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In response to warming climate, methane can be released to Arctic Ocean sediment and waters from thawing subsea permafrost and decomposing methane hydrates. However, it is unknown whether methane derived from this sediment storehouse of frozen ancient carbon reaches the atmosphere. We quantified the fraction of methane derived fromancient sources in shelf waters of the U.S. Beaufort Sea, a region that has both permafrost andmethane hydrates and is experiencing significant warming. Although the radiocarbon-methane analyses indicate that ancient carbon is being mobilized and emitted as methane into shelf bottom waters, surprisingly, we find that methane in surface waters is principally derived from modern-aged carbon. We report that at and beyond approximately the 30-m isobath, ancient sources that dominate in deep waters contribute, at most, 10 +/- 3% of the surface water methane. These results suggest that even if there is a heightened liberation of ancient carbon-sourced methane as climate change proceeds, oceanic oxidation and dispersion processes can strongly limit its emission to the atmosphere.

Author Posting. © The Author(s), 2018. This is the author's version of the work. It is posted here under a nonexclusive, irrevocable, paid-up, worldwide license granted to WHOI. It is made available for personal use, not for redistribution. The definitive version was published in Geochimica et Cosmochimica Acta 244 (2019): 502-521, doi:10.1016/j.gca.2018.09.034., Relatively little is known about the amount of time that lapses between the photosynthetic fixation of carbon by vascular land plants and its incorporation into the marine sedimentary record, yet the dynamics of terrestrial carbon sequestration have important implications for the carbon cycle. Vascular plant carbon may encounter multiple potential intermediate storage pools and transport trajectories, and the age of vascular plant carbon accumulating in marine sediments will reflect these different predepositional histories. Here, we examine down-core 14C profiles of higher plant leaf waxderived fatty acids isolated from high fidelity sedimentary sequences spanning the socalled “bomb-spike”, and encompassing a ca. 60-degree latitudinal gradient from tropical (Cariaco Basin), temperate (Saanich Inlet), and polar (Mackenzie Delta) watersheds to constrain integrated vascular plant carbon storage/transport times (“residence times”). Using a modeling framework, we find that, in addition to a "young" (conditionally defined as < 50 y) carbon pool, an old pool of compounds comprises 49 to 78 % of the fractional contribution of organic carbon (OC) and exhibits variable ages reflective of the environmental setting. For the Mackenzie Delta sediments, we find a mean age of the old pool of 28 ky (±9.4, standard deviation), indicating extensive pre-aging in permafrost soils, whereas the old pools in Saanich Inlet and Cariaco Basin sediments are younger, 7.9 (±5.0) and 2.4 (±0.50) to 3.2 (±0.54) ky, respectively, indicating less protracted storage in terrestrial reservoirs. The "young" pool showed clear annual contributions for Saanich Inlet and Mackenzie Delta sediments (comprising 24% and 16% of this pool, respectively), likely reflecting episodic transport of OC from steep hillside slopes surrounding Saanich Inlet and annual spring flood deposition in the Mackenzie Delta, respectively. Contributions of 5-10 year old OC to the Cariaco Basin show a short delay of OC inflow, poten, Financial support was provided by a Schlanger Ocean Drilling Graduate Fellowship (NJD), an EPA STAR Graduate Fellowship (NJD), a Dutch NWO Veni grant #825.10.022 (JEV), US NSF grants #OCE-0137005 (TIE and KAH), #OCE-052626800 (TIE), #OCE-0961980 (ERMD), and #EAR-0447323 (ERMD and JRS), a Swiss SNF grant #200021_140850 (TIE), a Swedish Research Council grant #2013-05204 (MS), as well as the Stanley Watson Chair for Excellence in Oceanography at WHOI (TIE) and the WHOI Arctic Research Initiative (TIE and LG).

