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Absorption Tails of Donor
(2017)
In disordered organic semiconductors, the transfer of a rather localized charge carrier from one site to another triggers a deformation of the molecular structure quantified by the intramolecular relaxation energy. A similar structural relaxation occurs upon population of intermolecular charge-transfer (CT) states formed at organic electron donor (D)-acceptor (A) interfaces. Weak CT absorption bands for D A complexes occur at photon energies below the optical gaps of both the donors and the C-60 acceptor as a result of optical transitions from the neutral ground state to the ionic CT state. In this work, we show that temperature-activated intramolecular vibrations of the ground state play a major role in determining the line shape of such CT absorption bands. This allows us to extract values for the relaxation energy related to the geometry change from neutral to ionic CT complexes. Experimental values for the relaxation energies of 20 D:C-60 CT complexes correlate with values calculated within density functional theory. These results provide an experimental method for determining the polaron relaxation energy in solid-state organic D-A blends and show the importance of a reduced relaxation energy, which we introduce to characterize thermally activated CT processes.
Background: Self-harm is highly prevalent in adolescence, often serving an emotion regulation function. Social stressors such as bullying are associated with self-harm. The neurobiological background of the relationship between social stressors and self-harm needs to be further understood to inform prevention and therapy. Methods: Participants were members of an epidemiological cohort study. 130 female participants underwent the Trier Social Stress Test (TSST) at age 19. Of them, 21 reported a history of self-harm as assessed by the Youth Self Report. Psychiatric diagnoses were recorded. Results: Participants with a history of self-harm showed significantly lower blood cortisol levels throughout the TSST. Early psychosocial adversity did not significantly differ between groups with and without self-harm, with self-harming participants reporting more childhood adversities. Conclusion: These results add to the limited field of studies showing an altered HPA axis activity in females with self-harm. Future studies need to address the causal mechanisms behind this association.
We analyze the effects of covalent interactions in Ni 2p3d resonant inelastic X-ray scattering (RIXS) spectra from aqueous Ni2+ ions and find that the relative RIXS intensities of ligand-to-metal charge-transfer final states with respect to the ligand-field final states reflect the covalent mixing between Ni 3d and water orbitals. Specifically, the experimental intensity ratio at the Ni L-3-edge allows to determine that the Ni 3d orbitals have on average 5.5% of water character. We propose that 2p3d RIXS at the Ni L-3-edge can be utilized to quantify covalency in Ni complexes without the use of external references or simulations.
Global earthquake locations are often associated with very large systematic travel-time residuals even for clear arrivals, especially for regional and near-regional stations in subduction zones because of their strongly heterogeneous velocity structure. Travel-time corrections can drastically reduce travel-time residuals at regional stations and, in consequence, improve the relative location accuracy. We have extended the shrinking-box source-specific station terms technique to regional and teleseismic distances and adopted the algorithm for probabilistic, nonlinear, global-search location. We evaluated the potential of the method to compute precise relative hypocentre locations on a global scale. The method has been applied to two specific test regions using existing P- and pP-phase picks. The first data set consists of 3103 events along the Chilean margin and the second one comprises 1680 earthquakes in the Tonga-Fiji subduction zone. Pick data were obtained from the GEOFON earthquake bulletin, produced using data from all available, global station networks. A set of timing corrections varying as a function of source position was calculated for each seismic station. In this way, we could correct the systematic errors introduced into the locations by the inaccuracies in the assumed velocity structure without explicitly solving for a velocity model. Residual statistics show that the median absolute deviation of the travel-time residuals is reduced by 40-60 per cent at regional distances, where the velocity anomalies are strong. Moreover, the spread of the travel-time residuals decreased by similar to 20 per cent at teleseismic distances (>28 degrees). Furthermore, strong variations in initial residuals as a function of recording distance are smoothed out in the final residuals. The relocated catalogues exhibit less scattered locations in depth and sharper images of the seismicity associated with the subducting slabs. Comparison with a high-resolution local catalogue reveals that our relocation process significantly improves the hypocentre locations compared to standard locations.
Near-surface geophysical techniques are extensively used in a variety of engineering, environmental, geologic, and hydrologic applications. While many of these applications ask for detailed, quantitative models of selected material properties, geophysical data are increasingly used to estimate such target properties. Typically, this estimation procedure relies on a two-step workflow including (1) the inversion of geophysical data and (2) the petrophysical translation of the inverted parameter models into the target properties. Standard deterministic implementations of such a quantitative interpretation result in a single best-estimate model, often without considering and propagating the uncertainties related to the two steps. We address this problem by using a rather novel, particle-swarm-based global joint strategy for data inversion and by implementing Monte Carlo procedures for petrophysical property estimation. We apply our proposed workflow to crosshole ground-penetrating radar, P-, and S-wave data sets collected at a well-constrained test site for a detailed geotechnical characterization of unconsolidated sands. For joint traveltime inversion, the chosen global approach results in ensembles of acceptable velocity models, which are analyzed to appraise inversion-related uncertainties. Subsequently, the entire ensembles of inverted velocity models are considered to estimate selected petrophysical properties including porosity, bulk density, and elastic moduli via well-established petrophysical relations implemented in a Monte Carlo framework. Our results illustrate the potential benefit of such an advanced interpretation strategy; i.e., the proposed workflow allows to study how uncertainties propagate into the finally estimated property models, while concurrently we are able to study the impact of uncertainties in the used petrophysical relations (e.g., the influence of uncertain, user-specified parameters). We conclude that such statistical approaches for the quantitative interpretation of geophysical data can be easily extended and adapted to other applications and geophysical methods and might be an important step toward increasing the popularity and acceptance of geophysical tools in engineering practice.
