bluuebunny/crossref_metadata_2025_split huggingface dataset:
Decadal hindcasts initialized using observed surface wind stress: Evaluation and prediction out to 2024
Authors: Thoma Malte , Greatbatch Richard J. , Kadow Christopher , Gerdes Ruediger 
Published: July 2015

AbstractWe use surface air temperature to evaluate the decadal forecast skill of the fully coupled Max Planck Institut Earth System Model (MPI‐ESM) initialized using only surface wind stress applied to the ocean component of the model (Modini: Model initialization by partially coupled spin‐up). Our analysis shows that the greenhouse gas forcing alone results in a significant forecast skill on the 2–5 and 6–9 year range even for uninitialized hindcasts. For the first forecast year, the forecast skill of Modini is generally comparable with previous initialization procedures applied to MPI‐ESM. But only Modini is able to generate a significant skill (correlation) in the tropical Pacific for a 2–5 year (and to a lesser extent for a 6–9 year) hindcast. Modini is also better able to capture the observed hiatus in global warming in hindcast mode than the other methods. Finally, we present forecasts for 2015 and the average of years 2016–2019 and 2020–2024, predicting an end to the hiatus.
Anatomy of an extinct magmatic system along a divergent plate boundary: Alftafjordur, Iceland
Authors: Urbani S. , Trippanera D. , Porreca M. , Kissel C. , Acocella V. 
Published: July 2015

AbstractRecent rifting episodes highlight the role of magmatic systems with propagating dikes on crustal spreading. However, our knowledge of magmatic systems is usually limited to surface observations and geophysical data. Eastern Iceland allows direct access to extinct and eroded deeper magmatic systems. Here we collected field structural and AMS (anisotropy of magnetic susceptibility) data on 187 and 19 dikes, respectively, in the 10–12 Ma old Alftafjordur magmatic system. At a paleodepth of ~1.5 km, the extension due to diking is at least 1–2 orders of magnitude larger than that induced by regional tectonics, confirming magmatism as the key mechanism for crustal spreading. This magma‐induced extension, inferred from the aspect ratio of the magmatic system, was of ~8 mm/yr, lower than the present one. AMS data suggest that most of dikes have geometrically normal fabric, at least at the margins, consistent with prevalent subvertical magma flow and propagation.
Down‐tail mass loss by plasmoids in Jupiter's and Saturn's magnetospheres
Authors: Cowley S. W. H. , Nichols J. D. , Jackman C. M. 
Published: July 2015

AbstractRecent estimates of the plasma mass‐loss rates by the formation and down‐tail propagation of plasmoids observed in the plasma sheet in Jupiter's and Saturn's magnetosphere fall short of inner moon source rates by at least an order of magnitude. Here we argue that on the time scale between large‐scale disconnection events, ~15 h at Jupiter and ~45 h at Saturn, mass‐loaded closed flux tubes will typically have stretched out a few hundred planetary radii down tail at speeds ~100–200 km s−1. Consequently, the “plasmoids” of order ~10 planetary radii in length observed at closer planetary distances represent only a small planetward portion of the overall structure that is disconnected and lost down tail. Plasmoid mass‐loss estimates are then revised upward by around an order of magnitude, becoming comparable to the moon source values. Additional “hidden,” e.g., small‐scale, mass‐loss processes of comparable strength may not then be required. The essentially continuous azimuthally flowing source plasma in the dusk sector is shown to correspond to a plasma sheet layer adjacent to the magnetopause of width typically ~10% of the distance to the magnetopause in that local time sector. This physical picture also provides a simple explanation for the asymmetry in the plasmoid bipolar field signature observed at both Jupiter and Saturn and predicts that the apparent plasmoid length will increase with distance down tail to a limit beyond a few hundred planetary radii where the full ~100–200 planetary radii structures will be observed.
An investigation of mineral dynamics in frozen seawater brines by direct measurement with synchrotron X‐ray powder diffraction
Authors: Butler Benjamin Miles , Kennedy Hilary 
Published: July 2015

