papers as scaffolds for enhanced neuronal cell growth were conducted to functionalize their surfaces with different functional groups and to roughen their surfaces. To evaluate the effects of the surface roughness and functionalization modifications of the SWCNT papers, we investigated the neuronal morphology, mitochondrial membrane potential, and acetylcholine/acetylcholinesterase levels of human neuroblastoma during SH-SY5Y cell growth on the treated SWCNT papers. Our results demonstrated that the plasma-chemical functionalization caused changes in the surface charge states with functional groups with negative and positive charges and then the increased surface roughness enhanced neuronal cell adhesion, mitochondrial membrane potential, and the level of neurotransmitter in vitro. The cell adhesion and mitochondrial membrane potential on the negatively charged SWCNT papers were improved more than on the positively charged SWCNT papers. Also, measurements of the neurotransmitter level showed an enhanced acetylcholine level on the negatively charged SWCNT papers compared to the positively charged SWCNT papers.

Proton transfer to charged platinum electrodes. A molecular dynamics trajectory study.

PubMed

Wilhelm, Florian; Schmickler, Wolfgang; Spohr, Eckhard

2010-05-05

A recently developed empirical valence bond (EVB) model for proton transfer on Pt(111) electrodes (Wilhelm et al 2008 J. Phys. Chem. C 112 10814) has been applied in molecular dynamics (MD) simulations of a water film in contact with a charged Pt surface. A total of seven negative surface charge densities σ between -7.5 and -18.9 µC cm(-2) were investigated. For each value of σ, between 30 and 84 initial conditions of a solvated proton within a water slab were sampled, and the trajectories were integrated until discharge of a proton occurred on the charged surfaces. We have calculated the mean rates for discharge and for adsorption of solvated protons within the adsorbed water layer in contact with the metal electrode as a function of surface charge density. For the less negative values of σ we observe a Tafel-like exponential increase of discharge rate with decreasing σ. At the more negative values this exponential increase levels off and the discharge process is apparently transport limited. Mechanistically, the Tafel regime corresponds to a stepwise proton transfer: first, a proton is transferred from the bulk into the contact water layer, which is followed by transfer of a proton to the charged surface and concomitant discharge. At the more negative surface charge densities the proton transfer into the contact water layer and the transfer of another proton to the surface and its discharge occur almost simultaneously.

Effect of dipolar fields, surface termination, and surface orientation on photochemical reactions on transition metal oxides

NASA Astrophysics Data System (ADS)

Giocondi, Jennifer Lynn

Experiments have been conducted to determine the effects of dipolar fields, surface termination, and surface orientation on the photochemical reactivity of several transition metal oxides. These compounds include BaTiO3, SrTiO3, BaTi4O9, Sr2Nb2O 7, and Sr2Ta2O7 which were studied as polycrystalline ceramics, single crystals, micron-sized faceted particles, or some combination of these forms. The reduction of Ag+ from an aqueous AgNO3 solution (Ag0 product) and the oxidation of Pb2+ from an aqueous lead acetate solution (PbO 2 product) were selected as probe reactions because they leave insoluble products on the oxide surfaces. The reactivity of ferroelectric BaTiO3 was dominated by the effect of dipolar fields on the transport of photogenerated charge carriers. Silver was reduced on domains with a positive surface charge while lead was oxidized on domains with a negative surface charge. This reactivity implies that the dipolar field in individual domains drives photogenerated charge carriers to oppositely charged surfaces. This reaction mechanism results in a physical separation of the photogenerated charge carriers and the locations of the oxidation and reduction half reactions on the catalyst surface. Experiments performed on polycrystalline ceramics, single crystals, and micron-sized particles all showed this domain specific reactivity. SrTiO3 has the ideal cubic perovskite structure from which the tetragonally distorted ferroelectric BaTiO3 phase is derived. Polished and annealed surfaces of randomly oriented grain surfaces were bound by some combination of the following three planes: {110}, {111}, and a complex facet inclined approximately 24° from {100}. Surfaces with the complex {100} facet were found to be the most active for Ag reduction. Single crystal studies also showed that the nonpolar (100) surface is the most reactive and that the composition of the termination layer does not influence this reaction. However, the polar (111) and (110) surfaces had a non-uniform distribution of reaction products. For these orientations, the location of the reduction and oxidation reactions is determined by the chemical and charge terminations of the different terraces or facets. The reactivity for silver reduction on the faceted particles is ranked as (100) > (111) > (110) while the (100) surface was least reactive for lead oxidation. Overall, these results show that the photochemical reactivity of SrTiO3 is anisotropic and that on polar surfaces, dipolar fields arising from charged surface domains influence the transport of photogenerated charge carriers and promote spatially selective oxidation and reduction reactions. (Abstract shortened by UMI.)

Applying simulation model to uniform field space charge distribution measurements by the PEA method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Y.; Salama, M.M.A.

1996-12-31

Signals measured under uniform fields by the Pulsed Electroacoustic (PEA) method have been processed by the deconvolution procedure to obtain space charge distributions since 1988. To simplify data processing, a direct method has been proposed recently in which the deconvolution is eliminated. However, the surface charge cannot be represented well by the method because the surface charge has a bandwidth being from zero to infinity. The bandwidth of the charge distribution must be much narrower than the bandwidths of the PEA system transfer function in order to apply the direct method properly. When surface charges can not be distinguished frommore » space charge distributions, the accuracy and the resolution of the obtained space charge distributions decrease. To overcome this difficulty a simulation model is therefore proposed. This paper shows their attempts to apply the simulation model to obtain space charge distributions under plane-plane electrode configurations. Due to the page limitation for the paper, the charge distribution originated by the simulation model is compared to that obtained by the direct method with a set of simulated signals.« less

Control of single-electron charging of metallic nanoparticles onto amorphous silicon surface.

PubMed

Weis, Martin; Gmucová, Katarína; Nádazdy, Vojtech; Capek, Ignác; Satka, Alexander; Kopáni, Martin; Cirák, Július; Majková, Eva

2008-11-01

Sequential single-electron charging of iron oxide nanoparticles encapsulated in oleic acid/oleyl amine envelope and deposited by the Langmuir-Blodgett technique onto Pt electrode covered with undoped hydrogenated amorphous silicon film is reported. Single-electron charging (so-called quantized double-layer charging) of nanoparticles is detected by cyclic voltammetry as current peaks and the charging effect can be switched on/off by the electric field in the surface region induced by the excess of negative/positive charged defect states in the amorphous silicon layer. The particular charge states in amorphous silicon are created by the simultaneous application of a suitable bias voltage and illumination before the measurement. The influence of charged states on the electric field in the surface region is evaluated by the finite element method. The single-electron charging is analyzed by the standard quantized double layer model as well as two weak-link junctions model. Both approaches are in accordance with experiment and confirm single-electron charging by tunnelling process at room temperature. This experiment illustrates the possibility of the creation of a voltage-controlled capacitor for nanotechnology.

Emergence of charge density waves and a pseudogap in single-layer TiTe2.

PubMed

Chen, P; Pai, Woei Wu; Chan, Y-H; Takayama, A; Xu, C-Z; Karn, A; Hasegawa, S; Chou, M Y; Mo, S-K; Fedorov, A-V; Chiang, T-C

2017-09-11

Two-dimensional materials constitute a promising platform for developing nanoscale devices and systems. Their physical properties can be very different from those of the corresponding three-dimensional materials because of extreme quantum confinement and dimensional reduction. Here we report a study of TiTe 2 from the single-layer to the bulk limit. Using angle-resolved photoemission spectroscopy and scanning tunneling microscopy and spectroscopy, we observed the emergence of a (2 × 2) charge density wave order in single-layer TiTe 2 with a transition temperature of 92 ± 3 K. Also observed was a pseudogap of about 28 meV at the Fermi level at 4.2 K. Surprisingly, no charge density wave transitions were observed in two-layer and multi-layer TiTe 2 , despite the quasi-two-dimensional nature of the material in the bulk. The unique charge density wave phenomenon in the single layer raises intriguing questions that challenge the prevailing thinking about the mechanisms of charge density wave formation.Due to reduced dimensionality, the properties of 2D materials are often different from their 3D counterparts. Here, the authors identify the emergence of a unique charge density wave (CDW) order in monolayer TiTe 2 that challenges the current understanding of CDW formation.

Electrification of particulate entrained fluid flows-Mechanisms, applications, and numerical methodology

NASA Astrophysics Data System (ADS)

Wei, Wei; Gu, Zhaolin

2015-10-01

Particulates in natural and industrial flows have two basic forms: liquid (droplet) and solid (particle). Droplets would be charged in the presence of the applied electric field (e.g. electrospray). Similar to the droplet charging, particles can also be charged under the external electric field (e.g. electrostatic precipitator), while in the absence of external electric field, tribo-electrostatic charging is almost unavoidable in gas-solid two-phase flows due to the consecutive particle contacts (e.g. electrostatic in fluidized bed or wind-blown sand). The particle charging may be beneficial, or detrimental. Although electrostatics in particulate entrained fluid flow systems have been so widely used and concerned, the mechanisms of particulate charging are still lack of a thorough understanding. The motivation of this review is to explore a clear understanding of particulate charging and movement of charged particulate in two-phase flows, by summarizing the electrification mechanisms, physical models of particulate charging, and methods of charging/charged particulate entrained fluid flow simulations. Two effective methods can make droplets charged in industrial applications: corona charging and induction charging. The droplet charge to mass ratio by corona charging is more than induction discharge. The particle charging through collisions could be attributed to electron transfer, ion transfer, material transfer, and/or aqueous ion shift on particle surfaces. The charges on charged particulate surface can be measured, nevertheless, the charging process in nature or industry is difficult to monitor. The simulation method might build a bridge of investigating from the charging process to finally charged state on particulate surface in particulate entrained fluid flows. The methodology combining the interface tracking under the action of the applied electric with the fluid flow governing equations is applicable to the study of electrohydrodynamics problems. The charge distribution and mechanical behaviors of liquid surface can be predicted by using this method. The methodology combining particle charging model with Computational Fluid Dynamics (CFD) and Discrete element method (DEM) is applicable to study the particle charging/charged processes in gas-solid two phase flows, the influence factors of particle charging, such as gas-particle interaction, contact force, contact area, and various velocities, are described systematically. This review would explore a clear understanding of the particulate charging and provide theoretical references to control and utilize the charging/charged particulate entrained fluid system.

From Folding to Function: Design of a New Switchable Biosurfactant Protein.

PubMed

Zhao, Chun-Xia; Dwyer, Mirjana Dimitrijev; Yu, Lei; Middelberg, Anton P J

2017-03-03

A new anionic biosurfactant protein (SP16) capable of tuning foaming behaviour by pH or salt has been designed. This biosurfactant exhibits unique foaming behaviour with high sensitivity to pH. A good level of foaming was observed at pH 2 but not at pH 3. A further increase by one pH unit to pH 4 restored good foaming. At pH 5-8, SP16 again showed low foaming propensity, whereas the presence of salt (NaCl) was able to restore foaming again. Interfacial tension and circular dichroism investigations revealed the foaming control mechanism. The high negative charge (-16.6) at pH 6 and above restricted the ability of SP16 to fold into an α-helical conformation and also restricted surface activity. For pH 5 (-13.6), even though SP16 folds in bulk to give α-helical structure, the high charge inhibited adsorption at the air-water interface, resulting in a significant lag time of about 150-200 sec to achieve a decrease in interfacial tension. In contrast to its low foaming behaviour at pH 5-8, the presence of salt (NaCl) was found to effectively screen negative charge, thus leading to its folding and a decrease of interfacial tension. This new design offers a new strategy to control foaming behaviour, and elaborates a clear link between charge, structure and interfacial activity for biosurfactants. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

{112} Polar surfaces of copper(indium,gallium)selenide: Properties and effects on crystal growth

NASA Astrophysics Data System (ADS)

Liao, Dongxiang

Cu(In,Ga)Se2 (GIGS) are promising materials for thin film photovoltaic applications. This work studies the epitaxial growth of CIGS single crystal films on GaAs substrates of various orientations and characterizes the properties of the thin films. A surprising finding is the strong tendency of film surfaces to facet to {112} planes. The work attempted to establish the connections between the film morphology, the surface energies, the surface chemical compositions, and the reconstruction of polar surfaces. Using angle-resolved photoelectron emission spectroscopy, I found that there is a severe Cu depletion at the first 1-2 layer of the free surface of CuInSe2 and the surface is semiconducting. The results strongly support the model of a reconstructed non-stoichiometric polar surface and exclude the previously believed existence of a bulk second phase on the CIS surface. Unique features of the film morphology suggest that the properties and structure of the polar surfaces have great effects on the growth of the crystals, and probably on the incorporation of the large amount of point defects. Measured chemical composition profiles indicate that the Cu depletion observed on free CIGS surface remains at the CIGS/CdS heterojunction interface and Cd is incorporated into the surface of CIGS. It is proposed that this non-stoichiometric composition leads to charge imbalance at the interface and causes the type-inversion of the CIGS surface, which are favorable for the device performance.

SEM Characterization of Extinguished Grains from Plasma-Ignited M30 Charges

NASA Technical Reports Server (NTRS)

Kinkennon, A.; Birk, A.; DelGuercio, M.; Kaste, P.; Lieb, R.; Newberry, J.; Pesce-Rodriguez, R.; Schroeder, M.

2000-01-01

M30 propellant grains that had been ignited in interrupted closed bomb experiments were characterize by scanning electron microscopy (SEM). Previous chemical analysis of extinguished grains had given no indications of plasma-propellant chemical interactions that could explain the increased burning rates that had been previously observed in full-pressure closed bomb experiments. (This does not mean that there is no unique chemistry occurring with plasma ignition. It may occur very early in the ignition event and then become obscured by the burning chemistry.) In this work, SEM was used to look at grain morphologies to determine if there were increases in the surface areas of the plasma-ignited grains which would contribute to the apparent increase in the burning rate. Charges were made using 30 propellant grains (approximately 32 grams) stacked in two tiers and in two concentric circles around a plastic straw. Each grain was notched so that, when the grains were expelled from the bomb during extinguishment, it could be determined in which tier and which circle each grain was originally packed. Charges were ignited in a closed bomb by either a nickel wire/Mylar-capillary plasma or black powder. The bomb contained a blowout disk that ruptured when the pressure reached 35 MPa, and the propellant was vented into a collection chamber packed with polyurethane foam. SEM analysis of the grains fired with a conventional black powder igniter showed no signs of unusual burning characteristics. The surfaces seemed to be evenly burned on the exteriors of the grains and in the perforations. Grains that had been subjected to plasma ignition, however, had pits, gouges, chasms, and cracks in the surfaces. The sides of the grains closest to the plasma had the greatest amount of damage, but even surfaces facing the outer wall of the bomb had small pits. The perforations contained gouges and abnormally burned regions (wormholes) that extended into the web. The SEM photos indicated that a grain from the top tier, which was farther away from the plasma ignition source, sustained more plasma-induced damage to the perforations and the web than did the grains on the bottom tier.

Charge Retention by Organometallic Dications on Self-Assembled Monolayer Surfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Laskin, Julia; Wang, Peng

2014-05-15

Charge retention by mass-selected ruthenium trisbipyridine dications, or Ru(bpy)32+, soft-landed onto self-assembled monolayer (SAM) surfaces of 1H, 1H, 2H, 2H-perfluorodecane-1-thiol (FSAM), 11-mercaptoundecanoic acid (COOH-SAM), and 11-amino-1-undecanethiol (HSAM) on gold was examined using in situ time-resolved secondary ion mass spectrometry in a Fourier transform ion cyclotron resonance apparatus (FT-ICR SIMS). FT-ICR SIMS analysis was performed during ion soft-landing and for 8–15 hours after the ion beam was switched off. Our results demonstrate efficient retention of the doubly charged precursor ion on the FSAM and COOH-SAM surfaces manifested by the abundant Ru(bpy)32+ ions in the SIMS spectra. In contrast, only the singlymore » charged Ru(bpy)3+ and Ru(bpy)2+ ions were observed on HSAM, indicating rapid loss of at least one charge by the deposited dications. The signal of Ru(bpy)32+ on COOH-SAM remained almost constant for more than 8 hours after the end of ion soft-landing, while a relatively fast decay followed by a plateau region was observed on the FSAM surface. However, we found that SIMS analysis of Ru(bpy)32+ ions soft-landed onto FSAM is complicated by facile ion-molecule reactivity occurring either on the surface or in the SIMS plume, making it difficult to accurately measure the charge reduction kinetics. Efficient retention of the doubly charged Ru(bpy)32+ ions on COOH-SAM is remarkably different from facile neutralization of protonated peptides deposited onto this surface reported in previous studies. Our results indicate different mechanisms of charge reduction of protonated molecules and permanent ions, such as Ru(bpy)32+, on SAM surfaces. Thus, we propose that proton loss is the major charge reduction channel for the protonated species, while electron transfer through the insulating SAM is responsible for the charge loss by permanent ions. Fundamental understanding of charge reduction phenomena is essential for controlled preparation of catalytically active substrates using ion soft-landing.« less

Characterization of triboelectrically charged particles deposited on dielectric surfaces

NASA Astrophysics Data System (ADS)

Nesterov, A.; Löffler, F.; Cheng, Yun-Chien; Torralba, G.; König, K.; Hausmann, M.; Lindenstruth, V.; Stadler, V.; Bischoff, F. R.; Breitling, F.

2010-04-01

A device for the measurement of q/m-values and charge degradation of triboelectrically charged particles deposited on a surface was developed. The setup is based on the integration of currents, which are induced in a Faraday cage by insertion of a solid support covered with charged particles. The conductivity of different particle supports was taken into account. The 'blow-off' method, in which the particles are first deposited, and then blown off using an air stream, can be used for characterization of triboelectric properties of particles relative to different surfaces.

Dust Grain Charge in the Lunar Environment

NASA Astrophysics Data System (ADS)

Vaverka, Jakub; Richterova, Ivana; Vysinka, Marek; Pavlu, Jiri; Safrankova, Jana; Nemecek, Zdenek

2014-05-01

Interaction of a lunar surface with solar wind and magnetosphere plasmas leads to it charging by several processes as photoemission, a collection of primary particles and secondary electron emission. Nevertheless, charging of the lunar surface is complicated by a presence of crustal magnetic anomalies with can generate a "mini-magnetosphere" capable for more or less complete shielding the surface. On the other hand, shielding of solar light and plasma particles by rocks and craters can also locally influence the surface potential as well as a presence of a plasma wake strongly changes this potential at the night side of the Moon. A typical surface potential varies from slightly positive (dayside) to negative values of the order of several hundred of volts (night side). At the night side, negative potentials can reach -4 kV during solar energetic particle (SEP) events. Recent measurements of the surface potential by Lunar Prospector and Artemis spacecraft have shown surprisingly high negative dayside surface potentials (-500 V) during the magnetotail crossings as well as the positive surface potential higher than 100 V. One possible explanation is its non-monotonic profile above a surface where the potential minimum is formed by the space charge. Dust grains presented in this complicated environment are also charged by similar processes as the lunar surface. A strong dependence of the secondary electron yield on the grain size can significantly influence dust charging mainly in the Earth's plasma sheet where an equilibrium grain potential can by different than the surface potential and can reach even the opposite sign. This process can lead to levitation of dust above a surface observed by the Surveyor spacecraft.

Development of Charge to Mass Ratio Microdetector for Future Mars Mission

NASA Technical Reports Server (NTRS)

Chen, Yuan-Lian Albert

2003-01-01

The Mars environment comprises a dry, cold and low air pressure atmosphere with low gravity (0.38g) and high resistivity soil. The global dust storms that cover a large portion of Mars are observed often from Earth. This environment provides an ideal condition for turboelectric charging. The extremely dry conditions on the Martian surface have raised concerns that electrostatic charge buildup will not be dissipated easily. If turboelectrically generated charge cannot be dissipated or avoided, then dust will accumulate on charged surfaces and electrostatic discharge may cause hazards for future exploration missions. The low surface on Mars helps to prolong the charge decay on the dust particles and soil. To better understanding the physics of Martian charged dust particles is essential to future Mars missions. We research and design two sensors, velocity/charge sensor and PZT momentum sensors, to measure the velocity distribution, charge distribution and mass distribution of Martian wed dust particles. These sensors are fabricated at NASA Kenney Space Center, Electrostatic and Surface Physics Laboratory. The sensors are calibrated. The momentum sensor is capable to measure 45 pan size particles. The designed detector is very simple, robust, without moving parts, and does not require a high voltage power supply. Two sensors are combined to form the Dust Microdetector - CHAL.

