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Surfaces, Volume 1, Issue 1 (December 2018)

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Open AccessArticle Disjoining Pressure Derived from the Lennard–Jones Potential, Diffusion Equation, and Diffusion Coefficient for Submonolayer Liquid Film
Surfaces 2018, 1(1), 122-137; https://doi.org/10.3390/surfaces1010010
Received: 1 October 2018 / Revised: 31 October 2018 / Accepted: 2 November 2018 / Published: 12 November 2018
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Abstract
In magnetic hard disk drives, it is important to evaluate the replenishment effect of a submonolayer lubricant film under a more severe condition that the head–disk spacing has to be reduced from the current 0.7 nm to ~0.5 nm. In contrast to the
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In magnetic hard disk drives, it is important to evaluate the replenishment effect of a submonolayer lubricant film under a more severe condition that the head–disk spacing has to be reduced from the current 0.7 nm to ~0.5 nm. In contrast to the prevailing conventional diffusion equation validated for multilayer liquid film, the author has already proposed a new diffusion equation more suitable for submonolayer film by intuitively incorporating the density reduction effect in the submonolayer liquid film. This paper presents a rigorous derivation of the disjoining pressure (DP) from Lennard–Jones potential (LJP) and formulated the diffusion equation incorporating the DP. The difference in the rigorous DP and diffusion equation from the previous versions is negligibly small except in a small film thickness less than the van der Waals (vdW) distance. The theoretical relationship between the vdW distance in the DP and the molecular force equilibrium distance in the LJP is elucidated. Rigorous derivations of the DP and diffusion equation for multilayer liquid film from the LJP are also presented. The superiority of the submonolayer diffusion equation over the conventional equation in the submonolayer film regime is demonstrated by comparing their theoretical diffusion coefficients with Waltman’s experimental data. Full article
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Open AccessReview Surface Functionalisation of Upconversion Nanoparticles with Different Moieties for Biomedical Applications
Surfaces 2018, 1(1), 96-121; https://doi.org/10.3390/surfaces1010009
Received: 14 October 2018 / Revised: 6 November 2018 / Accepted: 7 November 2018 / Published: 11 November 2018
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Abstract
Lanthanide ion-doped upconversion nanoparticles (UCNPs) that can convert low-energy infrared photons into high-energy visible and ultraviolet photons, are becoming highly sought-after for advanced biomedical and biophotonics applications. Their unique luminescent properties enable UCNPs to be applied for diagnosis, including biolabeling, biosensing, bioimaging, and
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Lanthanide ion-doped upconversion nanoparticles (UCNPs) that can convert low-energy infrared photons into high-energy visible and ultraviolet photons, are becoming highly sought-after for advanced biomedical and biophotonics applications. Their unique luminescent properties enable UCNPs to be applied for diagnosis, including biolabeling, biosensing, bioimaging, and multiple imaging modality, as well as therapeutic treatments including photothermal and photodynamic therapy, bio-reductive chemotherapy and drug delivery. For the employment of the inorganic nanomaterials into biological environments, it is critical to bridge the gap in between nanoparticles and biomolecules via surface modifications and subsequent functionalisation. This work reviews the various ways to surface modify and functionalise UCNPs so as to impart different functional molecular groups to the UCNPs surfaces for a broad range of applications in biomedical areas. We discussed commonly used base functionalities, including carboxyl, amino and thiol moieties that are typically imparted to UCNP surfaces so as to provide further functional capacity. Full article
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Open AccessArticle pH Controlled Impedimetric Sensing of Copper(II) Ion Using Oxytocin as Recognition Element
Surfaces 2018, 1(1), 90-95; https://doi.org/10.3390/surfaces1010008
Received: 19 August 2018 / Revised: 9 October 2018 / Accepted: 11 October 2018 / Published: 15 October 2018
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Abstract
We report the modulation of the specific metal gation properties of a peptide and demonstrate a highly selective sensor for copper(II) ion. The neuropeptide oxytocin (OT) is reported for its high affinity towards Zn2+ and Cu2+ at physiological pH. The binding
