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Polyelectrolyte multilayers (PEMs) with stratification of the internal structure were assembled from statistical amphiphilic copolyelectrolytes of opposite charges. These polyelectrolytes organize in aqueous solutions into micellar structures with fluoroalkyl and aromatic nanodomains, respectively, that were also preserved after deposition as thin films via layer-by-layer (LbL) electrostatic self-assembly. The unimolecular micelles, formed due to statistical compositions of amphiphilic polyelectrolytes used, were shown to suppress chain interdiffusion between adjacent layers in resulting micellar PEMs, as evidenced by spectroscopic ellipsometry, atomic force microscopy (AFM), and neutron reflectometry (NR) measurements. Additionally, hydrophobic cores of the micelles were used as hosts for photoactive molecules, namely, ferrocene and perfluorinated magnesium phthalocyanine. Stratified micellar multilayers were then deposited as hollow capsules using CaCO3 microparticles as templates. Photoinduced electron transfer (PET) between ferrocene and phthalocyanine solubilized in the polymer micelles was demonstrated to occur efficiently inside the stratified, polyelectrolyte walls of the capsules, due to the polarity gradient created by the incompatible aromatic and fluoroalkyl domains. The obtained results present a new approach to construct well-organized, self-assembled nanostructured materials for solar energy conversion.
BACKGROUND: The etiology of low back pain (LBP), one of the most prevalent and costly diseases of our time, is accepted to be multi-causal, placing functional factors in the focus of research. Thereby, pain models suggest a centrally controlled strategy of trunk stiffening in LBP. However, supporting biomechanical evidence is mostly limited to static measurements during maximum voluntary contractions (MVC), probably influenced by psychological factors in LBP. Alternatively, repeated findings indicate that the neuromuscular efficiency (NME), characterized by the strength-to-activation relationship (SAR), of lower back muscles is impaired in LBP. Therefore, a dynamic SAR protocol, consisting of normalized trunk muscle activation recordings during submaximal loads (SMVC) seems to be relevant. This thesis aimed to investigate the influence of LBP on the NME and activation pattern of trunk muscles during dynamic trunk extensions.
METHODS: The SAR protocol consisted of an initial MVC reference trial (MVC1), followed by SMVCs at 20, 40, 60 and 80% of MVC1 load. An isokinetic trunk dynamometer (Con-Trex TP, ROM: 45° flexion to 10° extension, velocity: 45°/s) and a trunk surface EMG setup (myon, up to 12 leads) was used. Extension torque output [Nm] and muscular activation [V] were assessed in all trials. Finally, another MVC trial was performed (MVC2) for reliability analysis. For SAR evaluation the SMVC trial values were normalized [%MVC1] and compared inter- and intra-individually.
The methodical validity of the approach was tested in an isometric SAR single-case pilot study (S1a: N = 2, female LBP patient vs. healthy male). In addition, the validity of the MVC reference method was verified by comparing different contraction modes (S1b: N = 17, healthy individuals). Next, the isokinetic protocol was validated in terms of content for its applicability to display known physiological differences between sexes in a cross-sectional study (S2: each n = 25 healthy males/females). Finally, the influence of acute pain on NME was investigated longitudinally by comparing N = 8 acute LBP patients with the retest after remission of pain (S3). The SAR analysis focused on normalized agonistic extensor activation and abdominal and synergistic extensor co-activation (t-tests, ANOVA, α = .05) as well as on reliability of MVC1/2 outcomes.
