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Sample records for aux interfaces liquide

  1. PREFACE: Functionalized Liquid Liquid Interfaces

    NASA Astrophysics Data System (ADS)

    Girault, Hubert; Kornyshev, Alexei A.; Monroe, Charles W.; Urbakh, Michael

    2007-09-01

    Most natural processes take place at interfaces. For this reason, surface science has been a focal point of modern research. At solid-liquid interfaces one can induce various species to adsorb or react, and thus may study interactions between the substrate and adsorbates, kinetic processes, optical properties, etc. Liquid-liquid interfaces, formed by immiscible liquids such as water and oil, have a number of distinctive features. Both sides of the interface are amenable to detailed physical and chemical analysis. By chemical or electrochemical means, metal or semiconductor nanoparticles can be formed or localised at the interface. Surfactants can be used to tailor surface properties, and also to place organic molecular or supermolecular constructions at the boundary between the liquids. Electric fields can be used to drive ions from one fluid to another, or even change the shape of the interface itself. In many cases, both liquids are optically transparent, making functionalized liquid-liquid interfaces promising for various optical applications based on the transmission or reflection of light. An advantage common to most of these systems is self-assembly; because a liquid-liquid interface is not mechanically constrained like a solid-liquid interface, it can easily access its most stable state, even after it has been driven far from equilibrium. This special issue focuses on four modes of liquid-liquid interfacial functionalization: the controlled adsorption of molecules or nanoparticles, the formation of adlayers or films, electrowetting, and ion transfer or interface-localized reactions. Interfacial adsorption can be driven electrically, chemically, or mechanically. The liquid-liquid interface can be used to study how anisotropic particles orient at a surface under the influence of a field, how surfactants interact with other adsorbates, and how nanoparticles aggregate; the transparency of the interface also makes the chirality of organic adsorbates amenable to

  2. Réactions aux interfaces de bicristaux compatibles et incompatibles

    NASA Astrophysics Data System (ADS)

    Taisne, A.; Décamps, B.; Priester, L.

    2003-03-01

    La rupture intergranulaire peut apparaître suite à la non accommodation des contraintes au voisinage de l'interface. La transmission du glissement au travers d'une interface est un des modes de relaxation possible qui dépend des paramètres suivants : facteurs géométriques (caractéristiques de l'interface et systèmes de glissement activés), constantes élastiques de chacune des phases. Dans cette étude, la microscopie électronique à transmission (MET) est utilisée pour analyser les configurations de dislocations résultant d'une déformation par fatigue de bicristaux d'acier austénoferritique de désorientations contrôlées. Deux types de bicristaux sont étudiés, compatible et incompatible plastiquement. Pour chacun d'eux, la déformation est initiée soit dans la phase ferritique α soit dans la phase austénitique γ selon la localisation d'une entaille préalable à l'essai mécanique. Les résultats permettent de remonter aux mécanismes élémentaires qui régissent le transfert “direct” ou “indirect” des dislocations à travers l'interface. Une corrélation avec le comportement des bicristaux à l'échelle macroscopique est également tentée.

  3. Reaction Dynamics at Liquid Interfaces

    NASA Astrophysics Data System (ADS)

    Benjamin, Ilan

    2015-04-01

    The liquid interface is a narrow, highly anisotropic region, characterized by rapidly varying density, polarity, and molecular structure. I review several aspects of interfacial solvation and show how these affect reactivity at liquid/liquid interfaces. I specifically consider ion transfer, electron transfer, and SN2 reactions, showing that solvent effects on these reactions can be understood by examining the unique structure and dynamics of the liquid interface region.

  4. Reaction dynamics at liquid interfaces.

    PubMed

    Benjamin, Ilan

    2015-04-01

    The liquid interface is a narrow, highly anisotropic region, characterized by rapidly varying density, polarity, and molecular structure. I review several aspects of interfacial solvation and show how these affect reactivity at liquid/liquid interfaces. I specifically consider ion transfer, electron transfer, and SN2 reactions, showing that solvent effects on these reactions can be understood by examining the unique structure and dynamics of the liquid interface region.

  5. Redox chemistry at liquid/liquid interfaces

    NASA Technical Reports Server (NTRS)

    Volkov, A. G.; Deamer, D. W.

    1997-01-01

    The interface between two immiscible liquids with immobilized photosynthetic pigments can serve as the simplest model of a biological membrane convenient for the investigation of photoprocesses accompanied by spatial separation of charges. As it follows from thermodynamics, if the resolvation energies of substrates and products are very different, the interface between two immiscible liquids may act as a catalyst. Theoretical aspects of charge transfer reactions at oil/water interfaces are discussed. Conditions under which the free energy of activation of the interfacial reaction of electron transfer decreases are established. The activation energy of electron transfer depends on the charges of the reactants and dielectric permittivity of the non-aqueous phase. This can be useful when choosing a pair of immiscible solvents to decrease the activation energy of the reaction in question or to inhibit an undesired process. Experimental interfacial catalytic systems are discussed. Amphiphilic molecules such as chlorophyll or porphyrins were studied as catalysts of electron transfer reactions at the oil/water interface.

  6. Redox chemistry at liquid/liquid interfaces

    NASA Technical Reports Server (NTRS)

    Volkov, A. G.; Deamer, D. W.

    1997-01-01

    The interface between two immiscible liquids with immobilized photosynthetic pigments can serve as the simplest model of a biological membrane convenient for the investigation of photoprocesses accompanied by spatial separation of charges. As it follows from thermodynamics, if the resolvation energies of substrates and products are very different, the interface between two immiscible liquids may act as a catalyst. Theoretical aspects of charge transfer reactions at oil/water interfaces are discussed. Conditions under which the free energy of activation of the interfacial reaction of electron transfer decreases are established. The activation energy of electron transfer depends on the charges of the reactants and dielectric permittivity of the non-aqueous phase. This can be useful when choosing a pair of immiscible solvents to decrease the activation energy of the reaction in question or to inhibit an undesired process. Experimental interfacial catalytic systems are discussed. Amphiphilic molecules such as chlorophyll or porphyrins were studied as catalysts of electron transfer reactions at the oil/water interface.

  7. Continuous Liquid Interface Production (CLIP)

    NASA Astrophysics Data System (ADS)

    Tumbleston, John

    Continuous liquid interface production (CLIP) can rapidly produce 3D parts using a range of polymeric materials. A DLP-based form of additive manufacturing, CLIP proceeds via projecting a sequence of UV images through an oxygen-permeable, UV-transparent window below a liquid resin bath. A thin uncured liquid layer, or dead zone, is created above the window and maintains a liquid interface below the advancing part. Above the dead zone, the curing part is drawn out of the resin bath creating suction forces that renew reactive liquid resin. The dead zone is created due to oxygen inhibition of photopolymerization, a process that is traditionally a nuisance in other photopolymerization applications. However, for CLIP oxygen inhibition and creation of the dead zone allows for a continuous mode of printing where UV exposure, resin renewal, and part elevation are conducted simultaneously. This continual process is fundamentally different from traditional bottom-up stereolithography printers where these steps must be conducted in separate and discrete steps. Furthermore, the relatively gentle nature of CLIP due to the established dead zone enables the use of unique materials with a wide range of mechanical properties. This presentation will showcase the CLIP technology and provide a detailed picture of interactions between different resin and process parameters. New applications for 3D printing that span the micro- to macro-scale enabled by CLIP's combination of unique materials and part production speed will also be presented.

  8. Pattern formation at liquid interfaces

    NASA Astrophysics Data System (ADS)

    Heidel, Barbara; Knobler, Charles M.

    1990-01-01

    Quantitative experimental investigations of pattern formation at a liquid interface are described. The reaction studied is the photoreduction of Fe 3+ in aqueous solution and the subsequent formation of Turnbull's Blue. Both the wavelength of the pattern and the time at which the break in homogeneity occurs have been studied as functions of the concentrations of the reactants and the viscosity of the solvent. Many of the features of the process are consistent with a mechanism in which autocatalysis is enhanced by double diffusion. Preliminary studies of pattern formation in the KI/starch/chloralhydrate system are also presented.

  9. Self-diffusion in liquid interfaces.

    PubMed

    Herth, Simone; Ye, Feng; Eggersmann, Martin; Gutfleisch, Oliver; Würschum, Roland

    2004-03-05

    For studying self-diffusion in liquid interfaces, 59Fe tracer diffusion was measured on ultrafine-grained Nd2Fe14B which undergoes an intergranular melting transition for low Nd excess. The diffusion coefficient in the intergranular liquid layers is found to be lower than in bulk melts indicating a hampered atomic mobility due to confinement. Well above the intergranular melting transition, the diffusivity in the liquid interfaces approaches a value characteristic for bulk melts.

  10. Understanding the liquid-liquid (water-hexane) interface

    NASA Astrophysics Data System (ADS)

    Murad, Sohail; Puri, Ishwar K.

    2017-10-01

    Nonequilibrium molecular dynamics simulations are employed to investigate the interfacial thermal resistance of nanoscale hexane-water interfaces subject to an applied heat flux. Our studies show that these liquid-liquid interfaces exhibit behavior significantly dissimilar to that of solid-liquid and solid-vapor interfaces. Notably, the thermal resistance of a hexane-water interface is contingent on the interfacial temperature gradient alone with negligible dependence on the mean interfacial temperature, while the solid-liquid dependent strongly on the interfacial temperature. Application of a heat flux also increases the interface thickness significantly as compared to an equilibrium isothermal interface. Since liquid-liquid interfaces have been proposed for diverse applications, e.g., sensors for wastewater treatment and for extraction of toxic ions from water, they can be designed to be wider by applying a heat flux. This may allow the interface to be used for other applications not possible currently because of the very limited thickness of the interface in isothermal systems.

  11. Polymer Crystallization at Curved Liquid/Liquid Interface

    NASA Astrophysics Data System (ADS)

    Wang, Wenda

    Liquid/liquid interface, either flat or curved, is a unique template for studying self-assembly of a variety of nanomaterials such as nanoparticles and nanorods. The resultant monolayer films can be ordered or disordered depending on the regularity of the nanomaterials. Integration of nanoparticles into two-dimensional structure leads to intriguing collective properties of the nanoparticles. Crystallization can also be guided by liquid/liquid interface. Due to the particular shape of the interface, crystallization can happen in a different manner comparing to the normal solution crystallization. In this dissertation, liquid/liquid interface is employed to guide the crystallization of polymers, mainly focusing on using curved liquid/liquid interface. Due to the unique shape of the interface and feasibility to control the curvature, polymer crystallization can take place in different manner and lead to the formation of curved or vesicular crystals. Curved liquid/liquid interface is typically created through o/w emulsions. With the presence of surfactant, the emulsions are controlled to be stable at least for the polymer crystallization periods. The difference to normal solution crystallization is: the nuclei will diffuse to the curved interface due to the Pickering effect and guide the crystallization along the curved liquid/liquid interface. If the supercooling can be controlled to be very small, crystal growth in the bulk droplets can be avoided. The advantages of this strategy are: 1) the formation process of vesicular type crystals can be monitored by controlling the polymer supply; 2) curved crystals, bowl-like structures and enclosed capsules can be easily obtained comparing to the self-assembly method for vesicle formation; 3) the obtained vesicles will be made of polymer crystals, which will possess the extraordinary mechanical properties. Based on the nucleation type, this dissertation is divided into two parts. The first part is focused on the self

  12. Nanomaterials at Liquid/Liquid Interfaces-A Review.

    PubMed

    Divya, V; Sangaranarayanan, M V

    2015-09-01

    The charge transfer processes occurring at the interface between two immiscible electrolyte solutions are of considerable importance in diverse fields of chemistry and biology. The introduction to nanoparticles and analysis of nanostructures in diverse branches of science and engineering are provided. The chemical and electrochemical techniques pertaining to the synthesis of metal nanoparticles, polymeric nanostructures and metal-polymer nanocomposites at liquid/liquid interfaces are surveyed. The unique features pertaining to the chemical synthesis of metal nanoparticles while employing diverse electrolytes and solvents are outlined. The advantages of various electrochemical synthetic protocols such as four-electrode assembly, thin film electrode, Scanning Electrochemical Microscopy and Solid/liquid/liquid interfaces for the study of nanoparticles at liquid/liquid interfaces are emphasized. The crucial role played by the liquid/liquid interfaces in altering the morphological patterns of metal nanoparticles, conducting polymers and metal-polymer nanocomposites is indicated. A few typical novel applications of these nanomaterials in fabrication of biosensors, electrochemical supercapacitors, and electrocatalysts have been outlined.

  13. Low frequency ionic conduction across liquid interfaces

    NASA Astrophysics Data System (ADS)

    Solis, Francisco J.; Guerrero, Guillermo Ivan; Olvera de La Cruz, Monica

    Ionic conduction in liquid media is a central component of many recently proposed technologies. As in the case of solid state systems, the presence of heterogeneous media gives rise to interesting nonlinear phenomena. We present simulations and theoretical analysis of the low frequency ionic conduction in a two-liquid system. In the case analyzed, the conduction is driven by an electric field perpendicular to the liquid-liquid interface. We show that the dielectric contrast between the liquids produces non-linear effects in the effective conductivity of the system and discuss the effects of the ion solubility in the media.

  14. Deformation of liquid-liquid interfaces by a rotating rod

    NASA Astrophysics Data System (ADS)

    Zhao, C. W.; Gentric, C.; Dietrich, N.; Ma, Y. G.; Li, Huai Z.

    2017-07-01

    The present study aims at investigating the deformation mechanism of liquid-liquid interfaces by both the experimental and numerical approaches. The experiments reveal that the topology of an initial flat interface composed of Newtonian aqueous and Newtonian oil phases can be modulated as climbing or descending along a rotating rod according to the ratio of the kinematic viscosity between these two liquid phases. The measurements of the fluid flow fields by particle image velocimetry highlight the relationship between the appearance of the Taylor-Couette instability in the less viscous phase and the interface's orientation. The increasing rod rotation speed expands the Taylor-Couette vortices and then intensifies the magnitude of the interface deformation. The numerical simulation by the volume of fluid method is in qualitative agreement with the experimental results, in particular the interface shape and the qualitative influence of different parameters, even under very high rotation speeds of the rod.

  15. Energy conversion at liquid/liquid interfaces: artificial photosynthetic systems

    NASA Technical Reports Server (NTRS)

    Volkov, A. G.; Gugeshashvili, M. I.; Deamer, D. W.

    1995-01-01

    This chapter focuses on multielectron reactions in organized assemblies of molecules at the liquid/liquid interface. We describe the thermodynamic and kinetic parameters of such reactions, including the structure of the reaction centers, charge movement along the electron transfer pathways, and the role of electric double layers in artificial photosynthesis. Some examples of artificial photosynthesis at the oil/water interface are considered, including water photooxidation to the molecular oxygen, oxygen photoreduction, photosynthesis of amphiphilic compounds and proton evolution by photochemical processes.

  16. Energy conversion at liquid/liquid interfaces: artificial photosynthetic systems

    NASA Technical Reports Server (NTRS)

    Volkov, A. G.; Gugeshashvili, M. I.; Deamer, D. W.

    1995-01-01

    This chapter focuses on multielectron reactions in organized assemblies of molecules at the liquid/liquid interface. We describe the thermodynamic and kinetic parameters of such reactions, including the structure of the reaction centers, charge movement along the electron transfer pathways, and the role of electric double layers in artificial photosynthesis. Some examples of artificial photosynthesis at the oil/water interface are considered, including water photooxidation to the molecular oxygen, oxygen photoreduction, photosynthesis of amphiphilic compounds and proton evolution by photochemical processes.

  17. Slip at liquid-liquid interfaces

    NASA Astrophysics Data System (ADS)

    Poesio, P.; Damone, A.; Matar, Omar K.

    2017-04-01

    We address a problem of fundamental importance in the physics of interfaces, which is central to the description of multiphase fluid dynamics. This work is important to study interfaces in systems such as polymer melts and solutions, where velocity jumps have been observed and interpreted as a manifestation of slip. This is in violation of classical interfacial conditions that require continuity of velocity and has been remedied in the literature via use of ad hoc models, such as the so-called Navier slip condition. This paper suggests that it is possible to obviate completely the need for such an approach. Instead, we show that one simply requires knowledge of the density field and the molar fraction of the fluid components and the dependence of the viscosity on the density. This information can be obtained easily through molecular dynamics simulations.

  18. Janus particles at liquid-liquid interfaces.

    PubMed

    Glaser, Nicole; Adams, Dave J; Böker, Alexander; Krausch, Georg

    2006-06-06

    Following recent theoretical predictions, we report on the first experiments on the interfacial activity of so-called Janus nanoparticles (i.e., bifacial particles consisting of a gold and an iron oxide moiety). Using pendant drop tensiometry, we show that the amphiphilicity derived from the Janus character of the particles leads to a significantly higher interfacial activity compared to that of the respective homogeneous particles of the same size. The self-assembly of Janus particles at the hexane-water interface results in a significant decrease in the interfacial tension. Furthermore, we demonstrate control over the interfacial activity by tuning the particles' amphiphilicity via ligand-exchange reactions.

  19. Reactions and Polymerizations at the Liquid-Liquid Interface.

    PubMed

    Piradashvili, Keti; Alexandrino, Evandro M; Wurm, Frederik R; Landfester, Katharina

    2016-02-24

    Reactions and polymerizations at the interface of two immiscible liquids are reviewed. The confinement of two reactants at the interface to form a new product can be advantageous in terms of improved reaction kinetics, higher yields, and selectivity. The presence of the liquid-liquid interface can accelerate the reaction, or a phase-transfer catalyst is employed to draw the reaction in one phase of choice. Furthermore, the use of immiscible systems, e.g., in emulsions, offers an easy means of efficient product separation and heat dissipation. A general overview on low molecular weight organic chemistry is given, and the applications of heterophase polymerization, occurring at or in proximity of the interface, (mostly) in emulsions are presented. This strategy can be used for the efficient production of nano- and microcarriers for various applications.

  20. Structural Transitions at Ionic Liquid Interfaces.

    PubMed

    Rotenberg, Benjamin; Salanne, Mathieu

    2015-12-17

    Recent advances in experimental and computational techniques have allowed for an accurate description of the adsorption of ionic liquids on metallic electrodes. It is now well-established that they adopt a multilayered structure and that the composition of the layers changes with the potential of the electrode. In some cases, potential-driven ordering transitions in the first adsorbed layer have been observed in experiments probing the interface on the molecular scale or by molecular simulations. This perspective gives an overview of the current understanding of such transitions and of their potential impact on the physical and (electro)chemical processes at the interface. In particular, peaks in the differential capacitance, slow dynamics at the interface, and changes in the reactivity have been reported in electrochemical studies. Interfaces between ionic liquids and metallic electrodes are also highly relevant for their friction properties, the voltage-dependence of which opens the way to exciting applications.

  1. Liquid crystal interfaces: Experiments, simulations and biosensors

    NASA Astrophysics Data System (ADS)

    Popov, Piotr

    Interfacial phenomena are ubiquitous and extremely important in various aspects of biological and industrial processes. For example, many liquid crystal applications start by alignment with a surface. The underlying mechanisms of the molecular organization of liquid crystals at an interface are still under intensive study and continue to be important to the display industry in order to develop better and/or new display technology. My dissertation research has been devoted to studying how complex liquid crystals can be guided to organize at an interface, and to using my findings to develop practical applications. Specifically, I have been working on developing biosensors using liquid-crystal/surfactant/lipid/protein interactions as well as the alignment of low-symmetry liquid crystals for potential new display and optomechanical applications. The biotechnology industry needs better ways of sensing biomaterials and identifying various nanoscale events at biological interfaces and in aqueous solutions. Sensors in which the recognition material is a liquid crystal naturally connects the existing knowledge and experience of the display and biotechnology industries together with surface and soft matter sciences. This dissertation thus mainly focuses on the delicate phenomena that happen at liquid interfaces. In the introduction, I start by defining the interface and discuss its structure and the relevant interfacial forces. I then introduce the general characteristics of biosensors and, in particular, describe the design of biosensors that employ liquid crystal/aqueous solution interfaces. I further describe the basic properties of liquid crystal materials that are relevant for liquid crystal-based biosensing applications. In CHAPTER 2, I describe the simulation methods and experimental techniques used in this dissertation. In CHAPTER 3 and CHAPTER 4, I present my computer simulation work. CHAPTER 3 presents insight of how liquid crystal molecules are aligned by

  2. Particle Behavior at Anisotropically Curved Liquid Interfaces

    NASA Astrophysics Data System (ADS)

    McEnnis, Kathleen; Zeng, Chuan; Davidovitch, Benny; Dinsmore, Anthony; Russell, Thomas

    2011-03-01

    A particle bound to an anisotropically curved liquid interface, such as a cylinder or catenoid, cannot maintain a constant contact angle without deforming the interface. Theory suggests that the particles will experience a force that depends on the interfacial shape and migrate to minimize the total interfacial energy. To test these predictions, particles were deposited on top of liquid semi-cylinders of ionic liquid or melted polystyrene confined on chemically patterned surfaces. Particles were also deposited on liquid catenoid structures created by placing a melted polymer film under an electric field. The location of the particles on these structures was observed by optical, confocal, and scanning electron microscopy. The implications for the directed assembly of particles and stability of Pickering emulsions are also discussed.

  3. A molecular theory of liquid interfaces.

    PubMed

    Kovalenko, Andriy; Hirata, Fumio

    2005-04-21

    We propose a site site generalization of the Lovett-Mow-Buff-Wertheim integro-differential equation for the one-particle density distributions to polyatomic fluids. The method provides microscopic description of liquid interfaces of molecular fluids and solutions. It uses the inhomogeneous site-site direct correlation function of molecular fluid consistently constructed by nonlinear interpolation between the homogeneous ones. The site site correlations of the coexisting bulk phases are obtained from the reference interaction site model (RISM) integral equation with our closure approximation. For illustration, we calculated the structure of the planar liquid-vapor as well as liquid-liquid interfaces of n-hexane and methanol at ambient conditions.

  4. Gas-liquid interface of room-temperature ionic liquids.

    PubMed

    Santos, Cherry S; Baldelli, Steven

    2010-06-01

    The organization of ions at the interface of ionic liquids and the vacuum is an ideal system to test new ideas and concepts on the interfacial chemistry of electrolyte systems in the limit of no solvent medium. Whilst electrolyte systems have numerous theoretical and experimental methods used to investigate their properties, the ionic liquids are relatively new and our understanding of the interfacial properties is just beginning to be explored. In this critical review, the gas-liquid interface is reviewed, as this interface does not depend on the preparation of another medium and thus produces a natural interface. The interface has been investigated by sum frequency generation vibrational spectroscopy and ultra-high vacuum techniques. The results provide a detailed molecular-level view of the surface composition and structure. These have been complemented by theoretical studies. The combinations of treatments on this interface are starting to provide a somewhat convergent description of how the ions are organized at this neat interface (108 references).

  5. Second harmonic studies of liquid interfaces

    SciTech Connect

    Ong, S.

    1992-12-31

    This thesis reports on experimental studies of kinetics and equilibria at liquid interfaces using the technique of Second Harmonic Generation (SHG). In the first part, SHG was used to study the kinetics of adsorption of p-nitrophenol at the air/water interface of a flowing liquid jet. Measurements of the SH signal strength and the polarization of the SH light at various distances (times) along the jet axis yield information about the development of the density and orientation of p-nitrophenol at the air/water interface. The kinetics of adsorption was interpreted in terms of the Langmuir theory and was found to be consistent with this model. The free energy of adsorption obtained from the jet experiments was found to be the same as that obtained from static (equilibrium) experiments. The orientation of p-nitrophenol at the jet air/solution interface was the same as for the static (equilibrium) interface,which indicates that orientational equilibrium was rapidly achieved. It was also found that adsorption of nitrophenol to the air/water interface is not diffusion controlled, but rather is kinetically controlled by a barrier. SHG was then used to probe the silica/water interface.

  6. Microrheology and Particle Dynamics at Liquid-Liquid Interfaces

    NASA Astrophysics Data System (ADS)

    Song, Yanmei

    The rheological properties at liquid-liquid interfaces are important in many industrial processes such as manufacturing foods, pharmaceuticals, cosmetics, and petroleum products. This dissertation focuses on the study of linear viscoelastic properties at liquid-liquid interfaces by tracking the thermal motion of particles confined at the interfaces. The technique of interfacial microrheology is first developed using one- and two-particle tracking, respectively. In one-particle interfacial microrheology, the rheological response at the interface is measured from the motion of individual particles. One-particle interfacial microrheology at polydimethylsiloxane (PDMS) oil-water interfaces depends strongly on the surface chemistry of different tracer particles. In contrast, by tracking the correlated motion of particle pairs, two-particle interfacial microrheology significantly minimizes the effects from tracer particle surface chemistry and particle size. Two-particle interfacial microrheology is further applied to study the linear viscoelastic properties of immiscible polymer-polymer interfaces. The interfacial loss and storage moduli at PDMS-polyethylene glycol (PEG) interfaces are measured over a wide frequency range. The zero-shear interfacial viscosity, estimated from the Cross model, falls between the bulk viscosities of two individual polymers. Surprisingly, the interfacial relaxation time is observed to be an order of magnitude larger than that of the PDMS bulk polymers. To explore the fundamental basis of interfacial nanorheology, molecular dynamics (MD) simulations are employed to investigate the nanoparticle dynamics. The diffusion of single nanoparticles in pure water and low-viscosity PDMS oils is reasonably consistent with the prediction by the Stokes-Einstein equation. To demonstrate the potential of nanorheology based on the motion of nanoparticles, the shear moduli and viscosities of the bulk phases and interfaces are calculated from single

  7. Solid-Liquid Interface Characterization Hardware

    NASA Technical Reports Server (NTRS)

    Peters, Palmer N.

    2000-01-01

    The objective is to develop enabling technology to characterize the solid-liquid interface during directional solidification to unprecedented levels with real-time measurement hardware. Existing x-ray imaging hardware is combined with compact Seebeck furnaces and thermal profiling hardware, under development, to accomplish the measurements. Furnace thermal profiles are continuously measured in addition to the sample characteristics.

  8. Liquid film/polymer interfaces

    SciTech Connect

    Allara, David L.

    2003-06-12

    The objectives were: (1) Through experimental studies, advance the fundamental understanding of the principles that govern adsorption and wetting phenomena at polymer and organic surfaces. (2) Establish a firm scientific basis for improving the design of coatings for metal fin cooling surfaces used to control the wetting of water condensate for optimum energy efficiency. Several important findings were: (1) water adsorbed at hydrophobic surfaces has a liquid-like structure, in contrast to the generally held view of an ordered structure; (2) Correlations of large amounts of contact angle wetting data of grafted alkyl chain compounds showed a distinct link between the contact angle and the conformational ordering of the chains; (3) water adsorption at long chain alkysiloxane films showed a strong pH dependence on the film stability, which can be attributed to interfacial chemical effects on the siloxane network.

  9. Orientation of semiflexible polymers at a liquid/liquid interface

    NASA Astrophysics Data System (ADS)

    ten Bosch, Alexandra

    2001-03-01

    The formation and control of ordered liquid layers at an interface is of fundamental and practical interest and useful in the many applications of lubricants and coatings and in the preparation of self assembled liquids. Orientational order is observed in polymer systems in the immediate vicinity of a surface or interface. Semiflexible polymers resist deformation perpendicular to the monomer and the anchoring force at the surface fixes the direction of preferred orientation by coupling the direction of the molecular axis and the surface plane. When a second incompatible liquid is added to the system, a sharp interface between the two liquids forms at a given distance from the supporting substrate. By changing the nature of the second liquid, this second constraint can control the order and force the polymer in the ordered surface layer to assume different conformations. The wormlike chain model is used to calculate the orientational order parameter, the extent of the ordered surface layer and the anisotropic chain conformation and the parameters are determined for which an extended or contracted conformation will occur.

  10. Liquid-vapor interfaces of patchy colloids

    NASA Astrophysics Data System (ADS)

    Oleksy, A.; Teixeira, P. I. C.

    2015-01-01

    We investigate the liquid-vapor interface of a model of patchy colloids. This model consists of hard spheres decorated with short-ranged attractive sites ("patches") of different types on their surfaces. We focus on a one-component fluid with two patches of type A and nine patches of type B (2 A 9 B colloids), which has been found to exhibit reentrant liquid-vapor coexistence curves and very low-density liquid phases. We have used the density-functional theory form of Wertheim's first-order perturbation theory of association, as implemented by Yu and Wu [J. Chem. Phys. 116, 7094 (2002), 10.1063/1.1463435], to calculate the surface tension, and the density and degree of association profiles, at the liquid-vapor interface of our model. In reentrant systems, where A B bonds dominate, an unusual thickening of the interface is observed at low temperatures. Furthermore, the surface tension versus temperature curve reaches a maximum, in agreement with Bernardino and Telo da Gama's mesoscopic Landau-Safran theory [Phys. Rev. Lett. 109, 116103 (2012), 10.1103/PhysRevLett.109.116103]. If B B attractions are also present, competition between A B and B B bonds gradually restores the monotonic temperature dependence of the surface tension. Lastly, the interface is "hairy," i.e., it contains a region where the average chain length is close to that in the bulk liquid, but where the density is that of the vapor. Sufficiently strong B B attractions remove these features, and the system reverts to the behavior seen in atomic fluids.

  11. Systems and methods for monitoring a solid-liquid interface

    DOEpatents

    Stoddard, Nathan G; Lewis, Monte A.; Clark, Roger F

    2013-06-11

    Systems and methods are provided for monitoring a solid-liquid interface during a casting process. The systems and methods enable determination of the location of a solid-liquid interface during the casting process.

  12. Surface Science at the Solid Liquid Interface

    DTIC Science & Technology

    1993-10-06

    quantitative changes of A4’ in the different adsorption of OH(ad) to molecular H20 and O(ad)] a further small states on Ni (221 ) and Ni (665) are not a... ADSORPTION * MODELING OF THE WATER-SOLID INTERFACE * THEORY OF CHARGED SOLID SURFACES A POSTER SESSION IS PLANNED FOR MONDAY EVENING WITH POSTERS ON DISPLAY...Pat Thiel [Iowa State] and by Dr. Fred Wagner [General Motors], who discussed adsorption of water and co- adsorption (leading to liquid interface

  13. Interfacing liquid metals with stretchable metal conductors.

    PubMed

    Kim, Bongsoo; Jang, Jaehyeok; You, Insang; Park, Jaeyoon; Shin, SangBaie; Jeon, Gumhye; Kim, Jin Kon; Jeong, Unyong

    2015-04-22

    Highly stretchable conductors are essential components in deformable electronics. Owing to their high stretchability and conductivity, liquid metals have attracted significant attention for use as circuits and interconnections. However, their poor wettability to stretchable metal electrodes prevents the formation of stable electrical connections. This study examined two approaches for creating a stable interface between a liquid metal (EGaIn) and stretchable metal electrodes via: (i) the use of honeycomb-structured stretchable metal electrodes and (ii) the addition of a conducting polymer interlayer. The line width of the honeycomb had a significant influence on the formation of a stable interface. The liquid metal formed a stable film layer on honeycomb metal electrodes, which have line widths of less than 50 μm. Coating PSS with a nonionic surfactant lowered the interfacial energy of EGaIn with flat stretchable metal surfaces; hence EGaIn was coated uniformly on the stretchable metal surfaces. Strain sensors were fabricated as a demonstrative example of an application that utilizes the stable interface.

  14. Interface for liquid chromatograph-mass spectrometer

    DOEpatents

    Andresen, Brian D.; Fought, Eric R.

    1989-01-01

    A moving belt interface for real-time, high-performance liquid chromatograph (HPLC)/mass spectrometer (MS) analysis which strips away the HPLC solvent as it emerges from the end of the HPLC column and leaves a residue suitable for mass-spectral analysis. The interface includes a portable, stand-alone apparatus having a plural stage vacuum station, a continuous ribbon or belt, a drive train magnetically coupled to an external drive motor, a calibrated HPLC delivery system, a heated probe tip and means located adjacent the probe tip for direct ionization of the residue on the belt. The interface is also capable of being readily adapted to fit any mass spectrometer.

  15. Interface for liquid chromatograph-mass spectrometer

    DOEpatents

    Andresen, B.D.; Fought, E.R.

    1989-09-19

    A moving belt interface is described for real-time, high-performance liquid chromatograph (HPLC)/mass spectrometer (MS) analysis which strips away the HPLC solvent as it emerges from the end of the HPLC column and leaves a residue suitable for mass-spectral analysis. The interface includes a portable, stand-alone apparatus having a plural stage vacuum station, a continuous ribbon or belt, a drive train magnetically coupled to an external drive motor, a calibrated HPLC delivery system, a heated probe tip and means located adjacent the probe tip for direct ionization of the residue on the belt. The interface is also capable of being readily adapted to fit any mass spectrometer. 8 figs.

  16. Polymer single crystal membrane from liquid/liquid interface

    NASA Astrophysics Data System (ADS)

    Wang, Wenda; Li, Christopher; Soft Matter Research Group-Drexel University Team

    2013-03-01

    Vesicles, mimicking the structure of cell membrane at the molecular scale, are small membrane-enclosed sacks that can store or transport substances. The weak mechanical properties and the nature of environment-sensitivity of the current available vesicles: liposomes, polymersomes, colloidsomes limit their applications as an excellent candidate for targeting delivery of drugs/genes in biomedical engineering and treatment. Recently, we developed an emulsion-based method to grow curved polymer single crystals. Varying the polymer concentration and/or the emulsification conditions (such as surfactant concentration, water-oil volume ratio), curved crystals with different sizes and different openness could be obtained. This growing process was attributed to polymer crystal growth along the liquid/liquid interface. In addition, the liquid/liquid interfacial crystal growth is promising for synthesis of enclosed hollow sphere.

  17. Solidification along the interface between demixed liquids in monotectic systems.

    PubMed

    Hüter, C; Boussinot, G; Brener, E A; Temkin, D E

    2011-05-01

    The steady-state solidification along the liquid-liquid interface in the monotectic system is discussed. A boundary-integral formulation describing the diffusion in the two liquid phases is given and the corresponding equations for the three interfaces (two solid-liquid interfaces and one liquid-liquid interface) are solved. Scaling relations are extracted from the results and supported by analytic arguments in the limit of small deviation from the monotectic temperature. We present also a complementary phase-field simulation, which proves the stability of the process.

  18. Electroviscoelasticity of liquid/liquid interfaces: fractional-order model.

    PubMed

    Spasic, Aleksandar M; Lazarevic, Mihailo P

    2005-02-01

    A number of theories that describe the behavior of liquid-liquid interfaces have been developed and applied to various dispersed systems, e.g., Stokes, Reiner-Rivelin, Ericksen, Einstein, Smoluchowski, and Kinch. A new theory of electroviscoelasticity describes the behavior of electrified liquid-liquid interfaces in fine dispersed systems and is based on a new constitutive model of liquids. According to this model liquid-liquid droplet or droplet-film structure (collective of particles) is considered as a macroscopic system with internal structure determined by the way the molecules (ions) are tuned (structured) into the primary components of a cluster configuration. How the tuning/structuring occurs depends on the physical fields involved, both potential (elastic forces) and nonpotential (resistance forces). All these microelements of the primary structure can be considered as electromechanical oscillators assembled into groups, so that excitation by an external physical field may cause oscillations at the resonant/characteristic frequency of the system itself (coupling at the characteristic frequency). Up to now, three possible mathematical formalisms have been discussed related to the theory of electroviscoelasticity. The first is the tension tensor model, where the normal and tangential forces are considered, only in mathematical formalism, regardless of their origin (mechanical and/or electrical). The second is the Van der Pol derivative model, presented by linear and nonlinear differential equations. Finally, the third model presents an effort to generalize the previous Van der Pol equation: the ordinary time derivative and integral are now replaced with the corresponding fractional-order time derivative and integral of order p<1.

  19. Single Fusion Events at Polarized Liquid-Liquid Interfaces.

    PubMed

    Laborda, Eduardo; Molina, Angela; Espín, Vanesa Fernández; Martínez-Ortiz, Francisco; García de la Torre, José; Compton, Richard G

    2017-01-16

    A new electrochemical framework for tracking individual soft particles in solution and monitoring their fusion with polarized liquid-liquid interfaces is reported. The physicochemical principle lies in the interfacial transfer of an ionic probe confined in the particles dispersed in solution and that is released upon their collision and fusion with the fluid interface. As a proof-of-concept, spike-like transients of a stochastic nature are reported in the current-time response of 1,2-dichloroethane(DCE)|water(W) submilli-interfaces after injection of DCE-in-W emulsions. The sign and potential dependence of the spikes reflect the charge and lipophilicity of the ionic load of the droplets. A comparison with dynamic light scattering measurements indicates that each spike is associated with the collision of a single sub-picoliter droplet. This opens a new framework for the study of single fusion events at the micro- and nanoscale and of ion transport across biomimetic soft interfaces.

  20. Layerless fabrication with continuous liquid interface production.

    PubMed

    Janusziewicz, Rima; Tumbleston, John R; Quintanilla, Adam L; Mecham, Sue J; DeSimone, Joseph M

    2016-10-18

    Despite the increasing popularity of 3D printing, also known as additive manufacturing (AM), the technique has not developed beyond the realm of rapid prototyping. This confinement of the field can be attributed to the inherent flaws of layer-by-layer printing and, in particular, anisotropic mechanical properties that depend on print direction, visible by the staircasing surface finish effect. Continuous liquid interface production (CLIP) is an alternative approach to AM that capitalizes on the fundamental principle of oxygen-inhibited photopolymerization to generate a continual liquid interface of uncured resin between the growing part and the exposure window. This interface eliminates the necessity of an iterative layer-by-layer process, allowing for continuous production. Herein we report the advantages of continuous production, specifically the fabrication of layerless parts. These advantages enable the fabrication of large overhangs without the use of supports, reduction of the staircasing effect without compromising fabrication time, and isotropic mechanical properties. Combined, these advantages result in multiple indicators of layerless and monolithic fabrication using CLIP technology.

  1. Layerless fabrication with continuous liquid interface production

    PubMed Central

    Janusziewicz, Rima; Tumbleston, John R.; Quintanilla, Adam L.; Mecham, Sue J.; DeSimone, Joseph M.

    2016-01-01

    Despite the increasing popularity of 3D printing, also known as additive manufacturing (AM), the technique has not developed beyond the realm of rapid prototyping. This confinement of the field can be attributed to the inherent flaws of layer-by-layer printing and, in particular, anisotropic mechanical properties that depend on print direction, visible by the staircasing surface finish effect. Continuous liquid interface production (CLIP) is an alternative approach to AM that capitalizes on the fundamental principle of oxygen-inhibited photopolymerization to generate a continual liquid interface of uncured resin between the growing part and the exposure window. This interface eliminates the necessity of an iterative layer-by-layer process, allowing for continuous production. Herein we report the advantages of continuous production, specifically the fabrication of layerless parts. These advantages enable the fabrication of large overhangs without the use of supports, reduction of the staircasing effect without compromising fabrication time, and isotropic mechanical properties. Combined, these advantages result in multiple indicators of layerless and monolithic fabrication using CLIP technology. PMID:27671641

  2. Wave-based liquid-interface metamaterials

    NASA Astrophysics Data System (ADS)

    Francois, N.; Xia, H.; Punzmann, H.; Fontana, P. W.; Shats, M.

    2017-02-01

    The control of matter motion at liquid-gas interfaces opens an opportunity to create two-dimensional materials with remotely tunable properties. In analogy with optical lattices used in ultra-cold atom physics, such materials can be created by a wave field capable of dynamically guiding matter into periodic spatial structures. Here we show experimentally that such structures can be realized at the macroscopic scale on a liquid surface by using rotating waves. The wave angular momentum is transferred to floating micro-particles, guiding them along closed trajectories. These orbits form stable spatially periodic patterns, the unit cells of a two-dimensional wave-based material. Such dynamic patterns, a mirror image of the concept of metamaterials, are scalable and biocompatible. They can be used in assembly applications, conversion of wave energy into mean two-dimensional flows and for organising motion of active swimmers.

  3. Wave-based liquid-interface metamaterials

    PubMed Central

    Francois, N; Xia, H; Punzmann, H; Fontana, P W; Shats, M

    2017-01-01

    The control of matter motion at liquid–gas interfaces opens an opportunity to create two-dimensional materials with remotely tunable properties. In analogy with optical lattices used in ultra-cold atom physics, such materials can be created by a wave field capable of dynamically guiding matter into periodic spatial structures. Here we show experimentally that such structures can be realized at the macroscopic scale on a liquid surface by using rotating waves. The wave angular momentum is transferred to floating micro-particles, guiding them along closed trajectories. These orbits form stable spatially periodic patterns, the unit cells of a two-dimensional wave-based material. Such dynamic patterns, a mirror image of the concept of metamaterials, are scalable and biocompatible. They can be used in assembly applications, conversion of wave energy into mean two-dimensional flows and for organising motion of active swimmers. PMID:28181490

  4. Dispersion of Particles on Fluid-Liquid Interfaces

    NASA Astrophysics Data System (ADS)

    Dalal, B.; Gurupatham, S.; Hossain, M.; Fischer, I.; Singh, P.; Joseph, D.

    2011-11-01

    This talk is concerned with the dispersion of particles on the fluid-liquid interface. In our previous studies we have shown that when small particles, e.g., flour, pollen, etc., come in contact with an air-liquid interface, they disperse in a manner that appears explosive. This is due to the fact that the capillary force pulls particles into the interface causing them to accelerate to a relatively-large velocity. The motion of particles in the direction normal to the interface is inertia dominated, and so they oscillate vertically about the equilibrium position before coming to a stop under viscous drag. This causes a radially-outward lateral flow on the interface that causes nearby particles to move away. In experiments the strength of the lateral flow was measured using tracer particles that were placed on the interface for this purpose. The dispersion on a liquid-liquid interface was relatively weaker than on an air-liquid interface, and occurred over a longer period of time. This partly was a consequence of the fact that particles became separated while sedimenting through the upper liquid and reached the interface over a time interval that lasted for several seconds. The rate of dispersion depended on the size of particles, the particle and liquids densities, the viscosities of the liquids involved, and the contact angle.

  5. Phase Segregation at the Liquid-Air Interface Prior to Liquid-Liquid Equilibrium.

    PubMed

    Bermúdez-Salguero, Carolina; Gracia-Fadrique, Jesús

    2015-08-13

    Binary systems with partial miscibility segregate into two liquid phases when their overall composition lies within the interval defined by the saturation points; out of this interval, there is one single phase, either solvent-rich or solute-rich. In most systems, in the one-phase regions, surface tension decreases with increasing solute concentration due to solute adsorption at the liquid-air interface. Therefore, the solute concentration at the surface is higher than in the bulk, leading to the hypothesis that phase segregation starts at the liquid-air interface with the formation of two surface phases, before the liquid-liquid equilibrium. This phenomenon is called surface segregation and is a step toward understanding liquid segregation at a molecular level and detailing the constitution of fluid interfaces. Surface segregation of aqueous binary systems of alkyl acetates with partial miscibility was theoretically demonstrated by means of a thermodynamic stability test based on energy minimization. Experimentally, the coexistence of two surface regions was verified through Brewster's angle microscopy. The observations were further interpreted with the aid of molecular dynamics simulations, which show the diffusion of the acetates from the bulk toward the liquid-air interface, where acetates aggregate into acetate-rich domains.

  6. (The physics of pattern formation at liquid interfaces)

    SciTech Connect

    Not Available

    1990-01-01

    This paper discusses pattern formation at liquid interfaces and interfaces within disordered materials. The particular topics discussed are: a racetrack for competing viscous fingers; an experimental realization of periodic boundary conditions; what sets the length scale for patterns between miscible liquids; the fractal dimension of radial Hele-Shaw patterns; detailed analyses of low-contrast Saffman-Taylor flows; and the wetting/absorption properties of polystyrene spheres in binary liquid mixtures. (LSP)

  7. LSPR properties of metal nanoparticles adsorbed at a liquid-liquid interface.

    PubMed

    Yang, Zhilin; Chen, Shu; Fang, Pingping; Ren, Bin; Girault, Hubert H; Tian, Zhongqun

    2013-04-21

    Unlike the solid-air and solid-liquid interfaces, the optical properties of metal nanoparticles adsorbed at the liquid-liquid interface have not been theoretically exploited to date. In this work, the three dimensional finite difference time domain (3D-FDTD) method is employed to clarify the localized surface plasmon resonance (LSPR) based optical properties of gold nanoparticles (NPs) adsorbed at the water-oil interface, including near field distribution, far field absorption and their relevance. The LSPR spectra of NPs located at a liquid-liquid interface are shown to differ significantly from those in a uniform liquid environment or at the other interfaces. The absorption spectra exhibit two distinct LSPR peaks, the positions and relative strengths of which are sensitive to the dielectric properties of each liquid and the exact positions of the NPs with respect to the interface. Precise control of the particles' position and selection of the appropriate wavelength of the excitation laser facilitates the rational design and selective excitation of localized plasmon modes for interfacial NPs, a necessary advance for the exploration of liquid-liquid interfaces via surface enhanced Raman spectroscopy (SERS). According to our calculations, the SERS enhancement factor for Au nanosphere dimers at the water-oil interface can be as high as 10(7)-10(9), implying significant promise for future investigations of interfacial structure and applications of liquid-liquid interfaces towards chemical analysis.

  8. Non-wetting drops at liquid interfaces: from liquid marbles to Leidenfrost drops

    NASA Astrophysics Data System (ADS)

    Wong, Clint Y. H.; Adda-Bedia, Mokhtar; Vella, Dominic

    We consider the flotation of deformable, non-wetting drops on a liquid interface. We consider the deflection of both the liquid interface and the droplet itself in response to the buoyancy forces, density difference and the various surface tensions within the system. Our results suggest new insight into a range of phenomena in which such drops occur, including Leidenfrost droplets and floating liquid marbles. In particular, we show that the floating state of liquid marbles is very sensitive to the tension of the particle-covered interface and suggest that this sensitivity may make such experiments a useful assay of the properties of these complex interfaces.

  9. Non-wetting drops at liquid interfaces: from liquid marbles to Leidenfrost drops.

    PubMed

    Wong, Clint Y H; Adda-Bedia, Mokhtar; Vella, Dominic

    2017-08-09

    We consider the flotation of deformable, non-wetting drops on a liquid interface. We consider the deflection of both the liquid interface and the droplet itself in response to the buoyancy forces, density difference and the various surface tensions within the system. Our results suggest new insight into a range of phenomena in which such drops occur, including Leidenfrost droplets and floating liquid marbles. In particular, we show that the floating state of liquid marbles is very sensitive to the tension of the particle-covered interface and suggest that this sensitivity may make such experiments a useful assay of the properties of these complex interfaces.

  10. Polarity of the interface in ionic liquid in oil microemulsions.

    PubMed

    Andújar-Matalobos, María; García-Río, Luis; López-García, Susana; Rodríguez-Dafonte, Pedro

    2011-11-01

    Ionic liquid based microemulsions were characterized by absorption solvatochromic shifts, (1)H NMR and kinetic measurements in order to investigate the properties of the ionic liquid within the restricted geometry provided by microemulsions and the interactions of the ionic liquid with the interface. Experimental results show a significant difference between the interfaces of normal water and the new ionic liquid microemulsions. Absorption solvatochromic shift experiments and kinetic studies on the aminolysis of 4-nitrophenyl laurate by n-decylamine show that the polarity at the interface of the ionic liquid in oil microemulsions (IL/O) is higher than at the interface of water in oil microemulsions (W/O) despite the fact that the polarity of [bmim][BF(4)(-)] is lower than the polarity of water. (1)H NMR experiments showed that an increase in the ionic liquid content of the microemulsion led to an increase in the interaction between [bmim][BF(4)(-)] and TX-100. The reason for the higher polarity of the microemulsions with the ionic liquid can be explained in terms of the incorporation of higher levels of the ionic liquid at the interface of the microemulsions, as compared to water in the traditional systems. Copyright © 2011 Elsevier Inc. All rights reserved.

  11. Thermal Convection Affects Shape Of Solid/Liquid Interface

    NASA Technical Reports Server (NTRS)

    Mennetrier, C.; Chopra, M. A.; Yao, M.; De Groh, H. C., III; Yeoh, G. H.; De Vahl Davis, G.; Leonardi, E.

    1994-01-01

    Report describes experimental and theoretical study of effect of thermal convection on shape of interface between solid and liquid succinonitrile, clear commercially available plastic, in Bridgman (directional-solidification) apparatus in vertical and horizontal orientations.

  12. Computer modelling of the surface tension of the gas-liquid and liquid-liquid interface.

    PubMed

    Ghoufi, Aziz; Malfreyt, Patrice; Tildesley, Dominic J

    2016-03-07

    This review presents the state of the art in molecular simulations of interfacial systems and of the calculation of the surface tension from the underlying intermolecular potential. We provide a short account of different methodological factors (size-effects, truncation procedures, long-range corrections and potential models) that can affect the results of the simulations. Accurate calculations are presented for the calculation of the surface tension as a function of the temperature, pressure and composition by considering the planar gas-liquid interface of a range of molecular fluids. In particular, we consider the challenging problems of reproducing the interfacial tension of salt solutions as a function of the salt molality; the simulations of spherical interfaces including the calculation of the sign and size of the Tolman length for a spherical droplet; the use of coarse-grained models in the calculation of the interfacial tension of liquid-liquid surfaces and the mesoscopic simulations of oil-water-surfactant interfacial systems.

  13. Enzyme Activity and Biomolecule Templating at Liquid and Solid Interfaces

    SciTech Connect

    Harvey W. Blanch

    2004-12-01

    There are two main components of this research program. The first involves studies of the adsorption and catalytic activity of proteins at fluid-fluid and fluid-solid interfaces; the second employs biological macromolecules as templates at the solid-liquid interface for controlled crystallization of inorganic materials, to provide materials with specific functionality.

  14. Nanofluidic transport governed by the liquid/vapour interface.

    PubMed

    Lee, Jongho; Laoui, Tahar; Karnik, Rohit

    2014-04-01

    Liquid/vapour interfaces govern the behaviour of a wide range of systems but remain poorly understood, leaving ample margin for the exploitation of intriguing functionalities for applications. Here, we systematically investigate the role of liquid/vapour interfaces in the transport of water across apposing liquid menisci in osmosis membranes comprising short hydrophobic nanopores that separate two fluid reservoirs. We show experimentally that mass transport is limited by molecular reflection from the liquid/vapour interface below a certain length scale, which depends on the transmission probability of water molecules across the nanopores and on the condensation probability of a water molecule incident on the liquid surface. This fundamental yet elusive condensation property of water is measured under near-equilibrium conditions and found to decrease from 0.36 ± 0.21 at 30 °C to 0.18 ± 0.09 at 60 °C. These findings define the regime in which liquid/vapour interfaces govern nanofluidic transport and have implications for understanding mass transport in nanofluidic devices, droplets and bubbles, biological components and porous media involving liquid/vapour interfaces.

  15. Self-assembly of a surfactin nanolayer at solid-liquid and air-liquid interfaces.

    PubMed

    Onaizi, Sagheer A; Nasser, M S; Al-Lagtah, Nasir M A

    2016-05-01

    Surfactin, a sustainable and environmentally friendly surface active agent, is used as a model to study the adsorption of biosurfactants at hydrophobic and hydrophilic solid-liquid interfaces as well as the air-liquid interface. Surfactin adsorption was monitored as a function of time and concentration using surface plasmon resonance (SPR) technique in the case of the solid-liquid interfaces or the drop shape analysis (DSA) technique in the case of the air-liquid interface. The results obtained in this study showed that surfactin adsorption at the "hard" hydrophobic (functionalized with octadecanethiol) solid-liquid and the "soft" air-liquid interface were 1.12 ± 0.01 mg m(-2) (area per molecule of 157 ± 2 Å(2)) and 1.11 ± 0.05 mg m(-2) (area per molecule of 159 ± 7 Å(2)), respectively, demonstrating the negligible effect of the interface "hardness" on surfactin adsorption. The adsorption of surfactin at the hydrophilic (functionalized with β-mercaptoethanol) solid-liquid interface was about threefold lower than its adsorption at the hydrophobic-liquid interfaces, revealing the importance of hydrophobic interaction in surfactin adsorption process. The affinity constant of surfactin for the investigated interfaces follows the following order: air > octadecanethiol > β-mercaptoethanol. Biosurfactants, such as surfactin, are expected to replace the conventional fossil-based surfactants in several applications, and therefore the current study is a contribution towards the fundamental understanding of biosurfactant behavior, on a molecular level, at hydrophobic and hydrophilic solid-liquid interfaces in addition to the air-liquid interface. Such understanding might aid further optimization of the utilization of surfactin in a number of industrial applications such as enhanced oil recovery, bioremediation, and detergency.

  16. Superhydrophobic-like tunable droplet bouncing on slippery liquid interfaces.

    PubMed

    Hao, Chonglei; Li, Jing; Liu, Yuan; Zhou, Xiaofeng; Liu, Yahua; Liu, Rong; Che, Lufeng; Zhou, Wenzhong; Sun, Dong; Li, Lawrence; Xu, Lei; Wang, Zuankai

    2015-08-07

    Droplet impacting on solid or liquid interfaces is a ubiquitous phenomenon in nature. Although complete rebound of droplets is widely observed on superhydrophobic surfaces, the bouncing of droplets on liquid is usually vulnerable due to easy collapse of entrapped air pocket underneath the impinging droplet. Here, we report a superhydrophobic-like bouncing regime on thin liquid film, characterized by the contact time, the spreading dynamics, and the restitution coefficient independent of underlying liquid film. Through experimental exploration and theoretical analysis, we demonstrate that the manifestation of such a superhydrophobic-like bouncing necessitates an intricate interplay between the Weber number, the thickness and viscosity of liquid film. Such insights allow us to tune the droplet behaviours in a well-controlled fashion. We anticipate that the combination of superhydrophobic-like bouncing with inherent advantages of emerging slippery liquid interfaces will find a wide range of applications.

  17. Superhydrophobic-like tunable droplet bouncing on slippery liquid interfaces

    PubMed Central

    Hao, Chonglei; Li, Jing; Liu, Yuan; Zhou, Xiaofeng; Liu, Yahua; Liu, Rong; Che, Lufeng; Zhou, Wenzhong; Sun, Dong; Li, Lawrence; Xu, Lei; Wang, Zuankai

    2015-01-01

    Droplet impacting on solid or liquid interfaces is a ubiquitous phenomenon in nature. Although complete rebound of droplets is widely observed on superhydrophobic surfaces, the bouncing of droplets on liquid is usually vulnerable due to easy collapse of entrapped air pocket underneath the impinging droplet. Here, we report a superhydrophobic-like bouncing regime on thin liquid film, characterized by the contact time, the spreading dynamics, and the restitution coefficient independent of underlying liquid film. Through experimental exploration and theoretical analysis, we demonstrate that the manifestation of such a superhydrophobic-like bouncing necessitates an intricate interplay between the Weber number, the thickness and viscosity of liquid film. Such insights allow us to tune the droplet behaviours in a well-controlled fashion. We anticipate that the combination of superhydrophobic-like bouncing with inherent advantages of emerging slippery liquid interfaces will find a wide range of applications. PMID:26250403

  18. Switchable Thermal Interfaces Based on Discrete Liquid Droplets

    SciTech Connect

    Jia, YB; Cha, G; Ju, YS

    2012-01-06

    We present a switchable thermal interface based on an array of discrete liquid droplets initially confined on hydrophilic islands on a substrate. The droplets undergo reversible morphological transition into a continuous liquid film when they are mechanically compressed by an opposing substrate to create low-thermal resistance heat conduction path. We investigate a criterion for reversible switching in terms of hydrophilic pattern size and liquid volume. The dependence of the liquid morphology and rupture distance on the diameter and areal fraction of hydrophilic islands, liquid volumes, as well as loading pressure is also characterized both theoretically and experimentally. The thermal resistance in the on-state is experimentally characterized for ionic liquids, which are promising for practical applications due to their negligible vapor pressure. A life testing setup is constructed to evaluate the reliability of the interface under continued switching conditions at relatively high switching frequencies.

  19. Superhydrophobic-like tunable droplet bouncing on slippery liquid interfaces

    NASA Astrophysics Data System (ADS)

    Hao, Chonglei; Wang, Zuankai

    2015-11-01

    Droplet impacting on solid or liquid interfaces is a ubiquitous phenomenon in nature. Although complete rebound of droplets is widely observed on superhydrophobic surfaces, the bouncing of droplets on liquid is usually vulnerable due to easy collapse of entrapped air pocket underneath the impinging droplet. Here, we report a superhydrophobic-like bouncing regime on thin liquid film, characterized by the contact time, the spreading dynamics, and the restitution coefficient independent of underlying liquid film. Through experimental exploration and theoretical analysis, we demonstrate that the manifestation of such a superhydrophobic-like bouncing necessitates an intricate interplay between the Weber number, the thickness and viscosity of liquid film. Such insights allow us to tune the droplet behaviors in a well-controlled fashion. We anticipate that the combination of superhydrophobic-like bouncing with inherent advantages of emerging slippery liquid interfaces will find a wide range of applications.

  20. Superhydrophobic-like tunable droplet bouncing on slippery liquid interfaces

    NASA Astrophysics Data System (ADS)

    Hao, Chonglei; Li, Jing; Liu, Yuan; Zhou, Xiaofeng; Liu, Yahua; Liu, Rong; Che, Lufeng; Zhou, Wenzhong; Sun, Dong; Li, Lawrence; Xu, Lei; Wang, Zuankai

    2015-08-01

    Droplet impacting on solid or liquid interfaces is a ubiquitous phenomenon in nature. Although complete rebound of droplets is widely observed on superhydrophobic surfaces, the bouncing of droplets on liquid is usually vulnerable due to easy collapse of entrapped air pocket underneath the impinging droplet. Here, we report a superhydrophobic-like bouncing regime on thin liquid film, characterized by the contact time, the spreading dynamics, and the restitution coefficient independent of underlying liquid film. Through experimental exploration and theoretical analysis, we demonstrate that the manifestation of such a superhydrophobic-like bouncing necessitates an intricate interplay between the Weber number, the thickness and viscosity of liquid film. Such insights allow us to tune the droplet behaviours in a well-controlled fashion. We anticipate that the combination of superhydrophobic-like bouncing with inherent advantages of emerging slippery liquid interfaces will find a wide range of applications.

  1. Methods and systems for monitoring a solid-liquid interface

    DOEpatents

    Stoddard, Nathan G.; Clark, Roger F.; Kary, Tim

    2010-07-20

    Methods and systems are provided for monitoring a solid-liquid interface, including providing a vessel configured to contain an at least partially melted material; detecting radiation reflected from a surface of a liquid portion of the at least partially melted material that is parallel with the liquid surface; measuring a disturbance on the surface; calculating at least one frequency associated with the disturbance; and determining a thickness of the liquid portion based on the at least one frequency, wherein the thickness is calculated based on.times. ##EQU00001## where g is the gravitational constant, w is the horizontal width of the liquid, and f is the at least one frequency.

  2. Interfacing dielectric elastomer actuators with liquids

    NASA Astrophysics Data System (ADS)

    Poulin, Alexandre; Maffli, Luc; Rosset, Samuel; Shea, Herbert

    2015-04-01

    Methods and materials for liquid encapsulation in thin (19 μm) silicone membranes are presented in this work. A set of 12 liquids including solvents, oils, silicone pre-polymers and one ionic liquid are experimentally tested. We show that all selected liquids are chemically inert to silicone and that vapor pressure is the key parameter for stable encapsulation. It is demonstrated that encapsulated volume of silicone pre-polymers and ionic liquids can stay stable for more than 1 month. The actuation of dielectric elastomer actuators (DEAs) in conductive liquids is also investigated. An analysis of the equivalent electrical circuits of immersed DEAs shows that non-overlapping regions of the electrodes should be minimized. It also provides guidelines to determine when the electrodes should be passivated. The effects of immersion in a conductive liquid are assessed by measuring the actuation strain and capacitance over periodic actuation. The experimental results show no sign of liquid-induced degradation over more than 45k actuation cycles.

  3. Ultrastable Liquid-Liquid Interface as Viable Route for Controlled Deposition of Biodegradable Polymer Nanocapsules.

    PubMed

    Vecchione, Raffaele; Iaccarino, Giulia; Bianchini, Paolo; Marotta, Roberto; D'autilia, Francesca; Quagliariello, Vincenzo; Diaspro, Alberto; Netti, Paolo A

    2016-06-01

    Liquid-liquid interfaces are highly dynamic and characterized by an elevated interfacial tension as compared to solid-liquid interfaces. Therefore, they are gaining an increasing interest as viable templates for ordered assembly of molecules and nanoparticles. However, liquid-liquid interfaces are more difficult to handle compared to solid-liquid interfaces; their intrinsic instability may affect the assembly process, especially in the case of multiple deposition. Indeed, some attempts have been made in the deposition of polymer multilayers at liquid-liquid interfaces, but with limited control over size and stability. This study reports on the preparation of an ultrastable liquid-liquid interface based on an O/W secondary miniemulsion and its possible use as a template for the self-assembly of polymeric multilayer nanocapsules. Such polymer nanocapsules are made of entirely biodegradable materials, with highly controlled size-well under 200 nm-and multi-compartment and multifunctional features enriching their field of application in drug delivery, as well as in other bionanotechnology fields.

  4. Study of a liquid bridge subjected to interface shear stresses

    NASA Astrophysics Data System (ADS)

    Gaponenko, Yu.; Glockner, S.; Mialdun, A.; Shevtsova, V.

    2011-08-01

    We report on numerical and experimental study of two-phase flows in a tall annulus. The geometry corresponds to a cylindrical liquid column co-axially placed into an outer cylinder with solid walls. The internal column consists of solid supports at the bottom and top, while the central part is a liquid zone filled with viscous liquid and kept in its position by surface tension. Gas enters into the annular duct and entrains initially quiescent liquid. The liquid bridge interface is deformed by gravity and by a co-axial gas flow which is co- and counter directed with respect to gravity. A new experimental set-up including an optical system for precise measurements of the interface displacement has been designed and developed. In the experiments silicone oil 5cSt was used as a test liquid and air as gas. On numerical side the dynamical response of an isothermal liquid bridge to a coaxial gas flow is examined by simulations of the Navier-Stokes equations. The attention is focused on the following points: time-dependent formation of the equilibrium shape of a liquid bridge in gravity conditions and its deformation by a gas flow, simulation of a flow pattern in a liquid/gas system with deformed free surface. The comparison of the numerical and experimental results for the interface deformation exhibits a satisfactory agreement.

  5. Nanoparticles at liquid interfaces: rotational dynamics and angular locking.

    PubMed

    Razavi, Sepideh; Kretzschmar, Ilona; Koplik, Joel; Colosqui, Carlos E

    2014-01-07

    Nanoparticles with different surface morphologies that straddle the interface between two immiscible liquids are studied via molecular dynamics simulations. The methodology employed allows us to compute the interfacial free energy at different angular orientations of the nanoparticle. Due to their atomistic nature, the studied nanoparticles present both microscale and macroscale geometrical features and cannot be accurately modeled as a perfectly smooth body (e.g., spheres and cylinders). Under certain physical conditions, microscale features can produce free energy barriers that are much larger than the thermal energy of the surrounding media. The presence of these energy barriers can effectively "lock" the particle at specific angular orientations with respect to the liquid-liquid interface. This work provides new insights on the rotational dynamics of Brownian particles at liquid interfaces and suggests possible strategies to exploit the effects of microscale features with given geometric characteristics.

  6. Nanoparticles at liquid interfaces: Rotational dynamics and angular locking

    SciTech Connect

    Razavi, Sepideh; Kretzschmar, Ilona; Koplik, Joel; Colosqui, Carlos E.

    2014-01-07

    Nanoparticles with different surface morphologies that straddle the interface between two immiscible liquids are studied via molecular dynamics simulations. The methodology employed allows us to compute the interfacial free energy at different angular orientations of the nanoparticle. Due to their atomistic nature, the studied nanoparticles present both microscale and macroscale geometrical features and cannot be accurately modeled as a perfectly smooth body (e.g., spheres and cylinders). Under certain physical conditions, microscale features can produce free energy barriers that are much larger than the thermal energy of the surrounding media. The presence of these energy barriers can effectively “lock” the particle at specific angular orientations with respect to the liquid-liquid interface. This work provides new insights on the rotational dynamics of Brownian particles at liquid interfaces and suggests possible strategies to exploit the effects of microscale features with given geometric characteristics.

  7. Vapor condensation on a turbulent liquid interface

    NASA Technical Reports Server (NTRS)

    Helmick, M. R.; Khoo, B. C.; Sonin, A. A.

    1987-01-01

    An experimental investigation which seeks the fundamental relationship between the interfacial condensation rate and the parameters which control it when the liquid side is turbulent is discussed. The scaling laws for free-surface condensation are discussed for this case. It is argued that the condensation of cryogenic liquids can, in principle, be simulated in experiments using steam and water. Data are presented for the condensation rate in terms of the dimensionless scaling parameters which involve the fluid properties and the liquid-side turbulence velocity and length scales.

  8. Multiple liquid bridges with non-smooth interfaces

    NASA Astrophysics Data System (ADS)

    Fel, Leonid G.; Rubinstein, Boris Y.; Ratner, Vadim

    2016-08-01

    We consider a coexistence of two axisymmetric liquid bridges LB i and LB m of two immiscible liquids i and m which are immersed in a third liquid (or gas) e and trapped between two smooth solid bodies with axisymmetric surfaces S 1, S 2 and free contact lines. Evolution of liquid bridges allows two different configurations of LB i and LB m with multiple (five or three) interfaces of non-smooth shape. We formulate a variational problem with volume constraints and present its governing equations supplemented by boundary conditions. We find a universal relationship between curvature of the interfaces and discuss the Neumann triangle relations at the singular curve where all liquids meet together.

  9. Real Space Imaging of Nanoparticle Assembly at Liquid-Liquid Interfaces with Nanoscale Resolution.

    PubMed

    Costa, Luca; Li-Destri, Giovanni; Thomson, Neil H; Konovalov, Oleg; Pontoni, Diego

    2016-09-14

    Bottom up self-assembly of functional materials at liquid-liquid interfaces has recently emerged as method to design and produce novel two-dimensional (2D) nanostructured membranes and devices with tailored properties. Liquid-liquid interfaces can be seen as a "factory floor" for nanoparticle (NP) self-assembly, because NPs are driven there by a reduction of interfacial energy. Such 2D assembly can be characterized by reciprocal space techniques, namely X-ray and neutron scattering or reflectivity. These techniques have drawbacks, however, as the structural information is averaged over the finite size of the radiation beam and nonperiodic isolated assemblies in 3D or defects may not be easily detected. Real-space in situ imaging methods are more appropriate in this context, but they often suffer from limited resolution and underperform or fail when applied to challenging liquid-liquid interfaces. Here, we study the surfactant-induced assembly of SiO2 nanoparticle monolayers at a water-oil interface using in situ atomic force microscopy (AFM) achieving nanoscale resolved imaging capabilities. Hitherto, AFM imaging has been restricted to solid-liquid interfaces because applications to liquid interfaces have been hindered by their softness and intrinsic dynamics, requiring accurate sample preparation methods and nonconventional AFM operational schemes. Comparing both AFM and grazing incidence X-ray small angle scattering data, we unambiguously demonstrate correlation between real and reciprocal space structure determination showing that the average interfacial NP density is found to vary with surfactant concentration. Additionally, the interaction between the tip and the interface can be exploited to locally determine the acting interfacial interactions. This work opens up the way to studying complex nanostructure formation and phase behavior in a range of liquid-liquid and complex liquid interfaces.

  10. Direct measurements of ionic liquid layering at a single mica-liquid interface and in nano-films between two mica-liquid interfaces.

