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- Institut für Mathematik (44)
- Institut für Germanistik (43)
Molecular phenotyping technologies (e.g., transcriptomics, proteomics, and metabolomics) offer the possibility to simultaneously obtain multivariate time series (MTS) data from different levels of information processing and metabolic conversions in biological systems. As a result, MTS data capture the dynamics of biochemical processes and components whose couplings may involve different scales and exhibit temporal changes. Therefore, it is important to develop methods for determining the time segments in MTS data, which may correspond to critical biochemical events reflected in the coupling of the system's components. Here we provide a novel network-based formalization of the MTS segmentation problem based on temporal dependencies and the covariance structure of the data. We demonstrate that the problem of partitioning MTS data into k segments to maximize a distance function, operating on polynomially computable network properties, often used in analysis of biological network, can be efficiently solved. To enable biological interpretation, we also propose a breakpoint-penalty (BP-penalty) formulation for determining MTS segmentation which combines a distance function with the number/length of segments. Our empirical analyses of synthetic benchmark data as well as time-resolved transcriptomics data from the metabolic and cell cycles of Saccharomyces cerevisiae demonstrate that the proposed method accurately infers the phases in the temporal compartmentalization of biological processes. In addition, through comparison on the same data sets, we show that the results from the proposed formalization of the MTS segmentation problem match biological knowledge and provide more rigorous statistical support in comparison to the contending state-of-the-art methods.
We investigate the properties of a recently introduced asymmetric association measure, called inner composition alignment (IOTA), aimed at inferring regulatory links (couplings). We show that the measure can be used to determine the direction of coupling, detect superfluous links, and to account for autoregulation. In addition, the measure can be extended to infer the type of regulation (positive or negative). The capabilities of IOTA to correctly infer couplings together with their directionality are compared against Kendall's rank correlation for time series of different lengths, particularly focussing on biological examples. We demonstrate that an extended version of the measure, bidirectional inner composition alignment (biIOTA), increases the accuracy of the network reconstruction for short time series. Finally, we discuss the applicability of the measure to infer couplings in chaotic systems.
The purpose of this study was to investigate the association between variables of lower extremity muscle strength, balance, and mobility assessed under various task conditions.
Twenty-one healthy children (mean age: 9 +/- 1 years) were tested for their isometric and dynamic strength as well as for their steady-state, proactive, and reactive balance and mobility. Balance and mobility tests were conducted under single and dual task conditions.
Significant positive correlations were detected between measures of isometric and dynamic leg muscle strength. Hardly any significant associations were observed between variables of strength and balance/mobility and between measures of steady-state, proactive, and reactive balance. Additionally, no significant correlations were detected between balance/mobility tests performed under single and dual task conditions.
The predominately non-significant correlations between different balance components and mobility imply that balance and mobility performance is task specific. Further, strength and balance/mobility as well as balance under single and dual task conditions seem to be independent of each other and may have to be tested and trained complementarily.
Soil moisture estimation under low vegetation cover using a multi-angular polarimetric decomposition
(2013)
The estimation of volumetric soil moisture under low agricultural vegetation from fully polarimetric synthetic aperture radar (SAR) data at L-band using a multi-angular polarimetric decomposition is investigated. Radar polarimetry provides the framework to decompose the backscattered signal into different canonical scattering mechanisms referring to scattering contributions from the underlying soil and the vegetation cover. Multiangular observation diversity further increases the information space for soil moisture inversion enabling higher inversion rates and a stable inversion performance. The developed approach was applied on the multi-angular L-band data set acquired by German Aerospace Center's ESAR sensor as part of the OPAQUE campaign in 2008. The obtained results are compared against ground measurements collected by the OPAQUE team over a variety of vegetated agricultural fields. The validation of the estimated against ground measured soil moisture results in an root mean square error level of 6-8 vol.% including all test fields with a variety of crop types.
Prinz, Julia ; Schreiber, Benjamin ; Olejko, Lydia ; Oertel, Jana ; Rackwitz, Jenny ; Keller, Adrian ; Bald, Ilko
DNA nanotechnology holds great promise for the fabrication of novel plasmonic nanostructures and the potential to carry out single-molecule measurements using optical spectroscopy. Here, we demonstrate for the first time that DNA origami nanostructures can be exploited as substrates for surface-enhanced Raman scattering (SERS). Gold nanoparticles (AuNPs) have been arranged into dimers to create intense Raman scattering hot spots in the interparticle gaps. AuNPs (15 nm) covered with TAMRA-modified DNA have been placed at a nominal distance of 25 nm to demonstrate the formation of Raman hot spots. To control the plasmonic coupling between the nanoparticles and thus the field enhancement in the hot spot, the size of AuNPs has been varied from 5 to 28 nm by electroless Au deposition. By the precise positioning of a specific number of TAMRA molecules in these hot spots, SERS with the highest sensitivity down to the few-molecule level is obtained.