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We report the modulation of the specific metal gation properties of a peptide and demonstrate a highly selective sensor for copper(II) ion. The neuropeptide oxytocin (OT) is reported for its high affinity towards Zn2+ and Cu2+ at physiological pH. The binding of the metal ions to OT is tuned by altering the pH of the medium. OT was self-assembled on glassy carbon electrode using surface chemistry, and electrochemical impedance spectroscopy (EIS) was used to probe the binding of Cu2+. Our results clearly indicate that at pH 10.0, the binding of Cu2+ to OT is increased compared to that at pH 7.0, while the binding to Zn2+ becomes almost negligible. This proves that the selectivity of OT towards each of the ions can be regulated simply by controlling the pH of the medium and hence allows the preparation of a sensing device with selectivity to Cu2+. Full article
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Open AccessArticle The Work Function of TiO2
Surfaces 2018, 1(1), 73-89; https://doi.org/10.3390/surfaces1010007
Received: 13 July 2018 / Revised: 31 August 2018 / Accepted: 1 September 2018 / Published: 7 September 2018
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Abstract
Polycrystalline anatase thin films, (001)- and (101)-oriented anatase TiO2 single crystals and (001)- and (110)-oriented rutile TiO2 single crystals with various surface treatments were studied by photoelectron spectroscopy to obtain their surface potentials. Regardless of orientations and polymorph, a huge variation
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Polycrystalline anatase thin films, (001)- and (101)-oriented anatase TiO 2 single crystals and (001)- and (110)-oriented rutile TiO 2 single crystals with various surface treatments were studied by photoelectron spectroscopy to obtain their surface potentials. Regardless of orientations and polymorph, a huge variation of the Fermi level and work function was achieved by varying the surface condition. The most strongly oxidized surfaces are obtained after oxygen plasma treatment with a Fermi level ∼2.6 eV above the valence band maximum and ionization potentials of up to 9.5 eV (work function 7.9 eV). All other treated anatase surfaces exhibit an ionization potential independent of surface condition of 7.96 ± 0.15 eV. The Fermi level positions and the work functions vary by up to 1 eV. The ionization potential of rutile is ∼0.56 eV lower than that of anatase in good agreement with recent band alignment studies. Full article
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Open AccessArticle Material Structure and Mechanical Properties of Silicon Nitride and Silicon Oxynitride Thin Films Deposited by Plasma Enhanced Chemical Vapor Deposition
Surfaces 2018, 1(1), 59-72; https://doi.org/10.3390/surfaces1010006
Received: 9 May 2018 / Revised: 22 August 2018 / Accepted: 27 August 2018 / Published: 30 August 2018
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Abstract
Silicon nitride and silicon oxynitride thin films are widely used in microelectronic fabrication and microelectromechanical systems (MEMS). Their mechanical properties are important for MEMS structures; however, these properties are rarely reported, particularly the fracture toughness of these films. In this study, silicon nitride
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Silicon nitride and silicon oxynitride thin films are widely used in microelectronic fabrication and microelectromechanical systems (MEMS). Their mechanical properties are important for MEMS structures; however, these properties are rarely reported, particularly the fracture toughness of these films. In this study, silicon nitride and silicon oxynitride thin films were deposited by plasma enhanced chemical vapor deposition (PECVD) under different silane flow rates. The silicon nitride films consisted of mixed amorphous and crystalline Si3N4 phases under the range of silane flow rates investigated in the current study, while the crystallinity increased with silane flow rate in the silicon oxynitride films. The Young’s modulus and hardness of silicon nitride films decreased with increasing silane flow rate. However, for silicon oxynitride films, Young’s modulus decreased slightly with increasing silane flow rate, and the hardness increased considerably due to the formation of a crystalline silicon nitride phase at the high flow rate. Overall, the hardness, Young modulus, and fracture toughness of the silicon nitride films were greater than the ones of silicon oxynitride films, and the main reason lies with the phase composition: the SiNx films were composed of a crystalline Si3N4 phase, while the SiOxNy films were dominated by amorphous Si–O phases. Based on the overall mechanical properties, PECVD silicon nitride films are preferred for structural applications in MEMS devices. Full article
