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Black carbon (BC) aerosol emitted by boreal fires has the potential to accelerate losses of snow and ice in many areas of the Arctic, yet the importance of this source relative to fossil fuel BC emissions from lower latitudes remains uncertain. Here we present measurements of the isotopic composition of BC and organic carbon (OC) aerosols collected at two locations in interior Alaska during the summer of 2013, as part of NASA's Carbon in Arctic Reservoirs Vulnerability Experiment. We isolated BC from fine air particulate matter (PM2.5) and measured its radiocarbon (Δ14C) content with accelerator mass spectrometry. We show that fires were the dominant contributor to variability in carbonaceous aerosol mass in interior Alaska during the summer by comparing our measurements with satellite data, measurements from an aerosol network and predicted concentrations from a fire inventory coupled to an atmospheric transport model. The Δ14C of BC from boreal fires was 131 ± 52‰ in the year 2013 when the Δ14C of atmospheric CO2 was 23 ± 3‰, corresponding to a mean fuel age of 20 years. Fire-emitted OC had a similar Δ14C (99 ± 21‰) as BC, but during background (low fire) periods OC (45 to 51‰) was more positive than BC (-354 to -57‰). We also analyzed the carbon and nitrogen elemental and stable isotopic composition of the PM2.5. Fire-emitted aerosol had an elevated carbon to nitrogen (C/N) ratio (29 ± 2) and δ15N (16 ± 4‰). Aerosol Δ14C and δ13C measurements were consistent with a mean depth of burning in organic soil horizons of 20 cm (and a range of 8 to 47 cm). Our measurements of fire-emitted BC and PM2.5 composition constrain the end-member of boreal forest fire contributions to aerosol deposition in the Arctic and may ultimately reduce uncertainties related to the impact of a changing boreal fire regime on the climate system.

Aerosol source apportionment remains a critical challenge for understanding the transport and aging of aerosols, as well as for developing successful air pollution mitigation strategies. The contributions of fossil and non-fossil sources to organic carbon (OC) and elemental carbon (EC) in carbonaceous aerosols can be quantified by measuring the radiocarbon (14C) content of each carbon fraction. However, the use of 14C in studying OC and EC has been limited by technical challenges related to the physical separation of the two fractions and small sample sizes. There is no common procedure for OC/EC 14C analysis, and uncertainty studies have largely focused on the precision of yields. Here, we quantified the uncertainty in 14C measurement of aerosols associated with the isolation and analysis of each carbon fraction with the Swiss-4S thermal-optical analysis (TOA) protocol. We used an OC/EC analyzer (Sunset Laboratory Inc., OR, USA) coupled to a vacuum line to separate the two components. Each fraction was thermally desorbed and converted to carbon dioxide (CO2) in pure oxygen (O2). On average, 91 % of the evolving CO2 was then cryogenically trapped on the vacuum line, reduced to filamentous graphite, and measured for its 14C content via accelerator mass spectrometry (AMS). To test the accuracy of our setup, we quantified the total amount of extraneous carbon introduced during the TOA sample processing and graphitization as the sum of modern and fossil (14C-depleted) carbon introduced during the analysis of fossil reference materials (adipic acid for OC and coal for EC) and contemporary standards (oxalic acid for OC and rice char for EC) as a function of sample size. We further tested our methodology by analyzing five ambient airborne particulate matter (PM2.5) samples with a range of OC and EC concentrations and 14C contents in an interlaboratory comparison. The total modern and fossil carbon blanks of our setup were 0.8 ± 0.4 and 0.67 ± 0.34 μg C, respectively, based on multiple measurements of ultra-small samples. The extraction procedure (Swiss-4S protocol and cryo-trapping only) contributed 0.37 ± 0.18 μg of modern carbon and 0.13 ± 0.07 μg of fossil carbon to the total blank of our system, with consistent estimates obtained for the two laboratories. There was no difference in the background correction between the OC and EC fractions. Our setup allowed us to efficiently isolate and trap each carbon fraction with the Swiss-4S protocol and to perform 14C analysis of ultra-small OC and EC samples with high accuracy and low 14C blanks.