    PubMed

    Griffin, Lucy R; Browning, Kathryn L; Clarke, Stuart M; Smith, Alexander M; Perkin, Susan; Skoda, M W A; Norman, Sarah E

    2016-12-21

    The layering of ionic liquids close to flat, charged interfaces has been identified previously through theoretical and some experimental measurements. Here we present evidence for oscillations in ion density ('layering') in a long chain ionic liquid (1-decyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide) near the interface with mica using two complementary approaches. Neutron reflection at the ionic liquid-mica interface is used to detect structure at a single interface, and surface force balance (SFB) measurements carried out with the same ionic liquid reveal oscillatory density in the liquid confined between two mica sheets. Our findings imply the interfacial structure is not induced by confinement alone. Structural forces between two mica surfaces extend to approximately twice the distance of the density oscillations measured at a single interface and have similar period in both cases.

  11. Chemical Identification at the Solid-Liquid Interface.

    PubMed

    Söngen, Hagen; Marutschke, Christoph; Spijker, Peter; Holmgren, Eric; Hermes, Ilka; Bechstein, Ralf; Klassen, Stefanie; Tracey, John; Foster, Adam S; Kühnle, Angelika

    2017-01-10

    Solid-liquid interfaces are decisive for a wide range of natural and technological processes, including fields as diverse as geochemistry and environmental science as well as catalysis and corrosion protection. Dynamic atomic force microscopy nowadays provides unparalleled structural insights into solid-liquid interfaces, including the solvation structure above the surface. In contrast, chemical identification of individual interfacial atoms still remains a considerable challenge. So far, an identification of chemically alike atoms in a surface alloy has only been demonstrated under well-controlled ultrahigh vacuum conditions. In liquids, the recent advent of three-dimensional force mapping has opened the potential to discriminate between anionic and cationic surface species. However, a full chemical identification will also include the far more challenging situation of alike interfacial atoms (i.e., with the same net charge). Here we demonstrate the chemical identification capabilities of dynamic atomic force microscopy at solid-liquid interfaces by identifying Ca and Mg cations at the dolomite-water interface. Analyzing site-specific vertical positions of hydration layers and comparing them with molecular dynamics simulations unambiguously unravels the minute but decisive difference in ion hydration and provides a clear means for telling calcium and magnesium ions apart. Our work, thus, demonstrates the chemical identification capabilities of dynamic AFM at the solid-liquid interface.

  12. Energy dispersive-EXAFS of Pd nucleation at a liquid/liquid interface

    NASA Astrophysics Data System (ADS)

    Chang, S.-Y.; Booth, S. G.; Uehara, A.; Mosselmans, J. F. W.; Cibin, G.; Pham, V.-T.; Nataf, L.; Dryfe, R. A. W.; Schroeder, S. L. M.

    2016-05-01

    Energy dispersive extended X-ray absorption fine structure (EDE) has been applied to Pd nanoparticle nucleation at a liquid/liquid interface under control over the interfacial potential and thereby the driving force for nucleation. Preliminary analysis focusing on Pd K edge-step height determination shows that under supersaturated conditions the concentration of Pd near the interface fluctuate over a period of several hours, likely due to the continuous formation and dissolution of sub-critical nuclei. Open circuit potential measurements conducted ex-situ in a liquid/liquid electrochemical cell support this view, showing that the fluctuations in Pd concentration are also visible as variations in potential across the liquid/liquid interface. By decreasing the interfacial potential through inclusion of a common ion (tetraethylammonium, TEA+) the Pd nanoparticle growth rate could be slowed down, resulting in a smooth nucleation process. Eventually, when the TEA+ ions reached an equilibrium potential, Pd nucleation and particle growth were inhibited.

  13. Snap-in of particles at curved liquid interfaces

    NASA Astrophysics Data System (ADS)

    Li, Chao; Moradiafrapoli, Momene; Marston, Jeremy

    2016-11-01

    The contact of particles with liquid interfaces constitutes the first stage in the formation of a particle-laden interface, the so-called "snap-in effect". Here, we report on an experimental study using high-speed video to directly visualize the snap-in process and the approach to the equilibrium state of a particle at a curved liquid interface (i.e. droplet surface). We image the evolution of the contact line, which is found to follow a power-law scaling in time, and the dynamic contact angle during the snap-in. Both hydrophilic and hydrophobic particles are explored and we match the lift-off stage of the particles with a simple force balance. We also explore some multi-particle experiments, eluding to the dynamics of particle-laden interface formation.

  14. Assessing the Plasma-Liquid Interface Using Single Bubble Studies

    NASA Astrophysics Data System (ADS)

    Foster, John; Sagadevan, Athena; Gucker, Sarah

    2014-10-01

    Interaction physics and chemistry between a plasma in contact with liquid water occurs at the interface. Energy transport as well as radical species production occurs in this region. An understanding of the physical processes occurring in this region is key to elucidating the effect that plasma has on water chemistry well beyond the interface. Such an understanding has implications in application areas such as plasma medicine and water purification. Here, we present preliminary results from a 2-D system aimed at elucidating the plasma-liquid interface through the study of the interfacial response under the influence of plasma produced in a single, trapped bubble. The spatial extent and associated reactivity of this active layer associated with the interface region is interrogated with chemical probes and optical imaging. Results from these studies are presented. This work is supported by NSF CBET 1336375.

  15. Enzyme structure and activity at liquid-liquid interfaces

    SciTech Connect

    Beverung, C.J.; Tupy, M.J.; Radke, C.J.; Blanch, H.W.

    1997-12-31

    Understanding the behavior of proteins interaction at oil/water interfaces is crucial to the design of two-phase bioprocesses (aqueous/organic). An examination of the mechanism of protein adsorption at the oil/water interface was undertaken using tensiometry, transmission electron microscopy (TEM) and a novel total internal reflection fluorescence spectrometer (TIRFS), constructed to monitor adsorption dynamics. Dynamic interfacial tension measurements of protein adsorption show three regimes which can be described by diffusion to the interface, adsorption and denaturation of the adsorbed protein. TEM micrographs show a network of proteins in the adsorbed layer at long times. TIRFS data show that this network formation or protein entanglement in the adsorbed state requires a long period of time to occur. A series of two-monomer random polyamino acids used as model proteins demonstrate many of the adsorption characteristics observed for natural proteins.

  16. Particle self-assembly at ionic liquid-based interfaces.

    PubMed

    Frost, Denzil S; Nofen, Elizabeth M; Dai, Lenore L

    2014-04-01

    This review presents an overview of the nature of ionic liquid (IL)-based interfaces and self-assembled particle morphologies of IL-in-water, oil- and water-in-IL, and novel IL-in-IL Pickering emulsions with emphasis on their unique phenomena, by means of experimental and computational studies. In IL-in-water Pickering emulsions, particles formed monolayers at ionic liquid-water interfaces and were close-packed on fully covered emulsion droplets or aggregated on partially covered droplets. Interestingly, other than equilibrating at the ionic liquid-water interfaces, microparticles with certain surface chemistries were extracted into the ionic liquid phase with a high efficiency. These experimental findings were supported by potential of mean force calculations, which showed large energy drops as hydrophobic particles crossed the interface into the IL phase. In the oil- and water-in-IL Pickering emulsions, microparticles with acidic surface chemistries formed monolayer bridges between the internal phase droplets rather than residing at the oil/water-ionic liquid interfaces, a significant deviation from traditional Pickering emulsion morphology. Molecular dynamics simulations revealed aspects of the mechanism behind this bridging phenomenon, including the role of the droplet phase, surface chemistry, and inter-particle film. Novel IL-in-IL Pickering emulsions exhibited an array of self-assembled morphologies including the previously observed particle absorption and bridging phenomena. The appearance of these morphologies depended on the particle surface chemistry as well as the ILs used. The incorporation of particle self-assembly with ionic liquid science allows for new applications at the intersection of these two fields, and have the potential to be numerous due to the tunability of the ionic liquids and particles incorporated, as well as the particle morphology by combining certain groups of particle surface chemistry, IL type (protic or aprotic), and whether oil

  17. Ionic structure in liquids confined by dielectric interfaces

    NASA Astrophysics Data System (ADS)

    Jing, Yufei; Jadhao, Vikram; Zwanikken, Jos W.; Olvera de la Cruz, Monica

    2015-11-01

    The behavior of ions in liquids confined between macromolecules determines the outcome of many nanoscale assembly processes in synthetic and biological materials such as colloidal dispersions, emulsions, hydrogels, DNA, cell membranes, and proteins. Theoretically, the macromolecule-liquid boundary is often modeled as a dielectric interface and an important quantity of interest is the ionic structure in a liquid confined between two such interfaces. The knowledge gleaned from the study of ionic structure in such models can be useful in several industrial applications, such as in the design of double-layer supercapacitors for energy storage and in the extraction of metal ions from wastewater. In this article, we compute the ionic structure in a model system of electrolyte confined by two planar dielectric interfaces using molecular dynamics simulations and liquid state theory. We explore the effects of high electrolyte concentrations, multivalent ions, dielectric contrasts, and external electric field on the ionic distributions. We observe the presence of non-monotonic ionic density profiles leading to a layered structure in the fluid which is attributed to the competition between electrostatic and steric (entropic) interactions. We find that thermal forces that arise from symmetry breaking at the interfaces can have a profound effect on the ionic structure and can oftentimes overwhelm the influence of the dielectric discontinuity. The combined effect of ionic correlations and inhomogeneous dielectric permittivity significantly changes the character of the effective interaction between the two interfaces.

  18. Electrostatic Debye layer formed at a plasma-liquid interface

    NASA Astrophysics Data System (ADS)

    Rumbach, Paul; Clarke, Jean Pierre; Go, David B.

    2017-05-01

    We construct an analytic model for the electrostatic Debye layer formed at a plasma-liquid interface by combining the Gouy-Chapman theory for the liquid with a simple parabolic band model for the plasma sheath. The model predicts a nonlinear scaling between the plasma current density and the solution ionic strength, and we confirmed this behavior with measurements using a liquid-anode plasma. Plots of the measured current density as a function of ionic strength collapse the data and curve fits yield a plasma electron density of ˜1019m-3 and an electric field of ˜104V /m on the liquid side of the interface. Because our theory is based firmly on fundamental physics, we believe it can be widely applied to many emerging technologies involving the interaction of low-temperature, nonequilibrium plasma with aqueous media, including plasma medicine and various plasma chemical synthesis techniques.

  19. Liquid-vapor interface of a polydisperse fluid.

    PubMed

    Buzzacchi, Matteo; Wilding, Nigel B

    2005-06-01

    We report a grand canonical Monte Carlo simulation study of the liquid-vapor interface of a model fluid exhibiting polydispersity in terms of the particle size sigma. The bulk density distribution, rho0(sigma), of the system is controlled by the imposed chemical potential distribution mu(sigma), the form of which is specified such that rho0(sigma) assumes a Schulz form with associated degree of polydispersity approximately = 14%. By introducing a smooth attractive wall, a planar liquid-vapor interface is formed for bulk state points within the region of liquid-vapor coexistence. Owing to fractionation, the pure liquid phase is enriched in large particles, with respect to the coexisting vapor. We investigate how the spatial variation of the density near the liquid-vapor interface affects the evolution of the local distribution of particle sizes between the limiting pure phase forms. We find [as previously predicted by density-functional theory, Bellier-Castella, Phys. Rev. E 65, 021503 (2002)] a segregation of smaller particles to the interface. The magnitude of this effect as a function of sigma is quantified via measurements of the relative adsorption. Additionally, we consider the utility of various estimators for the interfacial width and highlight the difficulty of isolating the intrinsic contribution of polydispersity to this width.

  20. Surface potential of the water liquid-vapor interface

    NASA Technical Reports Server (NTRS)

    Wilson, Michael A.; Pohorille, Andrew; Pratt, Lawrence R.

    1988-01-01

    An analysis of an extended molecular dynamics calculation of the surface potential (SP) of the water liquid-vapor interface is presented. The SP predicted by the TIP4P model is -(130 + or - 50) mV. This value is of reasonable magnitude but of opposite sign to the expectations based on laboratory experiments. The electrostatic potential shows a nonmonotonic variation with depth into the liquid.

  1. Universal fluctuations of growing interfaces: evidence in turbulent liquid crystals.

    PubMed

    Takeuchi, Kazumasa A; Sano, Masaki

    2010-06-11

    We investigate growing interfaces of topological-defect turbulence in the electroconvection of nematic liquid crystals. The interfaces exhibit self-affine roughening characterized by both spatial and temporal scaling laws of the Kardar-Parisi-Zhang theory in 1+1 dimensions. Moreover, we reveal that the distribution and the two-point correlation of the interface fluctuations are universal ones governed by the largest eigenvalue of random matrices. This provides quantitative experimental evidence of the universality prescribing detailed information of scale-invariant fluctuations.

  2. Slip length of confined liquid with small roughness of solid-liquid interfaces

    NASA Astrophysics Data System (ADS)

    Wan, Li; Huang, Yunmi

    2017-04-01

    We have studied the slip length of confined liquid with small roughness of solid-liquid interfaces. Dyadic Green function and perturbation expansion have been applied to get the slip length quantitatively. In the slip length, both the effects of the roughness of the interfaces and the chemical interaction between the liquid and the solid surface are involved. For the numerical calculation, Monte Carlo method has been used to simulate the rough interfaces and the physical quantities are obtained statistically over the interfaces. Results show that the total slip length of the system is linearly proportional to the slip length contributed from the chemical interaction. And the roughness of the interfaces plays its role as the proportionality factor. For the roughness, the variance of the roughness decreases the total slip length while the correlation length of the roughness can enhance the slip length dramatically to a saturation value.

  3. Slip length of confined liquid with small roughness of solid-liquid interfaces.

    PubMed

    Wan, Li; Huang, Yunmi

    2017-04-01

    We have studied the slip length of confined liquid with small roughness of solid-liquid interfaces. Dyadic Green function and perturbation expansion have been applied to get the slip length quantitatively. In the slip length, both the effects of the roughness of the interfaces and the chemical interaction between the liquid and the solid surface are involved. For the numerical calculation, Monte Carlo method has been used to simulate the rough interfaces and the physical quantities are obtained statistically over the interfaces. Results show that the total slip length of the system is linearly proportional to the slip length contributed from the chemical interaction. And the roughness of the interfaces plays its role as the proportionality factor. For the roughness, the variance of the roughness decreases the total slip length while the correlation length of the roughness can enhance the slip length dramatically to a saturation value.

  4. Charge-Controlled Colloids on Liquid-Liquid Interfaces

    NASA Astrophysics Data System (ADS)

    Kunz, Daniel A.; Reck, Bernd; Manoharan, Vinothan N.

    2014-03-01

    The tendency of colloidal particles to stabilize interfaces has been exploited for many years to generate Pickering emulsions with a variety of industrial applications. However, the exact stabilization mechanism and its dependence on the surface properties of the colloidal particles are not yet fully understood. We provide new interfacial studies on the nonequilibrium dynamics of a colloidal system with tunable surface charge density. We push individual sub-micron colloidal particles towards an oil-water interface and track their motion in three-dimensions using holographic microscopy to examine the influence of zeta potential on the dynamics of the system. This project was funded by the BASF Advanced Research Initiative, BASF SE, Germany.

  5. Investigation of Compact Layers at a Liquid/Liquid Interface

    DTIC Science & Technology

    1993-04-27

    Special 2 . i iI II Citation List (PART I) b. Papers published in refereed journals: Bruckner-Lea, C.; Janata, J.; Conroy, J.; Pungor , A. and Caldwell...Bruckner-Lea, C.; Conroy, J.; Pungor , A.; and Caldwell, K. "Scanning Tuneling Microscopy on a Compressible Mercury Sessile Drop", in ACS Series...Chemically Sensitive Interfaces, 1994. h. Invited presentation: Janata, J.; Bruckner-Lea, C.; Conroy, J.; Pungor , A. and Caldwell, K. "Molecular Vise

  6. Measuring the optical chirality of molecular aggregates at liquid-liquid interfaces.

    PubMed

    Watarai, Hitoshi; Adachi, Kenta

    2009-10-01

    Some new experimental methods for measuring the optical chirality of molecular aggregates formed at liquid-liquid interfaces have been reviewed. Chirality measurements of interfacial aggregates are highly important not only in analytical spectroscopy but also in biochemistry and surface nanochemistry. Among these methods, a centrifugal liquid membrane method was shown to be a highly versatile method for measuring the optical chirality of the liquid-liquid interface when used in combination with a commercially available circular dichroism (CD) spectropolarimeter, provided that the interfacial aggregate exhibited a large molar absorptivity. Therefore, porphyrin and phthalocyanine were used as chromophoric probes of the chirality of itself or guest molecules at the interface. A microscopic CD method was also demonstrated for the measurement of a small region of a film or a sheet sample. In addition, second-harmonic generation and Raman scattering methods were reviewed as promising methods for detecting interfacial optical molecules and measuring bond distortions of chiral molecules, respectively.

  7. Laser triangulation for liquid film thickness measurements through multiple interfaces.

    PubMed

    Peterson, Jerrod P; Peterson, Richard B

    2006-07-10

    Laser triangulation is used to measure the thickness of a liquid film in a test section consisting of a quartz viewing window, a water layer, and a hydrophobic membrane. The triangulation sensor acquires measurements to the bounding surfaces of the film while peering through multiple interfaces. This allows the difference between the two measurements to constitute the local film thickness. A refraction model is developed and applied to the analysis of data collected from the experiment. For verification, an empirical method is also developed and compared to the analytical approach. The measurement technique is intended to assess the stability of liquid films for use as gas-liquid contactors.

  8. Molecular structure of the coalescence of liquid interfaces

    NASA Technical Reports Server (NTRS)

    Koplik, Joel; Banavar, Jayanth R.

    1992-01-01

    When two bodies of liquid merge, their interfaces must also rupture and rearrange into one. Virtually no information is available concerning the small-scale dynamics of this process. Molecular dynamics simulations of coalescence in systems of about 10,000 Lennard-Jones particles have been performed, arranged so as to mimic laboratory experiments on dense liquids. The coalescence event begins when molecules near the boundary of one liquid body thermally fluctuate into the range of attraction of the other, forming a string of mutually attracting molecules. These molecules gradually thicken into a tendril, which continues to thicken as the bodies smoothly combine in a zipper-like merger.

  9. Molecular structure of the coalescence of liquid interfaces

    NASA Technical Reports Server (NTRS)

    Koplik, Joel; Banavar, Jayanth R.

    1992-01-01

    When two bodies of liquid merge, their interfaces must also rupture and rearrange into one. Virtually no information is available concerning the small-scale dynamics of this process. Molecular dynamics simulations of coalescence in systems of about 10,000 Lennard-Jones particles have been performed, arranged so as to mimic laboratory experiments on dense liquids. The coalescence event begins when molecules near the boundary of one liquid body thermally fluctuate into the range of attraction of the other, forming a string of mutually attracting molecules. These molecules gradually thicken into a tendril, which continues to thicken as the bodies smoothly combine in a zipper-like merger.

  10. LIQUID AIR INTERFACE CORROSION TESTING FOR FY2010

    SciTech Connect

    Zapp, P.

    2010-12-16

    An experimental study was undertaken to investigate the corrosivity to carbon steel of the liquid-air interface of dilute simulated radioactive waste solutions. Open-circuit potentials were measured on ASTM A537 carbon steel specimens located slightly above, at, and below the liquid-air interface of simulated waste solutions. The 0.12-inch-diameter specimens used in the study were sized to respond to the assumed distinctive chemical environment of the liquid-air interface, where localized corrosion in poorly inhibited solutions may frequently be observed. The practical inhibition of such localized corrosion in liquid radioactive waste storage tanks is based on empirical testing and a model of a liquid-air interface environment that is made more corrosive than the underlying bulk liquid due to chemical changes brought about by absorbed atmospheric carbon dioxide. The chemical changes were assumed to create a more corrosive open-circuit potential in carbon in contact with the liquid-air interface. Arrays of 4 small specimens spaced about 0.3 in. apart were partially immersed so that one specimen contacted the top of the meniscus of the test solution. Two specimens contacted the bulk liquid below the meniscus and one specimen was positioned in the vapor space above the meniscus. Measurements were carried out for up to 16 hours to ensure steady-state had been obtained. The results showed that there was no significant difference in open-circuit potentials between the meniscus-contact specimens and the bulk-liquid-contact specimens. With the measurement technique employed, no difference was detected between the electrochemical conditions of the meniscus versus the bulk liquid. Stable open-circuit potentials were measured on the specimen located in the vapor space above the meniscus, showing that there existed an electrochemical connection through a thin film of solution extending up from the meniscus. This observation supports the Hobbs-Wallace model of the development

  11. Liquid-Vapor Interface Configurations Investigated in Low Gravity

    NASA Technical Reports Server (NTRS)

    Concus, Paul; Finn, Robert; Weislogel, Mark M.

    1998-01-01

    The Interface Configuration Experiment (ICE) is part of a multifaceted study that is exploring the often striking behavior of liquid-vapor interfaces in low-gravity environments. Although the experiment was posed largely as a test of current mathematical theory, applications of the results should be manifold. In space almost every fluid system is affected, if not dominated, by capillarity (the effects of surface tension). As a result, knowledge of fluid interface behavior, in particular an equilibrium interface shape from which any analysis must begin, is fundamental--from the control of liquid fuels and oxygen in storage tanks to the design and development of inspace thermal systems, such as heat pipes and capillary pumped loops. ICE has increased, and should continue to increase, such knowledge as it probes the specific peculiarities of current theory upon which our present understanding rests. Several versions of ICE have been conducted in the drop towers at the NASA Lewis Research Center, on the space shuttles during the first and second United States Microgravity Laboratory missions (USML-1 and USML-2), and most recently aboard the Russian Mir space station. These studies focused on interfacial problems concerning the existence, uniqueness, configuration, stability, and flow characteristics of liquid-vapor interfaces. Results to date have clearly demonstrated the value of the present theory and the extent to which it can predict the behavior of capillary systems.

  12. Near Axisymmetric Partial Wetting Using Interface-Localized Liquid Dielectrophoresis.

    PubMed

    Brabcova, Zuzana; McHale, Glen; Wells, Gary George; Brown, Carl V; Newton, Michael Ian; Edwards, Andrew M J

    2016-10-03

    The wetting of solid surfaces can be modified by altering the surface free energy balance between the solid, liquid, and vapour phases. Liquid dielectrophoresis (L-DEP) can produce wetting on normally non-wetting surfaces, without modification of the surface topography or chemistry. L-DEP is a bulk force acting on the dipoles of a dielectric liquid and is not normally considered to be a localized effect acting at the interface between the liquid and a solid or other fluid. However, if this force is induced by a non-uniform electric field across a solid-liquid interface, it can be used to enhance and control the wetting of a dielectric liquid. Recently, it was reported theoretically and experimentally that this approach can cause a droplet of oil to spread along parallel interdigitated electrodes thus forming a stripe of liquid. Here we show that by using spiral shaped electrodes actuated with four 90º successive phase shifted signals, a near axisymmetric spreading of droplets can be achieved. Experimental observations show that the induced wetting can achieve film formation, an effect not possible with electrowetting. We show that the spreading is reversible thus enabling a wide range of partial wetting droplet states to be achieved in a controllable manner. Furthermore, we find that the cosine of the contact angle has a quadratic dependence on applied voltage during spreading and deduce a scaling law for the dependence of the strength of the effect on the electrode size. .

  13. Hydrodynamical entrapment of ciliates at the air-liquid interface

    NASA Astrophysics Data System (ADS)

    Ferracci, Jonathan; Ueno, Hironori; Numayama-Tsuruta, Keiko; Imai, Yohsuke; Yamaguchi, Takami; Ishikawa, Takuji

    2012-11-01

    We found the new phenomenon of the entrapment of ciliates at the air-water interface, though they are not trapped by a solid interface. We first characterize the behaviours of cells at the interface by comparing it to those away from interfaces. The results showed that the cell's swimming velocity is considerably reduced at the air-water interface. In order to experimentally verify the possible physiological causes of the entrapment, we observed their behaviours in absence of positive chemotaxis for oxygen and the negative geotaxis. The results illustrated that the entrapment phenomenon was not dependent on these physiological conditions. The experiments using surfactant revealed that the entrapment phenomenon was strongly affected by the velocity-stress conditions at the interface. This fact was confirmed numerically by a boundary element method, i.e. the stress-free condition at the air-liquid interface is one of the main mechanisms of the entrapment phenomenon found in the experiments. Since the entrapment phenomenon found in this study affects the cell-cell interactions and the mass transport at the interface, the knowledge obtained in this study is useful for better understanding the complex behaviours of swimming microorganisms in nature. PhD student in the Physiological Flow Studies Laboratory.

  14. Experiments on the impact and turbulent coalescence of a blob at a liquid-liquid interface

    NASA Astrophysics Data System (ADS)

    Landeau, Maylis; Olson, Peter; Deguen, Renaud; Hirsh, Ben; Earth; Planetary Sciences Team

    2015-11-01

    We present experiments on finite liquid volumes, hereafter referred to as blobs, of variable densities impacting an interface between two immiscible liquids at high Reynolds and Weber numbers. Such processes occurred on a massive scale during the giant impacts that formed terrestrial planets and satellites, including the Earth and the Moon. We find that the fall distance of the blob controls an abrupt transition in coalescence regime and in the amount of mixing with the lower liquid. This transition coincides with a brief and global breakup of the impacting blob into drops. For small fall distances, the large-scale flow following impact behaves as a turbulent fountain: a mixture of immiscible liquids penetrates in the lower liquid, collapses and spreads along the immiscible interface. We derive an experimental scaling relation for turbulent mixing of the impacting blob with the lower liquid as a function of a Richardson number.

  15. Interfaces Select Specific Stereochemical Conformations: The Isomerization of Glyoxal at the Liquid Water Interface.

    PubMed

    Zhu, Chongqin; Kais, Sabre; Zeng, Xiao Cheng; Francisco, Joseph S; Gladich, Ivan

    2017-01-11

    Interfacial chemistry involving glyoxal at aerosol surfaces is postulated to catalyze aerosol growth. This chemistry remains speculative due to a lack of detailed information concerning the physicochemical behavior of glyoxal at the interface of atmospheric aerosols. Here, we report results from high-level electronic structure calculations as well as both classical and Born-Oppenheimer ab initio molecular dynamics simulations of glyoxal solvation at the air/liquid water interface. When compared to the gas phase, the trans to cis isomerization of glyoxal at the liquid water interface is found to be catalyzed; additionally, the trans conformation is selectively solvated within the bulk to a greater degree than is the cis conformation. These two processes, i.e., the catalytic effect at the water interface and the differentially selective solvation, act to enhance the concentration of the cis isomer of glyoxal at the water interface. This has important consequences for the interpretation of experiments and for the modeling of glyoxal chemistry both at the interface of water clouds and at aerosols. Broader implications of this work relate to describing the role of interfaces in selecting specific stereo molecular structures at interfacial environments.

  16. Relaxation of surface tension in the liquid-solid interfaces of Lennard-Jones liquids.

    PubMed

    Lukyanov, Alex V; Likhtman, Alexei E

    2013-11-19

    We have established the surface tension relaxation time in the liquid-solid interfaces of Lennard-Jones (LJ) liquids by means of direct measurements in molecular dynamics (MD) simulations. The main result is that the relaxation time is found to be almost independent of the molecular structures and viscosity of the liquids (at 70-fold change) used in our study and lies in such a range that in slow hydrodynamic motion the interfaces are expected to be at equilibrium. The implications of our results for the modeling of dynamic wetting processes and interpretation of dynamic contact angle data are discussed.

  17. Nonlinear vibrational spectroscopy of surfactants at liquid interfaces

    SciTech Connect

    Miranda, Paulo B.

    1998-12-14

    Surfactants are widely used to modify physical and chemical properties of interfaces. They play an important role in many technological problems. Surfactant monolayer are also of great scientific interest because they are two-dimensional systems that may exhibit a very rich phase transition behavior and can also be considered as a model system for biological interfaces. In this Thesis, we use a second-order nonlinear optical technique (Sum-Frequency Generation - SFG) to obtain vibrational spectra of surfactant monolayer at Iiquidhapor and solid/liquid interfaces. The technique has several advantages: it is intrinsically surface-specific, can be applied to buried interfaces, has submonolayer sensitivity and is remarkably sensitive to the confirmational order of surfactant monolayers.

  18. Spatial scanning spectroelectrochemistry. Study of the electrodeposition of Pd nanoparticles at the liquid/liquid interface.

    PubMed

    Izquierdo, Daniel; Martinez, Alberto; Heras, Aranzazu; Lopez-Palacios, Jesus; Ruiz, Virginia; Dryfe, Robert A W; Colina, Alvaro

    2012-07-03

    Spatial scanning spectroelectrochemistry is a new analytical technique that provides spectral information at different distances from an electrified liquid/liquid interface where an electrochemical process takes place. As a proof of concept, we have studied two different electrochemical processes at the electrified liquid/liquid interface: (1) Ru(bpy)(3)(2+) transfer through the water/1,2-dichloroethane interface and (2) electrodeposition of Pd nanoparticles at the water/1,2-dichloroethane interface. The instrumental setup developed consists of a movable slit for the light beam to sample at well-defined positions on both sides of the interface, providing important information about the chemical process occurring. If the slit is scanned at different distances from the interface during an electrochemical experiment, a complete picture of the reactions and equilibria in the diffusion layer can be obtained. For example, in the case of the Ru(bpy)(3)(2+), the experiments show clearly how the complex is transferred from one phase to the other. In the case of electrosynthesis of Pd nanoparticles, it is demonstrated that nanoparticles are not only deposited at the interface but diffuse to the aqueous bulk solution. These in situ observations were confirmed by ex situ experiments using transmission electron microscopy.

  19. A moving mesh interface tracking method for simulation of liquid-liquid systems

    NASA Astrophysics Data System (ADS)

    Charin, A. H. L. M.; Tuković, Ž.; Jasak, H.; Silva, L. F. L. R.; Lage, P. L. C.

    2017-04-01

    This manuscript presents a moving mesh interface tracking procedure, with a novel treatment for phase coupling. The new coupling strategy allows accurate predictions for the interface behaviour in a wide range of macroscopic properties with great potential to explore liquid-liquid systems. In this approach, governing equations are applied to each phase individually while the interface is represented by a zero-thickness surface that contemplates inter-phase jumps. These equations are described in an arbitrary Lagrangian-Eulerian finite volume framework. Computations consider the pressure-corrector PISO method. The new treatment for phase coupling incorporates the interfacial jump updates within the pressure/velocity calculations. Additionally, cell-centred values from both phases are considered when calculating convective and diffusive terms at the interface. The employment of GGI (Generalized Grid-Interface) interpolation provides conservative data mapping between surfaces for non-conformal meshes. The prediction capability of the new formulation is evaluated under different dominant effects governing interface motion. Simulated cases include gravity and capillary waves in a sloshing tank, three-dimensional drop oscillation for liquid-liquid systems and drop deformation due to shear flow. The numerical results show good agreement with analytical transient profiles of interface position. The procedure is able to successfully represent systems with similar macroscopic properties, i.e. density and viscosity ratios approaching unity, and a broad range of interfacial tensions.

  20. Quantitative prediction of the position and orientation for an octahedral nanoparticle at liquid/liquid interfaces.

    PubMed

    Shi, Wenxiong; Lee, Yih Hong; Ling, Xing Yi; Li, Shuzhou

    2017-08-10

    Shape-controlled polyhedral particles and their assembled structures have important applications in plasmonics and biosensing, but the interfacial configurations that will critically determine their resultant assembled structures are not well-understood. Hence, a reliable theory is desirable to predict the position and orientation of a polyhedron at the vicinity of a liquid/liquid interface. Here we demonstrate that the free energy change theory can quantitatively predict the position and orientation of an isolated octahedral nanoparticle at a liquid/liquid interface, whose vertices and facets can play crucial roles in biosensing. We focus on two limiting orientations of an octahedral nanoparticle, vertex up and facet up. Our proposed theory indicates that the surface wettability (hydrophilic/hydrophobic ratio) of the nanoparticle determines its most stable position and the preferred orientation at a water/oil interface. The surface wettability of an octahedron is adjusted from extremely hydrophobic to extremely hydrophilic by changing the amount of charge on the Ag surface in molecular dynamics (MD) simulations. The MD simulations results are in excellent agreement with our theoretical prediction for an Ag octahedral nanoparticle at a hexane/water interface. Our proposed theory bridges the gap between molecular-level simulations and equilibrium configurations of polyhedral nanoparticles in experiments, where insights from nanoparticle intrinsic wettability details can be used to predict macroscopic superlattice formation experimentally. This work advances our ability to precisely predict the final structures of the polyhedral nanoparticle assemblies at a liquid/liquid interface.

  1. Crystalline Graphdiyne Nanosheets Produced at a Gas/Liquid or Liquid/Liquid Interface.

    PubMed

    Matsuoka, Ryota; Sakamoto, Ryota; Hoshiko, Ken; Sasaki, Sono; Masunaga, Hiroyasu; Nagashio, Kosuke; Nishihara, Hiroshi

    2017-02-15

    Synthetic two-dimensional polymers, or bottom-up nanosheets, are ultrathin polymeric frameworks with in-plane periodicity. They can be synthesized in a direct, bottom-up fashion using atomic, ionic, or molecular components. However, few are based on carbon-carbon bond formation, which means that there is a potential new field of investigation into these fundamentally important chemical bonds. Here, we describe the bottom-up synthesis of all-carbon, π-conjugated graphdiyne nanosheets. A liquid/liquid interfacial protocol involves layering a dichloromethane solution of hexaethynylbenzene on an aqueous layer containing a copper catalyst at room temperature. A multilayer graphdiyne (thickness, 24 nm; domain size, >25 μm) emerges through a successive alkyne-alkyne homocoupling reaction at the interface. A gas/liquid interfacial synthesis is more successful. Sprinkling a very small amount of hexaethynylbenzene in a mixture of dichloromethane and toluene onto the surface of the aqueous phase at room temperature generated single-crystalline graphdiyne nanosheets, which feature regular hexagonal domains, a lower degree of oxygenation, and uniform thickness (3.0 nm) and lateral size (1.5 μm).

  2. Particles adsorbed at various non-aqueous liquid-liquid interfaces.

    PubMed

    Fernandez-Rodriguez, Miguel Angel; Binks, Bernard P; Rodriguez-Valverde, Miguel Angel; Cabrerizo-Vilchez, Miguel Angel; Hidalgo-Alvarez, Roque

    2017-02-07

    Particles adsorbed at liquid interfaces are commonly used to stabilise water-oil Pickering emulsions and water-air foams. The fundamental understanding of the physics of particles adsorbed at water-air and water-oil interfaces is improving significantly due to novel techniques that enable the measurement of the contact angle of individual particles at a given interface. The case of non-aqueous interfaces and emulsions is less studied in the literature. Non-aqueous liquid-liquid interfaces in which water is replaced by other polar solvents have properties similar to those of water-oil interfaces. Nanocomposites of non-aqueous immiscible polymer blends containing inorganic particles at the interface are of great interest industrially and consequently more work has been devoted to them. By contrast, the behaviour of particles adsorbed at oil-oil interfaces in which both oils are immiscible and of low dielectric constant (ε<3) is scarcely studied. Hydrophobic particles are required to stabilise these oil-oil emulsions due to their irreversible adsorption, high interfacial activity and elastic shell behaviour.

  3. Emulsification at the Liquid/Liquid Interface: Effects of Potential, Electrolytes and Surfactants.

    PubMed

    Chowdhury, Mehrin; Kataky, Ritu

    2016-01-04

    Emulsification of oils at liquid/liquid interfaces is of fundamental importance across a range of applications, including detergency. Adsorption and partitioning of the anionic surface active ions at the interface between two immiscible solutions is known to cause predictable chaos at the transfer potential region of the surfactant. In this work, the phenomenon that leads to the chaotic behaviour shown by sodium dodecylbenzene sulfonate (SDBS) at the water/1,2-dichloroethane interface is applied to commercial surfactants and aqueous/glyceryl trioleate interface. Electrochemical methods, electrocapillary curves, optical microscopy and conductivity measurements demonstrated that at 1.5 mm of SDBS, surfactants are adsorbed at the interface and assemble into micelles, leading to interfacial instability. As the concentration of the anionic surfactant was enhanced to 8 and 13.4 mm, the Marangoni effect and the interfacial emulsification became more prominent. The chaotic behaviour was found to be dependent on the surfactant concentration and the electrolytes present.

  4. Final Report: Thermal Conductance of Solid-Liquid Interfaces

    SciTech Connect

    Cahil, David, G.; Braun, Paul, V.

    2006-05-31

    Research supported by this grant has significantly advanced fundamental understanding of the thermal conductance of solid-liquid interfaces, and the thermal conductivity of nanofluids and nanoscale composite materials. • The thermal conductance of interfaces between carbon nanotubes and a surrounding matrix of organic molecules is exceptionally small and this small value of the interface conductance limits the enhancement in thermal conductivity that can be achieved by loading a fluid or a polymer with nanotubes. • The thermal conductance of interfaces between metal nanoparticles coated with hydrophilic surfactants and water is relatively high and surprisingly independent of the details of the chemical structure of the surfactant. • We extended our experimental methods to enable studies of planar interfaces between surfactant-coated metals and water where the chemical functionalization can be varied between strongly hydrophobic and strongly hydrophilic. The thermal conductance of hydrophobic interfaces establishes an upper-limit of 0.25 nm on the thickness of the vapor-layer that is often proposed to exist at hydrophobic interfaces. • Our high-precision measurements of fluid suspensions show that the thermal conductivity of fluids is not significantly enhanced by loading with a small volume fraction of spherical nanoparticles. These experimental results directly contradict some of the anomalous results in the recent literature and also rule-out proposed mechanisms for the enhanced thermal conductivity of nanofluids that are based on modification of the fluid thermal conductivity by the coupling of fluid motion and the Brownian motion of the nanoparticles.

  5. Controlled Pattern Formation in Carbon Nanotube Arrays Using Liquid Interfaces

    NASA Astrophysics Data System (ADS)

    Sansom, Elijah; Noca, Flavio; Zhou, Jijie; Trevino, Lydia; Gharib, Morteza

    2004-11-01

    Thin liquid films undergoing evaporation and dewetting are subject to instabilities and film breakup. Such films may potentially be used to pattern small particles, even nanometer size ones. This possibility is investigated by studying drying liquid films within mats of vertically oriented carbon nanotubes while varying experimental conditions. Liquids of different surfactant concentration, surface tension, wettability, and viscosity are used while simultaneously varying evaporation rates. Rearrangements of the carbon nanotubes into interesting and perhaps useful patterns of uniformly distributed holes are produced, and controllability of these patterns is demonstrated. Lateral capillary forces acting on the partially immersed carbon nanotubes at the liquid interface and dewetting instabilities inherent in the film are the apparent cause of these patterns. Simple, controlled pattern formation is highly desirable in production of carbon nanotube devices as well as other nanoparticle systems.

  6. Vibration-Induced Gas-Liquid Interface Breakup

    NASA Astrophysics Data System (ADS)

    O'Hern, Timothy; Torczynski, John; Romero, Ed; Shelden, Bion

    2010-11-01

    Gas-liquid interfaces can be forced to break up when subjected to vibrations within critical ranges of frequency and amplitude. This breakup mechanism was examined experimentally using deep layers of silicone oils over a range of viscosity and sinusoidal, primarily axial vibration conditions that can produce dramatic disturbances at the gas-liquid free surface. Although small-amplitude vibrations produce standing Faraday waves, large-amplitude vibrations produce liquid jets into the gas, droplets pinching off from the jets, gas cavities in the liquid from droplet impact, and bubble transport below the interface. Experiments used several different silicone oils over a range of pressures and vibration conditions. Computational simulations exhibiting similar behavior will be included in the presentation. Applications include liquid fuel rockets, inertial sensing devices, moving vehicles, mixing processes, and acoustic excitation. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.

  7. Pressurization of a Flightweight, Liquid Hydrogen Tank: Evaporation & Condensation at a Liquid/Vapor Interface

    NASA Technical Reports Server (NTRS)

    Stewart, Mark E. M.

    2017-01-01

    This paper presents an analysis and simulation of evaporation and condensation at a motionless liquid/vapor interface. A 1-D model equation, emphasizing heat and mass transfer at the interface, is solved in two ways, and incorporated into a subgrid interface model within a CFD simulation. Simulation predictions are compared with experimental data from the CPST Engineering Design Unit tank, a cryogenic fluid management test tank in 1-g. The numerical challenge here is the physics of the liquid/vapor interface; pressurizing the ullage heats it by several degrees, and sets up an interfacial temperature gradient that transfers heat to the liquid phase-the rate limiting step of condensation is heat conducted through the liquid and vapor. This physics occurs in thin thermal layers O(1 mm) on either side of the interface which is resolved by the subgrid interface model. An accommodation coefficient of 1.0 is used in the simulations which is consistent with theory and measurements. This model is predictive of evaporation/condensation rates, that is, there is no parameter tuning.

  8. Hydrogen-bonding molecular ruler surfactants as probes of specific solvation at liquid/liquid interfaces.

    PubMed

    Siler, A Renee; Brindza, Michael R; Walker, Robert A

    2009-10-01

    Resonance-enhanced, second harmonic generation (SHG) is used to measure the electronic structure of solutes sensitive to specific solvation adsorbed to liquid/liquid and liquid/solid interfaces. Here, specific solvation refers to solvent-solute interactions that are directional and localized. N-methyl-p-methoxyaniline (NMMA) is a solute whose first allowed electronic transition wavelength remains almost constant (approximately 315 nm) in non-hydrogen-bonding solvents regardless of solvent polarity. However, in hydrogen-bond-accepting solvents such as dimethylsulfoxide, NMMA's absorbance shifts to longer wavelengths (320 nm), whereas in hydrogen-bond-donating solvents (e.g., water), the absorbance shifts to shorter wavelengths (approximately 300 nm). SHG experiments show that at alkane/silica interfaces, surface silanol groups serve as moderately strong hydrogen-bond donors as evidenced by NMMA's absorbance of 307 nm. At the carbon tetrachloride/water interface, NMMA absorbance also shifts to slightly shorter wavelengths (298 nm) implying that water molecules at this liquid/liquid interface are donating strong hydrogen bonds to the adsorbed NMMA solutes. In contrast, experiments using newly developed molecular ruler surfactants with NMMA as a model hydrophobic solute and a hydrophilic, cationic headgroup imply that, as NMMA migrates across an aqueous/alkane interface, it carries with it water that functions as a hydrogen-bond-accepting partner.

  9. Colloidal Particles and Liquid Interfaces: A Spectrum of Interactions

    NASA Astrophysics Data System (ADS)

    Kaz, David Martin

    Young's law predicts that a colloidal sphere in equilibrium with a liquid interface will straddle the two fluids, its height above the interface defined by an equilibrium contact angle. This equilibrium analysis has been used to explain why colloids often bind to liquid interfaces, an effect first observed a century ago by Ramsden and Pickering and later exploited in a wide range of material processes, including emulsification, water purification, mineral recovery, encapsulation, and the making of nanostructured materials. But little is known about the dynamics of binding, or any aspect of the interaction between a particle and an interface outside of equilibrium. This thesis explores the spectrum of particle-interface interactions, from non-binding to non-adsorptive binding and finally adsorptive binding and the relaxation toward equilibrium that ensues. Chapter 2 reviews the importance of interfacial particles in materials science, and serves as a partial motivation for the work presented here. Chapter 3 describes the apparatus and experimental procedures employed in the acquisition of our data, with a short review of experiments that led to the current set. Special attention is paid to the optical apparatus and the custom sample cells we designed. Chapter 4 deals with non-adsorptive interactions between colloidal particles and liquid interfaces. A theoretical discussion founded on (but not wedded to) classical DLVO theory is presented before the results of our experiments are analyzed. It is shown that particle-interface interactions may be purely repulsive or contain an attractive component that results in binding to the interface that is not associated with breach. In chapter 5 the adsorption of polystyrene microspheres to a water-oil interface is shown to be characterized by a sudden breach and an unexpectedly slow relaxation. Particles do not reach equilibrium even after 100 seconds, and the relaxation appears logarithmic in time, suggesting that complete

  10. Nanoscale thermal transport at solid-liquid interfaces

    NASA Astrophysics Data System (ADS)

    Ge, Zhenbin

    This thesis focuses on the experimental study of nanoscale thermal transport across solidliquid interfaces in both nanoparticle system and planar thin film system. Thermal conductance of solid-liquid interfaces, G, will be measured using time-domain thermo-reflectance and pump-probe transient absorption. Interface thermal conductance, G, relates the temperature drop DeltaT at an interface to the flux of heat F that crosses the interface, F = GDeltaT. In nanoparticle systems, using pump-probe transient absorption measurement, we find that nanoparticles, ranging in size from 3-24 rim. with widely varying hydrophilic surface chemistry, give thermal conductances G ˜ 100-300 MW m-2 K-1 for the particle-water interfaces, approximately an order of magnitude larger than the conductance of the interfaces between alkanethiol-terminated AuPd nanoparticles and toluene. The relatively large thermal conductances between particle-water interfaces indicate that the thermal coupling between hydrophilic nanoparticles and water is strong regardless of the self-assembled stabilizing group. In planar systems, using time-domain thermoreflectance, we find that the thermal conductance between water and planar hydrophilic surfaces ranges between 100 and 180 MW m-2 K-1, which is in good agreement with the nanoparticles systems. While in hydrophobic-water interfaces, interface thermal conductance is smaller, ranging between 45 and 65 MW m-2 K-1 indicating that the thermal coupling between hydrophobic surfaces and water is weaker than with hydrophilic surfaces. The Kapitza length---the thermal conductivity of water divided by the thermal conductance per unit area of the interface---at hydrophobic interfaces (10-12 nm) is a factor of 2-3 larger than the Kapitza length at hydrophilic interfaces (3-6 nm). We also utilized the pump-probe transient absorption measurement to probe thermal transport in Au-core polymer-shell nanoparticles. The addition of an organic co-solvent to the suspension

  11. Liquid-liquid interfaces of semifluorinated alkane diblock copolymers with water, alkanes, and perfluorinated alkanes.

    PubMed

    Pierce, Flint; Tsige, Mesfin; Perahia, Dvora; Grest, Gary S

    2008-12-18

    The liquid-liquid interface between semifluorinated alkane diblock copolymers of the form F3C(CF2)n-1-(CH2)m-1CH3 and water, protonated alkanes, and perfluorinated alkanes are studied by fully atomistic molecular dynamics simulations. A modified version of the OPLS-AA (Optimized Parameter for Liquid Simulation All-Atom) force field of Jorgensen et al. has been used to study the interfacial behavior of semifluorinated diblocks. Aqueous interfaces are found to be sharp, with correspondingly large values of the interfacial tension. Due to the reduced hydrophobicity of the protonated block compared to the fluorinated block, hydrogen enhancement is observed at the interface. Water dipoles in the interfacial region are found to be oriented nearly parallel to the liquid-liquid interface. A number of protonated alkanes and perfluorinated alkanes are found to be mutually miscible with the semifluorinated diblocks. For these liquids, interdiffusion follows the expected Fickian behavior, and concentration-dependent diffusivities are determined.

  12. Active colloids at liquid-liquid interfaces: dynamic self-assembly and functionality

    NASA Astrophysics Data System (ADS)

    Snezhko, Alexey; Aranson, Igor

    2012-02-01

    Self-assembled materials must actively consume energy and remain out of equilibrium in order to support structural complexity and functional diversity. Colloids of interacting particles suspended at liquid-liquid interfaces and maintained out of equilibrium by external alternating electromagnetic fields develop nontrivial collective dynamics and self-assembly. We use ferromagnetic colloidal micro-particles (so the magnetic moment is fixed in each particle and interactions between colloids is highly anisotropic and directional) suspended over an interface of two immiscible liquids and energized by vertical alternating magnetic fields to demonstrate novel dynamic and active self-assembled structures (``asters'') which are not accessible through thermodynamic assembly. Structures are attributed to the interplay between surface waves, generated at the liquid/liquid interface by the collective response of magnetic microparticles to the alternating magnetic field, and hydrodynamic fields induced in the boundary layers of both liquids forming the interface. Two types of magnetic order are reported. We demonstrate that asters develop self-propulsion in the presence of a small in-plane dc magnetic field. We show that asters can capture, transport, and position target microparticles.

  13. Liquid-liquid interfaces of semifluorinated alkane diblock copolymers with water, alkanes, and perfluorinated alkanes.

    SciTech Connect

    Perahia, Dvora, Dr.; Pierce, Flint; Tsige, Mesfin; Grest, Gary Stephen, Dr.

    2008-08-01

    The liquid-liquid interface between semifluorinated alkane diblock copolymers of the form F3C(CF2)n-1-(CH2)m-1CH3 and water, protonated alkanes, and perfluorinated alkanes are studied by fully atomistic molecular dynamics simulations. A modified version of the OPLS-AA (Optimized Parameter for Liquid Simulation All-Atom) force field of Jorgensen et al. has been used to study the interfacial behavior of semifluorinated diblocks. Aqueous interfaces are found to be sharp, with correspondingly large values of the interfacial tension. Due to the reduced hydrophobicity of the protonated block compared to the fluorinated block, hydrogen enhancement is observed at the interface. Water dipoles in the interfacial region are found to be oriented nearly parallel to the liquid-liquid interface. A number of protonated alkanes and perfluorinated alkanes are found to be mutually miscible with the semifluorinated diblocks. For these liquids, interdiffusion follows the expected Fickian behavior, and concentration-dependent diffusivities are determined.

  14. Ultrasonic fluid densitometer having liquid/wedge and gas/wedge interfaces

    DOEpatents

    Greenwood, Margaret S.

    2000-01-01

    The present invention is an ultrasonic liquid densitometer that uses a material wedge having two sections, one with a liquid/wedge interface and another with a gas/wedge interface. It is preferred that the wedge have an acoustic impedance that is near the acoustic impedance of the liquid, specifically less than a factor of 11 greater than the acoustic impedance of the liquid. Ultrasonic signals are internally reflected within the material wedge. Density of a liquid is determined by immersing the wedge into the liquid and measuring reflections of ultrasound at the liquid/wedge interface and at the gas/wedge interface.

  15. Additive manufacturing. Continuous liquid interface production of 3D objects.

    PubMed

    Tumbleston, John R; Shirvanyants, David; Ermoshkin, Nikita; Janusziewicz, Rima; Johnson, Ashley R; Kelly, David; Chen, Kai; Pinschmidt, Robert; Rolland, Jason P; Ermoshkin, Alexander; Samulski, Edward T; DeSimone, Joseph M

    2015-03-20

    Additive manufacturing processes such as 3D printing use time-consuming, stepwise layer-by-layer approaches to object fabrication. We demonstrate the continuous generation of monolithic polymeric parts up to tens of centimeters in size with feature resolution below 100 micrometers. Continuous liquid interface production is achieved with an oxygen-permeable window below the ultraviolet image projection plane, which creates a "dead zone" (persistent liquid interface) where photopolymerization is inhibited between the window and the polymerizing part. We delineate critical control parameters and show that complex solid parts can be drawn out of the resin at rates of hundreds of millimeters per hour. These print speeds allow parts to be produced in minutes instead of hours.

  16. Interaction of Porosity with a Planar Solid/Liquid Interface

    NASA Technical Reports Server (NTRS)

    Catalina, Adrian V.; Stefanescu, Doru M.; Sen, Subhayu; Kaukler, William F.

    2004-01-01

    In this article, an investigation of the interaction between gas porosity and a planar solid/liquid (SL) interface is reported. A two-dimensional numerical model able to accurately track sharp SL interfaces during solidification of pure metals and alloys is proposed. The finite-difference method and a rectangular undeformed grid are used for computation. The SL interface is described through the points of intersection with the grid lines. Its motion is determined by the thermal and solute gradients at each particular point. Changes of the interface temperature because of capillarity or solute redistribution as well as any perturbation of the thermal and solute field produced by the presence of non-metallic inclusions can be computed. To validate the model, the dynamics of the interaction between a gas pore and a solidification front in metal alloys was observed using a state of the art X-ray transmission microscope (XTM). The experiments included observation of the distortion of the SL interface near a pore, real-time measurements of the growth rate, and the change in shape of the porosity during interaction with the SL interface in pure Al and Al-0.25 wt pct Au alloy. In addition, porosity-induced solute segregation patterns surrounding a pore were also quantified.

  17. Interaction of Porosity with a Planar Solid/Liquid Interface

    NASA Technical Reports Server (NTRS)

    Catalina, Adrian V.; Stefanescu, Doru M.; Sen, Subhayu; Kaukler, William K.; Curreri, Peter A. (Technical Monitor)

    2002-01-01

    In this paper, an investigation of the interaction between gas porosity and a planar solid/liquid (SL) interface is reported. A two-dimensional numerical model able to accurately track sharp SL interfaces during solidification of pure metals and alloys is proposed. The finite difference method and a rectangular undeformed grid are used for computation. The SL interface is described through the points of intersection with the grid lines. Its motion is determined by the thermal and solute gradients at each particular point. Changes of the interface temperature because of capillarity or solute redistribution as well as any perturbation of the thermal and solute field produced by the presence of non-metallic inclusions can be computed. To validate the model, the dynamics of the interaction between a gas pore and a solidification front in metal alloys was observed using a state of the art X-ray Transmission Microscope. The experiments included observation of the distortion of the SL interface near a pore, real-time measurements of the growth rate and the change in shape of the porosity during interaction with an advancing SL interface in pure Al and Al-0.25 wt% Au alloy. In addition, porosity induced solute segregation patterns surrounding a pore were also quantified.

  18. Interaction of Porosity with a Planar Solid/Liquid Interface

    NASA Technical Reports Server (NTRS)

    Catalina, Adrian V.; Stefanescu, Doru M.; Sen, Subhayu; Kaukler, William K.; Curreri, Peter A. (Technical Monitor)

    2002-01-01

    In this paper, an investigation of the interaction between gas porosity and a planar solid/liquid (SL) interface is reported. A two-dimensional numerical model able to accurately track sharp SL interfaces during solidification of pure metals and alloys is proposed. The finite difference method and a rectangular undeformed grid are used for computation. The SL interface is described through the points of intersection with the grid lines. Its motion is determined by the thermal and solute gradients at each particular point. Changes of the interface temperature because of capillarity or solute redistribution as well as any perturbation of the thermal and solute field produced by the presence of non-metallic inclusions can be computed. To validate the model, the dynamics of the interaction between a gas pore and a solidification front in metal alloys was observed using a state of the art X-ray Transmission Microscope. The experiments included observation of the distortion of the SL interface near a pore, real-time measurements of the growth rate and the change in shape of the porosity during interaction with an advancing SL interface in pure Al and Al-0.25 wt% Au alloy. In addition, porosity induced solute segregation patterns surrounding a pore were also quantified.

  19. Use of the liquid-liquid interface for generating ultrathin nanocrystalline films of metals, chalcogenides, and oxides.

    PubMed

    Rao, C N R; Kulkarni, G U; Agrawal, Ved Varun; Gautam, Ujjal K; Ghosh, Moumita; Tumkurkar, Usha

    2005-09-15

    The air-water interface has traditionally been employed to prepare particle assemblies and films of metals and semiconductors. The interface between water and an organic liquid, however, has not been investigated sufficiently for possible use in preparing nanocrystals and thin films of materials. In this article, we demonstrate the use of the liquid-liquid interface as a medium for preparing ultrathin films of metals, chalcogenides and oxides. The method involves the reaction at the interface between a metal-organic compound in the organic layer and an appropriate reagent for reduction, sulfidation, etc. in the aqueous layer. Some of the materials discussed are nanocrystalline films of gold, CuS, CuSe, CuO, and Cu(OH)2 formed at the liquid-liquid interface. The results reported in this article should demonstrate the versatility and potential of the liquid-liquid interface for preparing nanomaterials and ultrathin films and encourage further research in this area.

  20. Molecular dynamics of the water liquid-vapor interface

    NASA Technical Reports Server (NTRS)

    Wilson, M. A.; Pohorille, A.; Pratt, L. R.; MacElroy, R. D. (Principal Investigator)

    1987-01-01

    The results of molecular dynamics calculations on the equilibrium interface between liquid water and its vapor at 325 K are presented. For the TIP4P model of water intermolecular pair potentials, the average surface dipole density points from the vapor to the liquid. The most common orientations of water molecules have the C2 nu molecular axis roughly parallel to the interface. The distributions are quite broad and therefore compatible with the intermolecular correlations characteristic of bulk liquid water. All near-neighbor pairs in the outermost interfacial layers are hydrogen bonded according to the common definition adopted here. The orientational preferences of water molecules near a free surface differ from those near rigidly planar walls which can be interpreted in terms of patterns found in hexagonal ice 1. The mean electric field in the interfacial region is parallel to the mean polarization which indicates that attention cannot be limited to dipolar charge distributions in macroscopic descriptions of the electrical properties of this interface. The value of the surface tension obtained is 132 +/- 46 dyn/cm, significantly different from the value for experimental water of 68 dyn/cm at 325 K.

  1. Molecular dynamics of the water liquid-vapor interface

    NASA Technical Reports Server (NTRS)

    Wilson, M. A.; Pohorille, A.; Pratt, L. R.; MacElroy, R. D. (Principal Investigator)

    1987-01-01

    The results of molecular dynamics calculations on the equilibrium interface between liquid water and its vapor at 325 K are presented. For the TIP4P model of water intermolecular pair potentials, the average surface dipole density points from the vapor to the liquid. The most common orientations of water molecules have the C2 nu molecular axis roughly parallel to the interface. The distributions are quite broad and therefore compatible with the intermolecular correlations characteristic of bulk liquid water. All near-neighbor pairs in the outermost interfacial layers are hydrogen bonded according to the common definition adopted here. The orientational preferences of water molecules near a free surface differ from those near rigidly planar walls which can be interpreted in terms of patterns found in hexagonal ice 1. The mean electric field in the interfacial region is parallel to the mean polarization which indicates that attention cannot be limited to dipolar charge distributions in macroscopic descriptions of the electrical properties of this interface. The value of the surface tension obtained is 132 +/- 46 dyn/cm, significantly different from the value for experimental water of 68 dyn/cm at 325 K.

  2. Boundary conditions on the vapor liquid interface at strong condensation

    NASA Astrophysics Data System (ADS)

    Kryukov, A. P.; Levashov, V. Yu.

    2016-07-01

    The problem of the formulation of boundary conditions on the vapor-liquid interface is considered. The different approaches to this problem and their difficulties are discussed. Usually, a quasi-equilibrium scheme is used. At sufficiently large deviations from thermodynamic equilibrium, a molecular kinetics approach should be used for the description of the vapor flow at condensation. The formulation of the boundary conditions at the vapor liquid interface to solve the Boltzmann kinetic equation for the distribution of molecules by velocity is a sophisticated problem. It appears that molecular dynamics simulation (MDS) can be used to provide this solution at the interface. The specific problems occur in the realization of MDS on large time and space scales. Some of these problems, and a hierarchy of continuum, kinetic and molecular dynamic time scales, are discussed in the paper. A description of strong condensation at the kinetic level is presented for the steady one-dimensional problem. A formula is provided for the calculation of the limiting condensation coefficient. It is shown that as the condensation coefficient approaches the limiting value, the vapor pressure rises significantly. The results of the corresponding calculations for the Mach number and temperature at different vapor flows are demonstrated. As a result of the application of the molecular kinetics method and molecular dynamics simulation to the problem of the determination of argon condensation coefficients in the range of temperatures of vapor and liquid ratio 1.0-4.0, it is concluded that the condensation coefficient is close to unity.

  3. Adsorption of nanoparticles at the solid-liquid interface.

    PubMed

    Brenner, Thorsten; Paulus, Michael; Schroer, Martin A; Tiemeyer, Sebastian; Sternemann, Christian; Möller, Johannes; Tolan, Metin; Degen, Patrick; Rehage, Heinz

    2012-05-15

    The adsorption of differently charged nanoparticles at liquid-solid interfaces was investigated by in situ X-ray reflectivity measurements. The layer formation of positively charged maghemite (γ-Fe(2)O(3)) nanoparticles at the aqueous solution-SiO(2) interface was observed while negatively charged gold nanoparticles show no adsorption at this interface. Thus, the electrostatic interaction between the particles and the charged surface was determined as the driving force for the adsorption process. The data analysis shows that a logarithmic particle size distribution describes the density profile of the thin adsorbed maghemite layer. The size distribution in the nanoparticle solution determined by small angle X-ray scattering shows an average particle size which is similar to that found for the adsorbed film. The formed magehemite film exhibits a rather high stability. Copyright © 2012 Elsevier Inc. All rights reserved.

  4. Manipulation of liquid-liquid interfaces for tunable optics on a chip in microfluidic systems

    NASA Astrophysics Data System (ADS)

    Tan, Kam Yan Sindy

    This thesis describes the design and development of optofluidics: a new class of optical components based on dynamic liquid-liquid interfaces between liquids possessing different optical properties in microfluidic systems. Devices with optical interfaces formed by liquids possess characteristics that are quite different from solid-gas and solid-liquid systems commonly used in conventional optics. Advantages of optofluidic systems include the simplicity to reconfigure optical properties and functions in real time. Examples of devices include liquid waveguides, lenses, and multi-color droplet dye laser. Potential applications include biochemical characterization and optical spectroscopy in micro-total analytical systems. Chapter 1 describers the motivation, general configuration and characteristics of devices with optical interfaces formed by liquids in microchannels. Chapter 2 describes the soft lithographic techniques used to make optofluidic devices. Chapter 3 describes the use of co-fabrication to design and fabricate multiple functional components in microfluidic systems in a single step. Chapters 4 to 6 describe the design and operation of three optofluidic devices: waveguides, lenses, and dye lasers.

  5. A polymer microgel at a liquid-liquid interface: theory vs. computer simulations.

    PubMed

    Rumyantsev, Artem M; Gumerov, Rustam A; Potemkin, Igor I

    2016-08-10

    We propose a mean-field theory and dissipative particle dynamics (DPD) simulations of swelling and collapse of a polymer microgel adsorbed at the interface of two immiscible liquids (A and B). The microgel reveals surface activity and lowers A-B interfacial tension. Attempting to occupy as large an interfacial area as possible, the microgel undergoes anisotropic deformation and adopts a flattened shape. Spreading over the interface is restricted by polymer subchain elasticity. The equilibrium shape of the microgel at the interface depends on its size. Small microgels are shown to be more oblate than the larger microgels. Increasing microgel cross-link density results in stronger reduction of the surface tension and weaker flattening. As the degree of immiscibility of A and B liquids increases, the microgel volume changes in a non-monotonous fashion: the microgel contraction at moderate immiscibility of A and B liquids is followed by its swelling at high incompatibility of the liquids. The segregation regime of the liquids within and outside the microgel is different. Being segregated outside the microgel, the liquids can be fully (homogeneously) mixed or weakly segregated within it. The density profiles of the liquids and the polymer were plotted under different conditions. The theoretical and the DPD simulation results are in good agreement. We hope that our findings will be useful for the design of stimuli responsive emulsions, which are stabilized by the microgel particles, as well as for their practical applications, for instance, in biocatalysis.

  6. Interface initiation and propagation in liquid demixing with electric fields.

    PubMed

    Galanis, Jennifer; Tsori, Yoav

    2014-12-07

    We investigate the dynamics of liquid-liquid phase separation confined in a charged concentric cylindrical geometry. Two main time scales characterize the non-equilibrium interface behavior: (1) the lag time t(L) for forming an interface, and (2) the relaxation time to equilibrium. We find that t(L) increases as parameters (temperature, bulk composition, and surface charge) approach the electrostatic spinodal line in the phase diagram. Close to this line, t(L) is proportional to a renormalized bulk concentration with an exponent of -1.16 ± 0.03. The relaxation of the interface to equilibrium can be divided into three phases: early, intermediate (power-law), and late (exponential). During power-law relaxation, the location of the rescaled interface is proportional to time with an exponent of -0.94 ± 0.04. Exponential relaxation occurs as a consequence of finite-size effects, and the associated time constant decreases with decreasing system size (with a power-law scaling), decreasing concentration, and increasing surface charge. The time constant also decreases with increasing (decreasing) temperature when the concentration is below (above) the critical concentration.

  7. Floating and sinking of self-assembled spheres on liquid-liquid interfaces: Rafts versus stacks

    NASA Astrophysics Data System (ADS)

    Jones, Steven G.; Abbasi, Niki; Ahuja, Abhinav; Truong, Vivian; Tsai, Scott S. H.

    2015-07-01

    The floating and sinking of objects on fluid-fluid interfaces occurs in nature and has many important implications in technology. Here, we study the stability of floating self-assembled spheres on an oil-water interface, and how the sphere deposition geometry affects the size limits of the assemblies before they collapse and sink through the interface. Specifically, we compare the critical size of particle rafts to particle stacks. We show that, on liquid-liquid interfaces, monolayer rafts and stacked spheres exhibit different scaling of the critical number of spheres to the Bond number—the dimensionless ratio of buoyancy to interfacial tension effects. Our results indicate that particle stacks will sink with a lower threshold number of particles than particle rafts. This finding may have important implications to engineering applications where interfacial assemblies are not monolayers.

  8. Pressurization of a Flightweight, Liquid Hydrogen Tank: Evaporation and Condensation at a Liquid Vapor Interface

    NASA Technical Reports Server (NTRS)

    Stewart, Mark

    2017-01-01

    Evaporation and condensation at a liquid-vapor interface is important for long-term, in-space cryogenic propellant storage. Yet the current understanding of inter-facial physics does not consistently predict behavior of evaporation or condensation rates. The proposed paper will present a physical model, based on the 1-D Heat equation and Schrage's equation, which demonstrates thin thermal layers at the fluid vapor interface.

  9. Mixing and transient interface condensation of a liquid hydrogen tank

    NASA Technical Reports Server (NTRS)

    Lin, C. S.; Hasan, M. M.; Nyland, T. W.

    1993-01-01

    Experiments were conducted to investigate the effect of axial jet-induced mixing on the pressure reduction of a thermally stratified liquid hydrogen tank. The tank was nearly cylindrical, having a volume of about 0.144 cu m with 0.559 m in diameter and 0.711 m length. A mixer/pump unit, which had a jet nozzle outlet of 0.0221 m in diameter was located 0.178 m from the tank bottom and was installed inside the tank to generate the axial jet mixing and tank fluid circulation. Mixing tests began with the tank pressures at which the thermal stratification results in 4.9-6.2 K liquid subcooling. The mixing time and transient vapor condensation rate at the liquid-vapor interface are determined. Two mixing time correlations, based on the thermal equilibrium and pressure equilibrium, are developed and expressed as functions of system and buoyancy parameters. The limited liquid hydrogen data of the present study shows that the modified steady state condensation rate correlation may be used to predict the transient condensation rate in a mixing process if the instantaneous values of jet sub cooling and turbulence intensity at the interface are employed.

  10. Air-Liquid Interfaces: I. Alcohols and Aromatic Hydrocarbons

    NASA Astrophysics Data System (ADS)

    Allen, Heather; van Loon, Lisa; Hommel, Elizabeth

    2004-03-01

    Alcohols and aromatic hydrocarbons solutions were investigated using broad bandwidth sum frequency generation (BBSFG), a highly surface-selective spectroscopy, and IR and Raman spectroscopies. For aqueous methanol solutions the surface hydrogen bonding environment is quite different relative to the bulk environment. The surface BBSFG studies suggest that methanol is a more efficient hydrogen bonding acceptor when the methanol molecule resides in the interfacial region. Methanol reaction with sulfuric acid was also studied to quantify and understand the formation of mono methyl sulfonate relative to the dimethyl sulfonate. We have also investigated several neat and water-saturated liquid aromatic hydrocarbon surfaces. The data indicate that benzene and similar molecules are tilted at their air-liquid interface. With the introduction of relatively few water molecules into a 1-methyl naphthalene (1-MN) liquid (1 water: 336 1-MN) a rearrangement of the surface molecules is induced, leading to an increased number density of the methyl groups arranged such that more methyl groups are oriented in the same direction into the air phase at the air-liquid 1-MN interface.

  11. Liquid-interfaced oscillating glow discharge detector for a flowing liquid system.

    PubMed

    Herring, C J; Piepmeier, E H

    1995-03-01

    A new liquid-interfaced oscillating glow discharge detector having a frequency and current response to femtomole and picomole quantities respectively of potassium nitrate and sucrose injected into an aqueous flowing eluent is presented. The glow discharge is formed in an argon atmosphere at ambient pressure between a platinum anode and a cathode consisting of an aqueous conducting solution. A detailed description of the appearance of the liquid-interfaced glow discharge at various electrode distances and the occurrence of high-frequency oscillations is given.