RESULTS: During the methodological validation of the protocol (S1a), the isometric SAR was found to be descriptively different between individuals. Whereas torque output was highest during eccentric MVC, no relevant difference in peak EMG activation was found between contraction modes (S1b). The isokinetic SAR sex comparison (S2), though showing no significant overall effects, revealed higher normalized extensor activation at moderate submaximal loads in females (13 ± 4%), primarily caused by pronounced thoracic activation. Similarly, co-activation analysis resulted in significantly higher antagonistic activation at moderate loads compared to males (33 ± 9%). During intra-individual analysis of SAR in LBP patients (S3), a significant effect of pain status on the SAR has been identified, manifesting as increased normalized EMG activation of extensors during acute LBP (11 ± 8%) particularly at high load. Abdominal co-activation tended to be elevated (27 ± 11%) just as the thoracic extensor parts seemed to take over proportions of lumbar activation. All together, the M. erector spinae behaviour during the SAR protocol was rather linear with the tendency to rise exponentially during high loads. For the level of normalized EMG activation during SMVCs, a clear increasing trend from healthy males to females over to non-acute and acute LBP patients was discovered. This was associated by elevated antagonistic activation and a shift of synergistic towards lumbar extensor activation. The MVC data revealed overall good reliability, with clearly higher variability during acute LBP.
DISCUSSION: The present thesis demonstrates that the NME of lower back muscles is impaired in LBP patients, especially during an acute pain episode. A new dynamic protocol has been developed that makes it possible to display the underlying SAR using normalized trunk muscle EMG during submaximal isokinetic loads. The protocol shows promise as a biomechanical tool for diagnostic analysis of NME in LBP patients and monitoring of rehabilitation progress. Furthermore, reliability not of maximum strength but rather of peak EMG of MVC measurements seems to be decreased in LBP patients. Meanwhile, the findings of this thesis largely substantiate the assumptions made by the recently presented ‘motor adaptation to pain’ model, suggesting a pain-related intra- and intermuscular activation redistribution affecting movement and stiffness of the trunk. Further research is needed to distinguish the grade of NME impairment between LBP subgroups.
This paper describes a strategy for preparing photosensitive polymeric grafts on flat solid surfaces by loading diblock-copolymer or homopolymer brushes with cationic azobenzene-containing surfactants. In contrast to previous work, we utilize photosensitive surfactants that bear positively-charged polyamine head groups whose charge varies between 1(+) and 3(+). Poly(methylmethacrylate-b-methacrylic acid) (PMMA-b-PMAA) brushes were prepared by employing atom transfer radical polymerization, where the bottom poly(methyl methacrylate) block was grown first followed by the synthesis of t-butyl methacrylate block that after de-protection yielded poly(methacrylic acid). We used PMMA-b-PMAA brushes with constant grafting density and length of the PMMA block, and three different lengths of the PMAA block. The azobenzene-based surfactants attached only to the PMAA block. The degree of binding (i.e., the number of surfactant molecules per binding site on the brush backbone) of the surfactants to the brush depends strongly on the valence of the surfactant head-group; within the brushes the concentration of the surfactant carrying unit charge is larger than that of multivalent surfactants. We detect pronounced response of the brush topography on irradiation with UV interference pattern even at very low degree of binding (as small as 0.08) of multi-valence surfactant. Areas on the sample that receive the highest UV dose exhibit chain scission. By removing the ruptured chains from the substrate via good solvent, one uncovers a surface topographical relief grating, whose spatial arrangement follows the intensity distribution of the UV light on the sample during irradiation. Due to strong coupling of the multi-valence surfactants to the polymer brush, it was possible in some cases to completely remove the polyelectrolyte block from the PMMA layer. The application of multi-valence azobenzene surfactants for triggering brush photosensitive has important advantage over usage of surfactant with unit charge because relative to single-valence surfactants much lower concentrations of the multivalent surfactant are needed to achieve comparable response upon UV irradiation. (C) 2016 Elsevier Ltd. All rights reserved.