Aerosol source apportionment remains a critical challenge for understanding the transport and aging of aerosols, as well as for developing successful air pollution mitigation strategies. The contributions of fossil and non-fossil sources to organic carbon (OC) and elemental carbon (EC) in carbonaceous aerosols can be quantified by measuring the radiocarbon (14C) content of each carbon fraction. However, the use of 14C in studying OC and EC has been limited by technical challenges related to the physical separation of the two fractions and small sample sizes. There is no common procedure for OC/EC 14C analysis, and uncertainty studies have largely focused on the precision of yields. Here, we quantified the uncertainty in 14C measurement of aerosols associated with the isolation and analysis of each carbon fraction with the Swiss-4S thermal-optical analysis (TOA) protocol. We used an OC/EC analyzer (Sunset Laboratory Inc., OR, USA) coupled to a vacuum line to separate the two components. Each fraction was thermally desorbed and converted to carbon dioxide (CO2) in pure oxygen (O2). On average, 91 % of the evolving CO2 was then cryogenically trapped on the vacuum line, reduced to filamentous graphite, and measured for its 14C content via accelerator mass spectrometry (AMS). To test the accuracy of our setup, we quantified the total amount of extraneous carbon introduced during the TOA sample processing and graphitization as the sum of modern and fossil (14C-depleted) carbon introduced during the analysis of fossil reference materials (adipic acid for OC and coal for EC) and contemporary standards (oxalic acid for OC and rice char for EC) as a function of sample size. We further tested our methodology by analyzing five ambient airborne particulate matter (PM2.5) samples with a range of OC and EC concentrations and 14C contents in an interlaboratory comparison. The total modern and fossil carbon blanks of our setup were 0.8 ± 0.4 and 0.67 ± 0.34 μg C, respectively, based on multiple measurements of ultra-small samples. The extraction procedure (Swiss-4S protocol and cryo-trapping only) contributed 0.37 ± 0.18 μg of modern carbon and 0.13 ± 0.07 μg of fossil carbon to the total blank of our system, with consistent estimates obtained for the two laboratories. There was no difference in the background correction between the OC and EC fractions. Our setup allowed us to efficiently isolate and trap each carbon fraction with the Swiss-4S protocol and to perform 14C analysis of ultra-small OC and EC samples with high accuracy and low 14C blanks.

Although Accelerator Mass Spectrometry (AMS) offers unparalleled sensitivity by investigating the fate of 14 C-labeled compounds within the organism, its widespread use in ADME (absorption, distribution, metabolism, excretion) studies is limited. Conventional approaches based on Liquid Scintillation Counting (LSC) are still preferred, in particular because of complexity and costs associated with AMS measurements. Progress made over the last decade towards more compact AMS systems increased the interest in a combustion-based AMS approach allowing the analysis of samples in gaseous form. Thus, a novel gas Double Trap Interface (DTI) was designed, providing high sample throughput for the analysis of biomedical samples. DTI allows the coupling of an Elemental Analyzer (EA) for sample combustion to the hybrid ion source of a MICADAS (MIni CArbon DAting System) AMS system. The performance was evaluated in two studies through the analysis of more than 1000 samples from 14 C-labeled biomatrices and fractions collected after liquid chromatography (LC). The covered activity ranged from 1 to 1000 mBq/g for labeled biomatrices and from 1 to 10000 mBq/g(C) for LC fractions. The implemented routine allows automated measurements requiring less than 5 min per sample (12-13 analyses per hour) without the need for sample conversion to graphite., Competing Interests: Declaration of competing interest F Lozac'h, C Marvalin, M Walles and G Camenisch are employees of Novartis Pharma AG. S Fahrni is an employee of Ionplus AG. L Wacker, H-A Synal and S Fahrni are shareholders of Ionplus AG. There is no competing financial interest between Novartis and Ionplus on this project. D De Maria has no financial involvement with any organization or financial interest with the subject discussed in the manuscript., (Copyright © 2021 The Japanese Society for the Study of Xenobiotics. Published by Elsevier Ltd. All rights reserved.)

The problem of fraud continues to plague the wine industry, and detecting cases where the original bottle has been refilled with an inferior vintage is especially difficult. A novel noninvasive procedure presented here relies on radiocarbon dating the so-called angel's share: the trace amounts of ethanol and other gases that diffuse into and through the cork as bottled wine ages and matures. These are collected by applying a vacuum to the top of the bottle and cryo-trapping the extracted gas, leaving the liquid contents untouched. Vintage verification is therefore possible without exposing the liquid contents to the atmosphere, which may render a bottle costing tens of thousands of dollars worthless for later resale and consumption. The method also has a potential for stable isotope ratio as well as chemical analysis to find indications for fraud or spoilage of fine and rare wines as well as other liquids with cork stoppers.

The New World Arctic, the last region of the Americas to be populated by humans, has a relatively well-researched archaeology, but an understanding of its genetic history is lacking. We present genome-wide sequence data from ancient and present-day humans from Greenland, Arctic Canada, Alaska, Aleutian Islands, and Siberia. We show that Paleo-Eskimos (~3000 BCE to 1300 CE) represent a migration pulse into the Americas independent of both Native American and Inuit expansions. Furthermore, the genetic continuity characterizing the Paleo-Eskimo period was interrupted by the arrival of a new population, representing the ancestors of present-day Inuit, with evidence of past gene flow between these lineages. Despite periodic abandonment of major Arctic regions, a single Paleo-Eskimo metapopulation likely survived in near-isolation for more than 4000 years, only to vanish around 700 years ago., (Copyright © 2014, American Association for the Advancement of Science.)