  12. Electrical control of Faraday rotation at a liquid-liquid interface.

    PubMed

    Marinescu, Monica; Kornyshev, Alexei A; Flatté, Michael E

    2015-01-01

    A theory is developed for the Faraday rotation of light from a monolayer of charged magnetic nanoparticles at an electrified liquid-liquid interface. The polarization fields of neighboring nanoparticles enhance the Faraday rotation. At such interfaces, and for realistic sizes and charges of nanoparticles, their adsorption-desorption can be controlled with a voltage variation<1 V, providing electrovariable Faraday rotation. A calculation based on the Maxwell-Garnett theory predicts that the corresponding redistribution of 40 nm nanoparticles of yttrium iron garnet can switch a cavity with a quality factor larger than 10(4) for light of wavelength 500 nm at normal incidence.

  13. Methods and systems for monitoring a solid-liquid interface

    DOEpatents

    Stoddard, Nathan G [Gettysburg, PA; Clark, Roger F [Frederick, MD

    2011-10-04

    Methods and systems are provided for monitoring a solid-liquid interface, including providing a vessel configured to contain an at least partially melted material; detecting radiation reflected from a surface of a liquid portion of the at least partially melted material; providing sound energy to the surface; measuring a disturbance on the surface; calculating at least one frequency associated with the disturbance; and determining a thickness of the liquid portion based on the at least one frequency, wherein the thickness is calculated based on L=(2m-1)v.sub.s/4f, where f is the frequency where the disturbance has an amplitude maximum, v.sub.s is the speed of sound in the material, and m is a positive integer (1, 2, 3, . . . ).

  14. Resolving amorphous solid-liquid interfaces by atomic force microscopy

    NASA Astrophysics Data System (ADS)

    Burson, Kristen M.; Gura, Leonard; Kell, Burkhard; Büchner, Christin; Lewandowski, Adrian L.; Heyde, Markus; Freund, Hans-Joachim

    2016-05-01

    Recent advancements in liquid atomic force microscopy make it an ideal technique for probing the structure of solid-liquid interfaces. Here, we present a structural study of a two-dimensional amorphous silica bilayer immersed in an aqueous solution utilizing liquid atomic force microscopy with sub-nanometer resolution. Structures show good agreement with atomically resolved ultra-high vacuum scanning tunneling microscopy images obtained on the same sample system, owing to the structural stability of the silica bilayer and the imaging clarity from the two-dimensional sample system. Pair distance histograms of ring center positions are utilized to develop quantitative metrics for structural comparison, and the physical origin of pair distance histogram peaks is addressed by direct assessment of real space structures.

  15. Resolving amorphous solid-liquid interfaces by atomic force microscopy

    SciTech Connect

    Burson, Kristen M.; Gura, Leonard; Kell, Burkhard; Büchner, Christin; Lewandowski, Adrian L.; Heyde, Markus Freund, Hans-Joachim

    2016-05-16

    Recent advancements in liquid atomic force microscopy make it an ideal technique for probing the structure of solid-liquid interfaces. Here, we present a structural study of a two-dimensional amorphous silica bilayer immersed in an aqueous solution utilizing liquid atomic force microscopy with sub-nanometer resolution. Structures show good agreement with atomically resolved ultra-high vacuum scanning tunneling microscopy images obtained on the same sample system, owing to the structural stability of the silica bilayer and the imaging clarity from the two-dimensional sample system. Pair distance histograms of ring center positions are utilized to develop quantitative metrics for structural comparison, and the physical origin of pair distance histogram peaks is addressed by direct assessment of real space structures.

  16. Rayleigh-Taylor stability boundary at solid-liquid interfaces.

    PubMed

    Piriz, A R; Sun, Y B; Tahir, N A

    2013-08-01

    A previous model for the Rayleigh-Taylor instability [A. R. Piriz, J. J. López Cela, and N. A. Tahir, Phys. Rev. E 80, 046305 (2009)] has been extended in order to study an interface between an elastic-plastic solid and a Newtonian liquid and determine the stability region given by the initial perturbation amplitude ξ(0) and wavelength λ. The stability region is found to be enhanced by the effect of the liquid viscosity, but it reaches an asymptote for a sufficiently high viscosity. In addition, it is also found that the boundary for the transition from the elastic to the plastic regime get closer to the stability boundary up to both boundaries coincide for a high enough liquid viscosity, thus making the onset of plastic flow a sufficient condition for instability.

  17. Thermocapillary Convection at the Interface of Two Liquids --

    NASA Astrophysics Data System (ADS)

    van Hook, Stephen J.; Andre, Carrie; McCormick, W. D.; Swift, J. B.; Swinney, Harry L.

    1997-11-01

    While convection due to surface tension (thermocapillary) effects at a liquid-gas interface has received much theoretical and experiment attention (S. J. Van Hook et al.), to appear in J. Fluid Mech.; A. A. Golovin, A. A. Nepomnyashchy, & L. M. Pismen, Phys. Fluids 6, 34--48 (1994); D. A. Goussis & R. E. Kelly, Int. J. Heat Mass Trans. 33, 2237--2245 (1990); S. Davis, Annu. Rev. Fluid Mech. 19, 403--435 (1987)., the problem of two-layer (liquid-liquid) surface-tension-driven convection has been relatively ignored. Stability theory predicts a wide range of instabilities---short- and long-wavelength, stationary and oscillatory---for heating the system from above or below. We examine the conditions under which these different instabilities can be observed in real fluid systems. While the short wavelength instabilities are analogous to convection in buoyancy-driven convection, the long-wavelength instabilities are exclusively a feature of thermocapillary flow.

  18. Capillary freezing of ionic liquids confined between metallic interfaces

    NASA Astrophysics Data System (ADS)

    Comtet, Jean; Niguès, Antoine; Kaiser, Vojtech; Bocquet, Lydéric; Siria, Alessandro

    2016-11-01

    Using a quartz tuning fork based AFM, we investigate the behavior of ionic liquids under confinement. Using nanorheological measurements, we show that nanometric confinements can lead to solidification and capillary freezing of the ionic liquid. We find that the critical confinement at which the liquid-solid transition occurs depends strongly on the bulk electronic properties of the confining substrate, with stronger effects observed for more metallic surfaces. This behavior is rationalized on the basis of a Gibbs-Thompson framework for the shift of the freezing transition, taking into account surface energies with the imperfect metal at the level of a Thomas-Fermi model. Finally, we show that capillary freezing can also be tuned by electrifying the confining interfaces.

  19. Dependence of solid-liquid interface free energy on liquid structure

    NASA Astrophysics Data System (ADS)

    Wilson, S. R.; Mendelev, M. I.

    2014-09-01

    The Turnbull relation is widely believed to enable prediction of solid-liquid interface (SLI) free energies from measurements of the latent heat and the solid density. Ewing proposed an additional contribution to the SLI free energy to account for variations in liquid structure near the interface. In the present study, molecular dynamics (MD) simulations were performed to investigate whether SLI free energy depends on liquid structure. Analysis of the MD simulation data for 11 fcc metals demonstrated that the Turnbull relation is only a rough approximation for highly ordered liquids, whereas much better agreement is observed with Ewing's theory. A modification to Ewing's relation is proposed in this study that was found to provide excellent agreement with MD simulation data.

  20. Crystallization of Polymers at liquid/liquid interface templated by single-walled carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Wang, Wenda; Li, Christopher

    2012-02-01

    Nanosized single-walled carbon nanotube rings were fabricated by using a Pickering emulsion-based method. By tuning a water/oil/SWNT miniemulsion system, SWNT rings with a diameter of ˜200 nm can be readily achieved. The formation mechanism is attributed to the bending force induced by the curved liquid/liquid interface. Crystallization of polyethylene homo- and copolymers using this unique SWNT rings as the nucleation agent was conducted at the curved liquid/liquid interface. Crystal structure, hybrid morphology and crystallization kinetics were systematically studied. The structure of controlled alternating patterns on SWNT rings has great potential in various applications in large-scale integrated circuits and single-electron devices.

  1. Dependence of solid-liquid interface free energy on liquid structure

    SciTech Connect

    Wilson, S R; Mendelev, M I

    2014-09-01

    The Turnbull relation is widely believed to enable prediction of solid–liquid interface (SLI) free energies from measurements of the latent heat and the solid density. Ewing proposed an additional contribution to the SLI free energy to account for variations in liquid structure near the interface. In the present study, molecular dynamics (MD) simulations were performed to investigate whether SLI free energy depends on liquid structure. Analysis of the MD simulation data for 11 fcc metals demonstrated that the Turnbull relation is only a rough approximation for highly ordered liquids, whereas much better agreement is observed with Ewing’s theory. A modification to Ewing’s relation is proposed in this study that was found to provide excellent agreement with MD simulation data.

  2. Assembly of metal nanoparticle-carbon nanotube composite materials at the liquid/liquid interface.

    PubMed

    Lee, Kang Yeol; Kim, Minjung; Hahn, Joeoong; Suh, Jung Sang; Lee, Inhyung; Kim, Kwan; Han, Sang Woo

    2006-02-14

    Carbon nanotubes (CNTs)-mediated self-assembly of metal (Au and Ag) nanoparticles at the liquid/liquid interface in the form of a stable nanocomposite film is reported. The metallic luster results from the electronic coupling of nanoparticles, suggesting the formation of closely packed nanoparticle thin films. The interfacial film could be transferred to mica substrates and carbon-coated transmission electron microscopy (TEM) grids. The transferred films were very stable for a prolonged time. The samples were characterized by UV-vis spectroscopy, scanning electron microscopy (SEM), TEM, and X-ray photoelectron spectroscopy (XPS). SEM and TEM results show that the films formed at the liquid/liquid interface are indeed composite materials consisting of CNTs and nanoparticles. XPS measurements further indicate the presence of the interaction between nanoparticles and CNTs.

  3. Electric double layer at the interface of ionic liquid-dielectric liquid under electric field.

    PubMed

    Lee, D W; Im, D J; Kang, I S

    2013-02-12

    The structure of the electric double layer (EDL) is analyzed in order to understand the electromechanical behavior of the interface of ionic liquid-dielectric liquid. The modified Poisson-Boltzmann equation proposed by Bazant et al. is solved to see the crowding and the overscreening effects that are the characteristics of an ionic liquid (Bazant, M. Z.; Storey, B. D.; Kornyshev, A. A. Double layer in ionic liquids: Overscreening versus crowding. Phys. Rev. Lett. 2011, 106, 046102.). From the simple one-dimensional (1-D) analysis, it is found that the changes of the composition and the material properties in the EDL are negligible except under some extreme conditions such as strong electric field over O(10(8)) V/m. From the electromechanical view points, an ionic liquid behaves like a pure conductor at the interface with a dielectric liquid. Based on these findings, three specific application problems are considered. In the first, a new method is suggested for measuring the interfacial tension of an ionic liquid-dielectric liquid system. The deformation of a charged ionic liquid droplet translating between two electrodes is used for this measurement. The second is for the Taylor cone problem, which includes an extreme electric field condition near the tip. The size of the critical region, where the EDL effect should be considered, is estimated by using the 1-D analysis result. Numerical computation is also performed to see the profiles of electric potential and the electric stress along the interface of the Taylor cone. Lastly, the electrowetting problem of the ionic liquid is considered. The discrepancies in the results of previous workers are interpreted by using the results of the present work. It is shown that all the results might be consistent if the leaking of the dielectric layer and/or the adsorption of ions is considered.

  4. Surface vibrational structure at alkane liquid/vapor interfaces.

    PubMed

    Esenturk, Okan; Walker, Robert A

    2006-11-07

    Broadband vibrational sum frequency spectroscopy (VSFS) has been used to examine the surface structure of alkane liquid/vapor interfaces. The alkanes range in length from n-nonane (C(9)H(20)) to n-heptadecane (C(17)H(36)), and all liquids except heptadecane are studied at temperatures well above their bulk (and surface) freezing temperatures. Intensities of vibrational bands in the CH stretching region acquired under different polarization conditions show systematic, chain length dependent changes. Data provide clear evidence of methyl group segregation at the liquid/vapor interface, but two different models of alkane chain structure can predict chain length dependent changes in band intensities. Each model leads to a different interpretation of the extent to which different chain segments contribute to the anisotropic interfacial region. One model postulates that changes in vibrational band intensities arise solely from a reduced surface coverage of methyl groups as alkane chain length increases. The additional methylene groups at the surface must be randomly distributed and make no net contribution to the observed VSF spectra. The second model considers a simple statistical distribution of methyl and methylene groups populating a three dimensional, interfacial lattice. This statistical picture implies that the VSF signal arises from a region extending several functional groups into the bulk liquid, and that the growing fraction of methylene groups in longer chain alkanes bears responsibility for the observed spectral changes. The data and resulting interpretations provide clear benchmarks for emerging theories of molecular structure and organization at liquid surfaces, especially for liquids lacking strong polar ordering.

  5. Self-Regulated Nanoparticle Assembly at Liquid/Liquid Interfaces: A Route to Adaptive Structuring of Liquids.

    PubMed

    Huang, Caili; Cui, Mengmeng; Sun, Zhiwei; Liu, Feng; Helms, Brett A; Russell, Thomas P

    2017-08-15

    The controlled structuring of liquids into arbitrary shapes can be achieved in biphasic liquid media using the interfacial assemblies of nanoparticle surfactants (NP-surfactants), that consist of a polar nanoparticle "head group" bound to one or more hydrophobic polymer "tails". The nonequilibrium shapes of the suspended liquid phase can be rendered permanent by the jamming of the NP-surfactants formed and assembled at the interface between the liquids as the system attempts to minimize the interfacial area between the liquids. While critical to the structuring process, little is known of the dynamic mechanical properties of the NP-surfactant monolayer at the interface as it is dictated by the characteristics of the component, including NP size and concentration and the molecular weight and concentration of polymers bound to the NPs. Here we provide the first comprehensive understanding of the dynamic mechanical character of two-dimensional NP-surfactant assemblies at liquid/liquid interfaces. Our results indicate that the dynamics of NP-polymer interactions are self-regulated across multiple time scales and are associated with specific mesoscale interactions between self-similar and cross-complementary components. Furthermore, the mechanical properties of the NP-surfactant monolayer are tunable over a broad range and deterministic on the basis of those component inputs. This control is key to tailoring the functional attributes of the reconfigurable structured liquids to suit specific applications.

  6. Non-capillary binding of colloidal particles to liquid interfaces

    NASA Astrophysics Data System (ADS)

    Kaz, David; McGorty, Ryan; Manoharan, Vinothan

    2012-02-01

    We observe colloidal polystyrene particles binding reversibly to an oil-water interface through the combination of a repulsive electrostatic force and an attractive van der Waals force. Previously studied interactions of an aqueous colloidal particle and a liquid interface have generally fallen into two categories: 1) electrostatic repulsion indicated by the dependence on salt and 2) capillary adsorption where surface tension brings the particle in contact with both phases and is indicated by practically irreversible binding. With our technique of pushing individual colloidal particles towards a planar oil-water interface and observing their motion in three-dimensions with holographic microscopy we have observed both interactions. However, our observations indicate that under certain conditions the electrostatic repulsion, which is due to repulsive image charges, is weak enough for a particle to experience a van der Waals attraction while strong enough to prevent a particle from penetrating the interface and becoming bound through capillary action. We observe individual particles transition between repulsive and attractive interactions with the interface suggesting that these colloidal particles have a heterogeneous surface charge.

  7. Production of Self-Assembled Fullerene (C60) Nanocrystals at Liquid-Liquid Interface.

    PubMed

    Shrestha, Rekha Goswami; Shrestha, Lok Kumar; Abe, Masahiko; Ariga, Katsuhiko

    2015-03-01

    Here we present self-assembled nanostructure of functional molecule fullerene (C60) at liquid-liquid interface. The nanostructured nanocrystals were grown at liquid-liquid interface of isopropyl alcohol (IPA) and C60 solution in butylbenzene under ambient condition of temperature and pressure, and characterized by Raman scattering, power X-ray diffraction (XRD), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The crystal formation mechanism is driven by supersaturation related to the low solubility of C60 in IPA. A slow diffusion of IPA towards the C60 solution causes unsaturation of C60 at the liquid-liquid interface and consequently small clusters of C60 is formed at the interface, which acts as the nucleation site. Further diffusion of IPA supplies the C60 molecules from bulk to the interface promoting the crystal growth. Based on SEM and TEM observation, the average size of the individual hexagonal bipyramid nanocrystal is found to be ca. 1.4 µm and the average size of their assembly is found to be approximately 2 µm. XRD measurements have shown that these materials are crystalline with mixed face-centered cubic (cell dimension: a = 1.352 nm, and V = 2.475 nm3) and hexagonal (cell dimension: a = 1.452 nm, c = 1.207 nm, c/a = 0.831, and V = 2.475 nm3) structures. Raman scattering measurements showed two Ag and six Hg vibration bands, which are similar to those obtained in the pristine C60.

  8. Probing Hydrophilic Interface of Solid/Liquid-Water by Nanoultrasonics

    PubMed Central

    Mante, Pierre-Adrien; Chen, Chien-Cheng; Wen, Yu-Chieh; Chen, Hui-Yuan; Yang, Szu-Chi; Huang, Yu-Ru; -Ju Chen, I.; Chen, Yun-Wen; Gusev, Vitalyi; Chen, Miin-Jang; Kuo, Jer-Lai; Sheu, Jinn-Kong; Sun, Chi-Kuang

    2014-01-01

    Despite the numerous devoted studies, water at solid interfaces remains puzzling. An ongoing debate concerns the nature of interfacial water at a hydrophilic surface, whether it is more solid-like, ice-like, or liquid-like. To answer this question, a complete picture of the distribution of the water molecule structure and molecular interactions has to be obtained in a non-invasive way and on an ultrafast time scale. We developed a new experimental technique that extends the classical acoustic technique to the molecular level. Using nanoacoustic waves with a femtosecond pulsewidth and an ångström resolution to noninvasively diagnose the hydration structure distribution at ambient solid/water interface, we performed a complete mapping of the viscoelastic properties and of the density in the whole interfacial water region at hydrophilic surfaces. Our results suggest that water in the interfacial region possesses mixed properties and that the different pictures obtained up to now can be unified. Moreover, we discuss the effect of the interfacial water structure on the abnormal thermal transport properties of solid/liquid interfaces. PMID:25176017

  9. Mixing and transient interface condensation of a liquid hydrogen tank

    NASA Technical Reports Server (NTRS)

    Lin, C. S.; Hasan, M. M.; Nyland, T. W.

    1993-01-01

    Experiments were conducted to investigate the effect of axial jet-induced mixing on the pressure reduction of a thermally stratified liquid hydrogen tank. The tank was nearly cylindrical, having a volume of about 0.144 cu m with 0.559 m in diameter and 0.711 m long. A mixer/pump unit, which had a jet nozzle outlet of 0.0221 m in diameter was located 0.178 m from the tank bottom and was installed inside the tank to generate the axial jet mixing and tank fluid circulation. The liquid fill and jet flow rate ranged from 42 to 85 percent (by volume) and 0.409 to 2.43 cu m/hr, respectively. Mixing tests began with the tank pressure ranging from 187.5 to 238.5 kPa at which the thermal stratification results in 4.9 to 6.2 K liquid sub cooling. The mixing time and transient vapor condensation rate at the liquid-vapor interface are determined. Two mixing time correlations, based on the thermal equilibrium and pressure equilibrium, are developed. Both mixing time correlations are expressed as functions of system and buoyancy parameters and compared well with other experimental data. The steady state condensation rate correlation of Sonin et al. based on steam-water data is modified and expressed as a function of jet subcooling. The limited liquid hydrogen data of the present study shows that the modified steady state condensation rate correlation may be used to predict the transient condensation rate in a mixing process if the instantaneous values of jet sub cooling and turbulence intensity at the interface are employed.

  10. The Atomic scale structure of liquid metal-electrolyte interfaces

    NASA Astrophysics Data System (ADS)

    Murphy, B. M.; Festersen, S.; Magnussen, O. M.

    2016-07-01

    Electrochemical interfaces between immiscible liquids have lately received renewed interest, both for gaining fundamental insight as well as for applications in nanomaterial synthesis. In this feature article we demonstrate that the atomic scale structure of these previously inaccessible interfaces nowadays can be explored by in situ synchrotron based X-ray scattering techniques. Exemplary studies of a prototypical electrochemical system - a liquid mercury electrode in pure NaCl solution - reveal that the liquid metal is terminated by a well-defined atomic layer. This layering decays on length scales of 0.5 nm into the Hg bulk and displays a potential and temperature dependent behaviour that can be explained by electrocapillary effects and contributions of the electronic charge distribution on the electrode. In similar studies of nanomaterial growth, performed for the electrochemical deposition of PbFBr, a complex nucleation and growth behaviour is found, involving a crystalline precursor layer prior to the 3D crystal growth. Operando X-ray scattering measurements provide detailed data on the processes of nanoscale film formation.

  11. Self-instability of finite sized solid-liquid interfaces

    PubMed Central

    Wu, L.K.; Xu, B.; Li, Q.L.; Liu, W.

    2015-01-01

    In solid-liquid systems, macroscopic solids lose their equilibrium and melt in a manner that results in overall movement of the solid-liquid interface. This phenomenon occurs when they are subjected to temperature gradients or external stress, for example. However, many experiments suggest that the melting of nano- and micro-sized metallic nuclei follows a different process not described by traditional melting theory. In this paper, we demonstrate through simulation that the melting of solid nuclei of these sizes occurs via random breaches at the interfaces. Moreover, this breaching process occurs at the exact solid-liquid equilibrium temperature and in the absence of any external disturbance, which suggests the name “self-instability” for this melting process. We attribute this spontaneous instability to the curvature of the samples; based on the relationship between the sample’s instability and its curvature, we propose a destabilizing model for small systems. This model fits well with experimental results and leads to new insights into the instability behavior of small-sized systems; these insights have broad implications for research topics ranging from dendrite self-fragmentation to nanoparticle instability. PMID:26685800

  12. Solvent Extraction: Structure of the Liquid-Liquid Interface Containing a Diamide Ligand.

    PubMed

    Scoppola, Ernesto; Watkins, Erik B; Campbell, Richard A; Konovalov, Oleg; Girard, Luc; Dufrêche, Jean-Francois; Ferru, Geoffroy; Fragneto, Giovanna; Diat, Olivier

    2016-08-01

    Knowledge of the (supra)molecular structure of an interface that contains amphiphilic ligand molecules is necessary for a full understanding of ion transfer during solvent extraction. Even if molecular dynamics already yield some insight in the molecular configurations in solution, hardly any experimental data giving access to distributions of both extractant molecules and ions at the liquid-liquid interface exist. Here, the combined application of X-ray and neutron reflectivity measurements represents a key milestone in the deduction of the interfacial structure and potential with respect to two different lipophilic ligands. Indeed, we show for the first time that hard trivalent cations can be repelled or attracted by the extractant-enriched interface according to the nature of the ligand.

  13. Biofilm formation at the solid-liquid and air-liquid interfaces by Acinetobacter species

    PubMed Central

    2011-01-01

    Background The members of the genus Acinetobacter are Gram-negative cocobacilli that are frequently found in the environment but also in the hospital setting where they have been associated with outbreaks of nosocomial infections. Among them, Acinetobacter baumannii has emerged as the most common pathogenic species involved in hospital-acquired infections. One reason for this emergence may be its persistence in the hospital wards, in particular in the intensive care unit; this persistence could be partially explained by the capacity of these microorganisms to form biofilm. Therefore, our main objective was to study the prevalence of the two main types of biofilm formed by the most relevant Acinetobacter species, comparing biofilm formation between the different species. Findings Biofilm formation at the air-liquid and solid-liquid interfaces was investigated in different Acinetobacter spp. and it appeared to be generally more important at 25°C than at 37°C. The biofilm formation at the solid-liquid interface by the members of the ACB-complex was at least 3 times higher than the other species (80-91% versus 5-24%). In addition, only the isolates belonging to this complex were able to form biofilm at the air-liquid interface; between 9% and 36% of the tested isolates formed this type of pellicle. Finally, within the ACB-complex, the biofilm formed at the air-liquid interface was almost 4 times higher for A. baumannii and Acinetobacter G13TU than for Acinetobacter G3 (36%, 27% & 9% respectively). Conclusions Overall, this study has shown the capacity of the Acinetobacter spp to form two different types of biofilm: solid-liquid and air-liquid interfaces. This ability was generally higher at 25°C which might contribute to their persistence in the inanimate hospital environment. Our work has also demonstrated for the first time the ability of the members of the ACB-complex to form biofilm at the air-liquid interface, a feature that was not observed in other

  14. [The physics of pattern formation of liquid interfaces

    SciTech Connect

    Not Available

    1993-05-01

    Energy consumption in fabrication of materials for all applications is process dependent. Improvements in the ability to process materials are of great importance to the DOE mission. This project addresses basic science questions related to the processing of materials and is aimed at understanding growth of interfaces and evolution of patterns on interfaces, both macroscopic and microscopic. Three laboratory experiments are proposed: A study of the changes in patterns available to the growth of a macroscopic interface when that interface is grown over one of a variety of ``microscopic`` lattices; a study of reversible aggregation of colloidal particles in a mixed solvent, and of the interactions and relaxations of both solvent and suspended particles when thermodynamic conditions are changed for a liquid matrix with suspended particles or fibres; and, an investigation of the sedimentation of particles in a quasi-two-dimensional viscous fluid, with attention both to the dynamics of the flow and to the roughness of the resulting surface of settled particles.

  15. [The physics of pattern formation of liquid interfaces

    SciTech Connect

    Not Available

    1993-01-01

    Energy consumption in fabrication of materials for all applications is process dependent. Improvements in the ability to process materials are of great importance to the DOE mission. This project addresses basic science questions related to the processing of materials and is aimed at understanding growth of interfaces and evolution of patterns on interfaces, both macroscopic and microscopic. Three laboratory experiments are proposed: A study of the changes in patterns available to the growth of a macroscopic interface when that interface is grown over one of a variety of microscopic'' lattices; a study of reversible aggregation of colloidal particles in a mixed solvent, and of the interactions and relaxations of both solvent and suspended particles when thermodynamic conditions are changed for a liquid matrix with suspended particles or fibres; and, an investigation of the sedimentation of particles in a quasi-two-dimensional viscous fluid, with attention both to the dynamics of the flow and to the roughness of the resulting surface of settled particles.

  16. Interface Superconductivity in Cuprates Defies Fermi-Liquid Description

    DOE PAGES

    Radović, Zoran; Vanević, Mihajlo; Wu, Jie; ...

    2016-07-26

    La2-xSrxCuO4/La2CuO4 bilayers show interface superconductivity that originates from accumulation and depletion of mobile charge carriers across the interface. Surprisingly, the doping level can be varied broadly (within the interval 0.15 < x < 0.47) without affecting the transition temperature, which stays essentially constant and equal to that in optimally doped material, Tc ≈ 40 K. Here we argue that this finding implies that doping up to the optimum level does not shift the chemical potential, unlike in ordinary Fermi liquids. Lastly, we discuss possible physical scenarios that can give doping-independent chemical potential in the pseudogap regime: electronic phase separation, formationmore » of charge-density waves, strong Coulomb interactions, or self-trapping of mobile charge carriers.« less

  17. Low-reflection-coefficient liquid interfaces for system characterization.

    PubMed

    Hall, T J; Madsen, E L; Dong, F; Medina, I R; Frank, G R

    2001-07-01

    The use of liquid brominated hydrocarbons to form a planar reflecting interface with water is described. Gravity-based planar reflecting surfaces with known reflection coefficients can be used in system characterization for quantitative ultrasonics, and a set of surfaces with a range of reflection coefficients allows calibration of the output power and receiver gain of ultrasonic imaging systems. The substances reported here are immiscible in water and form interfaces with water, resulting in a broad range of acoustic reflection coefficients. Reflection coefficients were measured at temperatures from 18-24 degrees C for "pure" substances and for mixtures of two brominated hydrocarbons. Results show that reflection coefficients are weakly dependent on temperature and that, at a specific temperature, a significant range of arbitrarily small reflection coefficients is available, in the case of the mixtures, by the appropriate choice of weight-percents of the two brominated hydrocarbons.

  18. Interface Superconductivity in Cuprates Defies Fermi-Liquid Description

    SciTech Connect

    Radović, Zoran; Vanević, Mihajlo; Wu, Jie; Bollinger, Anthony T.; Božović, Ivan

    2016-07-26

    La2-xSrxCuO4/La2CuO4 bilayers show interface superconductivity that originates from accumulation and depletion of mobile charge carriers across the interface. Surprisingly, the doping level can be varied broadly (within the interval 0.15 < x < 0.47) without affecting the transition temperature, which stays essentially constant and equal to that in optimally doped material, Tc ≈ 40 K. Here we argue that this finding implies that doping up to the optimum level does not shift the chemical potential, unlike in ordinary Fermi liquids. Lastly, we discuss possible physical scenarios that can give doping-independent chemical potential in the pseudogap regime: electronic phase separation, formation of charge-density waves, strong Coulomb interactions, or self-trapping of mobile charge carriers.

  19. Interface Superconductivity in Cuprates Defies Fermi-Liquid Description

    SciTech Connect

    Radović, Zoran; Vanević, Mihajlo; Wu, Jie; Bollinger, Anthony T.; Božović, Ivan

    2016-07-26

    La2-xSrxCuO4/La2CuO4 bilayers show interface superconductivity that originates from accumulation and depletion of mobile charge carriers across the interface. Surprisingly, the doping level can be varied broadly (within the interval 0.15 < x < 0.47) without affecting the transition temperature, which stays essentially constant and equal to that in optimally doped material, Tc ≈ 40 K. Here we argue that this finding implies that doping up to the optimum level does not shift the chemical potential, unlike in ordinary Fermi liquids. Lastly, we discuss possible physical scenarios that can give doping-independent chemical potential in the pseudogap regime: electronic phase separation, formation of charge-density waves, strong Coulomb interactions, or self-trapping of mobile charge carriers.

  20. Electrovariable gold nanoparticle films at liquid-liquid interfaces: from redox electrocatalysis to Marangoni-shutters.

    PubMed

    Gschwend, Grégoire C; Smirnov, Evgeny; Peljo, Pekka; Girault, Hubert H

    2017-07-01

    Control over the physical properties of nanoparticle assemblies at a liquid-liquid interface is a key technological advancement to realize the dream of smart electrovariable nanosystems. Electrified interfaces, such as the interface between two immiscible electrolytes solutions (ITIES), are almost an ideal platform for realizing this dream. Here, we show that the Galvani potential difference across soft interfaces can be effectively used to manipulate: (i) the reactivity of gold nanoparticle assemblies through varying the Fermi level (both chemically and electrochemically); (ii) the location distribution of the nanoparticles at the liquid-liquid interface. In the first case, in addition to our previous studies on electron transfer reactions (ET) across the ITIES, we used intensity modulated photocurrent spectroscopy (IMPS) to study the kinetics of photo-induced electrochemical reactions at the ITIES. As expected, the direct adsorption of gold nanoparticles at the interface modifies the kinetics of the ET reaction (so-called, interfacial redox electrocatalysis), however it did not lead to an increased photocurrent by "plasmonic enhancement". Rather, we found that the product separation depends on double layer effects while the product recombination is controlled by the Galvani potential difference between the two phases. In the second case, we demonstrated that polarizing the ITIES caused migration of gold nanoparticles from the middle region of the cell to its periphery. We called such systems "Marangoni-type shutters". This type of electrovariable plasmonic system did not experience diffusion limitation in terms of the adsorption/desorption of nanoparticles and the entire movement of nanoparticle assemblies happened almost instantly (within a second). It opens a fresh view on electrovariable plasmonics and presents new opportunities to create smart nanosystems at the ITIES driven with an electric field.

  1. The excess proton at the air-water interface: The role of instantaneous liquid interfaces.

    PubMed

    Giberti, Federico; Hassanali, Ali A

    2017-06-28

    The magnitude of the pH of the surface of water continues to be a contentious topic in the physical chemistry of aqueous interfaces. Recent theoretical studies have shown little or no preference for the proton to be at the surface compared to the bulk. Using ab initio molecular dynamics simulations, we revisit the propensity of the excess proton for the air-water interface with a particular focus on the role of instantaneous liquid interfaces. We find a more pronounced presence for the proton to be at the air-water interface. The enhanced water structuring around the proton results in the presence of proton wires that run parallel to the surface as well as a hydrophobic environment made up of under-coordinated topological defect water molecules, both of which create favorable conditions for proton confinement at the surface. The Grotthuss mechanism within the structured water layer involves a mixture of both concerted and closely spaced stepwise proton hops. The proton makes excursions within the first solvation layer either in proximity to or along the instantaneous interface.

  2. The excess proton at the air-water interface: The role of instantaneous liquid interfaces

    NASA Astrophysics Data System (ADS)

    Giberti, Federico; Hassanali, Ali A.

    2017-06-01

    The magnitude of the pH of the surface of water continues to be a contentious topic in the physical chemistry of aqueous interfaces. Recent theoretical studies have shown little or no preference for the proton to be at the surface compared to the bulk. Using ab initio molecular dynamics simulations, we revisit the propensity of the excess proton for the air-water interface with a particular focus on the role of instantaneous liquid interfaces. We find a more pronounced presence for the proton to be at the air-water interface. The enhanced water structuring around the proton results in the presence of proton wires that run parallel to the surface as well as a hydrophobic environment made up of under-coordinated topological defect water molecules, both of which create favorable conditions for proton confinement at the surface. The Grotthuss mechanism within the structured water layer involves a mixture of both concerted and closely spaced stepwise proton hops. The proton makes excursions within the first solvation layer either in proximity to or along the instantaneous interface.

  3. High temperature interaction behavior at liquid metal-ceramic interfaces.

    SciTech Connect

    McDeavitt, S. M.; Billings, G. W.; Indacochea, J. E.; Chemical Engineering; Integrated Thermal Sciences, Inc.

    2002-08-01

    Liquid metal/ceramic interaction experiments were undertaken at elevated temperatures with the purpose of developing reusable crucibles for melting reactive metals. The metals used in this work included zirconium (Zr), Zr-8 wt.% stainless steel, and stainless steel containing 15 wt.% Zr. The ceramic substrates include yttria, Zr carbide, and hafnium (Hf) carbide. The metal-ceramic samples were placed on top of a tungsten (W) dish. These experiments were conducted with the temperature increasing at a controlled rate until reaching set points above 2000 C; the systems were held at the peak temperature for about five min and then cooled. The atmosphere in the furnace was argon (Ar). An outside video recording system was used to monitor the changes on heating up and cooling down. All samples underwent a post-test metallurgical examination. Pure Zr was found to react with yttria, resulting in oxygen (O) evolution at the liquid metal-ceramic interface. In addition, dissolved O was observed in the as-cooled Zr metal. Yttrium (Y) was also present in the Zr metal, but it had segregated to the grain boundaries on cooling. Despite the normal expectations for reactive wetting, no transition interface was developed, but the Zr metal was tightly bound to yttria ceramic. Similar reactions occurred between the yttria and the Zr-stainless steel alloys. Two other ceramic samples were Zr carbide and Hf carbide; both carbide substrates were wetted readily by the molten Zr, which flowed easily to the sides of the substrates. The molten Zr caused a very limited dissolution of the Zr carbide, and it reacted more strongly with the Hf carbide. These reactive wetting results are relevant to the design of interfaces and the development of reactive filler metals for the fabrication of high temperature components through metal-ceramic joining. Parameters that have a marked impact on this interface reaction include the thermodynamic stability of the substrate, the properties of the modified

  4. Temperature and Depth Dependence of Order in Liquid Crystal Interfaces

    SciTech Connect

    Martinez-Miranda,L.; Hu, Y.

    2006-01-01

    We have studied the depth dependence and temperature behavior of the ordering of smectic-A films close to the smectic A-nematic transition, deposited on grated glass. X-ray grazing incidence geometry in reflection mode through the glass substrate was used to characterize the samples. Our results indicate the presence of a structure similar to the helical twist grain boundary phase. The structure has two maxima, one close to the glass-liquid crystal interface and another about 8 {mu}m above the surface. The structure at 8 {mu}m is the one that dominates at higher temperatures. In addition, we find that order is preserved to temperatures close to the nematic-isotropic transition temperature for the deeper gratings. We find also a dependence of the orientation of the structure with the depth of the grating and the elastic constant of the liquid crystal.

  5. Liquid bridges at the root-soil interface

    NASA Astrophysics Data System (ADS)

    Carminati, Andrea; Benard, Pascal; Ahmed, Mutez; Zarebanadkouki, Mohsen

    2017-04-01

    The role of the root-soil interface on soil-plant water relations is unclear. Despite many experimental studies proved that the soil close to the root surface, the rhizosphere, has different properties compared to the adjacent bulk soil, the mechanisms underlying such differences are poorly understood and the implications for plant-water relations remain largely speculative. The objective of this contribution is to discuss the key elements affecting water dynamics in the rhizosphere. Special attention is dedicated to the role of mucilage exuded by roots in shaping the hydraulic properties of the rhizosphere. We identified three key properties: 1) mucilage adsorbs water decreasing its water potential; 2) mucilage decreases the surface tension of the soil solution; 3) mucilage increases the viscosity of the soil solution. These three properties determine the retention and spatial configuration of the liquid phase in porous media. The increase in viscosity and the decrease in surface tension (quantified by the Ohnesorge number) allow the persistence of long liquid filaments even at very negative water potentials. At high mucilage concentrations these filaments form a network that creates an additional matric potential and maintains the continuity of the liquid phase during drying. The biophysical interactions between mucilage and the pore space determine the physical properties of the rhizosphere. Mucilage forms a network that provides mechanical stability to soils upon drying and that maintains the continuity of the liquid phase across the soil-root interface. Such biophysical properties are functional to create an interconnected matrix that maintains the roots in contact with the soil, which is of particular importance when the soil is drying and the transpiration rate is high.

  6. Non-lamellar lipid liquid crystalline structures at interfaces.

    PubMed

    Chang, Debby P; Barauskas, Justas; Dabkowska, Aleksandra P; Wadsäter, Maria; Tiberg, Fredrik; Nylander, Tommy

    2015-08-01

    The self-assembly of lipids leads to the formation of a rich variety of nano-structures, not only restricted to lipid bilayers, but also encompassing non-lamellar liquid crystalline structures, such as cubic, hexagonal, and sponge phases. These non-lamellar phases have been increasingly recognized as important for living systems, both in terms of providing compartmentalization and as regulators of biological activity. Consequently, they are of great interest for their potential as delivery systems in pharmaceutical, food and cosmetic applications. The compartmentalizing nature of these phases features mono- or bicontinuous networks of both hydrophilic and hydrophobic domains. To utilize these non-lamellar liquid crystalline structures in biomedical devices for analyses and drug delivery, it is crucial to understand how they interact with and respond to different types of interfaces. Such non-lamellar interfacial layers can be used to entrap functional biomolecules that respond to lipid curvature as well as the confinement. It is also important to understand the structural changes of deposited lipid in relation to the corresponding bulk dispersions. They can be controlled by changing the lipid composition or by introducing components that can alter the curvature or by deposition on nano-structured surface, e.g. vertical nano-wire arrays. Progress in the area of liquid crystalline lipid based nanoparticles opens up new possibilities for the preparation of well-defined surface films with well-defined nano-structures. This review will focus on recent progress in the formation of non-lamellar dispersions and their interfacial properties at the solid/liquid and biologically relevant interfaces. Copyright © 2014. Published by Elsevier B.V.

  7. The liquid-liquid interface as a medium to generate nanocrystalline films of inorganic materials.

    PubMed

    Rao, C N R; Kalyanikutty, K P

    2008-04-01

    Unlike the air-water interface, the organic-aqueous (liquid-liquid) interface has not been exploited sufficiently for materials synthesis. In this Account, we demonstrate how ultrathin nanocrystalline films of metals such as gold and silver as well as of inorganic materials such as semiconducting metal chalcogenides (e.g., CdS, CuS, CdSe) and oxides are readily generated at the liquid-liquid interface. What is particularly noteworthy is that single-crystalline films of certain metal chalcogenides are also obtained by this method. The as-prepared gold films at the toluene-water interface comprise fairly monodisperse nanocrystals that are closely packed, the nature and properties of the films being influenced by various reaction parameters such as reaction temperature, time, reactant concentrations, mechanical vibrations, and the viscosity of the medium. The surface plasmon band of gold is markedly red-shifted in the films due to electronic coupling between the particles. The shift of the surface plasmon band of the Au film toward higher wavelengths with an accompanying increase in intensity as a function of reaction time marks the growth of the film. Depending on the reaction temperature, the Au films show interesting electrical transport properties. Films of metals such as gold are disintegrated by the addition of alkanethiols, the effectiveness depending on the alkane chain length, clearly evidenced by shifts of the surface plasmon bands. A time evolution study of the polycrystalline Au and CdS films as well as the single-crystalline CuS films is carried out by employing atomic force microscopy. X-ray reflectivity studies reveal the formation of a monolayer of capped clusters having 13 gold atoms each, arranged in a hexagonal manner at the toluene-water interface. The measurements also reveal an extremely small value of the interfacial tension. Besides describing features of such nanocrystalline films and their mode of formation, their rheological properties have

  8. Ionic Liquid Anion Controlled Nanoscale Gold Morphology Grown at a Liquid Interface.

    PubMed

    Bhawawet, Nakara; Essner, Jeremy B; Wagle, Durgesh V; Baker, Gary A

    2017-06-20

    Two different ionic liquids comprising the tetrabutylphosphonium cation ([P4444]) paired with the strongly coordinating anions 6-aminocaproate ([6-AC]) or taurinate ([tau]) were prepared and employed in an aqueous/organic liquid bilayer system to generate nanoscale gold by Au(OH)4(-) photoreduction. Generally, as the concentration of ionic liquid in the organic phase was increased, the resulting quasi-spherical gold nanoparticles were smaller in size and presented less aggregation, leading to marked increases in the catalytic efficiency for 4-nitrophenol reduction using borohydride. The diffusion of the ionic liquids across the liquid/liquid interface was also investigated, revealing partition coefficients of 6.0 and 7.6 for [P4444][6-AC] and [P4444][tau], respectively. Control studies elucidated that biphasic interfacial reduction was necessary to achieve stable nanoparticles possessing high catalytic activity. When the ionic liquid anion was instead replaced by the weakly coordinating bis(trifluoromethylsulfonyl)imide ([Tf2N]), photoreduction of Au(OH)4(-) led to holey, wavy gold nanowires instead of spherical nanoparticles, indicating the dramatic morphological control exerted by the coordination strength of the ionic liquid anion. This strategy is straightforward and simple and opens up a number of intriguing avenues for controllably preparing plasmonic colloids for a range of applications from catalysis to optical sensing.

  9. Computer simulation of liquid/liquid interfaces. I. Theory and application to octane/water

    NASA Astrophysics Data System (ADS)

    Zhang, Yuhong; Feller, Scott E.; Brooks, Bernard R.; Pastor, Richard W.

    1995-12-01

    Statistical ensembles for simulating liquid interfaces at constant pressure and/or surface tension are examined, and equations of motion for molecular dynamics are obtained by various extensions of the Andersen extended system approach. Valid ensembles include: constant normal pressure and surface area; constant tangential pressure and length normal to the interface; constant volume and surface tension; and constant normal pressure and surface tension. Simulations at 293 K and 1 atm normal pressure show consistent results with each other and with a simulation carried out at constant volume and energy. Calculated surface tensions for octane/water (61.5 dyn/cm), octane/vacuum (20.4 dyn/cm) and water/vacuum (70.2 dyn/cm) are in very good agreement with experiment (51.6, 21.7, and 72.8 dyn/cm, respectively). The practical consequences of simulating with two other approaches commonly used for isotropic systems are demonstrated on octane/water: applying equal normal and tangential pressures leads to an instability; and applying a constant isotropic pressure of 1 atm leads to a large positive normal pressure. Both results are expected for a system of nonzero surface tension. Mass density and water polarization profiles in the liquid/liquid and liquid/vapor interfaces are also compared.

  10. Thermoelectric energy recovery at ionic-liquid/electrode interface

    NASA Astrophysics Data System (ADS)

    Bonetti, Marco; Nakamae, Sawako; Huang, Bo Tao; Salez, Thomas J.; Wiertel-Gasquet, Cécile; Roger, Michel

    2015-06-01

    A thermally chargeable capacitor containing a binary solution of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)-imide in acetonitrile is electrically charged by applying a temperature gradient to two ideally polarisable electrodes. The corresponding thermoelectric coefficient is -1.7 mV/K for platinum foil electrodes and -0.3 mV/K for nanoporous carbon electrodes. Stored electrical energy is extracted by discharging the capacitor through a resistor. The measured capacitance of the electrode/ionic-liquid interface is 5 μF for each platinum electrode while it becomes four orders of magnitude larger, ≈36 mF, for a single nanoporous carbon electrode. Reproducibility of the effect through repeated charging-discharging cycles under a steady-state temperature gradient demonstrates the robustness of the electrical charging process at the liquid/electrode interface. The acceleration of the charging by convective flows is also observed. This offers the possibility to convert waste-heat into electric energy without exchanging electrons between ions and electrodes, in contrast to what occurs in most thermogalvanic cells.

  11. Toxicity of Silver Nanoparticles at the Air-Liquid Interface

    PubMed Central

    Holder, Amara L.; Marr, Linsey C.

    2013-01-01

    Silver nanoparticles are one of the most prevalent nanomaterials in consumer products. Some of these products are likely to be aerosolized, making silver nanoparticles a high priority for inhalation toxicity assessment. To study the inhalation toxicity of silver nanoparticles, we have exposed cultured lung cells to them at the air-liquid interface. Cells were exposed to suspensions of silver or nickel oxide (positive control) nanoparticles at concentrations of 2.6, 6.6, and 13.2 μg cm−2 (volume concentrations of 10, 25, and 50 μg ml−1) and to 0.7 μg cm−2 silver or 2.1 μg cm−2 nickel oxide aerosol at the air-liquid interface. Unlike a number of in vitro studies employing suspensions of silver nanoparticles, which have shown strong toxic effects, both suspensions and aerosolized nanoparticles caused negligible cytotoxicity and only a mild inflammatory response, in agreement with animal exposures. Additionally, we have developed a novel method using a differential mobility analyzer to select aerosolized nanoparticles of a single diameter to assess the size-dependent toxicity of silver nanoparticles. PMID:23484109

  12. Universal electrode interface for electrocatalytic oxidation of liquid fuels.

    PubMed

    Liao, Hualing; Qiu, Zhipeng; Wan, Qijin; Wang, Zhijie; Liu, Yi; Yang, Nianjun

    2014-10-22

    Electrocatalytic oxidations of liquid fuels from alcohols, carboxylic acids, and aldehydes were realized on a universal electrode interface. Such an interface was fabricated using carbon nanotubes (CNTs) as the catalyst support and palladium nanoparticles (Pd NPs) as the electrocatalysts. The Pd NPs/CNTs nanocomposite was synthesized using the ethylene glycol reduction method. It was characterized using transmission electron microscopy, energy dispersive X-ray spectroscopy, X-ray diffraction, voltammetry, and impedance. On the Pd NPs/CNTs nanocomposite coated electrode, the oxidations of those liquid fuels occur similarly in two steps: the oxidations of freshly chemisorbed species in the forward (positive-potential) scan and then, in the reverse scan (negative-potential), the oxidations of the incompletely oxidized carbonaceous species formed during the forward scan. The oxidation charges were adopted to study their oxidation mechanisms and oxidation efficiencies. The oxidation efficiency follows the order of aldehyde (formaldehyde) > carboxylic acid (formic acid) > alcohols (ethanol > methanol > glycol > propanol). Such a Pd NPs/CNTs nanocomposite coated electrode is thus promising to be applied as the anode for the facilitation of direct fuel cells.

  13. Detection of solvated electrons at a plasma-liquid interface

    NASA Astrophysics Data System (ADS)

    Go, David B.; Rumbach, Paul; Bartels, David; Sankaran, R. Mohan

    2014-10-01

    We have recently shown that charge can be transferred from a DC microplasma jet into an aqueous solution to promote electrolytic reduction reactions [1,2]. However, the precise nature of these charge transfer reactions remains poorly understood---in particular, it is not known if plasma electrons solvate and solvated electrons are responsible for the reduction of solution species. To address these questions, we have designed and built an optical absorption spectroscopy system to directly detect solvated electrons at a plasma-liquid interface, which only have a lifetime of ~1 μs. Our preliminary results reveal that plasma electrons do indeed solvate, and survive up to depths of approximately 0.5 nm beneath the plasma-liquid interface. Adding electron scavengers such as nitrite and nitrate salts to the solution causes a decrease in optical absorption, indicating a decrease in the average lifetime of the solvated electrons, further confirming their existence. Measuring optical absorption as a function of scavenger concentration, we extrapolate rate constants that agree well with prior radiolysis experiments. These preliminary findings are consistent with the hypothesis that free electrons from atmospheric pressure plasmas solvate in aqueous solutions, and open potential applications of plasmas for solvated electron chemistry.

  14. Liquid chromatography/Fourier transform IR spectrometry interface flow cell

    DOEpatents

    Johnson, Charles C.; Taylor, Larry T.

    1986-01-01

    A zero dead volume (ZDV) microbore high performance liquid chromatography (.mu.HPLC)/Fourier transform infrared (FTIR) interface flow cell includes an IR transparent crystal having a small diameter bore therein through which a sample liquid is passed. The interface flow cell further includes a metal holder in combination with a pair of inner, compressible seals for directly coupling the thus configured spectrometric flow cell to the outlet of a .mu.HPLC column end fitting to minimize the transfer volume of the effluents exiting the .mu.HPLC column which exhibit excellent flow characteristics due to the essentially unencumbered, open-flow design. The IR beam passes transverse to the sample flow through the circular bore within the IR transparent crystal, which is preferably comprised of potassium bromide (KBr) or calcium fluoride (CaF.sub.2), so as to minimize interference patterns and vignetting encountered in conventional parallel-plate IR cells. The long IR beam pathlength and lensing effect of the circular cross-section of the sample volume in combination with the refractive index differences between the solvent and the transparent crystal serve to focus the IR beam in enhancing sample detection sensitivity by an order of magnitude.

  15. Thermoelectric energy recovery at ionic-liquid/electrode interface

    SciTech Connect

    Bonetti, Marco; Nakamae, Sawako; Huang, Bo Tao; Wiertel-Gasquet, Cécile; Roger, Michel; Salez, Thomas J.

    2015-06-28

    A thermally chargeable capacitor containing a binary solution of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)-imide in acetonitrile is electrically charged by applying a temperature gradient to two ideally polarisable electrodes. The corresponding thermoelectric coefficient is −1.7 mV/K for platinum foil electrodes and −0.3 mV/K for nanoporous carbon electrodes. Stored electrical energy is extracted by discharging the capacitor through a resistor. The measured capacitance of the electrode/ionic-liquid interface is 5 μF for each platinum electrode while it becomes four orders of magnitude larger, ≈36 mF, for a single nanoporous carbon electrode. Reproducibility of the effect through repeated charging-discharging cycles under a steady-state temperature gradient demonstrates the robustness of the electrical charging process at the liquid/electrode interface. The acceleration of the charging by convective flows is also observed. This offers the possibility to convert waste-heat into electric energy without exchanging electrons between ions and electrodes, in contrast to what occurs in most thermogalvanic cells.

  16. Liquid chromatography/Fourier transform IR spectrometry interface flow cell

    DOEpatents

    Johnson, C.C.; Taylor, L.T.

    1985-01-04

    A zero dead volume (ZDV) microbore high performance liquid chromatography (..mu.. HPLC)/Fourier transform infrared (FTIR) interface flow cell includes an IR transparent crystal having a small diameter bore therein through which a sample liquid is passed. The interface flow cell further includes a metal holder in combination with a pair of inner, compressible seals for directly coupling the thus configured spectrometric flow cell to the outlet of a ..mu.. HPLC column end fitting to minimize the transfer volume of the effluents exiting the ..mu.. HPLC column which exhibit excellent flow characteristics due to the essentially unencumbered, open-flow design. The IR beam passes transverse to the sample flow through the circular bore within the IR transparent crystal, which is preferably comprised of potassium bromide (KBr) or calcium fluoride (CaF/sub 2/), so as to minimize interference patterns and vignetting encountered in conventional parallel-plate IR cells. The long IR beam pathlength and lensing effect of the circular cross-section of the sample volume in combination with the refractive index differences between the solvent and the transparent crystal serve to focus the IR beam in enhancing sample detection sensitivity by an order of magnitude.

  17. Second harmonic generation studies of adsorption at a liquid-liquid electrochemical interface

    SciTech Connect

    Higgins, D.A.; Corn, R.M. )

    1993-01-14

    The technique of optical second harmonic generation (SHG) is applied to the measurement of molecular adsorption at the interface between two immiscible electrolyte solutions (ITIES). The resonant second harmonic response from 2-(n-octadecylamino) naphthalene-6-sulfonate (ONS) is used in conjunction with interfacial tension measurements to optically determine the relative surface coverage of the anionic surfactant molecule at a charged water-dichloroethane interface. At a pH of 9, ONS adsorption occurs at all potentials positive of the potential of zero charge. The potential-dependent adsorption of ONS can be described by a Frumkin isotherm with a free energy of adsorption that varies linearly with applied potential. The potential dependence of the SHG from the interface provides important information on the position of the adsorbed ONS molecules with respect to the ITIES. At a pH of 3, both the anionic form of ONS and the protonated zwitterionic form of ONS are present at the liquid-liquid interface. At very positive potentials, the anionic ONS at the interface undergoes a field-dependent conversion to the zwitterionic form. 32 refs., 6 figs.

  18. Advanced Technology Development: Solid-Liquid Interface Characterization Hardware

    NASA Technical Reports Server (NTRS)

    2003-01-01

    Characterizing the solid-liquid interface during directional solidification is key to understanding and improving material properties. The goal of this Advanced Technology Development (ATD) has been to develop hardware, which will enable real-time characterization of practical materials, such as aluminum (Al) alloys, to unprecedented levels. Required measurements include furnace and sample temperature gradients, undercooling at the growing interface, interface shape, or morphology, and furnace translation and sample growth rates (related). These and other parameters are correlated with each other and time. A major challenge was to design and develop all of the necessary hardware to measure the characteristics, nearly simultaneously, in a smaller integral furnace compatible with existing X-ray Transmission Microscopes, XTMs. Most of the desired goals have been accomplished through three generations of Seebeck furnace brassboards, several varieties of film thermocouple arrays, heaters, thermal modeling of the furnaces, and data acquisition and control (DAC) software. Presentations and publications have resulted from these activities, and proposals to use this hardware for further materials studies have been submitted as sequels to this last year of the ATD.

  19. Nematic liquid crystals at rough and fluctuating interfaces.

    PubMed

    Elgeti, J; Schmid, F

    2005-12-01

    Nematic liquid crystals at rough and fluctuating interfaces are analyzed within the Frank elastic theory and the Landau-de Gennes theory. We study specifically interfaces that locally favor planar anchoring. In the first part we reconsider the phenomenon of Berreman anchoring on fixed rough surfaces, and derive new simple expressions for the corresponding azimuthal anchoring energy. Surprisingly, we find that for strongly aligning surfaces, it depends only on the geometrical surface anisotropy and the bulk elastic constants, and not on the precise values of the chemical surface parameters. In the second part, we calculate the capillary waves at nematic-isotropic interfaces. If one neglects elastic interactions, the capillary wave spectrum is characterized by an anisotropic interfacial tension. With elastic interactions, the interfacial tension, i.e., the coefficient of the leading q(2) term of the capillary wave spectrum, becomes isotropic. However, the elastic interactions introduce a strongly anisotropic cubic q(3) term. The amplitudes of capillary waves are largest in the direction perpendicular to the director. These results are in agreement with previous molecular dynamics simulations.

  20. Giant Deformations of a Liquid-Liquid Interface Induced by the Optical Radiation Pressure

    SciTech Connect

    Casner, Alexis; Delville, Jean-Pierre

    2001-07-30

    Because of the small momentum of photons, very intense fields are generally required to bend a liquid interface with the optical radiation pressure. We explore this issue in a near-critical phase-separated liquid mixture to vary continuously the meniscus softness by tuning the temperature. Low power continuous laser waves become sufficient to induce huge stationary bulges. Using the beam size to build an ''optical'' Bond number, Bo , we investigate the crossover from low to large Bo . The whole set of data collapses onto a single master curve which illustrates the universality of the phenomenon.

  1. A general strategy for self-assembly of nanosized building blocks on liquid/liquid interfaces.

    PubMed

    Liu, Jian-Wei; Zhang, Shao-Yi; Qi, Hao; Wen, Wu-Cheng; Yu, Shu-Hong

    2012-08-06

    A family of water/oil interfaces is introduced to provide effective platforms for rapid fabrication of large-area self-assembled nanofilms composed of various nanosized building blocks, including nanoparticles (NPs), nanocubes (NC), nanowires (NWs), and nanosheets, at room temperature. As a general interfacial assembly method, NWs and NPs are co-assembled at the liquid/liquid interface. The as-prepared co-assembled Ag NW and Ag NC films show high surface-enhanced Raman spectroscopy (SERS) intensity, the SERS performance being strongly dependent on the number ratio of the two kinds of nanosized building blocks. The results demonstrate that this interfacial system provides a general method for the assembly of various nanosized building blocks with different shapes and dimensionalities, and thus paves an alternative pathway for further applications of macroscopic assemblies with different functionalities.

  2. Electrostatic Assembly of Polymers and Nanoparticles at Liquid-Liquid Interfaces

    NASA Astrophysics Data System (ADS)

    Hoagland, David

    The electrostatic attraction between charged solutes on opposite sides of the interface between immiscible liquids offers an efficient route to the self-assembly of two-dimensional films. As implemented by us, a hydrophobic polymer with amine end(s) or block(s) is presented in an oil phase, and a negatively charged nanoparticle is presented in an aqueous phase; both solutes are insoluble in the opposite phase but efficiently driven to the liquid-liquid interface by mutual electrostatically attraction to the solute in the opposite phase. Depending on experimental conditions (salt concentration, pH, solute concentrations, etc.), a continuous, nanoscopically thin composite film builds at the oil-water interface over the timescale of minutes, often accompanied by a dramatic reduction of interfacial tension akin to that observed for a surfactant. Film formation and properties by the new route will be discussed, as principally probed through pendant drop interfacial tensiometry and pendant drop interfacial rheometry. Components of model system are toluene-dissolved amine end-capped polystyrene and water-dispersed acid-treated carbon nanotubes or citrate-treated gold nanospheres. Film structures are complicated, as are crucial electrostatic interactions near the interface. With amine end-capped polystyrene partnered with acid-treated carbon nanotubes, high pH (above 5) and high polystyrene molecular weight (above 5000 g/mol) strongly hinder film formation. These films, which are liquid-like, show two viscoelastic relaxations, a fast relaxation (about 10 s) associated with polystyrene chain rearrangements (slightly impacted by carbon nanotube association) and a slow relaxation (about 20 min) associated with polystyrene adsorption/desorption; at intermediate times (or frequencies), the two-dimensional storage and loss moduli follow approximately the same power law dependences. Support by NSF through the Univ. of Massachusetts MRSEC.

  3. Anisotropic Self-Assembly of Supramolecular Polymers and Plasmonic Nanoparticles at the Liquid-Liquid Interface.

    PubMed

    Armao Iv, Joseph J; Nyrkova, Irina; Fuks, Gad; Osypenko, Artem; Maaloum, Mounir; Moulin, Emilie; Arenal, Raul; Gavat, Odile; Semenov, Alexander; Giuseppone, Nicolas

    2017-02-15

    The study of supramolecular polymers in the bulk, in diluted solution, and at the solid-liquid interface has recently become a major topic of interest, going from fundamental aspects to applications in materials science. However, examples of supramolecular polymers at the liquid-liquid interface are mostly unexplored. Here, we describe the supramolecular polymerization of triarylamine molecules and their light-triggered organization at a chloroform-water interface. The resulting interfacial nematic layer of these 1D supramolecular polymers is further used as a template for the precise alignment of spherical gold nanoparticles coming from the water phase. These hybrid thin films are spontaneously formed in a single process, without chemical prefunctionalization of the metallic nanoparticles, and their ordering is improved by centrifugation. The resulting polymer chains and strings of nanoparticles can be co-aligned with high anisotropy over very large distances. By using a combination of experimental and theoretical investigations, we decipher the full sequence of this oriented self-assembly process. In such a highly anisotropic configuration, electron energy loss spectroscopy reveals that the self-assembled nanoparticles behave as plasmonic waveguides.

  4. Solvent Extraction: Structure of the Liquid-Liquid Interface Containing a Diamide Ligand

    SciTech Connect

    Scoppola, Ernesto; Campbell, Richard A.; Konovalov, Oleg; Girard, Luc; Fragneto, Giovanna; Diat, Olivier

    2016-06-20

    Knowledge of the (supra)molecular structure of an interface that contains amphiphilic ligand molecules is necessary for a full understanding of ion transfer during solvent extraction. Even if molecular dynamics already yield some insight in the molecular configurations in solution, hardly any experimental data giving access to distributions of both extractant molecules and ions at the liquid–liquid interface exist. Here, the combined application of X-ray and neutron reflectivity measurements represents a key milestone in the deduction of the interfacial structure and potential with respect to two different lipophilic ligands. Indeed, we show for the first time that hard trivalent cations can be repelled or attracted by the extractant-enriched interface according to the nature of the ligand.

  5. Ion-transfer voltammetric behavior of propranolol at nanoscale liquid-liquid interface arrays.

    PubMed

    Liu, Yang; Strutwolf, Jörg; Arrigan, Damien W M

    2015-04-21

    In this work, the ion-transfer voltammetric detection of the protonated β-blocker propranolol was explored at arrays of nanoscale interfaces between two immiscible electrolyte solutions (ITIES). Silicon nitride nanoporous membranes with 400 pores in a hexagonal arrangement, with either 50 or 17 nm radius pores, were used to form regular arrays of nanoITIES. It was found that the aqueous-to-organic ion-transfer current continuously increased steadily rather than reaching a limiting current plateau after the ion-transfer wave; the slope of this limiting current region was concentration dependent and associated with the high ion flux at the nanointerfaces. Electrochemical data were examined in terms of an independent nanointerface approach and an equivalent microdisc approach, supported by finite element simulation. In comparison to the larger interface configuration (50 nm radius), the array of 17 nm radius nanoITIES exhibited a 6.5-times higher current density for propranolol detection due to the enhanced ion flux arising from the convergent diffusion to smaller electrochemical interfaces. Both nanoITIES arrays achieved the equivalent limits of detection, 0.8 μM, using cyclic voltammetry. Additionally, the effect of scan rate on the charging and faradaic currents at these nanoITIES arrays, as well as their stability over time, was investigated. The results demonstrate that arrays of nanoscale liquid-liquid interfaces can be applied to study electrochemical drug transfer, and provide the basis for the development of miniaturized and integrated detection platforms for drug analysis.

  6. Surface plasmon resonance of gold nanoparticles assemblies at liquid | liquid interfaces.

    PubMed

    Hojeij, Mohamad; Younan, Nathalie; Ribeaucourt, Lydie; Girault, Hubert H

    2010-09-01

    Surface plasmon resonance (SPR) was observed when a planar close-packed assembly of gold nanoparticles (Au NPs) is adsorbed at the water|1,2-dichloroethane interface. Aqueous gold nanoparticles, 13 or 16 nm in diameter, are deposited at the interface by adding methanol to form a close-packed film with a visible gold mirror reflectance. By total internal reflection of a light beam on the interface, the angular dependence of the interfacial reflectivity was measured in a pseudo-Kretschmann configuration and compared to Fresnel simulations for a homogeneous gold film. The experimental angles for minimum reflectivity were found to match the simulated values. Then, the fluorescence of dye molecules co-adsorbed within 13 and 16 nm gold nanoparticles assemblies at the liquid|liquid interface was measured. The fluorescence intensity under SPR is revealed to be much greater than under total internal reflection conditions, yielding an enhancement factor of approximately 30 and 50 for 13 and 16 nm Au NPs assemblies, respectively. Also, the fluorescence lifetime was found to decrease under SPR conditions.

  7. Thermodynamics and intrinsic structure of the Al-Pb liquid-liquid interface: a molecular dynamics simulation study.

    PubMed

    Yang, Yang; Laird, Brian B

    2014-07-17

    We examine the thermodynamics and intrinsic structure of the Al-Pb liquid-liquid interface using molecular dynamics simulation and embedded atom method potentials. The instantaneous interfacial positions, from which the intrinsic structure and the capillary fluctuation spectrum are determined, are calculated using a grid-based method. The interfacial free energy extracted from the capillary fluctuation spectrum is shown to be in excellent agreement with that calculated mechanically by integrating the stress profile. The intrinsic liquid-liquid interfacial density profile shows structural oscillations in the liquid phases in the interfacial region that are shown to be quantitatively similar to the radial distribution functions of the bulk liquid, consistent with theoretical predictions from classical density functional theory and with earlier simulations on liquid-liquid and liquid-vapor interfaces. In addition, we show the mean interfacial density profile for this system is well described as a convolution of the intrinsic density profile and the probability distribution of interfacial position.

  8. Air-Liquid Interface Cell Exposures to Nanoparticle Aerosols.

    PubMed

    Lewinski, Nastassja A; Liu, Nathan J; Asimakopoulou, Akrivi; Papaioannou, Eleni; Konstandopoulos, Athanasios; Riediker, Michael

    2017-01-01

    The field of nanomedicine is steadily growing and several nanomedicines are currently approved for clinical use with even more in the pipeline. Yet, while the use of nanotechnology to improve targeted drug delivery to the lungs has received some attention, the use of nanoparticles for inhalation drug delivery has not yet resulted in successful translation to market as compared to intravenous drug delivery. The reasons behind the lack of inhaled nanomedicines approved for clinical use or under preclinical development are unclear, but challenges related to safety are likely to contribute. Although inhalation toxicology studies often begin using animal models, there has been an increase in the development and use of in vitro air-liquid interface (ALI) exposure systems for toxicity testing of engineered nanoparticle aerosols, which will be useful for rapid testing of candidate substances and formulations. This chapter describes an ALI cell exposure assay for measuring toxicological effects, specifically cell viability and oxidative stress, resulting from exposure to aerosols containing nanoparticles.

