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- ItemInner solar system material discovered in the Oort cloud(Washington, DC [u.a.] : Assoc., 2016) Meech, Karen J.; Yang, Bin; Kleyna, Jan; Hainaut, Olivier R.; Berdyugina, Svetlana; Keane, Jacqueline V.; Micheli, Marco; Morbidelli, Alessandro; Wainscoat, Richard J.We have observed C/2014 S3 (PANSTARRS), a recently discovered object on a cometary orbit coming from the Oort cloud that is physically similar to an inner main belt rocky S-type asteroid. Recent dynamical models successfully reproduce the key characteristics of our current solar system; some of these models require significant migration of the giant planets, whereas others do not. These models provide different predictions on the presence of rocky material expelled from the inner solar system in the Oort cloud. C/2014 S3 could be the key to verifying these predictions of the migration-based dynamical models. Furthermore, this object displays a very faint, weak level of comet-like activity, five to six orders of magnitude less than that of typical ice-rich comets on similar Orbits coming from the Oort cloud. For the nearly tailless appearance, we are calling C/2014 S3 a Manx object. Various arguments convince us that this activity is produced by sublimation of volatile ice, that is, normal cometary activity. The activity implies that C/2014 S3 has retained a tiny fraction of the water that is expected to be present at its formation distance in the inner solar system. We may be looking at fresh inner solar system Earth-forming material that was ejected from the inner solar system and preserved for billions of years in the Oort cloud.
- ItemMolecular structure of bottlebrush polymers in melts(Washington, DC [u.a.] : Assoc., 2016) Paturej, Jarosław; Sheiko, Sergei S.; Panyukov, Sergey; Rubinstein, MichaelBottlebrushes are fascinating macromolecules that display an intriguing combination of molecular and particulate features having vital implications in both living and synthetic systems, such as cartilage and ultrasoft elastomers. However, the progress in practical applications is impeded by the lack of knowledge about the hierarchic organization of both individual bottlebrushes and their assemblies. We delineate fundamental correlations between molecular architecture, mesoscopic conformation, and macroscopic properties of polymer melts. Numerical simulations corroborate theoretical predictions for the effect of grafting density and side-chain length on the dimensions and rigidity of bottlebrushes, which effectively behave as a melt of flexible filaments. These findings provide quantitative guidelines for the design of novel materials that allow architectural tuning of their properties in a broad range without changing chemical composition.
- ItemTime-resolved structural evolution during the collapse of responsive hydrogels: The microgel-to-particle transition(Washington, DC [u.a.] : Assoc., 2018) Keidel, Rico; Ghavami, Ali; Lugo, Dersy M.; Lotze, Gudrun; Virtanen, Otto; Beumers, Peter; Pedersen, Jan Skov; Bardow, Andre; Winkler, Roland G.; Richtering, WalterAdaptive hydrogels, often termed smart materials, are macromolecules whose structure adjusts to external stimuli. Responsive micro- and nanogels are particularly interesting because the small length scale enables very fast response times. Chemical cross-links provide topological constraints and define the three-dimensional structure of the microgels, whereas their porous structure permits fast mass transfer, enabling very rapid structural adaption of the microgel to the environment. The change of microgel structure involves a unique transition from a flexible, swollen finite-size macromolecular network, characterized by a fuzzy surface, to a colloidal particle with homogeneous density and a sharp surface. In this contribution, we determine, for the first time, the structural evolution during the microgel-to-particle transition. Time-resolved small-angle x-ray scattering experiments and computer simulations unambiguously reveal a two-stage process: In a first, very fast process, collapsed clusters form at the periphery, leading to an intermediate, hollowish core-shell structure that slowly transforms to a globule. This structural evolution is independent of the type of stimulus and thus applies to instantaneous transitions as in a temperature jump or to slower stimuli that rely on the uptake of active molecules from and/or exchange with the environment. The fast transitions of size and shape provide unique opportunities for various applications as, for example, in uptake and release, catalysis, or sensing.