The Review on the Charge Distribution on the Conductor Surface

ERIC Educational Resources Information Center

Matehkolaee, M. Jafari; Asrami, A. Naderi

2013-01-01

In this paper we have a full review on the surface charge density at disordered conductor surfaces. Basically, reading text books does not resolve ambiguities in this field. As far as is possible, we have tried to the concepts easier to turn. In fact we will answer two questions. One of them is that why do charges tend to go where the curvature is…

Prominent metallic surface conduction and the singular magnetic response of topological Dirac fermion in three-dimensional topological insulator Bi1.5Sb0.5Te1.7Se1.3.

PubMed

Dutta, Prithwish; Pariari, Arnab; Mandal, Prabhat

2017-07-07

We report semiconductor to metal-like crossover in the temperature dependence of resistivity (ρ) due to the switching of charge transport from bulk to surface channel in three-dimensional topological insulator Bi 1.5 Sb 0.5 Te 1.7 Se 1.3 . Unlike earlier studies, a much sharper drop in ρ(T) is observed below the crossover temperature due to the dominant surface conduction. Remarkably, the resistivity of the conducting surface channel follows a rarely observable T 2 dependence at low temperature, as predicted theoretically for a two-dimensional Fermi liquid system. The field dependence of magnetization shows a cusp-like paramagnetic peak in the susceptibility (χ) at zero field over the diamagnetic background. The peak is found to be robust against temperature and χ decays linearly with the field from its zero-field value. This unique behavior of the χ is associated with the spin-momentum locked topological surface state in Bi 1.5 Sb 0.5 Te 1.7 Se 1.3 . The reconstruction of the surface state with time is clearly reflected through the reduction of the peak height with the age of the sample.

On the dependence of charge density on surface curvature of an isolated conductor

NASA Astrophysics Data System (ADS)

Bhattacharya, Kolahal

2016-03-01

A study of the relation between the electrostatic charge density at a point on a conducting surface and the curvature of the surface (at that point) is presented. Two major papers in the scientific literature on this topic are reviewed and the apparent discrepancy between them is resolved. Hence, a step is taken towards obtaining a general analytic formula for relating the charge density with surface curvature of conductors. The merit of this formula and its limitations are discussed.

Generation of neutral and high-density electron–positron pair plasmas in the laboratory

PubMed Central

Sarri, G.; Poder, K.; Cole, J. M.; Schumaker, W.; Di Piazza, A.; Reville, B.; Dzelzainis, T.; Doria, D.; Gizzi, L. A.; Grittani, G.; Kar, S.; Keitel, C. H.; Krushelnick, K.; Kuschel, S.; Mangles, S. P. D.; Najmudin, Z.; Shukla, N.; Silva, L. O.; Symes, D.; Thomas, A. G. R.; Vargas, M.; Vieira, J.; Zepf, M.

2015-01-01

Electron–positron pair plasmas represent a unique state of matter, whereby there exists an intrinsic and complete symmetry between negatively charged (matter) and positively charged (antimatter) particles. These plasmas play a fundamental role in the dynamics of ultra-massive astrophysical objects and are believed to be associated with the emission of ultra-bright gamma-ray bursts. Despite extensive theoretical modelling, our knowledge of this state of matter is still speculative, owing to the extreme difficulty in recreating neutral matter–antimatter plasmas in the laboratory. Here we show that, by using a compact laser-driven setup, ion-free electron–positron plasmas with unique characteristics can be produced. Their charge neutrality (same amount of matter and antimatter), high-density and small divergence finally open up the possibility of studying electron–positron plasmas in controlled laboratory experiments. PMID:25903920

Generation of neutral and high-density electron-positron pair plasmas in the laboratory.

PubMed

Sarri, G; Poder, K; Cole, J M; Schumaker, W; Di Piazza, A; Reville, B; Dzelzainis, T; Doria, D; Gizzi, L A; Grittani, G; Kar, S; Keitel, C H; Krushelnick, K; Kuschel, S; Mangles, S P D; Najmudin, Z; Shukla, N; Silva, L O; Symes, D; Thomas, A G R; Vargas, M; Vieira, J; Zepf, M

2015-04-23

Electron-positron pair plasmas represent a unique state of matter, whereby there exists an intrinsic and complete symmetry between negatively charged (matter) and positively charged (antimatter) particles. These plasmas play a fundamental role in the dynamics of ultra-massive astrophysical objects and are believed to be associated with the emission of ultra-bright gamma-ray bursts. Despite extensive theoretical modelling, our knowledge of this state of matter is still speculative, owing to the extreme difficulty in recreating neutral matter-antimatter plasmas in the laboratory. Here we show that, by using a compact laser-driven setup, ion-free electron-positron plasmas with unique characteristics can be produced. Their charge neutrality (same amount of matter and antimatter), high-density and small divergence finally open up the possibility of studying electron-positron plasmas in controlled laboratory experiments.

Unusual inhomogeneous microstructures in charge glass state of PbCrO3

NASA Astrophysics Data System (ADS)

Kurushima, Kosuke; Tsukasaki, Hirofumi; Ogata, Takahiro; Sakai, Yuki; Azuma, Masaki; Ishii, Yui; Mori, Shigeo

2018-05-01

We investigated the microstructures and local structures of perovskite PbCrO3, which shows a metal-to-insulator transition and a 9.8% volume collapse, by electron diffraction, high-resolution transmission electron microscopy (TEM), and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). It is revealed that the charge glass state is characterized by the unique coexistence of the crystalline state with a cubic symmetry on average and the noncrystalline state. HAADF-STEM observation at atomic resolution revealed that Pb ions were displaced from the ideal A site position of the cubic perovskite structure, which gives rise to characteristic diffuse scatterings around the fundamental Bragg reflections. These structural inhomogeneities are crucial to the understanding of the unique physical properties in the charge glass state of PbCrO3.

Charging of particles on a surface

NASA Astrophysics Data System (ADS)

Heijmans, Lucas; Nijdam, Sander

2016-09-01

This contribution focusses on the seemingly easy problem of the charging of micrometer sized particles on a substrate in a plasma. This seems trivial, because much is known about both the charging of surfaces near a plasma and of particles in the plasma bulk. The problem, however, becomes much more complicated when the particle is on the substrate surface. The charging currents to the particle are then highly altered by the substrate plasma sheath. Currently there is no consensus in literature about the resulting particle charge. We shall present both experimental measurements and numerical simulations of the charge on these particles. The experimental results are acquired by measuring the particle acceleration in an external electric field. For the simulations we have used our specially developed model. We shall compare these results to other estimates found in literature.

Enhanced electrohydrodynamic force generation in a two-stroke cycle dielectric-barrier-discharge plasma actuator

NASA Astrophysics Data System (ADS)

Sato, Shintaro; Takahashi, Masayuki; Ohnishi, Naofumi

2017-05-01

An approach for electrohydrodynamic (EHD) force production is proposed with a focus on a charge cycle on a dielectric surface. The cycle, consisting of positive-charging and neutralizing strokes, is completely different from the conventional methodology, which involves a negative-charging stroke, in that the dielectric surface charge is constantly positive. The two-stroke charge cycle is realized by applying a DC voltage combined with repetitive pulses. Simulation results indicate that the negative pulse eliminates the surface charge accumulated during constant voltage phase, resulting in repetitive EHD force generation. The time-averaged EHD force increases almost linearly with increasing repetitive pulse frequency and becomes one order of magnitude larger than that driven by the sinusoidal voltage, which has the same peak-to-peak voltage.

Simulation study of spheroidal dust gains charging: Applicable to dust grain alignment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zahed, H.; Sobhanian, S.; Mahmoodi, J.

2006-09-15

The charging process of nonspherical dust grains in an unmagnetized plasma as well as in the presence of a magnetic field is studied. It is shown that unlike the spherical dust grain, due to nonhomogeneity of charge distribution on the spheroidal dust surface, the resultant electric forces on electrons and ions are different. This process produces some surface charge density gradient on the nonspherical grain surface. Effects of a magnetic field and other plasma parameters on the properties of the dust particulate are studied. It has been shown that the alignment direction could be changed or even reversed with themore » magnetic field and plasma parameters. Finally, the charge distribution on the spheroidal grain surface is studied for different ambient parameters including plasma temperature, neutral collision frequency, and the magnitude of the magnetic field.« less

Model simulations of the adsorption of statherin to solid surfaces: Effects of surface charge and hydrophobicity

NASA Astrophysics Data System (ADS)

Skepö, M.

2008-11-01

The structural properties of the salivary protein statherin upon adsorption have been examined using a coarse-grained model and Monte Carlo simulation. A simple model system with focus on electrostatic interactions and short-ranged attractions among the uncharged amino acids has been used. To mimic hydrophobically modified surfaces, an extra short-ranged interaction was implemented between the amino acids and the surface. It has been shown that the adsorption and the thickness of the adsorbed layer are determined by (i) the affinity for the surface, i.e., denser layer with an extrashort-ranged potential, and (ii) the distribution of the charges along the chain. If all the amino acids have a high affinity for the surface, the protein adsorbs in a train conformation, if the surface is negatively charged the protein adsorbs in a tail-train conformation, whereas if the surface is positively charged the protein adsorbs in a loop conformation. The latter gives rise to a more confined adsorbed layer.

Tree branch-shaped cupric oxide for highly effective photoelectrochemical water reduction

NASA Astrophysics Data System (ADS)

Jang, Youn Jeong; Jang, Ji-Wook; Choi, Sun Hee; Kim, Jae Young; Kim, Ju Hun; Youn, Duck Hyun; Kim, Won Yong; Han, Suenghoon; Sung Lee, Jae

2015-04-01

Highly efficient tree branch-shaped CuO photocathodes are fabricated using the hybrid microwave annealing process with a silicon susceptor within 10 minutes. The unique hierarchical, one-dimensional structure provides more facile charge transport, larger surface areas, and increased crystallinity and crystal ordering with less defects compared to irregular-shaped CuO prepared by conventional thermal annealing. As a result, the photocathode fabricated with the tree branch-shaped CuO produces an unprecedently high photocurrent density of -4.4 mA cm-2 at 0 VRHE under AM 1.5 G simulated sunlight compared to -1.44 mA cm-2 observed for a photocathode fabricated by thermal annealing. It is also confirmed that stoichiometric hydrogen and oxygen are produced from photoelectrochemical water splitting on the tree branch-shaped CuO photocathode and a platinum anode.Highly efficient tree branch-shaped CuO photocathodes are fabricated using the hybrid microwave annealing process with a silicon susceptor within 10 minutes. The unique hierarchical, one-dimensional structure provides more facile charge transport, larger surface areas, and increased crystallinity and crystal ordering with less defects compared to irregular-shaped CuO prepared by conventional thermal annealing. As a result, the photocathode fabricated with the tree branch-shaped CuO produces an unprecedently high photocurrent density of -4.4 mA cm-2 at 0 VRHE under AM 1.5 G simulated sunlight compared to -1.44 mA cm-2 observed for a photocathode fabricated by thermal annealing. It is also confirmed that stoichiometric hydrogen and oxygen are produced from photoelectrochemical water splitting on the tree branch-shaped CuO photocathode and a platinum anode. Electronic supplementary information (ESI) available: The detailed schematic diagram for the HMA process, XRD results, the temperature profile during HMA, derivative XANES results, TEM images, J-V curves, lists of previously reported copper oxide photocathode, and parameters extracted from EIS. See DOI: 10.1039/c5nr00208g

A Proposed Model for Protein Crystal Nucleation and Growth

NASA Technical Reports Server (NTRS)

Pusey, Marc; Curreri, Peter A. (Technical Monitor)

2002-01-01

How does one take a molecule, strongly asymmetric in both shape and charge distribution, and assemble it into a crystal? We propose a model for the nucleation and crystal growth process for tetragonal lysozyme, based upon fluorescence, light, neutron, and X-ray scattering data, size exclusion chromatography experiments, dialysis kinetics, AFM, and modeling of growth rate data, from this and other laboratories. The first species formed is postulated to be a 'head to side' dimer. Through repeating associations involving the same intermolecular interactions this grows to a 4(sub 3) helix structure, that in turn serves as the basic unit for nucleation and subsequent crystal growth. High salt attenuates surface charges while promoting hydrophobic interactions. Symmetry facilitates subsequent helix-helix self-association. Assembly stability is enhanced when a four helix structure is obtained, with each bound to two neighbors. Only two unique interactions are required. The first are those for helix formation, where the dominant interaction is the intermolecular bridging anion. The second is the anti-parallel side-by-side helix-helix interaction, guided by alternating pairs of symmetry related salt bridges along each side. At this stage all eight unique positions of the P4(sub3)2(sub 1),2(sub 1) unit cell are filled. The process is one of a) attenuating the most strongly interacting groups, such that b) the molecules begin to self-associate in defined patterns, so that c) symmetry is obtained, which d) propagates as a growing crystal. Simple and conceptually obvious in hindsight, this tells much about what we are empirically doing when we crystallize macromolecules. By adjusting the growth parameters we are empirically balancing the intermolecular interactions, preferentially attenuating the dominant strong (for lysozyme the charged groups) while strengthening the lesser strong (hydrophobic) interactions. In the general case for proteins the lack of a singularly defined association pathway may lead to formation of multiple species, i.e., amorphous precipitation. Weak interactions, such as hydrogen bonds, are promiscuous, serving to strengthen rather than define specific interactions. Participation in an interaction sequesters that surface from subsequent interactions, and we expect the strongest bonds to form first. This model, its basis, how it fits into the currently understood osmotic second virial coefficient approach to crystallization, and what it suggests will be discussed.

Charge Storage, Conductivity and Charge Profiles of Insulators as Related to Spacecraft Charging

NASA Technical Reports Server (NTRS)

Dennison, J. R.; Swaminathan, Prasanna; Frederickson, A. R.

2004-01-01

Dissipation of charges built up near the surface of insulators due to space environment interaction is central to understanding spacecraft charging. Conductivity of insulating materials is key to determine how accumulated charge will distribute across the spacecraft and how rapidly charge imbalance will dissipate. To understand these processes requires knowledge of how charge is deposited within the insulator, the mechanisms for charge trapping and charge transport within the insulator, and how the profile of trapped charge affects the transport and emission of charges from insulators. One must consider generation of mobile electrons and holes, their trapping, thermal de-trapping, mobility and recombination. Conductivity is more appropriately measured for spacecraft charging applications as the "decay" of charge deposited on the surface of an insulator, rather than by flow of current across two electrodes around the sample. We have found that conductivity determined from charge storage decay methods is 102 to 104 smaller than values obtained from classical ASTM and IEC methods for a variety of thin film insulating samples. For typical spacecraft charging conditions, classical conductivity predicts decay times on the order of minutes to hours (less than typical orbit periods); however, the higher charge storage conductivities predict decay times on the order of weeks to months leading to accumulation of charge with subsequent orbits. We found experimental evidence that penetration profiles of radiation and light are exceedingly important, and that internal electric fields due to charge profiles and high-field conduction by trapped electrons must be considered for space applications. We have also studied whether the decay constants depend on incident voltage and flux or on internal charge distributions and electric fields; light-activated discharge of surface charge to distinguish among differing charge trapping centers; and radiation-induced conductivity. Our experiments also show that "Malter" electron emission occurs for hours after turning off the electron beam. This Malter emission similar to emission due to negative electron affinity in semiconductors is a result of the prior radiation or optical excitations of valence electrons and their slow drift among traps towards the surface where they are subsequently emitted. This work is supported through funding from the NASA Space Environments and Effects Program.

Investigations of charged particle motion on the surfaces of dusty, airless solar system bodies (Invited)

NASA Astrophysics Data System (ADS)

Dove, A.; Colwell, J. E.

2013-12-01

Dynamic charging conditions exist on the dusty surfaces of planetary bodies such as the Moon, asteroids, and the moons of Mars. On these so-called 'airless bodies', the motions of dust particles above the surface become complex due to grain-grain and grain-plasma interactions. For example, tribocharging and other charge transfer processes can occur due to relative dust grain movements, and charged dust grains immersed in plasma interact with local electromagnetic forces. This is thought to lead to effects such as the lunar 'horizon glow,' (Rennilson and Criswell, 1974, The Moon, 10) and potential dusty 'fountains' above the lunar surface (Stubbs et al., 2006, Adv. Sp. Res., 37). Regolith grains can be mobilized by impacts or other mechanical disturbances, or simply by the Coulomb force acting on grains. Previous work has increased our theoretical understanding of the behavior of charged particles in these low-gravity environments (i.e. Poppe and Horanyi, 2010, JGR, A115; Colwell et al., 2007, Rev. Geophys., 45 (and references therein)). Experimental work has also analyzed grain surface charging due to plasma or tribocharging (Sickafoose et al., 2001, JGR, 106) and the motion of grains on surfaces in the presence of an electric field (Wang et al., 2009, JGR, 114). Occasionally, there is disagreement between theoretical predictions and observations. We present the results of new laboratory experiments aimed at understanding particle charging and the dynamics of charged particles on the surfaces of airless bodies. In the initial experiments, we analyze the motion of particles in the presence of an electric field in vacuum, either in a bell-jar or in a 0.75-second microgravity drop tower experiment box. Prior to motion, particles may be charged due to triboelectric effects, plasma interactions, or a combination of the two. Motion is induced by shaking or by low-velocity impacts in order to simulate the natural motion of slow-moving objects on regolith surfaces, or induced motion such as that due to a spacecraft. The resulting particle dynamics are tracked using high-speed, high-resolution video. Future exploration on or near the surfaces of airless bodies will certainly experience complications arising from these dusty environments, where particles may contaminate or interfere with the operation of almost any mechanical equipment. By exploring the dynamic behavior of charged particles in these environments, we can work towards solutions that will enable exploration.

Differential photoelectric charging of nonconducting surfaces in space. [on sunlit strip

NASA Technical Reports Server (NTRS)

Pelizzari, M. A.; Criswell, D. R.

1978-01-01

The photoelectric charging caused by an infinitely long strip of sunlight across a nonconducting plane is studied by use of a model which contains an electrical cutoff radius, and the results of numerical calculations are presented. The model simulates charging of a sunlit area with dimensions equal to the strip's width, exposed to a plasma with a comparatively large Debye length. Uniform potential is quickly established on a uniformly sunlit strip as a result of charge redistribution by low-energy photoelectrons. The results are in accord with a theoretical surface conductivity derived for photoelectron sheaths above highly charged sunlit areas. The surface potential, which drops sharply across the sunlight-shadow boundary, is discussed.

On the theoretical description of weakly charged surfaces.

PubMed

Wang, Rui; Wang, Zhen-Gang

2015-03-14

It is widely accepted that the Poisson-Boltzmann (PB) theory provides a valid description for charged surfaces in the so-called weak coupling limit. Here, we show that the image charge repulsion creates a depletion boundary layer that cannot be captured by a regular perturbation approach. The correct weak-coupling theory must include the self-energy of the ion due to the image charge interaction. The image force qualitatively alters the double layer structure and properties, and gives rise to many non-PB effects, such as nonmonotonic dependence of the surface energy on concentration and charge inversion. In the presence of dielectric discontinuity, there is no limiting condition for which the PB theory is valid.

Dynamics of charges and solitons

NASA Astrophysics Data System (ADS)

Barros, Manuel; Ferrández, Ángel; Garay, Óscar J.

2018-02-01

We first show that trajectories traced by charges moving in rotational magnetic fields are, basically, the non-parallel geodesics of surfaces of revolution with coincident axis. Thus, people living in a surface of revolution are not able to sense the magnetic Hall effect induced by the surrounding magnetic field and perceive charges as influenced, exclusively, by the gravity action on the surface of revolution. Secondly, the extended Hasimoto transformations are introduced and then used to identify trajectories of charges moving through a Killing rotational magnetic field in terms of non-circular elastic curves. As a consequence, we see that in this case charges evolve along trajectories which are obtained as extended Hasimoto transforms of solitons of the filament equation.

Charged plate in asymmetric electrolytes: One-loop renormalization of surface charge density and Debye length due to ionic correlations.

PubMed

Ding, Mingnan; Lu, Bing-Sui; Xing, Xiangjun

2016-10-01

Self-consistent field theory (SCFT) is used to study the mean potential near a charged plate inside a m:-n electrolyte. A perturbation series is developed in terms of g=4πκb, where band1/κ are Bjerrum length and bare Debye length, respectively. To the zeroth order, we obtain the nonlinear Poisson-Boltzmann theory. For asymmetric electrolytes (m≠n), the first order (one-loop) correction to mean potential contains a secular term, which indicates the breakdown of the regular perturbation method. Using a renormalizaton group transformation, we remove the secular term and obtain a globally well-behaved one-loop approximation with a renormalized Debye length and a renormalized surface charge density. Furthermore, we find that if the counterions are multivalent, the surface charge density is renormalized substantially downwards and may undergo a change of sign, if the bare surface charge density is sufficiently large. Our results agrees with large MC simulation even when the density of electrolytes is relatively high.

