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The photochemical ring-opening of 1,3-cyclohexadiene imaged by ultrafast electron diffraction
(2019)
The ultrafast photoinduced ring-opening of 1,3-cyclohexadiene constitutes a textbook example of electrocyclic reactions in organic chemistry and a model for photobiological reactions in vitamin D synthesis. Although the relaxation from the photoexcited electronic state during the ring-opening has been investigated in numerous studies, the accompanying changes in atomic distance have not been resolved. Here we present a direct and unambiguous observation of the ring-opening reaction path on the femtosecond timescale and subangstrom length scale using megaelectronvolt ultrafast electron diffraction. We followed the carbon-carbon bond dissociation and the structural opening of the 1,3-cyclohexadiene ring by the direct measurement of time-dependent changes in the distribution of interatomic distances. We observed a substantial acceleration of the ring-opening motion after internal conversion to the ground state due to a steepening of the electronic potential gradient towards the product minima. The ring-opening motion transforms into rotation of the terminal ethylene groups in the photoproduct 1,3,5-hexatriene on the subpicosecond timescale.
The Brassicaceae, including Arabidopsis thaliana and Brassica crops, is unmatched among plants in its wealth of genomic and functional molecular data and has long served as a model for understanding gene, genome, and trait evolution. However, genome information from a phylogenetic outgroup that is essential for inferring directionality of evolutionary change has been lacking. We therefore sequenced the genome of the spider flower (Tarenaya hassleriana) from the Brassicaceae sister family, the Cleomaceae. By comparative analysis of the two lineages, we show that genome evolution following ancient polyploidy and gene duplication events affect reproductively important traits. We found an ancient genome triplication in Tarenaya (Th-alpha) that is independent of the Brassicaceae-specific duplication (At-alpha) and nested Brassica (Br-a) triplication. To showcase the potential of sister lineage genome analysis, we investigated the state of floral developmental genes and show Brassica retains twice as many floral MADS (for MINICHROMOSOME MAINTENANCE1, AGAMOUS, DEFICIENS and SERUM RESPONSE FACTOR) genes as Tarenaya that likely contribute to morphological diversity in Brassica. We also performed synteny analysis of gene families that confer self-incompatibility in Brassicaceae and found that the critical SERINE RECEPTOR KINASE receptor gene is derived from a lineage-specific tandem duplication. The T. hassleriana genome will facilitate future research toward elucidating the evolutionary history of Brassicaceae genomes.
Force-free equilibria containing two vertically arranged magnetic flux ropes of like chirality and current direction are considered as a model for split filaments/prominences and filament-sigmoid systems. Such equilibria are constructed analytically through an extension of the methods developed in Titov & Demoulin and numerically through an evolutionary sequence including shear flows, flux emergence, and flux cancellation in the photospheric boundary. It is demonstrated that the analytical equilibria are stable if an external toroidal (shear) field component exceeding a threshold value is included. If this component decreases sufficiently, then both flux ropes turn unstable for conditions typical of solar active regions, with the lower rope typically becoming unstable first. Either both flux ropes erupt upward, or only the upper rope erupts while the lower rope reconnects with the ambient flux low in the corona and is destroyed. However, for shear field strengths staying somewhat above the threshold value, the configuration also admits evolutions which lead to partial eruptions with only the upper flux rope becoming unstable and the lower one remaining in place. This can be triggered by a transfer of flux and current from the lower to the upper rope, as suggested by the observations of a split filament in Paper I. It can also result from tether-cutting reconnection with the ambient flux at the X-type structure between the flux ropes, which similarly influences their stability properties in opposite ways. This is demonstrated for the numerically constructed equilibrium.
