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Year of publication
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- English (75)
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- gamma rays: general (20)
- radiation mechanisms: non-thermal (13)
- ISM: supernova remnants (11)
- cosmic rays (11)
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Imaging CF3I conical intersection and photodissociation dynamics with ultrafast electron diffraction
(2018)
Yang, Jie ; Zhu, Xiaolei ; Wolf, Thomas J. A. ; Li, Zheng ; Nunes, João Pedro Figueira ; Coffee, Ryan ; Cryan, James P. ; Gühr, Markus ; Hegazy, Kareem ; Heinz, Tony F. ; Jobe, Keith ; Li, Renkai ; Shen, Xiaozhe ; Veccione, Theodore ; Weathersby, Stephen ; Wilkin, Kyle J. ; Yoneda, Charles ; Zheng, Qiang ; Martinez, Todd J. ; Centurion, Martin ; Wang, Xijie
Conical intersections play a critical role in excited-state dynamics of polyatomic molecules because they govern the reaction pathways of many nonadiabatic processes. However, ultrafast probes have lacked sufficient spatial resolution to image wave-packet trajectories through these intersections directly. Here, we present the simultaneous experimental characterization of one-photon and two-photon excitation channels in isolated CF3I molecules using ultrafast gas-phase electron diffraction. In the two-photon channel, we have mapped out the real-space trajectories of a coherent nuclear wave packet, which bifurcates onto two potential energy surfaces when passing through a conical intersection. In the one-photon channel, we have resolved excitation of both the umbrella and the breathing vibrational modes in the CF3 fragment in multiple nuclear dimensions. These findings benchmark and validate ab initio nonadiabatic dynamics calculations.
Distinct cellular roles for PDCD10 define a gut-brain axis in cerebral cavernous malformation
(2019)
Tang, Alan T. ; Sullivan, Katie Rose ; Hong, Courtney C. ; Goddard, Lauren M. ; Mahadevan, Aparna ; Ren, Aileen ; Pardo, Heidy ; Peiper, Amy ; Griffin, Erin ; Tanes, Ceylan ; Mattei, Lisa M. ; Yang, Jisheng ; Li, Li ; Mericko-Ishizuka, Patricia ; Shen, Le ; Hobson, Nicholas ; Girard, Romuald ; Lightle, Rhonda ; Moore, Thomas ; Shenkar, Robert ; Polster, Sean P. ; Roedel, Claudia Jasmin ; Li, Ning ; Zhu, Qin ; Whitehead, Kevin J. ; Zheng, Xiangjian ; Akers, Amy ; Morrison, Leslie ; Kim, Helen ; Bittinger, Kyle ; Lengner, Christopher J. ; Schwaninger, Markus ; Velcich, Anna ; Augenlicht, Leonard ; Abdelilah-Seyfried, Salim ; Min, Wang ; Marchuk, Douglas A. ; Awad, Issam A. ; Kahn, Mark L.
Cerebral cavernous malformation (CCM) is a genetic, cerebrovascular disease. Familial CCM is caused by genetic mutations in KRIT1, CCM2, or PDCD10. Disease onset is earlier and more severe in individuals with PDCD10 mutations. Recent studies have shown that lesions arise from excess mitogen-activated protein kinase kinase kinase 3 (MEKK3) signaling downstream of Toll-like receptor 4 (TLR4) stimulation by lipopolysaccharide derived from the gut microbiome. These findings suggest a gut-brain CCM disease axis but fail to define it or explain the poor prognosis of patients with PDCD10 mutations. Here, we demonstrate that the gut barrier is a primary determinant of CCM disease course, independent of microbiome configuration, that explains the increased severity of CCM disease associated with PDCD10 deficiency. Chemical disruption of the gut barrier with dextran sulfate sodium augments CCM formation in a mouse model, as does genetic loss of Pdcd10, but not Krit1, in gut epithelial cells. Loss of gut epithelial Pdcd10 results in disruption of the colonic mucosal barrier. Accordingly, loss of Mucin-2 or exposure to dietary emulsifiers that reduce the mucus barrier increases CCM burden analogous to loss of Pdcd10 in the gut epithelium. Last, we show that treatment with dexamethasone potently inhibits CCM formation in mice because of the combined effect of action at both brain endothelial cells and gut epithelial cells. These studies define a gut-brain disease axis in an experimental model of CCM in which a single gene is required for two critical components: gut epithelial function and brain endothelial signaling.