Coarse-grained modeling of proline rich protein 1 (PRP-1) in bulk solution and adsorbed to a negatively charged surface.

PubMed

Skepö, Marie; Linse, Per; Arnebrant, Thomas

2006-06-22

Structural properties of the acidic proline rich protein PRP-1 of salivary origin in bulk solution and adsorbed onto a negatively charged surface have been studied by Monte Carlo simulations. A simple model system with focus on electrostatic interactions and short-ranged attractions among the uncharged amino acids has been used. In addition to PRP-1, some mutants were considered to assess the role of the interactions in the systems. Contrary to polyelectrolytes, the protein has a compact structure in salt-free bulk solutions, whereas at high salt concentration the protein becomes more extended. The protein adsorbs to a negatively charged surface, although its net charge is negative. The adsorbed protein displays an extended structure, which becomes more compact upon addition of salt. Hence, the conformational response upon salt addition in the adsorbed state is the opposite as compared to that in bulk solution. The conformational behavior of PRP-1 in bulk solution and at charged surfaces as well as its propensity to adsorb to surfaces with the same net charge are rationalized by the block polyampholytic character of the protein. The presence of a triad of positively charged amino acids in the C-terminal was found to be important for the adsorption of the protein.

Cellulose nanocrystals with tunable surface charge for nanomedicine

NASA Astrophysics Data System (ADS)

Hosseinidoust, Zeinab; Alam, Md Nur; Sim, Goeun; Tufenkji, Nathalie; van de Ven, Theo G. M.

2015-10-01

Crystalline nanoparticles of cellulose exhibit attractive properties as nanoscale carriers for bioactive molecules in nanobiotechnology and nanomedicine. For applications in imaging and drug delivery, surface charge is one of the most important factors affecting the performance of nanocarriers. However, current methods of preparation offer little flexibility for controlling the surface charge of cellulose nanocrystals, leading to compromised colloidal stability under physiological conditions. We report a synthesis method that results in nanocrystals with remarkably high carboxyl content (6.6 mmol g-1) and offers continuous control over surface charge without any adjustment to the reaction conditions. Six fractions of nanocrystals with various surface carboxyl contents were synthesized from a single sample of softwood pulp with carboxyl contents varying from 6.6 to 1.7 mmol g-1 and were fully characterized. The proposed method resulted in highly stable colloidal nanocrystals that did not aggregate when exposed to high salt concentrations or serum-containing media. Interactions of these fractions with four different tissue cell lines were investigated over a wide range of concentrations (50-300 μg mL-1). Darkfield hyperspectral imaging and confocal microscopy confirmed the uptake of nanocrystals by selected cell lines without any evidence of membrane damage or change in cell density; however a charge-dependent decrease in mitochondrial activity was observed for charge contents higher than 3.9 mmol g-1. A high surface carboxyl content allowed for facile conjugation of fluorophores to the nanocrystals without compromising colloidal stability. The cellular uptake of fluoresceinamine-conjugated nanocrystals exhibited a time-dose dependent relationship and increased significantly with doubling of the surface charge.Crystalline nanoparticles of cellulose exhibit attractive properties as nanoscale carriers for bioactive molecules in nanobiotechnology and nanomedicine. For applications in imaging and drug delivery, surface charge is one of the most important factors affecting the performance of nanocarriers. However, current methods of preparation offer little flexibility for controlling the surface charge of cellulose nanocrystals, leading to compromised colloidal stability under physiological conditions. We report a synthesis method that results in nanocrystals with remarkably high carboxyl content (6.6 mmol g-1) and offers continuous control over surface charge without any adjustment to the reaction conditions. Six fractions of nanocrystals with various surface carboxyl contents were synthesized from a single sample of softwood pulp with carboxyl contents varying from 6.6 to 1.7 mmol g-1 and were fully characterized. The proposed method resulted in highly stable colloidal nanocrystals that did not aggregate when exposed to high salt concentrations or serum-containing media. Interactions of these fractions with four different tissue cell lines were investigated over a wide range of concentrations (50-300 μg mL-1). Darkfield hyperspectral imaging and confocal microscopy confirmed the uptake of nanocrystals by selected cell lines without any evidence of membrane damage or change in cell density; however a charge-dependent decrease in mitochondrial activity was observed for charge contents higher than 3.9 mmol g-1. A high surface carboxyl content allowed for facile conjugation of fluorophores to the nanocrystals without compromising colloidal stability. The cellular uptake of fluoresceinamine-conjugated nanocrystals exhibited a time-dose dependent relationship and increased significantly with doubling of the surface charge. Electronic supplementary information (ESI) available: Additional results are presented in the ESI in Fig. S1 through S4. See DOI: 10.1039/c5nr02506k

Surface correlation effects in two-band strongly correlated slabs.

PubMed

Esfahani, D Nasr; Covaci, L; Peeters, F M

2014-02-19

Using an extension of the Gutzwiller approximation for an inhomogeneous system, we study the two-band Hubbard model with unequal band widths for a slab geometry. The aim is to investigate the mutual effect of individual bands on the spatial distribution of quasi-particle weight and charge density, especially near the surface of the slab. The main effect of the difference in band width is the presence of two different length scales corresponding to the quasi-particle profile of each band. This is enhanced in the vicinity of the critical interaction of the narrow band where an orbitally selective Mott transition occurs and a surface dead layer forms for the narrow band. For the doped case, two different regimes of charge transfer between the surface and the bulk of the slab are revealed. The charge transfer from surface/center to center/surface depends on both the doping level and the average relative charge accumulated in each band. Such effects could also be of importance when describing the accumulation of charges at the interface between structures made of multi-band strongly correlated materials.

Surface Charge and Hydrophobicity of Endospores of Bacillus anthracis and Related Species in Aqueous Solution

EPA Science Inventory

The surface properties of microorganisms play an important role in attachment and detachment in the environment. The change in surface charge can effect coagulation, disinfection, adhesion to surfaces, uptake of chemicals, and environmental transport. In aqueous solution, cell s...

Convective transport of electric charge within the planetary boundary layer

NASA Astrophysics Data System (ADS)

Nicoll, Keri; Harrison, Giles; Silva, Hugo; Silgado, Rui; Melgao, Marta

2017-04-01

Turbulent and convective processes within the planetary boundary layer are responsible for the transport of moisture, momentum and particulate matter, but are also of major importance in determining the electrical charge structure of the lower atmosphere. This paper presents rare experimental measurements of vertical profiles of charge measured during fair weather conditions by specially instrumented radiosonde balloons over Alqueva, Portugal during the summer of 2014. Space charge was measured directly using a sensitive electrometer, rather than the conventional method of deriving it from electric field measurements. The high frequency of balloon flights enabled the diurnal variation in the vertical profile of charge within the boundary layer to be examined in detail, with much smaller levels of charge (up to 20pC m-3) observed during stable night time periods than during the day. Following sunrise, the evolution of the charge profile was much more complex, showing a dependence on lofting of surface aerosol due to daytime convection. This produced charge up to 92pC m-3 up to 500m above the surface. The diurnal variation in the integrated column of charge above the measurement site was also found to track closely with the diurnal variation in near surface charge as measured by an electric field mill at the same site, confirming the importance of the link between surface charge generation processes and aloft. Co-located lidar backscatter measurements were also made during the measurement campaign and will be discussed here in the context of the effect of aerosol on the vertical charge profile.

Rotaxane and catenane host structures for sensing charged guest species.

PubMed

Langton, Matthew J; Beer, Paul D

2014-07-15

CONSPECTUS: The promise of mechanically interlocked architectures, such as rotaxanes and catenanes, as prototypical molecular switches and shuttles for nanotechnological applications, has stimulated an ever increasing interest in their synthesis and function. The elaborate host cavities of interlocked structures, however, can also offer a novel approach toward molecular recognition: this Account describes the use of rotaxane and catenane host systems for binding charged guest species, and for providing sensing capability through an integrated optical or electrochemical reporter group. Particular attention is drawn to the exploitation of the unusual dynamic properties of interlocked molecules, such as guest-induced shuttling or conformational switching, as a sophisticated means of achieving a selective and functional sensor response. We initially survey interlocked host systems capable of sensing cationic guests, before focusing on our accomplishments in synthesizing rotaxanes and catenanes designed for the more challenging task of selective anion sensing. In our group, we have developed the use of discrete anionic templation to prepare mechanically interlocked structures for anion recognition applications. Removal of the anion template reveals an interlocked host system, possessing a unique three-dimensional geometrically restrained binding cavity formed between the interlocked components, which exhibits impressive selectivity toward complementary anionic guest species. By incorporating reporter groups within such systems, we have developed both electrochemical and optical anion sensors which can achieve highly selective sensing of anionic guests. Transition metals, lanthanides, and organic fluorophores integrated within the mechanically bonded structural framework of the receptor are perturbed by the binding of the guest, with a concomitant change in the emission profile. We have also exploited the unique dynamics of interlocked hosts by demonstrating that an anion-induced conformational change can be used as a means of signal transduction. Electrochemical sensing has been realized by integration of the redox-active ferrocene functionality within a range of rotaxane and catenanes; binding of an anion perturbs the metallocene, leading to a cathodic shift in the ferrocene/ferrocenium redox couple. In order to obtain practical sensors for target charged guest species, confinement of receptors at a surface is necessary in order to develop robust, reuseable devices. Surface confinement also offers advantages over solution based receptors, including amplification of signal, enhanced guest binding thermodynamics and the negation of solubility problems. We have fabricated anion-templated rotaxanes and catenanes on gold electrode surfaces and demonstrated that the resulting mechanically bonded self-assembled monolayers are electrochemically responsive to the binding of anions, a crucial first step toward the advancement of sophisticated, highly selective, anion sensory devices. Rotaxane and catenane host molecules may be engineered to offer a superior level of molecular recognition, and the incorporation of optical or electrochemical reporter groups within these interlocked frameworks can allow for guest sensing. Advances in synthetic templation strategies has facilitated the synthesis of interlocked architectures and widened their interest as prototype molecular machines. However, their unique host-guest properties are only now beginning to be exploited as a sophisticated approach to chemical sensing. The development of functional host-guest sensory systems such as these is of great interest to the interdisciplinary field of supramolecular chemistry.

Bounding Extreme Spacecraft Charging in the Lunar Environment

NASA Technical Reports Server (NTRS)

Minow, Joseph I.; Parker, Linda N.

2008-01-01

Robotic and manned spacecraft from the Apollo era demonstrated that the lunar surface in daylight will charge to positive potentials of a few tens of volts because the photoelectron current dominates the charging process. In contrast, potentials of the lunar surface in darkness which were predicted to be on the order of a hundred volts negative in the Apollo era have been shown more recently to reach values of a few hundred volts negative with extremes on the order of a few kilovolts. The recent measurements of night time lunar surface potentials are based on electron beams in the Lunar Prospector Electron Reflectometer data sets interpreted as evidence for secondary electrons generated on the lunar surface accelerated through a plasma sheath from a negatively charged lunar surface. The spacecraft potential was not evaluated in these observations and therefore represents a lower limit to the magnitude of the lunar negative surface potential. This paper will describe a method for obtaining bounds on the magnitude of lunar surface potentials from spacecraft measurements in low lunar orbit based on estimates of the spacecraft potential. We first use Nascap-2k surface charging analyses to evaluate potentials of spacecraft in low lunar orbit and then include the potential drops between the ambient space environment and the spacecraft to the potential drop between the lunar surface and the ambient space environment to estimate the lunar surface potential from the satellite measurements.

Enhancing image contrast of carbon nanotubes on cellular background using helium ion microscope by varying helium ion fluence.

PubMed

Dykas, M M; Poddar, K; Yoong, S L; Viswanathan, V; Mathew, S; Patra, A; Saha, S; Pastorin, G; Venkatesan, T

2018-01-01

Carbon nanotubes (CNTs) have become an important nano entity for biomedical applications. Conventional methods of their imaging, often cannot be applied in biological samples due to an inadequate spatial resolution or poor contrast between the CNTs and the biological sample. Here we report a unique and effective detection method, which uses differences in conductivities of carbon nanotubes and HeLa cells. The technique involves the use of a helium ion microscope to image the sample with the surface charging artefacts created by the He + and neutralised by electron flood gun. This enables us to obtain a few nanometre resolution images of CNTs in HeLa Cells with high contrast, which was achieved by tailoring the He + fluence. Charging artefacts can be efficiently removed for conductive CNTs by a low amount of electrons, the fluence of which is not adequate to discharge the cell surface, resulting in high image contrast. Thus, this technique enables rapid detection of any conducting nano structures on insulating cellular background even in large fields of view and fine spatial resolution. The technique demonstrated has wider applications for researchers seeking enhanced contrast and high-resolution imaging of any conducting entity in a biological matrix - a commonly encountered issue of importance in drug delivery, tissue engineering and toxicological studies. © 2017 The Authors Journal of Microscopy © 2017 Royal Microscopical Society.

Photo-inducible Crosslinked Nanoassemblies for pH-Controlled Drug Release

PubMed Central

Dickerson, Matthew; Winquist, Nickolas; Bae, Younsoo

2014-01-01

Purpose To control drug release from block copolymer nanoassemblies by variation in the degree of photo-crosslinking and inclusion of acid sensitive linkers. Methods Poly(ethylene glycol)-poly(aspartate-hydrazide-cinnamate) (PEG-CNM) block copolymers were prepared and conjugated with a model drug, doxorubicin (DOX), through acid sensitive hydrazone linkers. The block copolymers formed photo-inducible, self-assembled nanoassemblies (piSNAs), which were used to produce photo-inducible crosslinked nanoassemblies (piCNAs) through UV crosslinking. The nanoassemblies were characterized to determine particle size, surface charge, pH- and crosslinking-dependent DOX release, in vitro cytotoxicity, and intracellular uptake as a function of photo-crosslinking degree. Results Nanoassemblies with varying photo-crosslinking degrees were successfully prepared while retaining particle size and surface charge. Photo-crosslinking caused no noticeable change in DOX release from the nanoassemblies at pH 7.4, but the DOX-loaded nanoassemblies modulated drug release as a function of crosslinking at pH 6.0. The nanoassemblies showed similar cytotoxicity regardless of crosslinking degrees, presumably due to the low cellular uptake and cell nucleus drug accumulation. Conclusion Photo-crosslinking is useful to control drug release from pH-sensitive block copolymer nanoassemblies as a function of crosslinking without altering the particle properties, and thus providing unique tools to investigate the pharmaceutical effects of drug release on cellular response. PMID:24254196

Density of Trap States and Auger-mediated Electron Trapping in CdTe Quantum-Dot Solids.

PubMed

Boehme, Simon C; Azpiroz, Jon Mikel; Aulin, Yaroslav V; Grozema, Ferdinand C; Vanmaekelbergh, Daniël; Siebbeles, Laurens D A; Infante, Ivan; Houtepen, Arjan J

2015-05-13

Charge trapping is an ubiquitous process in colloidal quantum-dot solids and a major limitation to the efficiency of quantum dot based devices such as solar cells, LEDs, and thermoelectrics. Although empirical approaches led to a reduction of trapping and thereby efficiency enhancements, the exact chemical nature of the trapping mechanism remains largely unidentified. In this study, we determine the density of trap states in CdTe quantum-dot solids both experimentally, using a combination of electrochemical control of the Fermi level with ultrafast transient absorption and time-resolved photoluminescence spectroscopy, and theoretically, via density functional theory calculations. We find a high density of very efficient electron traps centered ∼0.42 eV above the valence band. Electrochemical filling of these traps increases the electron lifetime and the photoluminescence quantum yield by more than an order of magnitude. The trapping rate constant for holes is an order of magnitude lower that for electrons. These observations can be explained by Auger-mediated electron trapping. From density functional theory calculations we infer that the traps are formed by dicoordinated Te atoms at the quantum dot surface. The combination of our unique experimental determination of the density of trap states with the theoretical modeling of the quantum dot surface allows us to identify the trapping mechanism and chemical reaction at play during charge trapping in these quantum dots.

Palladium modified porous silicon as multi-functional MALDI chip for serum peptide detection.

PubMed

Li, Xiao; Chen, Xiaoming; Tan, Jie; Liang, Xiao; Wu, Jianmin

2017-02-14

Interest in using mesoporous materials for peptidomic research has increased recently. The present study reports a new type of matrix assisted laser desorption/ionization (MALDI) plate derived from electrochemically etched porous silicon (PSi) whose surface was modified with palladium nanoparticles (PdNPs). Owing to the well-tailored pore size and the molecular filtration effect of the PSi, peptides in serum samples can be selectively captured and enriched in the pore channel, thereby eliminating the interference from large proteins in subsequent MALDI-MS detection. On the other hand, the PdNPs with localized surface plasmon resonance (LSPR) effect can help to enhance the efficiency of energy absorption in the UV region. Meanwhile, the charge separation effect between the PSi semiconductor and PdNPs also can be applied to promote the accumulation of positive charges on PdNPs, resulting in an improvement in laser desorption/ionization (LDI) efficiency under positive linear detection mode. The interplay among these unique properties of PSi and PdNPs can synergistically increase the overall sensitivity in serum peptide detection. Using this technology, serum sample can be directly detected on the PSi-PdNPs chip without complicated pretreatment process. Therefore, a high fidelity serum peptide fingerprint can be acquired in a high throughput way. With the assistance of statistical analysis, colorectal cancer patients and healthy people can be accurately distinguished based on the serum peptide fingerprints.

Inhibition of melanin synthesis pathway by tricyclazole increases susceptibility of Fonsecaea pedrosoi against mouse macrophages.

PubMed

Cunha, Marcel M L; Franzen, Anderson J; Alviano, Daniela S; Zanardi, Erica; Alviano, Celuta S; De Souza, Wanderley; Rozental, Sonia

2005-12-15

Fonsecaea pedrosoi produces melanin, a pigment related to virulence in pathogenic fungi. To understand the involvement of melanin in the protection of fungi, the authors used tricyclazole to inhibit the melanin pathway in F. pedrosoi. Experiments of pigmentation suggested that F. pedrosoi uniquely produces dihydroxynaphthalene-melanin. Pigments produced on cultures modified or not with tricyclazole were extracted by an alkali-acid method and submitted to infrared and ion exchange chromatography analysis; also cytochemistry analysis for cationized ferritin of whole cells was carried out. This group of experiments showed that the tricyclazole treatment on F. pedrosoi produced a melanin-like pigment, but less negatively charged and with less affinity for iron ions than that without the tricyclazole treatment, and this in turn lead to a less negatively charge cell wall surface. Scanning electron microscopy of such pigments showed that the melanin from control cultures maintained their hyphae-like structures, which have been described as "melanin-ghosts," whereas the tricyclazole pigment showed an amorphous surface. Interaction of conidia from cultures of F. pedrosoi, modified by tricyclazole or not, with peritoneal activated macrophages suggested that tricyclazole causes higher association of fungus with macrophages, weakens the fungus capacity to destroy the macrophages, and diminishes the resistance to dry fracture procedures on samples prepared for high resolution scanning electron microscopy. Copyright (c) 2005 Wiley-Liss, Inc.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Laskin, Julia; Johnson, Grant E.; Prabhakaran, Venkateshkumar

Immobilization of complex molecules and clusters on supports plays an important role in a variety of disciplines including materials science, catalysis and biochemistry. In particular, deposition of clusters on surfaces has attracted considerable attention due to their non-scalable, highly size-dependent properties. The ability to precisely control the composition and morphology of clusters and small nanoparticles on surfaces is crucial for the development of next generation materials with rationally tailored properties. Soft- and reactive landing of ions onto solid or liquid surfaces introduces unprecedented selectivity into surface modification by completely eliminating the effect of solvent and sample contamination on the qualitymore » of the film. The ability to select the mass-to-charge ratio of the precursor 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 makes soft-landing an attractive approach for surface modification. High-purity uniform thin films on surfaces generated using mass-selected ion deposition facilitate understanding of critical interfacial phenomena relevant to catalysis, energy generation and storage, and materials science. Our efforts have been directed toward understanding charge retention by soft-landed metal and metal-oxide cluster ions, which may affect both their structure and reactivity. Specifically, we have examined the effect of the surface on charge retention by both positively and negatively charged cluster ions. We found that the electronic properties of the surface play an important role in charge retention by cluster cations. Meanwhile, the electron binding energy is a key factor determining charge retention by cluster anions. These findings provide the scientific foundation for the rational design of interfaces for advanced catalysts and energy storage devices. Further optimization of electrode-electrolyte interfaces for applications in energy storage and electrocatalysis may be achieved by understanding and controlling the properties of soft-landed cluster ions.« less

Investigation of surface charge density on solid-liquid interfaces by modulating the electrical double layer.