AbstractFrozen seawater is a composite material with a sponge‐like structure. The framework of the structure is composed of pure ice, and within the pores exists a concentrated seawater brine. When the temperature is reduced, the volume of this residual brine decreases, while its salinity increases. As a result of the paired changes to temperature and salinity, the brine eventually becomes supersaturated with respect to a mineral, resulting in the precipitation of microscopic crystals throughout the ice structure. Due to experimental constraints, the current understanding about the formation of these minerals relies on the analysis of the residual brine, rather than the mineral phase. Here synchrotron X‐ray powder diffraction was used to assess the dynamics that occur between ice, brine, and mineral phases within frozen seawater brines that were subjected to cooling and warming at subzero temperatures. The method was able to detect crystalline phases of ice, mirabilite (Na2SO4·10H2O), and hydrohalite (NaCl·2H2O). Results illustrate a highly dynamic geochemical environment where ice‐brine‐mineral interactions tend toward an equilibrium crystallization process, which supports the process of seawater freezing that is described by the Gitterman Pathway and FREZCHEM model. This study highlights the power of synchrotron techniques in observing the mineralogical dynamics of inaccessible environmental systems.
Chesapeake Bay nitrogen fluxes derived from a land‐estuarine ocean biogeochemical modeling system: Model description, evaluation, and nitrogen budgets
Authors: Feng Yang , Friedrichs Marjorie A. M. , Wilkin John , Tian Hanqin , Yang Qichun , Hofmann Eileen E. , Wiggert Jerry D. , Hood Raleigh R. 
Published: July 2015

AbstractThe Chesapeake Bay plays an important role in transforming riverine nutrients before they are exported to the adjacent continental shelf. Although the mean nitrogen budget of the Chesapeake Bay has been previously estimated from observations, uncertainties associated with interannually varying hydrological conditions remain. In this study, a land‐estuarine‐ocean biogeochemical modeling system is developed to quantify Chesapeake riverine nitrogen inputs, within‐estuary nitrogen transformation processes and the ultimate export of nitrogen to the coastal ocean. Model skill was evaluated using extensive in situ and satellite‐derived data, and a simulation using environmental conditions for 2001–2005 was conducted to quantify the Chesapeake Bay nitrogen budget. The 5 year simulation was characterized by large riverine inputs of nitrogen (154 × 109 g N yr−1) split roughly 60:40 between inorganic:organic components. Much of this was denitrified (34 × 109 g N yr−1) and buried (46 × 109 g N yr−1) within the estuarine system. A positive net annual ecosystem production for the bay further contributed to a large advective export of organic nitrogen to the shelf (91 × 109 g N yr−1) and negligible inorganic nitrogen export. Interannual variability was strong, particularly for the riverine nitrogen fluxes. In years with higher than average riverine nitrogen inputs, most of this excess nitrogen (50–60%) was exported from the bay as organic nitrogen, with the remaining split between burial, denitrification, and inorganic export to the coastal ocean. In comparison to previous simulations using generic shelf biogeochemical model formulations inside the estuary, the estuarine biogeochemical model described here produced more realistic and significantly greater exports of organic nitrogen and lower exports of inorganic nitrogen to the shelf.
Partial Verbal Redundancy in Multimedia Presentations for Writing Strategy Instruction
Authors: Roscoe Rod D. , Jacovina Matthew E. , Harry Danielle , Russell Devin G. , McNamara Danielle S. 
Published: July 2015

