Seasonal variations of atmospheric carbon dioxide (CO2) in the Northern Hemisphere have increased since the 1950s, but sparse observations have prevented a clear assessment of the patterns of long-term change and the underlying mechanisms. We compare recent aircraft-based observations of CO2 above the North Pacific and Arctic Oceans to earlier data from 1958 to 1961 and find that the seasonal amplitude at altitudes of 3 to 6 km increased by 50% for 45° to 90°N but by less than 25% for 10° to 45°N. An increase of 30 to 60% in the seasonal exchange of CO2 by northern extratropical land ecosystems, focused on boreal forests, is implicated, substantially more than simulated by current land ecosystem models. The observations appear to signal large ecological changes in northern forests and a major shift in the global carbon cycle.
Microstructure evolution of a low hard segment (<10 mol %) thermoplastic polyurethane (LHS-TPU) has been followed by in-situ wide-angle X-ray (WAX) and small-angle X-ray scattering (SAX) with a focus on elucidating peculiar microstructural changes during uniaxial deformation (λ ) 1-3.5). For the LHS-TPU, the hard segments, due to their low content and chemical structure, do not crystallize but form glassy regions that act as physical cross-links. Two types of soft segment crystallites are resolved upon elongation via DSC, SAX, and WAX experiments. Phase I consists of a small amount of initial crystallites (<2%) that function similar to conventional PU hard segment domains, deforming at small uniaxial strains (λ ) 1-2) to a chevrontype morphology, which exhibit equatorial 4-point patterns in SAX. Phase II evolves at higher deformations (λ > 2) due to strain-induced crystallization. Phase II exhibits a conventional meridional 2-point pattern along the deformation direction with lamellar crystallites aligning in the plane normal to the deformation. WAX, SAX, and DSC confirm that both phases coexist over a small strain window (λ ) 1.9-2.5), demonstrating the independent nature of the two crystalline phases. These findings indicate that the LHS-TPU in this study is similar to poly(butylene adipate) (PBA) in its morphological and structural behavior. This is further substantiated by NMR, which reveals that the LHS-TPU consists of 90% soft segments, which are identified as PBA via crystal structure analysis of a highly aligned fiber. The soft segments in the LHS-TPU dominate the morphology and the X-ray patterns upon deformation.
High-throughput, data-directed computational protocols for Structural Genomics (or Proteomics) are required in order to evaluate the protein products of genes for structure and function at rates comparable to current gene-sequencing technology. This paper presents the Jigsaw algorithm, a novel highthroughput, automated approach to protein structure characterization with nuclear magnetic resonance (NMR). Jigsaw applies graph algorithms and probabilistic reasoning techniques, enforcing first-principles consistency rules in order to overcome a 5-10% signal-to-noise ratio. It consists of two main components: (1) graph-based secondary structure pattern identification in unassigned heteronuclear NMR data, and (2) assignment of spectral peaks by probabilistic alignment of identified secondary structure elements against the primary sequence. Deferring assignment eliminates the bottleneck faced by traditional approaches, which begin by correlating peaks among dozens of experiments. Jigsaw utilizes only four experiments, none of which requires 13 C-labeled protein, thus dramatically reducing both the amount and expense of wet lab molecular biology and the total spectrometer time. Results for three test proteins demonstrate that Jigsaw correctly identifies 79-100% of α-helical and 46-65% of β-sheet NOE connectivities, and correctly aligns 33-100% of secondary structure elements. Jigsaw is very fast, running in minutes on a Pentium-class Linux workstation. This approach yields quick and reasonably accurate (as opposed to the traditional slow and extremely accurate) structure calculations. It could be useful for quick structural assays to speed data to the biologist early in an investigation, and could in principle be applied in an automation-like fashion to a large fraction of the proteome.2
Rapid fabrication of large area, ordered assemblies of polymer grafted (hairy) nanoparticles (PGNs) will enable additive manufacturing of novel membrane, electronic, and photonic elements. Herein, we discuss the relationship between select processing conditions, substrate surface energy, and canopy architecture on the hierarchical structure of sub- to monolayer PGN assemblies. Varying concentrations (10, 20, and 70 nM) of polystyrene (PS) grafted (σ ∼ 1 chain/nm2) gold nanoparticles (AuNP, r 0 = 9 nm) were flow-coated onto surface-modified silicon wafers (γs ∼ 20 mN/m, hydrophobic to 80 mN/m, hydrophilic). The profile of an isolated gold–polystyrene (PS) PGN depends on substrate–canopy interface energy. At low substrate–PS interface energy (20 mN/m), the PS canopy spreads to maximize contact with the surface, whereas at high substrate–PS interface energy (80 mN/m), the chains minimize contact area resulting in a more compact, thicker PGN corona. This behavior is translated up to monolayer assemblies, where rougher, less-ordered assemblies with smaller AuNP–surface separation form on substrates with low interface energy. These films are also thinner with greater Au volume fraction, indicating that the segment density within the PS canopy depends on substrate surface energy. The impact of these processing parameters on PGN film formation parallels classic colloidal deposition even though the PS concentration is within the Landau–Levich regime for film formation from linear chains. The factors influencing local morphology, however, resemble those that affect polymer thin films. Using this understanding, we demonstrate fabrication within seconds of large area monolayer films with close-packed order.
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