PubMed

Moon, Jong Kyun; Song, Myung Won; Pak, Hyuk Kyu

2015-05-20

A solid surface in contact with water or aqueous solution usually carries specific electric charges. These surface charges attract counter ions from the liquid side. Since the geometry of opposite charge distribution parallel to the solid-liquid interface is similar to that of a capacitor, it is called an electrical double layer capacitor (EDLC). Therefore, there is an electrical potential difference across an EDLC in equilibrium. When a liquid bridge is formed between two conducting plates, the system behaves as two serially connected EDLCs. In this work, we propose a new method for investigating the surface charge density on solid-liquid interfaces. By mechanically modulating the electrical double layers and simultaneously applying a dc bias voltage across the plates, an ac electric current can be generated. By measuring the voltage drop across a load resistor as a function of bias voltage, we can study the surface charge density on solid-liquid interfaces. Our experimental results agree very well with the simple equivalent electrical circuit model proposed here. Furthermore, using this method, one can determine the polarity of the adsorbed state on the solid surface depending on the material used. We expect this method to aid in the study of electrical phenomena on solid-liquid interfaces.

Study of space charge layer in silver bromide microcrystals by means of ultraviolet photoelectron spectroscopy

NASA Astrophysics Data System (ADS)

Tani, Tadaaki; Inami, Yoshiyasu

2000-09-01

Ultraviolet photoelectron spectroscopy has been successfully used to measure the heights of the tops of the valence bands of the surfaces of AgBr layers on Ag substrates for the verification of the space charge layer model. According to this model, the positive space charge layer (composed of negative charges with excess negative kink sites on the surface and corresponding positive charges with interstitial silver ions in the interior) is formed in silver halides, causing the difference in the electronic energy levels between their surface and interior. The depression of the positive space charge layer of AgBr caused by such adsorbates as photographic stabilizers and antifoggants was estimated from the decrease in the ionic conductivity of cubic AgBr microcrystals by the adsorbates. It was confirmed by the decrease in the heights of the tops of the valence bands of the surfaces of AgBr layers caused by the adsorbates in the presence of thin gelatin membranes on their surfaces. This result provided the explanation for the fact that the adsorbates increased the number of the microcrystals which formed latent image centers on the surface and decreased the number of the microcrystals, which formed latent image centers in the interior.

Instrumentation and Methodology Development for Mars Mission

NASA Technical Reports Server (NTRS)

Chen, Yuan-Liang Albert

2002-01-01

The Mars environment comprises a dry, cold and low air pressure atmosphere with low gravity (0.38g) and high resistivity soil. The global dust storms that cover a large portion of Mars were observed often from Earth. This environment provides an idea condition for triboelectric charging. The extremely dry conditions on the Martian surface have raised concerns that electrostatic charge buildup will not be dissipated easily. If triboelectrically generated charge cannot be dissipated or avoided, then dust will accumulate on charged surfaces and electrostatic discharge may cause hazards for future exploration missions. The low surface temperature on Mars helps to prolong the charge decay on the dust particles and soil. To better understand the physics of Martian charged dust particles is essential to future Mars missions. We research and design two sensors, velocity/charge sensor and PZT momentum sensors, to detect the velocity distribution, charge distribution and mass distribution of Martian charged dust particles. These sensors are fabricated at NASA Kenney Space Center, Electromagnetic Physics Testbed. The sensors will be tested and calibrated for simulated Mars atmosphere condition with JSC MARS-1 Martian Regolith simulant in this NASA laboratory.

The role of electrostatic interactions in protease surface diffusion and the consequence for interfacial biocatalysis.

PubMed

Feller, Bob E; Kellis, James T; Cascão-Pereira, Luis G; Robertson, Channing R; Frank, Curtis W

2010-12-21

This study examines the influence of electrostatic interactions on enzyme surface diffusion and the contribution of diffusion to interfacial biocatalysis. Surface diffusion, adsorption, and reaction were investigated on an immobilized bovine serum albumin (BSA) multilayer substrate over a range of solution ionic strength values. Interfacial charge of the enzyme and substrate surface was maintained by performing the measurements at a fixed pH; therefore, electrostatic interactions were manipulated by changing the ionic strength. The interfacial processes were investigated using a combination of techniques: fluorescence recovery after photobleaching, surface plasmon resonance, and surface plasmon fluorescence spectroscopy. We used an enzyme charge ladder with a net charge ranging from -2 to +4 with respect to the parent to systematically probe the contribution of electrostatics in interfacial enzyme biocatalysis on a charged substrate. The correlation between reaction rate and adsorption was determined for each charge variant within the ladder, each of which displayed a maximum rate at an intermediate surface concentration. Both the maximum reaction rate and adsorption value at which this maximum rate occurs increased in magnitude for the more positive variants. In addition, the specific enzyme activity increased as the level of adsorption decreased, and for the lowest adsorption values, the specific enzyme activity was enhanced compared to the trend at higher surface concentrations. At a fixed level of adsorption, the specific enzyme activity increased with positive enzyme charge; however, this effect offers diminishing returns as the enzyme becomes more highly charged. We examined the effect of electrostatic interactions on surface diffusion. As the binding affinity was reduced by increasing the solution ionic strength, thus weakening electrostatic interaction, the rate of surface diffusion increased considerably. The enhancement in specific activity achieved at the lowest adsorption values is explained by the substantial rise in surface diffusion at high ionic strength due to decreased interactions with the surface. Overall, knowledge of the electrostatic interactions can be used to control surface parameters such as surface concentration and surface diffusion, which intimately correlate with surface biocatalysis. We propose that the maximum reaction rate results from a balance between adsorption and surface diffusion. The above finding suggests enzyme engineering and process design strategies for improving interfacial biocatalysis in industrial, pharmaceutical, and food applications.

Electromagnetic dipole moments of charged baryons with bent crystals at the LHC

NASA Astrophysics Data System (ADS)

Bagli, E.; Bandiera, L.; Cavoto, G.; Guidi, V.; Henry, L.; Marangotto, D.; Martinez Vidal, F.; Mazzolari, A.; Merli, A.; Neri, N.; Ruiz Vidal, J.

2017-12-01

We propose a unique program of measurements of electric and magnetic dipole moments of charm, beauty and strange charged baryons at the LHC, based on the phenomenon of spin precession of channeled particles in bent crystals. Studies of crystal channeling and spin precession of positively- and negatively-charged particles are presented, along with feasibility studies and expected sensitivities for the proposed experiment using a layout based on the LHCb detector.

Microcapsule Structure with a Tunable Textured Surface via the Assembly of Polyoxomolybdate Clusters: A Bioinspired Strategy and Enhanced Activities in Alkene Oxidation.

PubMed

Chilivery, Rakesh; Rana, Rohit Kumar

2017-01-25

A polyamine-mediated bioinspired strategy to assemble Keggin-type phosphomolybdic acid (PMA) clusters is demonstrated for the fabrication of microcapsule (MC) structures with unique surface textures. It involves supramolecular aggregation of polyamines with multivalent anions, which then allows the assembly of negatively charged PMA into MCs in an aqueous medium under ambient conditions. Resembling the role of polyamines in biosilicification of diatoms, the polyamine-anion interaction is shown to be the key for the assembly process. It not only provides structural stability but also facilitates an interesting transition from a smooth to a wrinkled surface alongside a change in the Keggin form to its lacunary form depending on the pH of the medium. Moreover, the presence of isolated PMA units in the hybrid structure enables them to be active in catalyzing the aerobic oxidation of alkenes under solvent-free conditions with better selectivity and reusability. Hence, the assembly approach represents an effective way for heterogenization of PMA-based materials and is expected to find considerable application in the wider hybrid-cluster field.

Silver nanoparticles as a key feature of a plasma polymer composite layer in mitigation of charge injection into polyethylene under dc stress

NASA Astrophysics Data System (ADS)

Milliere, L.; Maskasheva, K.; Laurent, C.; Despax, B.; Boudou, L.; Teyssedre, G.

2016-01-01

The aim of this work is to limit charge injection from a semi-conducting electrode into low density polyethylene (LDPE) under dc field by tailoring the polymer surface using a silver nanoparticles-containing layer. The layer is composed of a plane of silver nanoparticles embedded in a semi-insulating organosilicon matrix deposited on the polyethylene surface by a plasma process. Size, density and surface coverage of the nanoparticles are controlled through the plasma process. Space charge distribution in 300 μm thick LDPE samples is measured by the pulsed-electroacoustic technique following a short term (step-wise voltage increase up to 50 kV mm-1, 20 min in duration each, followed by a polarity inversion) and a longer term (up to 12 h under 40 kV mm-1) protocols for voltage application. A comparative study of space charge distribution between a reference polyethylene sample and the tailored samples is presented. It is shown that the barrier effect depends on the size distribution and the surface area covered by the nanoparticles: 15 nm (average size) silver nanoparticles with a high surface density but still not percolating form an efficient barrier layer that suppress charge injection. It is worthy to note that charge injection is detected for samples tailored with (i) percolating nanoparticles embedded in organosilicon layer; (ii) with organosilicon layer only, without nanoparticles and (iii) with smaller size silver particles (<10 nm) embedded in organosilicon layer. The amount of injected charges in the tailored samples increases gradually in the samples ranking given above. The mechanism of charge injection mitigation is discussed on the basis of complementary experiments carried out on the nanocomposite layer such as surface potential measurements. The ability of silver clusters to stabilize electrical charges close to the electrode thereby counterbalancing the applied field appears to be a key factor in explaining the charge injection mitigation effect.

The Thomas-Fermi model in the theory of systems of charged particles above the surface of liquid dielectrics

NASA Astrophysics Data System (ADS)

Lytvtnenko, D. M.; Slyusarenko, Yu. V.; Kirdin, A. I.

2012-10-01

A consistent theory of equilibrium states of same sign charges above the surface of liquid dielectric film located on solid substrate in the presence of external attracting constant electric field is proposed. The approach to the development of the theory is based on the Thomas-Fermi model generalized to the systems under consideration and on the variational principle. The using of self-consistent field model allows formulating a theory containing no adjustable constants. In the framework of the variational principle we obtain the self-consistency equations for the parameters describing the system: the distribution function of charges above the liquid dielectric surface, the electrostatic field potentials in all regions of the system and the surface profile of the liquid dielectric. The self-consistency equations are used to describe the phase transition associated with the formation of spatially periodic structures in the system of charges on liquid dielectric surface. Assuming the non-degeneracy of the gas of charges above the surface of liquid dielectric film the solutions of the self-consistency equations near the critical point are obtained. In the case of the symmetric phase we obtain the expressions for the potentials and electric fields in all regions of the studied system. The distribution of the charges above the surface of liquid dielectric film for the symmetric phase is derived. The system parameters of the phase transition to nonsymmetric phase - the states with a spatially periodic ordering are obtained. We derive the expression determining the period of two-dimensional lattice as a function of physical parameters of the problem - the temperature, the external attractive electric field, the number of electrons per unit of the flat surface area of the liquid dielectric, the density of the dielectric, its surface tension and permittivity, and the permittivity of the solid substrate. The possibility of generalizing the developed theory in the case of degenerate gas of like-charged particles above the liquid dielectric surface is discussed.

Surface functionalization of dopamine coated iron oxide nanoparticles for various surface functionalities

NASA Astrophysics Data System (ADS)

Sherwood, Jennifer; Xu, Yaolin; Lovas, Kira; Qin, Ying; Bao, Yuping

2017-04-01

We present effective conjugation of four small molecules (glutathione, cysteine, lysine, and Tris(hydroxymethyl)aminomethane) onto dopamine-coated iron oxide nanoparticles. Conjugation of these molecules could improve the surface functionality of nanoparticles for more neutral surface charge at physiological pH and potentially reduce non-specific adsorption of proteins to nanoparticles surfaces. The success of conjugation was evaluated with dynamic light scattering by measuring the surface charge changes and Fourier transform infrared spectroscopy for surface chemistry analysis. The stability of dopamine-coated nanoparticles and the ability of conjugated nanoparticles to reduce the formation of protein corona were evaluated by measuring the size and charge of the nanoparticles in biological medium. This facile conjugation method opens up possibilities for attaching various surface functionalities onto iron oxide nanoparticle surfaces for biomedical applications.

Enhanced flashover strength in polyethylene nanodielectrics by secondary electron emission modification

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Weiwang; Li, Shengtao, E-mail: sli@xjtu.edu.cn; Min, Daomin

2016-04-15

This work studies the correlation between secondary electron emission (SEE) characteristics and impulse surface flashover in polyethylene nanodielectrics both theoretically and experimentally, and illustrates the enhancement of flashover voltage in low-density polyethylene (LDPE) through incorporating Al{sub 2}O{sub 3} nanoparticles. SEE characteristics play key roles in surface charging and gas desorption during surface flashover. This work demonstrates that the presence of Al{sub 2}O{sub 3} nanoparticles decreases the SEE coefficient of LDPE and enhances the impact energy at the equilibrium state of surface charging. These changes can be explained by the increase of surface roughness and of surface ionization energy, and themore » strong interaction between nanoparticles and the polymer dielectric matrix. The surface charge and flashover voltage are calculated according to the secondary electron emission avalanche (SEEA) model, which reveals that the positive surface charges are reduced near the cathode triple point, while the presence of more nanoparticles in high loading samples enhances the gas desorption. Consequently, the surface flashover performance of LDPE/Al{sub 2}O{sub 3} nanodielectrics is improved.« less

CdS/TiO2 photoanodes via solution ion transfer method for highly efficient solar hydrogen generation

NASA Astrophysics Data System (ADS)

Krishna Karuturi, Siva; Yew, Rowena; Reddy Narangari, Parvathala; Wong-Leung, Jennifer; Li, Li; Vora, Kaushal; Tan, Hark Hoe; Jagadish, Chennupati

2018-03-01

Cadmium sulfide (CdS) is a unique semiconducting material for solar hydrogen generation applications with a tunable, narrow bandgap that straddles water redox potentials. However, its potential towards efficient solar hydrogen generation has not yet been realized due to low photon-to-current conversions, high charge carrier recombination and the lack of controlled preparation methods. In this work, we demonstrate a highly efficient CdS/TiO2 heterostructured photoelectrode using atomic layer deposition and solution ion transfer reactions. Enabled by the well-controlled deposition of CdS nanocrystals on TiO2 inverse opal (TiIO) nanostructures using the proposed method, a saturation photocurrent density of 9.1 mA cm-2 is realized which is the highest ever reported for CdS-based photoelectrodes. We further demonstrate that the passivation of a CdS surface with an ultrathin amorphous layer (˜1.5 nm) of TiO2 improves the charge collection efficiency at low applied potentials paving the way for unassisted solar hydrogen generation.

Graphene/Sulfur/Carbon Nanocomposite for High Performance Lithium-Sulfur Batteries

PubMed Central

Jin, Kangke; Zhou, Xufeng; Liu, Zhaoping

2015-01-01

Here, we report a two-step synthesis of graphene/sulfur/carbon ternary composite with a multilayer structure. In this composite, ultrathin S layers are uniformly deposited on graphene nanosheets and covered by a thin layer of amorphous carbon derived from β-cyclodextrin on the surface. Such a unique microstructure, not only improves the electrical conductivity of sulfur, but also effectively inhibits the dissolution of polysulfides during charging/discharging processes. As a result, this ternary nanocomposite exhibits excellent electrochemical performance. It can deliver a high initial discharge and charge capacity of 1410 mAh·g−1 and 1370 mAh·g−1, respectively, and a capacity retention of 63.8% can be achieved after 100 cycles at 0.1 C (1 C = 1675 mA·g−1). A relatively high specific capacity of 450 mAh·g−1 can still be retained after 200 cycles at a high rate of 2 C. The synthesis process introduced here is simple and broadly applicable to the modification of sulfur cathode for better electrochemical performance. PMID:28347077

In situ electrochemical-electron spin resonance investigations of multi-electron redox reaction for organic radical cathodes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Huang, Qian; Walter, Eric D.; Cosimbescu, Lelia

2016-02-29

Organic radical batteries (ORBs) bearing robust radical polymers as energy storage species, are emerging promisingly with durable high energy and power characteristics by unique tunable redox properties. Here we report the development and application of in situ electrochemical-electron spin resonance (ESR) methodologies to identify the charge transfer mechanism of Poly(2,2,6,6- tetramethylpiperidinyloxy-4-yl methacrylate) (PTMA) based organic radical composite cathodes in the charge-discharge process of lithium half cells. The in situ experiments allow each electrochemical state to be associated with the chemical state (or environment) of the radical species upon the cell cycling. In situ ESR spectra of the composite cathode demonstratemore » a two-electron redox reaction of PTMA. Moreover, two different local environments of radical species are found in the composite electrode that includes both concentrated and isolated radicals. These two types of radicals show similarities during the redox reaction process while behave quite differently in the non-faradic reaction of ion sorption/desorption on the electrode surface.« less

In situ measurement of surface potential developed on MgO thin film surface under ion irradiation using ion scattering spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nagatomi, T.; Kuwayama, T.; Takai, Y.

2009-11-15

The application of ion scattering spectroscopy (ISS) to the in situ measurement of the surface potential developed on an insulator surface under positive ion irradiation was investigated. The ISS spectra measured for a MgO film of 600 nm thickness on a Si substrate by the irradiation of 950 eV He{sup +} ions revealed that the surface is positively charged by approximately 180 V. For accurate measurement of the surface potential, a correction to take into account the angular deflection of primary ions induced by the high surface potential is required. The dependence of the surface potential on the sample temperaturemore » revealed that no charging is induced above 700 deg. C, indicating that accumulated charges can be removed by heating to 700 deg. C. From the measurement of the ion-induced secondary electron yield using a collector electrode located in front of the sample surface, the surface potential and ion-induced secondary electron yield were found to be strongly affected by the experimental setup. Secondary electrons produced by the impact of slow positive secondary ions, the maximum energy of which corresponds to the surface potential, play an important role when the bias voltage applied to the collector electrode is positively high for the present experimental setup. The surface potential developed on the surface of MgO films of 600 and 200 nm thickness was measured in situ, revealing that the amount of accumulated charges and the time required to attain the steady state of charging are slightly dependent on the beam current of primary ions and strongly dependent on the thickness of the MgO film. The present results confirmed that the application of ISS has high potential for investigating charging phenomena and the secondary electron emission from insulator surfaces under positive ion irradiation.« less

Ferrocene Containing Copolymers with Improved Electrostatic Dissipation Properties for Advanced Applications

NASA Technical Reports Server (NTRS)

Smith, T. M.; Nelson, G. L.

2005-01-01

Electrostatic dissipative polymers are used for a variety of functions. Typical methods utilized to transform electrically insulating polymers into either charge dissipative or conductive materials involve incorporating a conductive filler, conductive polymer, oxidizing the surface using plasma, or incorporating surfactants that act as surface wetting agents. Another approach is to synthesize a block copolymer that is expected to result in better electrical properties with minimal impacts to physical, fire, and thermal properties. One such block that can be added into the main chain of polymers is a diol terminated ferrocene oligomer, which is expected to impart electrostatic dissipative properties into the host polymer while concurrently improving the overall fire properties. Previous work with polyurethanes incorporating a ferrocene oligomer into the main chain resulted in much improved fire retardancy. In dealing with electrostatic dissipative materials the important questions are: how easily does the material charge and how quickly can the charge move to ground. One normally describes the materials conductivity, but conductivity only measures the fastest path for an electron not the slowest path. The slowest path is the one of interest, since it is left on the surface and thus can cause discharges. In order to assess ease of charging and decay times corona charge dissipation measurements can accurately assess these properties by introducing a charge on the surface of the material then measuring the surface voltage and the amount of charge deposited. The charge decay curve then will give an indication of a materials electrostatic dissipation properties. Normally, triboelectric testing can be performed, but results vary. Corona charge dissipation results are more repeatable.

Self-consistent simulation of radio frequency multipactor on micro-grooved dielectric surface

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cai, Libing; Wang, Jianguo, E-mail: wanguiuc@mail.xjtu.edu.cn; Northwest Institute of Nuclear Technology, Xi'an, Shaanxi 710024

2015-02-07

The multipactor plays a key role in the surface breakdown on the feed dielectric window irradiated by high power microwave. To study the suppression of multipactor, a 2D electrostatic PIC-MCC simulation code was developed. The space charge field, including surface deposited charge and multipactor electron charge field, is obtained by solving 2D Poisson's equation in time. Therefore, the simulation is self-consistent and does not require presetting a fixed space charge field. By using this code, the self-consistent simulation of the RF multipactor on the periodic micro-grooved dielectric surface is realized. The 2D space distributions of the multipactor electrons and spacemore » charge field are presented. From the simulation results, it can be found that only half slopes have multipactor discharge when the slope angle exceeds a certain value, and the groove presents a pronounced suppression effect on the multipactor.« less

Hydrolysis-controlled protein adsorption and antifouling behaviors of mixed charged self-assembled monolayer: A molecular simulation study.