SummaryMultimedia instructional materials require learners to select, organize, and integrate information across multiple modalities. To facilitate these comprehension processes, a variety of multimedia design principles have been proposed. This study further explores the redundancy principle by manipulating the degree of partial redundancy between written and narrated content. Ninety high school students learned about cohesion via animated lesson videos from the Writing Pal intelligent tutoring system. Videos were crafted such that narrated and onscreen written content overlapped by 10%, 26%, or 50%. Across conditions, students gained significantly in their knowledge of cohesion‐building strategies and the effects of cohesion on writing quality. However, degree of redundancy did not influence learning gains. Additionally, although more‐skilled readers outperformed less‐skilled readers, reading skill did not interact with the degree of redundancy. These results provide evidence that a broad range of partially redundant multimedia materials may be viable instructional tools that benefit diverse learners. Copyright © 2015 John Wiley & Sons, Ltd.
Diastereo‐ and Enantioselective Synthesis of Chiral Pyrrolidine‐Fused Spirooxindoles via Organocatalytic [3+2] 1,3‐Dipolar Cycloaddition of Azomethine Ylides with Maleimides
Authors: Zhao Hong‐Wu , Yang Zhao , Meng Wei , Tian Ting , Li Bo , Song Xiu‐Qing , Chen Xiao‐Qin , Pang Hai‐Liang 
Published: July 2015

AbstractIn the presence of a Cinchona alkaloid‐based squaramide organocatalyst, the [3+2] cycloaddition of isatin‐derived azomethine ylides with maleimides proceeded readily, thus delivering the desired pyrrolidine‐fused spirooxindoles in 61–89% yields with >20:1 dr and 12 to >99 % ee. The absolute configuration of 5‐chloro‐1,5′‐dimethyl‐3′‐phenyl‐3′,3a′‐dihydro‐2′H‐spiro[indoline‐3,1′‐pyrrolo[3,4‐c]pyrrole]‐2,4′,6′(5′H,6a′H)‐trione was unambiguously determined by means of X‐ray single crystal structure analysis. The reaction mechanism was hypothesized to account for the enantioselective formation of 5‐chloro‐1,5′‐dimethyl‐3′‐phenyl‐3′,3a′‐dihydro‐2′H‐spiro[indoline‐3,1′‐pyrrolo[3,4‐c]pyrrole]‐2,4′,6′(5′H,6a′H)‐trione.magnified image
Construction of Multifunctionalized Azopyrazoles by Silver‐ Catalyzed Cascade Reaction of Diazo Compounds
Authors: Pandit Rameshwar Prasad , Lee Yong Rok 
Published: July 2015

AbstractA variety of multisubstituted azopyrazoles were synthesized in good yield from an efficient one‐pot silver trifluoromethanesulfonate (AgOTf)‐catalyzed cascade reaction of α‐diazo‐β‐keto esters with two arylhydrazines or two arylhydrazine hydrochlorides. This cascade reaction included pyrazolone formation, NH insertion, and oxidation. For the synthesis of more diverse azopyrazoles bearing two different aromatic rings, the silver(I)‐catalyzed cascade reaction of 4‐diazopyrazol‐3‐one with arylhydrazine hydrochlorides was also developed. The advantages of these methodologies are easy handling, mild reaction conditions, and an effective and non‐toxic catalyst usage.magnified image
Weather Effects on Household Demand for Coffee and Tea in Japan
Authors: Yohannes Michael Fesseha , Matsuda Toshinobu 
Published: July 2015

ABSTRACTThis paper estimates the weather effects on household demand for coffee and tea in Japan using the linear approximate quadratic almost ideal demand system model (LA/QUAIDS). Five expenditure shares and prices demand equations for coffee and tea group: green tea, black tea, tea beverage, coffee, and coffee beverage are estimated for two or more households in 49 cities, for the period January 2000 through March 2012. Empirical results show that demand for green tea, black tea, and tea beverage are own‐price elastic while coffee and coffee beverage are own‐price inelastic. The expenditure elasticity estimates that green tea and black tea are luxuries, while tea beverage, coffee and coffee beverage are necessities in the Japanese household. In addition, temperature has a positive effect on demand for tea beverage and coffee beverage and has a negative effect on green tea, black tea and coffee throughout the year. [EconLit citations: D12, Q11].
Long‐term follow‐up of imatinib plus combination chemotherapy in patients with newly diagnosed Philadelphia chromosome‐positive acute lymphoblastic leukemia
Authors: Lim Sung‐Nam , Joo Young‐Don , Lee Kyoo‐Hyung , Kim Dae‐Young , Lee Je‐Hwan , Lee Jung‐Hee , Chi Hyun‐Sook , Yun Sung‐Cheol , Lee Won Sik , Lee Sang Min , Park Seonyang , Kim Inho , Sohn Sang Kyun , Moon Joon Ho , Ryoo Hun‐Mo , Bae Sung Hwa , Hyun Myung Soo , Kim Min Kyoung , Kim Hyeoung Joon , Yang Deok‐Hwan , Eom1 Hyeon‐Seok , Lee Gyeong‐Won , Jung Chul Won , Won Jong‐Ho , Kim Hawk , Lee Jae‐Hoon , Shin Ho‐Jin , Jang Dae‐Young 
Published: July 2015

