Because of the pervasiveness, persistence, and toxicity of per-and polyfluoroalkyl substances (PFAS), there is growing concern over PFAS contamination, exposures, and health effects. The diversity of potential PFAS is astounding, with nearly 10,000 PFAS catalogued in databases to date (and growing). The ability to detect the thousands of known PFAS, and discover previously uncatalogued PFAS, is necessary to understand the scope of PFAS contamination and to identify appropriate remediation and regulatory solutions. Current non-targeted methods for PFAS analysis require manual curation and are time-consuming, prone to error, and not comprehensive. FluoroMatch Flow 2.0 is the first software to cover all steps of data processing for PFAS discovery in liquid chromatography-high-resolution tandem mass spectrometry samples. These steps include feature detection, feature blank filtering, exact mass matching to catalogued PFAS, mass defect filtering, homologous series detection, retention time pattern analysis, class-based MS/MS screening, fragment screening, and predicted MS/MS from SMILES structures. In addition, a comprehensive confidence level criterion is implemented to help users understand annotation certainty and integrate various layers of evidence to reduce overreporting. Applying the software to aqueous film forming foam analysis, we discovered over one thousand likely PFAS including previously unreported species. Furthermore, we were able to filter out 96% of features which were likely not PFAS. FluoroMatch Flow 2 increased coverage of likely PFAS by over tenfold compared to the previous release. This software will enable researchers to better characterize PFAS in the environment and in biological systems.

Antimicrobial peptides (AMPs) are promising candidates for battling multiresistant bacteria. Despite extensive research, structure-activity relationships of AMPs are not fully understood, and there is a lack of structural data relating to AMPs in lipids. Here we present the NMR structure of anoplin (GLLKRIKTLL-NH2 ) in a micellar environment. A vast library of substitutions was designed and tested for antimicrobial and hemolytic activity, as well as for changes in structure and lipid interactions. This showed that improvement of antimicrobial activity without concomitant introduction of strong hemolytic activity can be achieved through subtle increases in the hydrophobicity of the hydrophobic face or through subtle increases in the polarity of the hydrophilic face of the helix, or-most efficiently-a combination of both. A set of guidelines based on the results is given, for assistance in how to modify cationic α-helical AMPs in order to control activity and selectivity. The guidelines are finally tested on a different peptide.

[1] VHF coherent scatter radar observations of an auroral substorm over Alaska are analyzed in the context of multibeam incoherent scatter plasma density and drifts data and green-line all-sky optical imagery. Coherent scatter arises from Farley Buneman waves which are excited in the E region whenever the convection electric field is greater than about 20 mV/m. Aperture synthesis radar imaging and other aspects of the methodology facilitate the precise spatial registration of the coherent scatter with coincident optical and incoherent scatter radar measurements. Discrete auroral arcs were found to separate diffuse regions of coherent backscatter and, sometimes, to align with the boundaries of those regions. At other times, auroral arcs and torches lined up adjacent to discrete, structured regions or radar backscatter. Drastic variations in the Doppler shifts of the coherent scatter from one side of the auroral forms to the other suggest the presence of field-aligned currents. An empirical formula based on previous studies but adapted to account approximately for the effects of wave turning was used to estimate the convection electric field from the moments of the coherent scatter Doppler spectra. Line-of-sight F region plasma drift measurements from the Poker Flat Incoherent Scatter Radar (PFISR) were found to be in reasonable agreement with these convection field estimates. Reasons why the empirical formulas may be expected to hold are discussed.

An important component of ice sheet mass balance calculations is the snow accumulation rate, traditionally determined across the ice sheet from interpolated ice core data. We derive an accumulation rate map within the Greenland dry‐snow facies, using C‐band radar backscatter and the mean annual temperature. Values for the backscatter were obtained from the ERS‐1 synthetic aperture radar mosaic acquired during September–November 1992. An empirical equation, based on elevation and latitude, is used to determine the mean annual temperature. We examine the influence of accumulation rate, and mean annual temperature on C‐band (5.3 GHz) radar backscatter, using a forward model, which incorporates snow metamorphosis and radar backscatter components. Our model is run over a range of accumulation and temperature conditions, consistent with the Greenland dry‐snow facies. On the basis of our modeled results, a look‐up table is generated, which uniquely maps the measured radar backscatter and mean annual temperature to accumulation rate. Our results compare favorably (15.4% average difference) with 124 in situ accumulation rate measurements falling within our study area. We attribute some of the differences to (1) unreliable in situ data points, which were based on a single year's accumulation and (2) a systematic underestimate of accumulation rate by our forward model in the low‐accumulation regions associated with the northern portion of our map. With questionable data points and those above 77°N removed, the average differences were less than 10.3%, as determined from 73 ice cores.

Thermokarst lakes accelerate deep permafrost thaw and the mobilization of previously frozen soil organic carbon. This leads to microbial decomposition and large releases of carbon dioxide (CO2) and methane (CH4) that enhance climate warming. However, the time scale of permafrost-carbon emissions following thaw is not well known but is important for understanding how abrupt permafrost thaw impacts climate feedback. We combined field measurements and radiocarbon dating of CH4 ebullition with (a) an assessment of lake area changes delineated from high-resolution (1–2.5 m) optical imagery and (b) geophysical measurements of thaw bulbs (taliks) to determine the spatiotemporal dynamics of hotspot-seep CH4 ebullition in interior Alaska thermokarst lakes. Hotspot seeps are characterized as point-sources of high ebullition that release 14C-depleted CH4 from deep (up to tens of meters) within lake thaw bulbs year-round. Thermokarst lakes, initiated by a variety of factors, doubled in number and increased 37.5% in area from 1949 to 2009 as climate warmed. Approximately 80% of contemporary CH4 hotspot seeps were associated with this recent thermokarst activity, occurring where 60 years of abrupt thaw took place as a result of new and expanded lake areas. Hotspot occurrence diminished with distance from thermokarst lake margins. We attribute older 14C ages of CH4 released from hotspot seeps in older, expanding thermokarst lakes (14CCH4 20 079 ± 1227 years BP, mean ± standard error (s.e.m.) years) to deeper taliks (thaw bulbs) compared to younger 14CCH4 in new lakes (14CCH4 8526 ± 741 years BP) with shallower taliks. We find that smaller, non-hotspot ebullition seeps have younger 14C ages (expanding lakes 7473 ± 1762 years; new lakes 4742 ± 803 years) and that their emissions span a larger historic range. These observations provide a first-order constraint on the magnitude and decadal-scale duration of CH4-hotspot seep emissions following formation of thermokarst lakes as climate warms.