Salert, Beatrice Ch. D. ; Krueger, Hartmut ; Bagnich, Sergey A. ; Unger, Thomas ; Jaiser, Frank ; Al-Sa'di, Mahmoud ; Neher, Dieter ; Hayer, Anna ; Eberle, Thomas
A new matrix system for phosphorescent organic light-emitting diodes (OLEDs) based on an electron transporting component attached to an inert polymer backbone, an electronically neutral co-host, and a phosphorescent dye that serves as both emitter and hole conductor are presented. The inert co-host is used either as small molecules or covalently connected to the same chain as the electron-transporting host. The use of a small molecular inert co-host in the active layer is shown to be highly advantageous in comparison to a purely polymeric matrix bearing the same functionalities. Analysis of the dye phosphorescence decay in pure polymer, small molecular co-host film, and their blend lets to conclude that dye molecules distribute mostly in the small molecular co-host phase, where the co-host prevents agglomeration and self-quenching of the phosphorescence as well as energy transfer to the electron transporting units. In addition, the co-host accumulates at the anode interface where it acts as electron blocking layer and improves hole injection. This favorable phase separation between polymeric and small molecular components results in devices with efficiencies of about 47 cd/A at a luminance of 1000 cd/m(2). Investigation of OLED degradation demonstrates the presence of two time regimes: one fast component that leads to a strong decrease at short times followed by a slower decrease at longer times. Unlike the long time degradation, the efficiency loss that occurs at short times is reversible and can be recovered by annealing of the device at 180 degrees C. We also show that the long-time degradation must be related to a change of the optical and electrical bulk properties.
Inal, Sahika ; Koelsch, Jonas D. ; Chiappisi, Leonardo ; Kraft, Mario ; Gutacker, Andrea ; Janietz, Dietmar ; Scherf, Ullrich ; Gradzielski, Michael ; Laschewsky, André ; Neher, Dieter
Aqueous mixtures of a coumarin-labeled non-ionic thermoresponsive copolymer and a cationic polythiophene exhibit marked changes in their fluorescence properties upon heating. At room temperature, emission from the label is significantly quenched due to energy transfer to the conjugated polyelectrolyte. Heating the mixture reduces the energy-transfer efficiency markedly, resulting in a clearly visible change of the emission color. Although the two macromolecules associate strongly at room temperature, the number of interacting sites is largely reduced upon the phase transition. Crucially, the intermolecular association does not suppress the responsiveness of the smart polymer, meaning that this concept should be applicable to chemo- or bioresponsive polymers with optical read-out, for example, as a sensor device.
Inal, Sahika ; Kölsch, Jonas D. ; Chiappisi, Leonardo ; Janietz, Dietmar ; Gradzielski, Michael ; Laschewsky, André ; Neher, Dieter
We demonstrate new fluorophore-labelled materials based on acrylamide and on oligo(ethylene glycol) (OEG) bearing thermoresponsive polymers for sensing purposes and investigate their thermally induced solubility transitions. It is found that the emission properties of the polarity-sensitive (solvatochromic) naphthalimide derivative attached to three different thermoresponsive polymers are highly specific to the exact chemical structure of the macromolecule. While the dye emits very weakly below the LCST when incorporated into poly(N-isopropylacrylamide) (pNIPAm) or into a polyacrylate backbone bearing only short OEG side chains, it is strongly emissive in polymethacrylates with longer OEG side chains. Heating of the aqueous solutions above their cloud point provokes an abrupt increase of the fluorescence intensity of the labelled pNIPAm, whereas the emission properties of the dye are rather unaffected as OEG-based polyacrylates and methacrylates undergo phase transition. Correlated with laser light scattering studies, these findings are ascribed to the different degrees of pre-aggregation of the chains at low temperatures and to the extent of dehydration that the phase transition evokes. It is concluded that although the temperature-triggered changes in the macroscopic absorption characteristics, related to large-scale alterations of the polymer chain conformation and aggregation, are well detectable and similar for these LCST-type polymers, the micro-environment provided to the dye within each polymer network differs substantially. Considering sensing applications, this finding is of great importance since the temperature-regulated fluorescence response of the polymer depends more on the macromolecular architecture than the type of reporter fluorophore.