PubMed

Liu, Jie; Zhou, Jian

2016-08-01

Understanding the mechanism of the antimicrobial and antifouling properties of mixed charged materials is of great significance. The interactions between human gamma fibrinogen (γFg) and mixed carboxylic methyl ether-terminated (COOCH3-) and trimethylamino-terminated (N(CH3)3(+)-) SAMs and the influence of hydrolysis were studied by molecular simulations. After hydrolysis, the mixed SAMs exhibit behaviors from antimicrobial to antifouling, since the COOCH3-thiols were translated into carboxylic acid (COO(-)-) terminated thiols, which carried a net charge of -1 e. Simulation results showed that the main differences between COOCH3-/N(CH3)3(+)-SAM and COO(-)-/N(CH3)3(+)-SAM are the charged property and the hydration layer above the surface. γFg could stably adsorb on the positively-charged COOCH3-/N(CH3)3(+)-SAM. The adsorption behavior is mainly induced by the strong electrostatic attraction. There is a single hydration layer bound to the surface, which is related to the N(CH3)3(+) groups. The van der Waals repulsion between γFg and the single hydration layer are not strong enough to compensate the strong electrostatic attraction. After hydrolysis, the positively-charged SAM was transferred to a neutral mixed charged surface, the electrostatic attraction between γFg and the surface disappears. Meanwhile, the SAM surface is covered by double hydration layers, which is induced by the N(CH3)3(+) and COO(-) groups; water molecules around COO(-) groups are obviously denser than that around N(CH3)3(+) groups. With the combined contribution from double hydration layers and the vanishment of electrostatic attraction, γFg is forced to desorb from the surface. After hydrolysis, the internal structure of mixed SAM appears more ordered due to the electrostatic interactions between charged groups on the top of SAMs. The antimicrobial and antifouling materials are of great importance in many biological applications. The strong hydration property of surfaces and the interactions between proteins and surfaces play a key role in resisting protein adsorption. The mixed SAMs, constructed from a 1:1 combination of COOCH3- and N(CH3)3(+)-terminated thiols, can induce protein adsorption mainly through the electrostatic interaction. When the COOCH3-terminated thiols were hydrolyzed to negatively charged COO(-)-terminated thiols, the mixed-charged SAMs switched from antimicrobial to antifouling. Due to the strong hydration property of the mixed charged SAMs, the adsorbed γFg moved away from the surface. Understanding the interactions between protein and mixed-charged SAMs in the atomistic level is important for the practical design and development of new antimicrobial and antifouling materials. Copyright © 2016 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

NASCAP modelling computations on large optics spacecraft in geosynchronous substorm environments

NASA Technical Reports Server (NTRS)

Stevens, N. J.; Purvis, C. K.

1980-01-01

Satellites in geosynchronous orbits have been found to be charged to significant negative voltages during encounters with geomagnetic substorms. When satellite surfaces are charged, there is a probability of enhanced contamination from charged particles attracted back to the satellite by electrostatic forces. This could be particularly disturbing to large satellites using sensitive optical systems. In this study the NASA Charging Analyzer Program (NASCAP) is used to evaluate qualitatively the possibility of such enhanced contamination on a conceptual version of a large satellite. The evaluation is made by computing surface voltages on the satellite due to encounters with substorm environments and then computing charged-particle trajectories in the electric fields around the satellite. Particular attention is paid to the possibility of contaminants reaching a mirror surface inside a dielectric tube because this mirror represents a shielded optical surface in the satellite model used. Deposition of low energy charged particles from other parts of the spacecraft onto the mirror was found to be possible in the assumed moderate substorm environment condition. In the assumed severe substorm environment condition, however, voltage build up on the inside and edges of the dielectric tube in which the mirror is located prevents contaminants from reaching the mirror surface.

Extremely large nonsaturating magnetoresistance and ultrahigh mobility due to topological surface states in the metallic Bi2Te3 topological insulator

NASA Astrophysics Data System (ADS)

Shrestha, K.; Chou, M.; Graf, D.; Yang, H. D.; Lorenz, B.; Chu, C. W.

2017-05-01

Weak antilocalization (WAL) effects in Bi2Te3 single crystals have been investigated at high and low bulk charge-carrier concentrations. At low charge-carrier density the WAL curves scale with the normal component of the magnetic field, demonstrating the dominance of topological surface states in magnetoconductivity. At high charge-carrier density the WAL curves scale with neither the applied field nor its normal component, implying a mixture of bulk and surface conduction. WAL due to topological surface states shows no dependence on the nature (electrons or holes) of the bulk charge carriers. The observations of an extremely large nonsaturating magnetoresistance and ultrahigh mobility in the samples with lower carrier density further support the presence of surface states. The physical parameters characterizing the WAL effects are calculated using the Hikami-Larkin-Nagaoka formula. At high charge-carrier concentrations, there is a greater number of conduction channels and a decrease in the phase coherence length compared to low charge-carrier concentrations. The extremely large magnetoresistance and high mobility of topological insulators have great technological value and can be exploited in magnetoelectric sensors and memory devices.

Dangerous liaisons: anion-induced protonation in phosphate-polyamine interactions and their implications for the charge states of biologically relevant surfaces.

PubMed

Laucirica, Gregorio; Marmisollé, Waldemar A; Azzaroni, Omar

2017-03-22

Although not always considered a preponderant interaction, amine-phosphate interactions are omnipresent in multiple chemical and biological systems. This study aims to answer questions that are still pending about their nature and consequences. We focus on the description of the charge state as surface charges constitute directing agents of the interaction of amine groups with either natural or synthetic counterparts. Our results allow us to quantitatively determine the relative affinities of HPO 4 2- and H 2 PO 4 - from the analysis of the influence of phosphates on the zeta-potential of amino-functionalized surfaces in a broad pH range. We show that phosphate anions enhance the protonation of amino groups and, conversely, charged amines induce further proton dissociation of phosphates, yielding a complex dependence of the surface effective charge on the pH and phosphate concentration. We also demonstrate that phosphate-amine interaction is specific and the modulation of surface charge occurs in the physiological phosphate concentration range, emphasizing its biochemical and biotechnological relevance and the importance of considering this veiled association in both in vivo and in vitro studies.

Ligand-induced dependence of charge transfer in nanotube–quantum dot heterostructures

DOE PAGES

Wang, Lei; Han, Jinkyu; Sundahl, Bryan; ...

2016-07-01

As a model system to probe ligand-dependent charge transfer in complex composite heterostructures, we fabricated double-walled carbon nanotube (DWNT) – CdSe quantum dot (QD) composites. Whereas the average diameter of the QDs probed was kept fixed at ~4.1 nm and the nanotubes analyzed were similarly oxidatively processed, by contrast, the ligands used to mediate the covalent attachment between the QDs and DWNTs were systematically varied to include p-phenylenediamine (PPD), 2-aminoethanethiol (AET), and 4-aminothiophenol (ATP). Herein, we have put forth a unique compilation of complementary data from experiment and theory, including results from transmission electron microscopy (TEM), near-edge X-ray absorption finemore » structure (NEXAFS) spectroscopy, Raman spectroscopy, electrical transport measurements, and theoretical modeling studies, in order to fundamentally assess the nature of the charge transfer between CdSe QDs and DWNTs, as a function of the structure of various, intervening bridging ligand molecules. Specifically, we correlated evidence of charge transfer as manifested by changes and shifts associated with NEXAFS intensities, Raman peak positions, and threshold voltages both before and after CdSe QD deposition onto the underlying DWNT surface. Importantly, for the first time ever in these types of nanoscale composite systems, we have sought to use theoretical modeling to justify and account for our experimental results. Finally, our overall data suggest that (i) QD coverage density on the DWNTs varies, based upon the different ligand pendant groups used and that (ii) the presence of a π-conjugated carbon framework within the ligands themselves and the electron affinity of the pendant groups collectively play important roles in the resulting charge transfer from QDs to the underlying CNTs.« less

Mechanical Removal and Rescreening of Local Screening Charges on Ferroelectric Surfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tong, Sheng; Park, Woon Ik; Choi, YoonYoung

2015-01-20

We report the kinetics of screening charge removal and rescreening on periodically poled lithium niobate using charge-gradient microscopy and electrostatic force microscopy (EFM). A minimum pressure needs to be applied to initiate mechanical screening charge removal, and increasing the pressure leads to further removal of charge until a threshold is reached when all screening charges are removed. We fit all rescreening EFM contrast curves under various pressures into a universal exponential decay. The findings imply that we can control the screening degree of ferroelectric surfaces by mechanical means without affecting the polarization underneath.

Mechanical Removal and Rescreening of Local Screening Charges at Ferroelectric Surfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tong, Sheng; Park, Woon Ik; Choi, Yoon-Young

2015-01-20

In this paper, we report the kinetics of screening charge removal and rescreening on periodically poled lithium niobate using charge-gradient microscopy and electrostatic force microscopy (EFM). A minimum pressure needs to be applied to initiate mechanical screening charge removal, and increasing the pressure leads to further removal of charge until a threshold is reached when all screening charges are removed. We fit all rescreening EFM contrast curves under various pressures into a universal exponential decay. Finally, the findings imply that we can control the screening degree of ferroelectric surfaces by mechanical means without affecting the polarization underneath.

Field observations of the electrostatic charges of blowing snow in Hokkaido, Japan

NASA Astrophysics Data System (ADS)

Omiya, S.; Sato, A.

2011-12-01

An electrostatic charge of blowing snow may be a contributing factor in the formation of a snow drift and a snow cornice, and changing of the trajectory of own motion. However, detailed electrification characteristics of blowing snow are not known as there are few reports of charge measurements. We carried out field observations of the electrostatic charges of blowing snow in Tobetsu, Hokkaido, Japan in the mid winter of 2011. An anemovane and a thermohygrometer were used for the meteorological observation. Charge-to-mass ratios of blowing snow were obtained by a Faraday-cage, an electrometer and an electric balance. In this observation period, the air temperature during the blowing snow event was -6.5 to -0.5 degree Celsius. The measured charges in this observation were consistent with the previous studies in sign, which is negative, but they were smaller than the previous one. In most cases, the measured values increased with the temperature decrease, which corresponds with previous studies. However, some results contradicted the tendency, and the maximum value was obtained on the day of the highest air temperature of -0.5 degree Celsius. This discrepancy may be explained from the difference of the snow surface condition on observation day. The day when the maximum value was obtained, the snow surface was covered with old snow, and hard. On the other hand, in many other cases, the snow surface was covered with the fresh snow, and soft. Blowing snow particles on the hard surface can travel longer distance than on the soft one. Therefore, it can be surmised that the hard surface makes the blowing snow particles accumulate a lot of negative charges due to a large number of collisions to the surface. This can be supported by the results of the wind tunnel experiments by Omiya and Sato (2011). By this field observation, it was newly suggested that the electrostatic charge of blowing snow are influenced greatly by the difference of the snow surface condition. REFERENCE: Omiya and Sato,(2010):An electrostatic charge measurement of blowing snow particles focusing on collision frequency to the snow surface. AGU Abstract Database, 2010 Fall Meeting.

Influence of Protamine Functionalization on the Colloidal Stability of 1D and 2D Titanium Oxide Nanostructures.

PubMed

Rouster, Paul; Pavlovic, Marko; Horváth, Endre; Forró, László; Dey, Sandwip K; Szilagyi, Istvan

2017-09-26

The colloidal stability of titanium oxide nanosheets (TNS) and nanowires (TiONW) was studied in the presence of protamine (natural polyelectrolyte) in aqueous dispersions, where the nanostructures possessed negative net charge, and the protamine was positively charged. Regardless of their shape, similar charging and aggregation behaviors were observed for both TNS and TiONW. Electrophoretic experiments performed at different protamine loadings revealed that the adsorption of protamine led to charge neutralization and charge inversion depending on the polyelectrolyte dose applied. Light scattering measurements indicated unstable dispersions once the surface charge was close to zero or slow aggregation below and above the charge neutralization point with negatively or positively charged nanostructures, respectively. These stability regimes were confirmed by the electron microscopy images taken at different polyelectrolyte loadings. The protamine dose and salt-dependent colloidal stability confirmed the presence of DLVO-type interparticle forces, and no experimental evidence was found for additional interactions (e.g., patch-charge, hydrophobic, or steric forces), which are usually present in similar polyelectrolyte-particle systems. These findings indicate that the polyelectrolyte adsorbs on the TNS and TiONW surfaces in a flat and extended conformation giving rise to the absence of surface heterogeneities. Therefore, protamine is an excellent biocompatible candidate to form smooth surfaces, for instance in multilayers composed of polyelectrolytes and particles to be used in biomedical applications.

Recovery curves of the surface electric field after lightning discharges occurring between the positive charge pocket and negative charge centre in a thundercloud

NASA Astrophysics Data System (ADS)

Pawar, S. D.; Kamra, A. K.

2002-12-01

Surface observations of the electric field recovery curves of the lightning discharges occurring between the positive charge pocket and negative main charge centre in an overhead thundercloud are reported. Such recovery curves are observed to have an additional step of very slow field-change observed at an after-discharge value of electric field equal to 5-6 kV m-1. The behavior of recovery curves is explained in terms of the coronae charge and the relative efficiencies of the charge generating processes responsible for growth of positive charge pocket and main negative charge centre in the thundercloud. The charging currents responsible for the growth of charge in positive charge pockets is computed to be 2-4 times larger than that for the growth of the main negative charge. However, the charge destroyed in such a discharge is found to be comparable to that in a discharge between the main charge centres of the thundercloud.

A Closer Look at Solar Wind Sputtering of Lunar Surface Materials

NASA Technical Reports Server (NTRS)

Barghouty, A. F.; Adams, J. H., Jr.; Meyer, F.; Mansur, L.; Reinhold, C.

2008-01-01

Solar-wind induced potential sputtering of the lunar surface may be a more efficient erosive mechanism than the "standard" kinetic (or physical) sputtering. This is partly based on new but limited laboratory measurements which show marked enhancements in the sputter yields of slow-moving, highly-charged ions impacting oxides. The enhancements seen in the laboratory can be orders of magnitude for some surfaces and highly charged incident ions, but seem to depend very sensitively on the properties of the impacted surface in addition to the fluence, energy and charge of the impacting ion. For oxides, potential sputtering yields are markedly enhanced and sputtered species, especially hydrogen and light ions, show marked dependence on both charge and dose.

Time and voltage dependences of nanoscale dielectric constant modulation on indium tin oxide films

NASA Astrophysics Data System (ADS)

Li, Liang; Hao, Haoyue; Zhao, Hua

2017-01-01

The modulation of indium tin oxide (ITO) films through surface charge accumulation plays an important role in many different applications. In order to elaborately study the modulation, we measured the dielectric constant of the modulated layer through examining the excitation of surface plasmon polaritons. Charges were pumped on the surfaces of ITO films through applying high voltage in appropriate directions. Experiments unveiled that the dielectric constant of the modulated layer had large variation along with the nanoscale charge accumulation. Corresponding numerical results were worked out through combining Drude model and Mayadas-Shatzkes model. Based on the above results, we deduced the time and voltage dependences of accumulated charge density, which revealed a long-time charge accumulation process.

Photocurrent generation in SnO2 thin film by surface charged chemisorption O ions

NASA Astrophysics Data System (ADS)

Lee, Po-Ming; Liao, Ching-Han; Lin, Chia-Hua; Liu, Cheng-Yi

2018-06-01

We report a photocurrent generation mechanism in the SnO2 thin film surface layer by the charged chemisorption O ions on the SnO2 thin film surface induced by O2-annealing. A critical build-in electric field in the SnO2 surface layer resulted from the charged O ions on SnO2 surface prolongs the lifetime and reduces the recombination probability of the photo-excited electron-hole pairs by UV-laser irradiation (266 nm) in the SnO2 surface layer, which is the key for the photocurrent generation in the SnO2 thin film surface layer. The critical lifetime of prolonged photo-excited electron-hole pair is calculated to be 8.3 ms.

Activating the molecular spinterface

NASA Astrophysics Data System (ADS)

Cinchetti, Mirko; Dediu, V. Alek; Hueso, Luis E.

2017-05-01

The miniaturization trend in the semiconductor industry has led to the understanding that interfacial properties are crucial for device behaviour. Spintronics has not been alien to this trend, and phenomena such as preferential spin tunnelling, the spin-to-charge conversion due to the Rashba-Edelstein effect and the spin-momentum locking at the surface of topological insulators have arisen mainly from emergent interfacial properties, rather than the bulk of the constituent materials. In this Perspective we explore inorganic/molecular interfaces by looking closely at both sides of the interface. We describe recent developments and discuss the interface as an ideal platform for creating new spin effects. Finally, we outline possible technologies that can be generated thanks to the unique active tunability of molecular spinterfaces.

Ionic solutions of two-dimensional materials

NASA Astrophysics Data System (ADS)

Cullen, Patrick L.; Cox, Kathleen M.; Bin Subhan, Mohammed K.; Picco, Loren; Payton, Oliver D.; Buckley, David J.; Miller, Thomas S.; Hodge, Stephen A.; Skipper, Neal T.; Tileli, Vasiliki; Howard, Christopher A.

2017-03-01

Strategies for forming liquid dispersions of nanomaterials typically focus on retarding reaggregation, for example via surface modification, as opposed to promoting the thermodynamically driven dissolution common for molecule-sized species. Here we demonstrate the true dissolution of a wide range of important 2D nanomaterials by forming layered material salts that spontaneously dissolve in polar solvents yielding ionic solutions. The benign dissolution advantageously maintains the morphology of the starting material, is stable against reaggregation and can achieve solutions containing exclusively individualized monolayers. Importantly, the charge on the anionic nanosheet solutes is reversible, enables targeted deposition over large areas via electroplating and can initiate novel self-assembly upon drying. Our findings thus reveal a unique solution-like behaviour for 2D materials that enables their scalable production and controlled manipulation.

Recent advancements in plasmon-enhanced promising third-generation solar cells

NASA Astrophysics Data System (ADS)

Thrithamarassery Gangadharan, Deepak; Xu, Zhenhe; Liu, Yanlong; Izquierdo, Ricardo; Ma, Dongling

2017-01-01

The unique optical properties possessed by plasmonic noble metal nanostructures in consequence of localized surface plasmon resonance (LSPR) are useful in diverse applications like photovoltaics, sensing, non-linear optics, hydrogen generation, and photocatalytic pollutant degradation. The incorporation of plasmonic metal nanostructures into solar cells provides enhancement in light absorption and scattering cross-section (via LSPR), tunability of light absorption profile especially in the visible region of the solar spectrum, and more efficient charge carrier separation, hence maximizing the photovoltaic efficiency. This review discusses about the recent development of different plasmonic metal nanostructures, mainly based on Au or Ag, and their applications in promising third-generation solar cells such as dye-sensitized solar cells, quantum dot-based solar cells, and perovskite solar cells.

MULTIPLE SPARK GAP SWITCH

DOEpatents

Schofield, A.E.

1958-07-22

A multiple spark gap switch of unique construction is described which will permit controlled, simultaneous discharge of several capacitors into a load. The switch construction includes a disc electrode with a plurality of protuberances of generally convex shape on one surface. A firing electrode is insulatingly supponted In each of the electrode protuberances and extends substantially to the apex thereof. Individual electrodes are disposed on an insulating plate parallel with the disc electrode to form a number of spark gaps with the protuberances. These electrodes are each connected to a separate charged capacitor and when a voltage ls applied simultaneously between the trigger electrodes and the dlsc electrode, each spark gap fires to connect its capacitor to the disc electrode and a subsequent load.

Hydration of excess electrons trapped in charge pockets on molecular surfaces

NASA Astrophysics Data System (ADS)

Jalbout, Abraham F.; Del Castillo, R.; Adamowicz, Ludwik

2007-01-01

In this work we strive to design a novel electron trap located on a molecular surface. The process of electron trapping involves hydration of the trapped electron. Previous calculations on surface electron trapping revealed that clusters of OH groups can form stable hydrogen-bonded networks on one side of a hydrocarbon surface (i.e. cyclohexane sheets), while the hydrogen atoms on the opposite side of the surface form pockets of positive charge that can attract extra negative charge. The excess electron density on such surfaces can be further stabilized by interactions with water molecules. Our calculations show that these anionic systems are stable with respect to vertical electron detachment (VDE).

Design of asymmetric particles containing a charged interior and a neutral surface charge: comparative study on in vivo circulation of polyelectrolyte microgels.