Author Posting. © The Author(s), 2016. This is the author's version of the work. It is posted here by permission of Arizona Board of Regents on behalf of the University of Arizona for personal use, not for redistribution. The definitive version was published in Radiocarbon 58 (2016): 709-733, doi: 10.1017/RDC.2016.86., The Last Glacial-Interglacial Transition (LGIT; 15,000-11,000 cal BP) was characterized by complex spatiotemporal patterns of climate change, with numerous studies requiring accurate chronological control to decipher leads from lags in global paleoclimatic, -environmental and archaeological records. However, close scrutiny of the few available tree-ring chronologies and 14C-dated sequences composing the IntCal13 radiocarbon calibration curve, indicates significant weakness in 14C calibration across key periods of the LGIT. Here, we present a decadally-resolved atmospheric 14C record derived from New Zealand kauri spanning the Lateglacial from ~13,100 - 11,365 cal BP. Two floating kauri 14C time series, curve-matched to IntCal13, serve as a radiocarbon backbone through the Younger Dryas. The floating Northern Hemisphere (NH) 14C datasets derived from the YD-B and Central European Lateglacial Master tree-ring series are matched against the new kauri data, forming a robust NH 14C time series to ~14,200 cal BP. Our results show that IntCal13 is questionable from ~12,200 - 11,900 cal BP and the ~10,400 BP 14C plateau is approximately five decades too short. The new kauri record and re-positioned NH pine 14C series offer a refinement of the international 14C calibration curves IntCal13 and SHCal13, providing increased confidence in the correlation of global paleorecords., This work was part funded by the Foundation for Research, Science and Technology (FRST)—now Ministry for Business, Innovation & Employment (MBIE)-PROP-20224-SFK-UOA), a Royal Society of New Zealand grant, the Australian Research Council (FL100100195 and DP0664898) and the Natural Environment Research Council (NE/H009922/1, NE/I007660/1, NER/A/S/2001/01037 and NE/H007865/1).

© The Author(s), 2016. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Scientific Reports 6 (2016): 25902, doi:10.1038/srep25902., The Greenland Stadial 1 (GS-1; ~12.9 to 11.65 kyr cal BP) was a period of North Atlantic cooling, thought to have been initiated by North America fresh water runoff that caused a sustained reduction of North Atlantic Meridional Overturning Circulation (AMOC), resulting in an antiphase temperature response between the hemispheres (the ‘bipolar seesaw’). Here we exploit sub-fossil New Zealand kauri trees to report the first securely dated, decadally-resolved atmospheric radiocarbon (14C) record spanning GS-1. By precisely aligning Southern and Northern Hemisphere tree-ring 14C records with marine 14C sequences we document two relatively short periods of AMOC collapse during the stadial, at ~12,920-12,640 cal BP and 12,050-11,900 cal BP. In addition, our data show that the interhemispheric atmospheric 14C offset was close to zero prior to GS-1, before reaching ‘near-modern’ values at ~12,660 cal BP, consistent with synchronous recovery of overturning in both hemispheres and increased Southern Ocean ventilation. Hence, sustained North Atlantic cooling across GS-1 was not driven by a prolonged AMOC reduction but probably due to an equatorward migration of the Polar Front, reducing the advection of southwesterly air masses to high latitudes. Our findings suggest opposing hemispheric temperature trends were driven by atmospheric teleconnections, rather than AMOC changes., This work was part funded by the Foundation for Research, Science and Technology (FRST)—now Ministry for Business, Innovation & Employment (MBIE)-PROP-20224-SFK-UOA), a Royal Society of New Zealand grant, the Australian Research Council (FL100100195 and DP0664898) and the Natural Environment Research Council (NE/H009922/1, NE/I007660/1, NER/A/S/2001/01037 and NE/H007865/1).

The circulation of intermediate waters plays an important role in global heat and carbon transport in the ocean and changes in their distribution are closely tied to glacial-interglacial climate change. Coupled radiocarbon and U/Th measurements on deep-sea Desmophyllum dianthus corals allow for the reconstruction of past intermediate water ventilation. We present a high-resolution time series of Antarctic Intermediate Water radiocarbon from 44 corals spanning 30 ka through the start of the Holocene, encompassing the transition into the Last Glacial Maximum (LGM) and the last deglaciation. Corals were collected south of Tasmania from water depths between 1430 and 1950 m with 80% of them between 1500 and 1700 m, giving us a continuous record from a narrow depth range. The record shows three distinct periods of circulation: the MIS 3-2 transition, the LGM/Heinrich Stadial 1 (extending from similar to 22 to 16 kyr BP), and the Antarctic Cold Reversal (ACR). The MIS 3-2 transition and the ACR are characterized by abrupt changes in intermediate water radiocarbon while the LGM time period generally follows the atmosphere at a constant offset, in support of the idea that the LGM ocean was at steady state for its C-14 distribution. Closer inspection of the LGM time period reveals a 40 parts per thousand jump at similar to 19 ka from an atmospheric offset of roughly 230 parts per thousand to 190 parts per thousand, coincident with an observed 10-15 m rise in sea level and a southward shift of the Subantarctic and Polar Fronts, an abrupt change not seen in deeper records. During the ACR time period intermediate water radiocarbon is on average less offset from the atmosphere (similar to 110 parts per thousand) and much more variable. This variability has been captured within the lifetimes of three individual corals with changes of up to 35 parts per thousand over similar to 40 yr, likely caused by the movement of Southern Ocean fronts. This surprising result of relatively young