Background The aging process results in a number of functional (e.g., deficits in balance and strength/power performance), neural (e.g., loss of sensory/motor neurons), muscular (e.g., atrophy of type-II muscle fibers in particular), and bone-related (e.g., osteoporosis) deteriorations. Traditionally, balance and/or lower extremity resistance training were used to mitigate these age-related deficits. However, the effects of resistance training are limited and poorly translate into improvements in balance, functional tasks, activities of daily living, and fall rates. Thus, it is necessary to develop and design new intervention programs that are specifically tailored to counteract age-related weaknesses. Recent studies indicate that measures of trunk muscle strength (TMS) are associated with variables of static/dynamic balance, functional performance, and falls (i.e., occurrence, fear, rate, and/or risk of falls). Further, there is preliminary evidence in the literature that core strength training (CST) and Pilates exercise training (PET) have a positive influence on measures of strength, balance, functional performance, and falls in older adults.
Objective The objectives of this systematic literature review are: (a) to report potential associations between TMS/trunk muscle composition and balance, functional performance, and falls in old adults, and (b) to describe and discuss the effects of CST/PET on measures of TMS, balance, functional performance, and falls in seniors.
Data Sources A systematic approach was employed to capture all articles related to TMS/trunk muscle composition, balance, functional performance, and falls in seniors that were identified using the electronic databases PubMed and Web of Science (1972 to February 2013).
Study Selection A systematic approach was used to evaluate the 582 articles identified for initial review. Cross-sectional (i.e., relationship) or longitudinal (i.e., intervention) studies were included if they investigated TMS and an outcome-related measure of balance, functional performance, and/or falls. In total, 20 studies met the inclusionary criteria for review.
Study Appraisal and Synthesis Methods Longitudinal studies were evaluated using the Physiotherapy Evidence Database (PEDro) scale. Effect sizes (ES) were calculated whenever possible. For ease of discussion, the 20 articles were separated into three groups [i.e., cross-sectional (n = 6), CST (n = 9), PET (n = 5)].
Results The cross-sectional studies reported small-to-medium correlations between TMS/trunk muscle composition and balance, functional performance, and falls in older adults. Further, CST and/or PET proved to be feasible exercise programs for seniors with high-adherence rates. Age-related deficits in measures of TMS, balance, functional performance, and falls can be mitigated by CST (mean strength gain = 30 %, mean effect size = 0.99; mean balance/functional performance gain = 23 %, mean ES = 0.88) and by PET (mean strength gain = 12 %, mean ES = 0.52; mean balance/functional performance gain = 18 %, mean ES = 0.71).
Limitations Given that the mean PEDro quality score did not reach the predetermined cut-off of >= 6 for the intervention studies, there is a need for more high-quality studies to explicitly identify the relevance of CST and PET to the elderly population.
Conclusions Core strength training and/or PET can be used as an adjunct or even alternative to traditional balance and/or resistance training programs for old adults. Further, CST and PET are easy to administer in a group setting or in individual fall preventive or rehabilitative intervention programs because little equipment and space is needed to perform such exercises.
Inal, Sahika ; Chiappisi, Leonardo ; Kölsch, Jonas D. ; Kraft, Mario ; Appavou, Marie-Sousai ; Scherf, Ullrich ; Wagner, Manfred ; Hansen, Michael Ryan ; Gradzielski, Michael ; Laschewsky, André ; Neher, Dieter
Aqueous mixtures of a dye-labeled non-ionic thermoresponsive copolymer and a conjugated cationic polyelectrolyte are shown to exhibit characteristic changes in fluorescence properties in response to temperature and to the presence of salts, enabling a double-stimuli responsiveness. In such mixtures at room temperature, i.e., well below the lower critical solution temperature (LCST), the emission of the dye is strongly quenched due to energy transfer to the polycation, pointing to supramolecular interactions between the two macromolecules. Increasing the concentration of salts weakens the interpolymer interactions, the extent of which is simultaneously monitored from the change in the relative emission intensity of the components. When the mixture is heated above its LCST, the transfer efficiency is significantly reduced, signaling a structural reorganization process, however, surprisingly only if the mixture contains salt ions. To elucidate the reasons behind such thermo- and ion-sensitive fluorescence characteristics, we investigate the effect of salts of alkali chlorides, in particular of NaCl, on the association behavior of these macromolecules before and after the polymer phase transition by a combination of UV-vis, fluorescence, and H-1 NMR spectroscopy with light scattering and small-angle neutron scattering measurements.