- ItemCombustion of available fossil fuel resources sufficient to eliminate the Antarctic Ice Sheet(Washington, DC [u.a.] : Assoc., 2015) Winkelmann, Ricarda; Levermann, Anders; Ridgwell, Andy; Caldeira, KenThe Antarctic Ice Sheet stores water equivalent to 58 m in global sea-level rise. We show in simulations using the Parallel Ice Sheet Model that burning the currently attainable fossil fuel resources is sufficient to eliminate the ice sheet. With cumulative fossil fuel emissions of 10,000 gigatonnes of carbon (GtC), Antarctica is projected to become almost ice-free with an average contribution to sea-level rise exceeding 3 m per century during the first millennium. Consistent with recent observations and simulations, the West Antarctic Ice Sheet becomes unstable with 600 to 800 GtC of additional carbon emissions. Beyond this additional carbon release, the destabilization of ice basins in both West and East Antarctica results in a threshold increase in global sea level. Unabated carbon emissions thus threaten the Antarctic Ice Sheet in its entirety with associated sea-level rise that far exceeds that of all other possible sources.
- ItemIntermetallic nickel silicide nanocatalyst—A non-noble metal–based general hydrogenation catalyst(Washington, DC [u.a.] : Assoc., 2018) Ryabchuk, Pavel; Agostini, Giovanni; Pohl, Marga-Martina; Lund, Henrik; Agapova, Anastasiya; Junge, Henrik; Junge, Kathrin; Beller, MatthiasHydrogenation reactions are essential processes in the chemical industry, giving access to a variety of valuable compounds including fine chemicals, agrochemicals, and pharmachemicals. On an industrial scale, hydrogenations are typically performed with precious metal catalysts or with base metal catalysts, such as Raney nickel, which requires special handling due to its pyrophoric nature. We report a stable and highly active intermetallic nickel silicide catalyst that can be used for hydrogenations of a wide range of unsaturated compounds. The catalyst is prepared via a straightforward procedure using SiO2 as the silicon atom source. The process involves thermal reduction of Si–O bonds in the presence of Ni nanoparticles at temperatures below 1000°C. The presence of silicon as a secondary component in the nickel metal lattice plays the key role in its properties and is of crucial importance for improved catalytic activity. This novel catalyst allows for efficient reduction of nitroarenes, carbonyls, nitriles, N-containing heterocycles, and unsaturated carbon–carbon bonds. Moreover, the reported catalyst can be used for oxidation reactions in the presence of molecular oxygen and is capable of promoting acceptorless dehydrogenation of unsaturated N-containing heterocycles, opening avenues for H2 storage in organic compounds. The generality of the nickel silicide catalyst is demonstrated in the hydrogenation of over a hundred of structurally diverse unsaturated compounds. The wide application scope and high catalytic activity of this novel catalyst make it a nice alternative to known general hydrogenation catalysts, such as Raney nickel and noble metal–based catalysts.
- ItemAgreement between reconstructed and modeled boreal precipitation of the Last Interglacial(Washington, DC [u.a.] : Assoc., 2019) Scussolini, Paolo; Bakker, Pepijn; Guo, Chuncheng; Stepanek, Christian; Zhang, Qiong; Braconnot, Pascale; Cao, Jian; Guarino, Maria-Vittoria; Coumou, Dim; Prange, Matthias; Ward, Philip J.; Renssen, Hans; Kageyama, Masa; Otto-Bliesner, Bette; Aerts, Jeroen C. J. H.The last extended time period when climate may have been warmer than today was during the Last Interglacial (LIG; ca. 129 to 120 thousand years ago). However, a global view of LIG precipitation is lacking. Here, seven new LIG climate models are compared to the first global database of proxies for LIG precipitation. In this way, models are assessed in their ability to capture important hydroclimatic processes during a different climate. The models can reproduce the proxy-based positive precipitation anomalies from the preindustrial period over much of the boreal continents. Over the Southern Hemisphere, proxy-model agreement is partial. In models, LIG boreal monsoons have 42% wider area than in the preindustrial and produce 55% more precipitation and 50% more extreme precipitation. Austral monsoons are weaker. The mechanisms behind these changes are consistent with stronger summer radiative forcing over boreal high latitudes and with the associated higher temperatures during the LIG.