PubMed

Chen, Kai; Xu, Jing; Luft, J Christopher; Tian, Shaomin; Raval, Jay S; DeSimone, Joseph M

2014-07-16

Lowering the modulus of hydrogel particles could enable them to bypass in vivo physical barriers that would otherwise filter particles with similar size but higher modulus. Incorporation of electrolyte moieties into the polymer network of hydrogel particles to increase the swelling ratio is a straightforward and quite efficient way to decrease the modulus. In addition, charged groups in hydrogel particles can also help secure cargoes. However, the distribution of charged groups on the surface of a particle can accelerate the clearance of particles. Herein, we developed a method to synthesize highly swollen microgels of precise size with near-neutral surface charge while retaining interior charged groups. A strategy was employed to enable a particle to be highly cross-linked with very small mesh size, and subsequently PEGylated to quench the exterior amines only without affecting the internal amines. Acidic degradation of the cross-linker allows for swelling of the particles to microgels with a desired size and deformability. The microgels fabricated demonstrated extended circulation in vivo compared to their counterparts with a charged surface, and could potentially be utilized in in vivo applications including as oxygen carriers or nucleic acid scavengers.

Work Function of Oxide Ultrathin Films on the Ag(100) Surface.

PubMed

Sementa, Luca; Barcaro, Giovanni; Negreiros, Fabio R; Thomas, Iorwerth O; Netzer, Falko P; Ferrari, Anna Maria; Fortunelli, Alessandro

2012-02-14

Theoretical calculations of the work function of monolayer (ML) and bilayer (BL) oxide films on the Ag(100) surface are reported and analyzed as a function of the nature of the oxide for first-row transition metals. The contributions due to charge compression, charge transfer and rumpling are singled out. It is found that the presence of empty d-orbitals in the oxide metal can entail a charge flow from the Ag(100) surface to the oxide film which counteracts the decrease in the work function due to charge compression. This flow can also depend on the thickness of the film and be reduced in passing from ML to BL systems. A regular trend is observed along first-row transition metals, exhibiting a maximum for CuO, in which the charge flow to the oxide is so strong as to reverse the direction of rumpling. A simple protocol to estimate separately the contribution due to charge compression is discussed, and the difference between the work function of the bare metal surface and a Pauling-like electronegativity of the free oxide slabs is used as a descriptor quantity to predict the direction of charge transfer.

Effect of Ca2+ ion concentration on adsorption of poly(carboxylate ether)-based (PCE) superplasticizer on mica.

PubMed

Wu, Bo; Chun, Byong-Wa; Gu, Le; Kuhl, Tonya L

2018-05-09

Poly(carboxylate ether)-based (PCE) superplasticizers consist of a carboxylic acid backbone and grafted poly(ethylene glycol) (PEG) side chains. Ca 2+ ion bridging mechanism is commonly purported to control PCE's adsorption on negatively charged cement particle surfaces in cement suspension, thus PCE was expected to adsorb on negatively charged surfaces in synthetic pore solutions via Ca 2+ /COO - interactions. Adsorption behaviors of a commercial PCE on negatively charged mica were studied in aqueous electrolyte solutions by a surface forces apparatus. Direct force measurements indicated that the PCE adsorbed onto mica from 0.1 M K 2 SO 4 due to K + ion chelation by the ether oxygen units CH 2 CH 2 O on the PEG chains, but surprisingly did not adsorb from either 0.1 M K 2 SO 4 with saturated Ca(OH) 2 or 0.1 M Ca(NO 3 ) 2 . The adsorption in K 2 SO 4 was weak, enabling the adsorbed PCE layers to be squeezed out under modest compression. Upon separating the surfaces, the PCE immediately achieved an identical re-adsorption. In high-calcium conditions, the PCE was highly positively charged due to Ca 2+ ion chelation by PEG chains and backbone carboxylic groups COO - , and mica also underwent charge reversal due to electrostatic adsorption/binding of Ca 2+ ions. Consequently, the interaction between mica and PCE was electrostatically repulsive and no PCE adsorption occurred. These findings can be explained by the complex interplay of ion chelation by PEG chains, electrostatic binding and screening interactions with charged surfaces in the presence of monovalent and divalent counterions, and ultimately charge reversal of both the charged surfaces and polyelectrolyte in high divalent ion conditions. Copyright © 2018 Elsevier Inc. All rights reserved.

Nanoscale charge transfer and diffusion at the MoS2/SiO2 interface by atomic force microscopy: contact injection versus triboelectrification.

PubMed

Xu, Rui; Ye, Shili; Xu, Kunqi; Lei, Le; Hussain, Sabir; Zheng, Zhiyue; Pang, Fei; Xing, Shuya; Liu, Xinmeng; Ji, Wei; Cheng, Zhihai

2018-08-31

Understanding the process of charge generation, transfer, and diffusion between two-dimensional (2D) materials and their supporting substrates is very important for potential applications of 2D materials. Compared with the systematic studies of triboelectric charging in a bulk sample, a fundamental understanding of the triboelectrification of the 2D material/insulator system is rather limited. Here, the charge transfer and diffusion of both the SiO 2 surface and MoS 2 /SiO 2 interface through contact electrification and frictional electrification are investigated systematically in situ by scanning Kelvin probe microscopy and dual-harmonic electrostatic force microscopy. Different from the simple static charge transfer between SiO 2 and the PtSi alloy atomic force microscope (AFM) tip, the charge transfer between the tip and the MoS 2 /SiO 2 system is complicated. Triboelectric charges, generated by contact or frictional electrification with the AFM tip, are trapped at the MoS 2 /SiO 2 interface and act as floating gates. The local charge discharge processes can be obtained by monitoring the surface potential. The charge decay time (τ) of the MoS 2 /SiO 2 interface is one (or two) orders of magnitude larger than the decay time τ of the SiO 2 surface. This work facilitates an understanding of the triboelectric and de-electrification of the interface between 2D materials and substrates. In addition to the charge transfer and diffusion, we demonstrate the nanopatterns of surface and interfacial charges, which have great potential for the application of self-assembly of charged nanostructures.

Entropic effects in the electric double layer of model colloids with size-asymmetric monovalent ions

NASA Astrophysics Data System (ADS)

Guerrero-García, Guillermo Iván; González-Tovar, Enrique; Olvera de la Cruz, Mónica

2011-08-01

The structure of the electric double layer of charged nanoparticles and colloids in monovalent salts is crucial to determine their thermodynamics, solubility, and polyion adsorption. In this work, we explore the double layer structure and the possibility of charge reversal in relation to the size of both counterions and coions. We examine systems with various size-ratios between counterions and coions (ion size asymmetries) as well as different total ion volume fractions. Using Monte Carlo simulations and integral equations of a primitive-model electric double layer, we determine the highest charge neutralization and electrostatic screening near the electrified surface. Specifically, for two binary monovalent electrolytes with the same counterion properties but differing only in the coion's size surrounding a charged nanoparticle, the one with largest coion size is found to have the largest charge neutralization and screening. That is, in size-asymmetric double layers with a given counterion's size the excluded volume of the coions dictates the adsorption of the ionic charge close to the colloidal surface for monovalent salts. Furthermore, we demonstrate that charge reversal can occur at low surface charge densities, given a large enough total ion concentration, for systems of monovalent salts in a wide range of ion size asymmetries. In addition, we find a non-monotonic behavior for the corresponding maximum charge reversal, as a function of the colloidal bare charge. We also find that the reversal effect disappears for binary salts with large-size counterions and small-size coions at high surface charge densities. Lastly, we observe a good agreement between results from both Monte Carlo simulations and the integral equation theory across different colloidal charge densities and 1:1-elec-trolytes with different ion sizes.

Probing surface charge potentials of clay basal planes and edges by direct force measurements.

PubMed

Zhao, Hongying; Bhattacharjee, Subir; Chow, Ross; Wallace, Dean; Masliyah, Jacob H; Xu, Zhenghe

2008-11-18

The dispersion and gelation of clay suspensions have major impact on a number of industries, such as ceramic and composite materials processing, paper making, cement production, and consumer product formulation. To fundamentally understand controlling mechanisms of clay dispersion and gelation, it is necessary to study anisotropic surface charge properties and colloidal interactions of clay particles. In this study, a colloidal probe technique was employed to study the interaction forces between a silica probe and clay basal plane/edge surfaces. A muscovite mica was used as a representative of 2:1 phyllosilicate clay minerals. The muscovite basal plane was prepared by cleavage, while the edge surface was obtained by a microtome cutting technique. Direct force measurements demonstrated the anisotropic surface charge properties of the basal plane and edge surface. For the basal plane, the long-range forces were monotonically repulsive within pH 6-10 and the measured forces were pH-independent, thereby confirming that clay basal planes have permanent surface charge from isomorphic substitution of lattice elements. The measured interaction forces were fitted well with the classical DLVO theory. The surface potentials of muscovite basal plane derived from the measured force profiles were in good agreement with those reported in the literature. In the case of edge surfaces, the measured forces were monotonically repulsive at pH 10, decreasing with pH, and changed to be attractive at pH 5.6, strongly suggesting that the charge on the clay edge surfaces is pH-dependent. The measured force profiles could not be reasonably fitted with the classical DLVO theory, even with very small surface potential values, unless the surface roughness was considered. The surface element integration (SEI) method was used to calculate the DLVO forces to account for the surface roughness. The surface potentials of the muscovite edges were derived by fitting the measured force profiles with the surface element integrated DLVO model. The point of zero charge of the muscovite edge surface was estimated to be pH 7-8.

The Influence of Particle Charge on Heterogeneous Reaction Rate Coefficients

NASA Technical Reports Server (NTRS)

Aikin, A. C.; Pesnell, W. D.

2000-01-01

The effects of particle charge on heterogeneous reaction rates are presented. Many atmospheric particles, whether liquid or solid are charged. This surface charge causes a redistribution of charge within a liquid particle and as a consequence a perturbation in the gaseous uptake coefficient. The amount of perturbation is proportional to the external potential and the square of the ratio of debye length in the liquid to the particle radius. Previous modeling has shown how surface charge affects the uptake coefficient of charged aerosols. This effect is now included in the heterogeneous reaction rate of an aerosol ensemble. Extension of this analysis to ice particles will be discussed and examples presented.

Group IV nanocrystals with ion-exchangeable surface ligands and methods of making the same

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wheeler, Lance M.; Nichols, Asa W.; Chernomordik, Boris D.

Methods are described that include reacting a starting nanocrystal that includes a starting nanocrystal core and a covalently bound surface species to create an ion-exchangeable (IE) nanocrystal that includes a surface charge and a first ion-exchangeable (IE) surface ligand ionically bound to the surface charge, where the starting nanocrystal core includes a group IV element.

Single ion induced surface nanostructures: a comparison between slow highly charged and swift heavy ions.

PubMed

Aumayr, Friedrich; Facsko, Stefan; El-Said, Ayman S; Trautmann, Christina; Schleberger, Marika

2011-10-05

This topical review focuses on recent advances in the understanding of the formation of surface nanostructures, an intriguing phenomenon in ion-surface interaction due to the impact of individual ions. In many solid targets, swift heavy ions produce narrow cylindrical tracks accompanied by the formation of a surface nanostructure. More recently, a similar nanometric surface effect has been revealed for the impact of individual, very slow but highly charged ions. While swift ions transfer their large kinetic energy to the target via ionization and electronic excitation processes (electronic stopping), slow highly charged ions produce surface structures due to potential energy deposited at the top surface layers. Despite the differences in primary excitation, the similarity between the nanostructures is striking and strongly points to a common mechanism related to the energy transfer from the electronic to the lattice system of the target. A comparison of surface structures induced by swift heavy ions and slow highly charged ions provides a valuable insight to better understand the formation mechanisms. © 2011 IOP Publishing Ltd

The influence of size and charge of chitosan/polyglutamic acid hollow spheres on cellular internalization, viability and blood compatibility.

PubMed

Dash, Biraja C; Réthoré, Gildas; Monaghan, Michael; Fitzgerald, Kathleen; Gallagher, William; Pandit, Abhay

2010-11-01

Polymeric hollow spheres can be tailored as efficient carriers of various therapeutic molecules due to their tunable properties. However, the entry of these synthetic vehicles into cells, their cell viability and blood compatibility depend on their physical and chemical properties e.g. size, surface charge. Herein, we report the effect of size and surface charge on cell viability and cellular internalization behaviour and their effect on various blood components using chitosan/polyglutamic acid hollow spheres as a model system. Negatively charged chitosan/polyglutamic acid hollow spheres of various sizes 100, 300, 500 and 1000 nm were fabricated using a template based method and covalently surface modified using linear polyethylene glycol and methoxyethanol amine to create a gradient of surface charge from negative to neutrally charged spheres respectively. The results here suggest that both size and surface charge have a significant influence on the sphere's behaviour, most prominently on haemolysis, platelet activation, plasma recalcification time, cell viability and internalization over time. Additionally, cellular internalization behaviour and viability was found to vary with different cell types. These results are in agreement with those of inorganic spheres and liposomes, and can serve as guidelines for tailoring polymeric solid spheres for specific desired applications in biological and pharmaceutical fields, including the design of nanometer to submicron-sized delivery vehicles. Copyright (c) 2010 Elsevier Ltd. All rights reserved.

Catalytic Micromotors Moving Near Polyelectrolyte-Modified Substrates: The Roles of Surface Charges, Morphology, and Released Ions.

PubMed

Wei, Mengshi; Zhou, Chao; Tang, Jinyao; Wang, Wei

2018-01-24

Synthetic microswimmers, or micromotors, are finding potential uses in a wide range of applications, most of which involve boundaries. However, subtle yet important effects beyond physical confinement on the motor dynamics remain less understood. In this letter, glass substrates were functionalized with positively and negatively charged polyelectrolytes, and the dynamics of micromotors moving close to the modified surfaces was examined. Using acoustic levitation and numerical simulation, we reveal how the speed of a chemically propelled micromotor slows down significantly near a polyelectrolyte-modified surface by the combined effects of surface charges, surface morphology, and ions released from the films.

Unitized Regenerative Fuel Cell System Gas Storage/Radiator Development

NASA Technical Reports Server (NTRS)

Jakupca, Ian; Burke, Kenneth A.

2003-01-01

The ancillary components for Unitized Regenerative Fuel Cell (URFC) Energy Storage System are being developed at the NASA Glenn Research Center. This URFC system is unique in that it uses the surface area of the hydrogen and oxygen storage tanks as radiating heat surfaces for overall thermal control of the system. The waste heat generated by the URFC stack during charging and discharging is transferred from the cell stack to the surface of each tank by loop heat pipes. The heat pipes are coiled around each tank and covered with a thin layer of thermally conductive layer of carbon composite. The thin layer of carbon composite acts as a fin structure that spreads the heat away from the heat pipe and across the entire tank surface. Two different sized commercial grade composite tanks were constructed with integral heat pipes and tested in a thermal vacuum chamber to examine the feasibility of using the storage tanks as system radiators. The storage radiators were subjected to different steady-state heat loads and varying heat load profiles. The surface emissivity and specific heat capacity of each tank were calculated. The results were incorporated into a model that simulates the performance of similar radiators using lightweight, space rated carbon composite tanks.

Effect of solid surface charge on the binding behaviour of a metal-binding peptide

PubMed Central

Donatan, Senem; Sarikaya, Mehmet; Tamerler, Candan; Urgen, Mustafa

2012-01-01

Over the last decade, solid-binding peptides have been increasingly used as molecular building blocks coupling bio- and nanotechnology. Despite considerable research being invested in this field, the effects of many surface-related parameters that define the binding of peptide to solids are still unknown. In the quest to control biological molecules at solid interfaces and, thereby, tailoring the binding characteristics of the peptides, the use of surface charge of the solid surface may probably play an important role, which then can be used as a potential tuning parameter of peptide adsorption. Here, we report quantitative investigation on the viscoelastic properties and binding kinetics of an engineered gold-binding peptide, 3RGBP1, adsorbed onto the gold surface at different surface charge densities. The experiments were performed in aqueous solutions using an electrochemical dissipative quartz crystal microbalance system. Hydrodynamic mass, hydration state and surface coverage of the adsorbed peptide films were determined as a function of surface charge density of the gold metal substrate. Under each charged condition, binding of 3rGBP1 displayed quantitative differences in terms of adsorbed peptide amount, surface coverage ratio and hydration state. Based on the intrinsically disordered structure of the peptide, we propose a possible mechanism for binding of the peptide that can be used for tuning surface adsorption in further studies. Controlled alteration of peptide binding on solid surfaces, as shown here, may provide novel methods for surface functionalization used for bioenabled processing and fabrication of future micro- and nanodevices. PMID:22491974

The study of the dynamics of erythrocytes under the influence of an external electric field

NASA Astrophysics Data System (ADS)

Mamaeva, Sargylana N.; Maksimov, Georgy V.; Antonov, Stepan R.

2017-11-01

A mathematical model is considered for the determination of the surface charge of an erythrocyte with its shape approximated by a surface of revolution of the second order, and the investigation of the dynamics of erythrocytes under the influence of an external electric field. In the first part of this work, the electrical surface charge of the erythrocyte of the patient was calculated with the assumption that the change in the shape and size of the red blood cells leads to stabilization of the electric field, providing a normal electrostatic repulsion. In the second part of the work, the research results of dynamics of changes in the morphology of erythrocytes under the influence of an external electric field depending on the values of their surface charge and resistance of blood plasma is presented. In the course of the work, the dependence of the surface charge of red blood cells from their shape and size is presented. The determination of the relationship between the value of the charge field and the surface of erythrocytes in norm and in pathology is shown. The dependence of the velocity of the erythrocytes on the characteristics of the external electric field, surface charge of the erythrocyte and properties of the medium is obtained. The results of this study can be applied indirectly to diagnose diseases and to develop recommendations for experimental studies of hemodynamics under the influence of various external physical factors.

Rover wheel charging on the lunar surface

NASA Astrophysics Data System (ADS)

Jackson, Telana L.; Farrell, William M.; Zimmerman, Michael I.

2015-03-01

The environment at the Moon is dynamic, with highly variable solar wind plasma conditions at the lunar dayside, terminator, and night side regions. Moving objects such as rover wheels will charge due to contact electrification with the surface, but the degree of charging is controlled by the local plasma environment. Using a dynamic charging model of a wheel, it is demonstrated herein that moving tires will tribocharge substantially when venturing into plasma-current starved regions such as polar craters or the lunar nightside. The surface regolith distribution and the overall effect on charge accumulation of grains cohesively sticking to the rover tire has been incorporated into the model. It is shown that dust sticking can limit the overall charge accumulated on the system. However charge dissipation times are greatly increased in shadowed regions and can present a potential hazard to astronauts and electrical systems performing extra-vehicular activities. We show that dissipation times change with wheel composition and overall system tribocharging is dependent upon wheel velocity.

Carbodiimide-mediated immobilization of acidic biomolecules on reversed-charge zwitterionic sensor chip surfaces.

PubMed

Risse, Fabian; Gedig, Erk T; Gutmann, Jochen S

2018-04-30

The carbodiimide-mediated amine coupling of protein ligands to sensor chips coated with anionic polycarboxylate hydrogels, such as carboxymethyl dextran, is the predominant covalent immobilization procedure utilized in optical biosensors, namely surface plasmon resonance (SPR) biosensors. Usually, electrostatic interactions at a slightly acidic pH and low ionic strength are employed to efficiently accumulate neutral and basic ligands on the chip surface, which are then covalently coupled by surface-bound active N-hydroxysuccinimide (NHS) esters. Unfortunately, this approach is not suitable for acidic proteins or other ligands with low isoelectric points (IEPs), such as nucleic acids, because the charge density of the polycarboxylates is greatly reduced at acidic pH or because electrostatic attraction cannot be achieved. To overcome these drawbacks, we have established a charge-reversal approach that allows the preconcentration of acidic proteins above their IEPs. A precisely controlled amount of tertiary amines is applied to reverse the previous anionic surface charge while maintaining carbodiimide compatibility with future protein immobilization. The mechanism of this reversed-charge immobilization approach was demonstrated employing protein A as a model protein and using attenuated total reflectance Fourier transform infrared spectroscopy, dynamic contact angle measurements, colorimetric quantification, and SPR analysis to characterize surface derivatization. Furthermore, even though it had previously proven impossible to preconcentrate DNA electrostatically and to covalently couple it to polyanionic chip surfaces, we demonstrated that our approach allowed DNA to be preconcentrated and immobilized in good yields. Graphical abstract Principle of the covalent immobilization of acidic ligands on reversed-charge zwitterionic sensor chip surfaces.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Chunya; Skelton, Adam A.; Chen, Mingjun

Here the binding of a negatively charged residue, aspartic acid (Asp) in tripeptide arginine-glycine-aspartic acid, onto a negatively charged hydroxylated rutile (110) surface in aqueous solution, containing divalent (Mg 2+, Ca 2+, or Sr 2+) or monovalent (Na +, K +, or Rb +) cations, was studied by molecular dynamics (MD) simulations. The results indicate that ionic radii and charges will significantly affect the hydration, adsorption geometry, and distance of cations from the rutile surface, thereby regulating the Asp/rutile binding mode. The adsorption strength of monovalent cations on the rutile surface in the order Na + > K + >more » Rb + shows a “reverse” lyotropic trend, while the divalent cations on the same surface exhibit a “regular” lyotropic behavior with decreasing crystallographic radii (the adsorption strength of divalent cations: Sr 2+ > Ca 2+ > Mg 2+). The Asp side chain in NaCl, KCl, and RbCl solutions remains stably H-bonded to the surface hydroxyls and the inner-sphere adsorbed compensating monovalent cations act as a bridge between the COO – group and the rutile, helping to “trap” the negatively charged Asp side chain on the negatively charged surface. In contrast, the mediating divalent cations actively participate in linking the COO– group to the rutile surface; thus the Asp side chain can remain stably on the rutile (110) surface, even if it is not involved in any hydrogen bonds with the surface hydroxyls. Inner- and outer-sphere geometries are all possible mediation modes for divalent cations in bridging the peptide to the rutile surface.« less

Ground Simulations of Near-Surface Plasma Field and Charging at the Lunar Terminator

NASA Astrophysics Data System (ADS)

Polansky, J.; Ding, N.; Wang, J.; Craven, P.; Schneider, T.; Vaughn, J.