  9. Metal ion adsorption at the ionic liquid-mica interface

    NASA Astrophysics Data System (ADS)

    McDonald, Samila; Elbourne, Aaron; Warr, Gregory G.; Atkin, Rob

    2015-12-01

    Mica has been employed in many studies of ionic liquid (IL) interfaces on account of its atomic smoothness and well defined surface properties. However, until now it has been unclear whether ions dissolved in ILs can compete with the IL cation and adsorb to mica charge sites. In this work amplitude modulated atomic force microscopy (AM-AFM) has been used to probe metal ion adsorption at the interface of mica with propylammonium nitrate (PAN), a room temperature IL. Lithium, sodium, potassium, magnesium and calcium nitrate salts were added to PAN at a concentration of ~60 mM. Aluminum nitrate was also investigated, but only at 5 mM because its solubility in PAN is much lower. The AM-AFM images obtained when the metal ions were present are strikingly different to that of pure PAN, indicating that the ions compete effectively with the propylammonium cation and adsorb to negatively charged sites on the mica surface despite their much lower concentration. This is a consequence of electrostatic attractions between the mica charge sites and the metal ions being significantly stronger than for the propylammonium cation; compared to the metal ions the propylammonium charged group is relatively constrained sterically. A distinct honeycomb pattern is noted for the PAN + Al3+ system, less obviously for the divalent ions and not at all for monovalent ions. This difference is attributed to the strength of electrostatic interactions between metal ions and mica charge sites increasing with the ion charge, which means that divalent and (particularly) trivalent ions are located more precisely above the charged sites of the mica lattice. The images obtained allow important distinctions between metal ion adsorption at mica-water and mica-PAN interfaces to be made.Mica has been employed in many studies of ionic liquid (IL) interfaces on account of its atomic smoothness and well defined surface properties. However, until now it has been unclear whether ions dissolved in ILs can compete

  10. Patterned surface anchoring of nematic droplets at miscible liquid-liquid interfaces.

    PubMed

    Wang, Xiaoguang; Zhou, Ye; Kim, Young-Ki; Miller, Daniel S; Zhang, Rui; Martinez-Gonzalez, Jose A; Bukusoglu, Emre; Zhang, Bo; Brown, Thaddeus M; de Pablo, Juan J; Abbott, Nicholas L

    2017-08-30

    We report on the internal configurations of droplets of nematic liquid crystals (LCs; 10-50 μm-in-diameter; comprised of 4-cyano-4'-pentylbiphenyl and 4-(3-acryloyloxypropyloxy)benzoic acid 2-methyl-1,4-phenylene ester) sedimented from aqueous solutions of sodium dodecyl sulfate (SDS) onto interfaces formed with pure glycerol. We observed a family of internal LC droplet configurations and topological defects consistent with a remarkably abrupt transition from homeotropic (perpendicular) to tangential anchoring on the surface of the LC droplets in the interfacial environment. Calculations of the interdiffusion of water and glycerol at the aqueous-glycerol interface revealed the thickness of the diffuse interfacial region of the two miscible liquids to be small (0.2-0.5 μm) compared to the diameters of the LC droplets on the experimental time-scale (15-120 minutes), leading us to hypothesize that the patterned surface anchoring was induced by gradients in concentration of SDS and glycerol across the diameter of the LC droplets in the interfacial region. This hypothesis received additional support from experiments in which the time of sedimentation of the LC droplets onto the interface was systematically increased and the droplets were photo-polymerized to preserve their configurations: the configurations of the LC droplets were consistent with a time-dependent decrease in the fraction of the surface area of each droplet exhibiting homeotropic anchoring. Specifically, LC droplets with <10% surface area with tangential anchoring exhibited a bulk point defect within the LC droplet, whereas droplets with >10% surface area with tangential anchoring exhibited a boojum defect within the tangential region and a disclination loop separated the regions with tangential and homeotropic anchoring. The topological charge of these LC droplet configurations was found to be consistent with the geometrical theorems of Poincaré and Gauss and also well-described by computer

  11. Solid-Liquid Interface Characterization Hardware: Advanced Technology Development (ATD)

    NASA Technical Reports Server (NTRS)

    Peters, Palmer N.; Sisk, R. C.; Sen, S.; Kaukler, W. F.; Curreri, Peter A.; Wang, F. C.; Rose, M. Franklin (Technical Monitor)

    2000-01-01

    This ATD has the goal of enabling the integration of three separate measurement techniques to characterize the solid-liquid interface of directionally solidified materials in real-time. Arrays of film-based metal thermocouple elements are under development along with compact Seebeck furnaces suitable for interfacing with separately developed X-ray Transmission Microscopes. Results of applying film arrays to furnace profiling are shown, demonstrating their ability to identify a previously undetected hardware flaw in the development of a second-generation compact furnace. Results of real-time furnace profiling also confirmed that the compact furnace design effectively isolates the temperature profiles in two halves of the furnace, a necessary feature. This isolation had only been inferred previously from the characteristics of Seebeck data reported. Results from a 24-thermocouple array successfully monitoring heating and isothermal cooling of a tin sample are shown. The importance of non-intrusion by the arrays, as well as furnace design, on the profiling of temperature gradients is illustrated with example measurements. Further developments underway for effectively combining all three measurements are assessed in terms of improved x-ray transmission, increased magnification, integral arrays with minimum intrusion, integral scales for velocity measurements and other features being incorporated into the third generation Seebeck furnace under construction.

  12. Solid-Liquid Interface Characterization Hardware: Advanced Technology Development (ATD)

    NASA Technical Reports Server (NTRS)

    Peters, Palmer N.; Sisk, R. C.; Sen, S.; Kaukler, W. F.; Curreri, Peter A.; Wang, F. C.; Rose, M. Franklin (Technical Monitor)

    2000-01-01

    This ATD has the goal of enabling the integration of three separate measurement techniques to characterize the solid-liquid interface of directionally solidified materials in real-time. Arrays of film-based metal thermocouple elements are under development along with compact Seebeck furnaces suitable for interfacing with separately developed X-ray Transmission Microscopes. Results of applying film arrays to furnace profiling are shown, demonstrating their ability to identify a previously undetected hardware flaw in the development of a second-generation compact furnace. Results of real-time furnace profiling also confirmed that the compact furnace design effectively isolates the temperature profiles in two halves of the furnace, a necessary feature. This isolation had only been inferred previously from the characteristics of Seebeck data reported. Results from a 24-thermocouple array successfully monitoring heating and isothermal cooling of a tin sample are shown. The importance of non-intrusion by the arrays, as well as furnace design, on the profiling of temperature gradients is illustrated with example measurements. Further developments underway for effectively combining all three measurements are assessed in terms of improved x-ray transmission, increased magnification, integral arrays with minimum intrusion, integral scales for velocity measurements and other features being incorporated into the third generation Seebeck furnace under construction.

  13. Liquid-gated interface superconductivity on an atomically flat film.

    PubMed

    Ye, J T; Inoue, S; Kobayashi, K; Kasahara, Y; Yuan, H T; Shimotani, H; Iwasa, Y

    2010-02-01

    Liquid/solid interfaces are attracting growing interest not only for applications in catalytic activities and energy storage, but also for their new electronic functions in electric double-layer transistors (EDLTs) exemplified by high-performance organic electronics, field-induced electronic phase transitions, as well as superconductivity in SrTiO(3) (ref. 12). Broadening EDLTs to induce superconductivity within other materials is highly demanded for enriching the materials science of superconductors. However, it is severely hampered by inadequate choice of materials and processing techniques. Here we introduce an easy method using ionic liquids as gate dielectrics, mechanical micro-cleavage techniques for surface preparation, and report the observation of field-induced superconductivity showing a transition temperature T(c)=15.2 K on an atomically flat film of layered nitride compound, ZrNCl. The present result reveals that the EDLT is an extremely versatile tool to induce electronic phase transitions by electrostatic charge accumulation and provides new routes in the search for superconductors beyond those synthesized by traditional chemical methods.

  14. Production of Valuable Lipophilic Compounds by Using Three Types of Interface Bioprocesses: Solid-Liquid Interface Bioreactor, Liquid-Liquid Interface Bioreactor, and Extractive Liquid-Surface Immobilization System.

    PubMed

    Oda, Shinobu

    2017-01-01

    Bioconversions such as enzymatic and microbial transformations are attractive alternatives to organic synthesis because of practical advantages such as resource conservation, energy efficiency, and environmentally harmonic properties. In addition, the production of secondary metabolites through microbial fermentation is also useful for manufacturing pharmaceuticals, agricultural chemicals, and aroma compounds. For microbial production of useful chemicals, the authors have developed three unique interfacial bioprocesses: a solid-liquid interface bioreactor (S/L-IBR), a liquid-liquid interface bioreactor (L/L-IBR), and an extractive liquid-surface immobilization (Ext-LSI) system. The S/L-IBR comprises a hydrophobic organic solvent (upper phase), a microbial film (middle phase), and a hydrophilic gel such as an agar plate (lower phase); the L/L-IBR and the Ext-LSI consist of a hydrophobic organic solvent (upper phase), a fungal mat with ballooned microspheres (middle phase), and a liquid medium (lower phase). All three systems have unique and practically important characteristics such as utilization of living cells, high concentration of lipophilic substrates/products in an organic phase, no requirement for aeration and agitation, efficient supply of oxygen, easy recovery of product, high regio- and stereoselectivity, and wide versatility. This paper reviews the principle, construction, characteristics, and application of these interfacial systems for producing lipophilic compounds such as useful aroma compounds, citronellol-related compounds, β-caryophyllene oxide, and 6-penty-α-pyrone.

  15. Layered interfaces between immiscible liquids studied by density-functional theory and molecular-dynamics simulations

    NASA Astrophysics Data System (ADS)

    Geysermans, P.; Elyeznasni, N.; Russier, V.

    2005-11-01

    We present a study of the structure in the interface between two immiscible liquids by density-functional theory and molecular-dynamics calculations. The liquids are modeled by Lennard-Jones potentials, which achieve immiscibility by supressing the attractive interaction between unlike particles. The density profiles of the liquids display oscillations only in a limited part of the simple liquid-phase diagram (ρ,T). When approaching the liquid-vapor coexistence, a significant depletion appears while the layering behavior of the density profile vanishes. By analogy with the liquid-vapor interface and the analysis of the adsorption this behavior is suggested to be strongly related to the drying transition.

  16. Behavior of solute adsorbed at the liquid-liquid interface during solvent extraction with porous-membrane phase separators

    SciTech Connect

    Persaud, G.; Xiu-min, T.; Cantwell, F.F.

    1987-01-01

    Porous membranes are used effectively as phase separators in analytical solvent extraction. When the solute involved can be adsorbed at the liquid-liquid interface, it is found that more vigorous agitation of the mixture causes a decrease in concentration of solute in the liquid flowing through the porous membrane. It is shown experimentally for the interfacially adsorbed component methylene blue perchlorate that the distribution isotherm between chloroform and water is the same in stirred and unstirred mixtures. This suggests that the interfacially adsorbed solute remains at the interface and does not enter the bulk liquid phases during the membrane-induced coalescence and phase separation. Hydrodynamic and diffusion rate calculations confirm this conclusion by showing that the residence time of the solute deposited at the liquid-liquid interface near the membrane (0.1 s) is too short for solute to diffuse through the stagnant Nernst diffusion layer.

  17. Adsorption kinetics of surfactants at liquid-solid and liquid-vapor interfaces from atomic-scale simulations

    NASA Astrophysics Data System (ADS)

    Iskrenova, Eugeniya K.; Patnaik, Soumya S.

    2012-02-01

    Nucleate pool boiling of pure liquid is a complex process involving different size- and time-scale phenomena. The appearance of the first nanobubble in the liquid at the bottom of a hot pan, the detachment of the bubble from the solid surface, its subsequent coalescence with other bubbles, all represent complex multiscale phenomena. Surfactants added to water increase the complexity of the process by contributing to the dynamic surface tension at the liquid-vapor and liquid-solid interfaces and thus affecting the heat and mass transfer at those interfaces. We apply molecular dynamics simulations to study the adsorption kinetics of anionic, cationic, and non-ionic surfactants at liquid/solid and liquid/vapor interfaces. The all-atom vs. united-atom approaches for the solid and surfactants are surveyed in view of their applicability at near boiling temperatures and a range of model water potentials is assessed for reproducing the thermal properties of water at boiling conditions.

  18. Effect of Surfactants on Drop Coalescence at Liquid/liquid Interfaces

    NASA Astrophysics Data System (ADS)

    Weheliye, Weheliye Hashii; Dong, Teng; Angeli, Panagiota

    2016-11-01

    In this paper the coalescence of a drop with a liquid-liquid interface was investigated experimentally using Particle Image Velocimetry (PIV). Initially the drop rest on the interface was studied. It was found that during drop rest the interface deformed before rupture, and the deformation increased with increasing surfactant concentration. The results from PIV showed that two counter-rotating vortices formed inside the droplet during the rupture process which moved from the bottom to the top of the drop. The evolutions of vortices for three surfactant concentrations will be presented. The vortices moved faster in lower surfactant concentrations compared to the higher ones. The intensities of the vortices in different concentrations were also calculated. After the rupture, for low surfactant concentrations, the intensities increased with time and reached a maximum while at later times they decreased. At high surfactant concentrations, the increase and subsequent decrease in intensity was not as pronounced. The work is support by the MEMPHIS program and the University College London. The author Teng Dong would like to thank the Chinese Scholarship Council (CSC) for providing funds for his overseas research.

  19. Deconstructing Temperature Gradients across Fluid Interfaces: The Structural Origin of the Thermal Resistance of Liquid-Vapor Interfaces

    NASA Astrophysics Data System (ADS)

    Muscatello, Jordan; Chacón, Enrique; Tarazona, Pedro; Bresme, Fernando

    2017-07-01

    The interfacial thermal resistance determines condensation-evaporation processes and thermal transport across material-fluid interfaces. Despite its importance in transport processes, the interfacial structure responsible for the thermal resistance is still unknown. By combining nonequilibrium molecular dynamics simulations and interfacial analyses that remove the interfacial thermal fluctuations we show that the thermal resistance of liquid-vapor interfaces is connected to a low density fluid layer that is adsorbed at the liquid surface. This thermal resistance layer (TRL) defines the boundary where the thermal transport mechanism changes from that of gases (ballistic) to that characteristic of dense liquids, dominated by frequent particle collisions involving very short mean free paths. We show that the thermal conductance is proportional to the number of atoms adsorbed in the TRL, and hence we explain the structural origin of the thermal resistance in liquid-vapor interfaces.

  20. Exposure of Mammalian Cells to Air-Pollutant Mixtures at the Air-Liquid Interface

    EPA Science Inventory

    It has been widely accepted that exposure of mammalian cells to air-pollutant mixtures at the air-liquid interface is a more realistic approach than exposing cell under submerged conditions. The VITROCELL systems, are commercially available systems for air-liquid interface expo...

  1. Exposure of Mammalian Cells to Air-Pollutant Mixtures at the Air-Liquid Interface

    EPA Science Inventory

    It has been widely accepted that exposure of mammalian cells to air-pollutant mixtures at the air-liquid interface is a more realistic approach than exposing cell under submerged conditions. The VITROCELL systems, are commercially available systems for air-liquid interface expo...

  2. Evolution of the Inner Liquid-Solid Interface During Metal Freezing

    NASA Astrophysics Data System (ADS)

    Ivanova, A. G.; Fuksov, V. M.; Gerasimov, S. F.; Pokhodun, A. I.

    2017-02-01

    The influence of the inner interface initiation method on the interface shape (formation of the planar interface or the interface with the dendrites growing into the liquid metal) was studied both theoretically and experimentally. The results of numerical simulation of the process of heat removal from the metal, corresponding to different initiation methods, revealed the existence of different species of the inner interface. The interface modification during freezing arises from the inequality of temperature gradients on opposite sides of the interface, i.e., from imbalance of heat fluxes on the interphase boundary (Stefan problem). For indium point, the results of numerical simulation were confirmed experimentally.

  3. Liquid-vapor interface of the Stockmayer fluid in a uniform external field.

    PubMed

    Moore, Stan G; Stevens, Mark J; Grest, Gary S

    2015-02-01

    The effect of a uniform (nonspatially varying) external field on the liquid-vapor interface of the Stockmayer fluid (Lennard-Jones particles embedded with a point dipole) has been investigated by molecular-dynamics simulations. The long-ranged parts of both the dipole and Lennard-Jones interactions are treated using an Ewald summation, which removes the effects of the cutoff. The direction of the field shifts the critical point and interfacial properties in different directions. For an external field parallel to the interface, the critical temperature increases, while for a field applied perpendicular to the interface, it decreases. The effects of the field on surface tension and interfacial width are also investigated. For zero field, dipoles near the liquid-vapor interface show a weak orientation parallel to the interface. For fields parallel to the interface, ordering in the liquid phase is greater than the vapor, while for fields perpendicular to the interface, the opposite is true.

  4. Ion-transfer voltammetric determination of folic acid at meso-liquid-liquid interface arrays.

    PubMed

    Jiang, Xuheng; Gao, Kui; Hu, Daopan; Wang, Huanhuan; Bian, Shujuan; Chen, Yong

    2015-04-21

    Voltammetric studies on the simple ion transfer (IT) behaviors of an important water-soluble B-vitamin, folic acid (FA), at the liquid-liquid (L-L) interface were firstly performed and then applied as a novel detection method for FA under physiological conditions. Meso-water-1,6-dichlorohexane (W-DCH) and meso-water-organogel interface arrays were built by using a hybrid mesoporous silica membrane (HMSM) with a unique structure of pores-in-pores and employed as the new platforms for the IT voltammetric study. In view of the unique structure of the HMSM, the impact of the ionic surfactant cetyltrimethylammonium bromide (CTAB), self-assembled within the silica nanochannels of the HMSM, was investigated. In particular, its effect on the IT voltammetric behavior and detection of FA at meso-L-L interface arrays was systematically examined by cyclic voltammetry (CV), differential pulse voltammetry (DPV) and differential pulse stripping voltammetry (DPSV). It was found that all the voltammetric responses of CV, DPV, and DPSV and the corresponding detection limit of FA at such meso-L-L interface arrays are closely related to the CTAB in the HMSM. Significantly, the calculated detection limit of FA could be improved to 80 nM after the combination of the DPSV technique with the additional preconcentration of FA in the silica-CTAB nanochannels, achieved through an anion-exchange process between FA(-) and the bromide of CTAB in HMSM. This provides a new and attractive strategy for the detection of those biological anions.

  5. Rapid Decomposition of Cellulose Dissolved in Ionic Liquid Using Gas-Liquid Interface Discharge

    NASA Astrophysics Data System (ADS)

    Furukawa, Shoichiro; Inoue, Nobuhiro; Ishioka, Toshio; Furuya, Kenji; Harata, Akira

    2012-07-01

    Cellulose was dissolved at 3 wt % in 15 mL of 1-allyl-3-methylimidazolium chloride ([Amim]Cl) together with 2 wt % water, and then gas-liquid interface discharge was carried out at 20 W for 200 s. As a result, 7.6% of initially dissolved cellulose decomposed and 3.9% of initially dissolved cellulose changed into reducing sugar. Adding a small amount of water to the solution was essential for the decomposition of cellulose. [Amim]Cl was stable against the discharge, as determined from the NMR signals measured before and after the discharge.

  6. The interaction effects on the adsorption properties of an alternating copolymer chain at liquid-liquid interface

    NASA Astrophysics Data System (ADS)

    Khattari, Z.; Hamasha, S.

    2014-09-01

    Analytical and numerical methods have been combined to investigate the effect of monomers-interfacial interactions on the behavior of a single alternating polymer chain at liquid-liquid interface. The exact Green's function of a Gaussian copolymer chain at attractive penetrable interface has been employed to determine monomer distribution profiles ρ(z), mean-square end-to-end distance and the interfacial tension Δγ of the alternating copolymer chain. A comparison between the diblock and alternating copolymer chain is presented. Our model shows that, the alternating copolymer adsorbs more readily than the diblock copolymer at liquid-liquid interface. Also, these copolymers are able to reduce the interfacial tension when presented at the interface.

  7. Particle lithography from colloidal self-assembly at liquid-liquid interfaces.

    PubMed

    Isa, Lucio; Kumar, Karthik; Müller, Mischa; Grolig, Jan; Textor, Marcus; Reimhult, Erik

    2010-10-26

    Particle lithography has been extensively used as a robust and cost-effective method to produce large-area, close-packed arrays of nanometer scale features. Many technological applications, including biosensing, require instead non-close-packed patterns in order to avoid cross-talk between the features. We present a simple, scalable, single-step particle lithography process that employs colloidal self-assembly at liquid-liquid interfaces (SALI) to fabricate regular, open particle lithography masks, where the size of the features (40 to 500 nm) and their separation can be independently controlled between 3 and 10 particle diameters. Finally we show how the process can be practically employed to produce diverse biosensing structures.

  8. Copper phthalocyanine films deposited by liquid-liquid interface recrystallization technique (LLIRCT).

    PubMed

    Patil, K R; Sathaye, S D; Hawaldar, R; Sathe, B R; Mandale, A B; Mitra, A

    2007-11-15

    The simple recrystallization process is innovatively used to obtain the nanoparticles of copper phthalocyanine by a simple method. Liquid-liquid interface recrystallization technique (LLIRCT) has been employed successfully to produce small sized copper phthalocyanine nanoparticles with diameter between 3-5 nm. The TEM-SAED studies revealed the formation of 3-5 nm sized with beta-phase dominated mixture of alpha and beta copper phthalocyanine nanoparticles. The XRD, SEM, and the UV-vis studies were further carried out to confirm the formation of copper phthalocyanine thin films. The cyclic voltametry (CV) studies conclude that redox reaction is totally reversible one electron transfer process. The process is attributed to Cu(II)/Cu(I) redox reaction.

  9. Reduced graphene oxide based silver sulfide hybrid films formed at a liquid/liquid interface

    SciTech Connect

    Bramhaiah, K. John, Neena S.

    2014-04-24

    Free-standing, ultra-thin films of silver sulfide and reduced graphene oxide (RGO) based silver sulfide hybrids are prepared at a liquid/liquid interface employing in situ chemical reaction strategy. Ag{sub 2}S and RGO−Ag{sub 2}S hybrid films are characterized by various techniques such as UV-visible and photo luminescence spectroscopy, X-ray diffraction and scanning electron microscopy. The morphology of hybrid films consists of Ag{sub 2}S nanocrystals on RGO surface while Ag{sub 2}S films contains branched network of dendritic structures. RGO−Ag{sub 2}S exhibit interesting optical and electrical properties. The hybrid films absorb in the region 500–650 nm and show emission in the red region. A higher conductance is observed for the hybrid films arising from the RGO component. This simple low cost method can be extended to prepare other RGO based metal sulfides.

  10. Electrokinetic motion of a spherical polystyrene particle at a liquid-fluid interface.

    PubMed

    Zhang, Junyan; Song, Yongxin; Li, Dongqing

    2017-09-07

    Electrokinetic movement of spherical polystyrene particles at different liquid-fluid interfaces was experimentally investigated in this paper. A novel method was developed to place the particles rightly at the interfaces formed in a large plastic container. The velocity was measured by an optical microscope. The experimental results show that the particles (3, 5 and 10μm in diameter) at the water-air interface, water-dodecane interface and NaCl solution-air interface move in the opposite direction of the applied electric field. The magnitude of the particles' velocity increases linearly with the increase in the applied electric field. Moreover, for particles of the same size, the electrokinetic velocity at the liquid-fluid interfaces is larger than particles' electrophoretic velocity in the bulk liquid phase. Under the same electric field, however, the electrokinetic velocity of smaller particles at the liquid-fluid interfaces is larger than that of larger particles. Such results are attributed to the surface charges at the liquid-fluid interface and the particle-liquid interface. Copyright © 2017 Elsevier Inc. All rights reserved.

  11. Perspective: Chemical reactions in ionic liquids monitored through the gas (vacuum)/liquid interface

    NASA Astrophysics Data System (ADS)

    Maier, F.; Niedermaier, I.; Steinrück, H.-P.

    2017-05-01

    This perspective analyzes the potential of X-ray photoelectron spectroscopy under ultrahigh vacuum (UHV) conditions to follow chemical reactions in ionic liquids in situ. Traditionally, only reactions occurring on solid surfaces were investigated by X-ray photoelectron spectroscopy (XPS) in situ. This was due to the high vapor pressures of common liquids or solvents, which are not compatible with the required UHV conditions. It was only recently realized that the situation is very different when studying reactions in Ionic Liquids (ILs), which have an inherently low vapor pressure, and first studies have been performed within the last years. Compared to classical spectroscopy techniques used to monitor chemical reactions, the advantage of XPS is that through the analysis of their core levels all relevant elements can be quantified and their chemical state can be analyzed under well-defined (ultraclean) conditions. In this perspective, we cover six very different reactions which occur in the IL, with the IL, or at an IL/support interface, demonstrating the outstanding potential of in situ XPS to gain insights into liquid phase reactions in the near-surface region.

  12. Nonlinear laser-induced deformations of liquid-liquid interfaces: An optical fiber model

    NASA Astrophysics Data System (ADS)

    Birkeland, Ole Jakob; Brevik, Iver

    2008-12-01

    Experimentally, it turns out that radiation forces from a cw laser on a liquid-liquid interface are able to produce giant deformations (up to about 100μm ), if the system is close to the critical point where the surface tension becomes small. We present a model for such a fingerlike deformation, implying that the system is described as an optical fiber. One reason for introducing such a model is that the refractive index difference in modern experiments, such as those of the Bordeaux group, is small, of the same order as in practical fibers in optics. It is natural therefore to adopt the hybrid HE11 mode, known from fiber theory as the fundamental mode for the liquid system. We show how the balance between hydrodynamical and radiation forces leads to a stable equilibrium point for the liquid column. Also, we calculate the narrowing of the column radius as the depth increases. Comparison with experimental results of the Bordeaux group yields quite satisfactory agreement as regards the column width.

  13. Perspective: Chemical reactions in ionic liquids monitored through the gas (vacuum)/liquid interface.

    PubMed

    Maier, F; Niedermaier, I; Steinrück, H-P

    2017-05-07

    This perspective analyzes the potential of X-ray photoelectron spectroscopy under ultrahigh vacuum (UHV) conditions to follow chemical reactions in ionic liquids in situ. Traditionally, only reactions occurring on solid surfaces were investigated by X-ray photoelectron spectroscopy (XPS) in situ. This was due to the high vapor pressures of common liquids or solvents, which are not compatible with the required UHV conditions. It was only recently realized that the situation is very different when studying reactions in Ionic Liquids (ILs), which have an inherently low vapor pressure, and first studies have been performed within the last years. Compared to classical spectroscopy techniques used to monitor chemical reactions, the advantage of XPS is that through the analysis of their core levels all relevant elements can be quantified and their chemical state can be analyzed under well-defined (ultraclean) conditions. In this perspective, we cover six very different reactions which occur in the IL, with the IL, or at an IL/support interface, demonstrating the outstanding potential of in situ XPS to gain insights into liquid phase reactions in the near-surface region.

  14. Capillary wave theory of adsorbed liquid films and the structure of the liquid-vapor interface.

    PubMed

    MacDowell, Luis G

    2017-08-01

    In this paper we try to work out in detail the implications of a microscopic theory for capillary waves under the assumption that the density is given along lines normal to the interface. Within this approximation, which may be justified in terms of symmetry arguments, the Fisk-Widom scaling of the density profile holds for frozen realizations of the interface profile. Upon thermal averaging of capillary wave fluctuations, the resulting density profile yields results consistent with renormalization group calculations in the one-loop approximation. The thermal average over capillary waves may be expressed in terms of a modified convolution approximation where normals to the interface are Gaussian distributed. In the absence of an external field we show that the phenomenological density profile applied to the square-gradient free energy functional recovers the capillary wave Hamiltonian exactly. We extend the theory to the case of liquid films adsorbed on a substrate. For systems with short-range forces, we recover an effective interface Hamiltonian with a film height dependent surface tension that stems from the distortion of the liquid-vapor interface by the substrate, in agreement with the Fisher-Jin theory of short-range wetting. In the presence of long-range interactions, the surface tension picks up an explicit dependence on the external field and recovers the wave vector dependent logarithmic contribution observed by Napiorkowski and Dietrich. Using an error function for the intrinsic density profile, we obtain closed expressions for the surface tension and the interface width. We show the external field contribution to the surface tension may be given in terms of the film's disjoining pressure. From literature values of the Hamaker constant, it is found that the fluid-substrate forces may be able to double the surface tension for films in the nanometer range. The film height dependence of the surface tension described here is in full agreement with results of

  15. Capillary wave theory of adsorbed liquid films and the structure of the liquid-vapor interface

    NASA Astrophysics Data System (ADS)

    MacDowell, Luis G.

    2017-08-01

    In this paper we try to work out in detail the implications of a microscopic theory for capillary waves under the assumption that the density is given along lines normal to the interface. Within this approximation, which may be justified in terms of symmetry arguments, the Fisk-Widom scaling of the density profile holds for frozen realizations of the interface profile. Upon thermal averaging of capillary wave fluctuations, the resulting density profile yields results consistent with renormalization group calculations in the one-loop approximation. The thermal average over capillary waves may be expressed in terms of a modified convolution approximation where normals to the interface are Gaussian distributed. In the absence of an external field we show that the phenomenological density profile applied to the square-gradient free energy functional recovers the capillary wave Hamiltonian exactly. We extend the theory to the case of liquid films adsorbed on a substrate. For systems with short-range forces, we recover an effective interface Hamiltonian with a film height dependent surface tension that stems from the distortion of the liquid-vapor interface by the substrate, in agreement with the Fisher-Jin theory of short-range wetting. In the presence of long-range interactions, the surface tension picks up an explicit dependence on the external field and recovers the wave vector dependent logarithmic contribution observed by Napiorkowski and Dietrich. Using an error function for the intrinsic density profile, we obtain closed expressions for the surface tension and the interface width. We show the external field contribution to the surface tension may be given in terms of the film's disjoining pressure. From literature values of the Hamaker constant, it is found that the fluid-substrate forces may be able to double the surface tension for films in the nanometer range. The film height dependence of the surface tension described here is in full agreement with results of

  16. Solid-liquid interface free energy in binary systems: theory and atomistic calculations for the (110) Cu-Ag interface.

    PubMed

    Frolov, T; Mishin, Y

    2009-08-07

    We analyze thermodynamics of solid-liquid interfaces in binary systems when the solid is in a nonhydrostatic state of stress. The difficulty lies in the fact that chemical potential of at least one of the chemical components in a nonhydrostatic solid is an undefined quantity. We show, nevertheless, that the interface free energy gamma can be defined as excess of an appropriate thermodynamic potential that depends on the chemical potentials in the liquid phase. We derive different forms of the adsorption equation for solid-liquid interfaces, with differential coefficients representing excesses of extensive properties. This leads, in particular, to the formulation of interface stress tau(ij) as an appropriate excess over nonhydrostatic bulk stresses. The interface stress is not unique unless the solid is in a hydrostatic state of stress. We also derive Gibbs-Helmholtz type equations that can be applied for thermodynamic integration of gamma. All thermodynamic relations derived here are presented in forms suitable for atomistic simulations. In particular, the excess quantities can be computed without constructing interface profiles. As an application, we perform semigrand canonical Monte Carlo simulations of the (110) solid-liquid interface in the Cu-Ag system. We show that gamma computed by thermodynamic integration along a coexistence path decreases with increasing composition difference between the phases. At the same time, tau(ij) remains negative (i.e., the interface is in a state of compression), drastically increases in magnitude, and becomes highly anisotropic. Some of the interface excess properties are computed by different methods and demonstrate accurate agreement with each other, confirming the correctness of our analysis.

  17. Numerical simulation of drop impact on a liquid-liquid interface with a multiple marker front-capturing method

    NASA Astrophysics Data System (ADS)

    Coyajee, Emil; Boersma, Bendiks Jan

    2009-07-01

    The gravity-driven motion of a droplet impacting on a liquid-liquid interface is studied. The full Navier-Stokes equations are solved on a fixed, uniform grid using a finite difference/front-capturing method. For the representation of fluid-fluid interfaces, a coupled Level-Set/Volume-Of-Fluid method [M. Sussman, E.G. Puckett, A coupled Level-Set and Volume-of-Fluid method for computing 3D and axisymmetric incompressible two-phase flows, J. Comp. Phys. 162 (2000) 301-337] is used, in which we introduce the novel approach of describing separate interfaces with different marker functions. As a consequence, we prevent numerical coalescence of the droplet and the liquid-liquid interface without excessive (local) grid refinement. To validate our method, numerical simulations of the drop impact event are compared with experiments [Z. Mohamed-Kassim, E.K. Longmire, Drop impact on a liquid-liquid interface, Phys. Fluids 15 (2003) 3263-3273]. Furthermore, a comparison is made with the numerical results of [A. Esmaeeli, G. Tryggvason, Direct numerical simulations of bubbly flows. Part 2. Moderate Reynolds number arrays, J. Fluid Mech. 385 (1999) 325-358] for an array of rising bubbles. The investigation shows that the multiple marker approach successfully prevents numerical coalescence of interfaces and adequately captures the effect of surface tension.

  18. Pyroelectric energy harvesting using liquid-based switchable thermal interfaces

    SciTech Connect

    Cha, G; Ju, YS

    2013-01-15

    The pyroelectric effect offers an intriguing solid-state approach for harvesting ambient thermal energy to power distributed networks of sensors and actuators that are remotely located or otherwise difficult to access. There have been, however, few device-level demonstrations due to challenges in converting spatial temperature gradients into temporal temperature oscillations necessary for pyroelectric energy harvesting. We demonstrate the feasibility of a device concept that uses liquid-based thermal interfaces for rapid switching of the thermal conductance between a pyroelectric material and a heat source/sink and can thereby deliver high output power density. Using a thin film of a pyroelectric co-polymer together with a macroscale mechanical actuator, we operate pyroelectric thermal energy harvesting cycles at frequencies close to 1 Hz. Film-level power densities as high as 110 mW/cm(3) were achieved, limited by slow heat diffusion across a glass substrate. When combined with a laterally interdigitated electrode array and a MEMS actuator, the present design offers an attractive option for compact high-power density thermal energy harvesters. (C) 2012 Elsevier B.V. All rights reserved.

  19. Long DNA Molecules at Liquid-Solid Interfaces

    NASA Astrophysics Data System (ADS)

    Samuilov, Vladimir; Li, B.; Sokolov, J.; Rafailovich, M.; Chu, B.

    2006-03-01

    The electrophoresis of long DNA molecules was studied using a newly developed method of electrophoresis on flat surfaces [1] in the regime of strong electrostatic interaction. The mobility of lambda- DNA molecules on this surface was found to scale as the square root of the persistent length with the ionic strength at high buffer. This experimental result indicates that at high buffer concentration the separation mechanism of solid-liquid interface electrophoresis is expected to be due to surface friction rather than biased reptation [2-4]. At low buffer concentrations the DNA chains are stretched .The electric double layer is responsible for a velocity profile of the electroosmotic flow. The net electrophoretic mobility of longer DNA, being trapped closer to the surface as found to be higher then for the shorter ones in the electric field. [1]. N. Pernodet, V. Samuilov, K. Shin, et al. Physical Review Letters, 85 (2000) 5651-5654. [2] Y.-S. Seo, V.A. Samuilov, J. Sokolov, et al. Electrophoresis, 23 (2002) 2618-2625. [3] Y.-S. Seo, H.. Luo, V. A. Samuilov, et al. DNA Electrophoresis on nanopatterned surfaces, Nano Letters, 4, 2004, 659-664.

  20. Liquid-film assisted formation of alumina/niobium interfaces

    SciTech Connect

    Sugar, Joshua D.; McKeown, Joseph T.; Marks, Robert A.; Glaeser, Andreas M.

    2002-06-16

    Alumina has been joined at 1400 degrees C using niobium-based interlayers. Two different joining approaches were compared: solid-state diffusion bonding using a niobium foil as an interlayer, and liquid-film assisted bonding using a multilayer copper/niobium/copper interlayer. In both cases, a 127-(mu)m thick niobium foil was used; =1.4-(mu)m or =3-(mu)m thick copper films flanked the niobium. Room-temperature four-point bend tests showed that the introduction of a copper film had a significant beneficial effect on the average strength and the strength distribution. Experiments using sapphire substrates indicated that during bonding the initially continuous copper film evolved into isolated copper-rich droplets/particles at the sapphire/interlayer interface, and extensive regions of direct bonding between sapphire and niobium. Film breakup appeared to initiate at either niobium grain boundary ridges, or at asperities or irregularities on the niobium surface that caused localized contact with the sapphire.

  1. Vibrational sum frequency spectroscopy of surfactants and phospholipid monolayers at liquid-liquid interfaces

    NASA Astrophysics Data System (ADS)

    Smiley, Beth L.; Walker, R. A.; Gragson, D. E.; Hannon, T. E.; Richmond, Geraldine L.

    1998-04-01

    Work from our laboratory on vibrational sum frequency spectroscopic investigations of molecular ordering at the carbon tetrachloride-water interface is reviewed. Simple charged surfactants adsorbed at the liquid-liquid interface are seen to induce alignment of interfacial water molecules to a degree which is dependent on the induced surface potential. Saturation of water molecule alignment occurs at a surfactant surface concentration corresponding to a calculated surface potential of approximately 160 mV. In complementary studies, the relative degree of hydrocarbon chain ordering within monolayers of symmetric phosphatidylcholines of different chain lengths is inferred by the relative signal contributions of the methyl and methylene symmetric stretch modes. The degree of hydrocarbon chain disorder observed depends strongly on the method of monolayer preparation. By one method, a decrease in hydrocarbon chain order is seen with increasing chain length. Another method of monolayer formation yielded very well ordered hydrocarbon chains for the longest chain phosphatidylcholine studied, and showed much greater disorder in shorter chain species which was comparable to the other preparation method. These studies are a foundation for further work with this technique geared towards understanding molecular-level structural features in membrane-like assemblies and surface biochemical interactions of relevance to biomedical research.

  2. Dynamic single-interface hollow fiber liquid phase microextraction of Cr(VI) using ionic liquid containing supported liquid membrane.

    PubMed

    Pimparu, Rungaroon; Nitiyanontakit, Sira; Miró, Manuel; Varanusupakul, Pakorn

    2016-12-01

    The concept of dynamic single-interface hollow fiber membrane liquid-phase microextraction (HF-LPME), where the target analyte was extracted on-line and eluted inside the lumen of the HF membrane, was explored. An ionic liquid containing supported liquid membrane was used for the trace determination of Cr(VI) as a model compound. Since the extraction took place on-line inside the hollow fiber membrane, the mass transfer behavior was described and discussed in comparison with the conventional HF-LPME. The extraction efficiency was improved by a recirculation configuration of the sample solution at relatively high sampling flow rates as a result of the increased effective contact area. The positive pressure observed to be built up during extraction was overcome by a flow-balancing pressure design. The dynamic single-interface HF-LPME method with an enrichment factor of 41, a detection limit of 1.2µgL(-1) and determination limit of 4.0µgL(-1) was successfully applied to the reliable determination of Cr(VI) from environmental water samples. The quantification limit is below the maximum contaminant level in drinking water, set at 10µgL(-1) of hexavalent chromium by the California Environmental Protection Agency.

  3. Development of a liquid-junction/low-flow interface for phosphate buffer capillary electrophoresis mass spectrometry.

    PubMed

    Li, Fu-An; Huang, Ju-Li; Shen, Shang-Yu; Wang, Che-Wei; Her, Guor-Rong

    2009-04-01

    To alleviate ion suppression from phosphate buffer and to preserve separation integrity, a new capillary electrophoresis mass spectrometry (CE-MS) interface was developed. The interface consisted of a low-flow interface and a liquid junction. In this design, both the inlet reservoir and the liquid-junction reservoir were filled with phosphate running buffer. Because the phosphate anions in the column migrated toward the inlet reservoir (away from the electrospray ionization (ESI) source) the problem of ion suppression in ESI was avoided. The liquid junction was incorporated to eliminate issues of degraded separation observed when sheath liquid interfaces use different buffers for separation and MS analysis attributed to differences in anion velocity. The utility of the interface was demonstrated by the analysis of antihistamines at pH 3.5 and the analysis of perfluorocarboxylic acid at pH 9.5.

  4. Influence of ion size asymmetry on the properties of ionic liquid vapour interfaces

    NASA Astrophysics Data System (ADS)

    Bresme, Fernando; González-Melchor, Minerva; Alejandre, José

    2005-11-01

    The influence of ion size asymmetry on the properties of ionic liquid-vapour interfaces is investigated using molecular dynamics simulations of the soft primitive model. Ion size asymmetry results in charge separation at the liquid-vapour interface and therefore in a local violation of the electroneutrality condition. For moderate size asymmetries the electrostatic potential at the interface can reach values of the order of 0.1 V. Size asymmetry plays a very important role in determining ion adsorption at the liquid-vapour interface of ionic mixtures. The interfacial adsorption of the bigger component results in an increase of the electrostatic potential, and a reduction of the interfacial surface tension. Our results show that ionic mixtures provide a very efficient way to tune the electrostatics and surface properties of ionic liquid-vapour interfaces.

  5. Preparation and attachment of liquid-infused porous supra-particles to liquid interfaces.

    PubMed

    Al-Shehri, Hamza; Horozov, Tommy S; Paunov, Vesselin N

    2016-10-12

    We prepared model porous composite supra-particles and investigated the effect of the initial infused fluid phase on their attachment at the liquid-fluid interface. We used a simple method for fabrication of millimetre-sized spherical porous supra-particles from much smaller monodisperse latex microparticles as building blocks by evaporation of a polystyrene sulphate latex suspension on a hot super-hydrophobic surface. We annealed the dried supra-particles at the polymer's glass transition temperature to fuse partially their latex particle building blocks. Spherical porous supra-particles were produced above 40 wt% initial concentration of the latex particles in the suspension, which had a rough surface, with a porous and amorphous structure. We controlled the supra-particle size by varying the initial volume of the latex suspension drop, the latex particle concentration and the drop evaporation temperature. This preparation technique allowed limited control over the porosity of the supra-particles by varying the initial concentration of the latex particle suspension, the rate of evaporation and the annealing temperature. We characterised the surface morphology and the inner structure of supra-particles by SEM imaging. We report for the first time results of an MRI study of supra-particles attached to an air-water or an oil-water interface, which indicated that only the surface layer of the building block particles attaches to the liquid interface while the pore fluid was not displaced by the outer fluid. We observed that supra-particles infused with water had different wettability and attachment positions at the oil-water interface compared with the same particles infused with oil. Similarly, the infusion of the porous supra-particles with water led to a different attachment at the air-water interface compared to the attachment of the same supra-particle when dry. The fundamental importance of this result is that the porous particles (or colloid particle

  6. Interaction of a sodium ion with the water liquid-vapor interface

    NASA Technical Reports Server (NTRS)

    Wilson, M. A.; Pohorille, A.; Pratt, L. R.; MacElroy, R. D. (Principal Investigator)

    1989-01-01

    Molecular dynamics results are presented for the density profile of a sodium ion near the water liquid-vapor interface at 320 K. These results are compared with the predictions of a simple dielectric model for the interaction of a monovalent ion with this interface. The interfacial region described by the model profile is too narrow and the profile decreases too abruptly near the solution interface. Thus, the simple model does not provide a satisfactory description of the molecular dynamics results for ion positions within two molecular diameters from the solution interface where appreciable ion concentrations are observed. These results suggest that surfaces associated with dielectric models of ionic processes at aqueous solution interfaces should be located at least two molecular diameters inside the liquid phase. A free energy expense of about 2 kcal/mol is required to move the ion within two molecular layers of the free water liquid-vapor interface.

  7. Interaction of a sodium ion with the water liquid-vapor interface

    NASA Technical Reports Server (NTRS)

    Wilson, M. A.; Pohorille, A.; Pratt, L. R.; MacElroy, R. D. (Principal Investigator)

    1989-01-01

    Molecular dynamics results are presented for the density profile of a sodium ion near the water liquid-vapor interface at 320 K. These results are compared with the predictions of a simple dielectric model for the interaction of a monovalent ion with this interface. The interfacial region described by the model profile is too narrow and the profile decreases too abruptly near the solution interface. Thus, the simple model does not provide a satisfactory description of the molecular dynamics results for ion positions within two molecular diameters from the solution interface where appreciable ion concentrations are observed. These results suggest that surfaces associated with dielectric models of ionic processes at aqueous solution interfaces should be located at least two molecular diameters inside the liquid phase. A free energy expense of about 2 kcal/mol is required to move the ion within two molecular layers of the free water liquid-vapor interface.

  8. Nematic liquid crystals confined in microcapillaries for imaging phenomena at liquid-liquid interfaces.

    PubMed

    Zhong, Shenghong; Jang, Chang-Hyun

    2015-09-21

    Here, we report the development of an experimental system based on liquid crystals (LCs) confined in microcapillaries for imaging interfacial phenomena. The inner surfaces of the microcapillaries were modified with octadecyltrichlorosilane to promote an escaped-radial configuration of LCs. We checked the optical appearance of the capillary-confined LCs under a crossed polarizing microscope and determined their arrangement based on side and top views. We then placed the capillary-confined LCs in contact with non-surfactant and surfactant solutions, producing characteristic textures of two bright lines and a four-petal shape, respectively. We also evaluated the sensitivity, stability, and reusability of the system. Our imaging system was more sensitive than previously reported LC thin film systems. The textures formed in microcapillaries were stable for more than 120 h and the capillaries could be reused at least 10 times. Finally, we successfully applied our system to image the interactions of phospholipids and bivalent metal ions. In summary, we developed a simple, small, portable, sensitive, stable, and reusable experimental system that can be broadly applied to monitor liquid-liquid interfacial phenomena. These results provide valuable information for designs using confined LCs as chemoresponsive materials in optical sensors.

  9. Temperature dependence of local solubility of hydrophobic molecules in the liquid-vapor interface of water.

    PubMed

    Abe, Kiharu; Sumi, Tomonari; Koga, Kenichiro

    2014-11-14

    One important aspect of the hydrophobic effect is that solubility of small, nonpolar molecules in liquid water decreases with increasing temperature. We investigate here how the characteristic temperature dependence in liquid water persists or changes in the vicinity of the liquid-vapor interface. From the molecular dynamics simulation and the test-particle insertion method, the local solubility Σ of methane in the liquid-vapor interface of water as well as Σ of nonpolar solutes in the interface of simple liquids are calculated as a function of the distance z from the interface. We then examine the temperature dependence of Σ under two conditions: variation of Σ at fixed position z and that at fixed local solvent density around the solute molecule. It is found that the temperature dependence of Σ at fixed z depends on the position z and the system, whereas Σ at fixed local density decreases with increasing temperature for all the model solutions at any fixed density between vapor and liquid phases. The monotonic decrease of Σ under the fixed-density condition in the liquid-vapor interface is in accord with what we know for the solubility of nonpolar molecules in bulk liquid water under the fixed-volume condition but it is much robust since the solvent density to be fixed can be anything between the coexisting vapor and liquid phases. A unique feature found in the water interface is that there is a minimum in the local solubility profile Σ(z) on the liquid side of the interface. We find that with decreasing temperature the minimum of Σ grows and at the same time the first peak in the oscillatory density profile of water develops. It is likely that the minimum of Σ is due to the layering structure of the free interface of water.

  10. Investigation of Air-Liquid Interface Rings in Buffer Preparation Vessels: the Role of Slip Agents.

    PubMed

    Shi, Ting; Ding, Wei; Kessler, Donald W; De Mas, Nuria; Weaver, Douglas G; Pathirana, Charles; Martin, Russell D; Mackin, Nancy A; Casati, Michael; Miller, Scott A; Pla, Itzcoatl A

    2016-01-01

    Air-liquid interface rings were observed on the side walls of stainless steel buffer vessels after certain downstream buffer preparations. Those rings were resistant to regular cleaning-in-place procedures but could be removed by manual means. To investigate the root cause of this issue, multiple analytical techniques, including liquid chromatography with tandem mass spectrometry detection (LC-MS/MS), high-resolution accurate mass liquid chromatography with mass spectrometry, nuclear magnetic resonance, Fourier transform infrared spectroscopy, and scanning electron microscopy with energy-dispersive X-ray spectroscopy have been employed to characterize the chemical composition of air-liquid interface rings. The main component of air-liquid interface rings was determined to be slip agents, and the origin of the slip agents can be traced back to their presence on raw material packaging liners. Slip agents are commonly used in plastic industry as additives to reduce the coefficient of friction during the manufacturing process of thin films. To mitigate this air-liquid interface ring issue, an alternate liner with low slip agent was identified and implemented with minimal additional cost. We have also proactively tested the packaging liners of other raw materials currently used in our downstream buffer preparation to ensure slip agent levels are appropriate. Air-liquid interface rings were observed on the side walls of stainless steel buffer vessels after certain downstream buffer preparations. To investigate the root cause of this issue, multiple analytical techniques have been employed to characterize the chemical composition of air-liquid interface rings. The main components of air-liquid interface rings were determined to be slip agents, which are common additives used in the manufacturing process of thin films. The origin of the slip agents can be traced back to their presence on certain raw material packaging liners. To mitigate this air-liquid interface ring

  11. 2D-crystallization of Rhodococcus 20S proteasome at the liquid-liquid interface

    NASA Astrophysics Data System (ADS)

    Aoyama, Kazuhiro

    1996-10-01

    The 2D-crystallization method using the liquid-liquid interface between a aqueous phase (protein solution) and a thin organic liquid (dehydroabietylamine) layer has been applied to the Rhodococcus 20S proteasome. The 20S proteasome is known to be the core complex of the 26S proteasome, which is the central protease of the ubiquitin-dependent pathway. Two types of ordered arrays were obtained, both large enough for high resolution analysis by electron crystallography. The first one had a four-fold symmetry, whereas the second one was found out to be a hexagonally close-packed array. By image analysis based on a real space correlation averaging (CAV) technique, the close-packed array was found to be hexagonally packed, but the molecules had presumably rotational freedom. The four-fold array was found to be a true crystal with p4 symmetry. Lattice constants were a = b = 20.0 nm and α = 90°. The unit cell of this crystal contained two molecules. The diffraction pattern computed from the original picture showed spots up to (4, 5) that corresponds to 3.1 nm resolution. After applying an unbending procedure, the diffraction pattern showed spots extending to 1.8 nm resolution.

  12. Shapes and dynamics of miscible liquid/liquid interfaces in horizontal capillary tubes.

    PubMed

    Stevar, M S P; Vorobev, A

    2012-10-01

    We report optical observations of the dissolution behaviour of glycerol/water, soybean oil/hexane, and isobutyric acid (IBA)/water binary mixtures within horizontal capillary tubes. Tubes with diameters as small as 0.2mm were initially filled with one component of the binary mixture (solute) and then immersed into a solvent-filled thermostatic bath. Both ends of the tubes were open, and no pressure difference was applied between the ends. In the case of glycerol/water and soybean oil/hexane mixtures, we managed to isolate the dissolution (the interfacial mass transfer) from the hydrodynamic motion. Two phase boundaries moving from the ends into the middle section of the tube with the speeds v∼D(1/3)t(-2/3)d(2) (D,t and d are the coefficient of diffusion, time and the diameter of the tube, respectively) were observed. The boundaries slowly smeared but their smearing occurred considerably slower than their motion. The motion of the phase boundaries cannot be explained by the dependency of the diffusion coefficient on concentration, and should be explained by the effect of barodiffusion. The shapes of the solute/solvent boundaries are defined by the balance between gravity and surface tension effects. The contact line moved together with the bulk interface: no visible solute remained on the walls after the interface passage. Changes in temperature and in the ratio between gravity and capillary forces altered the apparent contact angles. The IBA/water system had different behaviour. Below the critical (consolute) point, no dissolution was observed: IBA and water behaved like two immiscible liquids, with the IBA phase being displaced from the tube by capillary pressure (the spontaneous imbibition process). Above the critical point, two IBA/water interfaces could be identified, however the interfaces did not penetrate much into the tube. Copyright © 2012 Elsevier Inc. All rights reserved.

  13. Green-Kubo relation for friction at liquid-solid interfaces

    NASA Astrophysics Data System (ADS)

    Huang, Kai; Szlufarska, Izabela

    2014-03-01

    We have developed a Green-Kubo relation that enables accurate calculations of friction at solid-liquid interfaces directly from equilibrium molecular dynamics (MD) simulations and that provides a pathway to bypass the time-scale limitations of typical nonequilibrium MD simulations. The theory has been validated for a number of different interfaces and it is demonstrated that the liquid-solid slip is an intrinsic property of an interface. Because of the high numerical efficiency of our method, it can be used in the design of interfaces for applications in aqueous environments, such as nano- and microfluidics.

  14. Total internal reflection resonance light scattering at solid/liquid interfaces.

    PubMed

    Tang, Yao-Ji; Chen, Ying; Yao, Min-Na; Li, Yao-Qun

    2008-08-05

    Total internal reflection (TIR) technique is an interface-specific tool and resonance light scattering (RLS) is of high sensitivity. The combination of both approaches is introduced into the solid/liquid interface for the first time. The behaviors of mixture of TPPS and BSA at the interface have been studied with total internal reflection resonance light scattering (TIR-RLS). The preliminary experimental results indicate that TIR-RLS is a good approach to study the interaction and distinguish the states of macromolecules at the solid/liquid interface.

  15. Swimming of a model ciliate near an air-liquid interface

    NASA Astrophysics Data System (ADS)

    Wang, S.; Ardekani, A. M.

    2013-06-01

    In this work, the role of the hydrodynamic forces on a swimming microorganism near an air-liquid interface is studied. The lubrication theory is utilized to analyze hydrodynamic effects within the narrow gap between a flat interface and a small swimmer. By using an archetypal low-Reynolds-number swimming model called “squirmer,” we find that the magnitude of the vertical swimming velocity is on the order of O(ɛlnɛ), where ɛ is the ratio of the gap width to the swimmer's body size. The reduced swimming velocity near an interface can explain experimental observations of the aggregation of microorganisms near a liquid interface.

  16. Swimming of a model ciliate near an air-liquid interface.

    PubMed

    Wang, S; Ardekani, A M

    2013-06-01

    In this work, the role of the hydrodynamic forces on a swimming microorganism near an air-liquid interface is studied. The lubrication theory is utilized to analyze hydrodynamic effects within the narrow gap between a flat interface and a small swimmer. By using an archetypal low-Reynolds-number swimming model called "squirmer," we find that the magnitude of the vertical swimming velocity is on the order of O(εlnε), where ε is the ratio of the gap width to the swimmer's body size. The reduced swimming velocity near an interface can explain experimental observations of the aggregation of microorganisms near a liquid interface.

  17. Isolating Reactions at the Picoliter Scale: Parallel Control of Reaction Kinetics at the Liquid-Liquid Interface.

    PubMed

    Phan-Quang, Gia Chuong; Lee, Hiang Kwee; Ling, Xing Yi

    2016-07-11

    Miniaturized liquid-liquid interfacial reactors offer enhanced surface area and rapid confinement of compounds of opposite solubility, yet they are unable to provide in situ reaction monitoring at a molecular level at the interface. A picoreactor operative at the liquid-liquid interface is described, comprising plasmonic colloidosomes containing Ag octahedra strategically assembled at the water-in-decane emulsion interface. The plasmonic colloidosomes isolate ultrasmall amounts of solutions (<200 pL), allowing parallel monitoring of multiple reactions simultaneously. Using the surface-enhanced Raman spectroscopy (SERS) technique, in situ monitoring of the interfacial protonation of dimethyl yellow (p-dimethylaminoazobenzene (DY)) is performed, revealing an apparent rate constant of 0.09 min(-1) for the first-order reaction. The presence of isomeric products with similar physical properties is resolved, which would otherwise be indiscernible by other analytical methods.

  18. Particle separation by a moving air-liquid interface in a microchannel.

    PubMed

    Wang, Fengkun; Chon, Chan Hee; Li, Dongqing

    2010-12-15

    Particle separation is an important topic in microfluidic field and has recently gained significant attention in sample preparations for biological and chemical studies. In this paper, a novel particle separation method was proposed. In this method, the particles were separated by the air-liquid interface in a microchannel. The motion of the air-liquid interface was controlled with a syringe pump. Depending on the air-liquid interface speed, the liquid film thickness and the viscous force on particles were changed and the particles were separated by sizes. We observed the separation of 1.01 μm particles from the larger particles when the air-liquid interface speed was less than 11 μm/s, and the separation of both 1.01 μm and 5.09 μm particles from the larger particles when the interface speed was between 11 μm/s and 120 μm/s. When the speed was higher than 120 μm/s, the drag force of the liquid flow generated by the advancing interface on particles was so strong that the flow removed all particles off from the bottom channel wall and there were no particles left behind the advancing interface.

  19. Segregation of ions at the interface: molecular dynamics studies of the bulk and liquid-vapor interface structure of equimolar binary mixtures of ionic liquids.

    PubMed

    Palchowdhury, Sourav; Bhargava, B L

    2015-08-14

    The structures of three different equimolar binary ionic liquid mixtures and their liquid-vapor interface have been studied using atomistic molecular dynamics simulations. Two of these binary mixtures were composed of a common cation 1-n-butyl-3-methylimidazolium and varying anions (chloride and hexafluorophosphate in one of the mixtures and chloride and trifluoromethanesulfonate in the other) and the third binary mixture was composed of a common anion, trifluoromethanesulfonate and two imidazolium cations with ethyl and octyl side chains. Binary mixtures with common cations are found to be homogeneous. The anions are preferentially located near the ring hydrogen atoms due to H-bonding interactions. Segregation of ions is observed at the interface with an enrichment of the liquid-vapor interface layer by longer alkyl chains and bigger anions with a distributed charge. The surface composition is drastically different from that of the bulk composition, with the longer alkyl tail groups and bigger anions populating the outermost layer of the interface. The longer alkyl chains of the cations and trifluoromethanesulfonate anions with a smaller charge density show orientational ordering at the liquid-vapor interface.

  20. Understanding Atomic-Scale Behavior of Liquid Crystals at Aqueous Interfaces.

    PubMed

    Ramezani-Dakhel, Hadi; Sadati, Monirosadat; Rahimi, Mohammad; Ramirez-Hernandez, Abelardo; Roux, Benoît; de Pablo, Juan J

    2017-01-10

    The ordered environment presented by liquid crystals at interfaces enables a range of novel functionalities that is only now beginning to be exploited in applications ranging from light focusing devices to biosensors. One key feature of liquid crystals is that molecular events occurring at an interface propagate over large distances through the bulk. In spite of their importance, our fundamental understanding of liquid crystal-water and liquid crystal-air interfaces remains limited. In this work, we present results from large-scale atomistic molecular dynamics simulations on the organization of the nematic and isotropic phases of the nitrile-containing mesogenic molecule 4-cyano-4'-pentylbiphenyl (5CB) in the vicinity of vacuum and aqueous interfaces. Hybrid boundary conditions are imposed by confining 5CB films between vacuum and an aqueous medium to examine how those two types of interfaces influence the specific structural arrangement and ordering of 5CB. Consistent with experiments, our results indicate that 5CB exhibits homeotropic anchoring at the vacuum interface, and planar alignment at aqueous interfaces. Two-dimensional molecular dynamics potential of mean force calculations and average polarization densities show that the polar nitrile group of 5CB remains hydrated near the aqueous interface, where it modulates the orientation of water molecules. Estimates of the anchoring strength reveal an oscillatory decay and a semilinear decay with distance from the interface in vacuum and water, respectively.

  1. Dynamic Mass Transfer of Hemoglobin at the Aqueous/Ionic-Liquid Interface Monitored with Liquid Core Optical Waveguide.

    PubMed

    Chen, Xuwei; Yang, Xu; Zeng, Wanying; Wang, Jianhua

    2015-08-04

    Protein transfer from aqueous medium into ionic liquid is an important approach for the isolation of proteins of interest from complex biological samples. We hereby report a solid-cladding/liquid-core/liquid-cladding sandwich optical waveguide system for the purpose of monitoring the dynamic mass-transfer behaviors of hemoglobin (Hb) at the aqueous/ionic liquid interface. The optical waveguide system is fabricated by using a hydrophobic IL (1,3-dibutylimidazolium hexafluorophosphate, BBimPF6) as the core, and protein solution as one of the cladding layer. UV-vis spectra are recorded with a CCD spectrophotometer via optical fibers. The recorded spectra suggest that the mass transfer of Hb molecules between the aqueous and ionic liquid media involve accumulation of Hb on the aqueous/IL interface followed by dynamic extraction/transfer of Hb into the ionic liquid phase. A part of Hb molecules remain at the interface even after the accomplishment of the extraction/transfer process. Further investigations indicate that the mass transfer of Hb from aqueous medium into the ionic liquid phase is mainly driven by the coordination interaction between heme group of Hb and the cationic moiety of ionic liquid, for example, imidazolium cation in this particular case. In addition, hydrophobic interactions also contribute to the transfer of Hb.

  2. Nematicons across interfaces: anomalous refraction and reflection of solitons in liquid Crystals.

    PubMed

    Peccianti, Marco; Assanto, Gaetano

    2007-06-25

    The robustness of nematicons, i. e. spatial solitons in nematic liquid crystals, can be exploited to implement counter-intuitive negative reflection and refraction schemes for optical signal manipulation at interfaces.

  3. Redistribution of fluorescent molecules at the solid/liquid interface with total internal reflection illumination.

    PubMed

    Wei, Lin; Ye, Zhongju; Luo, Wenjuan; Chen, Bo; Xiao, Lehui

    2016-08-01

    Many intriguing physical and chemical processes commonly take place at the solid/liquid interface. Total internal reflection illumination, together with single molecule spectroscopy, provides a robust platform for the selective exploration of kinetic processes close the interface. With these techniques, it was observed that the distribution of Rhodamine B molecules close to a solid/liquid interface could be regulated in a photo-induced route. The laser-induced repulsion force at this interface is enough to compromise the Brownian diffusion of single molecules in a range of several hundred nanometers normal to the solid/liquid interface. This observation is fundamentally and practically interesting because moderate laser intensity is enough to initiate this repulsion effect. Therefore, it might display extensive applications in the development of photo-modulation technique with high throughput capability.

  4. Electric Field Effect on Phospholipid Monolayers at an Aqueous-Organic Liquid-Liquid Interface.

    PubMed

    Yu, Hao; Yzeiri, Irena; Hou, Binyang; Chen, Chiu-Hao; Bu, Wei; Vanysek, Petr; Chen, Yu-Sheng; Lin, Binhua; Král, Petr; Schlossman, Mark L

    2015-07-23

    The electric potential difference across cell membranes, known as the membrane potential, plays an important role in the activation of many biological processes. To investigate the effect of the membrane potential on the molecular ordering of lipids within a biomimetic membrane, a self-assembled monolayer of 1-stearoyl-2-oleoyl-sn-glycero-3-phosphocholine (SOPC) lipids at an electrified 1,2-dichloroethane/water interface is studied with X-ray reflectivity and interfacial tension. Measurements over a range of electric potential differences, -150 to +130 mV, that encompass the range of typical biomembrane potentials demonstrate a nearly constant and stable structure whose lipid interfacial density is comparable to that found in other biomimetic membrane systems. Measurements at higher positive potentials, up to 330 mV, illustrate a monotonic decrease in the lipid interfacial density and accompanying variations in the interfacial configuration of the lipid. Molecular dynamics simulations, designed to mimic the experimental conditions, show that the measured changes in lipid configuration are due primarily to the variation in area per lipid with increasing applied electric field. Rotation of the SOPC dipole moment by the torque from the applied electric field appears to be negligible, except at the highest measured potentials. The simulations confirm in atomistic detail the measured potential-dependent characteristics of SOPC monolayers. Our hybrid study sheds light on phospholipid monolayer stability under different membrane potentials, which is important for understanding membrane processes. This study also illustrates the use of X-ray surface scattering to probe the ordering of surfactant monolayers at an electrified aqueous-organic liquid-liquid interface.

  5. Specific interface area in a thin layer system of two immiscible liquids with vapour generation at the contact interface

    NASA Astrophysics Data System (ADS)

    Pimenova, Anastasiya V.; Gazdaliev, Ilias M.; Goldobin, Denis S.

    2017-06-01

    For well-stirred multiphase fluid systems the mean interface area per unit volume, or “specific interface area” SV, is a significant characteristic of the system state. In particular, it is important for the dynamics of systems of immiscible liquids experiencing interfacial boiling. We estimate the value of parameter SV as a function of the heat influx {\\dot{Q}}V to the system or the average system overheat <Θ> above the interfacial boiling point. The derived results can be reformulated for the case of an endothermic chemical reaction between two liquid reagents with the gaseous form of one of the reaction products. The final results are restricted to the case of thin layers, where the potential gravitational energy of bubbles leaving the contact interface is small compared to their surface tension energy.

  6. Chiral induction and amplification in supramolecular systems at the liquid-solid interface.

    PubMed

    Xu, Hong; Ghijsens, Elke; George, Subi J; Wolffs, Martin; Tomović, Željko; Schenning, Albertus P H J; De Feyter, Steven

    2013-06-03

    Chiral induction and amplification in surface-confined supramolecular monolayers are investigated at the liquid-solid interface. Scanning tunneling microscopy (STM) proves that achiral molecules can self-assemble into globally chiral patterns through a variety of approaches, including induction by chiral solvents or by a novel chiral amplification method. Our study demonstrates the aptness of both approaches, which have already been applied to (supramolecular) polymers in solution, to create chiral supramolecular monolayers at the liquid-solid interface.

  7. Forming Nanoparticle Monolayers at Liquid-Air Interfaces by Using Miscible Liquids.

    PubMed

    Zhang, Datong; Hu, Jiayang; Kennedy, Kathleen M; Herman, Irving P

    2016-08-23

    One standard way of forming monolayers (MLs) of nanoparticles (NPs) is to drop-cast a NP dispersion made using one solvent onto a second, immiscible solvent; after this upper solvent evaporates, the NP ML can be transferred to a solid substrate by liftoff. We show that this previously universal use of only immiscible solvent pairs can be relaxed and close-packed, hexagonally ordered NP monolayers can self-assemble at liquid-air interfaces when some miscible solvent pairs are used instead. We demonstrate this by drop-casting an iron oxide NP dispersion in toluene on a dimethyl sulfoxide (DMSO) liquid substrate. The NPs are energetically stable at the DMSO surface and remain there even with solvent mixing. Excess NPs coagulate and precipitate in the DMSO, and this limits NPs at the surface to approximately 1 ML. The ML domains at the surface nucleate independently, which is in contrast to ML growth at the receding edge of the drying drop, as is common in immiscible solvent pair systems and seen here for the toluene/diethylene glycol immiscible solvent pair system. This new use of miscible solvent pairs can enable the formation of MLs for a wider range of NPs.

  8. Insulin Aggregation at a Dynamic Solid-Liquid-Air Triple Interface.

    PubMed

    Frachon, Thibaut; Bruckert, Franz; Le Masne, Quentin; Monnin, Emmanuel; Weidenhaupt, Marianne

    2016-12-13

    Therapeutic proteins are privileged in drug development because of their exquisite specificity, which is due to their three-dimensional conformation in solution. During their manufacture, storage, and delivery, interactions with material surfaces and air interfaces are known to affect their stability. The growing use of automated devices for handling and injection of therapeutics increases their exposure to protocols involving intermittent wetting, during which the solid-liquid and liquid-air interfaces meet at a triple contact line, which is often dynamic. Using a microfluidic setup, we analyze the effect of a moving triple interface on insulin aggregation in real time over a hydrophobic surface. We combine thioflavin T fluorescence and reflection interference microscopy to concomitantly monitor insulin aggregation and the morphology of the liquid as it dewets the surface. We demonstrate that insulin aggregates in the region of a moving triple interface and not in regions submitted to hydrodynamic shear stress alone, induced by the moving liquid. During dewetting, liquid droplets form on the surface anchored by adsorbed proteins, and the accumulation of amyloid aggregates is observed exclusively as fluorescent rings growing eccentrically around these droplets. The fluorescent rings expand until the entire channel surface sweeped by the triple interface is covered by amyloid fibers. On the basis of our experimental results, we propose a model describing the growth mechanism of insulin amyloid fibers at a moving triple contact line, where proteins adsorbed at a hydrophobic surface are exposed to the liquid-air interface.

  9. Effect of thermal convection on the shape of a solid-liquid interface

    NASA Technical Reports Server (NTRS)

    Mennetrier, C.; Chopra, M. A.; De Groh, H. C., III

    1991-01-01

    The effect of thermal convection on the shape of solid-liquid interface was investigated in experiments conducted in a transparent Bridgman-type directional solidification furnace. The relationship was numerically modeled using a standard 2D finite-difference approach, with the solid-liquid deformable interface approximated by a blocking-off technique. The directional solidification furnace was used with pure succinonitrile (which is also transparent) contained in a long square ampoule made of borosilicate glass. With the furnace in the vertical configuration, a flat interface was observed, in agreement with the model. On the other hand, a highly distorted interface was obtained in the horizontal configuration; the numerical results showed a strong recirculating cell in front of the interface due to natural thermal convection. The results indicate that thermal convection is responsible for the interface distortion.