Slow rise and partial eruption of a double-decker filament. I. observations and interpretation
(2012)
We study an active-region dextral filament that was composed of two branches separated in height by about 13 Mm, as inferred from three-dimensional reconstruction by combining SDO and STEREO-B observations. This "double-decker" configuration sustained for days before the upper branch erupted with a GOES-class M1.0 flare on 2010 August 7. Analyzing this evolution, we obtain the following main results. (1) During the hours before the eruption, filament threads within the lower branch were observed to intermittently brighten up, lift upward, and then merge with the upper branch. The merging process contributed magnetic flux and current to the upper branch, resulting in its quasi-static ascent. (2) This transfer might serve as the key mechanism for the upper branch to lose equilibrium by reaching the limiting flux that can be stably held down by the overlying field or by reaching the threshold of the torus instability. (3) The erupting branch first straightened from a reverse S shape that followed the polarity inversion line and then writhed into a forward S shape. This shows a transfer of left-handed helicity in a sequence of writhe-twist-writhe. The fact that the initial writhe is converted into the twist of the flux rope excludes the helical kink instability as the trigger process of the eruption, but supports the occurrence of the instability in the main phase, which is indeed indicated by the very strong writhing motion. (4) A hard X-ray sigmoid, likely of coronal origin, formed in the gap between the two original filament branches in the impulsive phase of the associated flare. This supports a model of transient sigmoids forming in the vertical flare current sheet. (5) Left-handed magnetic helicity is inferred for both branches of the dextral filament. (6) Two types of force-free magnetic configurations are compatible with the data, a double flux rope equilibrium and a single flux rope situated above a loop arcade.
We have developed lists of likely B3-A0 stars (called "late B" stars) in the young cluster Trumpler 16. The following criteria were used: location within 3' of eta Car, an appropriate V and B - V combination, and proper motion (where available). Color and magnitude cuts have been made assuming an E(B - V) = 0.55 mag +/- 0.1, which is a good approximation close to the center of Trumpler 16. These lists have been cross-correlated with X-ray sources found in the Chandra Carina Complex Project. Previous studies have shown that only very rarely (if at all) do late main-sequence B stars produce X-rays. We present evidence that the X-ray-detected sources are binaries with low-mass companions, since stars less massive than 1.4 M-circle dot are strong X-ray sources at the age of the cluster. Both the median X-ray energies and X-ray luminosities of these sources are in good agreement with values for typical low-mass coronal X-ray sources. We find that 39% of the late B stars based on a list with proper motions have low-mass companions. Similarly, 32% of a sample without proper motions have low-mass companions. We discuss the X-ray detection completeness. These results on low-mass companions of intermediate-mass stars are complementary to spectroscopic and interferometric results and probe new parameter space of low-mass companions at all separations. They do not support a steeply rising distribution of mass ratios to low masses for intermediate-mass (5 M-circle dot) primaries, such as would be found by random pairing from the initial mass function.
The largest uncertainty in projections of future sea-level change results from the potentially changing dynamical ice discharge from Antarctica. Basal ice-shelf melting induced by a warming ocean has been identified as a major cause for additional ice flow across the grounding line. Here we attempt to estimate the uncertainty range of future ice discharge from Antarctica by combining uncertainty in the climatic forcing, the oceanic response and the ice-sheet model response. The uncertainty in the global mean temperature increase is obtained from historically constrained emulations with the MAGICC-6.0 (Model for the Assessment of Greenhouse gas Induced Climate Change) model. The oceanic forcing is derived from scaling of the subsurface with the atmospheric warming from 19 comprehensive climate models of the Coupled Model Intercomparison Project (CMIP-5) and two ocean models from the EU-project Ice2Sea. The dynamic ice-sheet response is derived from linear response functions for basal ice-shelf melting for four different Antarctic drainage regions using experiments from the Sea-level Response to Ice Sheet Evolution (SeaRISE) intercomparison project with five different Antarctic ice-sheet models. The resulting uncertainty range for the historic Antarctic contribution to global sea-level rise from 1992 to 2011 agrees with the observed contribution for this period if we use the three ice-sheet models with an explicit representation of ice-shelf dynamics and account for the time-delayed warming of the oceanic subsurface compared to the surface air temperature. The median of the additional ice loss for the 21st century is computed to 0.07 m (66% range: 0.02-0.14 m; 90% range: 0.0-0.23 m) of global sea-level equivalent for the low-emission RCP-2.6 (Representative Concentration Pathway) scenario and 0.09 m (66% range: 0.04-0.21 m; 90% range: 0.01-0.37 m) for the strongest RCP-8.5. Assuming no time delay between the atmospheric warming and the oceanic subsurface, these values increase to 0.09 m (66% range: 0.04-0.17 m; 90% range: 0.02-0.25 m) for RCP-2.6 and 0.15 m (66% range: 0.07-0.28 m; 90% range: 0.04-0.43 m) for RCP-8.5. All probability distributions are highly skewed towards high values. The applied ice-sheet models are coarse resolution with limitations in the representation of grounding-line motion. Within the constraints of the applied methods, the uncertainty induced from different ice-sheet models is smaller than that induced by the external forcing to the ice sheets.