Qu, J. Q. ; Zhang, J. Y. ; Grimsdale, A. C. ; Mullen, K. ; Jaiser, Frank ; Yang, X. H. ; Neher, Dieter
Aggregation of chromophores in the solid state commonly causes undesirable red shifts in the emission spectra and/or emission quenching. To overcome this problem, we have prepared soluble perylenetetracarboxidiimide dyes in which the chromophores are effectively shielded by polyphenylene dendrimers attached in the bay positions. Models show that attachment of the shielding units in the bay position should provide more efficient shielding than attaching them via the imide moieties. The dendrimers possess excellent film-forming properties due to alkyl substituents on their peripheries. The lack of a red shift in emission upon going from solution to the solid state indicates the dendrons suppress interaction of the emissive cores, leading to pure red-orange emission. Single-layer LEDs produce red-orange emission with relatively low efficiency especially for the higher generation dendrons, which is attributed to poor charge conduction. LEDs using blends of the dendrimers and the undendronized dye as a model compound in PVK have been investigated, and a model to extract relative charge injection rates through the dendritic scaffold from the spectral contributions in the EL spectra is developed
Huang, Wentao ; Jackson, Michael J. ; Dekkers, Mark J. ; Zhang, Yang ; Zhang, Bo ; Guo, Zhaojie ; Dupont-Nivet, Guillaume
Carbonate rocks, widely used for paleomagnetically quantifying the drift history of the Gondwana derived continental blocks of the Tibetan Plateau and evolution of the Paleo/Meso/Neo-Tethys Oceans, are prone to pervasive remagnetization. Identifying remagnetization is difficult because it is commonly undetectable through the classic paleomagnetic field tests. Here we apply comprehensive paleomagnetic, rock magnetic, and petrographic studies to upper Triassic limestones in the eastern Qiangtang block. Our results reveal that detrital/biogenic magnetite, which may carry the primary natural remanent magnetization (NRM), is rarely preserved in these rocks. In contrast, authigenic magnetite and hematite pseudomorphs after pyrite, and monoclinic pyrrhotite record three episodes of remagnetization. The earliest remagnetization was induced by oxidation of early diagenetic pyrite to magnetite, probably related to the collision between the northeastern Tibetan Plateau and the Qiangtang block after closure of the Paleo-Tethys Ocean in the Late Triassic. The second remagnetization, residing in hematite and minor goethite, which is the further subsurface oxidation product of pyrite/magnetite, is possibly related to the development of the localized Cenozoic basins soon after India-Asia collision in the Paleocene. The youngest remagnetization is a combination of thermoviscous and chemical remanent magnetization carried by authigenic magnetite and pyrrhotite, respectively. Our analyses suggest that a high supply of organic carbon during carbonate deposition, prevailing sulfate reducing conditions during early diagenesis, and widespread orogenic fluid migration related to crustal shortening during later diagenesis, have altered the primary remanence of the shallow-water Tethyan carbonate rocks of the Tibetan Plateau. We emphasize that all paleomagnetic results from these rocks must be carefully examined for remagnetization before being used for paleogeographic reconstructions. Future paleomagnetic investigations of the carbonate rocks in orogenic belts should be accompanied by thorough rock magnetic and petrographic studies to determine the origin of the NRM. (C) 2019 Elsevier B.V. All rights reserved.
