Arctic precipitation in the form of rain is forecast to become more prevalent in a warmer world but with seasonal and interannual changes modulated by natural modes of variability. Experiencing rapid hydroclimatic changes in the Arctic, Svalbard serves as an ideal study location due to its exposure to oceanic and atmospheric variability in the North Atlantic region. Here we use climate data from paleoproxies, observations, and a climate model to demonstrate that wet and warm extremes in Svalbard over the last two millennia are linked to the presence of atmospheric blocking regimes over Scandinavia and the Ural mountain region.
View Article and Find Full Text PDFSingle-walled carbon nanotubes (SWCNTs) are candidate matrices for loading metal nanoparticles (NPs) for sensor and catalytic applications owing to their high electron conductivity and mechanical strength, larger surface area, excellent chemical stability, and ease of surface modification. The performance of the formed NP/SWCNT composites is dependent on the NP size, the physical and chemical interactions between the components, and the charge transfer capabilities. Anchoring metal complexes onto the surface of SWCNTs through noncovalent interactions is a viable strategy for achieving high-level metal dispersion and high charge transfer capacities between metal NPs and SWCNTs.
View Article and Find Full Text PDFThe chemical purity of materials is important for semiconductors, including the carbon nanotube material system, which is emerging in semiconductor applications. One approach to get statistically meaningful abundances and/or concentrations is to measure a large number of small samples. Automated multivariate classification algorithms can be used to draw conclusions from such large data sets.
View Article and Find Full Text PDFThe Little Ice Age (LIA) was one of the coldest periods of the postglacial period in the Northern Hemisphere. Although there is increasing evidence that this time interval was associated with weakening of the subpolar gyre (SPG), the sequence of events that led to its weakened state has yet to be explained. Here, we show that the LIA was preceded by an exceptional intrusion of warm Atlantic water into the Nordic Seas in the late 1300s.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
November 2020
Global warming due to anthropogenic factors can be amplified or dampened by natural climate oscillations, especially those involving sea surface temperatures (SSTs) in the North Atlantic which vary on a multidecadal scale (Atlantic multidecadal variability, AMV). Because the instrumental record of AMV is short, long-term behavior of AMV is unknown, but climatic teleconnections to regions beyond the North Atlantic offer the prospect of reconstructing AMV from high-resolution records elsewhere. Annually resolved titanium from an annually laminated sedimentary record from Ellesmere Island, Canada, shows that the record is strongly influenced by AMV via atmospheric circulation anomalies.
View Article and Find Full Text PDFThe hydrated electron has fundamental and practical significance in radiation and radical chemistry, catalysis, and radiobiology. While its bulk properties have been extensively studied, its behavior at solid/liquid interfaces is still unclear due to the lack of effective tools to characterize this short-lived species in between two condensed matter layers. In this study, we develop a novel optoelectronic technique for the characterization of the birth and structural evolution of solvated electrons at the metal/liquid interface with a femtosecond time resolution.
View Article and Find Full Text PDFHigh-purity semiconducting single-walled carbon nanotubes (sc-SWCNTs) are promising for portable and high-sensitivity gas sensors because of their excellent physical and electrical properties. Here, we describe the synthesis of a novel indigo-fluorene-based copolymer () that has been designed to selectively enrich sc-SWCNTs with excellent purity (>99.9%) yet contain a latent function in the form of a -butoxy (-BOC)-protected amine that can be later revealed and exploited for carbon dioxide (CO) gas sensing.
View Article and Find Full Text PDFACS Appl Mater Interfaces
October 2019
Although carbon nanotube transistors present outstanding performances based on key metrics, large-scale uniformity and repeatability required in printable electronics depend greatly on proper control of the electrostatic environment. Through a survey of polymer dielectric encapsulants compatible with printing processes, a simple correlation is found between the measured interfacial charge density and the onset of conduction in a transistor, providing a rational route to control the electrical characteristics of carbon nanotube transistors. Smooth and continuous balancing of the properties between unipolar p-type and n-type transport is achieved using a molar fraction series of poly(styrene--2-vinylpyridine) statistical copolymers combined with an electron-donating molecule.