The effects of imatinib plus chemotherapy were assessed in 87 patients with newly diagnosed Philadelphia chromosome‐positive (Ph+) acute lymphoblastic leukemia (ALL). Imatinib was administered continuously, starting from the eighth day of remission induction chemotherapy, then through five courses of consolidation or until allogeneic hematopoietic cell transplantation (HCT). Patients who were not transplanted were maintained on imatinib for 2 years. Eighty‐two patients (94.3%) achieved complete remission (CR). Among these 82 CR patients, 40 experienced recurrence of leukemia. The 5‐year relapse free survival (RFS) rate and overall survival (OS) rates were 39.0% and 33.4%, respectively. In total, 56 patients underwent allogeneic HCT in first CR. The 5‐year cumulative incidence of relapse and OS rate of them were 59.1% and 52.6%, respectively. Six of seven patients who were maintained on imatinib after completion of consolidation relapsed and the median time of RFS was 40.7 months. In total patient, cumulative molecular CR rate was 88.5% and median time of molecular CR duration was 13 months. Initial imatinib dose intensity was significantly associated with median CR duration (P < 0.0001), and overall survival (P = 0.002). During the initial phase of treatment of patients with Ph+ ALL, it is important to maintain imatinib dose intensity. Am. J. Hematol. 90:1013–1020, 2015. © 2015 Wiley Periodicals, Inc.
On the influence of underdamped vibrations on coherence and energy transfer times in light‐harvesting complexes
Authors: Mujica‐Martinez C. A. , Nalbach P. 
Published: July 2015

We study the quantum exciton dynamics in light‐harvesting complexes under the influence of underdamped vibrational molecular modes. We observe prolonged coherent population oscillations between different pigments due to an underdamped mode connected to the originally excited pigment. At the same time, an underdamped vibration at the exit site of the complex provides additional channels for the excitation energy transfer towards the reaction center which shortens the transfer times.
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Direct Ruthenium‐Catalyzed Hydrogenation of Carboxylic Acids to Alcohols
Authors: Cui Xinjiang , Li Yuehui , Topf Christoph , Junge Kathrin , Beller Matthias 
Published: July 2015

AbstractThe “green” reduction of carboxylic acids to alcohols is a challenging task in organic chemistry. Herein, we describe a general protocol for generation of alcohols by catalytic hydrogenation of carboxylic acids. Key to success is the use of a combination of Ru(acac)3, triphos and Lewis acids. The novel method showed broad substrate tolerance and a variety of aliphatic carboxylic acids including biomass‐derived compounds can be smoothly reduced.
An Activity‐Based Probe for Studying Crosslinking in Live Bacteria
Authors: Gautam Samir , Kim Taehan , Shoda Takuji , Sen Sounok , Deep Deeksha , Luthra Ragini , Ferreira Maria Teresa , Pinho Mariana G. , Spiegel David A. 
Published: July 2015