Müller, Katharina ; Foerstendorf, Harald ; Steudtner, Robin ; Tsushima, Satoru ; Kumke, Michael Uwe ; Lefèvre, Grégory ; Rothe, Jörg ; Mason, Harris ; Szabó, Zoltán ; Yang, Ping ; Adam, Christian K. R. ; André, Rémi ; Brennenstuhl, Katlen ; Chiorescu, Ion ; Cho, Herman M. ; Creff, Gaëlle ; Coppin, Frédéric ; Dardenne, Kathy ; Den Auwer, Christophe ; Drobot, Björn ; Eidner, Sascha ; Hess, Nancy J. ; Kaden, Peter ; Kremleva, Alena ; Kretzschmar, Jerome ; Krüger, Sven ; Platts, James A. ; Panak, Petra ; Polly, Robert ; Powell, Brian A. ; Rabung, Thomas ; Redon, Roland ; Reiller, Pascal E. ; Rösch, Notker ; Rossberg, André ; Scheinost, Andreas C. ; Schimmelpfennig, Bernd ; Schreckenbach, Georg ; Skerencak-Frech, Andrej ; Sladkov, Vladimir ; Solari, Pier Lorenzo ; Wang, Zheming ; Washton, Nancy M. ; Zhang, Xiaobin
A comprehensive molecular analysis of a simple aqueous complexing system. U(VI) acetate. selected to be independently investigated by various spectroscopic (vibrational, luminescence, X-ray absorption, and nuclear magnetic resonance spectroscopy) and quantum chemical methods was achieved by an international round-robin test (RRT). Twenty laboratories from six different countries with a focus on actinide or geochemical research participated and contributed to this scientific endeavor. The outcomes of this RRT were considered on two levels of complexity: first, within each technical discipline, conformities as well as discrepancies of the results and their sources were evaluated. The raw data from the different experimental approaches were found to be generally consistent. In particular, for complex setups such as accelerator-based X-ray absorption spectroscopy, the agreement between the raw data was high. By contrast, luminescence spectroscopic data turned out to be strongly related to the chosen acquisition parameters. Second, the potentials and limitations of coupling various spectroscopic and theoretical approaches for the comprehensive study of actinide molecular complexes were assessed. Previous spectroscopic data from the literature were revised and the benchmark data on the U(VI) acetate system provided an unambiguous molecular interpretation based on the correlation of spectroscopic and theoretical results. The multimethodologic approach and the conclusions drawn address not only important aspects of actinide spectroscopy but particularly general aspects of modern molecular analytical chemistry.
Xu, Jingsan ; Cao, Shaowen ; Brenner, Thomas J. K. ; Yang, Xiaofei ; Yu, Jiaguo ; Antonietti, Markus ; Shalom, Menny
Here, a new method for enhancing the photoelectrochemical properties of carbon nitride thin films by in situ supramolecular-driven preorganization of phenyl-contained monomers in molten sulfur is reported. A detailed analysis of the chemical and photophysical properties suggests that the molten sulfur can texture the growth and induce more effective integration of phenyl groups into the carbon nitride electrodes, resulting in extended light absorption alongside with improved conductivity and better charge transfer. Furthermore, photophysical measurements indicate the formation of sub-bands in the optical bandgap which is beneficial for exciton splitting. Moreover, the new bands can mediate hole transfer to the electrolyte, thus improving the photooxidation activity. The utilization of high temperature solvent as the polymerization medium opens new opportunities for the significant improvement of carbon nitride films toward an efficient photoactive material for various applications.