  10. Electrochemical behaviour and voltammetric sensitivity at arrays of nanoscale interfaces between immiscible liquids.

    PubMed

    Rimboud, Mickaël; Hart, Robert D; Becker, Thomas; Arrigan, Damien W M

    2011-11-21

    Arrays of nanoscale interfaces between immiscible electrolyte solutions were formed using silicon nitride nanopore array membranes. Nanopores in the range from 75 nm radius down to 17 nm radius were used to form the nano-interfaces. It was found that the liquid organic phase electrolyte solution filled the pores so that inlaid nano-interfaces were formed with the aqueous phase. Cyclic voltammetry at these nano-interface arrays demonstrated steady-state behaviour at the larger interfaces but the voltammetric wave-shape became progressively worse as the interface size decreased. It was found that the ion transfer currents were ca. 50% of those expected based on theoretical calculations, which is attributed to overlap of diffusion zones at adjacent nano-interfaces. Here, the separation between adjacent nano-interfaces was 20-times the interface radius. The analytical sensitivity for ion transfer from the aqueous to the 1,6-dichlorohexane organic phase was estimated from calibration plots of current density versus concentration of aqueous tetraethylammonium cation. The sensitivity was in the range of 65 μA cm(-2) μM(-1) (at 75 nm radius interfaces) to 265 μA cm(-2) μM(-1) (at 17 nm radius interfaces). The sensitivity depended directly on the inverse of the nano-interface radius, implying that smaller interfaces will provide better sensitivity, due to the enhanced flux of analyte arising from convergent diffusion to smaller electrochemical interfaces.

  11. Fast Responsive and Controllable Liquid Transport on a Magnetic Fluid/Nanoarray Composite Interface.

    PubMed

    Tian, Dongliang; Zhang, Na; Zheng, Xi; Hou, Guanglei; Tian, Ye; Du, Yi; Jiang, Lei; Dou, Shi Xue

    2016-06-28

    Controllable liquid transport on surface is expected to occur by manipulating the gradient of surface tension/Laplace pressure and external stimuli, which has been intensively studied on solid or liquid interface. However, it still faces challenges of slow response rate, and uncontrollable transport speed and direction. Here, we demonstrate fast responsive and controllable liquid transport on a smart magnetic fluid/nanoarray interface, i.e., a composite interface, via modulation of an external magnetic field. The wettability of the composite interface to water instantaneously responds to gradient magnetic field due to the magnetically driven composite interface gradient roughness transition that takes place within a millisecond, which is at least 1 order of magnitude faster than that of other responsive surfaces. A water droplet can follow the motion of the gradient composite interface structure as it responds to the gradient magnetic field motion. Moreover, the water droplet transport direction can be controlled by modulating the motion direction of the gradient magnetic field. The composite interface can be used as a pump for the transport of immiscible liquids and other objects in the microchannel, which suggests a way to design smart interface materials and microfluidic devices.

  12. Behavior of ceramic particles at the solid-liquid metal interface in metal matrix composites

    NASA Technical Reports Server (NTRS)

    Stefanescu, D. M.; Dhindaw, B. K.; Kacar, S. A.; Moitra, A.

    1988-01-01

    Directional solidification results were obtained in order to investigate particle behavior at the solid-liquid interface in Al-2 pct Mg (cellular interface) and Al-6.1 pct Ni (eutectic interface) alloys. It is found that particles can be entrapped in the solid if adequate solidification rates and temperature gradients are used. Model results showed critical velocity values slightly higher than those obtained experimentally.

  13. The molecular structure of the interface between water and a hydrophobic substrate is liquid-vapor like.

    PubMed

    Willard, Adam P; Chandler, David

    2014-11-14

    With molecular simulation for water and a tunable hydrophobic substrate, we apply the instantaneous interface construction [A. P. Willard and D. Chandler, "Instantaneous liquid interfaces," J. Phys. Chem. B 114, 1954-1958 (2010)] to examine the similarity between a water-vapor interface and a water-hydrophobic surface interface. We show that attractive interactions between a hydrophobic surface and water affect capillary wave fluctuations of the instantaneous liquid interface, but these attractive interactions have essentially no effect on the intrinsic interface. The intrinsic interface refers to molecular structure in terms of distances from the instantaneous interface. Further, the intrinsic interface of liquid water and a hydrophobic substrate differs little from that of water and its vapor. The same is not true, we show, for an interface between water and a hydrophilic substrate. In that case, strong directional substrate-water interactions disrupt the liquid-vapor-like interfacial hydrogen bonding network.

  14. A Method To Measure Protein Unfolding at an Air-Liquid Interface.

    PubMed

    Leiske, Danielle L; Shieh, Ian C; Tse, Martha Lovato

    2016-10-04

    Proteins are surface-active molecules that have a propensity to adsorb to hydrophobic interfaces, such as the air-liquid interface. Surface flow can increase aggregation of adsorbed proteins, which may be an undesirable consequence depending on the application. As changes in protein conformation upon adsorption are thought to induce aggregation, the ability to measure the folded state of proteins at interfaces is of particular interest. However, few techniques currently exist to measure protein conformation at interfaces. Here we describe a technique capable of measuring the hydrophobicity, and therefore the conformation and folded state, of proteins at air-liquid interfaces by exploiting the environmentally sensitive fluorophore Nile red. Two monoclonal antibodies (mAbs) with high (mAb1) and low (mAb2) surface activity were used to highlight the technique. Both mAbs showed low background fluorescence of Nile red in the liquid subphase and at a glass-liquid interface. In contrast, at the air-liquid interface Nile red fluorescence for mAb1 increased immediately after protein adsorption, whereas the Nile red fluorescence of the mAb2 film evolved more slowly in time even though the adsorbed quantity of protein remained constant. The results demonstrate that hydrophobicity upon mAb adsorption to the air-liquid interface evolves in a time-dependent manner. Interfacial hydrophobicity may be indicative of protein conformation or folded state, where rapid unfolding of mAb1 upon adsorption would be consistent with increased protein aggregation compared to mAb2. The ability to measure protein hydrophobicity at interfaces using Nile red, combined with small sample requirements and minimal sample preparation, fills a gap in existing interfacial techniques.

  15. Critical Evaluation of Air-Liquid Interface Exposure Devices for In Vitro Assessment of Atmospheric Pollutants

    EPA Science Inventory

    Exposure of cells to atmospheric pollutants at the air-liquid interface (ALI) is a more realistic approach than exposures of attached cells submerged in liquid medium. However, there is still limited understanding of the ideal ALI device design features that permit reproducible a...

  16. Critical Evaluation of Air-Liquid Interface Exposure Devices for In Vitro Assessment of Atmospheric Pollutants

    EPA Science Inventory

    Exposure of cells to atmospheric pollutants at the air-liquid interface (ALI) is a more realistic approach than exposures of attached cells submerged in liquid medium. However, there is still limited understanding of the ideal ALI device design features that permit reproducible a...

  17. Towards active microfluidics: Interface turbulence in thin liquid films with floating molecular machines

    NASA Astrophysics Data System (ADS)

    Alonso, Sergio; Mikhailov, Alexander S.

    2009-06-01

    Thin liquid films with floating active protein machines are considered. Cyclic mechanical motions within the machines, representing microscopic swimmers, lead to molecular propulsion forces applied to the air-liquid interface. We show that when the rate of energy supply to the machines exceeds a threshold, the flat interface becomes linearly unstable. As a result of this instability, the regime of interface turbulence, characterized by irregular traveling waves and propagating machine clusters, is established. Numerical investigations of this nonlinear regime are performed. Conditions for the experimental observation of the instability are discussed.

  18. Thermodynamic and kinetic solid-liquid interface properties from transition path sampling

    NASA Astrophysics Data System (ADS)

    Şopu, Daniel; Rogal, Jutta; Drautz, Ralf

    2016-12-01

    We perform transition path sampling simulations to determine two of the key quantities in solidification, the solid-liquid interface energy and velocity, in a Lennard-Jones system. Our approach is applicable to a wide range of temperature and pressure conditions, at the melting temperature and out-of-equilibrium. We show that small system sizes are sufficient for good values of interface energies and velocities. The transition path sampling method thus offers an attractive and robust alternative for the evaluation of solid-liquid interface properties.

  19. Photodissociation of ICN at the liquid/vapor interface of chloroform

    NASA Astrophysics Data System (ADS)

    Vieceli, John; Chorny, Ilya; Benjamin, Ilan

    2001-09-01

    The photodissociation of ICN initially adsorbed at the liquid/vapor interface of chloroform is studied using classical molecular dynamics computer simulations. The photodissociation and subsequent geminate recombination on the ground state of ICN is compared with the same reaction in the bulk liquid. We find that the probability for cage escape at the interface is significantly enhanced due to the possibility that one or both of the photodissociation fragments desorb into the gas phase. The desorption probability is sensitive to the initial location and orientation of the ICN. An examination of the energy disposal into these fragments provides additional information about the competition between geminate recombination and cage escape at the interface.

  20. Dynamic Self-Assembly and Self-Propulsion in Nonequilibrium Magnetic Colloidal Ensembles at a Liquid/Liquid Interface

    NASA Astrophysics Data System (ADS)

    Snezhko, Alexey; Aranson, Igor

    2011-03-01

    Ensembles of interacting particles subject to external periodic energy fluxes often develop nontrivial dynamics. Magnetic colloidal particles suspended over an interface of two immiscible liquids and energized by vertical alternating magnetic fields give rise to novel dynamic self-assembled structures (``asters'') which are not accessible at the liquid/air interfaces. Ferromagnetically ordered nickel spherical particles have been used in our experiments. Novel structures are attributed to the interplay between surface waves, generated at the liquid/liquid interface by the collective response of magnetic microparticles to the alternating magnetic field, and hydrodynamic fields induced in the boundary layers of both liquids forming the interface. Two types of magnetic order is reported. We show that self-assembled aster structures become distorted in the presence of a small in-plane dc magnetic field and develop self-propulsion. The speed of locomotion can be effectively tuned by the amplitude of the dc field. The research was supported by the U.S. DOE, Office of Basic Energy Sciences, Division of Materials Science and Engineering, under the Contract No. DE AC02-06CH11357.

  1. Dynamics of drop impact and coalescence at a liquid/liquid interface

    NASA Astrophysics Data System (ADS)

    Mohamed-Kassim, Ahmad Zulfaa

    Coalescence is a process where two fluidic bodies merge into one. Coalescence will occur, for example, after a raindrop impacts on a pool of water or when petroleum oil is collected in bulk after separating it from water. However, the topological transition and the short length and time scales associated with coalescence made it difficult to model analytically or simulate numerically. Hence, predictions of any coalescence phenomena are typically made through empirical or ad-hoc methods which can be cumbersome and costly. The objective of this investigation was to obtain detailed velocity field measurements using the particle image velocimetry (PIV) method on a simple two-fluid flow undergoing a coalescence process. These measurements will provide test cases against numerical simulations. The flow was modeled experimentally by releasing a single drop through a less dense ambient until it achieved a terminal velocity before impacting onto a liquid/liquid interface. Viscosity of the less dense ambient was varied to study the effect of Reynolds number on the flow. The drop approach and impact were also studied to observe their influence on the coalescence process. Index matching and a slight camera inclination were employed to eliminate optical distortions. Sequences of images and velocity fields were obtained using a high-speed video camera to study flow evolution during impact and coalescence. The experimental measurements showed that coalescence is decoupled from impact for the liquid/liquid combinations studied here. Prior to impact, a wake existed upstream of each drop due to viscous and pressure drag. Inside the drop, the fluid circulated around a vortex ring whose diameter extends near the drop boundary. After impact, the viscously-induced circulation inside the drop dissipated completely due to wake impingement and drop deformation. The interfacial rupture which led to coalescence was typically off-axis, followed by a retraction of the thin film free edge with

  2. A Microscopic Model for the Liquid Metal - Ionic Solution Interface.

    DTIC Science & Technology

    1983-02-10

    Chemistry 1. Laboratoire de Physique des Liquides et Electrochimie , Universite Pierre et Marie Curie, 4 place Jussieu, 752?0 PARIS CEDEX 05, FRANCE...Laboratoire de Physique des Liquides et Electrochimie , Universita Pie=re at Marie Curie, 4 place Jussieu, 75230 PARIS CEDEX 05, FRANCE. F. VERICAI 0

  3. Quantitative assessment of radiation force effect at the dielectric air-liquid interface

    PubMed Central

    Capeloto, Otávio Augusto; Zanuto, Vitor Santaella; Malacarne, Luis Carlos; Baesso, Mauro Luciano; Lukasievicz, Gustavo Vinicius Bassi; Bialkowski, Stephen Edward; Astrath, Nelson Guilherme Castelli

    2016-01-01

    We induce nanometer-scale surface deformation by exploiting momentum conservation of the interaction between laser light and dielectric liquids. The effect of radiation force at the air-liquid interface is quantitatively assessed for fluids with different density, viscosity and surface tension. The imparted pressure on the liquids by continuous or pulsed laser light excitation is fully described by the Helmholtz electromagnetic force density. PMID:26856622

  4. Semiconducting polymers: Probing the solid-liquid interface

    NASA Astrophysics Data System (ADS)

    Crispin, Xavier; Kalinin, Sergei V.

    2017-07-01

    Exploring the minute mechanical deformations induced by electrical bias at the interface with electrolytes allows the identification of local crystallinity and distinguishing adsorption and intercalation of ions in electroactive polymers.

  5. Nonequilibrium kinetic boundary condition at the vapor-liquid interface of argon.

    PubMed

    Ishiyama, Tatsuya; Fujikawa, Shigeo; Kurz, Thomas; Lauterborn, Werner

    2013-10-01

    A boundary condition for the Boltzmann equation (kinetic boundary condition, KBC) at the vapor-liquid interface of argon is constructed with the help of molecular dynamics (MD) simulations. The KBC is examined at a constant liquid temperature of 85 K in a wide range of nonequilibrium states of vapor. The present investigation is an extension of a previous one by Ishiyama, Yano, and Fujikawa [Phys. Rev. Lett. 95, 084504 (2005)] and provides a more complete form of the KBC. The present KBC includes a thermal accommodation coefficient in addition to evaporation and condensation coefficients, and these coefficients are determined in MD simulations uniquely. The thermal accommodation coefficient shows an anisotropic behavior at the interface for molecular velocities normal versus tangential to the interface. It is also found that the evaporation and condensation coefficients are almost constant in a fairly wide range of nonequilibrium states. The thermal accommodation coefficient of the normal velocity component is almost unity, while that of the tangential component shows a decreasing function of the density of vapor incident on the interface, indicating that the tangential velocity distribution of molecules leaving the interface into the vapor phase may deviate from the tangential parts of the Maxwell velocity distribution at the liquid temperature. A mechanism for the deviation of the KBC from the isotropic Maxwell KBC at the liquid temperature is discussed in terms of anisotropic energy relaxation at the interface. The liquid-temperature dependence of the present KBC is also discussed.

  6. Surfing liquid metal droplet on the same metal bath via electrolyte interface

    NASA Astrophysics Data System (ADS)

    Zhao, Xi; Tang, Jianbo; Liu, Jing

    2017-09-01

    We report a phenomenon that when exerting an electric field gradient across a liquid metal/electrolyte interface, a droplet of the same liquid metal can persistently surf on the interface without coalescence. A thin layer of the intermediate solution, which separates the droplet from direct metallic contacting and provides levitating force, is responsible for such surfing effect. The electric resistance of this solution film is measured, and the film thickness is further theoretically calculated. The fact that the levitating state can be switched on and off via a controlled manner paves the way for reliably manipulating liquid metal droplets or devices.

  7. Dynamics of a solid sphere bouncing on or penetrating through a liquid-air interface

    NASA Astrophysics Data System (ADS)

    Kim, Seong Jin; Jung, Sunghwan; Lee, Sungyon

    2014-11-01

    In this study, we investigate the dynamics of a solid particle moving from liquid to air through a liquid-air interface. The experimental setup consists of an air-piston system that shoots a solid particle into water towards the free surface from below. Experimental results indicate that the particle either penetrates or bounces back depending on the particle size, impact speed, and surface tension. In particular, the particle needs to overcome the resistive interfacial forces in order to penetrate through the liquid-air interface. This transition from bouncing to penetration regimes is captured theoretically by conducting a simple force balance and is further compared with experiments.

  8. Mobile Interfaces: Liquids as a Perfect Structural Material for Multifunctional, Antifouling Surfaces

    SciTech Connect

    Grinthal, A; Aizenberg, J

    2014-01-14

    Life creates some of its most robust, extreme surface materials not from solids but from liquids: a purely liquid interface, stabilized by underlying nanotexture, makes carnivorous plant leaves ultraslippery, the eye optically perfect and dirt-resistant, our knees lubricated and pressure-tolerant, and insect feet reversibly adhesive and shape-adaptive. Novel liquid surfaces based on this idea have recently been shown to display unprecedented omniphobic, self-healing, anti-ice, antifouling, optical, and adaptive properties. In this Perspective, we present a framework and a path forward for developing and designing such liquid surfaces into sophisticated, versatile multifunctional materials. Drawing on concepts from solid materials design and fluid dynamics, we outline how the continuous dynamics, responsiveness, and multiscale patternability of a liquid surface layer can be harnessed to create a wide range of unique, active interfacial functions able to operate in harsh, changing environments not achievable with static solids. We discuss how, in partnership with the underlying substrate, the liquid surface can be programmed to adaptively and reversibly reconfigure from a defect-free, molecularly smooth, transparent interface through a range of finely tuned liquid topographies in response to environmental stimuli. With nearly unlimited design possibilities and unmatched interfacial properties, liquid materials as long-term stable interfaces yet in their fully liquid state may potentially transform surface design everywhere from medicine to architecture to energy infrastructure.

  9. Mobile interfaces: Liquids as a perfect structural material for multifunctional, antifouling surfaces

    SciTech Connect

    Grinthal, Alison; Aizenberg, Joanna

    2013-10-14

    Life creates some of its most robust, extreme surface materials not from solids but from liquids: a purely liquid interface, stabilized by underlying nanotexture, makes carnivorous plant leaves ultraslippery, the eye optically perfect and dirt-resistant, our knees lubricated and pressure-tolerant, and insect feet reversibly adhesive and shape-adaptive. Novel liquid surfaces based on this idea have recently been shown to display unprecedented omniphobic, self-healing, anti-ice, antifouling, optical, and adaptive properties. In this Perspective, we present a framework and a path forward for developing and designing such liquid surfaces into sophisticated, versatile multifunctional materials. Drawing on concepts from solid materials design and fluid dynamics, we outline how the continuous dynamics, responsiveness, and multiscale patternability of a liquid surface layer can be harnessed to create a wide range of unique, active interfacial functions-able to operate in harsh, changing environments-not achievable with static solids. We discuss how, in partnership with the underlying substrate, the liquid surface can be programmed to adaptively and reversibly reconfigure from a defect-free, molecularly smooth, transparent interface through a range of finely tuned liquid topographies in response to environmental stimuli. In conclusion, with nearly unlimited design possibilities and unmatched interfacial properties, liquid materials-as long-term stable interfaces yet in their fully liquid state-may potentially transform surface design everywhere from medicine to architecture to energy infrastructure.

  10. Mobile interfaces: Liquids as a perfect structural material for multifunctional, antifouling surfaces

    DOE PAGES

    Grinthal, Alison; Aizenberg, Joanna

    2013-10-14

    Life creates some of its most robust, extreme surface materials not from solids but from liquids: a purely liquid interface, stabilized by underlying nanotexture, makes carnivorous plant leaves ultraslippery, the eye optically perfect and dirt-resistant, our knees lubricated and pressure-tolerant, and insect feet reversibly adhesive and shape-adaptive. Novel liquid surfaces based on this idea have recently been shown to display unprecedented omniphobic, self-healing, anti-ice, antifouling, optical, and adaptive properties. In this Perspective, we present a framework and a path forward for developing and designing such liquid surfaces into sophisticated, versatile multifunctional materials. Drawing on concepts from solid materials design andmore » fluid dynamics, we outline how the continuous dynamics, responsiveness, and multiscale patternability of a liquid surface layer can be harnessed to create a wide range of unique, active interfacial functions-able to operate in harsh, changing environments-not achievable with static solids. We discuss how, in partnership with the underlying substrate, the liquid surface can be programmed to adaptively and reversibly reconfigure from a defect-free, molecularly smooth, transparent interface through a range of finely tuned liquid topographies in response to environmental stimuli. In conclusion, with nearly unlimited design possibilities and unmatched interfacial properties, liquid materials-as long-term stable interfaces yet in their fully liquid state-may potentially transform surface design everywhere from medicine to architecture to energy infrastructure.« less

  11. Universal adsorption at the vapor-liquid interface near the consolute point

    NASA Technical Reports Server (NTRS)

    Schmidt, James W.

    1990-01-01

    The ellipticity of the vapor-liquid interface above mixtures of methylcyclohexane (C7H14) and perfluoromethylcyclohexane (C7F14) has been measured near the consolute point T(c) = 318.6 K. The data are consistent with a model of the interface that combines a short-ranged density-vs height profile in the vapor phase with a much longer-ranged composition-versus-height profile in the liquid. The value of the free parameter produced by fitting the model to the data is consistent with results from two other simple mixtures and a mixture of a polymer and solvent. This experiment combines precision ellipsometry of the vapor-liquid interface with in situ measurements of refractive indices of the liquid phases, and it precisely locates the consolute point.

  12. Preparation of a smooth GaN-Gallium solid-liquid interface

    NASA Astrophysics Data System (ADS)

    de Jong, A. E. F.; Vonk, V.; Ruat, M.; Boćkowski, M.; Kamler, G.; Grzegory, I.; Honkimäki, V.; Vlieg, E.

    2016-08-01

    We discuss the preparation of an atomically flat solid-liquid interface between solid gallium nitride and liquid gallium using in situ surface X-ray diffraction to probe the interface roughness. For the creation of this interface it is necessary to start the experiment with liquid gallium which first etches into the solid at a temperature of 823 K in a nitrogen free ambient. After this rigorous cleaning procedure there is perfect wetting between solid and liquid. The roughness created due to the fast etching of the solid has to be repaired at a nitrogen pressure of 10-20 bar and a temperature around 1150 K. The (2,1) crystal truncation rod data are excellently described by a surface model having 0±0.1 Å roughness, which indicates a successful repair. The lateral length scale on which the roughness is determined has a lower limit of 750±50 Å.

  13. Scale effect of slip boundary condition at solid-liquid interface.

    PubMed

    Nagayama, Gyoko; Matsumoto, Takenori; Fukushima, Kohei; Tsuruta, Takaharu

    2017-03-03

    Rapid advances in microelectromechanical systems have stimulated the development of compact devices, which require effective cooling technologies (e.g., microchannel cooling). However, the inconsistencies between experimental and classical theoretical predictions for the liquid flow in microchannel remain unclarified. Given the larger surface/volume ratio of microchannel, the surface effects increase as channel scale decreases. Here we show the scale effect of the boundary condition at the solid-liquid interface on single-phase convective heat transfer characteristics in microchannels. We demonstrate that the deviation from classical theory with a reduction in hydraulic diameters is due to the breakdown of the continuum solid-liquid boundary condition. The forced convective heat transfer characteristics of single-phase laminar flow in a parallel-plate microchannel are investigated. Using the theoretical Poiseuille and Nusselt numbers derived under the slip boundary condition at the solid-liquid interface, we estimate the slip length and thermal slip length at the interface.

  14. Liquid-vapor interface locations in a spheroidal container under low gravity

    NASA Technical Reports Server (NTRS)

    Carney, M. J.

    1986-01-01

    As a part of the general study of liquid behavior in low gravity environments, an experimental investigation was conducted to determine if there are equilibrium liquid-vapor interface configurations that can exist at more than one location in oblate spheroidal containers under reduced gravity conditions. Static contact angles of the test liquids on the spheroid surface were restricted to near 0 deg. The experiments were conducted in a low gravity environment. An oblate spheroidal tank was tested with an eccentricity of 0.68 and a semimajor axis of 2.0 cm. Both quantitative and qualitative data were obtained on the liquid-vapor interface configuration and position inside the container. The results of these data, and their impat on previous work in this area, are discussed. Of particular interest are those equilibrium interface configurations that can exist at multiple locations in the container.

  15. Scale effect of slip boundary condition at solid–liquid interface

    NASA Astrophysics Data System (ADS)

    Nagayama, Gyoko; Matsumoto, Takenori; Fukushima, Kohei; Tsuruta, Takaharu

    2017-03-01

    Rapid advances in microelectromechanical systems have stimulated the development of compact devices, which require effective cooling technologies (e.g., microchannel cooling). However, the inconsistencies between experimental and classical theoretical predictions for the liquid flow in microchannel remain unclarified. Given the larger surface/volume ratio of microchannel, the surface effects increase as channel scale decreases. Here we show the scale effect of the boundary condition at the solid–liquid interface on single-phase convective heat transfer characteristics in microchannels. We demonstrate that the deviation from classical theory with a reduction in hydraulic diameters is due to the breakdown of the continuum solid–liquid boundary condition. The forced convective heat transfer characteristics of single-phase laminar flow in a parallel-plate microchannel are investigated. Using the theoretical Poiseuille and Nusselt numbers derived under the slip boundary condition at the solid–liquid interface, we estimate the slip length and thermal slip length at the interface.

  16. Scale effect of slip boundary condition at solid–liquid interface

    PubMed Central

    Nagayama, Gyoko; Matsumoto, Takenori; Fukushima, Kohei; Tsuruta, Takaharu

    2017-01-01

    Rapid advances in microelectromechanical systems have stimulated the development of compact devices, which require effective cooling technologies (e.g., microchannel cooling). However, the inconsistencies between experimental and classical theoretical predictions for the liquid flow in microchannel remain unclarified. Given the larger surface/volume ratio of microchannel, the surface effects increase as channel scale decreases. Here we show the scale effect of the boundary condition at the solid–liquid interface on single-phase convective heat transfer characteristics in microchannels. We demonstrate that the deviation from classical theory with a reduction in hydraulic diameters is due to the breakdown of the continuum solid–liquid boundary condition. The forced convective heat transfer characteristics of single-phase laminar flow in a parallel-plate microchannel are investigated. Using the theoretical Poiseuille and Nusselt numbers derived under the slip boundary condition at the solid–liquid interface, we estimate the slip length and thermal slip length at the interface. PMID:28256536

  17. Templated synthesis of amphiphilic nanoparticles at the liquid-liquid interface.

    PubMed

    Andala, Dickson M; Shin, Sun Hae Ra; Lee, Hee-Young; Bishop, Kyle J M

    2012-02-28

    A simple and reliable method is described to produce inorganic nanoparticles functionalized asymmetrically with domains of hydrophobic and hydrophilic ligands on their respective hemispheres. These amphiphilic, Janus-type particles form spontaneously by a thermodynamically controlled process, in which the particle cores and two competing ligands assemble at the interface between two immiscible liquids to reduce the interfacial energy. The asymmetric surface chemistry resulting from this process was confirmed using contact angle measurements of water droplets on nanoparticle monolayers deposited onto hydrophobic and hydrophilic substrates-particles presenting their hydrophobic face give contact angles of ∼96°, those presenting their hydrophilic face ∼19°. The spontaneous assembly process is rationalized by a thermodynamic model, which accounts both for the energetic contributions driving the assembly and for the entropic penalties that must be overcome. Consistent with the model, amphiphilic NPs form only when there is sufficient interfacial area to accommodate them; however, this potential limitation is easily overcome by mechanical agitation of the two-phase mixture. While it is straightforward to vary the ratio of hydrophobic and hydrophilic ligands, the accumulation of amphiphilic particles at the interface is maximal for ligand ratios near 1:1. In addition to gold nanoparticles and thiolate ligands, we demonstrate the generality of this approach by extending it to the preparation of amphiphilic iron oxide nanoparticles using two types of diol-terminated ligands. Depending on the material properties of the inorganic cores, the resulting amphiphilic particles should find applications as responsive particle surfactants that respond dynamically to optical (plasmonic particles) and/or magnetic (magnetic particles) fields.

  18. Adsorption Kinetics at Silica Gel/Ionic Liquid Solution Interface.

    PubMed

    Flieger, Jolanta; Tatarczak-Michalewska, Małgorzata; Groszek, Anna; Blicharska, Eliza; Kocjan, Ryszard

    2015-12-10

    A series of imidazolium and pyridinium ionic liquids with different anions (Cl(-), Br(-), BF₄(-), PF₆(-)) has been evaluated for their adsorption activity on silica gel. Quantification of the ionic liquids has been performed by the use of RP-HPLC with organic-aqueous eluents containing an acidic buffer and a chaotropic salt. Pseudo-second order kinetic models were applied to the experimental data in order to investigate the kinetics of the adsorption process. The experimental data showed good fitting with this model, confirmed by considerably high correlation coefficients. The adsorption kinetic parameters were determined and analyzed. The relative error between the calculated and experimental amount of ionic liquid adsorbed at equilibrium was within 7%. The effect of various factors such as initial ionic liquid concentration, temperature, kind of solvent, kind of ionic liquid anion and cation on adsorption efficiency were all examined in a lab-scale study. Consequently, silica gel showed better adsorptive characteristics for imidazolium-based ionic liquids with chaotropic anions from aqueous solutions in comparison to pyridinium ionic liquids. The adsorption was found to decrease with the addition of organic solvents (methanol, acetonitrile) but it was not sensitive to the change of temperature in the range of 5-40 °C.

  19. Ripples on a rising bubble through an immiscible two-liquid interface generate numerous micro droplets

    NASA Astrophysics Data System (ADS)

    Uemura, T.; Ueda, Y.; Iguchi, M.

    2010-11-01

    The mass transfer between immiscible two liquid phases can be greatly accelerated by bubbling gas through a reactor (Bird R. B., Stewart W. E. and Lightfoot E. N., Transport Phenomena, 2nd edition (John Wiley and Sons) 2002). Therefore, the physical phenomenon occurring during the passage of a rising bubble through an immiscible two-liquid interface is of particular interest. The passage of the bubble through the oil (upper phase)/water (lower phase) interface starts with an upward lifting of the interface, and the bubble attracts a column of the water phase upwards keeping a film of the water phase around itself. In the present study, a particular remark is given to the influence of different interface tensions retracting the water film, after the water film ruptured, which lays on the interface between air and silicone oil. Unlike the previous studies on the rupture of a single liquid film in a gas which is pulled due to the identical surface tension, this system can form concentric ripples on the outer interface of the water film (oil/water interface) around the bubble due to the weak interface tension. Then, numerous micro water droplets break out from the fully grown ripples.

  20. Physical ageing of the contact line on colloidal particles at liquid interfaces.

    PubMed

    Kaz, David M; McGorty, Ryan; Mani, Madhav; Brenner, Michael P; Manoharan, Vinothan N

    2011-12-04

    Young's law predicts that a colloidal sphere in equilibrium with a liquid interface will straddle the two fluids, its height above the interface defined by an equilibrium contact angle. This has been used to explain why colloids often bind to liquid interfaces, and has been exploited in emulsification, water purification, mineral recovery, encapsulation and the making of nanostructured materials. However, little is known about the dynamics of binding. Here we show that the adsorption of polystyrene microspheres to a water/oil interface is characterized by a sudden breach and an unexpectedly slow relaxation. The relaxation appears logarithmic in time, indicating that complete equilibration may take months. Surprisingly, viscous dissipation appears to play little role. Instead, the observed dynamics, which bear strong resemblance to ageing in glassy systems, agree well with a model describing activated hopping of the contact line over nanoscale surface heterogeneities. These results may provide clues to longstanding questions on colloidal interactions at an interface.

  1. Atomic Resolution Images of Solid-Liquid Interfaces

    NASA Astrophysics Data System (ADS)

    Giambattista, Brian; McNairy, W. W.; Slough, C. G.; Johnson, A.; Bell, L. D.; Coleman, R. V.; Schneir, J.; Sonnenfeld, R.; Drake, B.; Hansma, P. K.

    1987-07-01

    A scanning tunneling microscope (STM) can provide atomic-resolution images of solids covered with a variety of liquids, including cryogenic fluids, both polar and nonpolar solvents, conductive aqueous solutions, oils, and even greases. This short overview includes images of solids covered with liquid nitrogen, liquid helium, paraffin oil, silicone oil, microscope immersion oil, silicone vacuum grease, fluorocarbon grease, glycerol, and salt water. These images show atoms, charge-density waves, grains in an evaporated metal film, and even corrosion processes as they occur in real time. The future includes not only basic research in surface science but also applied research in lithography, lubrication, catalysis, corrosion, electrochemistry, and perhaps even biology.

  2. Study on Orbital Liquid Transport and Interface Behavior in Vane Tank

    NASA Astrophysics Data System (ADS)

    Kang, Qi; Rui, Wei

    2016-07-01

    Liquid propellant tank is used to supply gas free liquid for spacecraft as an important part of propulsion system. The liquid behavior dominated by surface tension in microgravity is obviously different with that on the ground, which put forward a new challenge to the liquid transport and relocation. The experiments which are investigated at drop tower in National Microgravity Lab have concentrated on liquid relocation following thruster firing. Considered that the liquid located at the bottom in the direction of the acceleration vector, a sphere scale vane tank is used to study the liquid-gas interface behaviors with different acceleration vector and different filling independently and we obtain a series of stable equilibrium interface and relocation time. We find that there is an obvious sedimentation in the direction of acceleration vector when fill rate greater than 2% fill. Suggestions have been put forward that outer vanes transferring liquid to the outlet should be fixed and small holes should be dogged at the vane close to the center post to improve the liquid flow between different vanes when B0 is greater than 2.5. The research about liquid transport alone ribbon vanes is simulated though software Flow3D. The simulation process is verified by comparing the liquid lip and vapor-liquid interface obtained from drop tower experiment and simulation result when fill rate is 15%. Then the influence of fill rate, numbers of vanes and the gap between vane and wall is studied through the same simulate process. Vanes' configurations are also changed to study the effect on the lip and liquid volume below some section. Some suggestions are put forward for the design of vanes.

  3. Interaction of monovalent ions with the water liquid-vapor interface - A molecular dynamics study

    NASA Technical Reports Server (NTRS)

    Wilson, Michael A.; Pohorille, Andrew

    1991-01-01

    Results of molecular dynamics calculations are presented for a series of ions at infinite dilution near the water liquid-vapor interface. The free energies of ion transfer from the bulk to the interface are discussed, as are the accompanying changes of water structure at the surface and ion mobilities as a function of their proximity to the interface. It is shown that simple dielectric models do not provide an accurate description of ions at the water surface. The results of the study should be useful in the development of better models incorporating the shape and molecular structure of the interface.

  4. Interaction of monovalent ions with the water liquid-vapor interface - A molecular dynamics study

    NASA Technical Reports Server (NTRS)

    Wilson, Michael A.; Pohorille, Andrew

    1991-01-01

    Results of molecular dynamics calculations are presented for a series of ions at infinite dilution near the water liquid-vapor interface. The free energies of ion transfer from the bulk to the interface are discussed, as are the accompanying changes of water structure at the surface and ion mobilities as a function of their proximity to the interface. It is shown that simple dielectric models do not provide an accurate description of ions at the water surface. The results of the study should be useful in the development of better models incorporating the shape and molecular structure of the interface.

  5. Synthesis of pure iron nanoparticles at liquid-liquid interface using pulsed plasma

    NASA Astrophysics Data System (ADS)

    Kelgenbaeva, Zhazgul; Omurzak, Emil; Takebe, Shintaro; Sulaimankulova, Saadat; Abdullaeva, Zhypargul; Iwamoto, Chihiro; Mashimo, Tsutomu

    2014-09-01

    Pure α-Fe nanoparticles with ≤10 nm size were synthesized using a simple method—pulsed plasma in liquid. This is the first time that pure metallic nanoparticles were prepared by arc discharge method using water-toluene interface as a medium. Several experiments made evident that toluene-water ratio in emulsion influences the purity and size of Fe nanoparticles. The purity of the nanoparticles gradually increased from 48 to 98 %, while particle size decreased from 21 to 9.5 nm with smaller toluene volume fraction (from 40 to 5 %) in the microemulsions. Finally, toluene:water with 95:5 (%) ratio was found to be the most appropriate medium for pure Fe nanoparticle formation. Lattice parameters of the obtained Fe samples calculated from XRD found to be larger ( a = 0.2927 nm) than those previously reported Fe ( a (BCC-Fe) = 0.2866 nm). HRTEM showed spherical-shaped Fe nanoparticles with partial aggregation. Vibrating sample magnetometer indicated superparamagnetic properties of particles with high-saturation magnetization ( M s = 125 emu g-1) at room temperature.

  6. Using silicon diodes for detecting the liquid-vapor interface in hydrogen

    NASA Technical Reports Server (NTRS)

    Dempsey, Paula J.; Fabik, Richard H.

    1992-01-01

    Tests were performed using commercially available silicon diode temperature sensors to detect the location of the liquid-vapor interface in hydrogen during ground test programs. Results show that by increasing the current into the sensor, silicon diodes can be used as liquid level point sensors. After cycling the sensors from liquid to vapor several times, it was found that with a 30 mA (milliamps) input current, the sensors respond within 2 seconds by measuring a large voltage difference when transitioning from liquid to vapor across the interface. Nearly instantaneous response resulted during a transition from vapor to liquid. Detailed here are test procedures, experimental results, and guidelines for applying this information to other test facilities.

  7. Using silicon diodes for detecting the liquid-vapor interface in hydrogen

    NASA Technical Reports Server (NTRS)

    Dempsey, Paula J.; Fabik, Richard H.

    1992-01-01

    Tests were performed using commercially available silicon diode temperature sensors to detect the location of the liquid-vapor interface in hydrogen during ground test programs. Results show that by increasing the current into the sensor, silicon diodes can be used as liquid level point sensors. After cycling the sensors from liquid to vapor several times, it was found that with a 30 mA (milliamps) input current, the sensors respond within 2 seconds by measuring a large voltage difference when transitioning from liquid to vapor across the interface. Nearly instantaneous response resulted during a transition form vapor to liquid. Detailed here are test procedures, experimental results, and guidelines for applying this information to other test facilities.

  8. Chiral interactions of the drug propranolol and α1-acid-glycoprotein at a micro liquid-liquid interface.

    PubMed

    Lopes, Paula; Kataky, Ritu

    2012-03-06

    The investigation of chiral interactions of drugs with plasma proteins is of fundamental importance for drug efficacy and toxicity studies. In this paper, we demonstrate a simple liquid-liquid interface procedure for investigating chiral interactions. Chiral discrimination of the enantiomers of a basic drug, propranolol, was achieved at a micro liquid-liquid interface, using α(1)-acid-glycoprotein (AGP) as a chiral acute phase plasma protein. When the protein is added to an aqueous phase containing the enantiomers of propranalol hydrochloride, the binding of (S)- and (R)-propranolol hydrochloride to the protein results in a decrease in the cyclic voltammetry (CV) and differential pulse voltammetry (DPV) current responses corresponding to the decrease in transfer of propranolol at an aqueous-1,2-dichloroethane interface. This decrease is a consequence of the complexation of the drug and the protein. The complex drug-protein does not transfer across the interface nor changes the transfer potential of the uncomplexed form of propranolol enantiomers. The bound concentration of propranolol enantiomers in the presence of AGP was found to be greater for (S)-propranolol than (R)-propranolol for solutions containing constant concentrations of AGP (50 μM). Scatchard analysis yielded association constants of 2.7 and 1.3 × 10(5) M(-1) for (S)- and (R)-propranolol, respectively.

  9. Detachment force of particles from air-liquid interfaces of films and bubbles.

    PubMed

    Ally, Javed; Kappl, Michael; Butt, Hans-Jürgen; Amirfazli, A

    2010-12-07

    The detachment force required to pull a microparticle from an air-liquid interface is measured using atomic force microscopy (AFM) and the colloidal probe technique. Water, solutions of sodium dodecyl sulfate (SDS), and silicone oils are tested in order to study the effects of surface tension and viscosity. Two different liquid geometries are considered: the air-liquid interface of a bubble and a liquid film on a solid substrate. It was shown that detaching particles from liquid films is fundamentally different than from bubbles or drops due to the restricted flow of the liquid phase. Additional force is required to detach a particle from a film, and the maximum force during detachment is not necessarily at the position where the particle breaks away from the interface (as seen in bubble or drop systems). This is due to the dynamics of meniscus formation and viscous effects, which must be considered if the liquid is constrained in a film. The magnitude of these effects is related to the liquid viscosity, film thickness, and detachment speed.

  10. Pressurized nano-liquid-junction interface for coupling capillary electrochromatography and nano-liquid chromatography with mass spectrometry.

    PubMed

    D'Orazio, Giovanni; Fanali, Salvatore

    2013-11-22

    A new nano-liquid-junction interface for coupling both capillary electrochromatography (CEC) or nano-liquid chromatography (nano-LC) with mass spectrometry (MS) was studied. The interface was a small T piece of polymeric material where capillary column and tip capillary were positioned at 180° while the third exit (at 90°) was occupied by a capillary delivering a liquid-assisting spray ionization for CEC experiments or by the electrode for the high voltage spray for nano-LC. Experiments were carried out analyzing mixtures of some organophosphorus pesticides (OPPs) or anti-inflammatory and related acidic drugs with MS detection in positive or negative ion mode, respectively. Analyzed OPPs compounds were baseline resolved utilizing the novel interface in both nano-LC and CEC obtaining good sensitivity and repeatability. For CEC-MS, the limits of detection ranged between 0.03 and 6.80 μg/mL and the intra-day repeatability was RSD <3.8% and <13% for the retention times and peak areas, respectively. The interface was easy to handle and good reproducibility, between 2.5 and 3.5% for the retention time and <10% for the efficiencies, was obtained when the interface was installed by two different analysts. Furthermore, it could be used for both CEC and nano-LC. Copyright © 2013 Elsevier B.V. All rights reserved.

  11. Vibrational Spectroscopy of Water at Liquid/Solid Interface

    NASA Astrophysics Data System (ADS)

    Yeganeh, M. S.

    1997-03-01

    The importance of the water/solid interface demands a complete microscopic understanding of the chemistry and physics describing the water/solid interactions. To make progress toward that goal, infrared-visible sum-frequency generation (SFG) was used to spectroscopically probe a water/Al2O3 buried interface. The variation of the OH resonance signal intensities with pH of the solution was related to the interfacial charge density. This variation led to the determination of the isoelectric point of the surface (IEPS) of Al2O3 and the mechanism in which water molecules adsorb on the surface of the solid.

  12. Temporally Anticorrelated Motion of Nanoparticles at a Liquid Interface.

    PubMed

    Wang, Dapeng; Hu, Renfeng; Skaug, Michael J; Schwartz, Daniel K

    2015-01-02

    Quantum dots at the hexane-glycerol interface exhibited unexpected behavior including highly dynamic adsorption/desorption, where the lateral nanoparticle motion was anomalously fast immediately after adsorption and prior to desorption. At the interface, particles exhibited pseudo-Brownian lateral motion, in which the instantaneous diffusion coefficient was temporally anticorrelated, in agreement with our simulations involving fractional Brownian motion in the surface-normal direction. These phenomena suggest that, in contrast to the conventional picture for colloidal particles, nanoparticles explore a landscape of metastable interfacial positions, with different exposures to the two adjacent phases.

  13. Influence of process parameters to composite interface organization and performance of liquid/solid bimetal

    NASA Astrophysics Data System (ADS)

    Rong, S. F.; Zhu, Y. C.; Wu, Y. H.; Yang, P. H.; Duan, X. L.; Zhou, H. T.

    2015-12-01

    The liquid-solid composite technique was used to prepare the high carbon high chromium steel (HCHCS) and low alloy steel (LCS) bimetal composite materials by means of insert casting method. The influence of some process parameters such as liquid-solid ratio, preheat temperature, pouring temperature on the interface microstructure and mechanical properties were studied. Interface microstructure and element distribution were analyzed. The results show that the interface microstructure becomes better, and bonding area becomes thicker with the increase of the volume of liquid to solid ratio, preheating temperature and pouring temperature. When the liquid-solid ratio is 8:1, the preheating temperature is 300 °C and the pouring temperature is 1565 °C, a good metallurgical bonding area without any hole can be obtained with the interface combination of diffusion and fusion. The composite interface structure was composed of a core material diffusion layer, a cooling solidification layer, a direction growth layer and some cell particles. The elements of C, Cr and Mn diffuse from the HCHCS side to the alloy steel side. The microhardness increased in the gradient from the LCS side to the HCHCS. The microhardness of the interface is significantly higher than that of LCS.

  14. Molecular-dynamics computer simulations of electronic absorption line shapes at liquid interfaces

    NASA Astrophysics Data System (ADS)

    Benjamin, Ilan; Michael, David

    1998-04-01

    Molecular dynamics computer simulations are used to study the electronic absorption line shapes of adsorbed chromophores at several liquid interfaces. Specifically considered are the liquid/vapor interface of water and the interface between water and a number of different organic liquids which are characterized by different dielectric constants, structure and polarizability. The chromophore used in the calculations is modeled after the common dye molecule DEPNA. Both non-polarizable and polarizable liquid and solute models are considered. The calculations demonstrate the effect of solvent polarity on the spectra, in agreement with recent experiments. These calculations demonstrate the effect of solvent polarity on the spectra, in agreement with recent experiments. These calculations also highlight the important effect due to the microscopic structure of the interface. A comparison of the results with predictions of continuum models is presented. Although these models can qualitatively account for the effect of interface polarity on the spectra, they must be extended to include structural aspects of the interface for better quantitative agreement.

  15. LAnse Aux Meadows, Newfoundland

    NASA Image and Video Library

    2008-07-18

    LAnse aux Meadows is a site on the northernmost tip of the island of Newfoundland, located in the Province of Newfoundland and Labrador, Canada, where the remains of a Viking village were discovered in 1960. This image is from NASA Terra satellite.

  16. Biological membrane modeling with a liquid/liquid interface. Probing mobility and environment with total internal reflection excited fluorescence.

    PubMed Central

    Morrison, L E; Weber, G

    1987-01-01

    Total internal reflection of exciting light, in combination with fluorescence intensity and polarization measurements, was used to selectively study fluorescent compounds adsorbed to the interface region between two immiscible liquids. A fluorometer was constructed which provided excitation at variable angles of incidence and allowed sensitive detection of polarized fluorescence emitted from the interface. The compound 4,4'-bis-1-phenylamino-8-naphthalenesulfonate (bis-ANS) was examined at a decalin/water interface and was found to possess remarkable affinity for the interface region with the bulk of the adsorbed molecule residing in the decalin phase. The adsorbed fluorophore displayed an apparent hindered rotation in the plane of the interface with a rotational diffusion coefficient 3- to 12-fold lower than that expected for bis-ANS in solution. While other dyes examined were not found to be significantly surface active, the addition of cationic surfactant sufficed to induce adsorption of the anionic fluorophore 1-aminonaphthalene-3,6,8-trisulfonic acid. This fluoropore was found to reside in an aqueous environment when bound to the interface, and it also exhibited hindered rotation in the plane of the interface. As the concentrations of the dyes were increased, both adsorbed dyes exhibited polarization reductions consistent with excitation energy transfer. Adsorption of bis-ANS was reversed by addition of bovine serum albumin. The membrane protein cytochrome b5 was found not to bind at the decalin/water interface, indicating that interaction with lipid is required for its adherence to biological membranes. PMID:3651556

  17. Electrohydrodynamic Displacement of Polarizable Liquid Interfaces in an Alternating Current Electric Field

    NASA Astrophysics Data System (ADS)

    Gagnon, Zachary

    2015-11-01

    In this work, we investigate Maxwell-Wagner polarization at electrically polarizable liquid interfaces. An AC electric field is applied across a liquid electrical interface created between two co-flowing microfluidic fluid streams with different electrical properties. When potentials as low as 2 volts are applied, we observe a frequency dependent interfacial displacement that is dependent on the relative differences in the electrical conductivity and dielectric constant between the two liquids. At low frequency this deflection is dependent on electrical conductivity, and only depends on dielectric constant at high frequency. At intermediate frequencies, we observe a crossover that is independent of applied voltage, sensitive to both fluid electrical properties, and where no displacement is observed. An analytical polarization model is presented that predicts the liquid interfacial crossover frequency, the dependence of interfacial displacement on liquid electrical conductivity and dielectric constant, and accurately scales the interface displacement measurements. The results show that liquid interfaces are capable of polarizing under AC electric fields and being precisely deflected in a direction and magnitude that is dependent on the applied electric field frequency.

  18. Modeling the Interface Instability and Mixing Flow During the Process of Liquid Explosion Dissemination

    NASA Astrophysics Data System (ADS)

    Li, L.; Xu, S. L.; Ren, Y. J.; Liu, G. R.; Ren, X. B.; Xie, W. J.; Li, Y. C.; Wang, Z. L.

    The liquid flow during the process of liquid explosion dissemination is a typical complex high-speed unsteady motion with multi-scale in space and time. The motion of liquid flow may be partitioned to several stages. The first is initial liquid expansion by the action of shock wave and explosive gaseous products. The second is breakup of liquid annulus and turbulent mixing, which is called near-field flow. The third is two-phase mixing flow of gas and liquid drops, which is called far-field flow. To first stage, a compressible inviscid liquid model was used, while an elastic and plastic model was used to depict the expansion of solid shell. Numerical study in two dimensional has been made by using the Arbitrary Euler-Lagrange (ALE) methods. In near-field, the unstable flow of liquid annulus is dominated by many factors. (1) The shock action of gaseous expansive products. (2) The geometric structure of wave system in liquid. (3) The local bubble and cavitating flow in annulus, induce much of local unstable interface, tear up interfaces, and enhance the instability and breakup of liquid annulus. In this paper, some postulations are proposed that the cavitations in liquid annulus are induced by shock wave and the flow of liquid annulus is a two phase flow (liquid and a discrete bubble groups). Some experimental results will be presented that the breakup of interface and turbulent mixing is visualized qualitatively and measured quantitatively by using shadow photography method. The primary results are some flow patten of interfaces and some transient flow parameters by which the nonlinear character will be obtained, and provide an experiential support for modeling to unstable interface flow and turbulent mixing. The two-phase mixing flow between liquid drops and gas in far-field can be studied by numerical methods where the turbulent motion of gas phase is represented with k-ɛ model in Euler system, the motion of particle phase is represented with particle stochastic

  19. Liquid-liquid interfaces as potentiometric ion-sensors-I The n-butanol-water interface as indicating sensor for the potentiometric titration of some acids and bases.

    PubMed

    Liteanu, C; Mioşcu, M

    1972-07-01

    The property that liquid-liquid interfaces modify their electrical charge as a function of the composition of the two phases in contact has been used to detect the end-points in a series of acid-base titrations in the aqueous phase. Although the titration curves are not classical in shape, the equivalence points can be located if the solutions are not too dilute. Good results for concentrations down to 10(-3)N have been obtained. The electrode has a fast response. The influence of surface-active substances on the titration has also been investigated.

  20. Semiconductor/Liquid Junctions: Molecular Manipulation of Interface Energetics.

    DTIC Science & Technology

    1980-11-21

    S. Wrighton. (Published: Acc. Chem. Res., 1979, 12, 303.) ONR-TR-3 "N-Type Molybdenum Diselenide-Based Liquid Junction Solar Cells : A Non-Aqueous...579. The high hts of our accomplishments in these areas are given in the paragraphs \\elow. N-Type MoY2/Liquid Electrolyte Junctions. N-type MoS2 and...examination of a wider range of redox reagents than is possible in H20; we found that both n-type MoS2 and MoSe 2 resist photoanodic decomposition in CH3CN

  1. Self-assembly of iron oxide-poly(ethylene glycol) core-shell nanoparticles at liquid-liquid interfaces.

    PubMed

    Isa, Lucio; Amstad, Esther; Textor, Marcus; Reimhult, Erik

    2010-01-01

    Nanoparticles (NPs) play an increasingly important role in the fabrication of functional advanced materials. Two major steps need to be carried out in order to achieve control of the material properties. First of all, the properties of the single NPs have to be under control, especially in relation to colloidal stability; aggregation and corrosion negate all the benefits associated to the nanoscopic dimensions. Secondly, the assembly process has to be controlled to achieve a material with the desired properties. We propose here to use stabilized ceramic NPs consisting of a magnetite core, coated by a poly(ethylene glycol) (PEG) shell and study their assembly at polar/ non-polar liquid interfaces, en route to fabricating functional NP membranes. These NPs show extraordinary stability in aqueous solutions achieved by anchoring linear PEG chains through an end-terminating nitroDOPA group to their surface. Furthermore, the core and shell sizes of these NPs can be independently varied with ease. We first describe the details of the NP synthesis and stabilization in bulk solutions, discussing the PEG molecular weight needed to achieve bulk stability. Subsequently, we demonstrate self-assembly of these particles at liquid-liquid interfaces (SALI) into monolayers of stable properties. SALI has been chosen as path for the assembly given its suitability for fabricating two-dimensional materials. We report here results from pendant drop tensiometry which illustrate the kinetics of NP adsorption at the liquid-liquid interface and highlight the role played by the molecular weight of the PEG shell in the interfacial assembly. In particular we show that the requisites to ensure particle stability at a liquid interface are more stringent compared to the bulk case.

  2. Self-healing gold mirrors and filters at liquid-liquid interfaces.

    PubMed

    Smirnov, Evgeny; Peljo, Pekka; Scanlon, Micheál D; Gumy, Frederic; Girault, Hubert H

    2016-04-14

    The optical and morphological properties of lustrous metal self-healing liquid-like nanofilms were systematically studied for different applications (e.g., optical mirrors or filters). These nanofilms were formed by a one-step self-assembly methodology of gold nanoparticles (AuNPs) at immiscible water-oil interfaces, previously reported by our group. We investigated a host of experimental variables and herein report their influence on the optical properties of nanofilms: AuNP mean diameter, interfacial AuNP surface coverage, nature of the organic solvent, and nature of the lipophilic organic molecule that caps the AuNPs in the interfacial nanofilm. To probe the interfacial gold nanofilms we used in situ (UV-vis-NIR spectroscopy and optical microscopy) as well as ex situ (SEM and TEM of interfacial gold nanofilms transferred to silicon substrates) techniques. The interfacial AuNP surface coverage strongly influenced the morphology of the interfacial nanofilms, and in turn their maximum reflectance and absorbance. We observed three distinct morphological regimes; (i) smooth 2D monolayers of "floating islands" of AuNPs at low surface coverages, (ii) a mixed 2D/3D regime with the beginnings of 3D nanostructures consisting of small piles of adsorbed AuNPs even under sub-full-monolayer conditions and, finally, (iii) a 3D regime characterised by the 2D full-monolayer being covered in significant piles of adsorbed AuNPs. A maximal value of reflectance reached 58% in comparison with a solid gold mirror, when 38 nm mean diameter AuNPs were used at a water-nitrobenzene interface. Meanwhile, interfacial gold nanofilms prepared with 12 nm mean diameter AuNPs exhibited the highest extinction intensities at ca. 690 nm and absorbance around 90% of the incident light, making them an attractive candidate for filtering applications. Furthermore, the interparticle spacing, and resulting interparticle plasmon coupling derived optical properties, varied significantly on replacing

  3. Influence of Melt Convection on Solid-Liquid Interface Under Terrestrial and Reduced Gravity Environments

    NASA Technical Reports Server (NTRS)

    Glicksman, M. E.

    1985-01-01

    Solidification and crystal growth processes involve thermal and solutal gradients within a molten phase. In the presence of gravity, such gradients result in convective flows which interact with diffusion fields at the solid-liquid interface. Dendritic growth kinetics was studied in transparent model systems which freeze similarily to most metals. Succinonitrile shows a strong influence of convection at supercoolings below about 1K. Fluid flows adjacent to solid-liquid interfaces and the behavior of shear flows in vertical annular geometries are studied. Novel low-frequency eigenstates were discovered and classified as coupled modes, for their involvement with interfacial deformation coupled to the fluid flow, and are unknown in systems without deformable interfaces. The dependence of coupled convection modes on interfacial geometry, gravity, fluid properties, and transformation characteristics studied for several annual flow arrangements with nominally pure solid-liquid systems.

  4. Understanding the lateral movement of particles adsorbed at a solid-liquid interface.

    PubMed

    Savaji, Kunal; Li, Xue; Couzis, Alexander

    2015-09-01

    In this paper we study the phenomenon of lateral movement of particles that are electrostatically adsorbed at a solid-liquid interface. The experimental system involves negatively charged silica particles of two different sizes (65 nm and 90 nm) that are exposed to the positively charged solid surface (silane coated silicon wafer) in sequential steps. The particle-adsorbed wafers are analyzed under a scanning electron microscope and the images are processed to determine the pair-correlation function for the particles adsorbed in the first step. From the pair correlation data and the particle surface coverage data we show that the adsorbed particles are mobile at the solid-liquid interface. In specific, we show that the adsorbed particles are mobile at the solid-liquid interface when there is a driving force for the adsorbed particles to move. The driving force in the scheme of experiments discussed in this paper is the reduction in the free energy of the system.

  5. Recent advances in Many Body Dissipative Particles Dynamics simulations of liquid-vapor interfaces.

    PubMed

    Ghoufi, Aziz; Emile, Janine; Malfreyt, Patrice

    2013-01-01

    Many Body Dissipative Particles Dynamics (MDPD) simulation is a novel promising mesoscopic method to model the liquid-vapor interfaces. Based upon works of Paganobarraga and Frenkel (J. Chem. Phys. 15, 5015 (2001)) and Trofimov (J. Chem. Phys. 117, 9383 (2002)) and of Warren (Phys. Rev. E 68, 066702 (2003)) this method has been critically reviewed during this last decade. We propose here to give an overview of the Many Body Dissipative Particles Dynamic simulation within the framework of the liquid-vapor interfaces. We recall the theoretical background of MDPD and we present some recent results of systems of interest such as water liquid-vapor interfaces and salt effect on water surface tension. Additionally we discuss the ability of MDPD to capture the mechanisms at the mesoscopic scale through the formation of micelles and the coalescence of a nanodroplet water on water surface.

  6. Spectral mapping of heat transfer mechanisms at liquid-solid interfaces

    NASA Astrophysics Data System (ADS)

    Sääskilahti, K.; Oksanen, J.; Tulkki, J.; Volz, S.

    2016-05-01

    Thermal transport through liquid-solid interfaces plays an important role in many chemical and biological processes, and better understanding of liquid-solid energy transfer is expected to enable improving the efficiency of thermally driven applications. We determine the spectral distribution of thermal current at liquid-solid interfaces from nonequilibrium molecular dynamics, delivering a detailed picture of the contributions of different vibrational modes to liquid-solid energy transfer. Our results show that surface modes located at the Brillouin zone edge and polarized along the liquid-solid surface normal play a crucial role in liquid-solid energy transfer. Strong liquid-solid adhesion allows also for the coupling of in-plane polarized modes in the solid with the liquid, enhancing the heat-transfer rate and enabling efficient energy transfer up to the cutoff frequency of the solid. Our results provide fundamental understanding of the energy-transfer mechanisms in liquid-solid systems and enable detailed investigations of energy transfer between, e.g., water and organic molecules.

  7. Interface reorientation of cryogenic liquids under non-isothermal boundary conditions

    NASA Astrophysics Data System (ADS)

    Kulev, Nikolai; Basting, Steffen; Bänsch, Eberhard; Dreyer, Michael

    2014-07-01

    We investigate the capillary driven oscillations of the liquid-vapor interface in cryogenic systems under non-isothermal boundary conditions. The oscillations took place in a partly filled cylinder during the interface reorientation from its 1 g equilibrium position to the microgravity equilibrium position after a step reduction of gravity. The latter was achieved by dropping the experimental device in the drop tower of Bremen, providing 4.7 s of microgravity. Liquid argon (Tsat=87.3 K at 1013 hPa) and liquid methane (Tsat=111.7 K at 1013 hPa) were used as experimental liquids. Axial wall temperature gradients, corresponding to a linear increase of the wall temperature, were applied above the interface position prior to the experiments with values varying between 0.2 K/mm and 2.9 K/mm. Both liquids showed a qualitatively similar reorientation behavior. The reorientation characteristics were found to depend on the value of the applied gradient and on the material properties of the experimental liquids. Numerical simulation showed a good qualitative agreement with a previous experiment with 1.34 K/mm using liquid argon, demonstrating main characteristic features of the experiment.

  8. Ab initio study on the dynamics of furfural at the liquid-solid interfaces

    NASA Astrophysics Data System (ADS)

    Dang, Hongli; Xue, Wenhua; Shields, Darwin; Liu, Yingdi; Jentoft, Friederike; Resasco, Daniel; Wang, Sanwu

    2013-03-01

    Catalytic biomass conversion sometimes occurs at the liquid-solid interfaces. We report ab initio molecular dynamics simulations at finite temperatures for the catalytic reactions involving furfural at the water-Pd and water-Cu interfaces. We found that, during the dynamic process, the furan ring of furfural prefers to be parallel to the Pd surface and the aldehyde group tends to be away from the Pd surface. On the other hand, at the water-Cu(111) interface, furfural prefers to be tilted to the Cu surface while the aldehyde group is bonded to the surface. In both cases, interaction of liquid water and furfural is identified. The difference of dynamic process of furfural at the two interfaces suggests different catalytic reaction mechanisms for the conversion of furfural, consistent with the experimental investigations. Supported by DOE (DE-SC0004600). Simulations and calculations were performed on XSED's and NERSC's supercomputers

  9. Surfactant-Triggered Nanoarchitectonics of Fullerene C60 Crystals at a Liquid-Liquid Interface.

    PubMed

    Shrestha, Lok Kumar; Shrestha, Rekha Goswami; Hill, Jonathan P; Tsuruoka, Tohru; Ji, Qingmin; Nishimura, Toshiyuki; Ariga, Katsuhiko

    2016-11-29

    Here, we report the structural and morphological modulation of fullerene C60 crystals induced by nonionic surfactants diglycerol monolaurate (C12G2) and monomyristate (C14G2). C60 crystals synthesized at a liquid-liquid interface comprising isopropyl alcohol (IPA) and a saturated solution of C60 in ethylbenzene (EB) exhibited a one-dimensional (1D) morphology with well-defined faceted structure. Average length and diameter of the faceted rods were ca. 4.8 μm and 747 nm, respectively. Powder X-ray diffraction pattern (pXRD) confirmed a hexagonal-close packed (hcp) structure with cell dimensions ca. a = 2.394 nm and c = 1.388 nm. The 1D rod morphology of C60 crystals was transformed into "Konpeito candy-like" crystals (average diameter ca. 1.2 μm) when the C60 crystals were grown in the presence of C12G2 or C14G2 surfactant (1%) in EB. The pXRD spectra of "Konpeito-like" crystals could be assigned to the face-centered cubic (fcc) phase with cell dimensions ca. a = 1.4309 nm (for C12G2) and a = 1.4318 nm (for C14G2). However, clusters or aggregates of C60 lacking a uniform morphology were observed at lower surfactant concentrations (0.1%), although these crystals exhibited an fcc crystal structure. The self-assembled 1D faceted C60 crystals and "Konpeito-like" C60 crystals exhibited intense photoluminescence (PL) (∼35 times greater than pC60) and a blue-shifted PL intensity maximum (∼15 nm) compared to those of pC60, demonstrating the potential use of this method for the control of the optoelectronic properties of fullerene nanostructures. The "Konpeito-like" crystals were transformed into high surface area nanoporous carbon with a graphitic microstructure upon heat-treatment at 2000 °C. The heat-treated samples showed enhanced electrochemical supercapacitance performance (specific capacitance is ca. 175 F g(-1), which is about 20 times greater than pC60) with long cyclic stability demonstrating the potential of the materials in supercapacitor device

  10. A sharp interface method for compressible liquid-vapor flow with phase transition and surface tension

    NASA Astrophysics Data System (ADS)

    Fechter, Stefan; Munz, Claus-Dieter; Rohde, Christian; Zeiler, Christoph

    2017-05-01

    The numerical approximation of non-isothermal liquid-vapor flow within the compressible regime is a difficult task because complex physical effects at the phase interfaces can govern the global flow behavior. We present a sharp interface approach which treats the interface as a shock-wave like discontinuity. Any mixing of fluid phases is avoided by using the flow solver in the bulk regions only, and a ghost-fluid approach close to the interface. The coupling states for the numerical solution in the bulk regions are determined by the solution of local two-phase Riemann problems across the interface. The Riemann solution accounts for the relevant physics by enforcing appropriate jump conditions at the phase boundary. A wide variety of interface effects can be handled in a thermodynamically consistent way. This includes surface tension or mass/energy transfer by phase transition. Moreover, the local normal speed of the interface, which is needed to calculate the time evolution of the interface, is given by the Riemann solution. The interface tracking itself is based on a level-set method. The focus in this paper is the description of the two-phase Riemann solver and its usage within the sharp interface approach. One-dimensional problems are selected to validate the approach. Finally, the three-dimensional simulation of a wobbling droplet and a shock droplet interaction in two dimensions are shown. In both problems phase transition and surface tension determine the global bulk behavior.

  11. An Open Port Sampling Interface for Liquid Introduction Atmospheric Pressure Ionization Mass Spectrometry

    DOE PAGES

    Van Berkel, Gary J.; Kertesz, Vilmos

    2015-01-01

    RATIONALE: A simple method to introduce unprocessed samples into a solvent for rapid characterization by liquid introduction atmospheric pressure ionization mass spectrometry has been lacking. The continuous flow, self-cleaning open port sampling interface introduced here fills this void. METHODS: The open port sampling interface used a vertically aligned, co-axial tube arrangement enabling solvent delivery to the sampling end of the device through the tubing annulus and solvent aspiration down the center tube and into the mass spectrometer ionization source via the commercial APCI emitter probe. The solvent delivery rate to the interface was set to exceed the aspiration rate creatingmore » a continuous sampling interface along with a constant, self-cleaning spillover of solvent from the top of the probe. RESULTS: Using the open port sampling interface with positive ion mode APCI and a hybrid quadrupole time of flight mass spectrometer, rapid, direct sampling and analysis possibilities are exemplified with plastics, ballpoint and felt tip ink pens, skin, and vegetable oils. These results demonstrated that the open port sampling interface could be used as a simple, versatile and self-cleaning system to rapidly introduce multiple types of unprocessed, sometimes highly concentrated and complex, samples into a solvent flow stream for subsequent ionization and analysis by mass spectrometry. The basic setup presented here could be incorporated with any self-aspirating liquid introduction ionization source (e.g., ESI, APCI, APPI, ICP, etc.) or any type of atmospheric pressure sampling ready mass spectrometer system. CONCLUSIONS: The open port sampling interface provides a means to introduce and quickly analyze unprocessed solid or liquid samples with liquid introduction atmospheric pressure ionization source without fear of sampling interface or ionization source contamination.« less

  12. An Open Port Sampling Interface for Liquid Introduction Atmospheric Pressure Ionization Mass Spectrometry

    SciTech Connect

    Van Berkel, Gary J.; Kertesz, Vilmos

    2015-01-01

    RATIONALE: A simple method to introduce unprocessed samples into a solvent for rapid characterization by liquid introduction atmospheric pressure ionization mass spectrometry has been lacking. The continuous flow, self-cleaning open port sampling interface introduced here fills this void. METHODS: The open port sampling interface used a vertically aligned, co-axial tube arrangement enabling solvent delivery to the sampling end of the device through the tubing annulus and solvent aspiration down the center tube and into the mass spectrometer ionization source via the commercial APCI emitter probe. The solvent delivery rate to the interface was set to exceed the aspiration rate creating a continuous sampling interface along with a constant, self-cleaning spillover of solvent from the top of the probe. RESULTS: Using the open port sampling interface with positive ion mode APCI and a hybrid quadrupole time of flight mass spectrometer, rapid, direct sampling and analysis possibilities are exemplified with plastics, ballpoint and felt tip ink pens, skin, and vegetable oils. These results demonstrated that the open port sampling interface could be used as a simple, versatile and self-cleaning system to rapidly introduce multiple types of unprocessed, sometimes highly concentrated and complex, samples into a solvent flow stream for subsequent ionization and analysis by mass spectrometry. The basic setup presented here could be incorporated with any self-aspirating liquid introduction ionization source (e.g., ESI, APCI, APPI, ICP, etc.) or any type of atmospheric pressure sampling ready mass spectrometer system. CONCLUSIONS: The open port sampling interface provides a means to introduce and quickly analyze unprocessed solid or liquid samples with liquid introduction atmospheric pressure ionization source without fear of sampling interface or ionization source contamination.