AbstractPenicillin‐binding proteins (PBPs) catalyze the crosslinking of peptidoglycan (PG), an essential process for bacterial growth and survival, and a common antibiotic target. Yet, despite its importance, little is known about the spatiotemporal aspects of crosslinking—largely because of a lack of experimental tools for studying the reaction in live bacteria. Here we introduce such a tool: an activity‐based probe that enables visualization and relative quantitation of crosslinking in vivo. In Staphylococcus aureus, we show that fluorescent mimics of the natural substrate of PBPs (PG stem peptide) are covalently incorporated into the cell wall, installing fluorophores in place of natural crosslinks. These fluorescent stem peptide mimics (FSPMs) are selectively recognized by a single PBP in S. aureus: PBP4. Thus, we were able to use FSPM pulse‐labeling to localize PBP4 activity in live cells, showing that it is recruited to the septum in a manner dependent on wall teichoic acid.
A Thiol–Ene Coupling Approach to Native Peptide Stapling and Macrocyclization
Authors: Wang Yuanxiang , Chou Danny Hung‐Chieh 
Published: July 2015

AbstractWe report the discovery of a peptide stapling and macrocyclization method using thiol–ene reactions between two cysteine residues and an α,ω‐diene in high yields. This new approach enabled us to selectively modify cysteine residues in native, unprotected peptides with a variety of stapling modifications for helix stabilization or general macrocyclization. We synthesized stapled Axin mimetic analogues and demonstrated increased alpha helicity upon peptide stapling. We then synthesized stapled p53 mimetic analogues using pure hydrocarbon linkers and demonstrated their abilities to block the p53‐MDM2 interaction and selectively kill p53 wild‐type colorectal carcinoma HCT‐116 cells but not p53 null cells. In summary, we demonstrated a robust and versatile peptide stapling method that could be potentially applied to both synthetic and expressed peptides.
RhIII‐katalysierte C‐H‐Aktivierung mit Pyridotriazolen: direkter Zugang zu Fluorophoren zur Metallerkennung
Authors: Kim Ju Hyun , Gensch Tobias , Zhao Dongbing , Stegemann Linda , Strassert Cristian A. , Glorius Frank 
Published: July 2015

AbstractDie erste C‐H‐Aktivierung mit Pyridotriazolen als Kupplungspartner wurde mit einem RhIII‐Katalysator verwirklicht. Die Pyridotriazole können dabei als neue Carbenvorstufen in der C‐H‐Aktivierung genutzt werden, um gezielt neue fluoreszierende Strukturen zu synthetisieren. Diese Fluorophore mit wählbaren Eigenschaften können zur Detektion von Metallionen genutzt werden.
Biomimetic Total Synthesis of (−)‐Penibruguieramine A Using Memory of Chirality and Dynamic Kinetic Resolution
Authors: Kim Jae Hyun , Lee Seokwoo , Kim Sanghee 
Published: July 2015

AbstractThe fully stereocontrolled total synthesis of (−)‐penibruguieramine A, a naturally occurring marine pyrrolizidine alkaloid, is described in this study for the first time. The key synthetic sequence is the biomimetic aldol reaction of the proline pentaketide amide. The principles of “memory of chirality” (MOC) and “dynamic kinetic resolution” (DKR) are applied to this reaction for the asymmetric synthesis using proline as the only chiral source. A mechanistic rationale is discussed for the excellent stereochemical outcome in a protic solvent environment.
Controllable Chemoselectivity in Visible‐Light Photoredox Catalysis: Four Diverse Aerobic Radical Cascade Reactions
Authors: Liu Xinfei , Ye Xinyi , Bureš Filip , Liu Hongjun , Jiang Zhiyong 
Published: July 2015

AbstractReported is the controllable selectivity syntheses of four distinct products from the same starting materials by visible‐light photoredox catalysis. By employing a dicyanopyrazine‐derived chromophore (DPZ) as photoredox catalyst, an aerobic radical mechanism has been developed, and allows the reactions of N‐tetrahydroisoquinolines (THIQs) with N‐itaconimides to through four different pathways, including addition‐cyclization, addition‐elimination, addition‐coupling, and addition‐protonation, with satisfactory chemoselectivity. The current strategy provide straightforward access to four different but valuable N‐heterocyclic adducts in moderate to excellent yields.
Design von Decorin‐basierten Peptiden, die an Kollagen I binden, und ihr Potenzial als Adhäsionssequenzen in Biomaterialien
Authors: Federico Stefania , Pierce Benjamin F. , Piluso Susanna , Wischke Christian , Lendlein Andreas , Neffe Axel T. 
Published: July 2015