Author Posting. © Arizona Board of Regents on behalf of the University of Arizona, 2004. This article is posted here by permission of Dept. of Geosciences, University of Arizona for personal use, not for redistribution. The definitive version was published in Radiocarbon 46 (2004): 1225-1238., The radiocarbon calibration curve IntCal04 extends back to 26 cal kyr BP. While several high-resolution records exist beyond this limit, these data sets exhibit discrepancies of up to several millennia. As a result, no calibration curve for the time range 26–50 cal kyr BP can be recommended as yet, but in this paper the IntCal04 working group compares the available data sets and offers a discussion of the information that they hold.

Author Posting. © Arizona Board of Regents on behalf of the University of Arizona, 2009. This article is posted here by permission of Dept. of Geosciences, University of Arizona for personal use, not for redistribution. The definitive version was published in Radiocarbon 51 (2009): 1111-1150., The IntCal04 and Marine04 radiocarbon calibration curves have been updated from 12 cal kBP (cal kBP is here defined as thousands of calibrated years before AD 1950), and extended to 50 cal kBP, utilizing newly available data sets that meet the IntCal Working Group criteria for pristine corals and other carbonates and for quantification of uncertainty in both the 14C and calendar timescales as established in 2002. No change was made to the curves from 0–12 cal kBP. The curves were constructed using a Markov chain Monte Carlo (MCMC) implementation of the random walk model used for IntCal04 and Marine04. The new curves were ratified at the 20th International Radiocarbon Conference in June 2009 and are available in the Supplemental Material at www.radiocarbon.org., We would like to acknowledge support for this project from the UK Natural Environment Research Council NE/E018807/1 and IGBP PAGES (Past Global Changes).

Author Posting. © Arizona Board of Regents on behalf of the University of Arizona, 2004. This article is posted here by permission of Dept. of Geosciences, University of Arizona for personal use, not for redistribution. The definitive version was published in Radiocarbon 46 (2004): 1029-1058., A new calibration curve for the conversion of radiocarbon ages to calibrated (cal) ages has been constructed and internationally ratified to replace IntCal98, which extended from 0–24 cal kyr BP (Before Present, 0 cal BP = AD 1950). The new calibration data set for terrestrial samples extends from 0–26 cal kyr BP, but with much higher resolution beyond 11.4 cal kyr BP than IntCal98. Dendrochronologically-dated tree-ring samples cover the period from 0–12.4 cal kyr BP. Beyond the end of the tree rings, data from marine records (corals and foraminifera) are converted to the atmospheric equivalent with a site-specific marine reservoir correction to provide terrestrial calibration from 12.4–26.0 cal kyr BP. A substantial enhancement relative to IntCal98 is the introduction of a coherent statistical approach based on a random walk model, which takes into account the uncertainty in both the calendar age and the 14C age to calculate the underlying calibration curve (Buck and Blackwell, this issue). The tree-ring data sets, sources of uncertainty, and regional offsets are discussed here. The marine data sets and calibration curve for marine samples from the surface mixed layer (Marine04) are discussed in brief, but details are presented in Hughen et al. (this issue a). We do not make a recommendation for calibration beyond 26 cal kyr BP at this time; however, potential calibration data sets are compared in another paper (van der Plicht et al., this issue).

Author Posting. © Arizona Board of Regents on behalf of the University of Arizona, 2004. This article is posted here by permission of Dept. of Geosciences, University of Arizona for personal use, not for redistribution. The definitive version was published in Radiocarbon 46 (2004): 1059-1086., New radiocarbon calibration curves, IntCal04 and Marine04, have been constructed and internationally ratified to replace the terrestrial and marine components of IntCal98. The new calibration data sets extend an additional 2000 yr, from 0–26 cal kyr BP (Before Present, 0 cal BP = AD 1950), and provide much higher resolution, greater precision, and more detailed structure than IntCal98. For the Marine04 curve, dendrochronologically-dated tree-ring samples, converted with a box diffusion model to marine mixed-layer ages, cover the period from 0–10.5 cal kyr BP. Beyond 10.5 cal kyr BP, high-resolution marine data become available from foraminifera in varved sediments and U/Th-dated corals. The marine records are corrected with site-specific 14C reservoir age information to provide a single global marine mixed-layer calibration from 10.5–26.0 cal kyr BP. A substantial enhancement relative to IntCal98 is the introduction of a random walk model, which takes into account the uncertainty in both the calendar age and the 14C age to calculate the underlying calibration curve (Buck and Blackwell, this issue). The marine data sets and calibration curve for marine samples from the surface mixed layer (Marine04) are discussed here. The tree-ring data sets, sources of uncertainty, and regional offsets are presented in detail in a companion paper by Reimer et al. (this issue)., A portion of this work was performed under National Science Foundation grant ATM-0407554. A portion of this work was performed under the auspices of the U S Department of Energy by the University of California, Lawrence Livermore National Laboratory under Contract No. W-7405-Eng-48.