2012-12-01

Charging in the lunar terminator region is the most complex and is still not well understood. In this region, the surface potential is sensitively influenced by both solar illumination and plasma flow. The combined effects from localized shadow generated by low sun elevation angles and localized wake generated by plasma flow over the rugged terrain can generate strongly differentially charged surfaces. Few models currently exist that can accurately resolve the combined effects of plasma flow and solar illumination over realistic lunar terminator topographies. This paper presents an experimental investigation of lunar surface charging at the terminator region in simulated plasma environments in a vacuum chamber. The solar wind plasma flow is simulated using an electron bombardment gridded Argon ion source. An electrostatic Langmuir probe, nude Faraday probes, a floating emissive probe, and retarding potential analyzer are used to quantify the plasma flow field. Surface potentials of both conducting and dielectric materials immersed in the plasma flow are measured with a Trek surface potential probe. The conducting material surface potential will simultaneously be measured with a high impedance voltmeter to calibrate the Trek probe. Measurement results will be presented for flat surfaces and objects-on-surface for various angles of attack of the plasma flow. The implications on the generation of localized plasma wake and surface charging at the lunar terminator will be discussed. (This research is supported by the NASA Lunar Advanced Science and Exploration Research program.)

Holographic charged Rényi entropies

NASA Astrophysics Data System (ADS)

Belin, Alexandre; Hung, Ling-Yan; Maloney, Alexander; Matsuura, Shunji; Myers, Robert C.; Sierens, Todd

2013-12-01

We construct a new class of entanglement measures by extending the usual definition of Rényi entropy to include a chemical potential. These charged Rényi entropies measure the degree of entanglement in different charge sectors of the theory and are given by Euclidean path integrals with the insertion of a Wilson line encircling the entangling surface. We compute these entropies for a spherical entangling surface in CFT's with holographic duals, where they are related to entropies of charged black holes with hyperbolic horizons. We also compute charged Rényi entropies in free field theories.

An Investigation of Low Earth Orbit Internal Charging

NASA Technical Reports Server (NTRS)

NeergaardParker, Linda; Minow, Joseph I.; Willis, Emily M.

2014-01-01

Low Earth orbit is usually considered a relatively benign environment for internal charging threats due to the low flux of penetrating electrons with energies of a few MeV that are encountered over an orbit. There are configurations, however, where insulators and ungrounded conductors used on the outside of a spacecraft hull may charge when exposed to much lower energy electrons of some 100's keV in a process that is better characterized as internal charging than surface charging. For example, the minimal radiation shielding afforded by thin thermal control materials such as metalized polymer sheets (e.g., aluminized Kapton or Mylar) and multilayer insulation may allow electrons of 100's of keV to charge underlying materials. Yet these same thermal control materials protect the underlying insulators and ungrounded conductors from surface charging currents due to electrons and ions at energies less than a few keV as well as suppress the photoemission, secondary electron, and backscattered electron processes associated with surface charging. We investigate the conditions required for this low Earth orbit "internal charging" to occur and evaluate the environments for which the process may be a threat to spacecraft. First, we describe a simple one-dimensional internal charging model that is used to compute the charge accumulation on materials under thin shielding. Only the electron flux that penetrates exposed surface shielding material is considered and we treat the charge balance in underlying insulation as a parallel plate capacitor accumulating charge from the penetrating electron flux and losing charge due to conduction to a ground plane. Charge dissipation due to conduction can be neglected to consider the effects of charging an ungrounded conductor. In both cases, the potential and electric field is computed as a function of time. An additional charge loss process is introduced due to an electrostatic discharge current when the electric field reaches a prescribed breakdown strength. For simplicity, the amount of charge lost in the discharge is treated as a random percentage of the total charge between a set maximum and minimum amount so a user can consider partial discharges of insulating materials (small loss of charge) or arcing from a conductor (large loss of charge). We apply the model to electron flux measurements from the NOAA-19 spacecraft to demonstrate that charging can reach levels where electrostatic discharges occur and estimate the magnitude of the discharge.

Direct Observation of Individual Charges and Their Dynamics on Graphene by Low-Energy Electron Holography.

PubMed

Latychevskaia, Tatiana; Wicki, Flavio; Longchamp, Jean-Nicolas; Escher, Conrad; Fink, Hans-Werner

2016-09-14

Visualizing individual charges confined to molecules and observing their dynamics with high spatial resolution is a challenge for advancing various fields in science, ranging from mesoscopic physics to electron transfer events in biological molecules. We show here that the high sensitivity of low-energy electrons to local electric fields can be employed to directly visualize individual charged adsorbates and to study their behavior in a quantitative way. This makes electron holography a unique probing tool for directly visualizing charge distributions with a sensitivity of a fraction of an elementary charge. Moreover, spatial resolution in the nanometer range and fast data acquisition inherent to lens-less low-energy electron holography allows for direct visual inspection of charge transfer processes.

Charge effects on the hindered transport of macromolecules across the endothelial surface glycocalyx layer.

PubMed

Sugihara-Seki, Masako; Akinaga, Takeshi; O-Tani, Hideyuki

2012-01-01

A fluid mechanical and electrostatic model for the transport of solute molecules across the vascular endothelial surface glycocalyx layer (EGL) was developed to study the charge effect on the diffusive and convective transport of the solutes. The solute was assumed to be a spherical particle with a constant surface charge density, and the EGL was represented as an array of periodically arranged circular cylinders of like charge, with a constant surface charge density. By combining the fluid mechanical analyses for the flow around a solute suspended in an electrolyte solution and the electrostatic analyses for the free energy of the interaction between the solute and cylinders based on a mean field theory, we estimated the transport coefficients of the solute across the EGL. Both of diffusive and convective transports are reduced compared to those for an uncharged system, due to the stronger exclusion of the solute that results from the repulsive electrostatic interaction. The model prediction for the reflection coefficient for serum albumin agreed well with experimental observations if the charge density in the EGL is ranged from approximately -10 to -30 mEq/l.

Model for thickness dependence of radiation charging in MOS structures

NASA Technical Reports Server (NTRS)

Viswanathan, C. R.; Maserjian, J.

1976-01-01

The model considers charge buildup in MOS structures due to hole trapping in the oxide and the creation of sheet charge at the silicon interface. The contribution of hole trapping causes the flatband voltage to increase with thickness in a manner in which square and cube dependences are limiting cases. Experimental measurements on samples covering a 200 - 1000 A range of oxide thickness are consistent with the model, using independently obtained values of hole-trapping parameters. An important finding of our experimental results is that a negative interface charge contribution due to surface states created during irradiation compensates most of the positive charge in the oxide at flatband. The tendency of the surface states to 'track' the positive charge buildup in the oxide, for all thicknesses, applies both in creation during irradiation and in annihilation during annealing. An explanation is proposed based on the common defect origin of hole traps and potential surface states.

Adsorption properties of subtropical and tropical variable charge soils: Implications from climate change and biochar amendment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, Ren-Kou; Qafoku, Nikolla; Van Ranst, Eric

2016-01-25

This review paper attempts to summarize the progress made in research efforts conducted over the last years to study the surface chemical properties of the tropical and subtropical soils, usually called variable charge soils, and the way they response to different management practices. The paper is composed of an introductory section that provides a brief discussion on the surface chemical properties of these soils, and five other review sections. The focus of these sections is on the evolution of surface chemical properties during the development of the variable charge properties (second section), interactions between oppositely charged particles and the resultingmore » effects on the soil properties and especially on soil acidity (third section), the surface effects of low molecular weight organic acids sorbed to mineral surfaces and the chemical behavior of aluminum (fourth section), and the crop straw derived biochar induced changes of the surface chemical properties of these soils (fifth section). A discussion on the effect of climate change variables on the properties of the variable charge soils is included at the end of this review paper (sixth section).« less

Influence of surface charge on the rate, extent, and structure of adsorbed Bovine Serum Albumin to gold electrodes.

PubMed

Beykal, Burcu; Herzberg, Moshe; Oren, Yoram; Mauter, Meagan S

2015-12-15

The objective of this work is to investigate the rate, extent, and structure of amphoteric proteins with charged solid surfaces over a range of applied potentials and surface charges. We use Electrochemical Quartz Crystal Microbalance with Dissipation Monitoring (E-QCM-D) to investigate the adsorption of amphoteric Bovine Serum Albumin (BSA) to a gold electrode while systematically varying the surface charge on the adsorbate and adsorbent by manipulating pH and applied potential, respectively. We also perform cyclic voltammetry-E-QCM-D on an adsorbed layer of BSA to elucidate conformational changes in response to varied applied potentials. We confirm previous results demonstrating that increasing magnitude of applied potential on the gold electrode is positively correlated with increasing mass adsorption when the protein and the surface are oppositely charged. On the other hand, we find that the rate of BSA adsorption is not governed by simple electrostatics, but instead depends on solution pH, an observation not well documented in the literature. Cyclic voltammetry with simultaneous E-QCM-D measurements suggest that BSA protein undergoes a conformational change as the surface potential varies. Copyright © 2015 Elsevier Inc. All rights reserved.

On charging of snow particles in blizzard

NASA Technical Reports Server (NTRS)

Shio, Hisashi

1991-01-01

The causes of the charge polarity on the blizzard, which consisted of fractured snow crystals and ice particles, were investigated. As a result, the charging phenomena showed that the characteristics of the blizzard are as follows: (1) In the case of the blizzard with snowfall, the fractured snow particles drifting near the surface of snow field (lower area: height 0.3 m) had positive charge, while those drifting at higher area (height 2 m) from the surface of snow field had negative charge. However, during the series of blizzards two kinds of particles positively and negatively charged were collected in equal amounts in a Faraday Cage. It may be considered that snow crystals with electrically neutral properties were separated into two kinds of snow flakes (charged positively and negatively) by destruction of the snow crystals. (2) In the case of the blizzard which consisted of irregularly formed ice drops (generated by peeling off the hardened snow field), the charge polarity of these ice drops salting over the snow field was particularly controlled by the crystallographic characteristics of the surface of the snow field hardened by the powerful wind pressure.

Hamiltonian surface charges using external sources

DOE Office of Scientific and Technical Information (OSTI.GOV)

Troessaert, Cédric, E-mail: troessaert@cecs.cl

2016-05-15

In this work, we interpret part of the boundary conditions as external sources in order to partially solve the integrability problem present in the computation of surface charges associated to gauge symmetries in the hamiltonian formalism. We start by describing the hamiltonian structure of external symmetries preserving the action up to a transformation of the external sources of the theory. We then extend these results to the computation of surface charges for field theories with non-trivial boundary conditions.

Molecular Self-Assembly and Interfacial Engineering for Highly Efficient Organic Field Effect Transistors and Solar Cells

DTIC Science & Technology

2012-09-23

balance between disordered SAMs to promote large pentacene grains and thick SAMs to aid in physically buffering the charge carriers in pentacene from...to 0.76 µF/cm2), and enhanced pentacene OFET device performance such as higher charge carrier mobility, current on/off ratio, and lower threshold...surface charge trap • Tuning of surface energy • Control of surface group orientation SAM/MO ultrathin dielectric: • Low-voltage operation

On the Applicability of DLVO Theory to the Prediction of Clay Colloids Stability.

PubMed

Missana; Adell

2000-10-01

The stability behavior of Na-montmorillonite colloids has been studied by combining the analysis of their surface charge properties and time-resolved dynamic light scattering experiments. The chemical surface model for several types of clays, including montmorillonite, has to take into account the double surface charge contribution due to their permanent structural charge and to their pH-dependent charge, which is developed at the edge sites, therefore, these stability studies were carried out as a function of both ionic strength and pH. DLVO theory is largely applied for the prediction of the stability of many colloidal systems, including the natural ones. This work shows that the stability behavior of Na-montmorillonite colloids cannot be satisfactorily reproduced by DLVO theory, using the surface parameters experimentally obtained. Particularly, this theory is unable to explain their pH-dependent stability behavior caused by the small charge at the edge sites. Based on these results, a literature review of DLVO stability prediction of clay colloids was performed. It confirmed that this theory is not capable of taking into account the double contribution to the total surface charge and, at the same time, pointed out the main uncertainties related to the appropriate use of the input parameters for the calculation as, for example, the Hamaker constant or the surface potential. Copyright 2000 Academic Press.

Surface charge effects in protein adsorption on nanodiamonds

NASA Astrophysics Data System (ADS)

Aramesh, M.; Shimoni, O.; Ostrikov, K.; Prawer, S.; Cervenka, J.

2015-03-01

Understanding the interaction of proteins with charged diamond nanoparticles is of fundamental importance for diverse biomedical applications. Here we present a thorough study of protein binding, adsorption kinetics and structure on strongly positively (hydrogen-terminated) and negatively (oxygen-terminated) charged nanodiamond particles using a quartz crystal microbalance by dissipation and infrared spectroscopy. By using two model proteins (bovine serum albumin and lysozyme) of different properties (charge, molecular weight and rigidity), the main driving mechanism responsible for the protein binding to the charged nanoparticles was identified. Electrostatic interactions were found to dominate the protein adsorption dynamics, attachment and conformation. We developed a simple electrostatic model that can qualitatively explain the observed adsorption behaviour based on charge-induced pH modifications near the charged nanoparticle surfaces. Under neutral conditions, the local pH around the positively and negatively charged nanodiamonds becomes very high (11-12) and low (1-3) respectively, which has a profound impact on the protein charge, hydration and affinity to the nanodiamonds. Small proteins (lysozyme) were found to form multilayers with significant conformational changes to screen the surface charge, while larger proteins (albumin) formed monolayers with minor conformational changes. The findings of this study provide a step forward toward understanding and eventually predicting nanoparticle interactions with biofluids.Understanding the interaction of proteins with charged diamond nanoparticles is of fundamental importance for diverse biomedical applications. Here we present a thorough study of protein binding, adsorption kinetics and structure on strongly positively (hydrogen-terminated) and negatively (oxygen-terminated) charged nanodiamond particles using a quartz crystal microbalance by dissipation and infrared spectroscopy. By using two model proteins (bovine serum albumin and lysozyme) of different properties (charge, molecular weight and rigidity), the main driving mechanism responsible for the protein binding to the charged nanoparticles was identified. Electrostatic interactions were found to dominate the protein adsorption dynamics, attachment and conformation. We developed a simple electrostatic model that can qualitatively explain the observed adsorption behaviour based on charge-induced pH modifications near the charged nanoparticle surfaces. Under neutral conditions, the local pH around the positively and negatively charged nanodiamonds becomes very high (11-12) and low (1-3) respectively, which has a profound impact on the protein charge, hydration and affinity to the nanodiamonds. Small proteins (lysozyme) were found to form multilayers with significant conformational changes to screen the surface charge, while larger proteins (albumin) formed monolayers with minor conformational changes. The findings of this study provide a step forward toward understanding and eventually predicting nanoparticle interactions with biofluids. Electronic supplementary information (ESI) available: The FTIR spectrum of nanodiamonds, QCM-D profiles of 50 nm nanodiamond adsorption on silica surfaces, QCM-D profiles of protein desorption after rinsing with water (rinsing experiment) and the full FTIR spectrum of proteins before and after adsorption on ND particles. See DOI: 10.1039/c5nr00250h

Surface potential-governed cellular osteogenic differentiation on ferroelectric polyvinylidene fluoride trifluoroethylene films.

PubMed

Tang, Bolin; Zhang, Bo; Zhuang, Junjun; Wang, Qi; Dong, Lingqing; Cheng, Kui; Weng, Wenjian

2018-07-01

Surface potential of biomaterials can dramatically influence cellular osteogenic differentiation. In this work, a wide range of surface potential on ferroelectric polyvinylidene fluoride trifluoroethylene (P(VDF-TrFE)) films was designed to get insight into the interfacial interaction of cell-charged surface. The P(VDF-TrFE) films poled by contact electric poling at various electric fields obtained well stabilized surface potential, with wide range from -3 to 915 mV. The osteogenic differentiation level of cells cultured on the films was strongly dependent on surface potential and reached the optimum at 391 mV in this system. Binding specificity assay indicated that surface potential could effectively govern the binding state of the adsorbed fibronectin (FN) with integrin. Molecular dynamic (MD) simulation further revealed that surface potential brought a significant difference in the relative distance between RGD and synergy PHSRN sites of adsorbed FN, resulting in a distinct integrin-FN binding state. These results suggest that the full binding of integrin α5β1 with both RGD and PHSRN sites of FN possesses a strong ability to activate osteogenic signaling pathway. This work sheds light on the underlying mechanism of osteogenic differentiation behavior on charged material surfaces, and also provides a guidance for designing a reasonable charged surface to enhance osteogenic differentiation. The ferroelectric P(VDF-TrFE) films with steady and a wide range of surface potential were designed to understand underlying mechanism of cell-charged surface interaction. The results showed that the charged surface well favored upregulation of osteogenic differentiation of MC3T3-E1 cells, and more importantly, a highest level occurred on the film with a moderate surface potential. Experiments and molecular dynamics simulation demonstrated that the surface potential could govern fibronectin conformation and then the integrin-fibronectin binding. We propose that a full binding state of integrin α5β1 with fibronectin induces effective activation of integrin-mediated FAK/ERK signaling pathway to upregulate cellular osteogenic differentiation. This work provides a guidance for designing a reasonable charged surface to enhance osteogenic differentiation. Copyright © 2018 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Surface Oxide Net Charge of a Titanium Alloy; Comparison Between Effects of Treatment With Heat or Radiofrequency Plasma Glow Discharge

PubMed Central

MacDonald, Daniel E.; Rapuano, Bruce E.; Schniepp, Hannes C.

2010-01-01

In the current study, we have compared the effects of heat and radiofrequency plasma glow discharge (RFGD) treatment of a Ti6Al4V alloy on the physico-chemical properties of the alloy’s surface oxide. Titanium alloy (Ti6Al4V) disks were passivated alone, heated to 600 °C, or RFGD plasma treated in pure oxygen. RFGD treatment did not alter the roughness, topography, elemental composition or thickness of the alloy’s surface oxide layer. In contrast, heat treatment altered oxide topography by creating a pattern of oxide elevations approximately 50–100 nm in diameter. These nanostructures exhibited a three-fold increase in roughness compared to untreated surfaces when RMS roughness was calculated after applying a spatial high-pass filter with a 200 nm cutoff wavelength. Heat treatment also produced a surface enrichment in aluminum and vanadium oxides. Both RFGD and heat treatment produced similar increases in oxide wettability. Atomic force microscopy (AFM) measurements of metal surface oxide net charge signified by a long range force of attraction to or repulsion from a (negatively charged) silicon nitride AFM probe were also obtained for all three experimental groups. Force measurements showed that the RFGD-treated Ti6Al4V samples demonstrated a higher net positive surface charge at pH values below 6 and a higher net negative surface charge at physiological pH (pH values between 7 and 8) compared to control and heat-treated samples These findings suggest that RFGD treatment of metallic implant materials can be used to study the role of negatively charged surface oxide functional groups in protein bioactivity, osteogenic cell behavior and osseointegration independently of oxide topography. PMID:20880672

LUNAR SURFACE AND DUST GRAIN POTENTIALS DURING THE EARTH’S MAGNETOSPHERE CROSSING

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vaverka, J.; Richterová, I.; Pavlu, J.