AbstractDas Nachbilden der Bindungsepitope von Protein‐Protein‐Wechselwirkungen mithilfe kleiner Peptide ist wichtig bei der Entwicklung modularer biomimetischer Systeme. Hier beschreiben wir eine Strategie zum Design solcher bioaktiver Peptide, ohne dass Strukturdaten des Proteinkomplexes benötigt werden, und weisen den Effekt der Inkorporierung solcher Adhäsionssequenzen in komplexen Biomaterialsystemen nach. Dazu wurde die hochrepetitive Struktur von Decorin analysiert. Für dessen innere sowie äußere Oberfläche wurden repräsentative Peptide identifiziert und synthetisiert. Nur Peptide auf Basis der inneren Oberfläche binden an Kollagen. Das Peptid mit der höchsten Bindungsaffinität für Kollagen I führte zu einer geringeren Diffusionsgeschwindigkeit eines gekuppelten Farbstoffs in einem Kollagengel. Dimere des Peptids ermöglichten eine physikalische Vernetzung von Kollagen, wodurch der Speichermodul eines Gels stark erhöht werden konnte. Dies belegt das Potenzial der Peptide für das Design von Biomaterialien für die regenerative Medizin.
Catalytic Degradation of Sulfur Hexafluoride by Rhodium Complexes
Authors: Zámostná Lada , Braun Thomas 
Published: July 2015

AbstractThe development of a safe and efficient method for the degradation of SF6 is of current environmental interest, because SF6 is one of the most potent greenhouse gases. SF6 is thermally and chemically extremely inert, and therefore, it has been used in various industrial applications. However, this inertness results in a major challenge for its depletion. We report on a process for a catalytic degradation of SF6 in the homogeneous phase by using rhodium complexes as precatalysts. The SF6 activation reactions feature mild reaction conditions, low catalyst loadings, and a high selectivity. The employment of phosphines and hydrosilanes for scavenging the sulfur and fluorine atoms of the SF6 molecule allows the selective transformation of SF6 into nongaseous and nontoxic compounds.
Experimental Detection of the Intrinsic Difference in Raman Optical Activity of a Photoreceptor Protein under Preresonance and Resonance Conditions
Authors: Haraguchi Shojiro , Hara Miwa , Shingae Takahito , Kumauchi Masato , Hoff Wouter D. , Unno Masashi 
Published: July 2015

AbstractRaman optical activity (ROA) is an advanced technique capable of detecting structural deformations of light‐absorbing molecules embedded in chromophoric proteins. Resonance Raman (RR) spectroscopy is widely used to enhance the band intensities. However, theoretical work has predicted that under resonance conditions the ROA spectrum resembles the shape of the RR spectrum. Herein, we use photoactive yellow protein (PYP) to measure the first experimental data on the effect of changing the excitation wavelength on the ROA spectra of a protein. We observe a close similarity between the shape of the RR spectrum and the resonance ROA spectrum of PYP. Furthermore, we experimentally verify the theoretical prediction concerning the ratio of the amplitudes of the ROA and Raman spectra. Our data demonstrate that selecting an appropriate excitation wavelength is a key factor for extracting structural information on a protein active site using ROA spectroscopy.
Head‐to‐Tail Zig‐Zag Packing of Dipolar Merocyanine Dyes Affords High‐Performance Organic Thin‐Film Transistors
Authors: Lv Aifeng , Stolte Matthias , Würthner Frank 
Published: July 2015

AbstractAttachment of bulky substituents at both thiophene donor (D) and thiazole acceptor (A) heterocycles of a dipolar (μg=10.4 D) D‐π‐A merocyanine dye affords a more than 1 Å expansion of the common antiparallel supramolecular dimer motif in the solid state, enabling very close π‐contacts (3.36 Å) to two other neighbor molecules on each of the two remaining π‐faces. This unusual packing motif leads to three‐dimensional percolation pathways for hole transport and affords thin‐film transistors with mobility up to 0.64 cm2 V−1 s−1.