  13. An open port sampling interface for liquid introduction atmospheric pressure ionization mass spectrometry.

    PubMed

    Van Berkel, Gary J; Kertesz, Vilmos

    2015-10-15

    A simple method to introduce unprocessed samples into a solvent for rapid characterization by liquid introduction atmospheric pressure ionization mass spectrometry has been lacking. The continuous flow, self-cleaning open port sampling interface introduced here fills this void. The open port sampling interface used a vertically aligned, co-axial tube arrangement enabling solvent delivery to the sampling end of the device through the tubing annulus and solvent aspiration down the center tube and into the ionization source of the mass spectrometer via the commercial APCI emitter probe. The solvent delivery rate to the interface was set to exceed the aspiration rate, creating a continuous sampling interface along with a constant, self-cleaning spillover of solvent from the top of the probe. Using the open port sampling interface with positive ion mode APCI and a hybrid quadrupole time-of-flight mass spectrometer, rapid, direct sampling and analysis possibilities are exemplified with plastics, ballpoint and felt tip ink pens, skin, and vegetable oils. These results demonstrated that the open port sampling interface could be used as a simple, versatile and self-cleaning system to rapidly introduce multiple types of unprocessed, sometimes highly concentrated and complex, samples into a solvent flow stream for subsequent ionization and analysis by mass spectrometry. The basic setup presented here could be incorporated with any self-aspirating liquid introduction ionization source (e.g., ESI, APCI, APPI, ICP, etc.) or any type of atmospheric pressure sampling-ready mass spectrometer system. The open port sampling interface provides a means to introduce and quickly analyze unprocessed solid or liquid samples with the liquid introduction atmospheric pressure ionization source without fear of sampling interface or ionization source contamination. Copyright © 2015 John Wiley & Sons, Ltd.

  14. Molecular dynamics study on condensation/evaporation coefficients of chain molecules at liquid-vapor interface

    NASA Astrophysics Data System (ADS)

    Nagayama, Gyoko; Takematsu, Masaki; Mizuguchi, Hirotaka; Tsuruta, Takaharu

    2015-07-01

    The structure and thermodynamic properties of the liquid-vapor interface are of fundamental interest for numerous technological implications. For simple molecules, e.g., argon and water, the molecular condensation/evaporation behavior depends strongly on their translational motion and the system temperature. Existing molecular dynamics (MD) results are consistent with the theoretical predictions based on the assumption that the liquid and vapor states in the vicinity of the liquid-vapor interface are isotropic. Additionally, similar molecular condensation/evaporation characteristics have been found for long-chain molecules, e.g., dodecane. It is unclear, however, whether the isotropic assumption is valid and whether the molecular orientation or the chain length of the molecules affects the condensation/evaporation behavior at the liquid-vapor interface. In this study, MD simulations were performed to study the molecular condensation/evaporation behavior of the straight-chain alkanes, i.e., butane, octane, and dodecane, at the liquid-vapor interface, and the effects of the molecular orientation and chain length were investigated in equilibrium systems. The results showed that the condensation/evaporation behavior of chain molecules primarily depends on the molecular translational energy and the surface temperature and is independent of the molecular chain length. Furthermore, the orientation at the liquid-vapor interface was disordered when the surface temperature was sufficiently higher than the triple point and had no significant effect on the molecular condensation/evaporation behavior. The validity of the isotropic assumption was confirmed, and we conclude that the condensation/evaporation coefficients can be predicted by the liquid-to-vapor translational length ratio, even for chain molecules.

  15. Molecular dynamics study on condensation/evaporation coefficients of chain molecules at liquid-vapor interface.

    PubMed

    Nagayama, Gyoko; Takematsu, Masaki; Mizuguchi, Hirotaka; Tsuruta, Takaharu

    2015-07-07

    The structure and thermodynamic properties of the liquid-vapor interface are of fundamental interest for numerous technological implications. For simple molecules, e.g., argon and water, the molecular condensation/evaporation behavior depends strongly on their translational motion and the system temperature. Existing molecular dynamics (MD) results are consistent with the theoretical predictions based on the assumption that the liquid and vapor states in the vicinity of the liquid-vapor interface are isotropic. Additionally, similar molecular condensation/evaporation characteristics have been found for long-chain molecules, e.g., dodecane. It is unclear, however, whether the isotropic assumption is valid and whether the molecular orientation or the chain length of the molecules affects the condensation/evaporation behavior at the liquid-vapor interface. In this study, MD simulations were performed to study the molecular condensation/evaporation behavior of the straight-chain alkanes, i.e., butane, octane, and dodecane, at the liquid-vapor interface, and the effects of the molecular orientation and chain length were investigated in equilibrium systems. The results showed that the condensation/evaporation behavior of chain molecules primarily depends on the molecular translational energy and the surface temperature and is independent of the molecular chain length. Furthermore, the orientation at the liquid-vapor interface was disordered when the surface temperature was sufficiently higher than the triple point and had no significant effect on the molecular condensation/evaporation behavior. The validity of the isotropic assumption was confirmed, and we conclude that the condensation/evaporation coefficients can be predicted by the liquid-to-vapor translational length ratio, even for chain molecules.

  16. Rapid X-ray reflectivity measurement using a new liquid interface reflectometer at SPring-8

    NASA Astrophysics Data System (ADS)

    Yano, Y. F.; Uruga, T.; Tanida, H.; Toyokawa, H.; Terada, Y.; Takagaki, M.; Yamada, H.

    2009-02-01

    X-ray reflectivity measurements of liquid surfaces were demonstrated using a recently developed liquid interface reflectometer at SPring-8. The reflectometer, equipped with a two-dimensional hybrid pixel array detector (PILATUS), achieved x-ray reflectivity towards 10-9 with an integration time at each angle of only 1 sec, offering enormous potential for rapid measurements. Time-resolved measurements at a time resolution of 1 min were performed on the adsorption process of a globular protein lysozyme on a water/air interface.

  17. The Wolf method applied to the liquid-vapor interface of water.

    PubMed

    Noé Mendoza, Francisco; López-Lemus, Jorge; Chapela, Gustavo A; Alejandre, José

    2008-07-14

    The Wolf method for the calculation of electrostatic interactions is applied in a liquid phase and at the liquid-vapor interface of water and its results are compared with those from the Ewald sums method. Molecular dynamics simulations are performed to calculate the radial distribution functions at room temperature. The interface simulations are used to obtain the coexisting densities and surface tension along the coexistence curve. The water model is a flexible version of the extended simple point charge model. The Wolf method gives good structural results, fair coexistence densities, and poor surface tensions as compared with those obtained using the Ewald sums method.

  18. Determinative factors of competitive advantage between aerobic bacteria for niches at the air-liquid interface.

    PubMed

    Yamamoto, Kyosuke; Haruta, Shin; Kato, Souichiro; Ishii, Masaharu; Igarashi, Yasuo

    2010-01-01

    We focused on bacterial interspecies relationships at the air-liquid interface where the formation of pellicles by aerobes was observed. Although an obligate aerobe (Brevibacillus sp. M1-5) was initially dominant in the pellicle population, a facultative aerobe (Pseudoxanthomonas sp. M1-3) emerged and the viability of M1-5 rapidly decreased due to severe competition for oxygen. Supplementation of the medium with carbohydrates allowed the two species to coexist at the air-liquid interface. These results indicate that the population dynamics within pellicles are primarily governed by oxygen utilization which was affected by a combination of carbon sources.

  19. Self-healing gold mirrors and filters at liquid-liquid interfaces

    NASA Astrophysics Data System (ADS)

    Smirnov, Evgeny; Peljo, Pekka; Scanlon, Micheál D.; Gumy, Frederic; Girault, Hubert H.

    2016-03-01

    The optical and morphological properties of lustrous metal self-healing liquid-like nanofilms were systematically studied for different applications (e.g., optical mirrors or filters). These nanofilms were formed by a one-step self-assembly methodology of gold nanoparticles (AuNPs) at immiscible water-oil interfaces, previously reported by our group. We investigated a host of experimental variables and herein report their influence on the optical properties of nanofilms: AuNP mean diameter, interfacial AuNP surface coverage, nature of the organic solvent, and nature of the lipophilic organic molecule that caps the AuNPs in the interfacial nanofilm. To probe the interfacial gold nanofilms we used in situ (UV-vis-NIR spectroscopy and optical microscopy) as well as ex situ (SEM and TEM of interfacial gold nanofilms transferred to silicon substrates) techniques. The interfacial AuNP surface coverage strongly influenced the morphology of the interfacial nanofilms, and in turn their maximum reflectance and absorbance. We observed three distinct morphological regimes; (i) smooth 2D monolayers of ``floating islands'' of AuNPs at low surface coverages, (ii) a mixed 2D/3D regime with the beginnings of 3D nanostructures consisting of small piles of adsorbed AuNPs even under sub-full-monolayer conditions and, finally, (iii) a 3D regime characterised by the 2D full-monolayer being covered in significant piles of adsorbed AuNPs. A maximal value of reflectance reached 58% in comparison with a solid gold mirror, when 38 nm mean diameter AuNPs were used at a water-nitrobenzene interface. Meanwhile, interfacial gold nanofilms prepared with 12 nm mean diameter AuNPs exhibited the highest extinction intensities at ca. 690 nm and absorbance around 90% of the incident light, making them an attractive candidate for filtering applications. Furthermore, the interparticle spacing, and resulting interparticle plasmon coupling derived optical properties, varied significantly on replacing

  20. Ion-specific induced fluctuations and free energetics of aqueous protein hydrophobic interfaces: toward connecting to specific-ion behaviors at aqueous liquid-vapor interfaces.

    PubMed

    Cui, Di; Ou, Shuching; Peters, Eric; Patel, Sandeep

    2014-05-01

    We explore anion-induced interface fluctuations near protein-water interfaces using coarse-grained representations of interfaces as proposed by Willard and Chandler ( J. Phys. Chem. B 2010 , 114 , 1954 - 1958 ). We use umbrella sampling molecular dynamics to compute potentials of mean force along a reaction coordinate bridging the state where the anion is fully solvated and one where it is biased via harmonic restraints to remain at the protein-water interface. Specifically, we focus on fluctuations of an interface between water and a hydrophobic region of hydrophobin-II (HFBII), a 71 amino acid residue protein expressed by filamentous fungi and known for its ability to form hydrophobically mediated self-assemblies at interfaces such as a water/air interface. We consider the anions chloride and iodide that have been shown previously by simulations as displaying specific-ion behaviors at aqueous liquid-vapor interfaces. We find that as in the case of a pure liquid-vapor interface, at the hydrophobic protein-water interface, the larger, less charge-dense iodide anion displays a marginal interfacial stability compared with that of the smaller, more charge-dense chloride anion. Furthermore, consistent with the results at aqueous liquid-vapor interfaces, we find that iodide induces larger fluctuations of the protein-water interface than chloride.

  1. Dynamic Evolution of the Evaporating Liquid-Vapor Interface in Micropillar Arrays.

    PubMed

    Antao, Dion S; Adera, Solomon; Zhu, Yangying; Farias, Edgardo; Raj, Rishi; Wang, Evelyn N

    2016-01-19

    Capillary assisted passively pumped thermal management devices have gained importance due to their simple design and reduction in energy consumption. The performance of these devices is strongly dependent on the shape of the curved interface between the liquid and vapor phases. We developed a transient laser interferometry technique to investigate the evolution of the shape of the liquid-vapor interface in micropillar arrays during evaporation heat transfer. Controlled cylindrical micropillar arrays were fabricated on the front side of a silicon wafer, while thin-film heaters were deposited on the reverse side to emulate a heat source. The shape of the meniscus was determined using the fringe patterns resulting from interference of a monochromatic beam incident on the thin liquid layer. We studied the evolution of the shape of the meniscus on these surfaces under various operating conditions including varying the micropillar geometry and the applied heating power. By monitoring the transient behavior of the evaporating liquid-vapor interface, we accurately measured the absolute location and shape of the meniscus and calculated the contact angle and the maximum capillary pressure. We demonstrated that the receding contact angle which determines the capillary pumping limit is independent of the microstructure geometry and the rate of evaporation (i.e., the applied heating power). The results of this study provide fundamental insights into the dynamic behavior of the liquid-vapor interface in wick structures during phase-change heat transfer.

  2. Nanoparticle self-assembly at the interface of liquid crystal droplets.

    PubMed

    Rahimi, Mohammad; Roberts, Tyler F; Armas-Pérez, Julio C; Wang, Xiaoguang; Bukusoglu, Emre; Abbott, Nicholas L; de Pablo, Juan J

    2015-04-28

    Nanoparticles adsorbed at the interface of nematic liquid crystals are known to form ordered structures whose morphology depends on the orientation of the underlying nematic field. The origin of such structures is believed to result from an interplay between the liquid crystal orientation at the particles' surface, the orientation at the liquid crystal's air interface, and the bulk elasticity of the underlying liquid crystal. In this work, we consider nanoparticle assembly at the interface of nematic droplets. We present a systematic study of the free energy of nanoparticle-laden droplets in terms of experiments and a Landau-de Gennes formalism. The results of that study indicate that, even for conditions under which particles interact only weakly at flat interfaces, particles aggregate at the poles of bipolar droplets and assemble into robust, quantized arrangements that can be mapped onto hexagonal lattices. The contributions of elasticity and interfacial energy corresponding to different arrangements are used to explain the resulting morphologies, and the predictions of the model are shown to be consistent with experimental observations. The findings presented here suggest that particle-laden liquid crystal droplets could provide a unique and versatile route toward building blocks for hierarchical materials assembly.

  3. Nanoparticle self-assembly at the interface of liquid crystal droplets

    PubMed Central

    Rahimi, Mohammad; Roberts, Tyler F.; Armas-Pérez, Julio C.; Wang, Xiaoguang; Bukusoglu, Emre; Abbott, Nicholas L.; de Pablo, Juan J.

    2015-01-01

    Nanoparticles adsorbed at the interface of nematic liquid crystals are known to form ordered structures whose morphology depends on the orientation of the underlying nematic field. The origin of such structures is believed to result from an interplay between the liquid crystal orientation at the particles’ surface, the orientation at the liquid crystal’s air interface, and the bulk elasticity of the underlying liquid crystal. In this work, we consider nanoparticle assembly at the interface of nematic droplets. We present a systematic study of the free energy of nanoparticle-laden droplets in terms of experiments and a Landau–de Gennes formalism. The results of that study indicate that, even for conditions under which particles interact only weakly at flat interfaces, particles aggregate at the poles of bipolar droplets and assemble into robust, quantized arrangements that can be mapped onto hexagonal lattices. The contributions of elasticity and interfacial energy corresponding to different arrangements are used to explain the resulting morphologies, and the predictions of the model are shown to be consistent with experimental observations. The findings presented here suggest that particle-laden liquid crystal droplets could provide a unique and versatile route toward building blocks for hierarchical materials assembly. PMID:25870304

  4. Anharmonicity, solvation forces, and resolution in atomic force microscopy at the solid-liquid interface

    NASA Astrophysics Data System (ADS)

    Voïtchovsky, Kislon

    2013-08-01

    Solid-liquid interfaces are central to nanoscale science and technology and control processes as diverse as self-assembly, heterogeneous catalysis, wetting, electrochemistry, or protein function. Experimentally, measuring the structure and dynamics of solid-liquid interfaces with molecular resolution remains a challenge. This task can, in principle, be achieved with atomic force microscopy (AFM), which functions locally, and with nanometer precision. When operated dynamically and at small amplitudes, AFM can provide molecular-level images of the liquid solvation layers at the interfaces. At larger amplitudes, results in the field of multifrequency AFM have shown that anharmonicities in the tip motion can provide quantitative information about the solid's mechanical properties. The two approaches probe opposite aspects of the interface and are generally seen as distinct. Here it is shown that, for amplitudes Aliquid, and subnanometer resolution can be achieved through solvation forces. For A>d, the tip trajectory becomes rapidly anharmonic due to the tip tapping the solid, and the resolution decreases. A nonlinear transition between the two regimes occurs for A˜d and can be quantified with the second harmonic of the tip oscillation. These results, confirmed by computer simulations, remain valid in most experimental conditions. Significantly, they provide an objective criterion to enhance resolution and to decide whether the results are dominated by the properties of the solid or of the liquid.

  5. Synergistic effect of dicarbollide anions in liquid-liquid extraction: a molecular dynamics study at the octanol-water interface.

    PubMed

    Chevrot, G; Schurhammer, R; Wipff, G

    2007-04-28

    We report a molecular dynamics study of chlorinated cobalt bis(dicarbollide) anions [(B(9)C(2)H(8)Cl(3))(2)Co](-)"CCD(-)" in octanol and at the octanol-water interface, with the main aim to understand why these hydrophobic species act as strong synergists in assisted liquid-liquid cation extraction. Neat octanol is quite heterogeneous and is found to display dual solvation properties, allowing to well solubilize CCD(-), Cs(+) salts in the form of diluted pairs or oligomers, without displaying aggregation. At the aqueous interface, octanol behaves as an amphiphile, forming either monolayers or bilayers, depending on the initial state and confinement conditions. In biphasic octanol-water systems, CCD(-) anions are found to mainly partition to the organic phase, thus attracting Cs(+) or even more hydrophilic counterions like Eu(3+) into that phase. The remaining CCD(-) anions adsorb at the interface, but are less surface active than at the chloroform interface. Finally, we compare the interfacial behavior of the Eu(BTP)(3)(3+) complex in the absence and in the presence of CCD(-) anions and extractant molecules. It is found that when the CCD(-)'s are concentrated enough, the complex is extracted to the octanol phase. Otherwise, it is trapped at the interface, attracted by water. These results are compared to those obtained with chloroform as organic phase and discussed in the context of synergistic effect of CCD(-) in liquid-liquid extraction, pointing to the importance of dual solvation properties of octanol and of the hydrophobic character of CCD(-) for synergistic extraction of cations.

  6. Water-mediated ion–ion interactions are enhanced at the water vapor–liquid interface

    PubMed Central

    Venkateshwaran, Vasudevan; Vembanur, Srivathsan; Garde, Shekhar

    2014-01-01

    There is overwhelming evidence that ions are present near the vapor–liquid interface of aqueous salt solutions. Charged groups can also be driven to interfaces by attaching them to hydrophobic moieties. Despite their importance in many self-assembly phenomena, how ion–ion interactions are affected by interfaces is not understood. We use molecular simulations to show that the effective forces between small ions change character dramatically near the water vapor–liquid interface. Specifically, the water-mediated attraction between oppositely charged ions is enhanced relative to that in bulk water. Further, the repulsion between like-charged ions is weaker than that expected from a continuum dielectric description and can even become attractive as the ions are drawn to the vapor side. We show that thermodynamics of ion association are governed by a delicate balance of ion hydration, interfacial tension, and restriction of capillary fluctuations at the interface, leading to nonintuitive phenomena, such as water-mediated like charge attraction. “Sticky” electrostatic interactions may have important consequences on biomolecular structure, assembly, and aggregation at soft liquid interfaces. We demonstrate this by studying an interfacially active model peptide that changes its structure from α-helical to a hairpin-turn–like one in response to charging of its ends. PMID:24889634

  7. Acoustic radiation forces at liquid interfaces impact the performance of acoustophoresis.

    PubMed

    Deshmukh, Sameer; Brzozka, Zbigniew; Laurell, Thomas; Augustsson, Per

    2014-09-07

    Acoustophoresis is a method well suited for cell and microbead separation or concentration for downstream analysis in microfluidic settings. One of the main limitations that acoustophoresis share with other microfluidic techniques is that the separation efficiency is poor for particle-rich suspensions. We report that flow laminated liquids can be relocated in a microchannel when exposed to a resonant acoustic field. Differences in acoustic impedance between two liquids cause migration of the high-impedance liquid towards an acoustic pressure node. In a set of experiments we charted this phenomenon and show herein that it can be used to either relocate liquids with respect to each other, or to stabilize the interface between them. This resulted in decreased medium carry-over when transferring microbeads (4% by volume) between suspending liquids using acoustophoresis. Furthermore we demonstrate that acoustic relocation of liquids occurs for impedance differences as low as 0.1%.

  8. AUX: a scripting language for auditory signal processing and software packages for psychoacoustic experiments and education.

    PubMed

    Kwon, Bomjun J

    2012-06-01

    This article introduces AUX (AUditory syntaX), a scripting syntax specifically designed to describe auditory signals and processing, to the members of the behavioral research community. The syntax is based on descriptive function names and intuitive operators suitable for researchers and students without substantial training in programming, who wish to generate and examine sound signals using a written script. In this article, the essence of AUX is discussed and practical examples of AUX scripts specifying various signals are illustrated. Additionally, two accompanying Windows-based programs and development libraries are described. AUX Viewer is a program that generates, visualizes, and plays sounds specified in AUX. AUX Viewer can also be used for class demonstrations or presentations. Another program, Psycon, allows a wide range of sound signals to be used as stimuli in common psychophysical testing paradigms, such as the adaptive procedure, the method of constant stimuli, and the method of adjustment. AUX Library is also provided, so that researchers can develop their own programs utilizing AUX. The philosophical basis of AUX is to separate signal generation from the user interface needed for experiments. AUX scripts are portable and reusable; they can be shared by other researchers, regardless of differences in actual AUX-based programs, and reused for future experiments. In short, the use of AUX can be potentially beneficial to all members of the research community-both those with programming backgrounds and those without.

  9. Rocket engine coaxial injector liquid/gas interface flow phenomena

    NASA Astrophysics Data System (ADS)

    Mayer, Wolfgang; Kruelle, Gerd

    1992-07-01

    Coaxial injectors are used for injecting and mixing propellants in cryogenic rocket engines. Theoretical and experimental studies are reported which show the significance for atomization and mixing of the physical processes involved in the coaxial injector flow. The impact of internal fluid jet motions on surface irritation is demonstrated. A model is presented which calculates droplet atomization quantities such as frequency, droplet diameter, and liquid core shape.

  10. Electron transport across metal/discotic liquid crystal interfaces

    NASA Astrophysics Data System (ADS)

    Boden, N.; Bushby, R. J.; Clements, J.; Movaghar, B.

    1998-03-01

    Electron transport across micron thick films of columnar hexagonal discotic liquid crystal phases homeotropically aligned between metal electrode surfaces has been studied both experimentally and theoretically. These molecules are unique in their combination of charge transport along individual molecular columns with liquidlike self-organization. Typical of organic insulators, a high resistance Ohmic regime is evident at fields of less than 0.05 MV cm-1, due to a low concentration of chemical impurities (n<109cm-3), and a space-charge injection regime at higher fields. Breakdown fields are reasonably high: in hexakis(hexyloxy)triphenylene they reach ˜5 MV cm-1 at room temperature. Our results show that triphenylene-based discotics form an excellent class of highly ordered optically transparent insulators. At high temperatures and high fields the current is injection controlled and exhibits typical tunneling and space charge limited, nonlinear I-V characteristics. Dramatic jumps in injection currents are observed at phase transitions. The change at the crystalline to liquid crystalline phase transition is mainly due to more efficient "wetting" of the electrode surface in the liquid crystalline phase, whilst at the liquid crystalline to isotropic phase transition it arises from the enhancement in the molecular mobility. The concepts of semiconducting gaps, band mobilities, and carrier injection rates are extended to these new materials. The experimental observations are interpreted in a framework which takes into account the important role played by liquidlike dynamics in establishing the microscopic structural order in, what is, otherwise a highly anisotropic and weakly bonded "molecular crystal."

  11. Economizer Based Data Center Liquid Cooling with Advanced Metal Interfaces

    SciTech Connect

    Timothy Chainer

    2012-11-30

    A new chiller-less data center liquid cooling system utilizing the outside air environment has been shown to achieve up to 90% reduction in cooling energy compared to traditional chiller based data center cooling systems. The system removes heat from Volume servers inside a Sealed Rack and transports the heat using a liquid loop to an Outdoor Heat Exchanger which rejects the heat to the outdoor ambient environment. The servers in the rack are cooled using a hybrid cooling system by removing the majority of the heat generated by the processors and memory by direct thermal conduction using coldplates and the heat generated by the remaining components using forced air convection to an air- to- liquid heat exchanger inside the Sealed Rack. The anticipated benefits of such energy-centric configurations are significant energy savings at the data center level. When compared to a traditional 10 MW data center, which typically uses 25% of its total data center energy consumption for cooling this technology could potentially enable a cost savings of up to $800,000-$2,200,000/year (assuming electricity costs of 4 to 11 cents per kilowatt-hour) through the reduction in electrical energy usage.

  12. Liquid-liquid extraction assisted by a carbon nanoparticles interface. Electrophoretic determination of atrazine in environmental samples.

    PubMed

    Caballero-Díaz, Encarnación; Simonet, Bartolomé; Valcárcel, Miguel

    2013-10-21

    A novel method for the determination of atrazine, using liquid-liquid extraction assisted by a nanoparticles film formed in situ and composed of organic solvent stabilized-carbon nanoparticles, is described. The presence of nanoparticles located at the liquid-liquid interface reinforced the extraction of analyte from matrix prior to capillary electrophoresis (CE) analysis. Some influential experimental variables were optimized in order to enhance the extraction efficiency. The developed procedure confirmed that carbon nanoparticles, especially multi-walled carbon nanotubes, are suitable to be used in sample treatment processes introducing new mechanisms of interaction with the analyte. The application of the proposed preconcentration method followed by CE detection enabled the determination of atrazine in spiked river water providing acceptable RSD values (11.6%) and good recoveries (about 87.0-92.0%). Additionally, a similar extraction scheme was tested in soil matrices with a view to further applications in real soil samples.

  13. Note: Sample cells to investigate solid/liquid interfaces with neutrons

    SciTech Connect

    Rennie, Adrian R. Hellsing, Maja S.; Lindholm, Eric; Olsson, Anders

    2015-01-15

    The design of sample cells to study solid/liquid interfaces by neutron reflection is presented. Use of standardized components and a modular design has allowed a wide range of experiments that include grazing incidence scattering and conventional small-angle scattering. Features that reduce background scattering are emphasized. Various flow arrangements to fill and replenish the liquid in the cell as well as continuous stirring are described.

  14. The physics of pattern formation at liquid interfaces

    SciTech Connect

    Maher, J.V.

    1992-06-01

    During the past year we have submitted six papers for publication, three related to the dynamics of macroscopic interfaces, and ultimately all related to solidification, and three related to the internal structure of disorderly materials, with possible applications to the processing of composite materials. In addition to completing all these projects during the past year, we have begun two new projects, one on pattern formation and one on aggregation within a composite system. A brief description is given of this research in this paper.

  15. Anisotropic solid-liquid interface kinetics in silicon: an atomistically informed phase-field model

    NASA Astrophysics Data System (ADS)

    Bergmann, S.; Albe, K.; Flegel, E.; Barragan-Yani, D. A.; Wagner, B.

    2017-09-01

    We present an atomistically informed parametrization of a phase-field model for describing the anisotropic mobility of liquid-solid interfaces in silicon. The model is derived from a consistent set of atomistic data and thus allows to directly link molecular dynamics and phase field simulations. Expressions for the free energy density, the interfacial energy and the temperature and orientation dependent interface mobility are systematically fitted to data from molecular dynamics simulations based on the Stillinger-Weber interatomic potential. The temperature-dependent interface velocity follows a Vogel-Fulcher type behavior and allows to properly account for the dynamics in the undercooled melt.

  16. PREFACE: Liquid-solid interfaces: structure and dynamics from spectroscopy and simulations Liquid-solid interfaces: structure and dynamics from spectroscopy and simulations

    NASA Astrophysics Data System (ADS)

    Gaigeot, Marie-Pierre; Sulpizi, Marialore

    2012-03-01

    Liquid-solid interfaces play an important role in a number of phenomena encountered in biological, chemical and physical processes. Surface-induced changes of the material properties are not only important for the solid support but also for the liquid itself. In particular, it is now well established that water at the interface is substantially different from bulk water, even in the proximity of apparently inert surfaces such as a simple metal. The complex chemistry at liquid-solid interfaces is typically fundamental to heterogeneous catalysis and electrochemistry, and has become especially topical in connection with the search for new materials for energy production. A quite remarkable example is the development of cheap yet efficient solar cells, whose basic components are dye molecules grafted to the surface of an oxide material and in contact with an electrolytic solution. In life science, the most important liquid-solid interfaces are the water-cell-membrane interfaces. Phenomena occurring at the surface of phospholipid bilayers control the docking of proteins, the transmission of signals as well as transport of molecules in and out of the cell. Recently the development of bio-compatible materials has lead to research on the interface between bio-compatible material and lipid/proteins in aqueous solution. Gaining a microscopic insight into the processes occurring at liquid-solid interfaces is therefore fundamental to a wide range of disciplines. This special section collects some contributions to the CECAM Workshop 'Liquid/Solid interfaces: Structure and Dynamics from Spectroscopy and Simulations' which took place in Lausanne, Switzerland in June 2011. Our main aim was to bring together knowledge and expertise from different communities in order to advance our microscopic understanding of the structure and dynamics of liquids at interfaces. In particular, one of our ambitions was to foster discussion between the experimental and theoretical

  17. Reduction in the surface energy of liquid interfaces at short length scales

    PubMed

    Fradin; Braslau; Luzet; Smilgies; Alba; Boudet; Mecke; Daillant

    2000-02-24

    Liquid-vapour interfaces, particularly those involving water, are common in both natural and artificial environments. They were first described as regions of continuous variation of density, caused by density fluctuations within the bulk phases. In contrast, the more recent capillary-wave models assumes a step-like local density profile across the liquid-vapour interface, whose width is the result of the propagation of thermally excited capillary waves. The model has been validated for length scales of tenths of micrometres and larger, but the structure of liquid surfaces on submicrometre length scales--where the capillary theory is expected to break down--remains poorly understood. Here we report grazing-incidence X-ray scattering experiments that allow for a complete determination of the free surface structure and surface energy for water and a range of organic liquids. We observe a large decrease of up to 75% in the surface energy of submicrometre waves that cannot be explained by capillary theory, but is in accord with the effects arising from the non-locality of attractive intermolecule interactions as predicted by a recent density functional theory. Our data, and the results of comparable measurements on liquid solutions, metallic alloys, surfactants, lipids and wetting films should thus provide a stringent test for any new theories that attempt to describe the structure of liquid interfaces with nanometre-scale resolution.

  18. Appropriate Formulations for Velocity and Pressure Calculations at Gas-liquid Interface with Collocated Variable Arrangement

    NASA Astrophysics Data System (ADS)

    Ito, Kei; Kunugi, Tomoaki

    A high-precision simulation algorithm for gas-liquid two-phase flows on unstructured meshes has been developed to simulate gas entrainment phenomenon in a sodium-cooled fast reactor. In this study, it became clear that unphysical behaviors near gas-liquid interfaces were caused by conventional algorithms. Then, physics-basis considerations were conducted for mechanical balances at gas-liquid interfaces to derive appropriate formulations. By defining momentum and velocity independently and developing the momentum transport equations for both gas and liquid phases, the physically appropriate formulation of momentum transport was derived, which eliminated the unphysical pressure distribution caused by the conventional formulation. In addition, the physically appropriate formulation was derived for the pressure gradient to satisfy the mechanical balances between pressure and surface tension at gas-liquid interfaces. As the validation test, the rising gas bubble in liquid was simulated by the developed simulation algorithm with the physically appropriate formulations, and the simulated terminal bubble shapes on the structured and highly-distorted unstructured meshes coincided with the experimental data under each simulation condition determined by the Morton and Eötvös numbers.

  19. Instructional Review: An Introduction to Optical Methods for Characterizing Liquid Crystals at Interfaces

    PubMed Central

    Miller, Daniel S.; Carlton, Rebecca J.; Mushenheim, Peter C.; Abbott, Nicholas L.

    2013-01-01

    This Instructional Review describes methods and underlying principles that can be used to characterize both the orientations assumed spontaneously by liquid crystals (LCs) at interfaces and the strength with which the LCs are held in those orientations (so-called anchoring energies). The application of these methods to several different classes of LC interfaces is described, including solid and aqueous interfaces as well as planar and non-planar interfaces (such as those that define a LC-in-water emulsion droplet). These methods, which enable fundamental studies of the ordering of LCs at polymeric, chemically-functionalized and biomolecular interfaces, are described in this article at a level that can be easily understood by a non-expert reader such as an undergraduate or graduate student. We focus on optical methods because they are based on instrumentation that is found widely in research and teaching laboratories. PMID:23347378

  20. Solute rotational dynamics at the water liquid/vapor interface

    NASA Astrophysics Data System (ADS)

    Benjamin, Ilan

    2007-11-01

    The rotational dynamics of a number of diatomic molecules adsorbed at different locations at the interface between water and its own vapors are studied using classical molecular dynamics computer simulations. Both equilibrium orientational and energy correlations and nonequilibrium orientational and energy relaxation correlations are calculated. By varying the dipole moment of the molecule and its location, and by comparing the results with those in bulk water, the effects of dielectric and mechanical frictions on reorientation dynamics and on rotational energy relaxation can be studied. It is shown that for nonpolar and weekly polar solutes, the equilibrium orientational relaxation is much slower in the bulk than at the interface. As the solute becomes more polar, the rotation slows down and the surface and bulk dynamics become similar. The energy relaxation (both equilibrium and nonequilibrium) has the opposite trend with the solute dipole (larger dipoles relax faster), but here again the bulk and surface results converge as the solute dipole is increased. It is shown that these behaviors correlate with the peak value of the solvent-solute radial distribution function, which demonstrates the importance of the first hydration shell structure in determining the rotational dynamics and dependence of these dynamics on the solute dipole and location.

  1. Morphological stability of a solid-liquid interface growing in a cylindrical mold

    NASA Astrophysics Data System (ADS)

    Kato, Hiroshi

    2016-12-01

    The morphological stability of the planar interface of dilute alloys solidifying in a cylindrical mold is analyzed based on the perturbation model presented by Mullins and Sekerka under the assumption that the interface crosses the mold wall at right angles, to examine the effect of the inside diameter of the mold. When the interface grows in a mold of a larger inside diameter, the stability-instability criterion of the planar interface is coincident with the MS criterion. On the other hand, in a mold of a smaller diameter, the rippled interface is permitted to take a frequency of discrete values (the permitted frequency), and the planar interface grows stably under thermal conditions slightly exceeding the MS criterion. Also, there exists a minimum permitted frequency ωmin, and the critical inside diameter dc is derived from ωmin. When the alloy solidifies in a mold of an inside diameter less than dc, the interface grows stably under thermal conditions in which the MS model predicts unstable growth of the interface. Moreover, there is a lower limit dG in dc, and when the alloy solidifies in a mold of an inside diameter less than dG, the interface grows stably even at a zero temperature gradient in the liquid.

  2. Rocket engine coaxial injector liquid/gas interface flow phenomena

    NASA Astrophysics Data System (ADS)

    Mayer, Wolfgang; Kruelle, Gerd

    1995-05-01

    Coaxial injectors are used for the injection and mixing of propellants H2/O2 in cryogenic rocket engines. The aim of the theoretical and experimental investigations presented here is to elucidate some of the physical processes in coaxial injector flow with respect to their significance for atomization and mixing. Experiments with the simulation fluids H2O and air were performed under ambient conditions and at elevated counter pressures up to 20 bar. This article reports on phenomenological studies of spray generation under a broad variation of parameters using nanolight photography and high-speed cinematography (up to 3 x 10(exp 4) frames/s). Detailed theoretical and experimental studies of the surface evolution of turbulent jets were performed. Proof was obtained of the impact of internal fluid jet motions on surface deformation. The m = 1 nonaxisymmetric instability of the liquid jet seems to be superimposed onto the small-scale atomization process. A model is presented that calculates droplet atomization quantities as frequency, droplet diameter, and liquid core shape. The overall procedure for implementing this model as a global spray model is also described and an example calculation is presented.

  3. Rocket engine coaxial injector liquid/gas interface flow phenomena

    SciTech Connect

    Mayer, W.; Kruelle, G.

    1995-05-01

    Coaxial injectors are used for the injection and mixing of propellants H2/O2 in cryogenic rocket engines. The aim of the theoretical and experimental investigations presented here is to elucidate some of the physical processes in coaxial injector flow with respect to their significance for atomization and mixing. Experiments with the simulation fluids H2O and air were performed under ambient conditions and at elevated counter pressures up to 20 bar. This article reports on phenomenological studies of spray generation under a broad variation of parameters using nanolight photography and high-speed cinematography (up to 3 x 10(exp 4) frames/s). Detailed theoretical and experimental studies of the surface evolution of turbulent jets were performed. Proof was obtained of the impact of internal fluid jet motions on surface deformation. The m = 1 nonaxisymmetric instability of the liquid jet seems to be superimposed onto the small-scale atomization process. A model is presented that calculates droplet atomization quantities as frequency, droplet diameter, and liquid core shape. The overall procedure for implementing this model as a global spray model is also described and an example calculation is presented. 15 refs.

  4. Coarse-Graining the Liquid-Liquid Interfaces with the MARTINI Force Field: How Is the Interfacial Tension Reproduced?

    PubMed

    Ndao, Makha; Devémy, Julien; Ghoufi, Aziz; Malfreyt, Patrice

    2015-08-11

    We report two-phase coarse-grained (CG) simulations of organic-water liquid-liquid interfaces with the MARTINI force field. We discuss the ability of the CG force field to predict quantitatively the interfacial tension of alkanes-water, benzene-water, chloroform-water, and alcohol-water systems. The performance of the prediction of the interfacial tension is evaluated through its dependence on temperature and alkane length. This study contributes to the challenging discussion about the robustness and the transferability of the MARTINI force field to interfacial properties. We have also used the distributions of the molecules along the direction normal to the interface to investigate the composition of the interfacial region and to compare the simulated densities of the coexisting phases with experiments.

  5. Possible fossil H2O liquid-ice interfaces in the Martian crust

    NASA Technical Reports Server (NTRS)

    Soderblom, L. A.; Wenner, D. B.

    1978-01-01

    The extensive chaotic and fretted terrains in the equatorial regions of Mars are explained on the basis of the vertical distribution of H2O liquid and ice which once existed in the crust. This account assumes that below the permafrost containing water ice, there was a second zone in which liquid water resided for at least a time. Diagenetic alteration and cementation characterized the material in the subpermafrost zone; above, pristine fragmented material with various ice concentrations was found. Later, the ice-laden zone was stripped away by a number of erosional processes, exposing the former ice-liquid water interface.

  6. Possible fossil H2O liquid-ice interfaces in the Martian crust

    NASA Technical Reports Server (NTRS)

    Soderblom, L. A.; Wenner, D. B.

    1978-01-01

    The extensive chaotic and fretted terrains in the equatorial regions of Mars are explained on the basis of the vertical distribution of H2O liquid and ice which once existed in the crust. This account assumes that below the permafrost containing water ice, there was a second zone in which liquid water resided for at least a time. Diagenetic alteration and cementation characterized the material in the subpermafrost zone; above, pristine fragmented material with various ice concentrations was found. Later, the ice-laden zone was stripped away by a number of erosional processes, exposing the former ice-liquid water interface.

  7. DNA separation at a liquid-solid interface.

    PubMed

    Seo, Young-Soo; Samuilov, Vladimir A; Sokolov, Jonathan; Rafailovich, Miriam; Tinland, Bernard; Kim, Jaeseung; Chu, Benjamin

    2002-08-01

    We demonstrate that it is possible to separate a broad band of DNA on a solid substrate without topological obstacles. The mobility was found to scale with molecular size (N) as N(-0.25), while the resolution scaled as N(0.75) indicating that diffusivity on this substrate was minimal. By varying the buffer concentration we were able to show that the mobility for a given chain length scaled with the persistent length (p) as p(1/2). This could be shown to be related to the Gaussian conformation of the chains adsorbed on the surface. A two-dimensional corrugated surface of nonporous silica beads was produced using a self-assembling process at the air/water interface. Even though the surface corrugations were comparable to persistence length we show that they do not affect the mobility, indicating that surface friction rather than topological constraints are the predominant mechanism of separation on a surface.

  8. Spherical Monovalent Ions at Aqueous Liquid-Vapor Interfaces: Interfacial Stability and Induced Interface Fluctuations

    PubMed Central

    Ou, Shuching; Hu, Yuan; Patel, Sandeep; Wan, Hongbin

    2014-01-01

    Ion-specific interfacial behaviors of monovalent halides impact processes such as protein denaturation, interfacial stability, surface tension modulation, and as such, their molecular and thermodynamic underpinnings garner much attention. We use molecular dynamics simulations of monovalent anions in water to explore effects on distant interfaces. We observe long-ranged ion-induced perturbations of the aqueous environment as suggested by experiment and theory. Surface stable ions, characterized as such by minima in potentials of mean force computed using umbrella sampling MD simulations, induce larger interfacial fluctuations compared to non-surface active species, conferring more entropy approaching the interface. Smaller anions and cations show no interfacial potential of mean force minima. The difference is traced to hydration shell properties of the anions, and the coupling of these shells with distant solvent. The effects correlate with the positions of the anions in the Hofmeister series (acknowledging variations in force field ability to recapitulate essential underlying physics), suggesting how differences in induced, non-local perturbations of interfaces may be related to different specific-ion effects in dilute biophysical and nanomaterial systems. PMID:24032752

  9. Mean-Field Approximation to the Hydrophobic Hydration in the Liquid-Vapor Interface of Water.

    PubMed

    Abe, Kiharu; Sumi, Tomonari; Koga, Kenichiro

    2016-03-03

    A mean-field approximation to the solvation of nonpolar solutes in the liquid-vapor interface of aqueous solutions is proposed. It is first remarked with a numerical illustration that the solvation of a methane-like solute in bulk liquid water is accurately described by the mean-field theory of liquids, the main idea of which is that the probability (Pcav) of finding a cavity in the solvent that can accommodate the solute molecule and the attractive interaction energy (uatt) that the solute would feel if it is inserted in such a cavity are both functions of the solvent density alone. It is then assumed that the basic idea is still valid in the liquid-vapor interface, but Pcav and uatt are separately functions of different coarse-grained local densities, not functions of a common local density. Validity of the assumptions is confirmed for the solvation of the methane-like particle in the interface of model water at temperatures between 253 and 613 K. With the mean-field approximation extended to the inhomogeneous system the local solubility profiles across the interface at various temperatures are calculated from Pcav and uatt obtained at a single temperature. The predicted profiles are in excellent agreement with those obtained by the direct calculation of the excess chemical potential over an interfacial region where the solvent local density varies most rapidly.

  10. Evaluation of air-liquid interface exposure systems for in vitro assessment of airborne pollutants

    EPA Science Inventory

    Exposure of cells to airborne pollutants at the air-liquid interface (ALI) is a more realistic approach than exposures of submerged cells. The published literature, however, describes irreproducible and/or unrealistic experimental conditions using ALI systems. We have compared fi...

  11. Step free energies at faceted solid-liquid interfaces from equilibrium molecular dynamics simulations.

    PubMed

    Frolov, T; Asta, M

    2012-12-07

    In this work a method is proposed for computing step free energies for faceted solid-liquid interfaces based on atomistic simulations. The method is demonstrated in an application to (111) interfaces in elemental Si, modeled with the classical Stillinger-Weber potential. The approach makes use of an adiabatic trapping procedure, and involves simulations of systems with coexisting solid and liquid phases separated by faceted interfaces containing islands with different sizes, for which the corresponding equilibrium temperatures are computed. We demonstrate that the calculated coexistence temperature is strongly affected by the geometry of the interface. We find that island radius is inversely proportional to superheating, allowing us to compute the step free energy by fitting simulation data within the formalism of classical nucleation theory. The step free energy value is computed to be γ(st) = 0.103 ± 0.005 × 10(-10) J/m. The approach outlined in this work paves the way to the calculation of step free energies relevant to the solidification of faceted crystals from liquid mixtures, as encountered in nanowire growth by the vapor-liquid-solid mechanism and in alloy casting. The present work also shows that at low undercoolings the Stillinger-Weber interatomic potential for Si tends to crystallize in the wurtzite, rather than the diamond-cubic structure.

  12. Molecular dynamics of phenol at the liquid-vapor interface of water

    NASA Technical Reports Server (NTRS)

    Pohorille, Andrew; Benjamin, Ilan

    1991-01-01

    Results of molecular dynamics calculations on phenol at the water liquid-vapor interface are presented. The density profile of the center of mass of phenol exhibits a maximum 1 A from the Gibbs surface toward the vapor phase, indicating that the molecule is surface-active. Changes in the profile caused by the interface extend 6 A from the Gibbs surface into the liquid, significantly more than change in the density profile of water. The most probable orientation of the solute at the surface is such that its symmetry axis is perpendicular to the interface with the OH substituent pointing toward the liquid. An additional simulation with benzene shows that this molecule at the surface most often adopts orientations parallel to the interface. Deeper in the liquid all the solutes are preferentially ordered perpendicular to the surface. In the interfacial region the orientational preferences of the solute are primarily determined by cavity formation needed to accommodate the hydrophobic portion of the dissolved molecule.

  13. Monitoring the solid-liquid interface in tanks using profiling sonar and 3D visualization techniques

    NASA Astrophysics Data System (ADS)

    Sood, Nitin; Zhang, Jinsong; Roelant, David; Srivastava, Rajiv

    2005-03-01

    Visualization of the interface between settled solids and the optically opaque liquid above is necessary to facilitate efficient retrieval of the high-level radioactive waste (HLW) from underground storage tanks. A profiling sonar was used to generate 2-D slices across the settled solids at the bottom of the tank. By incrementally rotating the sonar about its centerline, slices of the solid-liquid interface can be imaged and a 3-D image of the settled solids interface generated. To demonstrate the efficacy of the sonar in real-time solid-liquid interface monitoring systems inside HLW tanks, two sets of experiments were performed. First, various solid objects and kaolin clay (10 μm dia) were successfully imaged while agitating with 30% solids (by weight) entrained in the liquid. Second, a solid with a density similar to that of the immersed fluid density was successfully imaged. Two dimensional (2-D) sonar images and the accuracy and limitations of the in-tank imaging will be presented for these two experiments. In addition, a brief review of how to utilize a 2-D sonar image to generate a 3-D surface of the settled layer within a tank will be discussed.

  14. Molecular dynamics of phenol at the liquid-vapor interface of water

    NASA Technical Reports Server (NTRS)

    Pohorille, Andrew; Benjamin, Ilan

    1991-01-01

    Results of molecular dynamics calculations on phenol at the water liquid-vapor interface are presented. The density profile of the center of mass of phenol exhibits a maximum 1 A from the Gibbs surface toward the vapor phase, indicating that the molecule is surface-active. Changes in the profile caused by the interface extend 6 A from the Gibbs surface into the liquid, significantly more than change in the density profile of water. The most probable orientation of the solute at the surface is such that its symmetry axis is perpendicular to the interface with the OH substituent pointing toward the liquid. An additional simulation with benzene shows that this molecule at the surface most often adopts orientations parallel to the interface. Deeper in the liquid all the solutes are preferentially ordered perpendicular to the surface. In the interfacial region the orientational preferences of the solute are primarily determined by cavity formation needed to accommodate the hydrophobic portion of the dissolved molecule.

  15. Pattern formation at liquid interfaces II. The KI/chloral hydrate/starch system

    NASA Astrophysics Data System (ADS)

    Liu, Cliff Zeh-Wen; Knobler, Charles M.

    1992-02-01

    Measurements are reported of pattern formation at a liquid interface produced by a photochemical reaction involving the system KI/chloral hydrate/ starch. The dependence of the wavelength on the concentrations of the reactants, the viscosity, and the height of the sample has been examined. It is concluded that the pattern is produced by a hydrodynamic mechanism.

  16. Thermocapillary Interaction between a Solid Particle and a Liquid-Gas Interface

    NASA Astrophysics Data System (ADS)

    Golovin, A. A.; Leshansky, A. M.; Nir, A.

    1996-11-01

    Interaction between solid particles and a free liquid-gas interface is very important for flotation processes and for various processes involving multiphase flows. In the present contribution, interaction between a hot solid particle submerged into an ambient fluid, and a free liquid-gas interface is considered. A non-uniform temperature field around the solid particle produces surface tension gradients at the liquid-gas interface which generate a thermocapillary flow in the surrounding fluid. This flow yields the motion of the solid particle itself. Three cases are considered: (i) interaction between a solid particle and a spherical gas bubble at a finite separation distance; (ii) thermocapillary motion of a solid particle and an attached gas bubble; (iii) interaction between a solid particle and a plane undeformable liquid-gas interface. In all cases the velocity of the thermocapillarity induced motion of the solid particle is calculated in the approximation of the Stokes flow and a low Peclet number as a function of the separation distance and the bubble-to-particle radii ratio. Some preliminary results of the present work have been published in (A.A.Golovin, Int. J. Multiphase Flow 21), 715 (1995)..

  17. Evaluation of air-liquid interface exposure systems for in vitro assessment of airborne pollutants

    EPA Science Inventory

    Exposure of cells to airborne pollutants at the air-liquid interface (ALI) is a more realistic approach than exposures of submerged cells. The published literature, however, describes irreproducible and/or unrealistic experimental conditions using ALI systems. We have compared fi...

  18. Shape and Effective Spring Constant of Liquid Interfaces Probed at the Nanometer Scale: Finite Size Effects.

    PubMed

    Dupré de Baubigny, Julien; Benzaquen, Michael; Fabié, Laure; Delmas, Mathieu; Aimé, Jean-Pierre; Legros, Marc; Ondarçuhu, Thierry

    2015-09-15

    We investigate the shape and mechanical properties of liquid interfaces down to nanometer scale by atomic force microscopy (AFM) and scanning electron microscopy (SEM) combined with in situ micromanipulation techniques. In both cases, the interface is probed with a cylindrical nanofiber with radius R of the order of 25-100 nm. The effective spring constant of the nanomeniscus oscillated around its equilibrium position is determined by static and frequency-modulation (FM) AFM modes. In the case of an unbounded meniscus, we find that the effective spring constant k is proportional to the surface tension γ of the liquid through k = (0.51 ± 0.06)γ, regardless of the excitation frequency from quasi-static up to 450 kHz. A model based on the equilibrium shape of the meniscus reproduces well the experimental data. Electron microscopy allowed to visualize the meniscus profile around the fiber with a lateral resolution of the order of 10 nm and confirmed its catenary shape. The influence of a lateral confinement of the interface is also investigated. We showed that the lateral extension L of the meniscus influences the effective spring constant following a logarithmic evolution k ∼ 2πγ/ln(L/R) deduced from the model. This comprehensive study of liquid interface properties over more than 4 orders of magnitude in meniscus size shows that advanced FM-AFM and SEM techniques are promising tools for the investigation of mechanical properties of liquids down to nanometer scale.

  19. Pressurization of a Flightweight, Liquid Hydrogen Tank: Evaporation and Condensation at a Liquid Vapor Interface

    NASA Technical Reports Server (NTRS)

    Stewart, Mark E.

    2017-01-01

    Evaporation and condensation at a liquidvapor interface is important for long-term, in-space cryogenic propellant storage. Yet the current understanding of interfacial physics does not predict behavior or evaporation condensation rates. The proposed paper will present a physical model, based on the 1-D Heat equation and Schrages equation which demonstrates thin thermal layers at the fluidvapor interface.

  20. The Assembly of DNA Amphiphiles at Liquid Crystal-Aqueous Interface

    PubMed Central

    Zhou, Jingsheng; Dong, Yuanchen; Zhang, Yiyang; Liu, Dongsheng; Yang, Zhongqiang

    2016-01-01

    In this article, we synthesized a type of DNA amphiphiles (called DNA-lipids) and systematically studied its assembly behavior at the liquid crystal (LC)—aqueous interface. It turned out that the pure DNA-lipids at various concentrations cannot trigger the optical transition of liquid crystals from planar anchoring to homeotropic anchoring at the liquid crystal—aqueous interface. The co-assembly of DNA-lipid and l-dilauroyl phosphatidylcholine (l-DLPC) indicated that the DLPC assembled all over the LC-aqueous interface, and DNA-lipids prefer to couple with LC in certain areas, particularly in polarized and fluorescent image, forming micron sized net-like structures. The addition of DNA complementary to DNA-lipids forming double stranded DNA-lipids caused de-assembly of DNA-lipids from LC-aqueous interface, resulting in the disappearance of net-like structures, which can be visualized through polarized microscope. The optical changes combined with DNA unique designable property and specific interaction with wide range of target molecules, the DNA-lipids decorated LC-aqueous interface would provide a new platform for biological sensing and diagnosis.

  1. Capillary-driven interface oscillations of cryogenic liquids under non-isothermal boundary conditions

    NASA Astrophysics Data System (ADS)

    Kulev, Nikolai; Dreyer, Michael

    2012-11-01

    Experiments were conducted in the Drop Tower in Bremen for 4.7 s under conditions, similar to the end of thrust in a rocket tank when the cold propellant flows along the warmer tank wall driven by capillary forces. The interface oscillations of liquid argon and liquid methane were investigated in a partly filled cylinder. The oscillations take place during the interface reorientation from its normal gravity (1g) position towards a new position upon step transition to microgravity (10-6g). Axial wall temperature gradients of 0.15 K/mm - 1.93 K/mm were applied above the 1g interface position. The contact line motion changed from aperiodic to oscillatory and the dynamic contact angle increased with the increasing value of the wall temperature gradient. The frequency of the interface center point oscillation increased too. The vapor pressure evolution followed the contact line motion, presumably due to relation of the evaporation to the contact line motion. The vapor temperature above the interface decreased (up to 3.5 K), apparently because of the enhanced evaporation by the contact line motion. The wall temperature in the region of the contact line motion decreased too (up to 8.5 K), hinting to an increased heat transfer by the evaporation between liquid and wall. The funding by the German Federal Ministry of Education and Research (BMBF) through the German Aerospace Center (DLR) under grant number 50 RL 0921 is gratefully acknowledged.

  2. The Assembly of DNA Amphiphiles at Liquid Crystal-Aqueous Interface.

    PubMed

    Zhou, Jingsheng; Dong, Yuanchen; Zhang, Yiyang; Liu, Dongsheng; Yang, Zhongqiang

    2016-12-01

    In this article, we synthesized a type of DNA amphiphiles (called DNA-lipids) and systematically studied its assembly behavior at the liquid crystal (LC)-aqueous interface. It turned out that the pure DNA-lipids at various concentrations cannot trigger the optical transition of liquid crystals from planar anchoring to homeotropic anchoring at the liquid crystal-aqueous interface. The co-assembly of DNA-lipid and l-dilauroyl phosphatidylcholine (l-DLPC) indicated that the DLPC assembled all over the LC-aqueous interface, and DNA-lipids prefer to couple with LC in certain areas, particularly in polarized and fluorescent image, forming micron sized net-like structures. The addition of DNA complementary to DNA-lipids forming double stranded DNA-lipids caused de-assembly of DNA-lipids from LC-aqueous interface, resulting in the disappearance of net-like structures, which can be visualized through polarized microscope. The optical changes combined with DNA unique designable property and specific interaction with wide range of target molecules, the DNA-lipids decorated LC-aqueous interface would provide a new platform for biological sensing and diagnosis.

  3. Formative evaluation of a mobile liquid portion size estimation interface for people with varying literacy skills

    PubMed Central

    Connelly, Kay; Siek, Katie A.; Welch, Janet L.

    2012-01-01

    Chronically ill people, especially those with low literacy skills, often have difficulty estimating portion sizes of liquids to help them stay within their recommended fluid limits. There is a plethora of mobile applications that can help people monitor their nutritional intake but unfortunately these applications require the user to have high literacy and numeracy skills for portion size recording. In this paper, we present two studies in which the low- and the high-fidelity versions of a portion size estimation interface, designed using the cognitive strategies adults employ for portion size estimation during diet recall studies, was evaluated by a chronically ill population with varying literacy skills. The low fidelity interface was evaluated by ten patients who were all able to accurately estimate portion sizes of various liquids with the interface. Eighteen participants did an in situ evaluation of the high-fidelity version incorporated in a diet and fluid monitoring mobile application for 6 weeks. Although the accuracy of the estimation cannot be confirmed in the second study but the participants who actively interacted with the interface showed better health outcomes by the end of the study. Based on these findings, we provide recommendations for designing the next iteration of an accurate and low literacy-accessible liquid portion size estimation mobile interface. PMID:24443659

  4. Elasto-capillary torsion at a liquid interface

    NASA Astrophysics Data System (ADS)

    Oratis, Alexandros; Farmer, Timothy; Bird, James

    2016-11-01

    When a liquid drop wets a solid, the droplet typically spreads over the solid. By contrast, for sufficiently compliant solids, the solid can instead spread around the drop. This wrapping phenomenon has been exploited to assemble 3-dimensional structures from 2-dimensional sheets, a process often referred to as capillary origami. Although existing studies of this self-assembly have demonstrated bending and folding, methods of inducing spontaneous twisting by means of capillarity are less clear. Here we demonstrate that spontaneous twist can be initiated in a compliant solid through a combination of surface chemistry and capillarity. Experimentally, we measure the angle of twist on a surface with binary patterns of surface wettability as we vary the solid's geometric and material properties. We develop a scaling law to relate this angle of twist to the elastic and interfacial properties, which compares well with our experimental results.

  5. Angstrom-Resolved Metal-Organic Framework-Liquid Interfaces.

    PubMed

    Chiodini, Stefano; Reinares-Fisac, Daniel; Espinosa, Francisco M; Gutiérrez-Puebla, Enrique; Monge, Angeles; Gándara, Felipe; Garcia, Ricardo

    2017-09-11

    Metal-organic frameworks (MOFs) are a class of crystalline materials with a variety of applications in gas storage, catalysis, drug delivery or light harvesting. The optimization of those applications requires the characterization of MOF structure in the relevant environment. Dynamic force microscopy has been applied to follow dynamic processes of metal-organic-framework material. We provide images with spatial and time resolutions, respectively, of angstrom and seconds that show that Ce-RPF-8 surfaces immersed in water and glycerol experience a surface reconstruction process that is characterized by the diffusion of the molecular species along the step edges of the open terraces. The rate of the surface reconstruction process depends on the liquid. In water it happens spontaneously while in glycerol is triggered by applying an external force.

  6. Using Si Diodes To Detect H2 Liquid/Vapor Interfaces

    NASA Technical Reports Server (NTRS)

    Dempsey, Paula Jean; Fabik, Richard

    1994-01-01

    Commercially available silicon-diode temperature sensors used to detect interfaces between hydrogen liquid and hydrogen vapor at steady-state saturation conditions. Sensors mounted at short intervals along rod to form rake-like array. Array inserted in tank with rod oriented vertically, where it senses level of liquid hydrogen to resolution equal to interval between sensors. Basic idea to measure voltage across sensor while supplying small electric current that heats sensor. Because vapor cools sensor less effectively than liquid does, sensor's steady-state temperature greater when sensor surrounded by vapor than when immersed in liquid. Voltage output decreases as temperature increases for silicon diodes. Thus, temperature (voltage) reading used to determine whether liquid level above or below sensor.

  7. Observation of total external reflection of x rays from a liquid-solid interface

    NASA Astrophysics Data System (ADS)

    Touryanski, A. G.; Pirshin, I. V.

    2007-07-01

    A new experimental scheme for the measurement of the x-ray reflectivity R from a liquid-solid interface in the range of angles of total external reflection is proposed. An x-ray beam is transmitted through a plane channel filled with a liquid under investigation. The channel is formed by two optically polished plates, one of which being the substrate under study. To eliminate the edge effects caused by surface tension, polymer films with a lyophilic coating are used as windows of the channel. For wate-silicon and glycerol-silicon interfaces, the angular dependences of R and the parameters of the interfaces are measured with the scheme developed using the CuK α (8.05 keV) and CuK β (8.91 keV) lines.

  8. Dynamic equilibrium under vibrations of H₂ liquid-vapor interface at various gravity levels.

    PubMed

    Gandikota, G; Chatain, D; Lyubimova, T; Beysens, D

    2014-06-01

    Horizontal vibration applied to the support of a simple pendulum can deviate from the equilibrium position of the pendulum to a nonvertical position. A similar phenomenon is expected when a liquid-vapor interface is subjected to strong horizontal vibration. Beyond a threshold value of vibrational velocity the interface should attain an equilibrium position at an angle to the initial horizontal position. In the present paper experimental investigation of this phenomenon is carried out in a magnetic levitation device to study the effect of the vibration parameters, gravity acceleration, and the liquid-vapor density on the interface position. The results compare well with the theoretical expression derived by Wolf [G. H. Wolf, Z. Phys. B 227, 291 (1969)].

  9. A theory for time-dependent solvation structure near solid-liquid interface.

    PubMed

    Iida, Kenji; Sato, Hirofumi

    2012-06-28

    We propose a theory to describe time-dependent solvation structure near solid-liquid interface. Recently, we have developed two-dimensional-reference interaction site model to describe solvation structure near solid-liquid interface at the equilibrium state. In the present study, the theory is extended to treat dynamical aspect of the solvation; site-site Smoluchowski-Vlasov equation and surrogate Hamiltonian description are utilized to deal with the time-dependency. This combination enables us to access a long-time behavior of solvation dynamics. We apply the theory to a model system consisting of an atomistic wall and water solvent, and discuss the hydration structure dynamics near the interface at the molecular-level.

  10. Gradual improvements of charge carrier mobility at ionic liquid/rubrene single crystal interfaces

    NASA Astrophysics Data System (ADS)

    Yokota, Yasuyuki; Hara, Hisaya; Morino, Yusuke; Bando, Ken-ichi; Ono, Sakurako; Imanishi, Akihito; Okada, Yugo; Matsui, Hiroyuki; Uemura, Takafumi; Takeya, Jun; Fukui, Ken-ichi

    2016-02-01

    We report evolution of electric characteristics of an electric double layer field-effect transistor based on the ionic liquid/rubrene single crystal interfaces. In contrast to usual devices, the field effect mobility was found to gradually increase with time for a day, followed by minor long-term fluctuations. Although the details of the evolution were somewhat device dependent, the final values of the mobility turned out to be 3-4 times larger irrespective of the initial values. These observations are explained by the evolution of the flat interface by defect-induced spontaneous dissolution of rubrene molecules at the ionic liquid/rubrene single crystal interfaces, revealed by frequency modulation atomic force microscopy.

  11. Reversible Photoresponsive Molecular Alignment of Liquid Crystals at Fluid Interfaces with Persistent Stability.

    PubMed

    Tian, Tongtong; Hu, Qiongzheng; Wang, Yi; Gao, Yanan; Yu, Li

    2016-04-25

    This work demonstrates a noninvasive approach to control alignment of liquid crystals persistently and reversibly at fluid interfaces by using a photoresponsive azobenzene-based surfactant dissolved in an ionic liquid (IL), ethylammonium nitrate (EAN). As the first report on the orientational behavior of LCs at the IL/LC interface, our study also expands current understanding of alignment control of LCs at the aqueous/LC interface by adding electrolytes into aqueous solutions. The threshold concentration for switching the optical responses of LCs can be changed just by simply manipulating the ratio of EAN to H2 O. This work will inspire fundamental studies and novel applications of using the LC-based imaging technique to investigate various chemical and biological events in ILs.

  12. First-principles quantum-mechanical investigations of biomass conversion at the liquid-solid interfaces

    NASA Astrophysics Data System (ADS)

    Dang, Hongli; Xue, Wenhua; Liu, Yingdi; Jentoft, Friederike; Resasco, Daniel; Wang, Sanwu

    2014-03-01

    We report first-principles density-functional calculations and ab initio molecular dynamics (MD) simulations for the reactions involving furfural, which is an important intermediate in biomass conversion, at the catalytic liquid-solid interfaces. The different dynamic processes of furfural at the water-Cu(111) and water-Pd(111) interfaces suggest different catalytic reaction mechanisms for the conversion of furfural. Simulations for the dynamic processes with and without hydrogen demonstrate the importance of the liquid-solid interface as well as the presence of hydrogen in possible catalytic reactions including hydrogenation and decarbonylation of furfural. Supported by DOE (DE-SC0004600). This research used the supercomputer resources of the XSEDE, the NERSC Center, and the Tandy Supercomputing Center.

  13. Lanthanide cation extraction by malonamide ligands: from liquid-liquid interfaces to microemulsions. A molecular dynamics study?

    PubMed

    Diss, Romain; Wipff, Georges

    2005-01-21

    According to molecular dynamics simulations, uncomplexed malonamide ligands L and their neutral Eu(NO3)3L2 or charged EuL4(3+) complexes are surface active and adsorb at a water-"oil" interface, where "oil" is modeled by chloroform. Aqueous solvation at the interface is found to induce a trans to gauche rearrangement of the carbonyl groups, i.e., to preorganize the chelating L ligands for complexation. The interface also induces a larger proportion of extended amphiphilic forms, of EE-gauche type. The effect of increased oil/water ratio is also investigated. It shown that the system evolves from a well-defined interface between immiscible phases to water-in-oil cylindrical micelles and micro-droplets, onto which L ligands and the lanthanide complexes adsorb, while other ligands are extracted in organic phase. Two electrostatic models of the complexes are compared and, in no case is the neutral or charged complex fully extracted to the organic phase. These features allow us to better understand synergistic and solvation effects in the assisted liquid-liquid extraction of lanthanide or actinide cations.

  14. Thermal-hydraulic behaviors of vapor-liquid interface due to arrival of a pressure wave

    SciTech Connect

    Inoue, Akira; Fujii, Yoshifumi; Matsuzaki, Mitsuo

    1995-09-01

    In the vapor explosion, a pressure wave (shock wave) plays a fundamental role for triggering, propagation and enhancement of the explosion. Energy of the explosion is related to the magnitude of heat transfer rate from hot liquid to cold volatile one. This is related to an increasing rate of interface area and to an amount of transient heat flux between the liquids. In this study, the characteristics of transient heat transfer and behaviors of vapor film both on the platinum tube and on the hot melt tin drop, under same boundary conditions have been investigated. It is considered that there exists a fundamental mechanism of the explosion in the initial expansion process of the hot liquid drop immediately after arrival of pressure wave. The growth rate of the vapor film is much faster on the hot liquid than that on the solid surface. Two kinds of roughness were observed, one due to the Taylor instability, by rapid growth of the explosion bubble, and another, nucleation sites were observed at the vapor-liquid interface. Based on detailed observation of early stage interface behaviors after arrival of a pressure wave, the thermal fragmentation mechanism is proposed.

  15. Study of surface charge density on solid/liquid interfaces by modulating the electrical double layer

    NASA Astrophysics Data System (ADS)

    Pak, Hyuk Kyu; Moon, Jong Kyun

    2014-11-01

    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 difference between the plates 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 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. This work was supported by Center for Soft and Living Matter through IBS program in Korea.

  16. Novel surface adsorption behavior of liquid at the air-liquid interface

    NASA Astrophysics Data System (ADS)

    Chen, Feiwu; Ren, Qing

    2017-10-01

    Surface tension is one of the most important properties of liquid. A new theory is proposed and applied to the phenomena related to the surface tension of pure liquid compounds and strong electrolyte solutions. We first found that the phase transitions of pure liquid compounds from bulk to surface are exothermic and transition heats of 38 liquid compounds are determined quantitatively. This theory also describes successfully the variations of the surface tensions with the concentrations of solutes in strong electrolyte solutions. As a byproduct, minimum thicknesses of the surface layers of these solutions are deduced.

  17. Numerical studies of the effects of jet-induced mixing on liquid-vapor interface condensation

    NASA Technical Reports Server (NTRS)

    Lin, Chin-Shun

    1989-01-01

    Numerical solutions of jet-induced mixing in a partially full cryogenic tank are presented. An axisymmetric laminar jet is discharged from the central part of the tank bottom toward the liquid-vapor interface. Liquid is withdrawn at the same volume flow rate from the outer part of the tank. The jet is at a temperature lower than the interface, which is maintained at a certain saturation temperature. The interface is assumed to be flat and shear-free and the condensation-induced velocity is assumed to be negligibly small compared with radial interface velocity. Finite-difference method is used to solve the nondimensional form of steady state continuity, momentum, and energy equations. Calculations are conducted for jet Reynolds numbers ranging from 150 to 600 and Prandtl numbers ranging from 0.85 to 2.65. The effects of above stated parameters on the condensation Nusselt and Stanton numbers which characterize the steady-state interface condensation process are investigated. Detailed analysis to gain a better understanding of the fundamentals of fluid mixing and interface condensation is performed.

