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Using quasi-in-situ scanning force microscopy we study the details of nanopattern alignment in ABC terblock copolymer thin films in the presence of an in-plane electric field. Because of the surface interactions and electric field the lamellae are oriented both perpendicular to the plane of the film and parallel to the electric field. We identified two distinct defect types which govern the orientation mechanism. Ring-like (tori) and open-end defects dominate at the early stage of the orientation process, while mainly classic topological defects (disclinations and dislocations) are involved in long-range ordering at the late stages. Comparison of the time evolution of the defect density with the evolution of the orientational order parameter suggests that tori-defects are essential for the effective reorientation. Further, the quasi-in-situ SFM imaging allowed us to elucidate the influence of the electric field strength on the propagation velocity of the topological defects.
ACS Nano 2009 May 26
PMID:Electric field alignment of a block copolymer nanopattern: direct observation of the microscopic mechanism. 1938 3

Semifluorinated-quaternized triblock copolymers (SQTCs) were synthesized by chemical modification of polystyrene-block-poly(ethylene-ran-butylene)-block-polyisoprene ABC triblock copolymers. Surface characterization of the polymers was performed by X-ray photoelectron spectroscopy (XPS) and near-edge X-ray absorption fine structure (NEXAFS) analysis. The surface of the SQTC showed very high antibacterial activity against the airborne bacterium Staphylococcus aureus with >99 % inhibition of growth. In contrast in marine fouling assays, zoospores of the green alga Ulva settled on the SQTC, which can be attributed to the positively charged surface. The adhesion strength of sporelings (young plants) of Ulva and Navicula diatoms (a unicellular alga) was high. The SQTC did not show marked algicidal activity.
ACS Appl Mater Interfaces 2010 Mar
PMID:Antimicrobial behavior of semifluorinated-quaternized triblock copolymers against airborne and marine microorganisms. 2035 71

We report on the quasi in situ scanning force microscopy nanotomography which proved to be a key method to effectively obtain a three-dimensional (3D) microdomain structure of a complex ABC triblock morphology. As an example, we studied polybutadiene-block-poly(2-vinyl pyridine)-block-poly(tert-butyl methacrylate) (BVT) thin triblock terpolymer films. We realized a controlled erosion of the material by using low-pressure plasma etching coupled to the scanning force microscope. The 3D reconstruction provides insights into the structural behavior in very thin volume elements revealing morphological details not accessible with other methods.
ACS Nano 2010 Oct 26
PMID:Going beyond the surface: revealing complex block copolymer morphologies with 3D scanning force microscopy. 2084 44

In this study, we have investigated the transcriptome of Ralstonia eutropha H16 during cultivation with gluconate in presence of 3,3'-thiodipropionic acid (TDP) or 3,3'-dithiodipropionic acid (DTDP) during biosynthesis of poly(3-hydroxybutyrate-co-3-mercaptopropionate). Genome-wide transcriptome analyses revealed several genes which were upregulated during cultivation in presence of the above-mentioned compounds. Obtained data strongly suggest that two ABC-type transport system and three probable extracytoplasmic solute receptors mediate the uptake of TDP and DTDP, respectively. In addition, genes encoding the hydrolase S-adenosylhomocysteinase AhcY and the thiol-disulfide interchange proteins DsbA, DsbD, and FrnE were upregulated during cultivation on DTDP and, in case of AhcY and FrnE, on TDP as well. It is assumed that the corresponding enzymes are involved in the cleavage of TDP and DTDP. Several genes of the fatty acid metabolism exhibited increased expression levels: genes encoding two acetyltransferases, a predicted acyltransferase, the acetoacetyl-CoA reductase phaB3, an enoyl-CoA hydratase as well as an acyl dehydratase, an acetyl-CoA synthetase, two acyl-CoA dehydrogenases, the methylmalonyl-CoA mutase encoded by sbm1 and sbm2 and phaY1 were detected. Furthermore, ORF H16_A0217 encoding a hypothetical protein and exhibiting 54% amino acids identical to an acyl-CoA thioesterase from Saccharomonospora viridis was found to be highly upregulated. As the 2-methylcitrate synthase PrpC exhibited a three- to fourfold increased activity in cells grown in presence of TDP or DTDP as compared to gluconate, metabolization of the cleavage products 3MP and 3-hydroxypropionate to propionyl-CoA is proposed.
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PMID:Investigations on the microbial catabolism of the organic sulfur compounds TDP and DTDP in Ralstonia eutropha H16 employing DNA microarrays. 2092 76

Bernal (ABA stacking order) and rhombohedral (ABC) trilayer graphene (3LG) are characterized by Raman spectroscopy. From a systematic experimental and theoretical analysis of the Raman modes in both of these 3LGs, we show that the G band, G' (2D) band, and the intermediate-frequency combination modes of 3LGs are sensitive to the stacking order of 3LG. The phonon wavevector q, that gives the double resonance Raman spectra is larger in ABC than ABA, which is the reason why we get the different Raman frequencies and their spectral widths for ABA and ABC 3LG. The weak electron-phonon interaction in ABC-stacked 3LG and the localized strain at the boundary between ABC- and ABA-stacked domains are clearly reflected by the softening of the G mode and the G' mode, respectively.
ACS Nano 2011 Nov 22
PMID:Raman characterization of ABA- and ABC-stacked trilayer graphene. 2196 35