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Open AccessArticle Diazonium Salts: Versatile Molecular Glues for Sticking Conductive Polymers to Flexible Electrodes
Surfaces 2018, 1(1), 43-58; https://doi.org/10.3390/surfaces1010005
Received: 20 June 2018 / Revised: 20 July 2018 / Accepted: 22 July 2018 / Published: 8 August 2018
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Abstract
Adhesion of polymers to surfaces is of the upmost importance in timely applications such as protective coatings, biomaterials, sensors, new power sources and soft electronics. In this context, this work examines the role of molecular interactions in the adhesion of polypyrrole thin films
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Adhesion of polymers to surfaces is of the upmost importance in timely applications such as protective coatings, biomaterials, sensors, new power sources and soft electronics. In this context, this work examines the role of molecular interactions in the adhesion of polypyrrole thin films to flexible Indium Tin Oxide (ITO) electrodes grafted with aryl layers from various diazonium salts, namely 4-carboxybenzenediazonium (ITO-CO2H), 4-sulfonicbenzenediazonium (ITO-SO3H), 4-N,N-dimethylbenzenediazonium (ITO-N(CH3)2), 4-aminobenzenediazonium (ITO-NH2), 4-cyanobenzenediazonium (ITO-CN) and 4-N-phenylbenzenediazonium (ITO-NHPh). It was demonstrated that PPy thin layers were adherent to all aryl-modified surfaces, whereas adhesive failure was noted for bare ITO following simple solvent washing or sonication. Adhesion of polypyrrole was investigated in terms of hydrophilic/hydrophobic character of the underlying aryl layer as probed by contact angle measurements. It was found that sulfonic acid-doped polypyrrole (PPy-BSA) thin films were preferably deposited on the most hydrophobic surfaces. More importantly, the redox properties and electrochemical impedance of PPy were closely related to the hydrophobic character of the aryl layers. This work demonstrates that diazonium compounds are unique molecular glues for conductive polymers and permit to tune their interfacial properties. With robust, diazonium-based architectured interfaces, one can design high performance materials for e.g., sensors, printed soft electronics and flexible thermoelectrics. Full article
(This article belongs to the Special Issue Electrochemical Surface Science: Basics and Applications)
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Open AccessArticle On the Contrasting Effect Exerted by a Thin Layer of CdS against the Passivation of Silver Electrodes Coated with Thiols
Surfaces 2018, 1(1), 29-42; https://doi.org/10.3390/surfaces1010004
Received: 14 June 2018 / Revised: 27 July 2018 / Accepted: 27 July 2018 / Published: 31 July 2018
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Abstract
The passivation of metal electrodes covered by self-assembled monolayers of long-chain thiols is well known. The disappearance of the voltammetric peak of redox species in solution is a classical test for the formation of full layers of thiols. Similar studies on semiconductors are
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The passivation of metal electrodes covered by self-assembled monolayers of long-chain thiols is well known. The disappearance of the voltammetric peak of redox species in solution is a classical test for the formation of full layers of thiols. Similar studies on semiconductors are still very limited. We used silver surfaces covered by an ultrathin layer of CdS as substrate for self-assembling of n-hexadecanethiol (C16SH), and we compared the experimental results with those obtained by using the bare silver surface as substrate. The strong insulating effect of C16SH deposited on Ag(III) is shown by the inhibition of the voltammetric peak of Ru(NH3)63+/2+. On the contrary, the voltammogram obtained on CdS-covered Ag(III) is very similar to that obtained on the bare Ag(III) electrode, thus suggesting that the presence of CdS exerts a contrasting effect on the passivation of the silver electrode. A crucial point of our work is to demonstrate the effective formation of C16SH monolayers on Ag(III) covered by CdS. The formation of full layers of C16SH was strongly suggested by the inhibition of the stripping peak of Cd from the CdS deposit covered by C16SH. The presence of C16SH was confirmed by electrochemical quartz crystal microbalance (EQCM) measurements as well as by Auger electron spectroscopy (AES) analysis. Full article
