We have studied the spectral (UV−vis absorption and fluorescence) and thermally spectral stability of seven fluorene-based blue-light-emitting polymers in film states. These polymers have different side chain and backbone structure. Spiro-functionalization at the C-9 bridge position of fluorene unit could significantly improve the emission spectral quality (narrower spectrum and shorter tail extended to longer wavelength direction) and thermally spectral stability of 9,9-disubstituted polyfluorene derivatives. A glass transition temperature dependence for excimer emission in the polymers was demonstrated, and the improvement of thermally spectral stability by the spiro-functionalization is attributed to the increase of glass transition temperature. The backbone structural modification for 9,9-disubstituted polyfluorenes by alternatively inserting substituted phenylene units could provide blue emission with the spectral quality and thermally spectral stability even better than spiro-functionalized polyfluorenes, and no glass transition temperature dependence for excimer formation was observed in the backbone-modified polymers. The spectral properties of the polymers are dependent on the substitution on the phenylene ring. Thermotropic liquid crystallization was observed in the polymers bearing long alkoxy substituents. The good thermally spectral stability of the polymers is attributed to the poor planar configuration of the backbone and the efficient separation of the side chains on phenylene units for backbones.
The success of Pseudomonas species as opportunistic pathogens derives in great part from their ability to form stable biofilms that offer protection against chemical and mechanical attack. The extracellular matrix of biofilms contains numerous biomolecules, and it has recently been discovered that in Pseudomonas one of the components includes β-sheet rich amyloid fibrils (functional amyloid) produced by the fap operon. However, the role of the functional amyloid within the biofilm has not yet been investigated in detail. Here we investigate how the fap-based amyloid produced by Pseudomonas affects biofilm hydrophobicity and mechanical properties. Using atomic force microscopy imaging and force spectroscopy, we show that the amyloid renders individual cells more resistant to drying and alters their interactions with hydrophobic probes. Importantly, amyloid makes Pseudomonas more hydrophobic and increases biofilm stiffness 20-fold. Deletion of any one of the individual members of in the fap operon (except the putative chaperone FapA) abolishes this ability to increase biofilm stiffness and correlates with the loss of amyloid. We conclude that amyloid makes major contributions to biofilm mechanical robustness.
We have developed an unconventional method for the layer-by-layer (LbL) assembly of graphene multilayer films. Unconventional LbL assembly was achieved by the following two-step process. Graphene sheets were modified by pyrene-grafted poly(acrylic acid) (PAA) in aqueous solution, and then the modified graphene sheets were used for layer-by-layer alternating deposition with poly(ethyleneimine) (PEI). The graphene-multilayer-film-modified electrode shows enhanced electron transfer for the redox reactions of Fe(CN)(6)(3-) and excellent electrocatalytic activity of H(2)O(2). On the basis of this property, a bienzyme biosensing system for the detection of maltose was fabricated by successive LbL assembly of graphene, glucose oxidase (GOx), and glucoamylase (GA). LbL assembly of graphene combines the excellent electrochemical properties of graphene and the versatility of LbL assembly, showing great promise in highly efficient sensors and advanced biosensing systems.
Bringing the study of bacterial adhesion down to a single-cell level is critical for understanding the molecular mechanisms involved in initial bacterial attachment. We have developed a simple and versatile method for making single-cell bacterial probes to study the adhesion of single bacterial cells by atomic force microscopy (AFM). A single-cell probe was made by picking up a bacterial cell from a glass surface using a tipless AFM cantilever coated with a commercial cell adhesive Cell-Tak. The method was applied to four different bacterial strains, and single-cell adhesion was measured on three surfaces (fresh glass, hydrophilic glass, and mica). Attachment to the cantilever was stable during the AFM force measurements that were conducted for 2 h, and viability was confirmed by Live/Dead fluorescence staining at the end of each experiment. The adhesion force and final rupture length were dependent on bacterial strains, surfaces properties, and contact time. The single-cell probe offers control of cell immobilization and thus holds advantages over the commonly used multicell probes with which random immobilization is obtained by submerging the cantilever in a bacterial suspension. The reported method provides a general platform for investigating single-cell interactions of bacteria with different surfaces and other cells by AFM force spectroscopy, thus improving our understanding of the mechanisms of bacterial attachment.