- ItemOrganic carbon burial is paced by a ∼173-ka obliquity cycle in the middle to high latitudes(Washington, DC [u.a.] : Assoc., 2021) Huang, He; Gao, Yuan; Ma, Chao; Jones, Matthew M.; Zeeden, Christian; Ibarra, Daniel E.; Wu, Huaichun; Wang, ChengshanEarth’s climate system is complex and inherently nonlinear, which can induce some extraneous cycles in paleoclimatic proxies at orbital time scales. The paleoenvironmental consequences of these extraneous cycles are debated owing to their complex origin. Here, we compile high-resolution datasets of total organic carbon (TOC) and stable carbon isotope (δ13Corg) datasets to investigate organic carbon burial processes in middle to high latitudes. Our results document a robust cyclicity of ~173 thousand years (ka) in both TOC and δ13Corg. The ~173-ka obliquity–related forcing signal was amplified by internal climate feedbacks of the carbon cycle under different geographic and climate conditions, which control a series of sensitive climatic processes. In addition, our new and compiled records from multiple proxies confirm the presence of the obliquity amplitude modulation (AM) cycle during the Mesozoic and Cenozoic and indicate the usefulness of the ~173-ka cycle as geochronometer and for paleoclimatic interpretation.
- ItemVoltage control of magnetic order in RKKY coupled multilayers(Washington, DC [u.a.] : Assoc., 2023) Kossak, Alexander E.; Huang, Mantao; Reddy, Pooja; Wolf, Daniel; Beach, Geoffrey S. D.In the field of antiferromagnetic (AFM) spintronics, there is a substantial effort present to make AFMs viable active components for efficient and fast devices. Typically, this is done by manipulating the AFM Néel vector. Here, we establish a method of enabling AFM active components by directly controlling the magnetic order. We show that magneto-ionic gating of hydrogen enables dynamic control of the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction in solid-state synthetic AFM multilayer devices. Using a gate voltage, we tune the RKKY interaction to drive continuous transitions from AFM to FM and vice versa. The switching is submillisecond at room temperature and fully reversible. We validate the utility of this method by demonstrating that magneto-ionic gating of the RKKY interaction allows for 180° field-free deterministic switching. This dynamic method of controlling a fundamental exchange interaction can engender the manipulation of a broader array of spin textures, e.g., chiral domain walls and skyrmions.
- ItemReconstruction of the time-dependent electronic wave packet arising from molecular autoionization(Washington, DC [u.a.] : Assoc., 2018) Bello, Roger Y.; Canton, Sophie E.; Jelovina, Denis; Bozek, John D.; Rude, Bruce; Smirnova, Olga; Ivanov, Mikhail Y.; Palacios, Alicia; MartÃn, FernandoAutoionizing resonances are paradigmatic examples of two-path wave interferences between direct photoionization, which takes a few attoseconds, and ionization via quasi-bound states, which takes much longer. Time-resolving the evolution of these interferences has been a long-standing goal, achieved recently in the helium atom owing to progress in attosecond technologies. However, already for the hydrogen molecule, similar time imaging has remained beyond reach due to the complex interplay between fast nuclear and electronic motions. We show how vibrationally resolved photoelectron spectra of H2 allow one to reconstruct the associated subfemtosecond autoionization dynamics by using the ultrafast nuclear dynamics as an internal clock, thus forgoing ultrashort pulses. Our procedure should be general for autoionization dynamics in molecules containing light nuclei, which are ubiquitous in chemistry and biology.
- ItemQuantitative hyperspectral coherent diffractive imaging spectroscopy of a solid-state phase transition in vanadium dioxide(Washington, DC [u.a.] : Assoc., 2021) Johnson, Allan S.; Conesa, Jordi Valls; Vidas, Luciana; Perez-Salinas, Daniel; Günther, Christian M.; Pfau, Bastian; Hallman, Kent A.; Haglund, Richard F.; Eisebitt, Stefan; Wall, SimonSolid-state systems can host a variety of thermodynamic phases that can be controlled with magnetic fields, strain, or laser excitation. Many phases that are believed to exhibit exotic properties only exist on the nanoscale, coexisting with other phases that make them challenging to study, as measurements require both nanometer spatial resolution and spectroscopic information, which are not easily accessible with traditional x-ray spectromicroscopy techniques. Here, we use coherent diffractive imaging spectroscopy (CDIS) to acquire quantitative hyperspectral images of the prototypical quantum material vanadium oxide across the vanadium L2,3 and oxygen K x-ray absorption edges with nanometer-scale resolution. We extract the full complex refractive indices of the monoclinic insulating and rutile conducting phases of VO2 from a single sample and find no evidence for correlation-driven phase transitions. CDIS will enable quantitative full-field x-ray spectromicroscopy for studying phase separation in time-resolved experiments and other extreme sample environments where other methods cannot operate.