(This article belongs to the Special Issue Electrochemical Surface Science: Basics and Applications)
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Open AccessArticle Potential Driven Non-Reactive Phase Transitions of Ordered Porphyrin Molecules on Iodine-Modified Au(100): An Electrochemical Scanning Tunneling Microscopy (EC-STM) Study
Surfaces 2018, 1(1), 12-28; https://doi.org/10.3390/surfaces1010003
Received: 3 July 2018 / Revised: 22 July 2018 / Accepted: 24 July 2018 / Published: 25 July 2018
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Abstract
The modelling of long-range ordered nanostructures is still a major issue for the scientific community. In this work, the self-assembly of redox-active tetra(N-methyl-4-pyridyl)-porphyrin cations (H2TMPyP) on an iodine-modified Au(100) electrode surface has been studied by means of Cyclic Voltammetry
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The modelling of long-range ordered nanostructures is still a major issue for the scientific community. In this work, the self-assembly of redox-active tetra(N-methyl-4-pyridyl)-porphyrin cations (H2TMPyP) on an iodine-modified Au(100) electrode surface has been studied by means of Cyclic Voltammetry (CV) and in-situ Electrochemical Scanning Tunneling Microscopy (EC-STM) with submolecular resolution. While the CV measurements enable conclusions about the charge state of the organic species, in particular, the potentio-dynamic in situ STM results provide new insights into the self-assembly phenomena at the solid-liquid interface. In this work, we concentrate on the regime of positive electrode potentials in which the adsorbed molecules are not reduced yet. In this potential regime, the spontaneous adsorption of the H2TMPyP molecules on the anion precovered surface yields the formation of up to five different potential-dependent long-range ordered porphyrin phases. Potentio-dynamic STM measurements, as a function of the applied electrode potential, show that the existing ordered phases are the result of a combination of van der Waals and electrostatic interactions. Full article
(This article belongs to the Special Issue Electrochemical Surface Science: Basics and Applications)
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Open AccessArticle Switchable Interfaces: Redox Monolayers on Si(100) by Electrochemical Trapping of Alcohol Nucleophiles
Surfaces 2018, 1(1), 3-11; https://doi.org/10.3390/surfaces1010002
Received: 29 June 2018 / Accepted: 17 July 2018 / Published: 20 July 2018
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Abstract
Organic electrosynthesis is going through its renaissance but its scope in surface science as a tool to introduce specific molecular signatures at an electrode/electrolyte interface is under explored. Here, we have investigated an electrochemical approach to generate in situ surface-tethered and highly-reactive carbocations.
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Organic electrosynthesis is going through its renaissance but its scope in surface science as a tool to introduce specific molecular signatures at an electrode/electrolyte interface is under explored. Here, we have investigated an electrochemical approach to generate in situ surface-tethered and highly-reactive carbocations. We have covalently attached an alkoxyamine derivative on an Si(100) electrode and used an anodic bias stimulus to trigger its fragmentation into a diffusive nitroxide (TEMPO) and a surface-confined carbocation. As a proof-of-principle we have used this reactive intermediate to trap a nucleophile dissolved in the electrolyte. The nucleophile was ferrocenemethanol and its presence and surface concentration after its reaction with the carbocation were assessed by cyclic voltammetry. The work expands the repertoire of available electrosynthetic methods and could in principle lay the foundation for a new form of electrochemical lithography. Full article
(This article belongs to the Special Issue Electrochemical Surface Science: Basics and Applications)
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Open AccessEditorial Welcome to Surfaces—A New Open Access Journal for an Interdisciplinary Scientific Community
Surfaces 2018, 1(1), 1-2; https://doi.org/10.3390/surfaces1010001
Received: 27 March 2018 / Accepted: 27 March 2018 / Published: 30 March 2018
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Abstract
Surfaces are ubiquitous. Everyday life gives plenty of examples where surfaces and interfaces play a leading role[...] Full article
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