We investigate light-induced changes in thickness and roughness of photosensitive polymer brushes containing azobenzene cationic surfactants by atomic force microscopy (AFM) in real time during light irradiation. Because the cis-state of azobenzene unit requires more free volume than its trans counterpart, the UV light-induced expansion of polymer thin films associated with the trans-to-cis isomerism of azobenzene groups is expected to occur. This phenomenon is well documented in physisorbed polymer films containing azobenzene groups. In contrast, photosensitive polymer brushes show a decrease in thickness under UV irradiation. We have found that the azobenzene surfactants in their trans-state form aggregates within the brush. Under irradiation, the surfactants undergo photoisomerization to the cis-state, which is more hydrophilic. As a consequence, the aggregates within the brush are disrupted, and the polymer brush contracts. When subsequently irradiated with blue light the polymer brush thickness returns back to its initial value. This behavior is related to isomerization of the surfactant to the more hydrophobic trans-state and subsequent formation of surfactant aggregates within the polymer brush. The photomechanical function of the dry polymer brush, i.e., contraction and expansion, was found to be reversible with repeated irradiation cycles and requires only a few seconds for switching. In addition to the thickness change, the roughness of the brush also changes reversibly between a few Angstroms (blue light) and several nanometers (UV light). Photosensitive polymer brushes represent smart films with light responsive thickness and roughness that could be used for generating dynamic fluctuating surfaces, the function of which can be turned on and off in a controllable manner on a nanometer length scale.
Singular quantified terms
(2016)
In this paper, I discuss the behavior of singular partitives, focusing on Hebrew. I show that group noun-headed singular quantified terms behave essentially different from other singular quantified terms. Specifically, the domain of quantification in the former is a discrete set (the members of the group), while in the latter the domain of quantification is a set of mass entities. I propose a preliminary analysis of singular quantified terms in Hebrew, respecting the properties peculiar to this language as well as the observations about group vs. non-group singular quantified terms. This analysis is based on a novel class of quantifiers I name ’Measure Quantifiers’, which instantiate relations between algebraic sums. Using shifts between algebraic sums, we can represent the different readings of singular and plural individual or group terms.
Several recent northern hemisphere summer extremes have been linked to persistent high-amplitude wave patterns (e.g. heat waves in Europe 2003, Russia 2010 and in the US 2011, Floods in Pakistan 2010 and Europe 2013). Recently quasi-resonant amplification (QRA) was proposed as a mechanism that, when certain dynamical conditions are fulfilled, can lead to such high-amplitude wave events. Based on these resonance conditions a detection scheme to scan reanalysis data for QRA events in boreal summer months was implemented. With this objective detection scheme we analyzed the occurrence and duration of QRA events and the associated atmospheric flow patterns in 1979-2015 reanalysis data. We detect a total number of 178 events for wave 6, 7 and 8 and find that during roughly one-third of all high amplitude events QRA conditions were met for respective waves. Our analysis reveals a significant shift for quasi-stationary waves 6 and 7 towards high amplitudes during QRA events, lagging first QRA-detection by typically one week. The results provide further evidence for the validity of the QRA hypothesis and its important role in generating high amplitude waves in boreal summer.
Due to the adsorption of biomolecules, the control of the biodistribution of nanoparticles is still one of the major challenges of nanomedicine. Poly(2-ethyl-2-oxazoline) (PEtOx) for surface modification of nanoparticles is applied and both protein adsorption and cellular uptake of PEtOxylated nanoparticles versus nanoparticles coated with poly(ethylene glycol) (PEG) and non-coated positively and negatively charged nanoparticles are compared. Therefore, fluorescent poly(organosiloxane) nanoparticles of 15 nm radius are synthesized, which are used as a scaffold for surface modification in a grafting onto approach. With multi-angle dynamic light scattering, asymmetrical flow field-flow fractionation, gel electrophoresis, and liquid chromatography-mass spectrometry, it is demonstrated that protein adsorption on PEtOxylated nanoparticles is extremely low, similar as on PEGylated nanoparticles. Moreover, quantitative microscopy reveals that PEtOxylation significantly reduces the non-specific cellular uptake, particularly by macrophage-like cells. Collectively, studies demonstrate that PEtOx is a very effective alternative to PEG for stealth modification of the surface of nanoparticles.