We distinguish between Bernal and rhombohedral stacked trilayer graphene using aberration-corrected high-resolution transmission electron microscopy. By using a monochromator to reduce chromatic aberration effects, angstrom resolution can be achieved at an accelerating voltage of 80 kV, which enables the atomic structure of ABC rhombohedral trilayer graphene to be unambiguously resolved. Our images of ABC rhombohedral trilayer graphene provide a clear signature for its identification. Few-layer graphene interfaces with ABC:BC:BCAB structure have also been studied, and we have determined the stacking sequence of each graphene layer and consequently the 3D structure. These results confirm that CVD-grown few-layer graphene can adopt an ABC rhombohedral stacking.
ACS Nano 2012 Jun 26
PMID:Atomic structure of ABC rhombohedral stacked trilayer graphene. 2266 63

Directed self-assembly processes of polymeric systems represent a powerful approach for the generation of structural hierarchy in analogy to biological systems. Herein, we utilize triiodide as a strongly polarizable counterion to induce hierarchical self-assembly of an ABC miktoarm star terpolymer comprising a polybutadiene (PB), a poly(tert-butyl methacrylate) (PtBMA), and a poly(N-methyl-2-vinylpyridinium) (P2VPq) segment. Hereby, the miktoarm architecture in conjunction with an increasing ratio of triiodide versus iodide counterions allows for a stepwise assembly of spherical micelles as initial building blocks into cylindrical structures and superstructures thereof. Finally, micrometer-sized multicompartment particles with a periodic lamellar fine structure are observed, for which we introduce the term "woodlouse". The counterion-mediated decrease in hydrophilicity of the corona-forming P2VPq block is the underlying trigger to induce this hierarchical structure formation. All individual steps and the corresponding intermediates toward these well-defined superstructures were intensively studied by scattering and electron microscopic techniques, including transmission electron microtomography.
ACS Nano 2013 May 28
PMID:Counterion-mediated hierarchical self-assembly of an ABC miktoarm star terpolymer. 2354 50

We report here the design and synthesis of an ABC miktoarm star peptide connecting through a lysine junction a short peptide sequence and two hydrophobic but immiscible blocks (a hydrocarbon and a fluorocarbon). The designed molecule can self-assemble into one-dimensional nanostructures with a great diversity of kinetically evolving morphologies in aqueous solution, while molecules that contain only one of the two hydrophobic blocks form structurally similar filaments. We believe the rich assembly behavior and morphological evolution are a direct reflection of the molecular frustration present within the filament core as a result of the in-compatibility of the fluorocarbon and hydrocarbon segments. Our finding opens new opportunities for creating complex supramolecular polymers through the architecture design of small molecular building units.
ACS Macro Lett 2013 Dec 17
PMID:Supramolecular Polymers Formed by ABC Miktoarm Star Peptides. 2449 Jan 24

We present the design and synthesis of a linear ABC triblock terpolymer for the bottom-up synthesis of anisotropic organic/inorganic hybrid materials: polyethylene-block-poly(2-(4-(tert-butoxycarbonyl)amino)butyl-2-oxazoline)-block-poly(2-iso-propyl-2-oxazoline) (PE-b-PBocAmOx-b-PiPrOx). The synthesis was realized via the covalent linkage of azide-functionalized polyethylene and alkyne functionalized poly(2-alkyl-2-oxazoline) (POx)-based diblock copolymers exploiting copper-catalyzed azide-alkyne cycloaddition (CuAAC) chemistry. After purification of the resulting triblock terpolymer, the middle block was deprotected, resulting in a primary amine in the side chain. In the next step, solution self-assembly into core-shell-corona micelles in aqueous solution was investigated by dynamic light scattering (DLS) and transmission electron microscopy (TEM). Subsequent directional crystallization of the corona-forming block, poly(2-iso-propyl-2-oxazoline), led to the formation of anisotropic superstructures as demonstrated by electron microscopy (SEM and TEM). We present hypotheses concerning the aggregation mechanism as well as first promising results regarding the selective loading of individual domains within such anisotropic nanostructures with metal nanoparticles (Au, Fe3O4).
ACS Nano 2015 Oct 27
PMID:Toward Anisotropic Hybrid Materials: Directional Crystallization of Amphiphilic Polyoxazoline-Based Triblock Terpolymers. 2637 93

We investigate a morphological transition of surface-immobilized triblock terpolymer micelles: the splitting into well-defined clusters of satellite micelles upon pH changes. The multicompartment micelles are formed in aqueous solution of ABC triblock terpolymers consisting of a hydrophobic polybutadiene block, a weak polyanionic poly(methacrylic acid) block, and a weak polycationic poly(2-(dimethylamino)ethyl methacrylate) block. They are subsequently immobilized on silicon wafer surfaces by dip-coating. The splitting process is triggered by a pH change to strongly basic pH, which goes along with a charge reversal of the micelles. We find that the aggregation number of the submicelles is well-defined and that larger micelles have a tendency to split into a larger number of submicelles. Furthermore, there is a clear preference for clusters consisting of doublets and triplets of submicelles. The morphology of surface-immobilized clusters can be "quenched" by returning to the original pH. Thus, such well-defined micellar clusters can be stabilized and are available as colloidal building blocks for the formation of hierarchical surface structures. We discuss the underlying physicochemical principles of the splitting process considering changes in charge and total free energy of the micelles upon pH change.
ACS Nano 2016 05 24
PMID:Splitting of Surface-Immobilized Multicompartment Micelles into Clusters upon Charge Inversion. 2710 41


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