Colliding Wolf-Rayet (WR) winds produce thermal X-ray emission widely observed by X-ray telescopes. In wide WR+O binaries, such as WR 140, the X-ray flux is tied to the orbital phase, and is a direct probe of the winds’ properties. In the Galactic center, ~30 WRs orbit the super massive black hole (SMBH) within ~10”, leading to a smorgasbord of wind-wind collisions. To model the X-ray emission of WR 140 and the Galactic center, we perform 3D hydrodynamic simulations to trace the complex gaseous flows, and then carry out 3D radiative transfer calculations to compute the variable X-ray spectra. The model WR 140 RXTE light curve matches the data well for all phases except the X-ray minimum associated with periastron, while the model spectra agree with the RXTE hardness ratio and the shape of the Suzaku observations throughout the orbit. The Galactic center model of the Chandra flux and spectral shape match well in the region r ≤ 3”, but the model flux falls off too rapidly beyond this radius.
The thermal behavior of poly(methoxydiethylenglycol acrylate) (PMDEGA) is studied in thin hydrogel films on solid supports and is compared with the behavior in aqueous solution. The PMDEGA hydrogel film thickness is varied from 2 to 422 nm. Initially, these films are homogenous, as measured with optical microscopy, atomic force microscopy, X-ray reflectivity, and grazing-incidence small-angle X-ray scattering (GISAXS). However, they tend to de-wet when stored under ambient conditions. Along the surface normal, no long-ranged correlations between substrate and film surface are detected with GISAXS, due to the high mobility of the polymer at room temperature. The swelling of the hydrogel films as a function of the water vapor pressure and the temperature are probed for saturated water vapor pressures between 2,380 and 3,170 Pa. While the swelling capability is found to increase with water vapor pressure, swelling in dependence on the temperature revealed a collapse phase transition of a lower critical solution temperature type. The transition temperature decreases from 40.6 A degrees C to 36.6 A degrees C with increasing film thickness, but is independent of the thickness for very thin films below a thickness of 40 nm. The observed transition temperature range compares well with the cloud points observed in dilute (0.1 wt.%) and semi-dilute (5 wt.%) solution which decrease from 45 A degrees C to 39 A degrees C with increasing concentration.
Although quantitative isotope data from speleothems has been used to evaluate isotope-enabled model simulations, currently no consensus exists regarding the most appropriate methodology through which to achieve this. A number of modelling groups will be running isotope-enabled palaeoclimate simulations in the framework of the Coupled Model Intercomparison Project Phase 6, so it is timely to evaluate different approaches to using the speleothem data for data–model comparisons. Here, we illustrate this using 456 globally distributed speleothem δ18O records from an updated version of the Speleothem Isotopes Synthesis and Analysis (SISAL) database and palaeoclimate simulations generated using the ECHAM5-wiso isotope-enabled atmospheric circulation model. We show that the SISAL records reproduce the first-order spatial patterns of isotopic variability in the modern day, strongly supporting the application of this dataset for evaluating model-derived isotope variability into the past. However, the discontinuous nature of many speleothem records complicates the process of procuring large numbers of records if data–model comparisons are made using the traditional approach of comparing anomalies between a control period and a given palaeoclimate experiment. To circumvent this issue, we illustrate techniques through which the absolute isotope values during any time period could be used for model evaluation. Specifically, we show that speleothem isotope records allow an assessment of a model's ability to simulate spatial isotopic trends. Our analyses provide a protocol for using speleothem isotope data for model evaluation, including screening the observations to take into account the impact of speleothem mineralogy on δ18O values, the optimum period for the modern observational baseline and the selection of an appropriate time window for creating means of the isotope data for palaeo-time-slices.