Lange, Ilja ; Kniepert, Juliane ; Pingel, Patrick ; Dumsch, Ines ; Allard, Sybille ; Janietz, Silvia ; Scherf, Ullrich ; Neher, Dieter
A detailed investigation of the open circuit voltage (V-OC) of organic bulk heterojunction solar cells comprising three different donor polymers and two different fullerene-based acceptors is presented. Bias amplified charge extraction (BACE) is combined with Kelvin Probe measurements to derive information on the relevant energetics in the blend. On the example of P3HT:PC70BM the influence of composition and preparation conditions on the relevant transport levels will be shown. Moderate upward shifts of the P3HT HOMO depending on crystallinity are observed, but contrarily to common believe, the dependence of V-OC on blend composition and thermal history is found to be largely determined by the change in the PCBM LUMO energy. Following this approach, we quantified the energetic contribution to the V-OC in blends with fluorinated polymers or higher adduct fullerenes.
Here we report a new and simple synthetic pathway to form ordered, hollow carbon nitride structures, using a cyanuric acid melamine (CM) complex in ethanol as a starting product. A detailed analysis of the optical and photocatalytic properties shows that optimum hollow carbon nitride structures are formed after 8 h of condensation. For this condensation time, we find a significantly reduced fluorescence intensity and lifetime, indicating the formation of new, nonradiative deactivation pathways, probably involving charge-transfer processes. Enhanced charge transfer is seen as well from a drastic increase of the photocatalytic activity in the degradation of rhodamine B dye, which is shown to proceed via photoinduced hole transfer. Moreover, we show that various CM morphologies can be obtained using different solvents, which leads to diverse ordered carbon nitride architectures. In all cases, the CM-C3N4 structures exhibited superior photocatalytic activity compared to the bulk material. The utilization of CM hydrogen-bonded complexes opens new opportunities for the significant improvement of carbon nitride synthesis, structure, and optical properties toward an efficient photoactive material for catalysis.
Hoffmann, Sebastian T. ; Jaiser, Frank ; Hayer, Anna ; Baessler, Heinz ; Unger, Thomas ; Athanasopoulos, Stavros ; Neher, Dieter ; Koehler, Anna
In order to unravel the intricate interplay between disorder effects, molecular reorganization, and charge carrier localization, a comprehensive study was conducted on hole transport in a series of conjugated alternating phenanthrene indenofluorene copolymers. Each polymer in the series contained one further comonomer comprising monoamines, diamines, or amine-free structures, whose influence on the electronic, optical, and charge transport properties was studied. The series covered a wide range of highest occupied molecular orbital (HOMO) energies as determined by cyclovoltammetry. The mobility, inferred from time-of-flight (ToF) experiments as a function of temperature and electric field, was found to depend exponentially on the HOMO energy. Since possible origins for this effect include energetic disorder, polaronic effects, and wave function localization, the relevant parameters were determined using a range of methods. Disorder and molecular reorganization were established first by an analysis of absorption and emission measurements and second by an analysis of the ToF measurements. In addition, density functional theory calculations were carried out to determine how localized or delocalized holes on a polymer chain are and to compare calculated reorganization energies with those that have been inferred from optical spectra. In summary, we conclude that molecular reorganization has little effect on the hole mobility in this system while both disorder effects and hole localization in systems with low-lying HOMOs are predominant. In particular, as the energetic disorder is comparable for the copolymers, the absolute value of the hole mobility at room temperature is determined by the hole localization associated with the triarylamine moieties.
Inal, Sahika ; Koelsch, Jonas D. ; Chiappisi, Leonardo ; Janietz, Dietmar ; Gradzielski, Michael ; Laschewsky, André ; Neher, Dieter
We demonstrate new fluorophore-labelled materials based on acrylamide and on oligo(ethylene glycol) (OEG) bearing thermoresponsive polymers for sensing purposes and investigate their thermally induced solubility transitions. It is found that the emission properties of the polarity-sensitive (solvatochromic) naphthalimide derivative attached to three different thermoresponsive polymers are highly specific to the exact chemical structure of the macromolecule. While the dye emits very weakly below the LCST when incorporated into poly(N-isopropylacrylamide) (pNIPAm) or into a polyacrylate backbone bearing only short OEG side chains, it is strongly emissive in polymethacrylates with longer OEG side chains. Heating of the aqueous solutions above their cloud point provokes an abrupt increase of the fluorescence intensity of the labelled pNIPAm, whereas the emission properties of the dye are rather unaffected as OEG-based polyacrylates and methacrylates undergo phase transition. Correlated with laser light scattering studies, these findings are ascribed to the different degrees of pre-aggregation of the chains at low temperatures and to the extent of dehydration that the phase transition evokes. It is concluded that although the temperature-triggered changes in the macroscopic absorption characteristics, related to large-scale alterations of the polymer chain conformation and aggregation, are well detectable and similar for these LCST-type polymers, the micro-environment provided to the dye within each polymer network differs substantially. Considering sensing applications, this finding is of great importance since the temperature-regulated fluorescence response of the polymer depends more on the macromolecular architecture than the type of reporter fluorophore.