Epigallocatechin-3-gallate (EGCG) is the major polyphenol in green tea. It has antimicrobial properties and disrupts the ordered structure of amyloid fibrils involved in human disease. The antimicrobial effect of EGCG against the opportunistic pathogen Pseudomonas aeruginosa has been shown to involve disruption of quorum sensing (QS). Functional amyloid fibrils in P. aeruginosa (Fap) are able to bind and retain quorum-sensing molecules, suggesting that EGCG interferes with QS through structural remodeling of amyloid fibrils. Here we show that EGCG inhibits the ability of Fap to form fibrils; instead, EGCG stabilizes protein oligomers. Existing fibrils are remodeled by EGCG into non-amyloid aggregates. This fibril remodeling increases the binding of pyocyanin, demonstrating a mechanism by which EGCG can affect the QS function of functional amyloid. EGCG reduced the amyloid-specific fluorescent thioflavin T signal in P. aeruginosa biofilms at concentrations known to exert an antimicrobial effect. Nanoindentation studies showed that EGCG reduced the stiffness of biofilm containing Fap fibrils but not in biofilm with little Fap. In a combination treatment with EGCG and tobramycin, EGCG had a moderate effect on the minimum bactericidal eradication concentration against wild-type P. aeruginosa biofilms, whereas EGCG had a more pronounced effect when Fap was overexpressed. Our results provide a direct molecular explanation for the ability of EGCG to disrupt P. aeruginosa QS and modify its biofilm and strengthens the case for EGCG as a candidate in multidrug treatment of persistent biofilm infections.
[1] We present a generalized multipoint analysis of physical quantities, such as magnetic field and plasma flow, based on spatial gradient properties, where the multipoint data may be taken by irregular (distorted) configurations of any number of spacecraft. The methodology is modified from a previous, fully 3-D gradient analysis technique, designed to apply strictly to 4-point measurements and to be stable for regular spacecraft configurations. Here, we adapt the method to be tolerant against distorted configurations and to return a partial result when fewer spacecraft measurements are available. We apply the method to a variety of important physical quantities, such as the electric current density and the vorticity of plasma flows based on Cluster and THEMIS multiple-point measurements. The method may also have valuable applications on the coming Swarm mission.
Magnetic disturbances caused by the Earth's ring current, particularly during storm time activity, have a dominant effect on the geomagnetic field. Strong currents and large kinetic and magnetic energies can change considerably local field geometry and depress the ground geomagnetic field. The multispacecraft magnetic measurements of Cluster allow extensive in situ coverage of the ring current. We select 48 storm time Cluster crossing events to investigate the variation of the local current density distribution and magnetic configuration of the ring current. We find direct evidence for the existence of an inner, eastward flowing current in addition to the dominant westward current, in the ring plane. The radius of curvature of the magnetic field lines (MFLs) is found to be increasingly reduced at all local times during increasing storm activity, changing the resulting ring current magnetic geometry considerably, where the MFL configuration and the azimuthal current density distribution are asymmetric with the local time. During similar storm activity the radius of curvature of the local MFLs, R c , is smallest on the nightside to duskside, medium on the dawnside, and largest on the dayside. This change in geometry may have significant influence on the spatial distribution of the particles with various energies in the plasmasphere, ring current, and radiation belts.
BackgroundPropionibacteria are part of the human microbiota. Many studies have addressed the predominant colonizer of sebaceous follicles of the skin, Propionibacterium acnes, and investigated its association with the skin disorder acne vulgaris, and lately with prostate cancer. Much less is known about two other propionibacterial species frequently found on human tissue sites, Propionibacterium granulosum and Propionibacterium avidum. Here we analyzed two and three genomes of P. granulosum and P. avidum, respectively, and compared them to two genomes of P. acnes; we further highlight differences among the three cutaneous species with proteomic and microscopy approaches.ResultsElectron and atomic force microscopy revealed an exopolysaccharide (EPS)-like structure surrounding P. avidum cells, that is absent in P. acnes and P. granulosum. In contrast, P. granulosum possesses pili-like appendices, which was confirmed by surface proteome analysis. The corresponding genes were identified; they are clustered with genes encoding sortases. Both, P. granulosum and P. avidum lack surface or secreted proteins for predicted host-interacting factors of P. acnes, including several CAMP factors, sialidases, dermatan-sulphate adhesins, hyaluronidase and a SH3 domain-containing lipoprotein; accordingly, only P. acnes exhibits neuraminidase and hyaluronidase activities. These functions are encoded on previously unrecognized island-like regions in the genome of P. acnes.ConclusionsDespite their omnipresence on human skin little is known about the role of cutaneous propionibacteria. All three species are associated with a variety of diseases, including postoperative and device-related abscesses and infections. We showed that the three organisms have evolved distinct features to interact with their human host. Whereas P. avidum and P. granulosum produce an EPS-like surface structure and pili-like appendices, respectively, P. acnes possesses a number of unique surface-exposed proteins with host-interacting properties. The different surface properties of the three cutaneous propionibacteria are likely to determine their colonizing ability and pathogenic potential on the skin and at non-skin sites.
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