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Aggregate formation in poly(3-hexylthiophene) depends on molecular weight, solvent, and synthetic method. The interplay of these parameters thus largely controls device performance. In order to obtain a quantitative understanding on how these factors control the resulting electronic properties of P3HT, we measured absorption in solution and in thin films as well as the resulting field effect mobility in transistors. By a detailed analysis of the absorption spectra, we deduce the fraction of aggregates formed, the excitonic coupling within the aggregates, and the conjugation length within the aggregates, all as a function of solvent quality for molecular weights from 5 to 19 kDa. From this, we infer in which structure the aggregated chains pack. Although the 5 kDa samples form straight chains, the 11 and 19 kDa chains are kinked or folded, with conjugation lengths that increase as the solvent quality reduces. There is a maximum fraction of aggregated chains (about 55 +/- 5%) that can be obtained, even for poor solvent quality. We show that inducing aggregation in solution leads to control of aggregate properties in thin films. As expected, the field-effect mobility correlates with the propensity to aggregation. Correspondingly, we find that a well-defined synthetic approach, tailored to give a narrow molecular weight distribution, is needed to obtain high field effect mobilities of up to 0.01 cm2/Vs for low molecular weight samples (=11 kDa), while the influence of synthetic method is negligible for samples of higher molecular weight, if low molecular weight fractions are removed by extraction.
The significance of biogenic silicon (BSi) pools as a key factor for the control of Si fluxes from terrestrial to aquatic ecosystems has been recognized for decades. However, while most research has been focused on phytogenic Si pools, knowledge of other BSi pools is still limited. We hypothesized that different BSi pools influence short-term changes in the water-soluble Si fraction in soils to different extents. To test our hypothesis we took plant (Calamagrostis epigejos, Phragmites australis) and soil samples in an artificial catchment in a post-mining landscape in the state of Brandenburg, Germany. We quantified phytogenic (phytoliths), protistic (diatom frustules and testate amoeba shells) and zoogenic (sponge spicules) Si pools as well as Tironextractable and water-soluble Si fractions in soils at the beginning (t(0)) and after 10 years (t(10)) of ecosystem development. As expected the results of Tiron extraction showed that there are no consistent changes in the amorphous Si pool at Chicken Creek (Huhnerwasser) as early as after 10 years. In contrast to t(0) we found increased water-soluble Si and BSi pools at t(10); thus we concluded that BSi pools are the main driver of short-term changes in water-soluble Si. However, because total BSi represents only small proportions of water-soluble Si at t(0) (< 2 %) and t(10) (2.8-4.3 %) we further concluded that smaller (< 5 mu m) and/or fragile phytogenic Si structures have the biggest impact on short-term changes in water-soluble Si. In this context, extracted phytoliths (> 5 mu m) only amounted to about 16% of total Si con-tents of plant materials of C. epigejos and P. australis at t(10); thus about 84% of small-scale and/or fragile phytogenic Si is not quantified by the used phytolith extraction method. Analyses of small-scale and fragile phytogenic Si structures are urgently needed in future work as they seem to represent the biggest and most reactive Si pool in soils. Thus they are the most important drivers of Si cycling in terrestrial biogeosystems.