Schubert, Marcel ; Preis, Eduard ; Blakesley, James C. ; Pingel, Patrick ; Scherf, Ullrich ; Neher, Dieter
To address the nature of charge transport and the origin of severe (intrinsic) trapping in electron-transporting polymers, transient and steady-state charge transport measurements have been conducted on the prototype donor/acceptor copolymer poly[2,7-(9,9-dialkyl-fluorene)-alt-5,5-(4',7'-di-2-thienyl-2',1',3'-benzothiadiazole)] (PFTBTT). A charge-generation layer technique is used to selectively address transport of the desired charge carrier type, to perform time-of-flight measurements on samples with < 200 nm thickness, and to combine the time-of-flight and the photocharge extraction by linearly increasing voltage (photo-CELIV) techniques to investigate charge carrier dynamics over a wide time range. Significant trapping of free electrons is observed in the bulk of dioctyl-substituted PFTBTT (alt-PF8TBTT), introducing a strong relaxation of the charge carrier mobility with time. We used Monte-Carlo simulation to simulate the measured transient data and found that all measurements can be modeled with a single parameter set, with the charge transport behavior determined by multiple trapping and detrapping of electrons in an exponential trap distribution. The influence of the concomitant mobility relaxation on the transient photocurrent characteristics in photo-CELIV experiments is discussed and shown to explain subtle features that were seen in former publications but were not yet assigned to electron trapping. Comparable studies on PFTBTT copolymers with chemical modifications of the side chains and backbone suggest that the observed electron trapping is not caused by a distinct chemical species but rather is related to interchain interactions.
Moderate doping leads to high performance of semiconductor/insulator polymer blend transistors
(2013)
Lu, Guanghao ; Blakesley, James C. ; Himmelberger, Scott ; Pingel, Patrick ; Frisch, Johannes ; Lieberwirth, Ingo ; Salzmann, Ingo ; Oehzelt, Martin ; Di Pietro, Riccardo ; Salleo, Alberto ; Koch, Norbert ; Neher, Dieter
Polymer transistors are being intensively developed for next-generation flexible electronics. Blends comprising a small amount of semiconducting polymer mixed into an insulating polymer matrix have simultaneously shown superior performance and environmental stability in organic field-effect transistors compared with the neat semiconductor. Here we show that such blends actually perform very poorly in the undoped state, and that mobility and on/off ratio are improved dramatically upon moderate doping. Structural investigations show that these blend layers feature nanometre-scale semiconductor domains and a vertical composition gradient. This particular morphology enables a quasi three-dimensional spatial distribution of semiconductor pathways within the insulating matrix, in which charge accumulation and depletion via a gate bias is substantially different from neat semiconductor, and where high on-current and low off-current are simultaneously realized in the stable doped state. Adding only 5 wt% of a semiconducting polymer to a polystyrene matrix, we realized an environmentally stable inverter with gain up to 60.
By means of optical spectroscopy, Kelvin probe, and conductivity measurements, we study the p-type doping of the donor polymer poly(3-hexylthiophene), P3HT, with the molecular acceptor tetrafluorotetracyanoquin-odimethane, F(4)TCNQ, covering a broad range of molar doping ratios from the ppm to the percent regime. Thorough quantitative analysis of the specific near-infrared absorption bands of ionized F(4)TCNQ reveals that almost every F(4)TCNQ dopant undergoes integer charge transfer with a P3HT site. However, only about 5% of these charge carrier pairs are found to dissociate and contribute a free hole for electrical conduction. The nonlinear behavior of the conductivity on doping ratio is rationalized by a numerical mobility model that accounts for the broadening of the energetic distribution of transport sites by the Coulomb potentials of ionized F(4)TCNQ dopants. DOI: 10.1103/PhysRevB.87.115209