Motivated by observations of cell orientation at biofilm-substrate interfaces and reports that cell orientation and adhesion play important roles in biofilm evolution and function, we investigated the influence of surface chemistry on the orientation of cells captured from flow onto surfaces that were cationic, hydrophobic, or anionic. We characterized the initial orientations of nonmotile cells captured from gentle shear relative to the surface and flow directions. The broad distribution of captured cell orientations observed on cationic surfaces suggests that rapid electrostatic attractions of cells to oppositely charged surfaces preserve the instantaneous orientations of cells as they rotate in the near-surface shearing flow.
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2021
Bacterial swimming in flow near surfaces is critical to the spread of infection and device colonization. Understanding how material properties affect flagella- and motility-dependent bacteria-surface interactions is a first step in designing new medical devices that mitigate the risk of infection. We report that, on biomaterial coatings such as polyethylene glycol (PEG) hydrogels and end-tethered layers that prevent adhesive bacteria accumulation, the coating mechanics and hydration control the near-surface travel and dynamic surface contact of cells in gentle shear flow (order 10 s).
View Article and Find Full Text PDFStudies on the mechanisms for extracellular electron transfer in Geobacter species have primarily focused on Geobacter sulfurreducens, but the poor conservation of genes for some electron transfer components within the Geobacter genus suggests that there may be a diversity of extracellular electron transport strategies among Geobacter species. Examination of the gene sequences for PilA, the type IV pilus monomer, in Geobacter species revealed that the PilA sequence of Geobacter uraniireducens was much longer than that of G. sulfurreducens.
View Article and Find Full Text PDFGenetic modification to add tryptophan to PilA, the monomer for the electrically conductive pili of Geobacter sulfurreducens, yields conductive protein filaments 2000-fold more conductive than the wild-type pili while cutting the diameter in half to 1.5 nm.
View Article and Find Full Text PDFSolar cells fabricated using alkyl ammonium metal halides as light absorbers have the right combination of high power conversion efficiency and ease of fabrication to realize inexpensive but efficient thin film solar cells. However, they degrade under prolonged exposure to sunlight. Herein, we show that this degradation is quasi-reversible, and that it can be greatly lessened by simple modifications of the solar cell operating conditions.
View Article and Find Full Text PDFThiol (-SH) groups within a Zr(IV)-based metal-organic framework (MOF) anchor Hg(II) atoms; oxidation by H2O2 then leads to acidic sulfonate functions for catalyzing acetylene hydration at room temperature.
View Article and Find Full Text PDFUnlabelled: Direct measurement of multiple physical properties of Geobacter sulfurreducens pili have demonstrated that they possess metallic-like conductivity, but several studies have suggested that metallic-like conductivity is unlikely based on the structures of the G. sulfurreducens pilus predicted from homology models. In order to further evaluate this discrepancy, pili were examined with synchrotron X-ray microdiffraction and rocking-curve X-ray diffraction.
View Article and Find Full Text PDFThe nanoscale imaging of charge flow in proteins is crucial to understanding several life processes, including respiration, metabolism and photosynthesis. However, existing imaging methods are only effective under non-physiological conditions or are limited to photosynthetic proteins. Here, we show that electrostatic force microscopy can be used to directly visualize charge propagation along pili of Geobacter sulfurreducens with nanometre resolution and under ambient conditions.
View Article and Find Full Text PDFColloidal assembly of nC60 fullerene with naturally abundant magnetic iron oxide NPs will affect their fate and transformation in environmental media. In solution, fullerene association to aggregating iron oxide NPs/clusters greatly enhanced the overall colloidal stability. Development of depletion-mediated structured fullerene layers between pure and surface modified γFe2O3 NPs possibly resulted in such stabilization.
View Article and Find Full Text PDFWe describe the spontaneous assembly of ligand-stabilized gold nanoparticles on the surfaces of gallium droplets in suspension. By subsequent deposition of these coated droplets onto substrates with patterned electrodes, we form devices that have controlled architecture on the nanometer scale, which allows control of electron transport. In particular, we show that microscopic droplets can be brought into contact with one another with a monolayer of nanoparticles between them, resulting in a junction where electron transport is limited by the Coulomb blockade effect.
View Article and Find Full Text PDFJ Inorg Organomet Polym Mater
January 2013
Here we demonstrate patterning of protein/quantum dot hybrid bionanostructures electrostatic assembly of engineered negatively charged fluorescent protein with positively charged CdSe/ZnS QD patterns formed through e-beam lithography and post-patterning modification with cationic ligands.