View Article and Find Full Text PDFNanomaterials are ideal for electrochemical biosensors, with their nanoscale dimensions enabling the sensitive probing of biomolecular interactions. In this study, we compare field-effect transistors (FET) comprised of unsorted (un-) and semiconducting-enriched (sc-) single-walled carbon nanotubes (SWCNTs). un-SWCNTs have both metallic and semiconducting SWCNTs in the ensemble, while sc-SWCNTs have a >99.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
April 2017
Quantitative description of reaction mechanisms in aqueous phase electrochemistry requires experimental characterization of local water structure at the electrode/aqueous interface and its evolution with changing potential. Gaining such insight experimentally under electrochemical conditions is a formidable task. The potential-dependent structure of a subpopulation of interfacial water with one OH group pointing towards a gold working electrode is characterized using interface specific vibrational spectroscopy in a thin film electrochemical cell.
View Article and Find Full Text PDFLiquid-phase encapsulation of α-sexithiophene (6T) molecules inside individualized single-walled carbon nanotubes (SWCNTs) is investigated using Raman imaging and spectroscopy. By taking advantage of the strong Raman response of this system, we probe the encapsulation isotherms at 30 and 115 °C using a statistical ensemble of SWCNTs deposited on a oxidized silicon substrate. Two distinct and sequential stages of encapsulation are observed: Stage 1 is a one-dimensional (1D) aggregation of 6T aligned head-to-tail inside the nanotube, and stage 2 proceeds with the assembly of a second row, giving pairs of aligned 6Ts stacked together side-by-side.
View Article and Find Full Text PDFEnhanced phosphorus (P) export from land into streams and lakes is a primary factor driving the expansion of deep-water hypoxia in lakes during the Anthropocene. However, the interplay of regional scale environmental stressors and the lack of long-term instrumental data often impede analyses attempting to associate changes in land cover with downstream aquatic responses. Herein, we performed a synthesis of data that link paleolimnological reconstructions of lake bottom-water oxygenation to changes in land cover/use and climate over the past 300 years to evaluate whether the spread of hypoxia in European lakes was primarily associated with enhanced P exports from growing urbanization, intensified agriculture, or climatic change.
View Article and Find Full Text PDFThe spread of hypoxia is a threat to aquatic ecosystem functions and services as well as to biodiversity. However, sparse long-term monitoring of lake ecosystems has prevented reconstruction of global hypoxia dynamics while inhibiting investigations into its causes and assessing the resilience capacity of these systems. This study compiles the onset and duration of hypoxia recorded in sediments of 365 lakes worldwide since AD 1700, showing that lacustrine hypoxia started spreading before AD 1900, 70 years prior to hypoxia in coastal zones.
View Article and Find Full Text PDFThis work revisits the physics giving rise to the carbon nanotube phonon bands in the midinfrared. Our measurements of doped and undoped samples of single-walled carbon nanotubes in Fourier transform infrared spectroscopy show that the phonon bands exhibit an asymmetric line shape and that their effective cross section is enhanced upon doping. We relate these observations to electron-phonon coupling or, more specifically, to a Fano resonance phenomenon.
View Article and Find Full Text PDFDouble-walled carbon nanotubes (DWNTs) present an original coaxial geometry in which the inner wall is naturally protected from the environment by the outer wall. Covalent functionalization is introduced here as an effective approach to investigate DWNT devices. Performed using an aryldiazonium salt, the functionalization is reversible upon thermal annealing and occurs strictly at the surface of the outer wall, leaving the inner wall essentially unaltered by the chemical bonding.
View Article and Find Full Text PDFIn this paper, we evaluate the relative performance of competing approaches for estimating phylogenies from incomplete distance matrices. The direct approach proceeds with phylogenetic reconstruction while ignoring missing cells, whereas the indirect approach proceeds by estimating the missing distances prior to phylogenetic analysis. Two distinct indirect procedures based on the ultrametric inequality and the four-point condition are further compared.
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