  18. Effect of the Thermocouple on Measuring the Temperature Discontinuity at a Liquid-Vapor Interface.

    PubMed

    Kazemi, Mohammad Amin; Nobes, David S; Elliott, Janet A W

    2017-07-18

    The coupled heat and mass transfer that occurs in evaporation is of interest in a large number of fields such as evaporative cooling, distillation, drying, coating, printing, crystallization, welding, atmospheric processes, and pool fires. The temperature jump that occurs at an evaporating interface is of central importance to understanding this complex process. Over the past three decades, thermocouples have been widely used to measure the interfacial temperature jumps at a liquid-vapor interface during evaporation. However, the reliability of these measurements has not been investigated so far. In this study, a numerical simulation of a thermocouple when it measures the interfacial temperatures at a liquid-vapor interface is conducted to understand the possible effects of the thermocouple on the measured temperature and features in the temperature profile. The differential equations of heat transfer in the solid and fluids as well as the momentum transfer in the fluids are coupled together and solved numerically subject to appropriate boundary conditions between the solid and fluids. The results of the numerical simulation showed that while thermocouples can measure the interfacial temperatures in the liquid correctly, they fail to read the actual interfacial temperatures in the vapor. As the results of our numerical study suggest, the temperature jumps at a liquid-vapor interface measured experimentally by using a thermocouple are larger than what really exists at the interface. For a typical experimental study of evaporation of water at low pressure, it was found that the temperature jumps measured by a thermocouple are overestimated by almost 50%. However, the revised temperature jumps are still in agreement with the statistical rate theory of interfacial transport. As well as addressing the specific application of the liquid-vapor temperature jump, this paper provides significant insight into the role that heat transfer plays in the operation of thermocouples

  19. Effect of asymmetric gravity jitter excited slosh waves at liquid-vapor interface under microgravity

    NASA Technical Reports Server (NTRS)

    Hung, R. J.; Pan, H. L.; Lee, C. C.; Leslie, F. W.

    1992-01-01

    The dynamical behavior of fluids affected by the asymmetric gravity jitter oscillations, in particular the effect of surface tension on partially-filled rotating fluids (cryogenic liquid helium and helium vapor) in a sub-scale Gravity Probe-B Spacecraft propellant dewar tank imposed by time-dependent various directions of background gravity environment have been investigated. Results show that lower frequency gravity jitter imposed on the time-dependent variations of the direction of background gravity induced a greater amplitude of oscillations and a stronger degree of asymmetry in liquid-vapor interface geometry than that made by the higher frequency gravity jitter. Furthermore, the greater the components of background gravity in radial and circumferential directions will provide a greater contribution in driving more to the increasing amplitude and degrees of symmetry of liquid-vapor interface profiles which, in turn, modify the disturbance of moment of inertia and angular momentum of spacecraft.

  20. Modeling of ultrasound transmission through a solid-liquid interface comprising a network of gas pockets

    SciTech Connect

    Paumel, K.; Baque, F.; Moysan, J.; Corneloup, G.; Chatain, D.

    2011-08-15

    Ultrasonic inspection of sodium-cooled fast reactor requires a good acoustic coupling between the transducer and the liquid sodium. Ultrasonic transmission through a solid surface in contact with liquid sodium can be complex due to the presence of microscopic gas pockets entrapped by the surface roughness. Experiments are run using substrates with controlled roughness consisting of a network of holes and a modeling approach is then developed. In this model, a gas pocket stiffness at a partially solid-liquid interface is defined. This stiffness is then used to calculate the transmission coefficient of ultrasound at the entire interface. The gas pocket stiffness has a static, as well as an inertial component, which depends on the ultrasonic frequency and the radiative mass.

  1. Modeling of ultrasound transmission through a solid-liquid interface comprising a network of gas pockets

    NASA Astrophysics Data System (ADS)

    Paumel, K.; Moysan, J.; Chatain, D.; Corneloup, G.; Baqué, F.

    2011-08-01

    Ultrasonic inspection of sodium-cooled fast reactor requires a good acoustic coupling between the transducer and the liquid sodium. Ultrasonic transmission through a solid surface in contact with liquid sodium can be complex due to the presence of microscopic gas pockets entrapped by the surface roughness. Experiments are run using substrates with controlled roughness consisting of a network of holes and a modeling approach is then developed. In this model, a gas pocket stiffness at a partially solid-liquid interface is defined. This stiffness is then used to calculate the transmission coefficient of ultrasound at the entire interface. The gas pocket stiffness has a static, as well as an inertial component, which depends on the ultrasonic frequency and the radiative mass.

  2. Density functional theory for crystal-liquid interfaces of Lennard-Jones fluid.

    PubMed

    Wang, Xin; Mi, Jianguo; Zhong, Chongli

    2013-04-28

    A density functional approach is presented to describe the crystal-liquid interfaces and crystal nucleations of Lennard-Jones fluid. Within the theoretical framework, the modified fundamental measure theory is applied to describe the free energy functional of hard sphere repulsion, and the weighted density method based on first order mean spherical approximation is used to describe the free energy contribution arising from the attractive interaction. The liquid-solid equilibria, density profiles within crystal cells and at liquid-solid interfaces, interfacial tensions, nucleation free energy barriers, and critical cluster sizes are calculated for face-centered-cubic and body-centered-cubic nucleus. Some results are in good agreement with available simulation data, indicating that the present model is quantitatively reliable in describing nucleation thermodynamics of Lennard-Jones fluid.

  3. Delivery of minimally dispersed liquid interfaces for sequential surface chemistry.

    PubMed

    Ostromohov, N; Bercovici, M; Kaigala, G V

    2016-08-02

    We present a method for sequential delivery of reagents to a reaction site with minimal dispersion of their interfaces. Using segmented flow to encapsulate the reagents as droplets, the dispersion between reagent plugs remains confined in a limited volume, while being transmitted to the reaction surface. In close proximity to the target surface, we use a passive array of microstructures for removal of the oil phase such that the original reagent sequence is reconstructed, and only the aqueous phase reaches the reaction surface. We provide a detailed analysis of the conditions under which the method can be applied and demonstrate maintaining a transition time of 560 ms between reagents transported to a reaction site over a distance of 60 cm. We implemented the method using a vertical microfluidic probe on an open surface, allowing contact-free interaction with biological samples, and demonstrated two examples of assays implemented using the method: measurements of receptor-ligand reaction kinetics and of the fluorescence response of immobilized GFP to local variations in pH. We believe that the method can be useful for studying the dynamic response of cells and proteins to various stimuli, as well as for highly automated multi-step assays.

  4. Competitive adsorption of plasma proteins at solid-liquid interfaces.

    PubMed

    Lensen, H G; Breemhaar, W; Smolders, C A; Feijen, J

    1986-04-11

    The competitive adsorption of human serum albumin (HSA), human immuno-gamma-globulin (HIgG) and human fibrinogen (HFb) onto polystyrene (PS) at 20 degrees C and a pH of 7.35 (phosphate-buffered saline) was studied. Protein adsorption was studied using enzyme immunoassay. The results obtained with the immunoassay were compared with those obtained using radiolabelled proteins. Recent studies revealed that the adsorption behaviour of radiolabelled proteins onto surfaces differs from that of the non-labelled proteins, which may lead to misinterpretation of adsorption data. Differences in the adsorption behaviour of the labelled proteins as compared to non-labelled proteins can possibly be explained by the formation of modified proteins during the labelling procedure as shown by ion-exchange high-performance liquid chromatography (HPLC). The competitive adsorption of HSA, HIgG and HFb onto a PS latex was studied by measuring the depletion of proteins in solution. The decrease in protein concentration in solution was determined by HPLC techniques. A strong preferential adsorption of HFb was observed with maximum adsorption values of 0.6 micrograms/cm2.

  5. Electrochemical Investigation of Adsorption of Single‐Wall Carbon Nanotubes at a Liquid/Liquid Interface

    PubMed Central

    Rabiu, Aminu K.; Toth, Peter S.; Rodgers, Andrew N. J.

    2016-01-01

    Abstract There is much interest in understanding the interfacial properties of carbon nanotubes, particularly at water/oil interfaces. Here, the adsorption of single‐wall carbon nanotubes (SWCNTs) at the water/1,2‐dichloroethane (DCE) interface, and the subsequent investigation of the influence of the adsorbed nanotube layer on interfacial ion transfer, is studied by using the voltammetric transfer of tetramethylammonium (TMA+) and hexafluorophosphate (PF6 −) as probe ions. The presence of the interfacial SWCNT layer significantly suppresses the transfer of both ions across the interface, with a greater degree of selectivity towards the PF6 − ion. This effect was attributed both to the partial blocking of the interface by the SWCNTs and to the potential dependant adsorption of background electrolyte ions on the surface of the SWCNTs, as confirmed by X‐ray photoelectron spectroscopy, which is caused by an electrostatic interaction between the interfacial SWCNTs and the transferring ion. PMID:28168151

  6. Electrochemical Investigation of Adsorption of Single-Wall Carbon Nanotubes at a Liquid/Liquid Interface.

    PubMed

    Rabiu, Aminu K; Toth, Peter S; Rodgers, Andrew N J; Dryfe, Robert A W

    2017-02-01

    There is much interest in understanding the interfacial properties of carbon nanotubes, particularly at water/oil interfaces. Here, the adsorption of single-wall carbon nanotubes (SWCNTs) at the water/1,2-dichloroethane (DCE) interface, and the subsequent investigation of the influence of the adsorbed nanotube layer on interfacial ion transfer, is studied by using the voltammetric transfer of tetramethylammonium (TMA(+)) and hexafluorophosphate (PF6(-)) as probe ions. The presence of the interfacial SWCNT layer significantly suppresses the transfer of both ions across the interface, with a greater degree of selectivity towards the PF6(-) ion. This effect was attributed both to the partial blocking of the interface by the SWCNTs and to the potential dependant adsorption of background electrolyte ions on the surface of the SWCNTs, as confirmed by X-ray photoelectron spectroscopy, which is caused by an electrostatic interaction between the interfacial SWCNTs and the transferring ion.

  7. Water distribution at solid/liquid interfaces visualized by frequency modulation atomic force microscopy

    PubMed Central

    Fukuma, Takeshi

    2010-01-01

    Interfacial phenomena at solid/water interfaces play an important role in a wide range of industrial technologies and biological processes. However, it has been a great challenge to directly probe the molecular-scale behavior of water at solid/water interfaces. Recently, there have been tremendous advancements in frequency modulation atomic force microscopy (FM-AFM), enabling its operation in liquids with atomic resolution. The high spatial and force resolutions of FM-AFM have enabled the visualization of one-dimensional (1D) profiles of the hydration force, two-dimensional (2D) images of hydration layers and three-dimensional (3D) images of the water distribution at solid/water interfaces. Here I present an overview of the recent advances in FM-AFM instrumentation and its applications to the study of solid/water interfaces. PMID:27877337

  8. Fast Interconversion of Hydrogen Bonding at the Hematite (001)–Liquid Water Interface

    SciTech Connect

    von Rudorff, Guido Falk; Jakobsen, Rasmus; Rosso, Kevin M.; Blumberger, Jochen

    2016-04-07

    The interface between transition-metal oxides and aqueous solutions plays an important role in biogeochemistry and photoelectrochemistry, but the atomistic structure is often elusive. Here we report on the surface geometry, solvation structure, and thermal fluctuations of the hydrogen bonding network at the hematite (001)–water interface as obtained from hybrid density functional theory-based molecular dynamics. We find that the protons terminating the surface form binary patterns by either pointing in-plane or out-of-plane. The patterns exist for about 1 ps and spontaneously interconvert in an ultrafast, solvent-driven process within 50 fs. This results in only about half of the terminating protons pointing toward the solvent and being acidic. The lifetimes of all hydrogen bonds formed at the interface are shorter than those in pure liquid water. The solvation structure reported herein forms the basis for a better fundamental understanding of electron transfer coupled to proton transfer reactions at this important interface.

  9. Atomic-Scale Structure of a Liquid Metal-Insulator Interface

    SciTech Connect

    Ocko, B.M.; Tamam, L.; Pontoni, D.; Hofmann, T.; Reichert, H.; Deutsch, M.

    2010-04-01

    The structure of the liquid Hg/sapphire interface was measured with angstrom-scale resolution by high-energy X-ray reflectivity. The atomic Hg layering found at the interface is less pronounced than at the Hg/vapor interface, showing a twice-shorter decay length with depth, and a weaker peak/valley density contrast. We also find a near-interface, 8 {+-} 3 {angstrom} thick layer, the density of which, although depth-varying, is enhanced, on average, by 10 {+-} 5% relative to the bulk. The enhancement is assigned to a 0.13 {+-} 0.05 e/atom charge transfer from the Hg to the substrate, somewhat less than theory. The unexplained anomalous temperature dependence previously reported for the mercury/vapor density profile is absent here, implying a nonstructural origin for the anomaly.

  10. Simulation and theory of ions at atmospherically relevant aqueous liquid-air interfaces.

    PubMed

    Tobias, Douglas J; Stern, Abraham C; Baer, Marcel D; Levin, Yan; Mundy, Christopher J

    2013-01-01

    Chemistry occurring at or near the surface of aqueous droplets and thin films in the atmosphere influences air quality and climate. Molecular dynamics simulations are becoming increasingly useful for gaining atomic-scale insight into the structure and reactivity of aqueous interfaces in the atmosphere. Here we review simulation studies of atmospherically relevant aqueous liquid-air interfaces, with an emphasis on ions that play important roles in the chemistry of atmospheric aerosols. In addition to surveying results from simulation studies, we discuss challenges to the refinement and experimental validation of the methodology for simulating ion adsorption to the air-water interface and recent advances in elucidating the driving forces for adsorption. We also review the recent development of a dielectric continuum theory capable of reproducing simulation and experimental data on ion behavior at aqueous interfaces.

  11. Theoretical study of ion solvation at the water liquid-vapor interface

    NASA Astrophysics Data System (ADS)

    Benjamin, Ilan

    1991-09-01

    Molecular dynamics calculations are reported for several ions at the liquid-vapor interface of water. The transition from the bulk to the interface region is investigated from structural, energetic, and dynamical points of view by calculating ion-water geometries, radial distribution functions, solvent molecular reorientation times, solvent polarization fluctuations, and solvation free energy as a function of distance from the interface. It is shown that ions tend to keep most of the structural and dynamical properties of their first solvation shell intact as they are moved into the interface, and that the tendency for negative adsorption (positive free energy of adsorption) is associated with weaker and fewer long range interactions. A comparison of some of the molecular dynamics results to predictions of simple continuum models is discussed, showing generally poor quantitative agreement.

  12. Thermodynamic Investigation of the Effect of Interface Curvature on the Solid-Liquid Equilibrium and Eutectic Point of Binary Mixtures.

    PubMed

    Liu, Fanghui; Zargarzadeh, Leila; Chung, Hyun-Joong; Elliott, Janet A W

    2017-09-29

    Thermodynamic phase behavior is affected by curved interfaces in micro- and nanoscale systems. For example, capillary freezing point depression is associated with the pressure difference between the solid and liquid phases caused by interface curvature. In this study, the thermal, mechanical, and chemical equilibrium conditions are derived for binary solid-liquid equilibrium with a curved solid-liquid interface due to confinement in a capillary. This derivation shows the equivalence of the most general forms of the Gibbs-Thomson and Ostwald-Freundlich equations. As an example, the effect of curvature on solid-liquid equilibrium is explained quantitatively for the water/glycerol system. Considering the effect of a curved solid-liquid interface, a complete solid-liquid phase diagram is developed over a range of concentrations for the water/glycerol system (including the freezing of pure water or precipitation of pure glycerol depending on the concentration of the solution). This phase diagram is compared with the traditional phase diagram in which the assumption of a flat solid-liquid interface is made. We show the extent to which nanoscale interface curvature can affect the composition-dependent freezing and precipitating processes, as well as the change in the eutectic point temperature and concentration with interface curvature. Understanding the effect of curvature on solid-liquid equilibrium in nanoscale capillaries has applications in the food industry, soil science, cryobiology, nanoporous materials, and various nanoscience fields.

  13. Fabrication of composite polymer foam films at the liquid/liquid interface through emulsion-directed assembly and adsorption processes.

    PubMed

    Geng, Yuanyuan; Liu, Mei; Tong, Kun; Xu, Jian; Lee, Yong-Ill; Hao, Jingcheng; Liu, Hong-Guo

    2014-03-04

    The foam films of polystyrene-b-poly(acrylic acid)-b-polystyrene (PS-b-PAA-b-PS) doped with Cd(II) or Pb(II) species were fabricated at the planar liquid/liquid interfaces between a DMF/chloroform (v/v: 1/1) solution of the polymer and aqueous solutions containing cadmium acetate or lead acetate at ambient temperature. Optical microscopic observation shows the thin film is uniform on a larger length scale. Transmission electron microscopic (TEM) investigations reveal that the foam films are made up of microcapsules with the size of several hundreds of nanometers to micrometers. The walls of the microcapsules have a layered structure decorating with nanofibers and hollow nanospheres, where numerous inorganic fine nanoparticles are dispersed homogeneously. The film formation is a result of emulsion droplet-templated assembly and adsorption of the formed microcapsules at the planar liquid/liquid interface. Because of the miscibility of DMF with chloroform and water, DMF migrates to the aqueous phase while water migrates to the organic phase across the interface, resulting in the formation of a W/O emulsion, as revealed by optical microscopic observation, freeze fracture transmission electron microscopic (FF-TEM) observation, and dynamic laser scattering (DLS) investigation. The triblock copolymer molecules and the inorganic species adsorb and self-assemble around the emulsion drops, leading to the formation of the composite microcapsules. X-ray photoelectron spectroscopic (XPS) and FTIR spectroscopic results indicate that two kinds of Cd(II) or Pb(II) species, metal oxide or hydroxide, resulting from the hydrolysis of the metal ions and the coordinated metal ions to the carboxyl groups coexist in the formed thin films, which transform to metal sulfide completely after treating with hydrogen sulfide to get metal sulfide nanoparticle-doped polymer thin films.

  14. Sample cells for probing solid/liquid interfaces with broadband sum-frequency-generation spectroscopy

    NASA Astrophysics Data System (ADS)

    Verreault, Dominique; Kurz, Volker; Howell, Caitlin; Koelsch, Patrick

    2010-06-01

    Two sample cells designed specifically for sum-frequency-generation (SFG) measurements at the solid/liquid interface were developed: one thin-layer analysis cell allowing measurement of films on reflective metallic surfaces through a micrometer layer of solution and one spectroelectrochemical cell allowing investigation of processes at the indium tin oxide/solution interface. Both sample cells are described in detail and data illustrating the capabilities of each are shown. To further improve measurements at solid/liquid interfaces, the broadband SFG system was modified to include a reference beam which can be measured simultaneously with the sample signal, permitting background correction of SFG spectra in real time. Sensitivity tests of this system yielded a signal-to-noise ratio of 100 at a surface coverage of 0.2 molecules/nm2. Details on data analysis routines, pulse shaping methods of the visible beam, as well as the design of a purging chamber and sample stage setup are presented. These descriptions will be useful to those planning to set up a SFG spectrometer or seeking to optimize their own SFG systems for measurements of solid/liquid interfaces.

  15. Capillary waves at the liquid-vapor interface and the surface tension of water.

    PubMed

    Ismail, Ahmed E; Grest, Gary S; Stevens, Mark J

    2006-07-07

    Capillary waves occurring at the liquid-vapor interface of water are studied using molecular dynamics simulations. In addition, the surface tension, determined thermodynamically from the difference in the normal and tangential pressure at the liquid-vapor interface, is compared for a number of standard three- and four-point water models. We study four three-point models (SPC/E, TIP3P, TIP3P-CHARMM, and TIP3P-Ew) and two four-point models (TIP4P and TIP4P-Ew). All of the models examined underestimate the surface tension; the TIP4P-Ew model comes closest to reproducing the experimental data. The surface tension can also be determined from the amplitude of capillary waves at the liquid-vapor interface by varying the surface area of the interface. The surface tensions determined from the amplitude of the logarithmic divergence of the capillary interfacial width and from the traditional thermodynamic method agree only if the density profile is fitted to an error function instead of a hyperbolic tangent function.

  16. Determination of the Solid-Liquid Interface Energy in the Al-Cu-Ag System

    NASA Astrophysics Data System (ADS)

    Bulla, A.; Carreno-Bodensiek, C.; Pustal, B.; Berger, R.; Bührig-Polaczek, A.; Ludwig, A.

    2007-09-01

    The solid-liquid interface energy, σ SL , is of major importance during phase transformation. It has a strong influence on solidification morphologies and the final grain structure. The “grain boundary groove in an applied temperature gradient” method developed by Gündüz et al.[6] was found to be suitable for measuring the solid-liquid interface energy in ternary alloy systems (e.g., Al-Cu-Ag). In order to measure the solid-liquid interface energy, a radial heat flow apparatus was constructed and assembled. This apparatus ensures a stable temperature gradient for hours and leads to grain boundary grooves in chemical equilibrium. After rapid quenching, the samples were metallographically prepared and the local curvature of the grooves was analyzed. To determine the interface energy, the Gibbs Thomson equation was used, which requires the local curvature of the grain boundary grooves and the adherent local undercooling obtained from heat flux simulations on the scale of the grooves.

  17. Dynamic microscopy of nanoscale cluster growth at the solid-liquid interface.

    PubMed

    Williamson, M J; Tromp, R M; Vereecken, P M; Hull, R; Ross, F M

    2003-08-01

    Dynamic processes at the solid-liquid interface are of key importance across broad areas of science and technology. Electrochemical deposition of copper, for example, is used for metallization in integrated circuits, and a detailed understanding of nucleation, growth and coalescence is essential in optimizing the final microstructure. Our understanding of processes at the solid-vapour interface has advanced tremendously over the past decade due to the routine availability of real-time, high-resolution imaging techniques yielding data that can be compared quantitatively with theory. However, the difficulty of studying the solid-liquid interface leaves our understanding of processes there less complete. Here we analyse dynamic observations--recorded in situ using a novel transmission electron microscopy technique--of the nucleation and growth of nanoscale copper clusters during electrodeposition. We follow in real time the evolution of individual clusters, and compare their development with simulations incorporating the basic physics of electrodeposition during the early stages of growth. The experimental technique developed here is applicable to a broad range of dynamic phenomena at the solid-liquid interface.

  18. Interaction between a disclination and a uniaxial-isotropic phase interface in a nematic liquid crystal.

    PubMed

    Shklyaev, Oleg E; Fried, Eliot

    2008-01-01

    We consider the interaction between a disclination line of strength +/-1/2 and an interface between the uniaxial and isotropic phases of a nematic liquid crystal. We apply a recently developed set of interface conditions including a configurational force balance which generalizes the Gibbs-Thomson equation to account for the curvature elasticity of the uniaxial phase and the orientation dependence of the interfacial free-energy density. We consider a rectangular vessel containing both phases and a disclination. We formulate a relevant free-boundary problem and use numerical methods to determine equilibrium shapes of the interface. When the interfacial free-energy is constant, the shape of the interface is insensitive to whether the strength of the defect is +1/2 or -1/2 and to rotations of the director field consistent with the boundary conditions. Accounting for the dependence of the interfacial free-energy density on the angle between the interfacial unit normal field and the director field eliminates these degeneracies. In particular, when such dependence is taken into account, different solution branches are found, indicating the presence of a bifurcation. We find also that, depending on the magnitude of the anisotropic contribution to the interfacial free-energy density, the interaction between the disclination and the interface may be repulsive or attractive. When the interaction is repulsive, the disclination line positions itself at an energetically optimal distance adjacent to the interface. Otherwise, the uniaxial phase expels the disclination to the interface where a cusp forms.

  19. Adsorption of the natural protein surfactant Rsn-2 onto liquid interfaces.

    PubMed

    Brandani, Giovanni B; Vance, Steven J; Schor, Marieke; Cooper, Alan; Kennedy, Malcolm W; Smith, Brian O; MacPhee, Cait E; Cheung, David L

    2017-03-22

    To stabilize foams, droplets and films at liquid interfaces a range of protein biosurfactants have evolved in nature. Compared to synthetic surfactants, these combine surface activity with biocompatibility and low solution aggregation. One recently studied example is Rsn-2, a component of the foam nest of the frog Engystomops pustulosus, which has been predicted to undergo a clamshell-like opening transition at the air-water interface. Using atomistic molecular dynamics simulations and surface tension measurements we study the adsorption of Rsn-2 onto air-water and cyclohexane-water interfaces. The protein adsorbs readily at both interfaces, with adsorption mediated by the hydrophobic N-terminus. At the cyclohexane-water interface the clamshell opens, due to the favourable interaction between hydrophobic residues and cyclohexane molecules and the penetration of cyclohexane molecules into the protein core. Simulations of deletion mutants showed that removal of the N-terminus inhibits interfacial adsorption, which is consistent with the surface tension measurements. Deletion of the hydrophilic C-terminus also affects adsorption, suggesting that this plays a role in orienting the protein at the interface. The characterisation of the interfacial behaviour gives insight into the factors that control the interfacial adsorption of proteins, which may inform new applications of this and similar proteins in areas including drug delivery and food technology and may also be used in the design of synthetic molecules showing similar changes in conformation at interfaces.

  20. Instability of the Liquid Metal-Pattern Interface in the Lost Foam Casting of Aluminum Alloys

    NASA Astrophysics Data System (ADS)

    Griffiths, W. D.; Ainsworth, M. J.

    2016-06-01

    The nature of the liquid metal-pattern interface during mold filling in the Lost Foam casting of aluminum alloys was investigated using real-time X-ray radiography for both normal expanded polystyrene, and brominated polystyrene foam patterns. Filling the pattern under the action of gravity from above or below had little effect on properties, both cases resulting in a large scatter of tensile strength values, (quantified by their Weibull Modulus). Countergravity filling at different velocities demonstrated that the least scatter of tensile strength values (highest Weibull Modulus) was associated with the slowest filling, when a planar liquid metal-pattern interface occurred. Real-time X-ray radiography showed that the advancing liquid metal front became unstable above a certain critical velocity, leading to the entrainment of the degrading pattern material and associated defects. It has been suggested that the transition of the advancing liquid metal-pattern interface into an unstable regime may be a result of Saffman-Taylor Instability.

  1. Strong collective attraction in colloidal clusters on a liquid-air interface.

    PubMed

    Pergamenshchik, V M

    2009-01-01

    It is shown that in a cluster of many colloids, trapped at a liquid-air interface, the well-known vertical-force-induced pairwise logarithmic attraction changes to a strongly enhanced power-law attraction. In large two-dimensional clusters, the attraction energy scales as the inverse square of the distance between colloids. The enhancement is given by the ratio eta = (square of the capillary length) / (interface surface area per colloid) and can be as large as 10;{5} . This explains why a very small vertical force on colloids, which is too weak to bring two of them together, can stabilize many-body structures on a liquid-air interface. The profile of a cluster is shown to consist of a large slow collective envelope modulated by a fast low-amplitude perturbation due to individual colloids. A closed equation for the slow envelope, which incorporates an arbitrary power-law repulsion between colloids, is derived. For example, this equation is solved for a large circular cluster with the hard-core colloid repulsion. It is suggested that the predicted effect is responsible for mysterious stabilization of colloidal structures observed in experiments on a surface of isotropic liquid and nematic liquid crystal.

  2. Marangoni instability at a contaminated liquid-vapor interface of a burning thin film

    NASA Astrophysics Data System (ADS)

    Armendáriz, Javier; Matalon, Moshe

    2003-05-01

    We consider the evaporation and subsequent burning of thin films of liquid fuels on which a nonsoluble surface active agent (surfactant) is present. This work complements a previous study where we have considered the same problem but in the absence of surfactant. Surfactant may result from impurities of the liquid fuel or from backward diffusion of unoxidized combustion intermediaries and heavy soot precursors. When burning occurs in a quiescent ambient, the mathematical problem can be systematically reduced to a pair of nonlinear evolution equations for the film's thickness and surfactant's concentration. These equations contain, in particular, the temperature and mass flux at the liquid-vapor interface as additional parameters, determined from full consideration of the gas-phase processes. We show that in the absence of combustion or, when the heat released by the chemical reactions is relatively small, thermo-capillary effects tend to destabilize a nominally planar interface. The presence of surfactant brings about a slower growth and can possibly stabilize the film. Combustion generally acts to reverse these trends: When the heat release is large, thermo-capillary effects stabilize the liquid-vapor interface while the presence of surfactant leads to destabilization.

  3. Interaction of Porosity with an Advancing Solid/Liquid Interface: a Real-Time Investigation

    NASA Technical Reports Server (NTRS)

    Sen, S.; Kaukler, W.; Catalina, A.; Stefanescu, D.; Curreri, P.

    1999-01-01

    Problems associated with formation of porosity during solidification continue to have a daily impact on the metal forming industry. Several past investigations have dealt with the nucleation and growth aspects of porosity. However, investigations related to the interaction of porosity with that of a solidification front has been limited mostly to organic analogues. In this paper we report on real time experimental observations of such interactions in metal alloys. Using a state of the art X-Ray Transmission Microscope (XTM) we have been able to observe and record the dynamics of the interaction. This includes distortion of the solid/liquid interface near a poro.sity, solute segr,egation patterns surrounding a porosity and the change in shape of the porosity during interaction with an advancing solid/liquid interface. Results will be presented for different Al alloys and growth conditions. The experimental data will be compared to theory using a recently developed 2D numerical model. The model employs a finite difference approach where the solid/liquid interface is defined through the points at which the interface intersects the grid lines. The transport variables are calculated at these points and the motion of the solidification front is determined by the magnitude of the transport variables. The model accounts for the interplay of the thermal and solutal field and the influence of capilarity to predict the shape of the solid/liquid interface with time in the vicinity of porosity. One can further calculate the perturbation of the solutal field by the presence of porosity in the melt.

  4. Interaction of Porosity with an Advancing Solid/Liquid Interface: a Real-Time Investigation

    NASA Technical Reports Server (NTRS)

    Sen, S.; Kaukler, W.; Catalina, A.; Stefanescu, D.; Curreri, P.

    1999-01-01

    Problems associated with formation of porosity during solidification continue to have a daily impact on the metal forming industry. Several past investigations have dealt with the nucleation and growth aspects of porosity. However, investigations related to the interaction of porosity with that of a solidification front has been limited mostly to organic analogues. In this paper we report on real time experimental observations of such interactions in metal alloys. Using a state of the art X-Ray Transmission Microscope (XTM) we have been able to observe and record the dynamics of the interaction. This includes distortion of the solid/liquid interface near a poro.sity, solute segr,egation patterns surrounding a porosity and the change in shape of the porosity during interaction with an advancing solid/liquid interface. Results will be presented for different Al alloys and growth conditions. The experimental data will be compared to theory using a recently developed 2D numerical model. The model employs a finite difference approach where the solid/liquid interface is defined through the points at which the interface intersects the grid lines. The transport variables are calculated at these points and the motion of the solidification front is determined by the magnitude of the transport variables. The model accounts for the interplay of the thermal and solutal field and the influence of capilarity to predict the shape of the solid/liquid interface with time in the vicinity of porosity. One can further calculate the perturbation of the solutal field by the presence of porosity in the melt.

  5. Heat flow at solid-liquid interfaces: confrontation between experiment and simulation

    NASA Astrophysics Data System (ADS)

    Cahill, David

    2007-03-01

    Heat transport in nanostructures and nanostructured materials provides a novel paradigm for direct comparisons between the results of experiment and simulation. Time-resolved, pump-probe optical techniques enable measurements of the evolution of temperature on time scales from ps to ns. Our pump-probe experiments take two basic forms: measurements of heat transport across planar interfaces using time-domain thermoreflectance and measurements of heat flow from a metal or semiconductor nanostructure into its surroundings using transient absorption. The systems that we are studying are directly accessible to simulation by classical molecular dynamics on the same time and length scales that are encountered in the experiments. Working with our collaborators, P. Keblinski and his colleagues at RPI, we have made quantitative comparisons between experiment and simulation for heat transport from carbon nanotubes and fullerene molecules into a surrounding fluid; and heat transport across hydrophilic and hydrophobic interfaces with water. Any such comparison must take into account i) non-idealities in the experiments; ii) uncertainties in the potentials and atomic geometries in the computational model; and iii) the fact that classical simulations may include high frequency vibrational modes that are not thermally excited in the experiments. Despite the fact that transport at solid-liquid interfaces is more difficult to measure than more commonly studied solid-solid interfaces, we argue that solid-liquid interfaces provide a more reliable system for quantitative comparisons between experiment and simulation.

  6. Computational study of ion distributions at the air/liquid methanol interface

    SciTech Connect

    Sun, Xiuquan; Wick, Collin D.; Dang, Liem X.

    2011-06-16

    Molecular dynamic simulations with polarizable potentials were performed to systematically investigate the distribution of NaCl, NaBr, NaI, and SrCl2 at the air/liquid methanol interface. The density profiles indicated that there is no substantial enhancement of anions at the interface for the NaX systems in contrast to what was observed at the air/aqueous interface. The surfactant-like shape of the larger more polarizable halide anions is compensated by the surfactant nature of methanol itself. As a result, methanol hydroxy groups strongly interacted with one side of polarizable anions, in which their induced dipole points, and methanol methyl groups were more likely to be found near the positive pole of anion induced dipoles. Furthermore, salts were found to disrupt the surface structure of methanol, reducing the observed enhancement of methyl groups at the outer edge of the air/liquid methanol interface. With the additional of salts to methanol, the computed surface potentials increased, which is in contrast to what is observed in corresponding aqueous systems, where the surface potential decreases with the addition of salts. Both of these trends have been indirectly observed with experiments. This was found to be due to the propensity of anions for the air/water interface that is not present at the air/liquid methanol interface. This work was supported by the US Department of Energy Basic Energy Sciences' Chemical Sciences, Geosciences & Biosciences Division. Pacific Northwest National Laboratory is operated by Battelle for the US Department of Energy.

  7. Interface for the rapid analysis of liquid samples by accelerator mass spectrometry

    SciTech Connect

    Turteltaub, Kenneth; Ognibene, Ted; Thomas, Avi; Daley, Paul F; Salazar Quintero, Gary A; Bench, Graham

    2014-02-04

    An interface for the analysis of liquid sample having carbon content by an accelerator mass spectrometer including a wire, defects on the wire, a system for moving the wire, a droplet maker for producing droplets of the liquid sample and placing the droplets of the liquid sample on the wire in the defects, a system that converts the carbon content of the droplets of the liquid sample to carbon dioxide gas in a helium stream, and a gas-accepting ion source connected to the accelerator mass spectrometer that receives the carbon dioxide gas of the sample in a helium stream and introduces the carbon dioxide gas of the sample into the accelerator mass spectrometer.

  8. Dynamic electrowetting and dewetting of ionic liquids at a hydrophobic solid-liquid interface.

    PubMed

    Li, Hua; Paneru, Mani; Sedev, Rossen; Ralston, John

    2013-02-26

    The dynamic electrowetting and dewetting of ionic liquids are investigated with high-speed video microscopy. Five imidazolium-based ionic liquids ([BMIM]BF(4), [BMIM]PF(6), [BMIM]NTf(2), [HMIM]NTf(2), and [OMIM]BF(4)) are used as probe liquids. Droplets of ionic liquids are first spread on an insulated electrode by applying an external voltage (electrowetting) and then allowed to retract (dewetting) when the voltage is switched off. The base area of the droplet varies exponentially during both the electrowetting and retraction processes. The characteristic time increases with the viscosity of the ionic liquid. The electrowetting and retraction kinetics (dynamic contact angle vs contact line speed) can be described by the hydrodynamic or the molecular-kinetic model. Energy dissipation occurs by viscous and molecular routes with a larger proportion of energy dissipated at the three-phase contact line when the liquid meniscus retracts from the solid surface. The outcomes from this research have implications for the design and control of electro-optical imaging systems, microfluidics, and fuel cells.

  9. Formation of Ag nanoparticle-doped foam-like polymer films at the liquid-liquid interface.

    PubMed

    Lin, Li; Shang, Ke; Xu, Xingtao; Chu, Chunxiao; Ma, Huihui; Lee, Yong-Ill; Hao, Jingcheng; Liu, Hong-Guo

    2011-09-29

    The composite poly(2-vinylpyridine) (P2VP)-Ag(+) foam-like thin films were prepared at the interface between AgNO(3) aqueous solution and polymer chloroform solution at 25 °C. An X-ray photoelectron spectroscopy (XPS) investigation indicated that Ag(+) ions in the composite films were partially transformed to Ag atoms after irradiated by UV-light and completely transformed to Ag atoms after being treated with KBH(4) aqueous solution. Ag nanoparticles with the average sizes of 2.71 ± 0.82 and 3.28 ± 1.20 nm were generated in these two transferred films with different treatments, respectively. Transmission electron microscopy (TEM) and high-resolution TEM (HRTEM) images showed clearly that the composite films were composed of microcapsules whose walls had multilayer structures, and the nanoparticles were incorporated in the walls. The formation of the composite films at the liquid-liquid interface was attributed to the adsorption of the polymer molecules at the interface, coordination between the pyridine groups and Ag(+) ions, and self-assembly of the composite molecules. Furthermore, the catalytic activity of the composite films was evaluated using the reduction of 4-nitrophenol (4-NP) by KBH(4). The results demonstrated that the composite thin films have high and durable catalytic activity. © 2011 American Chemical Society

  10. In situ X-ray studies of adlayer-induced crystal nucleation at the liquid-liquid interface

    SciTech Connect

    Elsen, Annika; Festersen, Sven; Runge, Benjamin; Koops, Christian T.; Ocko, Benjamin M.; Deutsch, Moshe; Seeck, Oliver H.; Murphy, Bridget M.; Magnussen, Olaf M.

    2013-05-29

    Crystal nucleation and growth at a liquid–liquid interface is studied on the atomic scale by in situ Å-resolution X-ray scattering methods for the case of liquid Hg and an electrochemical dilute electrolyte containing Pb2+, F-, and Br- ions. In the regime negative of the Pb amalgamation potential Φrp = -0.70 V, no change is observed from the surface-layered structure of pure Hg. Upon potential-induced release of Pb2+ from the Hg bulk at Graphic, the formation of an intriguing interface structure is observed, comprising a well-defined 7.6-Å–thick adlayer, decorated with structurally related 3D crystallites. Both are identified by their diffraction peaks as PbFBr, preferentially aligned with their Graphic axis along the interface normal. X-ray reflectivity shows the adlayer to consist of a stack of five ionic layers, forming a single-unit-cell–thick crystalline PbFBr precursor film, which acts as a template for the subsequent quasiepitaxial 3D crystal growth. This growth behavior is assigned to the combined action of electrostatic and short-range chemical interactions.

  11. Thermodynamic Study of the Role of Interface Curvature on Multicomponent Vapor-Liquid Phase Equilibrium.

    PubMed

    Shardt, Nadia; Elliott, Janet A W

    2016-04-14

    The effect of interface curvature on phase equilibrium has been much more studied for single-component than multicomponent systems. We isolate the effect of curvature on multicomponent vapor-liquid equilibrium (VLE) phase envelopes and phase composition diagrams using the ideal system methanol/ethanol and the nonideal system ethanol/water as illustrative examples. An important finding is how nanoscale interface curvature shifts the azeotrope (equal volatility point) of nonideal systems. Understanding of the effect of curvature on VLE can be exploited in future nanoscale prediction and design.

  12. Molecular electrocatalysis for oxygen reduction by cobalt porphyrins adsorbed at liquid/liquid interfaces.

    PubMed

    Su, Bin; Hatay, Imren; Trojánek, Antonín; Samec, Zdenek; Khoury, Tony; Gros, Claude P; Barbe, Jean-Michel; Daina, Antoine; Carrupt, Pierre-Alain; Girault, Hubert H

    2010-03-03

    Molecular electrocatalysis for oxygen reduction at a polarized water/1,2-dichloroethane (DCE) interface was studied, involving aqueous protons, ferrocene (Fc) in DCE and amphiphilic cobalt porphyrin catalysts adsorbed at the interface. The catalyst, (2,8,13,17-tetraethyl-3,7,12,18-tetramethyl-5-p-amino-phenylporphyrin) cobalt(II) (CoAP), functions like conventional cobalt porphyrins, activating O(2) via coordination by the formation of a superoxide structure. Furthermore, due to the hydrophilic nature of the aminophenyl group, CoAP has a strong affinity for the water/DCE interface as evidenced by lipophilicity mapping calculations and surface tension measurements, facilitating the protonation of the CoAP-O(2) complex and its reduction by ferrocene. The reaction is electrocatalytic as its rate depends on the applied Galvani potential difference between the two phases.

  13. Quantum chemical approach in the description of the amphiphile clusterization at the air/liquid and liquid/liquid interfaces with phase nature accounting. I. Aliphatic normal alcohols at the air/water interface.

    PubMed

    Vysotsky, Yuri B; Belyaeva, Elena A; Kartashynska, Elena S; Fainerman, Valentine B; Smirnova, Natalia A

    2015-02-19

    A new model based on the quantum chemical approach is proposed to describe structural and thermodynamic parameters of clusterization for substituted alkanes at the air/liquid and liquid/liquid interfaces. The new model by the authors, unlike the previous one, proposes an explicit account of the liquid phase (phases) influence on the parameters of monomers, clusters and monolayers of substituted alkanes at the regarded interface. The calculations were carried out in the frameworks of the quantum chemical semiempirical PM3 method (Mopac 2012), using the COSMO procedure. The new model was tested in the calculations of the clusterization parameters of fatty alcohols under the standard conditions at the air/water interface. The enthalpy, Gibbs' energy and absolute entropy of formation for alcohol monomers alongside with clusterization parameters for the cluster series including the monolayer at air/water interface were calculated. In our calculations the sinkage of monomers, molecules in clusters and monolayers was varied from 1 up to 5 methylene groups. Thermodynamic parameters calculated using the proposed model for the alcohol monolayers are in a good agreement with the corresponding experimental data. However, the proposed model cannot define the most energetically preferable immersion of the monolayer molecules in the water phase.

  14. Proton-coupled oxygen reduction at liquid-liquid interfaces catalyzed by cobalt porphine.

    PubMed

    Hatay, Imren; Su, Bin; Li, Fei; Méndez, Manuel Alejandro; Khoury, Tony; Gros, Claude P; Barbe, Jean-Michel; Ersoz, Mustafa; Samec, Zdenek; Girault, Hubert H

    2009-09-23

    Cobalt porphine (CoP) dissolved in the organic phase of a biphasic system is used to catalyze O(2) reduction by an electron donor, ferrocene (Fc). Using voltammetry at the interface between two immiscible electrolyte solutions (ITIES), it is possible to drive this catalytic reduction at the interface as a function of the applied potential difference, where aqueous protons and organic electron donors combine to reduce O(2). The current signal observed corresponds to a proton-coupled electron transfer (PCET) reaction, as no current and no reaction can be observed in the absence of either the aqueous acid, CoP, Fc, or O(2).

  15. Understanding Charge Transfer Reactions at the Interface of Plasmas in Contact with Liquids

    NASA Astrophysics Data System (ADS)

    Go, David

    2015-09-01

    Plasmas in and in contact with liquids offer a very rich physical and chemical environment where a multitude of species (electrons, ions, neutrals) and physical phenomena (light, electric fields) intersect. With emerging applications in medicine, environmental remediation, and materials synthesis, it has become paramount to understand the many processes occurring at the interface in order to design and optimize new technologies. Perhaps the most important plasma species is the electron, and it thus reasonable to assume it can play a critical role when plasmas are brought in contact with liquids as well. Over the past several years, our group has focused on deciphering the nature of electron transfer from a plasma to liquid and the subsequent chemistry the electrons induce. Our experimental configuration is the plasma equivalent of an electrochemical or electrolytic cell, where the cathode and anode are submerged in an electrolyte solution and current is carried by reduction reactions at the cathode and oxidation reactions at the anode. When the cathode is replaced by a plasma, the circuit is explicitly completed by the injection of plasma electrons into the solution where they stably solvate before inducing reduction reactions. Recently, we have demonstrated the first direct detection of these stably solvated electrons using a novel total internal reflection absorption spectroscopy experiment, resulting in the first measurement of the optical absorption spectrum for plasma-solvated electrons. Further, we have shown that the lifetime of these electrons can be significantly reduced if suitable solution- and plasma-phase scavengers are used to react quickly with these electrons. These results highlight the complexity of the plasma-liquid interface and how charge-transfer processes often compete with other chemistry that occurs at the plasma-liquid interface, such as the dissolution of plasma species into the liquid. This work was supported by the U.S. Army Research

  16. Atomically Abrupt Liquid-Oxide Interface Stabilized by Self-Regulated Interfacial Defects: The Case of Al/Al2O3 Interfaces

    SciTech Connect

    Kang, J.; Zhu, J. Y.; Curtis, C.; Blake, D.; Glatzmaier, G.; Kim, Y. H.; Wei, S. H.

    2012-06-01

    The atomic and electronic structures of the liquid Al/(0001) {alpha}-Al{sub 2}O{sub 3} interfaces are investigated by first-principles molecular dynamics simulations. Surprisingly, the formed liquid-solid interface is always atomically abrupt and is characterized by a transitional Al layer that contains a fixed concentration of Al vacancies ({approx}10 at.%). We find that the self-regulation of the defect density in the metal layer is due to the fact that the formation energy of the Al vacancies is readjusted in a way that opposes changes in the defect density. The negative-feedback effect stabilizes the defected transitional layer and maintains the atomic abruptness at the interface. The proposed mechanism is generally applicable to other liquid-metal/metal-oxide systems, and thus of significant importance in understanding the interface structures at high temperature.

  17. Diffuse-interface modeling of liquid-vapor coexistence in equilibrium drops using smoothed particle hydrodynamics.

    PubMed

    Sigalotti, Leonardo Di G; Troconis, Jorge; Sira, Eloy; Peña-Polo, Franklin; Klapp, Jaime

    2014-07-01

    We study numerically liquid-vapor phase separation in two-dimensional, nonisothermal, van der Waals (vdW) liquid drops using the method of smoothed particle hydrodynamics (SPH). In contrast to previous SPH simulations of drop formation, our approach is fully adaptive and follows the diffuse-interface model for a single-component fluid, where a reversible, capillary (Korteweg) force is added to the equations of motion to model the rapid but smooth transition of physical quantities through the interface separating the bulk phases. Surface tension arises naturally from the cohesive part of the vdW equation of state and the capillary forces. The drop models all start from a square-shaped liquid and spinodal decomposition is investigated for a range of initial densities and temperatures. The simulations predict the formation of stable, subcritical liquid drops with a vapor atmosphere, with the densities and temperatures of coexisting liquid and vapor in the vdW phase diagram closely matching the binodal curve. We find that the values of surface tension, as determined from the Young-Laplace equation, are in good agreement with the results of independent numerical simulations and experimental data. The models also predict the increase of the vapor pressure with temperature and the fitting to the numerical data reproduces very well the Clausius-Clapeyron relation, thus allowing for the calculation of the vaporization pressure for this vdW fluid.

  18. Surface Tension, Adsorption, and Molecular Orientations at the Liquid-Vapor Interface of Molecular Mixtures.

    NASA Astrophysics Data System (ADS)

    Thurtell, John Harland

    A generalized van der Waal's Mean Field Theory and Molecular Dynamics computer simulations have been used to study the liquid-vapor interface of simple liquid crystals, atomic mixtures, polar mixtures, and polar solvent-surfactant mixtures. Surface tensions, density profiles, and orientational order parameters have been calculated at the planar liquid -vapor interfaces of liquid crystals, argon-krypton mixtures, and polar mixtures using a mean field theory of molecular liquids. The effect of size, shape and dipole strength on the thickness, concentration and orientational ordering of adsorbed layers have been studied in detail. These parameters yield widely varying interfacial structures and can lead to interfacial and bulk phase transitions. Molecular dynamics simulations of simple surfactant models in a polar solvent have been carried out for varying intermolecular potentials. In particular the effect of the surfactant dipole strength, orientation and position were examined. The dipole has a large influence on the surface tension, molecular orientations and thickness of the interfacial region of these systems. We find a number of competing effects which result in unpredictable behavior in some situations.

  19. Formation of H-type liquid crystal dimer at air-water interface

    SciTech Connect

    Karthik, C. Gupta, Adbhut Joshi, Aditya Manjuladevi, V. Gupta, Raj Kumar; Varia, Mahesh C.; Kumar, Sandeep

    2014-04-24

    We have formed the Langmuir monolayer of H-shaped Azo linked liquid crystal dimer molecule at the air-water interface. Isocycles of the molecule showed hysteresis suggesting the ir-reversible nature of the monolayer formed. The thin film deposited on the silicon wafer was characterized using Atomic Force Microscopy (AFM) and Field Emission Scanning Electron Microscopy (FESEM). The images showed uniform domains of the dimer molecule. We propose that these molecules tend to take book shelf configuration in the liquid phase.

  20. The DNA Adsorption by the Charged Cholesterol Monolayer at the Air-liquid Interface

    NASA Astrophysics Data System (ADS)

    Lin, Tsang-Lang; Hu, Yuan; Wu, Jui-Ching; Yang, Chun-Pang; Jeng, U.-Ser; Shih, M.-C.

    2004-04-01

    The adsorption of DNA by the 3-,-[N-(N',N'-dimethyl amino ethane) carbamoyl] cholesterol (DC-Chol) monolayer at the air-liquid interface was studied by using the Langmuir-Blodgett film balance. With the presence of 1 μ M DNA in the subphase, the surface pressure increases right at the beginning of the compression. The liquid expanded phase of the DC-Chol disappears due to the adsorption of DNA. The AFM image of the prepared DC-Chol/DNA film has tree-branch-like fractal structure with a height of 2 nm that correspond to the diameter of DNA.

  1. Apparent slip over a solid-liquid interface with a no-slip boundary condition.

    PubMed

    Zhang, Junfeng; Kwok, Daniel Y

    2004-11-01

    We studied solid-liquid slip by a mean-field free-energy lattice Boltzmann approach recently proposed [Phys. Rev. E 69, 032602 (2004)]. With a general bounce-back no-slip boundary condition applied to the interface, liquid slip was observed because of the specific solid-fluid interactions. Our work relates interfacial slip to a more realistic solid-fluid interaction and hence contact angle. The kinetic nature of LBM is manifested in this interfacial study. A small negative slip length can also be produced with a stronger solid-fluid attraction.

  2. Water permeability of primary mouse keratinocyte cultures grown at the air-liquid interface

    SciTech Connect

    Cumpstone, M.B.; Kennedy, A.H.; Harmon, C.S.; Potts, R.O.

    1989-04-01

    In order to study the development of the epidermal permeability barrier in vitro, tritiated water (HTO) flux was measured across murine keratinocytes cultured at the air-liquid interface. Using a micro-diffusion technique, it was shown that air-liquid cultures form areas where the water diffusion is comparable to that of intact neonatal mouse skin. When water permeability is measured over a large area of the culture surface, however, significantly higher flux is obtained. These results show that under the culture conditions used, areas of water barrier comparable to intact neonatal mouse skin coexist with regions of less complete barrier formation.

  3. The production of drops by the bursting of a bubble at an air liquid interface

    NASA Technical Reports Server (NTRS)

    Darrozes, J. S.; Ligneul, P.

    1982-01-01

    The fundamental mechanism arising during the bursting of a bubble at an air-liquid interface is described. A single bubble was followed from an arbitrary depth in the liquid, up to the creation and motion of the film and jet drops. Several phenomena were involved and their relative order of magnitude was compared in order to point out the dimensionless parameters which govern each step of the motion. High-speed cinematography is employed. The characteristic bubble radius which separates the creation of jet drops from cap bursting without jet drops is expressed mathematically. The corresponding numerical value for water is 3 mm and agrees with experimental observations.

  4. Effect of Schmidt number on mass transfer across a sheared gas-liquid interface in a wind-driven turbulence

    PubMed Central

    Takagaki, Naohisa; Kurose, Ryoichi; Kimura, Atsushi; Komori, Satoru

    2016-01-01

    The mass transfer across a sheared gas-liquid interface strongly depends on the Schmidt number. Here we investigate the relationship between mass transfer coefficient on the liquid side, kL, and Schmidt number, Sc, in the wide range of 0.7 ≤ Sc ≤ 1000. We apply a three-dimensional semi direct numerical simulation (SEMI-DNS), in which the mass transfer is solved based on an approximated deconvolution model (ADM) scheme, to wind-driven turbulence with mass transfer across a sheared wind-driven wavy gas-liquid interface. In order to capture the deforming gas-liquid interface, an arbitrary Lagrangian-Eulerian (ALE) method is employed. Our results show that similar to the case for flat gas-liquid interfaces, kL for the wind-driven wavy gas-liquid interface is generally proportional to Sc−0.5, and can be roughly estimated by the surface divergence model. This trend is endorsed by the fact that the mass transfer across the gas-liquid interface is controlled mainly by streamwise vortices on the liquid side even for the wind-driven turbulence under the conditions of low wind velocities without wave breaking. PMID:27841325

  5. Effect of Schmidt number on mass transfer across a sheared gas-liquid interface in a wind-driven turbulence

    NASA Astrophysics Data System (ADS)

    Takagaki, Naohisa; Kurose, Ryoichi; Kimura, Atsushi; Komori, Satoru

    2016-11-01

    The mass transfer across a sheared gas-liquid interface strongly depends on the Schmidt number. Here we investigate the relationship between mass transfer coefficient on the liquid side, kL, and Schmidt number, Sc, in the wide range of 0.7 ≤ Sc ≤ 1000. We apply a three-dimensional semi direct numerical simulation (SEMI-DNS), in which the mass transfer is solved based on an approximated deconvolution model (ADM) scheme, to wind-driven turbulence with mass transfer across a sheared wind-driven wavy gas-liquid interface. In order to capture the deforming gas-liquid interface, an arbitrary Lagrangian-Eulerian (ALE) method is employed. Our results show that similar to the case for flat gas-liquid interfaces, kL for the wind-driven wavy gas-liquid interface is generally proportional to Sc-0.5, and can be roughly estimated by the surface divergence model. This trend is endorsed by the fact that the mass transfer across the gas-liquid interface is controlled mainly by streamwise vortices on the liquid side even for the wind-driven turbulence under the conditions of low wind velocities without wave breaking.

  6. Effect of Schmidt number on mass transfer across a sheared gas-liquid interface in a wind-driven turbulence.

    PubMed

    Takagaki, Naohisa; Kurose, Ryoichi; Kimura, Atsushi; Komori, Satoru

    2016-11-14

    The mass transfer across a sheared gas-liquid interface strongly depends on the Schmidt number. Here we investigate the relationship between mass transfer coefficient on the liquid side, kL, and Schmidt number, Sc, in the wide range of 0.7 ≤ Sc ≤ 1000. We apply a three-dimensional semi direct numerical simulation (SEMI-DNS), in which the mass transfer is solved based on an approximated deconvolution model (ADM) scheme, to wind-driven turbulence with mass transfer across a sheared wind-driven wavy gas-liquid interface. In order to capture the deforming gas-liquid interface, an arbitrary Lagrangian-Eulerian (ALE) method is employed. Our results show that similar to the case for flat gas-liquid interfaces, kL for the wind-driven wavy gas-liquid interface is generally proportional to Sc(-0.5), and can be roughly estimated by the surface divergence model. This trend is endorsed by the fact that the mass transfer across the gas-liquid interface is controlled mainly by streamwise vortices on the liquid side even for the wind-driven turbulence under the conditions of low wind velocities without wave breaking.

  7. Universal emulsion stabilization from the arrested adsorption of rough particles at liquid-liquid interfaces

    PubMed Central

    Zanini, Michele; Marschelke, Claudia; Anachkov, Svetoslav E.; Marini, Emanuele; Synytska, Alla; Isa, Lucio

    2017-01-01

    Surface heterogeneities, including roughness, significantly affect the adsorption, motion and interactions of particles at fluid interfaces. However, a systematic experimental study, linking surface roughness to particle wettability at a microscopic level, is currently missing. Here we synthesize a library of all-silica microparticles with uniform surface chemistry, but tuneable surface roughness and study their spontaneous adsorption at oil–water interfaces. We demonstrate that surface roughness strongly pins the particles' contact lines and arrests their adsorption in long-lived metastable positions, and we directly measure the roughness-induced interface deformations around isolated particles. Pinning imparts tremendous contact angle hysteresis, which can practically invert the particle wettability for sufficient roughness, irrespective of their chemical nature. As a unique consequence, the same rough particles stabilize both water-in-oil and oil-in-water emulsions depending on the phase they are initially dispersed in. These results both shed light on fundamental phenomena concerning particle adsorption at fluid interfaces and indicate future design rules for particle-based emulsifiers. PMID:28589932

  8. Alkyl Chain Ordering of Asymmetric Phosphatidyicholines Adsorbed at a Liquid-Liquid Interface

    DTIC Science & Technology

    1998-05-30

    in the commercial use of natural phosphatidylcholines (or lecithins ) as emulsifiers , including their use in delivery of water-insoluble drugs (Davis...saturated di-acyl lecithins at the n-heptane/aqueous sodium chloride interface. J. Am. Chem. Soc, Faraday Trans. 1 78:323-339. Ogino, K. and M. Onishi

  9. Conventional and microwave hydrothermal synthesis of monodispersed metal oxide nanoparticles at liquid-liquid interface

    EPA Science Inventory

    Monodispersed nanoparticles of metal oxide including ferrites MFe2O4 (M=, Ni, Co, Mn) and γ-Fe2O3, Ta2O5 etc. have been synthesized using a water-toluene interface under both conventional and microwave hydrothermal conditions. This general synthesis procedure uses readily availab...

  10. Universal emulsion stabilization from the arrested adsorption of rough particles at liquid-liquid interfaces

    NASA Astrophysics Data System (ADS)

    Zanini, Michele; Marschelke, Claudia; Anachkov, Svetoslav E.; Marini, Emanuele; Synytska, Alla; Isa, Lucio

    2017-06-01

    Surface heterogeneities, including roughness, significantly affect the adsorption, motion and interactions of particles at fluid interfaces. However, a systematic experimental study, linking surface roughness to particle wettability at a microscopic level, is currently missing. Here we synthesize a library of all-silica microparticles with uniform surface chemistry, but tuneable surface roughness and study their spontaneous adsorption at oil-water interfaces. We demonstrate that surface roughness strongly pins the particles' contact lines and arrests their adsorption in long-lived metastable positions, and we directly measure the roughness-induced interface deformations around isolated particles. Pinning imparts tremendous contact angle hysteresis, which can practically invert the particle wettability for sufficient roughness, irrespective of their chemical nature. As a unique consequence, the same rough particles stabilize both water-in-oil and oil-in-water emulsions depending on the phase they are initially dispersed in. These results both shed light on fundamental phenomena concerning particle adsorption at fluid interfaces and indicate future design rules for particle-based emulsifiers.

  11. Effect of polyelectrolyte-surfactant complexation on Marangoni transport at a liquid-liquid interface.

    PubMed

    Dunér, Gunnar; Kim, Michelle; Tilton, Robert D; Garoff, Stephen; Przybycien, Todd M

    2016-04-01

    Complexation of surfactants and oppositely charged polyelectrolytes is expected to alter Marangoni transport at a fluid interface compared to either single component system due to altered interfacial tension isotherms and mass transfer rates as well as adsorption irreversibility effects. We investigate Marangoni transport at the oil/water interface by passing mixtures of the anionic surfactant sodium dodecyl sulfate (SDS) and cationic polyelectrolyte poly(3-(2-methylpropionamide)propyl) trimethylammonium chloride-acrylamide (poly[AM-MAPTAC]), or rinsing solutions, over an oil/water interface in a radial, stagnation point flow. The displacements of adsorbed tracer particles are recorded through optical microscopy. The net displacement, defined as the sum of the displacements occurring during the adsorption and desorption stages of one application and rinsing cycle, is up to 10 times greater for complexing surfactant/polymer mixtures compared to either single component system. The enhanced net displacement is largely determined by the enhanced transport upon adsorption, while the reverse displacement that would normally occur upon rinsing is partially suppressed by partially irreversible polymer adsorption at the oil/water interface. In addition to effects of complexation on interfacial tension gradient induced flow, complexation effects on the bulk, and possibly interfacial, viscosity also influence the interfacial transport. Copyright © 2016 Elsevier Inc. All rights reserved.

  12. Conventional and microwave hydrothermal synthesis of monodispersed metal oxide nanoparticles at liquid-liquid interface

    EPA Science Inventory

    Monodispersed nanoparticles of metal oxide including ferrites MFe2O4 (M=, Ni, Co, Mn) and γ-Fe2O3, Ta2O5 etc. have been synthesized using a water-toluene interface under both conventional and microwave hydrothermal conditions. This general synthesis procedure uses readily availab...

  13. Near-field deformation of a liquid interface by atomic force microscopy

    NASA Astrophysics Data System (ADS)

    Mortagne, C.; Chireux, V.; Ledesma-Alonso, R.; Ogier, M.; Risso, F.; Ondarçuhu, T.; Legendre, D.; Tordjeman, Ph.

    2017-07-01

    We experiment the interaction between a liquid puddle and a spherical probe by Atomic Force Microscopy (AFM) for a probe radius R ranging from 10 nm to 30 μ m . We have developed a new experimental setup by coupling an AFM with a high-speed camera and an inverted optical microscope. Interaction force-distance curves (in contact mode) and frequency shift-distance curves (in frequency modulation mode) are measured for different bulk model liquids for which the probe-liquid Hamaker constant Hp l is known. The experimental results, analyzed in the frame of the theoretical model developed in Phys. Rev. Lett. 108, 106104 (2012), 10.1103/PhysRevLett.108.106104 and Phys. Rev. E 85, 061602 (2012), 10.1103/PhysRevE.85.061602, allow to determine the "jump-to-contact" critical distance dmin below which the liquid jumps and wets the probe. Comparison between theory and experiments shows that the probe-liquid interaction at nanoscale is controlled by the liquid interface deformation. This work shows a very good agreement between the theoretical model and the experiments and paves the way to experimental studies of liquids at the nanoscale.

  14. Nudged elastic band calculation of the binding potential for liquids at interfaces.

    PubMed

    Buller, Oleg; Tewes, Walter; Archer, Andrew J; Heuer, Andreas; Thiele, Uwe; Gurevich, Svetlana V

    2017-07-14

    The wetting behavior of a liquid on solid substrates is governed by the nature of the effective interaction between the liquid-gas and the solid-liquid interfaces, which is described by the binding or wetting potential g(h) which is an excess free energy per unit area that depends on the liquid film height h. Given a microscopic theory for the liquid, to determine g(h), one must calculate the free energy for liquid films of any given value of h, i.e., one needs to create and analyze out-of-equilibrium states, since at equilibrium there is a unique value of h, specified by the temperature and chemical potential of the surrounding gas. Here we introduce a Nudged Elastic Band (NEB) approach to calculate g(h) and illustrate the method by applying it in conjunction with a microscopic lattice density functional theory for the liquid. We also show that the NEB results are identical to those obtained with an established method based on using a fictitious additional potential to stabilize the non-equilibrium states. The advantages of the NEB approach are discussed.

  15. Nudged elastic band calculation of the binding potential for liquids at interfaces

    NASA Astrophysics Data System (ADS)

    Buller, Oleg; Tewes, Walter; Archer, Andrew J.; Heuer, Andreas; Thiele, Uwe; Gurevich, Svetlana V.

    2017-07-01

    The wetting behavior of a liquid on solid substrates is governed by the nature of the effective interaction between the liquid-gas and the solid-liquid interfaces, which is described by the binding or wetting potential g(h) which is an excess free energy per unit area that depends on the liquid film height h. Given a microscopic theory for the liquid, to determine g(h), one must calculate the free energy for liquid films of any given value of h, i.e., one needs to create and analyze out-of-equilibrium states, since at equilibrium there is a unique value of h, specified by the temperature and chemical potential of the surrounding gas. Here we introduce a Nudged Elastic Band (NEB) approach to calculate g(h) and illustrate the method by applying it in conjunction with a microscopic lattice density functional theory for the liquid. We also show that the NEB results are identical to those obtained with an established method based on using a fictitious additional potential to stabilize the non-equilibrium states. The advantages of the NEB approach are discussed.

  16. Asymmetric gravity jitter excited slosh waves at a liquid-vapor-solid interface in microgravity

    NASA Technical Reports Server (NTRS)

    Hung, R. J.; Pan, H. L.; Leslie, F. W.

    1992-01-01

    The dynamical behavior of fluids affected by the asymmetric gravity jitter oscillations is investigated focusing on the surface tension effect on partially filled rotating fluids in a sub-scale gravity probe-B spacecraft propellant dewar tank. Data obtained revealed that the lower frequency gravity jitter imposed on the time-dependent variations of the background gravity direction induced a greater amplitude of oscillations and a stronger degree of asymmetry in liquid-vapor interface geometry than that caused by the higher frequency gravity jitter. It is also found that the greater the components of background gravity in radial and circumferential directions the greater the contribution to driving more toward increasing amplitude and degrees of asymmetry of the liquid-vapor interface profiles, which in turn modify the disturbance of moment of inertia and angular momentum of spacecraft.

  17. Quantification of ordering at a solid-liquid interface using plasmon electron energy loss spectroscopy

    SciTech Connect

    Gandman, Maria; Kauffmann, Yaron; Kaplan, Wayne D.

    2015-02-02

    We present an in situ electron energy loss spectroscopy (EELS) study of ordering of liquid Al at various Al-Al{sub 2}O{sub 3} interfaces. This technique utilizes precise measurements of the shifts in bulk plasmon resonance and their sensitivity to the valence electron density. Plasmon EELS combined with high resolution transmission electron microscopy provides information regarding the chemical composition in liquid Al at Al-Al{sub 2}O{sub 3} interfaces. Preferential oxygen segregation to the (0006) Al{sub 2}O{sub 3} plane was verified, and the (101{sup ¯}2) Al{sub 2}O{sub 3} plane was found to contain the lowest amount of segregated species.

  18. In Situ Probing of Ion Ordering at an Electrified Ionic Liquid/Au Interface

    DOE PAGES

    Sitaputra, Wattaka; Stacchiola, Dario; Wishart, James F.; ...

    2017-05-12

    Charge transport at the interface of electrodes and ionic liquids is critical for the use of the latter as electrolytes. In this study, a room-temperature ionic liquid, 1-ethyl-2,3-dimethylimidazolium bis(trifluoromethanesulfonyl)imide (EMMIM TFSI), is investigated in situ under applied bias voltage with a novel method using low-energy electron and photoemission electron microscopy. Changes in photoelectron yield as a function of bias applied to electrodes provide a direct measure of the dynamics of ion reconfiguration and electrostatic responses of the EMMIM TFSI. Finally, long-range and correlated ionic reconfigurations that occur near the electrodes are found to be a function of temperature and thickness,more » which, in turn, relate to ionic mobility and different configurations for out-of-plane ordering near the electrode interfaces, with a critical transition in ion mobility for films thicker than three monolayers.« less

  19. Characterisation of the solid electrolyte interface during lithiation/delithiation of germanium in an ionic liquid.

    PubMed

    Lahiri, Abhishek; Borisenko, Natalia; Borodin, Andriy; Olschewski, Mark; Endres, Frank

    2016-02-21

    In this paper, we present investigations of the interface of electrodeposited Ge during lithiation/delithiation in the ionic liquid 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide containing 0.5 M lithium bis(trifluoromethylsulfonyl)imide (LiTFSI/[Py1,4]TFSI). Cyclic voltammetry (CV) and infrared spectroscopy were used to study the electrochemistry and the changes in the electrolyte during the Li intercalation/deintercalation processes. From infrared spectroscopic analysis, it was found that the TFSI(-) anion decomposes during the lithiation process, resulting in the formation of a solid-liquid interface (SEI) layer. X-ray photoelectron spectroscopy was used to analyse the composition of the SEI layer and the changes in the electrodeposited germanium. Furthermore, atomic force microscopy (AFM) was used to evaluate the changes in the SEI layer which showed that the SEI layer was inhomogenous and changed during the lithiation/delithiation processes.

  20. Capillary wave analysis of rough solid-liquid interfaces in nickel

    NASA Astrophysics Data System (ADS)

    Rozas, R. E.; Horbach, J.