2016-07-10

Interaction between the lunar surface and the solar UV radiation and surrounding plasma environment leads to its charging by different processes like photoemission, collection of charged particles, or secondary electron emission (SEE). Whereas the photoemission depends only on the angle between the surface and direction to the Sun and varies only slowly, plasma parameters can change rapidly as the Moon orbits around the Earth. This paper presents numerical simulations of one Moon pass through the magnetospheric tail including the real plasma parameters measured by THEMIS as an input. The calculations are concentrated on different charges of the lunar surface itselfmore » and a dust grain lifted above this surface. Our estimations show that (1) the SEE leads to a positive charging of parts of the lunar surface even in the magnetosphere, where a high negative potential is expected; (2) the SEE is generally more important for isolated dust grains than for the lunar surface covered by these grains; and (3) the time constant of charging of dust grains depends on their diameter being of the order of hours for sub-micrometer grains. In view of these results, we discuss the conditions under which and the areas where a levitation of the lifted dust grains could be observed.« less

Liouville master equation for multielectron dynamics: Neutralization of highly charged ions near a LiF surface

NASA Astrophysics Data System (ADS)

Wirtz, Ludger; Reinhold, Carlos O.; Lemell, Christoph; Burgdörfer, Joachim

2003-01-01

We present a simulation of the neutralization of highly charged ions in front of a lithium fluoride surface including the close-collision regime above the surface. The present approach employs a Monte Carlo solution of the Liouville master equation for the joint probability density of the ionic motion and the electronic population of the projectile and the target surface. It includes single as well as double particle-hole (de)excitation processes and incorporates electron correlation effects through the conditional dynamics of population strings. The input in terms of elementary one- and two-electron transfer rates is determined from classical trajectory Monte Carlo calculations as well as quantum-mechanical Auger calculations. For slow projectiles and normal incidence, the ionic motion depends sensitively on the interplay between image acceleration towards the surface and repulsion by an ensemble of positive hole charges in the surface (“trampoline effect”). For Ne10+ we find that image acceleration is dominant and no collective backscattering high above the surface takes place. For grazing incidence, our simulation delineates the pathways to complete neutralization. In accordance with recent experimental observations, most ions are reflected as neutral or even as singly charged negative particles, irrespective of the charge state of the incoming ions.

FY04 LDRD Final Report: Interaction of Viruses with Membranes and Soil Materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schaldach, C M

2005-02-08

The influence of ionic strength on the electrostatic interaction of viruses with environmentally relevant surfaces was determined for three viruses, MS2, Q{beta} and Norwalk. The environmental surface is modeled as charged Gouy-Chapman plane with and without a finite atomistic region (patch) of opposite charge. The virus is modeled as a particle comprised of ionizable amino acid residues in a shell surrounding a spherical RNA core of negative charge, these charges being compensated for by a Coulomb screening due to intercalated ions. Surface potential calculations for each of the viruses show excellent agreement with electrophoretic mobility and zeta potential measurements asmore » a function of pH. The results indicate that the electrostatic interaction between the virus and the planar surface, mitigated by the ionic strength of the solute, is dependent upon the spatial distribution of the amino acid residues in the different viruses. Specifically, the order of interaction energies with the patch (MS2 greatest at 5 mM; Norwalk greatest at 20 mM) is dependent upon the ionic strength of the fluid as a direct result of the viral coat amino acid distributions. We have developed an atomistic-scale method of calculation of the binding energy of viruses to surfaces including electrostatic, van der Waals, electron-overlap repulsion, surface charge polarization (images), and hydrophobic effects. The surface is treated as a Gouy-Chapman plane allowing inclusion of pH and ionic strength effects on the electrostatic potential at each amino acid charge. Van der Waals parameters are obtained from the DREIDING force field and from Hamaker constant measurements. We applied this method to the calculation of the Cowpea Mosaic Virus (CPMV), a negatively charged virus at a pH of 7.0, and find that the viral-gold surface interaction is very long range for both signs of surface potential, a result due to the electrostatic forces. For a negative (Au) surface potential of -0.05 volts, a nearly 4 eV barrier must be overcome to reach 1 nm from the surface.« less

Developing the next generation of graphene-based platforms for cancer therapeutics: The potential role of reactive oxygen species.

PubMed

Tabish, Tanveer A; Zhang, Shaowei; Winyard, Paul G

2018-05-01

Graphene has a promising future in applications such as disease diagnosis, cancer therapy, drug/gene delivery, bio-imaging and antibacterial approaches owing to graphene's unique physical, chemical and mechanical properties alongside minimal toxicity to normal cells, and photo-stability. However, these unique features and bioavailability of graphene are fraught with uncertainties and concerns for environmental and occupational exposure. Changes in the physicochemical properties of graphene affect biological responses including reactive oxygen species (ROS) production. Lower production of ROS by currently available theranostic agents, e.g. magnetic nanoparticles, carbon nanotubes, gold nanostructures or polymeric nanoparticles, restricts their clinical application in cancer therapy. Oxidative stress induced by graphene accumulated in living organs is due to acellular factors which may affect physiological interactions between graphene and target tissues and cells. Acellular factors include particle size, shape, surface charge, surface containing functional groups, and light activation. Cellular responses such as mitochondrial respiration, graphene-cell interactions and pH of the medium are also determinants of ROS production. The mechanisms of ROS production by graphene and the role of ROS for cancer treatment, are poorly understood. The aim of this review is to set the theoretical basis for further research in developing graphene-based theranostic platforms. Copyright © 2017 The Authors. Published by Elsevier B.V. All rights reserved.

Role of surface charge and oxidative stress in cytotoxicity of organic monolayer-coated silicon nanoparticles towards macrophage NR8383 cells

PubMed Central

2010-01-01

Background Surface charge and oxidative stress are often hypothesized to be important factors in cytotoxicity of nanoparticles. However, the role of these factors is not well understood. Hence, the aim of this study was to systematically investigate the role of surface charge, oxidative stress and possible involvement of mitochondria in the production of intracellular reactive oxygen species (ROS) upon exposure of rat macrophage NR8383 cells to silicon nanoparticles. For this aim highly monodisperse (size 1.6 ± 0.2 nm) and well-characterized Si core nanoparticles (Si NP) were used with a surface charge that depends on the specific covalently bound organic monolayers: positively charged Si NP-NH2, neutral Si NP-N3 and negatively charged Si NP-COOH. Results Positively charged Si NP-NH2 proved to be more cytotoxic in terms of reducing mitochondrial metabolic activity and effects on phagocytosis than neutral Si NP-N3, while negatively charged Si NP-COOH showed very little or no cytotoxicity. Si NP-NH2 produced the highest level of intracellular ROS, followed by Si NP-N3 and Si NP-COOH; the latter did not induce any intracellular ROS production. A similar trend in ROS production was observed in incubations with an isolated mitochondrial fraction from rat liver tissue in the presence of Si NP. Finally, vitamin E and vitamin C induced protection against the cytotoxicity of the Si NP-NH2 and Si NP-N3, corroborating the role of oxidative stress in the mechanism underlying the cytotoxicity of these Si NP. Conclusion Surface charge of Si-core nanoparticles plays an important role in determining their cytotoxicity. Production of intracellular ROS, with probable involvement of mitochondria, is an important mechanism for this cytotoxicity. PMID:20831820

Field-induced charge transport at the surface of pentacene single crystals: A method to study charge dynamics of two-dimensional electron systems in organic crystals

NASA Astrophysics Data System (ADS)

Takeya, J.; Goldmann, C.; Haas, S.; Pernstich, K. P.; Ketterer, B.; Batlogg, B.

2003-11-01

A method has been developed to inject mobile charges at the surface of organic molecular crystals, and the dc transport of field-induced holes has been measured at the surface of pentacene single crystals. To minimize damage to the soft and fragile surface, the crystals are attached to a prefabricated substrate which incorporates a gate dielectric (SiO2) and four probe pads. The surface mobility of the pentacene crystals ranges from 0.1 to 0.5 cm2/V s and is nearly temperature independent above ˜150 K, while it becomes thermally activated at lower temperatures when the induced charges become localized. Ruling out the influence of electric contacts and crystal grain boundaries, the results contribute to the microscopic understanding of trapping and detrapping mechanisms in organic molecular crystals.

Nanotoxicological and teratogenic effects: A linkage between dendrimer surface charge and zebrafish developmental stages.

PubMed

Calienni, Maria Natalia; Feas, Daniela Agustina; Igartúa, Daniela Edith; Chiaramoni, Nadia Silvia; Alonso, Silvia Del Valle; Prieto, Maria Jimena

2017-12-15

This article reports novel results about nanotoxicological and teratogenic effects of the PAMAM dendrimers DG4 and DG4.5 in zebrafish (Danio rerio). Zebrafish embryos and larvae were used as a rapid, high-throughput, cost-effective whole-animal model. The objective was to provide a more comprehensive and predictive developmental toxicity screening of DG4 and DG4.5 and test the influence of their surface charge. Nanotoxicological and teratogenic effects were assessed at developmental, morphological, cardiac, neurological and hepatic level. The effect of surface charge was determined in both larvae and embryos. DG4 with positive surface charge was more toxic than DG4.5 with negative surface charge. DG4 and DG4.5 induced teratogenic effects in larvae, whereas DG4 also induced lethal effects in both zebrafish embryos and larvae. However, larvae were less sensitive than embryos to the lethal effects of DG4. The platform of assays proposed and data obtained may contribute to the characterization of hazards and differential effects of these nanoparticles. Copyright © 2017 Elsevier Inc. All rights reserved.

Polyelectrolyte Multilayer Film Coated Silver Nanorods: An Effective Carrier System for Externally Activated Drug Delivery

NASA Astrophysics Data System (ADS)

Paramasivam, Gokul; Sharma, Varsha; Sundaramurthy, Anandhakumar

2017-08-01

Nanoparticle anisotropy offers unique functions and features in comparison with spherical nanoparticles (NPs) and makes anisotropic nanoparticles (ANPs) promising candidates in applications like drug delivery, imaging, biosensing and theranostics. Presence of surface active groups (e.g. amine, and carboxylate groups) on their surface provides binding sites for ligands or other biomolecules, and hence, this could be targeted for specific part or cells in our body. In the quest of such surface modification, functionalization of ANPs along Layer-by-Layer (LbL) coating of oppositely charged polyelectrolytes (PE) reduces cellular toxicity and promotes easy encapsulation of drugs. In this work, we report the silver nanorods (AgNRs) synthesis by adsorbate directed synthetic approach using cetyltrimethyl ammonium bromide (CTAB). The formed ANPs is investigated by scanning electron microscopy (SEM) and UV-Visible (UV-Vis) spectroscopy revealing the shaping of AgNRs of 3-16 nm aspect ratio with some presence of triangles. These NRs were further coated with bio polymers of chitosan (CH) and dextran sulphate (DS) through LbL approach and used for encapsulation of water soluble anti-bacterial drugs like ciprofloxacin hydrochloride (CFH). The encapsulation of drugs and profiles of drug release were investigated and compared to that of spherical silver nanoparticles (AgNPs). The added advantages of the proposed drug delivery system (DDS) can be externally activated to release the loaded drug and used as contrast agents for biological imaging under exposure to NIR light. Such system shows unique and attractive characteristics required for drug delivery and bioimaging thus offering the scope for further development as theranostic material.

CHARGED PARTICLE MULTIPLICITIES IN ULTRA-RELATIVISTIC AU+AU AND CU+CU COLLISIONS

NASA Astrophysics Data System (ADS)

Back, B. B.; Alver, B.; Back, B. B.; Baker, M. D.; Ballintijn, M.; Barton, D. S.; Betts, R. R.; Bickley, A. A.; Bindel, R.; Busza, W.; Carroll, A.; Chai, Z.; Chetluru, V.; Decowski, M. P.; Garcia, E.; Gburek, T.; George, N.; Gulbrandsen, K.; Halliwell, C.; Hamblen, J.; Harnarine, I.; Hauer, M.; Henderson, C.; Hofman, D. J.; Hollis, R. S.; Holynski, R.; Holzman, B.; Iordanova, A.; Johnson, E.; Kane, J. L.; Khan, N.; Kulinich, P.; Kuo, C. M.; Li, W.; Lin, W. T.; Loizides, C.; Manly, S.; Mignerey, A. C.; Nouicer, R.; Olszewski, A.; Pak, R.; Reed, C.; Richardson, E.; Roland, C.; Roland, G.; Sagerer, J.; Seals, H.; Sedykh, I.; Smith, C. E.; Stankiewicz, M. A.; Steinberg, P.; Stephans, G. S. F.; Sukhanov, A.; Szostak, A.; Tonjes, M. B.; Trzupek, A.; Vale, C.; Vannieuwenhuizen, G. J.; Vaurynovich, S. S.; Verdier, R.; Veres, G. I.; Walters, P.; Wenger, E.; Willhelm, D.; Wolfs, F. L. H.; Wosiek, B.; Wozniak, K.; Wyngaardt, S.; Wyslouch, B.

The PHOBOS collaboration has carried out a systematic study of charged particle multiplicities in Cu+Cu and Au+Au collisions at the Relativistic Heavy-Ion Collider (RHIC) at Brookhaven National Laboratory. A unique feature of the PHOBOS detector is its ability to measure charged particles over a very wide angular range from 0.5° to 179.5° corresponding to |η| <5.4. The general features of the charged particle multiplicity distributions as a function of pseudo-rapidity, collision energy and centrality, as well as system size, are discussed.

Dependence of Lunar Surface Charging on Solar Wind Plasma Conditions and Solar Irradiation

NASA Technical Reports Server (NTRS)

Stubbs, T. J.; Farrell, W. M.; Halekas, J. S.; Burchill, J. K.; Collier, M. R.; Zimmerman, M. I.; Vondrak, R. R.; Delory, G. T.; Pfaff, R. F.

2014-01-01

The surface of the Moon is electrically charged by exposure to solar radiation on its dayside, as well as by the continuous flux of charged particles from the various plasma environments that surround it. An electric potential develops between the lunar surface and ambient plasma, which manifests itself in a near-surface plasma sheath with a scale height of order the Debye length. This study investigates surface charging on the lunar dayside and near-terminator regions in the solar wind, for which the dominant current sources are usually from the pohotoemission of electrons, J(sub p), and the collection of plasma electrons J(sub e) and ions J(sub i). These currents are dependent on the following six parameters: plasma concentration n(sub 0), electron temperature T(sub e), ion temperature T(sub i), bulk flow velocity V, photoemission current at normal incidence J(sub P0), and photo electron temperature T(sub p). Using a numerical model, derived from a set of eleven basic assumptions, the influence of these six parameters on surface charging - characterized by the equilibrium surface potential, Debye length, and surface electric field - is investigated as a function of solar zenith angle. Overall, T(sub e) is the most important parameter, especially near the terminator, while J(sub P0) and T(sub p) dominate over most of the dayside.

Selective binding of proteins on functional nanoparticles via reverse charge parity model: an in vitro study

NASA Astrophysics Data System (ADS)

Ghosh, Goutam; Panicker, Lata; Barick, K. C.

2014-03-01

The conformation of proteins absorbed on nanoparticles surface plays a crucial role in applications of nanoparticles in biomedicine. The surface protein conformation depends on several factors, namely, nature of protein-nanoparticles interaction, chemical composition of the surface of nanoparticles etc. A model of the electrostatic binding of proteins on charged surface nanoparticles has been proposed earlier (Ghosh et al 2013 Colloids Surf. B 103 267). Also, the irreversible denaturation of the protein conformation due to binding of counterions was reported. In this paper, we have used this model, involving reverse charge parity, to show selective binding of proteins on charged surface iron oxide nanoparticles (IONPs). IONPs were surface functionalized with cetylpyridinium chloride (CPC), cetyl(trimethyl)ammonium bromide (CTAB) and cetylpyridinium iodide (CPI). The effect of counterions (Cl-, Br- and I-) on protein conformation has also been investigated. Several proteins such as α-lactalbumin (ALA), β-lactoglobulin (BLG), ovalbumin (OVA), bovin serum albumin (BSA) and HEWL were chosen for this investigation.

Electromagnetic Field Redistribution in Metal Nanoparticle on Graphene.

PubMed

Li, Keke; Liu, Anping; Wei, Dapeng; Yu, Keke; Sun, Xiaonan; Yan, Sheng; Huang, Yingzhou

2018-04-25

Benefiting from the induced image charge on metal film, the light energy is confined on a film surface under metal nanoparticle dimer, which is called electromagnetic field redistribution. In this work, electromagnetic field distribution of metal nanoparticle monomer or dimer on graphene is investigated through finite-difference time-domain method. The results point out that the electromagnetic field (EM) redistribution occurs in this nanoparticle/graphene hybrid system at infrared region where light energy could also be confined on a monolayer graphene surface. Surface charge distribution was analyzed using finite element analysis, and surface-enhanced Raman spectrum (SERS) was utilized to verify this phenomenon. Furthermore, the data about dielectric nanoparticle on monolayer graphene demonstrate this EM redistribution is attributed to strong coupling between light-excited surface charge on monolayer graphene and graphene plasmon-induced image charge on dielectric nanoparticle surface. Our work extends the knowledge of monolayer graphene plasmon, which has a wide range of applications in monolayer graphene-related film.

Enhanced charging kinetics of porous electrodes: surface conduction as a short-circuit mechanism.

PubMed

Mirzadeh, Mohammad; Gibou, Frederic; Squires, Todd M

2014-08-29

We use direct numerical simulations of the Poisson-Nernst-Planck equations to study the charging kinetics of porous electrodes and to evaluate the predictive capabilities of effective circuit models, both linear and nonlinear. The classic transmission line theory of de Levie holds for general electrode morphologies, but only at low applied potentials. Charging dynamics are slowed appreciably at high potentials, yet not as significantly as predicted by the nonlinear transmission line model of Biesheuvel and Bazant. We identify surface conduction as a mechanism which can effectively "short circuit" the high-resistance electrolyte in the bulk of the pores, thus accelerating the charging dynamics and boosting power densities. Notably, the boost in power density holds only for electrode morphologies with continuous conducting surfaces in the charging direction.

Interfaces Charged by a Nonionic Surfactant.

PubMed

Lee, Joohyung; Zhou, Zhang-Lin; Behrens, Sven Holger

2018-05-24

Highly hydrophobic, water-insoluble nonionic surfactants are often considered irrelevant to the ionization of interfaces at which they adsorb, despite observations that suggest otherwise. In the present study, we provide unambiguous evidence for the participation of a water-insoluble surfactant in interfacial ionization by conducting electrophoresis experiments for surfactant-stabilized nonpolar oil droplets in aqueous continuous phase. It was found that the surfactant with amine headgroup positively charged the surface of oil suspended in aqueous continuous phase (oil/water interface), which is consistent with its basic nature. In nonpolar oil continuous phase, the same surfactant positively charged the surface of solid silica (solid/oil interface) which is often considered acidic. The latter observation is exactly opposite to what the traditional acid-base mechanism of surface charging would predict, most clearly suggesting the possibility for another charging mechanism.

Anomalous mobility of highly charged particles in pores

DOE Office of Scientific and Technical Information (OSTI.GOV)

Qiu, Yinghua; Yang, Crystal; Hinkle, Preston

2015-07-16

Single micropores in resistive-pulse technique were used to understand a complex dependence of particle mobility on its surface charge density. We show that the mobility of highly charged carboxylated particles decreases with the increase of the solution pH due to an interplay of three effects: (i) ion condensation, (ii) formation of an asymmetric electrical double layer around the particle, and (iii) electroosmotic flow induced by the charges on the pore walls and the particle surfaces. The results are important for applying resistive-pulse technique to determine surface charge density and zeta potential of the particles. As a result, the experiments alsomore » indicate the presence of condensed ions, which contribute to the measured current if a sufficiently high electric field is applied across the pore.« less

Charged drop dynamics experiment using an electrostatic-acoustic hybrid system

NASA Technical Reports Server (NTRS)

Rhim, W. K.; Chung, S. K.; Trinh, E. H.; Elleman, D. D.

1987-01-01

The design and the performance of an electrostatic-acoustic hybrid system and its application to a charge drop rotation experiment are presented. This system can levitate a charged drop electrostatically and induce drop rotation or oscillation by imposing an acoustic torque or an oscillating acoustic pressure. Using this system, the equilibrium shapes and stability of a rotating charged drop were experimentally investigated. A 3 mm size water drop was rotated as a rigid body and its gyrostatic equilibrium shapes were observed. Families of axisymmetric shapes, two-lobed shapes, and eventual fissioning have been observed. With the assumption of 'effective surface tension' in which the surface charge simply modified the surface tension of neutral liquid, the results agree exceptionally well with the Brown and Scriven's (1980) prediction for uncharged drops.