View Article and Find Full Text PDFGeobacter sulfurreducens can form electrically conductive biofilms, but the potential for conductivity through mixed-species biofilms has not been examined. A current-producing biofilm grown from a wastewater sludge inoculum was highly conductive with low charge transfer resistance even though microorganisms other than Geobacteraceae accounted for nearly half the microbial community.
View Article and Find Full Text PDFIn this communication, we introduce squaric acid derivatives as anhydrous proton conductors. We report the synthesis, characterization and proton conductivities of four squaric acid derivatives. The anhydrous proton conductivity of one of the derivatives was 2.
View Article and Find Full Text PDFSupercapacitors have attracted interest in energy storage because they have the potential to complement or replace batteries. Here, we report that c-type cytochromes, naturally immersed in a living, electrically conductive microbial biofilm, greatly enhance the device capacitance by over two orders of magnitude. We employ genetic engineering, protein unfolding and Nernstian modeling for in vivo demonstration of charge storage capacity of c-type cytochromes and perform electrochemical impedance spectroscopy, cyclic voltammetry and charge-discharge cycling to confirm the pseudocapacitive, redox nature of biofilm capacitance.
View Article and Find Full Text PDFNanotechnology
December 2011
We demonstrate magnetic switching between two 360° domain wall vortex states in cobalt nanorings, which are candidate magnetic states for robust and low power magnetoresistive random access memory (MRAM) devices. These 360° domain wall (DW) or 'twisted onion' states can have clockwise or counterclockwise circulation, the two states for data storage. Reliable switching between the states is necessary for any realistic device.
View Article and Find Full Text PDFElectronic nanostructures made from natural amino acids are attractive because of their relatively low cost, facile processing and absence of toxicity. However, most materials derived from natural amino acids are electronically insulating. Here, we report metallic-like conductivity in films of the bacterium Geobacter sulfurreducens and also in pilin nanofilaments (known as microbial nanowires) extracted from these bacteria.
View Article and Find Full Text PDFThe dynamic nature of hydrogen bonds in phenolic polymers, where the hydrogen bond donor/acceptor reorientation can occur in a single site, presents lower barriers for proton transport.
View Article and Find Full Text PDFIn this communication, we show that liquid crystalline phases lower the activation energy barrier for proton transport. The liquid crystalline phases were obtained using a triphenylene core with alkyl chains bearing a triazole moiety at their termini.
View Article and Find Full Text PDFElectron-beam lithography was used to pattern poly(styrene-co-(methyldiaminotriazine) styrene) (PS-Triaz). These polymer nanopatterns were utilized as molecular scaffolds for assembling complementary thymine-functionalized CdSe-ZnS quantum dots (Thy-QDs) via three-point hydrogen-bonding molecular recognition. This interaction was very specific, with N-methyl thymine-functionalized QDs (MeThy-QDs) not depositing on the surfaces.
View Article and Find Full Text PDFWe discuss the coupling between optically excited semiconductor nanocrystals (NC) and thin metal films in both the single and multi-exciton regime. Using time-resolved photoluminescence spectroscopy, we determine the decay dynamics of free space and surface plasmon polariton (SPP) coupled emission. The two dynamics are found to be distinctly different at very small NC-metal separations and at photon energies close to the SPP resonance frequency.
View Article and Find Full Text PDFTransporting protons is essential in several biological processes as well as in renewable energy devices, such as fuel cells. Although biological systems exhibit precise supramolecular organization of chemical functionalities on the nanoscale to effect highly efficient proton conduction, to achieve similar organization in artificial systems remains a daunting challenge. Here, we are concerned with transporting protons on a micron scale under anhydrous conditions, that is proton transfer unassisted by any solvent, especially water.
View Article and Find Full Text PDFWe have developed a depth-resolved confocal thermal imaging technique that is capable of measuring the temperature distribution of an encapsulated or semi-obstructed device. The technique employs lock-in charge coupled device-based thermoreflectance imaging via a Nipkow disk confocal microscope, which is used to eliminate extraneous reflections from above or below the imaging plane. We use the confocal microscope to predict the decrease in contrast and dynamic range due to an obstruction for widefield thermoreflectance, and we demonstrate the ability of confocal thermoreflectance to maintain a high contrast and thermal sensitivity in the presence of large reflecting obstructions in the optical path.
View Article and Find Full Text PDFWe report on the fabrication and optical characterization of dense and ordered arrays of metal nanoparticles. The metal arrays are produced by reducing metal salts in block copolymer (BCP) templates made by solvent annealing of poly(styrene-b-4-vinylpyridine) (PS-b-P4VP) or poly(styrene-b-ethylene oxide) (PS-b-PEO) diblock copolymer thin films in mixed solvents. The gold and gold/silver composite nanoparticle arrays show characteristic surface plasmon resonances in the visible wavelength range.
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