The goal of China's sloping land conversion programme (SLCP) is to combat soil erosion and to reduce rural poverty. An ex-ante assessment of possible SLCP impacts was conducted with a focus on rural sustainability, taking the drought-prone region of Guyuan in Western China as an example. The Framework for Participatory Impact Assessment (FoPIA) was used to conduct two complementary impact assessments, one assessing SLCP impacts at regional level and a second one assessing alternative forest management options, to explore possible trade-offs among the economic, social and environmental dimensions of sustainability. Regional stakeholders assessed the SLCP to be capable of reducing soil erosion but felt it negatively affected rural employment, and a further continuation of the Programme was advocated. Assessment of three forest management scenarios by scientists showed that an orientation towards energy forests is potentially beneficial to all three sustainability dimensions. Ecological forests had disproportionate positive impacts on environmental functions and adverse impact on the other two sustainability dimensions. Economic forests were assessed to serve primarily the economic and social sustainability dimensions, while environmental impacts were still tolerable. The FoPIA results were evaluated against the available literature on the SLCP. Overall, the assessment results appeared to be reasonable, but the results of the regional stakeholders appeared to be too optimistic compared with the more critical assessment of the scientists. The SLCP seems to have the potential to tackle soil erosion but requires integrated forest management to minimize the risk of water stress while contributing to economic and social benefits in Guyuan. Copyright (C) 2012 John Wiley & Sons, Ltd.
Li, Chenhong ; Corrigan, Shannon ; Yang, Lei ; Straube, Nicolas ; Harris, Mark ; Hofreiter, Michael ; White, William T. ; Naylor, Gavin J. P.
For over a hundred years, the "river sharks" of the genus Glyphis were only known from the type specimens of species that had been collected in the 19th century. They were widely considered extinct until populations of Glyphis-like sharks were rediscovered in remote regions of Borneo and Northern Australia at the end of the 20th century. However, the genetic affinities between the newly discovered Glyphis-like populations and the poorly preserved, original museum-type specimens have never been established. Here, we present the first (to our knowledge) fully resolved, complete phylogeny of Glyphis that includes both archival-type specimens and modern material. We used a sensitive DNA hybridization capture method to obtain complete mitochondrial genomes from all of our samples and show that three of the five described river shark species are probably conspecific and widely distributed in Southeast Asia. Furthermore we show that there has been recent gene flow between locations that are separated by large oceanic expanses. Our data strongly suggest marine dispersal in these species, overturning the widely held notion that river sharks are restricted to freshwater. It seems that species in the genus Glyphis are euryhaline with an ecology similar to the bull shark, in which adult individuals live in the ocean while the young grow up in river habitats with reduced predation pressure. Finally, we discovered a previously unidentified species within the genus Glyphis that is deeply divergent from all other lineages, underscoring the current lack of knowledge about the biodiversity and ecology of these mysterious sharks.
The selaginella genome identifies genetic changes associated with the evolution of vascular plants
(2011)