The origin of flowers has puzzled plant biologists ever since Darwin referred to their sudden appearance in the fossil record as an abominable mystery. Flowers are considered to be an assembly of protective, attractive, and reproductive male and female leaf-like organs. Their origin cannot be understood by a morphological comparison to gymnosperms, their closest relatives, which develop separate male or female cones. Despite these morphological differences, gymnosperms and angiosperms possess a similar genetic toolbox consisting of phylogenetically related MADS domain proteins. Using ancestral MADS domain protein reconstruction, we trace the evolution of organ identity quartets along the stem lineage of crown angiosperms. We provide evidence that current floral quartets specifying male organ identity, which consist of four types of subunits, evolved from ancestral complexes of two types of subunits through gene duplication and integration of SEPALLATA proteins just before the origin of flowering plants. Our results suggest that protein interaction changes underlying this compositional shift were the result of a gradual and reversible evolutionary trajectory. Modeling shows that such compositional changes may have facilitated the evolution of the perfect, bisexual flower.
Veto player theory is a powerful approach to comparative politics. This article argues that the debate about its explanatory success would benefit from more systematic distinctions. The theory not only comes in different theoretical variants, it is also used in radically different ways empirically. Starting from recent debates about the ‘testing’ of theoretical models, the article distinguishes five ways in which theoretical models can be used empirically: contrastive, axiomatic, exploratory, presumptive and modular. The typology is applied to veto player theory and illustrated with exemplary studies and debates. The article concludes that each type raises different questions that should be answered in individual studies. Moreover, while veto player theory has an excellent track record on four empirical uses, the picture on its contrastive use is far more nuanced. More explicitly contrastive testing of the theory is desirable.
Ancient genomes have revolutionized our understanding of Holocene prehistory and, particularly, the Neolithic transition in western Eurasia. In contrast, East Asia has so far received little attention, despite representing a core region at which the Neolithic transition took place independently ~3 millennia after its onset in the Near East. We report genome-wide data from two hunter-gatherers from Devil’s Gate, an early Neolithic cave site (dated to ~7.7 thousand years ago) located in East Asia, on the border between Russia and Korea. Both of these individuals are genetically most similar to geographically close modern populations from the Amur Basin, all speaking Tungusic languages, and, in particular, to the Ulchi. The similarity to nearby modern populations and the low levels of additional genetic material in the Ulchi imply a high level of genetic continuity in this region during the Holocene, a pattern that markedly contrasts with that reported for Europe.
Physical size modulates the efficiency of digit comparison, depending on whether the relation of numerical magnitude and physical size is congruent or incongruent (Besner & Coltheart, Neuropsychologia, 17, 467–472, 1979), the number-size congruency effect (NSCE). In addition, Henik and Tzelgov (Memory & Cognition, 10, 389–395, 1982) first reported an NSCE for the reverse task of comparing the physical size of digits such that the numerical magnitude of digits modulated the time required to compare their physical sizes. Does the NSCE in physical comparisons simply reflect a number-mediated bias mechanism related to making decisions and selecting responses about the digit’s sizes? Alternatively, or in addition, the NSCE might indicate a true increase in the ability to discriminate small and large font sizes when these sizes are congruent with the digit’s symbolic numerical meaning, over and above response bias effects. We present a new research design that permits us to apply signal detection theory to a task that required observers to judge the physical size of digits. Our results clearly demonstrate that the NSCE cannot be reduced to mere response bias effects, and that genuine sensitivity gains for congruent number-size pairings contribute to the NSCE.
We show a connection between the CDE′ inequality introduced in Horn et al. (Volume doubling, Poincaré inequality and Gaussian heat kernel estimate for nonnegative curvature graphs. arXiv:1411.5087v2, 2014) and the CDψ inequality established in Münch (Li–Yau inequality on finite graphs via non-linear curvature dimension conditions. arXiv:1412.3340v1, 2014). In particular, we introduce a CDφψ inequality as a slight generalization of CDψ which turns out to be equivalent to CDE′ with appropriate choices of φ and ψ. We use this to prove that the CDE′ inequality implies the classical CD inequality on graphs, and that the CDE′ inequality with curvature bound zero holds on Ricci-flat graphs.