    2011-01-01

    Crystal-liquid interfaces in nickel are investigated by molecular-dynamics computer simulations. Inhomogeneous systems of size Lx×Ly×Lz with Lz=5Ly are prepared where the crystal fcc phase at different orientations coexists with the liquid phase, separated by planar interfaces in the xy-plane. The lateral dimensions are varied, using two different geometries with Lx=Ly and with LyGtLx. In the framework of capillary wave theory (CWT), anisotropic interfacial stiffnesses and tensions are determined using different predictions of CWT with respect to the spectrum, finite-size broadening and different geometries. From a parameterization in terms of cubic harmonics up to 8th order, the anisotropic interfacial free energy is obtained.

  1. Numerical formulation of composition segregation at curved solid-liquid interface during steady state solidification process

    NASA Technical Reports Server (NTRS)

    Wang, Jai-Ching

    1994-01-01

    The lateral solute segregation that results from a curved solid-liquid interface shape during steady state unidirectional solidification of a binary alloy system has been studied both analytically and numerically by Coriell, Bosivert, Rehm, and Sekerka. The system under their study is a two dimensional rectangular system. However, most real growth systems are cylindrical systems. Thus, in a previous study, we have followed Coriell etc. formalism and obtained analytical results for lateral solute segregation for an azimuthal symmetric cylindrical binary melt system during steady state solidification process. The solid-liquid interface shape is expressed as a series combination of Bessel functions. In this study a computer program has been developed to simulate the lateral solute segregation.

  2. A new interface for coupling solid phase microextraction with liquid chromatography.

    PubMed

    Chen, Yong; Sidisky, Leonard M

    2014-03-19

    A modified Rheodyne 7520 microsample injector was used as a new solid phase microextraction (SPME)-liquid chromatography (LC) interface. The modification was focused on the construction of a new sample rotor, which was built by gluing two sample rotors together. The new sample rotor was further reinforced with 3 pieces of stainless steel tubing. The enlarged central flow passage in the new sample rotor was used as a desorption chamber. SPME fiber desorption occurred in static mode. But all desorption solvent in the desorption chamber was injected into LC system with the interface. The analytical performance of the interface was evaluated by SPME-LC analysis of PAHs in water. At least 90% polycyclic aromatic hydrocarbons (PAHs) were desorbed from a polyacrylonitrile (PAN)/C18 bonded fuse silica fiber in 30s. And injection was completed in 20s. About 10-20% total carryovers were found on the fiber and in the interface. The carryover in the interface was eliminated by flushing the desorption chamber with acetonitrile at 1mL min(-1) for 2min. The repeatability of the method was from 2% to 8%. The limit of detection (LOD) was in the mid pg mL(-1) range. The linear ranges were from 0.1 to 100ng mL(-1). The new SPME-LC interface was reliable for coupling SPME with LC for both qualitative and quantitative analysis.

  3. Adsorption and solvation of ethanol at the water liquid-vapor interface: a molecular dynamics study

    NASA Technical Reports Server (NTRS)

    Wilson, M. A.; Pohorille, A.

    1997-01-01

    The free energy profiles of methanol and ethanol at the water liquid-vapor interface at 310K were calculated using molecular dynamics computer simulations. Both alcohols exhibit a pronounced free energy minimum at the interface and, therefore, have positive adsorption at this interface. The surface excess was computed from the Gibbs adsorption isotherm and was found to be in good agreement with experimental results. Neither compound exhibits a free energy barrier between the bulk and the surface adsorbed state. Scattering calculations of ethanol molecules from a gas phase thermal distribution indicate that the mass accommodation coefficient is 0.98, and the molecules become thermalized within 10 ps of striking the interface. It was determined that the formation of the solvation structure around the ethanol molecule at the interface is not the rate-determining step in its uptake into water droplets. The motion of an ethanol molecule in a water lamella was followed for 30 ns. The time evolution of the probability distribution of finding an ethanol molecule that was initially located at the interface is very well described by the diffusion equation on the free energy surface.

  4. Faceting of a rough solid-liquid interface of a metal induced by forced convection

    NASA Astrophysics Data System (ADS)

    Binder, Sven; Galenko, Peter K.; Herlach, Dieter M.

    2013-10-01

    The solid-liquid interface of metallic systems of small entropy of fusion is characterized by a rough interface and dendritic morphology. In contrast, systems of high entropy of fusion like semimetals and semiconductors show smooth interfaces and facetted interfaces. The present work demonstrates that, in an undercooled melt of a metal-metalloid alloy Ni2B of intermediate entropy of fusion, a transition from a rough to a smooth interface is induced by forced convection of the melt. Electrostatic levitation is used to container-less undercool droplets in a quiescent state with no convection while electromagnetic levitation (EML) is used to undercool droplets with forced convection. The growth velocity of the solid phase is monitored as a function of undercooling by a high-speed video camera. The data are analysed within dendrite growth theory. In the case of EML, a transition from a rough to a smooth interface is indicated during dendrite growth in the undercooled melt. This is confirmed by facetted microstructures of samples solidified upon undercooling by EML. Hopper-like crystals are formed like in non-metals as bismuth, halite and ice.

  5. Adsorption and solvation of ethanol at the water liquid-vapor interface: a molecular dynamics study

    NASA Technical Reports Server (NTRS)

    Wilson, M. A.; Pohorille, A.

    1997-01-01

    The free energy profiles of methanol and ethanol at the water liquid-vapor interface at 310K were calculated using molecular dynamics computer simulations. Both alcohols exhibit a pronounced free energy minimum at the interface and, therefore, have positive adsorption at this interface. The surface excess was computed from the Gibbs adsorption isotherm and was found to be in good agreement with experimental results. Neither compound exhibits a free energy barrier between the bulk and the surface adsorbed state. Scattering calculations of ethanol molecules from a gas phase thermal distribution indicate that the mass accommodation coefficient is 0.98, and the molecules become thermalized within 10 ps of striking the interface. It was determined that the formation of the solvation structure around the ethanol molecule at the interface is not the rate-determining step in its uptake into water droplets. The motion of an ethanol molecule in a water lamella was followed for 30 ns. The time evolution of the probability distribution of finding an ethanol molecule that was initially located at the interface is very well described by the diffusion equation on the free energy surface.

  6. Video-microscopic observation of ionic liquid/alcohol interface and the corresponding molecular simulation study

    NASA Astrophysics Data System (ADS)

    Zhu, Peixi

    This research is aimed at studying the ionic liquid/n-pentanol interface via video-microscopy and molecular dynamic simulations. Understanding the interfacial phenomena and interfacial transport between ionic liquids and other liquids is of interest to the development and application of ionic liquids in a number of areas. One such area is the biphasic hydroformylation of alkenes to obtain alcohol and aldehyde, in which case ionic liquid is the reaction medium where a catalyst resides. The dissolution of an ionic liquid into an alcohol was studied by microscopically observing and measuring the shrinking of a micropipette-produced droplet in real time. Although microscopic investigation of droplet dissolution has been studied before, no attempt had been made to measure the diffusion coefficient D of the droplet species in the surrounding medium. A key finding of this work is that the Epstein-Plesset mathematical model, which describes the dissolution of a droplet/bubble in another fluid medium, can be used to measure D. Other experimental studies of the ionic liquid/alcohol system include electrical conductivity and UV-visible spectroscopy measurements of solutions of 1-hexyl-3-methylimidazolium tetrafluoroborate in n-pentanol. Those experiments were done in order to understand the molecular state of the particular ionic liquid in n-pentanol, as well as obtaining the dissociation constant K of such weak electrolyte solution. The experimental results provide an entry to the assessment of ionic liquid interaction with n-pentanol at molecular scale. Subsequently, molecular dynamics simulation was implemented for the investigation of such interaction. The computation started with simulation of the bulk phase of 1-butyl-3-methylimidazolium tetrafluoroborate, an affine ionic liquid on which molecular simulations had already been reported. A generalized probability based on Fuoss approximation for the closest ion to a distinguished countercharge ion was developed. In

  7. Fully coupled simulation of the plasma liquid interface and interfacial coefficient effects

    NASA Astrophysics Data System (ADS)

    Lindsay, Alexander D.; Graves, David B.; Shannon, Steven C.

    2016-06-01

    There is a growing interest in the study of coupled plasma-liquid systems because of their applications to biomedicine, biological and chemical disinfection, agriculture, and other areas. Optimizing these applications requires a fundamental understanding of the coupling between phases. Though much progress has been made in this regard, there is still more to be done. One area that requires more research is the transport of electrons across the plasma-liquid interface. Some pioneering works (Rumbach et al 2015 Nat. Commun. 6, Rumbach et al 2015 J. Phys. D: Appl. Phys. 48 424001) have begun revealing the near-surface liquid characteristics of electrons. However, there has been little work to determine the near-surface gas phase electron characteristics. Without an understanding of the near-surface gas dynamics, modellers are left to make assumptions about the interfacial conditions. For instance it is commonly assumed that the surface loss or sticking coefficient of gas-phase electrons at the interface is equal to 1. In this work we explore the consequences of this assumption and introduce a couple of ways to think about the electron interfacial condition. In one set of simulations we impose a kinetic condition with varying surface loss coefficient on the gas phase interfacial electrons. In a second set of simulations we introduce a Henry’s law like condition at the interface in which the gas-phase electron concentration is assumed to be in thermodynamic equilibrium with the liquid-phase electron concentration. It is shown that for a range of electron Henry coefficients spanning a range of known hydrophilic specie Henry coefficients, the gas phase electron density in the anode can vary by orders of magnitude. Varying reflection of electrons by the interface also has consequences for the electron energy profile; increasing reflection may lead to increasing thermalization of electrons depending on choices about the electron energy boundary condition. This variation

  8. Break-down of a planar liquid-solid interface during directional solidification - Influence of convection

    NASA Technical Reports Server (NTRS)

    Tewari, S. N.; Chopra, M. A.

    1992-01-01

    The influence of convection on the development of morphological instability at the liquid-solid interface during directional solidification in a positive thermal gradient has been examined in Pb-10 wt pct Sn and succinonitrile-1.9 wt pct acetone. The onset of interfacial breakdown occurs at higher growth speeds in the presence of convection. The linear stability analysis due to Favier and Rouzaud which uses the 'deformable' mass flow boundary layer concept shows a good agreement with the experimentally observed behavior.

  9. Emergent Phenomena in Far-From-Equilibrium Magnetic Granular Ensembles at a Liquid-Air Interface

    NASA Astrophysics Data System (ADS)

    Snezhko, Alexey; Aranson, Igor; Belkin, Maxim

    2009-06-01

    Remarkable nontrivially ordered self-assembled structures are formed in ensembles of magnetic microparticles suspended at a liquid/air interface and energized by an alternating magnetic field. These dynamic structures emerge as a result of a competition between magnetic and hydrodynamic forces. Each structure (snake) is accompanied by a hydrodynamic vortex quadrupole. Under certain conditions snakes spontaneously break the symmetry of surface flows and turn into swimmers. Observed phenomena have been successfully described by a phenomenological model.

  10. Emergent phenomena in far-from-equilibrium magnetic granular ensembles at a liquid-air interface.

    SciTech Connect

    Snezhko, A.; Aranson, I.; Belkin, M.; Materials Science Division

    2009-01-01

    Remarkable nontrivially ordered self-assembled structures are formed in ensembles of magnetic microparticles suspended at a liquid/air interface and energized by an alternating magnetic field. These dynamic structures emerge as a result of a competition between magnetic and hydrodynamic forces. Each structure (snake) is accompanied by a hydrodynamic vortex quadrupole. Under certain conditions snakes spontaneously break the symmetry of surface flows and turn into swimmers. Observed phenomena have been successfully described by a phenomenological model.

  11. Manifestations of non-planar adsorption geometries of lead pyrenocyanine at the liquid-solid interface.

    PubMed

    Mali, Kunal S; Zöphel, Lukas; Ivasenko, Oleksandr; Müllen, Klaus; De Feyter, Steven

    2013-10-01

    In this work, we provide evidence for multiple non-planar adsorption geometries of a novel pyrenocyanine derivative at the liquid-solid interface under ambient conditions. When adsorbed at the organic liquid-solid interface, lead pyrenocyanine forms well-ordered monolayers that exhibit peculiar non-periodic contrast variation. The different contrast of the adsorbed molecules is attributed to dissimilar adsorption geometries which arise from the non-planar conformation of the molecules. The non-planarity of the molecular backbone in turn arises due to a combination of the angularly extended pyrene subunits and the presence of the large lead ion, which is too big to fit inside the central cavity and thus is located out of the aromatic plane. The two possible locations of the lead atom, namely below and above the aromatic plane, could be identified as depression and protrusion in the central cavity, respectively. The manifestation of such multiple adsorption geometries on the structure of the resultant monolayer is discussed in detail. The packing density of these 2D arrays of molecules could be tuned by heating of the sample wherein the molecular packing changes from a low-density, pseudo six-fold symmetric to a high-density, two-fold symmetric arrangement. Finally, a well-ordered two-component system could be constructed by incorporating C60 molecules in the adlayer of lead pyrenocyanine at the liquid-solid interface.

  12. Reduced equations of motion of the interface of dielectric liquids in vertical electric and gravitational fields

    NASA Astrophysics Data System (ADS)

    Kochurin, Evgeny A.; Zubarev, Nikolay M.

    2012-07-01

    The dynamics of the interface between two dielectric fluids in the presence of vertical electric and gravitational fields is studied theoretically. It is shown that, in the particular case where the rate of change of the electric field is proportional to the effective gravitational acceleration, a special flow regime can be realized for which the velocity and electric potentials are linearly dependent functions. This means that there exists a frame of reference in which liquids move along the electric field lines. We derive and analyze the corresponding reduced equations of motion of a liquid-liquid interface. For small density ratio, they turn into the equations describing the Laplacian growth. In the case of two spatial dimensions, we show that these equations determine the asymptotic behavior of the system. For arbitrary density ratios, the Laplacian growth equations adequately describe the initial (weakly nonlinear) stage of the interface instability development. The integrability of these equations makes it possible to investigate the evolution of nonlinear waves at the boundary and, in particular, to demonstrate the tendency to the formation of singularities (cusps).

  13. UV-Vis reflection spectroscopy under variable angle incidence at the air-liquid interface.

    PubMed

    Roldán-Carmona, Cristina; Rubia-Payá, Carlos; Pérez-Morales, Marta; Martín-Romero, María T; Giner-Casares, Juan J; Camacho, Luis

    2014-03-07

    The UV-Vis reflection spectroscopy (UV-Vis-RS) in situ at the air-liquid interface provides information about tilt and aggregation of chromophores in Langmuir monolayers. This information is particularly important given in most cases the chromophore is located at the polar region of the Langmuir monolayer. This region of the Langmuir monolayers has been hardly accessible by other experimental techniques. In spite of its enormous potential, the application of UV-Vis-RS has been limited mainly to reflection measurements under light normal incidence or at lower incidence angles than the Brewster angle. Remarkably, this technique is quite sensitive to the tilt of the chromophores at values of incidence angles close to or larger than the Brewster angle. Therefore, a novel method to obtain the order parameter of the chromophores at the air-liquid interface by using s- and p-polarized radiation at different incidence angles is proposed. This method allowed for the first time the experimental observation of the two components with different polarization properties of a single UV-Vis band at the air-liquid interface. The method of UV-Vis spectroscopy under variable angle incidence is presented as a new tool for obtaining rich detailed information on Langmuir monolayers.

  14. On the Electronic Nature of the Surface Potential at the Vapor-Liquid Interface of Water

    SciTech Connect

    Kathmann, S M; Kuo, I; Mundy, C J

    2008-02-05

    The surface potential at the vapor-liquid interface of water is relevant to many areas of chemical physics. Measurement of the surface potential has been experimentally attempted many times, yet there has been little agreement as to its magnitude and sign (-1.1 to +0.5 mV). We present the first computation of the surface potential of water using ab initio molecular dynamics. We find that the surface potential {chi} = -18 mV with a maximum interfacial electric field = 8.9 x 10{sup 7} V/m. A comparison is made between our quantum mechanical results and those from previous molecular simulations. We find that explicit treatment of the electronic density makes a dramatic contribution to the electric properties of the vapor-liquid interface of water. The E-field can alter interfacial reactivity and transport while the surface potential can be used to determine the 'chemical' contribution to the real and electrochemical potentials for ionic transport through the vapor-liquid interface.

  15. Combined Gravity Gradient and Jitter Accelerations Acting on Liquid-Vapor Interface Oscillations in Reduced Gravity

    NASA Technical Reports Server (NTRS)

    Hung, R. J.; Pan, H. L.

    1995-01-01

    The dynamical behavior of fluids affected by the asymmetric combined gravity gradient and jitter accelerations, in particular the effect of surface tension on partially-filled rotating fluids applicable to a full-scale Gravity Probe-B Spacecraft dewar tank, have been investigated. Three different cases of accelerations, one gravity gradient-dominated, one equally weighted between gravity gradient and jitter, and the others gravity jitter-dominated are studied. Results of slosh wave excitation along the liquid-vapor interface induced by gravity gradient-dominated acceleration indicate that the gravity gradient-dominated acceleration is equivalent to the combined effect of a twisting force and torsional moment acting on the spacecraft. Results of the slosh wave excitation along the liquid vapor interface induced by gravity jitter-dominated acceleration indicate that the gravity jitter-dominated acceleration is equivalent to time-dependent oscillatory forces which push the bubble in the combined directions of down-and-up and sideward -and-middleward as the bubble is rotating with respect to rotating dewar axis. This study discloses the slosh wave excitation along the liquid-vapor interface driven by the combined effects of gravity gradient and jitter accelerations which are two major driving forces affecting the stability of the fluid system in microgravity.

  16. Binary Solvent Organization at Silica/Liquid Interfaces: Preferential Ordering in Acetonitrile-Methanol Mixtures.

    PubMed

    Gobrogge, Eric A; Walker, Robert A

    2014-08-07

    Nonlinear vibrational spectroscopy experiments examined solvent organization at the silica/binary solvent interface where the binary solvent consisted of methanol and acetonitrile in varying mole fractions. Data were compared with surface vibrational spectra acquired from silica surfaces exposed to a vapor phase saturated with the same binary solvent mixtures. Changes in vibrational band intensities suggest that methanol ideally adsorbs to the silica/vapor interface but acetonitrile accumulates in excess relative to vapor-phase composition. At the silica/liquid interface, acetonitrile's signal increases until a solution phase mole fraction of ∼0.85. At higher acetonitrile concentrations, acetonitrile's signal decreases dramatically until only a weak signature persists with the neat solvent. This behavior is ascribed to dipole-paired acetonitrile forming a bilayer with the first sublayer associating with surface silanol groups and a second sublayer consisting of weakly associating, antiparallel partners. On the basis of recent simulations, we propose that the second sublayer accumulates in excess.

  17. Capillary waves at liquid-vapor interfaces: a molecular dynamics simulation.

    PubMed

    Sides, S W; Grest, G S; Lacasse, M D

    1999-12-01

    Evidence for capillary waves at a liquid-vapor interface are presented from extensive molecular dynamics simulations of a system containing up to 1.24 million Lennard-Jones particles. Careful measurements show that the total interfacial width depends logarithmically on L(axially), the length of the simulation cell parallel to the interface, as predicted theoretically. The strength of the divergence of the interfacial width on L(axially) depends inversely on the surface tension gamma. This allows us to measure gamma two ways since gamma can also be obtained from the difference in the pressure parallel and perpendicular to the interface. These two independent measures of gamma agree provided that the interfacial order parameter profile is fit to an error function and not a hyperbolic tangent, as often assumed. We explore why these two common fitting functions give different results for gamma.

  18. Numerical Calculation of the Morphology of a Solid/Liquid Interface Near an Insoluble Particle

    NASA Technical Reports Server (NTRS)

    Catalina, Adrian V.; Stefanescu, Doru M.; Sen, Subhayu

    2003-01-01

    A numerical mathematical model capable of accurately describing the evolution of the shape of the solid/liquid interface in the proximity of a foreign particle is presented in this paper. The model accounts for the influence of the temperature gradient and the Gibbs-Thomson and disjoining pressure effects. It shows that for the systems characterized by k(sub P) < k(sub L) the disjoining pressure causes the interface curvature to change its sign in the close-contact particle/interface region. It also shows that the increase of the temperature gradient diminishes the effect of the disjoining pressure. Calculated critical solidification velocities for the pushing/engulfment transition are compared with experimental measurements performed in microgravity conditions.

  19. Observation of Charge Inversion of an Ionic Liquid at the Solid Salt-Liquid Interface by Sum Frequency Generation Spectroscopy.

    PubMed

    Peñalber, Chariz Y; Baldelli, Steven

    2012-04-05

    Sum frequency generation (SFG) vibrational spectroscopy of the ionic liquid, 1-butyl-3-methylimidazolium dicyanamide [BMIM][DCA], in contact with two different solid salt surfaces, BaF2(111) single crystal and solid NaCl{100}, are discussed in this Letter. This investigation describes the nature of an ionic liquid-(solid) salt interface using SFG, contributing a new understanding to the molecular-level interactions involved in salts, which are conceptually similar compounds (of purely ionic character) but of different physical properties (liquid versus solid at room temperature). Results show the presence of [BMIM](+) at the NaCl{100} surface and [DCA](-) at the BaF2(111) surface. [BMIM](+) cations adhere closely via Coulombic interactions to the negatively charged NaCl{100} surface, while [DCA](-) anions subsequently have a strong electrostatic affinity to the positively charged BaF2(111) surface. Ions of the ionic liquid adsorb to the solid salt surface to form a Helmholtz-like electric double layer.

  20. Two-Phase Model of Liquid-Liquid Interactions With Interface Capturing: Application to Water Assisted Injection Molding

    NASA Astrophysics Data System (ADS)

    Silva, Luisa; Lanrivain, Rodolphe; Zerguine, Walid; Rodriguez-Villa, Andrès; Coupez, Thierry

    2007-05-01

    In this paper, a two phase model to compute liquid-liquid flows is presented. We consider that one phase is a highly viscous thermodependent liquid (polymer phase), whereas the second one is a low viscosity low temperature fluid (water). The first part of this paper concerns capture of the interface between the water and the polymer (or determination of the phase field function). Classical VOF and Level set techniques have been implemented and were ameliorated using mesh adaptation techniques. To accurately determine the velocity field, a two-phase formulation is considered, based in the theory of mixtures, and we introduce a scalar parameter, the phase fraction quantifying the presence of each phase in each point of the computational domain. A friction type coupling between both phases is retained. Using the mixed finite element method within an eulerian framework, we calculate in a single system the whole kinematic variables for both liquids (velocity and pressure of each phase). Results are shown, for 2D and 3D parts.

  1. Density-functional theory of the water liquid-vapour interface

    NASA Astrophysics Data System (ADS)

    Yang, B.; Sullivan, D. E.; Tjipto-Margo, B.; Gray, C. G.

    An extended mean-field density-functional theory of the liquid-vapour interface of water is described. The theory generalizes standard mean-field theories of inhomogeneous molecular fluids by including quadratic orders of the anisotropic component of the intermolecular pair potential in the free energy functional. The pair interaction is modelled by an isotropic plus point dipolar and quadrupolar potential. Analysis shows that dipole-quadrupole coupling terms in the potential are responsible for inducing spontaneous polarization at the liquid-vapour interface. The direction of the surface polarization is determined by the sign of the axial component of the molecular quadrupole tensor, as in the earlier phenomenological theory of Stillinger and Ben-Naim. Explicit calculations are performed using molecular interaction parameters given by the TIP4P potential model for water, employed in recent computer simulations of the water interface by Wilson, Pohorille and Pratt. The preferred molecular orientations at the interface predicted by the theory are analysed in detail and compared with previous simulation results.

  2. Nonlinear internal wave at the interface of two-layer liquid due to a moving hydrofoil

    NASA Astrophysics Data System (ADS)

    Wang, Zhen; Wu, Changhong; Zou, Li; Wang, Qianxi; Ding, Qi

    2017-07-01

    This paper is concerned with the internal wave at the interface of two layers of liquids due to a hydrofoil in the lower layer liquid. The two-layer fluid is assumed moving parallel to the interface at different velocities. The stratified flow is modeled based on the incompressible potential flow theory, with the nonlinear boundary conditions at the interface. Boundary integral equations are formulated for the fully nonlinear interfacial wave generated by the hydrofoil. The numerical model results in a set of nonlinear algebra equations, which are solved using the quasi-Newton method. We show that the quasi-Newton method is more efficient than Newton's method, which is often used for solving these types of equations in the literature. The wave profiles were analyzed in terms of the location and thickness of the hydrofoil, the Froude number, and the ratio of the densities of the two fluids. The computations show that the interfacial wave amplitude showed a trend first of increase and then of decrease with the distance between the hydrofoil and the still interface.

  3. Polymer-polymer and hybrid clay-polymer complexes at liquid-liquid interfaces

    NASA Astrophysics Data System (ADS)

    Wang, Yuhao; Sukhishvili, Svetlana

    2014-03-01

    We report on polymer-polymer and hybrid clay-polymer complex formation at oil-water interfaces. The complexes were composed of poly(methacrylic acid) (PMAA) and poly(N-isopropylacrylamide) (PNIPAM) or PNIPAM modified Laponite (L@PN). Interfacial surface tension, confocal laser scanning microscopy (CLSM) and cryogenic scanning electron microscopy (cryo-SEM) measurements were performed at various ratios of complex components and as a function of solution pH. The results reveal that interfacial PNIPAM/PMAA and L@PN/PMAA complexes are significantly more stable across the pH scale than their solution counterparts, probably because of the suppressed ionization of PMAA at the oil-water interface. In addition, we will discuss the effect of interfacial complex formation on PMAA chain dynamics, as measured by fluorescence-correlation spectroscopy (FCS), and demonstrate the use of these systems to control emulsion stability via changes in solution pH or temperature.

  4. Interaction of magnetic nanoparticles with phospholipid films adsorbed at a liquid/liquid interface.

    PubMed

    Cámara, C I; Monzón, L M A; Coey, J M D; Yudi, L M

    2015-01-07

    The interaction of Co hexagonal magnetic nanoparticles (MNPs) with distearoyl phosphatidyl glycerol (DSPG) and distearoyl phosphatidic acid (DSPA) films adsorbed at a water/1,2-dichloroethane interface is studied employing cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), capacity curves and interfacial pressure-area isotherms. DSPA and DSPG adsorb at the interface forming homogenous films and producing a blocking effect on the transfer process of tetraethyl ammonium (TEA(+)), used as a probe cation. In the presence of Co NPs this effect is reversed and the reversible transfer process for TEA(+) is reestablished, to a greater or lesser extent depending on the structuration of the film. Co-DSPA hybrid films have a homogeneous structure while Co-DSPG films present different domains. Moreover, the presence of Co on DSPA film modifies the partition coefficient of the organic electrolyte into the hydrocarbon layer.

  5. Real Time Characterization of Solid/Liquid Interfaces During Directional Solidification

    NASA Technical Reports Server (NTRS)

    Sen, S.; Kaukler, W. K.; Curreri, P. A.; Peters, P.

    1997-01-01

    A X-Ray Transmission Microscope (XTM) has been developed to observe in real time and in-situ solidification phenomenon at the solid/liquid interface. Recent improvements in the horizontal Bridgman furnace design provides real-time magnification (during solidification) up to 12OX. The increased magnification has enabled for the first time the XTM imaging of real-time growth of fibers and particles with diameters of 3-6 micrometers. Further, morphological transitions from planar to cellular interfaces have also been imaged. Results from recent XTM studies on Al-Bi monotectic system, Al-Au eutectic system and interaction of insoluble particles with s/I interfaces in composite materials will be presented. An important parameter during directional solidification of molten metal is the interfacial undercooling. This parameter controls the morphology and composition at the s/I interface. Conventional probes such as thermocouples, due to their large bead size, do not have sufficient resolution for measuring undercooling at the s/I interface. Further, the intrusive nature of the thermocouples also distorts the thermal field at the s/I interface. To overcome these inherent problems we have recently developed a compact furnace which utilizes a non-intrusive technique (Seebeck) to measure undercooling at the S/I interface. Recent interfacial undercooling measurements obtained for the Pb-Sn system will be presented. The Seebeck measurement furnace in the future will be integrated with the XTM to provide the most comprehensive tool for real time characterization of s/I interfaces during solidification.

  6. A polarized liquid-liquid interface meets visible light-driven catalytic water oxidation.

    PubMed

    Rastgar, Shokoufeh; Pilarski, Martin; Wittstock, Gunther

    2016-09-15

    Hyperbranched nanostructured bismuth vanadate at a chemically polarized water/organic interface is applied for efficient visible light-driven catalytic oxidation of water in the presence of [Co(bpy)3](PF6)3 as an organic soluble electron acceptor. The photocurrent response originating from the transfer of photo-excited electrons in BiVO4 to [Co(bpy)3](3+) is measured by scanning electrochemical microscopy.

  7. UV-Vis Reflection-Absorption Spectroscopy at air-liquid interfaces.

    PubMed

    Rubia-Payá, Carlos; de Miguel, Gustavo; Martín-Romero, María T; Giner-Casares, Juan J; Camacho, Luis

    2015-11-01

    UV-Visible Reflection-Absorption Spectroscopy (UVRAS) technique is reviewed with a general perspective on fundamental and applications. UVRAS is formally identical to IR Reflection-Absorption Spectroscopy (IRRAS), and therefore, the methodology developed for this IR technique can be applied in the UV-visible region. UVRAS can be applied to air-solid, air-liquid or liquid-liquid interfaces. This review focuses on the use of UVRAS for studying Langmuir monolayers. We introduce the theoretical framework for a successful understanding of the UVRAS data, and we illustrate the usage of this data treatment to a previous study from our group comprising an amphiphilic porphyrin. For ultrathin films with a thickness of few nm, UVRAS produces positive or negative bands when p-polarized radiation is used, depending on the incidence angle and the orientation of dipole absorption. UVRAS technique provides highly valuable information on tilt of chromophores at the air-liquid interface, and moreover allows the determination of optical parameters. We propose UVRAS as a powerful technique to investigate the in situ optical properties of Langmuir monolayers. Copyright © 2015 Elsevier B.V. All rights reserved.

  8. Diffusivity and hydrodynamic drag of nanoparticles at a vapor-liquid interface

    NASA Astrophysics Data System (ADS)

    Koplik, Joel; Maldarelli, Charles

    2017-02-01

    Measurements of the surface diffusivity of colloidal spheres translating along a vapor-liquid interface show an unexpected decrease in diffusivity, or increase in surface drag (from the Stokes-Einstein relation), when the particles situate further into the vapor phase. However, direct measurements of the surface drag from the colloid velocity due to an external force find the expected decrease with deeper immersion into the vapor. We perform molecular dynamics simulations of the diffusivity and force experiments for a nanoparticle with a small surface roughness at a vapor-liquid interface to examine the effect of contact line fluctuations. The drag calculated from both calculations agree and decrease as the particle positions further into the vapor. The surface drag is smaller than the bulk liquid drag due to the partial submersion into the liquid and the finite thickness of the interfacial zone relative to the nanoparticle size. We observe weak contact line fluctuations and transient pinning events, but these do not give rise to an anomalous increase in drag in this system.

  9. Preliminary drop-tower experiments on liquid-interface geometry in partially filled containers at zero gravity

    NASA Technical Reports Server (NTRS)

    Smedley, G.

    1990-01-01

    Plexiglass containers with rounded trapezoidal cross sections were designed and built to test the validity of Concus and Finn's existence theorem (1974, 1983) for a bounded free liquid surface at zero gravity. Experiments were carried out at the NASA Lewis two-second drop tower. Dyed ethanol-water solutions and three immiscible liquid pairs, with one liquid dyed, were tested. High-speed movies were used to record the liquid motion. Liquid rose to the top of the smaller end of the containers when the contact angle was small enough, in agreement with the theory. Liquid interface motion demonstrated a strong dependence on physical properties, including surface roughness and contamination.

  10. Designing icephobic surfaces by passively sustaining liquid film at ice-substrate interface

    NASA Astrophysics Data System (ADS)

    Zhao, Tom; Jones, Paul; Patankar, Neelesh

    2016-11-01

    Ice formation poses a significant barrier to transportation, energy generation and transport, gas extraction, etc. We propose to design icephobic surfaces that reduce ice formation and lower ice adhesion by sustaining a film of liquid water at the interface between bulk ice and the substrate. The liquid layer is in phase equilibrium with the surrounding bulk ice, and thus exists without constant energy input. Using molecular dynamic simulations, we show this liquid film can be maintained indefinitely by exploiting the phenomena of interfacial premelting and the freezing point depression of ice confined in surface texture due to the Gibbs Thomson effect. We demonstrate the reduction of both the work and strength of ice adhesion as a function of surface wettability and geometric parameters of the surface texture.

  11. An Interface for the Direct Coupling of Small Liquid Samples to AMS.

    PubMed

    Ognibene, T J; Thomas, A T; Daley, P F; Bench, G; Turteltaub, K W

    2015-10-15

    We describe the moving wire interface attached to the 1-MV AMS system at LLNL's Center for Accelerator Mass Spectrometry for the analysis of nonvolatile liquid samples as either discrete drops or from the direct output of biochemical separatory instrumentation, such as high-performance liquid chromatography. Discrete samples containing at least a few 10s of nanograms of carbon and as little as 50 zmol (14)C can be measured with a 3-5% precision in a few minutes. The dynamic range of our system spans approximately 3 orders in magnitude. Sample to sample memory is minimized by the use of fresh targets for each discrete sample or by minimizing the amount of carbon present in a peak generated by an HPLC containing a significant amount of (14)C. Liquid Sample AMS provides a new technology to expand our biomedical AMS program by enabling the capability to measure low-level biochemicals in extremely small samples that would otherwise be inaccessible.

  12. Shape-Selectivity with Liquid Crystal and Side-Chain Liquid Crystalline Polymer SAW Sensor Interfaces

    SciTech Connect

    FRYE-MASON,GREGORY CHARLES; OBORNY,MICHAEL C.; PUGH,COLEEN; RICCO,ANTONIO; THOMAS,ROSS C.; ZELLERS,EDWARD T.; ZHANG,GUO-ZHENG

    1999-09-23

    A liquid crystal (LC) and a side-chain liquid crystalline polymer (SCLCP) were tested as surface acoustic wave (SAW) vapor sensor coatings for discriminating between pairs of isomeric organic vapors. Both exhibit room temperature smectic mesophases. Temperature, electric-field, and pretreatment with self-assembled monolayers comprising either a methyl-terminated or carboxylic acid-terminated alkane thiol anchored to a gold layer in the delay path of the sensor were explored as means of affecting the alignment and selectivity of the LC and SCLCP films. Results for the LC were mixed, while those for the SCLCP showed a consistent preference for the more rod-like isomer of each isomer pair examined.

  13. Viscoelasticity measurement of gel formed at the liquid-liquid reactive interfaces

    NASA Astrophysics Data System (ADS)

    Ujiie, Tomohiro

    2012-11-01

    We have experimentally studied a reacting liquid flow with gel formation by using viscous fingering (VF) as a flow field. Here, two systems were employed. In one system, sodium polyacrylate (SPA) solution and ferric ion solution were used as the more and less viscous liquids, respectively. In another system, xthantan gum (XG) solution and the ferric ion solution were used as the more and less viscous liquids, respectively. We showed that influence of gel formation on VF were qualitatively different in these two systems. We consider that the difference in the two systems will be caused by the difference in the properties of the gels. Therefore, we have measured the rheological properties of the gels by means of a rheometer. In the present study, viscoelasticity measurement was performed by two methods. One is the method which uses Double Wall Ring sensor (TA instrument) and another is the method using parallel plate. In both viscoelasticity measurements, the behavior of the formed gel was qualitatively consistent. We have found that the gel in the SPA system shows viscoelastic fluid like behavior. Moreover, we have found that the gel in the XG system shows solid like behavior.

  14. A model of blind zone for in situ monitoring the solid/liquid interface using ultrasonic wave.

    PubMed

    Peng, Song; Ouyang, Qi; Zhu, Z Z; Zhang, X L

    2015-07-01

    To in situ monitor a solid/liquid interface to control metal qualities, the paper analysis blind models of the ultrasonic propagation in the solidifying molten metal with a solid/liquid interface in the Bridgman type furnace, and a mathematical calculation model of blind zone with different source locations and surface concavities is built. The study points out that the blind zone I is caused by ray bending in the interface edge, and the blind zone II is caused by totally reflection which is related with initial ray angle, critical refraction angle of solid/liquid media. A serial of simulation experiments are operated on the base of the model, and numerical computation results coincide with model calculated results very well. Therefore, receiver should locate beyond these blind zones in the right boundary to obtain time of flight data which is used to reconstruct the solid/liquid interface.

  15. Bottom-up assembly of high density molecular nanowire cross junctions at a solid/liquid interface.

    PubMed

    Lei, Shengbin; Puigmartí-Luis, Josep; Minoia, Andrea; Van der Auweraer, Mark; Rovira, Concepció; Lazzaroni, Roberto; Amabilino, David B; De Feyter, Steven

    2008-02-14

    A monoalkylated tetrathiafulvalene derivative forms multilayer structures at the solid-liquid interface, with high density of cross junctions, which are interesting for molecular electronic circuit self-assembly.

  16. Disruption of E. coli amyloid-integrated biofilm formation at the air-liquid interface by a polysorbate surfactant

    PubMed Central

    Wu, Cynthia; Lim, Ji Youn; Fuller, Gerald G.; Cegelski, Lynette

    2013-01-01

    Functional amyloid fibers termed curli contribute to bacterial adhesion and biofilm formation in E. coli. We discovered that the nonionic surfactant Tween 20 inhibits biofilm formation by uropathogenic E. coli at the air-liquid interface, referred to as pellicle formation, and at the solid-liquid interface. At Tween 20 concentrations near and above the critical micelle concentration, the interfacial viscoelastic modulus is reduced to zero as cellular aggregates at the air-liquid interface are locally disconnected and eventually eliminated. Tween 20 does not inhibit the production of curli, but prevents curli-integrated film formation. Our results support a model in which the hydrophobic curli fibers associated with bacteria near the air-liquid interface require access to the gas phase to formed strong physical entanglements and to form a network that can support shear stress. PMID:23259693

  17. Influence of Simple Electrolytes on the Orientational Ordering of Thermotropic Liquid Crystals at Aqueous Interfaces

    PubMed Central

    Carlton, Rebecca J.; Gupta, Jugal K.; Swift, Candice L.; Abbott, Nicholas L.

    2011-01-01

    We report orientational anchoring transitions at aqueous interfaces of a water-immiscible, thermotropic liquid crystal (LC; nematic phase of 4′-pentyl-4-cyanobiphenyl) that are induced by changes in pH of the aqueous solution and the addition of simple electrolytes (NaCl) to the aqueous phase. Whereas measurements of the zeta potential on the aqueous side of the interface of LC-in-water emulsions prepared with 5CB confirm pH-dependent formation of an electrical double layer extending into the aqueous phase, quantification of the orientational ordering of the LC leads to the proposition that an electrical double layer is also formed on the LC-side of the interface with an internal electric field that drives the LC anchoring transition. Further support for this conclusion is obtained from measurements of the dependence of LC ordering on pH and ionic strength, as well as a simple model based on the Poisson-Boltzmann equation from which we calculate the contribution of an electrical double layer to the orientational anchoring energy of the LC. Overall, the results presented herein provide new fundamental insights into ionic phenomena at LC-aqueous interfaces, and expand the range of solutes known to cause orientational anchoring transitions at LC-aqueous interfaces beyond previously examined amphiphilic adsorbates. PMID:22106820

  18. Systematic Approach to Electrostatically Induced 2D Crystallization of Nanoparticles at Liquid Interfaces

    SciTech Connect

    Fukuto, M.; Kewalramani, S.; Wang, S.; Lin, Y.; Nguyen, G.; Wang, Q.; Yang, L.

    2011-02-07

    We report an experimental demonstration of a strategy for inducing two-dimensional (2D) crystallization of charged nanoparticles on oppositely charged fluid interfaces. This strategy aims to maximize the interfacial adsorption of nanoparticles, and hence their lateral packing density, by utilizing a combination of weakly charged particles and a high surface charge density on the planar interface. In order to test this approach, we investigated the assembly of cowpea mosaic virus (CPMV) on positively charged lipid monolayers at the aqueous solution surface, by means of in situ X-ray scattering measurements at the liquid-vapor interface. The assembly was studied as a function of the solution pH, which was used to vary the charge on CPMV, and of the mole fraction of the cationic lipid in the binary lipid monolayer, which set the interface charge density. The 2D crystallization of CPMV occurred in a narrow pH range just above the particle's isoelectric point, where the particle charge was weakly negative, and only when the cationic-lipid fraction in the monolayer exceeded a threshold. The observed 2D crystals exhibited nearly the same packing density as the densest lattice plane within the known 3D crystals of CPMV. The above electrostatic approach of maximizing interfacial adsorption may provide an efficient route to the crystallization of nanoparticles at aqueous interfaces.

  19. Self-assembly of microscopic chiplets at a liquid-liquid-solid interface forming a flexible segmented monocrystalline solar cell.

    PubMed

    Knuesel, Robert J; Jacobs, Heiko O

    2010-01-19

    This paper introduces a method for self-assembling and electrically connecting small (20-60 micrometer) semiconductor chiplets at predetermined locations on flexible substrates with high speed (62500 chips/45 s), accuracy (0.9 micrometer, 0.14 degrees), and yield (> 98%). The process takes place at the triple interface between silicone oil, water, and a penetrating solder-patterned substrate. The assembly is driven by a stepwise reduction of interfacial free energy where chips are first collected and preoriented at an oil-water interface before they assemble on a solder-patterned substrate that is pulled through the interface. Patterned transfer occurs in a progressing linear front as the liquid layers recede. The process eliminates the dependency on gravity and sedimentation of prior methods, thereby extending the minimal chip size to the sub-100 micrometer scale. It provides a new route for the field of printable electronics to enable the integration of microscopic high performance inorganic semiconductors on foreign substrates with the freedom to choose target location, pitch, and integration density. As an example we demonstrate a fault-tolerant segmented flexible monocrystalline silicon solar cell, reducing the amount of Si that is used when compared to conventional rigid cells.

  20. Permselective Ion Transport Across the Nanoscopic Liquid/Liquid Interface Array.

    PubMed

    Huang, Xiao; Xie, Lisiqi; Lin, Xingyu; Su, Bin

    2016-06-21

    Free-standing silica nanochannel membrane (SNM) with perforated channels was utilized to create arrays of nanoscale interfaces between two immiscible electrolyte solutions (nano-ITIES), at which permselective ion transfer and detection were achieved. The SNM consisted of a high density of straight nanochannels with a diameter of 2-3 nm and a length of 70 nm. The silicon wafer coated by 150 nm-thick porous silicon nitride film (p-SiNF) with pores of 5 μm-in-diameter was used to support the SNM in a form of nanochannel-on-micropore. Considering the material surface lipophilicity, the nano-ITIES array was formed at the boundary between SNM and p-SiNF, with a diffusion geometry equivalent to two back-to-back inlaid microdisc interfaces. Thus, the transfer of tetraethylammonium (TEA(+)) across the nano-ITIES array yielded symmetric sigmoidal current responses. In addition, because of the ultrasmall size and negatively charged surface of silica nanochannels, the nano-ITIES displayed obvious size and charge permselectivities. Transfer of ions with a size comparable with or larger than the nanochannel was sterically blocked. Also that of anions with a size smaller than the nanochannels encountered the strong electrostatic repulsion from channel walls, showing obvious dependence on the ionic strength of aqueous solution. The present approach is facile and inexpensive for building a nano-ITIES array with potential applications in ion detection and separation.

  1. Stability analysis of the interface between two weak viscoelastic liquids under periodic oscillations

    NASA Astrophysics Data System (ADS)

    Garcia-Gonzalez, Sergio; Fernandez-Feria, Ramon

    2017-01-01

    We consider the motion and the linear hydrodynamic instabilities of two immiscible viscoelastic liquids above a horizontal solid surface induced by the periodic oscillations of the horizontal plate along its plane. A planar interface, parallel to the oscillating plate, separates the lower layer from the other viscoelastic fluid that extends vertically to infinity. The two-dimensional motion of these fluids is studied together with the conditions under which the flow becomes unstable, deforming the planar interface and promoting the mixing of both liquids. The study extends the previous work by Isakova et al. ["A model for the linear stability of the interface between aqueous humor and vitreous substitutes after vitreoretinal surgery," Phys. Fluids 26, 124101 (2014)] by considering non-Newtonian fluids, particularly liquids with weak viscoelasticity (neglecting normal stress differences), which may model more accurately the physical behavior of the aqueous humor and, especially, the vitreous humour substitute in the vitreous chamber of the eye after vitrectomy. A novel approach to the quasi-steady stability analysis of unsteady flows of Maxwell liquids is developed in the present paper. We focus on the effect of the small Deborah numbers on the motion and on the hydrodynamic instability of the two fluids as the other non-dimensional parameters are varied within the range of interest for the biofluiddynamics of the eye. The special case in which the lower layer modelling the aqueous humor is a Newtonian liquid and the upper vitreous substitute is a Maxwell liquid is considered with detail. We find that, even for a very small Deborah number of the vitreous substitute, the dynamics and the hydrodynamic stability of the two fluids can be qualitatively very different to the Newtonian case, especially as the viscosity ratio is varied, showing that weak viscoelasticity may change dramatically the dynamics of the eye. An exhaustive characterization of the influence of the

  2. Structural ordering at solid-liquid interfaces in Al-Sm system: A molecular-dynamics study

    SciTech Connect

    Sun, Yang; Zhang, Feng; Ye, Zhuo; Ding, Zejun; Mendelev, Mikhail I.; Kramer, Matthew J.; Wang, Cai -Zhuang; Ho, Kai -Ming

    2016-07-12

    The structural ordering at solid-liquid interfaces far from equilibrium is studied with molecular dynamics simulations for the Al-Sm system. Using the van-Hove self-correlation function as the criterion to identify attachment/detachment events that occur at the interface, we are able to determine the time-dependent interface position, and characterize the detailed interfacial structure ordering surrounding the attached atoms. For the interface between an undercooled Al90Sm10 liquid and a metastable cubic structure, the solid induces the crystalline order of the cubic phase in the liquid layers, promoting the continuous growth of the crystal phase. When the same liquid is put in contact with f.c.c. Al, Sm from the liquid can still attach to the solid interface despite its insolubility in the Al lattice. Non-f.c.c. order is revealed surrounding the attached Sm atoms. Lastly, we show that the local structure ordering at interface is highly correlated to solid packing and liquid ordering.

  3. Structural ordering at solid-liquid interfaces in Al-Sm system: A molecular-dynamics study

    DOE PAGES

    Sun, Yang; Zhang, Feng; Ye, Zhuo; ...

    2016-07-12

    The structural ordering at solid-liquid interfaces far from equilibrium is studied with molecular dynamics simulations for the Al-Sm system. Using the van-Hove self-correlation function as the criterion to identify attachment/detachment events that occur at the interface, we are able to determine the time-dependent interface position, and characterize the detailed interfacial structure ordering surrounding the attached atoms. For the interface between an undercooled Al90Sm10 liquid and a metastable cubic structure, the solid induces the crystalline order of the cubic phase in the liquid layers, promoting the continuous growth of the crystal phase. When the same liquid is put in contact withmore » f.c.c. Al, Sm from the liquid can still attach to the solid interface despite its insolubility in the Al lattice. Non-f.c.c. order is revealed surrounding the attached Sm atoms. Lastly, we show that the local structure ordering at interface is highly correlated to solid packing and liquid ordering.« less

  4. Surface thermodynamics of planar, cylindrical, and spherical vapour-liquid interfaces of water.

    PubMed

    Lau, Gabriel V; Ford, Ian J; Hunt, Patricia A; Müller, Erich A; Jackson, George

    2015-03-21

    The test-area (TA) perturbation approach has been gaining popularity as a methodology for the direct computation of the interfacial tension in molecular simulation. Though originally implemented for planar interfaces, the TA approach has also been used to analyze the interfacial properties of curved liquid interfaces. Here, we provide an interpretation of the TA method taking the view that it corresponds to the change in free energy under a transformation of the spatial metric for an affine distortion. By expressing the change in configurational energy of a molecular configuration as a Taylor expansion in the distortion parameter, compact relations are derived for the interfacial tension and its energetic and entropic components for three different geometries: planar, cylindrical, and spherical fluid interfaces. While the tensions of the planar and cylindrical geometries are characterized by first-order changes in the energy, that of the spherical interface depends on second-order contributions. We show that a greater statistical uncertainty is to be expected when calculating the thermodynamic properties of a spherical interface than for the planar and cylindrical cases, and the evaluation of the separate entropic and energetic contributions poses a greater computational challenge than the tension itself. The methodology is employed to determine the vapour-liquid interfacial tension of TIP4P/2005 water at 293 K by molecular dynamics simulation for planar, cylindrical, and spherical geometries. A weak peak in the curvature dependence of the tension is observed in the case of cylindrical threads of condensed liquid at a radius of about 8 Å, below which the tension is found to decrease again. In the case of spherical drops, a marked decrease in the tension from the planar limit is found for radii below ∼ 15 Å; there is no indication of a maximum in the tension with increasing curvature. The vapour-liquid interfacial tension tends towards the planar limit for large

  5. A Molecular Dynamics Study on the Local Structure of Liquid-Vapor Interface of Water and L-J Fluid

    NASA Astrophysics Data System (ADS)

    Kikugawa, Gota; Takagi, Shu; Matsumoto, Yoichiro; Ohara, Taku

    Microscopic structures of a liquid-vapor interface are investigated by molecular dynamics simulations. In the previous studies, we proposed the local and instantaneous definition of the interface at the molecular level, which can capture the thermal fluctuation of the interface. By using this definition, the layering structure of water molecules at the interface was found, in other words, the structurization phenomena of water at the molecular level were clearly seen as usually found at the liquid-solid interface. In this study, we investigated the liquid-vapor interface of Lenard-Jones fluid. The effect of well depth of L-J potential parameter on the structure was also studied. Although the structurization was found at the L-J fluid as well as water, characteristic of this structure was clearly different from that of water. We consider that the difference is ascribed to the intrinsic structure of liquid and associative trend of molecules. We also discussed the anisotropic characteristics of the molecular diffusion at the interface. The anisotropy of the translational diffusion at the interface of water is stronger than that of the L-J fluid.

  6. Evidence of contact epitaxy in the self-assembly of HgSe nanocrystals formed at a liquid-liquid interface.

    PubMed

    Maiti, Santanu; Sanyal, Milan K; Jana, Manoj K; Runge, Benjamin; Murphy, Bridget M; Biswas, Kanishka; Rao, C N R

    2017-03-08

    The grazing incidence x-ray scattering results presented here show that the self-assembly process of HgSe nanocrystals formed at a liquid-liquid interface is quite different along the in-plane direction and across the interface. In situ x-ray reflectivity and ex situ microscopy measurements suggest quantized out-of-plane growth for HgSe nanoparticles of a size of about [Formula: see text] nm initially. Grazing incidence small-angle x-ray scattering measurements for films transferred from the water-toluene interface at various stages of reaction show that these nanoparticles first form random clusters with an average radius of 2.2 nm, giving rise to equally spaced rings of several orders. Finally, these clusters self-organize into face-centered cubic superstructures, giving sharp x-ray diffraction peaks oriented normal to the liquid-liquid interface with more than 100 nm-coherent domains. We also observed the x-ray diffraction pattern of the HgSe crystalline phase, with the superlattice peaks in these grazing incidence measurements of the transferred films. The electron microscopy and atomic force microscopy results support the x-ray observation of the self-organization of HgSe nanocrystals into close-packed superlattices. These results show that capillary wave fluctuation promotes the oriented attachment of clusters at the liquid-liquid interface, giving direct experimental evidence of contact epitaxy.

  7. Topological defects in electric double layers of ionic liquids at carbon interfaces

    SciTech Connect

    Black, Jennifer M.; Okatan, Mahmut Baris; Feng, Guang; Cummings, Peter T.; Kalinin, Sergei V.; Balke, Nina

    2015-06-07

    The structure and properties of the electrical double layer in ionic liquids is of interest in a wide range of areas including energy storage, catalysis, lubrication, and many more. Theories describing the electrical double layer for ionic liquids have been proposed, however a full molecular level description of the double layer is lacking. To date, studies have been predominantly focused on ion distributions normal to the surface, however the 3D nature of the electrical double layer in ionic liquids requires a full picture of the double layer structure not only normal to the surface, but also in plane. Here we utilize 3D force mapping to probe the in plane structure of an ionic liquid at a graphite interface and report the direct observation of the structure and properties of topological defects. The observation of ion layering at structural defects such as step-edges, reinforced by molecular dynamics simulations, defines the spatial resolution of the method. Observation of defects allows for the establishment of the universality of ionic liquid behavior vs. separation from the carbon surface and to map internal defect structure. In conclusion, these studies offer a universal pathway for probing the internal structure of topological defects in soft condensed matter on the nanometer level in three dimensions.

  8. Topological defects in electric double layers of ionic liquids at carbon interfaces

    DOE PAGES

    Black, Jennifer M.; Okatan, Mahmut Baris; Feng, Guang; ...

    2015-06-07

    The structure and properties of the electrical double layer in ionic liquids is of interest in a wide range of areas including energy storage, catalysis, lubrication, and many more. Theories describing the electrical double layer for ionic liquids have been proposed, however a full molecular level description of the double layer is lacking. To date, studies have been predominantly focused on ion distributions normal to the surface, however the 3D nature of the electrical double layer in ionic liquids requires a full picture of the double layer structure not only normal to the surface, but also in plane. Here wemore » utilize 3D force mapping to probe the in plane structure of an ionic liquid at a graphite interface and report the direct observation of the structure and properties of topological defects. The observation of ion layering at structural defects such as step-edges, reinforced by molecular dynamics simulations, defines the spatial resolution of the method. Observation of defects allows for the establishment of the universality of ionic liquid behavior vs. separation from the carbon surface and to map internal defect structure. In conclusion, these studies offer a universal pathway for probing the internal structure of topological defects in soft condensed matter on the nanometer level in three dimensions.« less

  9. Electrochemical Sensing and Imaging Based on Ion Transfer at Liquid/Liquid Interfaces

    PubMed Central

    Amemiya, Shigeru; Kim, Jiyeon; Izadyar, Anahita; Kabagambe, Benjamin; Shen, Mei; Ishimatsu, Ryoichi

    2013-01-01

    Here we review the recent applications of ion transfer (IT) at the interface between two immiscible electrolyte solutions (ITIES) for electrochemical sensing and imaging. In particular, we focus on the development and recent applications of the nanopipet-supported ITIES and double-polymer-modified electrode, which enable the dynamic electrochemical measurements of IT at nanoscopic and macroscopic ITIES, respectively. High-quality IT voltammograms are obtainable using either technique to quantitatively assess the kinetics and dynamic mechanism of IT at the ITIES. Nanopipet-supported ITIES serves as an amperometric tip for scanning electrochemical microscopy to allow for unprecedentedly high-resolution electrochemical imaging. Voltammetric ion sensing at double-polymer-modified electrodes offers high sensitivity and unique multiple-ion selectivity. The promising future applications of these dynamic approaches for bioanalysis and electrochemical imaging are also discussed. PMID:24363454

  10. Photocurrents at polarized liquid|liquid interfaces enhanced by a gold nanoparticle film.

    PubMed

    Schaming, Delphine; Hojeij, Mohamad; Younan, Nathalie; Nagatani, Hirohisa; Lee, Hye Jin; Girault, Hubert H

    2011-10-21

    Photocurrent responses associated with the interfacial quenching of the photo-excited water-soluble zinc meso-tetra(4-carboxyphenyl)porphyrin (ZnTPPC) by ferrocene have been studied at a water|1,2-dichloroethane interface in the absence and in the presence of adsorbed gold nanoparticles. Upon addition of methanol, a mirror-like gold film is formed and an important enhancement of the photocurrent response can be observed. Intensity modulated photocurrent spectroscopy experiments (IMPS) have been performed, in order to deconvolute in the frequency domain the contribution from the competition between the recombination and the product separation arising after the electron transfer, and the attenuation associated with the resistance and interfacial capacitance (RC(int)) time constant of the cell. This journal is © the Owner Societies 2011

  11. Nanocrystalline Janus films of inorganic materials prepared at the liquid-liquid interface.

    PubMed

    Biswas, Kanishka; Rao, C N R

    2009-05-01

    The interface between toluene and water has been employed to prepare ultrathin Janus nanocrystalline films of metal oxides, metal chalcogenides and gold, wherein the surface on the organic-side is hydrophobic and the aqueous-side is hydrophilic. We have changed the nature of the metal precursor or capping agent in the organic layer to increase the hydrophobicity. The strategy employed for this purpose is to increase the length of the alkane chain in the precursor or use a perfluroalkane derivative as precursor or as a capping agent. The hydrophobicity and hydrophilicity of the Janus films have been determined by contact angle measurements. The morphology of hydrophobic and hydrophilic sides of the film have been examined by field emission scanning electron microscopy.

  12. Crystallization induced block copolymer assembly at curved liquid-liquid interface

    NASA Astrophysics Data System (ADS)

    Qi, Hao; Zhou, Tian; Zhou, Hao; Li, Christopher; Soft Materials Lab Team

    In a selected solvent, amphiphilic block copolymers can self-assemble into various micelle structures which find widespread applications in nanomedicine. Herein we report a directed assembly of poly (l-lactide acid)-b-poly (ethylene glycol) (PLLA-b-PEG) at curved oil/water interfaces. Oil droplets were dispersed in water phase upon sonication with amphiphilic PLLA-b-PEG as the surfactant. Subsequent crystallization of PLLA segments resulted in the formation of lamellasomes consisting of crystalline PLLA shell and densely-grafted (approx.1chain/nm2) PEG layer. The structure, morphology, and mechanical properties of these unique polymer ensembles were investigated using transmission electron microscopy and atomic force microscopy. Detailed formation mechanism will be discussed in detail.

  13. Molecular simulation of fluid mixtures in bulk and at solid-liquid interfaces

    NASA Astrophysics Data System (ADS)

    Kern, Jesse L.

    The properties of a diverse range of mixture systems at interfaces are investigated using a variety of computational techniques. Molecular simulation is used to examine the thermodynamic, structural, and transport properties of heterogeneous systems of theoretical and practical importance. The study of binary hard-sphere mixtures at a hard wall demonstrates the high accuracy of recently developed classical-density functionals. The study of aluminum--gallium solid--liquid heterogeneous interfaces predicts a significant amount of prefreezing of the liquid by adopting the structure of the solid surface. The study of ethylene-expanded methanol within model silica mesopores shows the effect of confinement and surface functionalzation on the mixture composition and transport inside of the pores. From our molecular-dynamics study of binary hard-sphere fluid mixtures at a hard wall, we obtained high-precision calculations of the wall-fluid interfacial free energies, gamma. We have considered mixtures of varying diameter ratio, alpha = 0.7,0.8,0.9; mole fraction, x 1 = 0.25,0.50,0.75; and packing fraction, eta < 0.50. Using Gibbs-Cahn Integration, gamma is calculated from the system pressure, chemical potentials, and density profiles. Recent classical density-functional theory predictions agree very well with our results. Structural, thermodynamic, and transport properties of the aluminum--gallium solid--liquid interface at 368 K are obtained for the (100), (110), and (111) orientations using molecular dynamics. Density, potential energy, stress, and diffusion profiles perpendicular to the interface are calculated. The layers of Ga that form on the Al surface are strongly adsorbed and take the in-plane structure of the underlying crystal layers for all orientations, which results in significant compressive stress on the Ga atoms. Bulk methanol--ethylene mixtures under vapor-liquid equilibrium conditions have been characterized using Monte Carlo and molecular dynamics. The

  14. Solid mesostructured polymer-surfactant films at the air-liquid interface.

    PubMed

    Pegg, Jonathan C; Eastoe, Julian

    2015-08-01

    Pioneering work by Edler et al. has spawned a new sub-set of mesostructured materials. These are solid, self-supporting films comprising surfactant micelles encased within polymer hydrogel; composite polymer-surfactant films can be grown spontaneously at the air-liquid interface and have defined and controllable mesostructures. Addition of siliconalkoxide to polymer-surfactant mixtures allows for the growth of mesostructured hybrid polymer-surfactant silica films that retain film geometry after calcinations and exhibit superior mechanical properties to typically brittle inorganic films. Growing films at the air-liquid interface provides a rapid and simple means to prepare ordered solid inorganic films, and to date the only method for generating mesostructured films thick enough (up to several hundred microns) to be removed from the interface. Applications of these films could range from catalysis to encapsulation of hydrophobic species and drug delivery. Film properties and mesostructures are sensitive to surfactant structure, polymer properties and polymer-surfactant phase behaviour: herein it will be shown how film mesostructure can be tailored by directing these parameters, and some interesting analogies will be drawn with more familiar mesostructured silica materials.

  15. A novel method for pulmonary research: assessment of bioenergetic function at the air-liquid interface.

    PubMed

    Xu, Weiling; Janocha, Allison J; Leahy, Rachel A; Klatte, Ryan; Dudzinski, Dave; Mavrakis, Lori A; Comhair, Suzy A A; Lauer, Mark E; Cotton, Calvin U; Erzurum, Serpil C

    2014-01-01

    Air-liquid interface cell culture is an organotypic model for study of differentiated functional airway epithelium in vitro. Dysregulation of cellular energy metabolism and mitochondrial function have been suggested to contribute to airway diseases. However, there is currently no established method to determine oxygen consumption and glycolysis in airway epithelium in air-liquid interface. In order to study metabolism in differentiated airway epithelial cells, we engineered an insert for the Seahorse XF24 Analyzer that enabled the measure of respiration by oxygen consumption rate (OCR) and glycolysis by extracellular acidification rate (ECAR). Oxidative metabolism and glycolysis in airway epithelial cells cultured on the inserts were successfully measured. The inserts did not affect the measures of OCR or ECAR. Cells under media with apical and basolateral feeding had less oxidative metabolism as compared to cells on the inserts at air-interface with basolateral feeding. The design of inserts that can be used in the measure of bioenergetics in small numbers of cells in an organotypic state may be useful for evaluation of new drugs and metabolic mechanisms that underlie airway diseases.

  16. Hematite(001)-liquid water interface from hybrid density functional-based molecular dynamics

    SciTech Connect

    von Rudorff, Guido Falk; Jakobsen, Rasmus; Rosso, Kevin M.; Blumberger, Jochen

    2016-07-28

    The atom-scale characterisation of interfaces between transition metal oxides and liquid water is fundamental to our mechanistic understanding of diverse phenomena ranging from crystal growth to biogeochemical transformations to solar fuel production. Here we report on the results of large-scale hybrid density functional theory-based molecular dynamics simulations for the hematite(001)-liquid water interface. A specific focus is placed on understanding how different terminations of the same surface influence surface solvation. We find that the two dominant terminations for the hematite(001) surface exhibit strong differences both in terms of the active species formed on the surface and the strength of surface solvation. According to present simulations, we find that charged oxyanions (-O-) and doubly protonated oxygens (-OH$_{2}^{+}$ ) can be formed on the iron terminated layer via autoionization of neutral -OH groups. No such charged species are found for the oxygen terminated surface. In addition, the missing iron sublayer in the iron terminated surface strongly influences the solvation structure, which becomes less well ordered in the vicinity of the interface. These pronounced differences are likely to affect the reactivity of the two surface terminations, and in particular the energetics of excess charge carriers at the surface.

  17. Hematite(001)-liquid water interface from hybrid density functional-based molecular dynamics

    NASA Astrophysics Data System (ADS)

    Falk von Rudorff, Guido; Jakobsen, Rasmus; Rosso, Kevin M.; Blumberger, Jochen

    2016-10-01

    The atom-scale characterisation of interfaces between transition metal oxides and liquid water is fundamental to our mechanistic understanding of diverse phenomena ranging from crystal growth to biogeochemical transformations to solar fuel production. Here we report on the results of large-scale hybrid density functional theory-based molecular dynamics simulations for the hematite(001)-liquid water interface. A specific focus is placed on understanding how different terminations of the same surface influence surface solvation. We find that the two dominant terminations for the hematite(001) surface exhibit strong differences both in terms of the active species formed on the surface and the strength of surface solvation. According to present simulations, we find that charged oxyanions (-O-) and doubly protonated oxygens (-OH2+ ) can be formed on the iron terminated layer via autoionization of neutral -OH groups. No such charged species are found for the oxygen terminated surface. In addition, the missing iron sublayer in the iron terminated surface strongly influences the solvation structure, which becomes less well ordered in the vicinity of the interface. These pronounced differences are likely to affect the reactivity of the two surface terminations, and in particular the energetics of excess charge carriers at the surface.

  18. The vapour-liquid interface for a Lennard-Jones model of argon-krypton mixtures

    NASA Astrophysics Data System (ADS)

    Lee, D. J.; Telo da Gama, M. M.; Gubbins, K. E.

    We report a molecular dynamics study of the planar vapour-liquid interface for mixtures of Ar and Kr modelled by truncated Lennard-Jones potentials at 115·77 K and at two compositions. The simulations yield the density profiles, surface tension, surface of tension, adsorption, and normal and transverse components of the pressure tensor. Both the Irving-Kirkwood (IK) and Harasima (H) forms of the pressure tensor are calculated. The values of the surface tension calculated by the thermodynamic and mechanical (for both the IK and H pressure tensors) routes are in agreement, but the IK and H pressure tensors yield different values for the surface of tension, as expected. These results are compared with predictions of the mean field theory (MFT) of the interface. The agreement is generally good, the principal differences being due to the fact that the MFT predicts too low a liquid density. The MFT is also used to predict properties of the mixture interface for the full Lennard-Jones potential. For low concentrations of argon, the argon density profile is predicted to be weakly non-monotonic; this effect is larger for the full than for the truncated Lennard-Jones potential.

  19. A fully automated liquid–liquid extraction system utilizing interface detection

    PubMed Central

    Maslana, Eugene; Schmitt, Robert; Pan, Jeffrey

    2000-01-01

    The development of the Abbott Liquid-Liquid Extraction Station was a result of the need for an automated system to perform aqueous extraction on large sets of newly synthesized organic compounds used for drug discovery. The system utilizes a cylindrical laboratory robot to shuttle sample vials between two loading racks, two identical extraction stations, and a centrifuge. Extraction is performed by detecting the phase interface (by difference in refractive index) of the moving column of fluid drawn from the bottom of each vial containing a biphasic mixture. The integration of interface detection with fluid extraction maximizes sample throughput. Abbott-developed electronics process the detector signals. Sample mixing is performed by high-speed solvent injection. Centrifuging of the samples reduces interface emulsions. Operating software permits the user to program wash protocols with any one of six solvents per wash cycle with as many cycle repeats as necessary. Station capacity is eighty, 15 ml vials. This system has proven successful with a broad spectrum of both ethyl acetate and methylene chloride based chemistries. The development and characterization of this automated extraction system will be presented. PMID:18924693

  20. Photodissociation of ICN at the liquid/vapor interface of water

    NASA Astrophysics Data System (ADS)

    Winter, Nicole; Benjamin, Ilan

    2004-08-01

    The photodissociation of ICN adsorbed at the liquid/vapor interface of water is studied using classical molecular dynamics with nonadiabatic surface hopping. The cage escape, geminate recombination to form ICN and INC and the subsequent vibrational relaxation of these two molecules (on their ground electronic states) is compared with the same process in bulk water and with previous photodissociation studies at liquid interfaces. We find that the reduced surface density and weaker solvent-solute interactions give rise to reduced rate of nonadiabatic transitions and that the probability for cage escape at the interface is significantly enhanced due to the possibility that one or both of the photodissociation fragments desorb into the gas phase. The overall desorption probability varies from 75% to 92% for ICN initially located just below the Gibbs surface (50% bulk density) to ICN located just above the Gibbs surface, respectively. The corresponding geminate recombination probabilities are 18% and 9%, respectively. The vibrational relaxation rate of the recombined ICN is slower than in the bulk by a factor of 2.3.