Banks, Jo Ann ; Nishiyama, Tomoaki ; Hasebe, Mitsuyasu ; Bowman, John L. ; Gribskov, Michael ; dePamphilis, Claude ; Albert, Victor A. ; Aono, Naoki ; Aoyama, Tsuyoshi ; Ambrose, Barbara A. ; Ashton, Neil W. ; Axtell, Michael J. ; Barker, Elizabeth ; Barker, Michael S. ; Bennetzen, Jeffrey L. ; Bonawitz, Nicholas D. ; Chapple, Clint ; Cheng, Chaoyang ; Correa, Luiz Gustavo Guedes ; Dacre, Michael ; DeBarry, Jeremy ; Dreyer, Ingo ; Elias, Marek ; Engstrom, Eric M. ; Estelle, Mark ; Feng, Liang ; Finet, Cedric ; Floyd, Sandra K. ; Frommer, Wolf B. ; Fujita, Tomomichi ; Gramzow, Lydia ; Gutensohn, Michael ; Harholt, Jesper ; Hattori, Mitsuru ; Heyl, Alexander ; Hirai, Tadayoshi ; Hiwatashi, Yuji ; Ishikawa, Masaki ; Iwata, Mineko ; Karol, Kenneth G. ; Koehler, Barbara ; Kolukisaoglu, Uener ; Kubo, Minoru ; Kurata, Tetsuya ; Lalonde, Sylvie ; Li, Kejie ; Li, Ying ; Litt, Amy ; Lyons, Eric ; Manning, Gerard ; Maruyama, Takeshi ; Michael, Todd P. ; Mikami, Koji ; Miyazaki, Saori ; Morinaga, Shin-ichi ; Murata, Takashi ; Müller-Röber, Bernd ; Nelson, David R. ; Obara, Mari ; Oguri, Yasuko ; Olmstead, Richard G. ; Onodera, Naoko ; Petersen, Bent Larsen ; Pils, Birgit ; Prigge, Michael ; Rensing, Stefan A. ; Mauricio Riano-Pachon, Diego ; Roberts, Alison W. ; Sato, Yoshikatsu ; Scheller, Henrik Vibe ; Schulz, Burkhard ; Schulz, Christian ; Shakirov, Eugene V. ; Shibagaki, Nakako ; Shinohara, Naoki ; Shippen, Dorothy E. ; Sorensen, Iben ; Sotooka, Ryo ; Sugimoto, Nagisa ; Sugita, Mamoru ; Sumikawa, Naomi ; Tanurdzic, Milos ; Theissen, Guenter ; Ulvskov, Peter ; Wakazuki, Sachiko ; Weng, Jing-Ke ; Willats, William W. G. T. ; Wipf, Daniel ; Wolf, Paul G. ; Yang, Lixing ; Zimmer, Andreas D. ; Zhu, Qihui ; Mitros, Therese ; Hellsten, Uffe ; Loque, Dominique ; Otillar, Robert ; Salamov, Asaf ; Schmutz, Jeremy ; Shapiro, Harris ; Lindquist, Erika ; Lucas, Susan ; Rokhsar, Daniel ; Grigoriev, Igor V.
Vascular plants appeared similar to 410 million years ago, then diverged into several lineages of which only two survive: the euphyllophytes (ferns and seed plants) and the lycophytes. We report here the genome sequence of the lycophyte Selaginella moellendorffii (Selaginella), the first nonseed vascular plant genome reported. By comparing gene content in evolutionarily diverse taxa, we found that the transition from a gametophyte- to a sporophyte-dominated life cycle required far fewer new genes than the transition from a nonseed vascular to a flowering plant, whereas secondary metabolic genes expanded extensively and in parallel in the lycophyte and angiosperm lineages. Selaginella differs in posttranscriptional gene regulation, including small RNA regulation of repetitive elements, an absence of the trans-acting small interfering RNA pathway, and extensive RNA editing of organellar genes.
Chepkirui, Carolyne ; Ochieng, Purity J. ; Sarkar, Biswajyoti ; Hussain, Aabid ; Pal, Chiranjib ; Yang, Li Jun ; Coghi, Paolo ; Akala, Hoseah M. ; Derese, Solomon ; Ndakala, Albert ; Heydenreich, Matthias ; Wong, Vincent K. W. ; Erdelyi, Mate ; Yenesew, Abiy
Five known compounds (1-5) were isolated from the extract of Mundulea sericea leaves. Similar investigation of the roots of this plant afforded an additional three known compounds (6-8). The structures were elucidated using NMR spectroscopic and mass spectrometric analyses. The absolute configuration of 1 was established using ECD spectroscopy. In an antiplasmodial activity assay, compound 1 showed good activity with an IC50 of 2.0 mu M against chloroquine-resistant W2, and 6.6 mu M against the chloroquine-sensitive 3D7 strains of Plasmodium falciparum. Some of the compounds were also tested for antileishmanial activity. Dehydrolupinifolinol (2) and sericetin (5) were active against drug-sensitive Leishmania donovani (MHOM/IN/83/AG83) with IC50 values of 9.0 and 5.0 mu M, respectively. In a cytotoxicity assay, lupinifolin (3) showed significant activity on BEAS-2B (IC50 4.9 mu M) and HePG2 (IC50 10.8 mu M) human cell lines. All the other compounds showed low cytotoxicity (IC50 > 30 mu M) against human lung adenocarcinoma cells (A549), human liver cancer cells (HepG2), lung/bronchus cells (epithelial virus transformed) (BEAS-2B) and immortal human hepatocytes (LO2)