Author Posting. © Arizona Board of Regents on behalf of the University of Arizona, 2004. This article is posted here by permission of Dept. of Geosciences, University of Arizona for personal use, not for redistribution. The definitive version was published in Radiocarbon 46 (2004): 1161-1187., This paper describes the methods used to develop the Cariaco Basin PL07-58PC marine radiocarbon calibration data set. Background measurements are provided for the period when Cariaco samples were run, as well as revisions leading to the most recent version of the floating varve chronology. The floating Cariaco chronology has been anchored to an updated and expanded Preboreal pine tree-ring data set, with better estimates of uncertainty in the wiggle-match. Pending any further changes to the dendrochronology, these results represent the final Cariaco 58PC calibration data set., This work was supported by LLNL (97-ERI-009), DOE (W-7405-Eng-48), and NSF (ATM- 9709563).

Author Posting. © Arizona Board of Regents on behalf of the University of Arizona, 2007. This article is posted here by permission of Dept. of Geosciences, University of Arizona for personal use, not for redistribution. The definitive version was published in Radiocarbon 49 (2007): 441-445., A preliminary determination of the absolute 14C/12C ratio of the oxalic acid I standard (NBS SRM 4990B) has been made. Using an accelerator mass spectrometry (AMS) system, a known number of radiocarbon ions were implanted in a thin copper foil. The foil was then combusted with the addition of 14C-free carrier material. This resulting gas (which had a known 14C/12C ratio) was graphitized and compared to OX-I material. This comparison yielded an absolute 14C/12C ratio of OX-I. The absolute 14C/12C ratio of OX-I, coupled with knowledge of the specific activity of OX-1, provides an alternative determination of the 14C half-life.

Author Posting. © The Authors. This work is licensed under a Creative Commons Attribution 3.0 License The definitive version was published in Radiocarbon 52 (2010): 301-309., We present a status report of the accelerator mass spectrometry (AMS) facility at the University of California, Irvine, USA. Recent spectrometer upgrades and repairs are discussed. Modifications to preparation laboratory procedures designed to improve sample throughput efficiency while maintaining precision of 2–3‰ for 1-mg samples (Santos et al. 2007c) are presented.

Flask samples from two sites in East Asia, Tae-Ahn Peninsula, Korea (TAP), and Shangdianzi, China (SDZ), were measured for trace gases including CO2, CO and fossil fuel CO2(CO(2)ff, derived from Delta(CO2)-C-14 observations). The five-year TAP record shows high CO(2)ff when local air comes from the Korean Peninsula. Most samples, however, reflect air masses from Northeastern China with lower CO(2)ff. Our small set of SDZ samples from winter 2009/2010 have strongly elevated CO(2)ff. Biospheric CO2 contributes substantially to total CO2 variability at both sites, even in winter when non-fossil CO2 sources (including photosynthesis, respiration, biomass burning and biofuel use) contribute 20-30% of the total CO2 enhancement. Carbon monoxide (CO) correlates strongly with CO(2)ff. The SDZ and TAP far-field (China influenced) samples have CO: CO(2)ff ratios (R-CO:CO2ff) of 47 +/- 2 and 44 +/- 3 ppb/ppm respectively, consistent with recent bottom-up inventory estimates and other observational studies. Locally influenced TAP samples fall into two distinct data sets, ascribed to air sourced from South Korea and North Korea. The South Korea samples have low R-CO:CO2ff of 13 +/- 3 ppb/ppm, slightly higher than bottom-up inventories, but consistent with emission ratios for other developed nations. We compare our CO(2)ff observations with modeled CO(2)ff using the FLEXPART Lagrangian particle dispersion model convolved with a bottom-up CO(2)ff emission inventories. The modeled annual mean CO(2)ff mole fractions are consistent with our observations when the model inventory includes the reported 63% increase in Chinese emissions from 2004 to 2010, whereas a model version which holds Chinese emissions flat is unable to replicate the observations.

We present a status report of the accelerator mass spectrometry (AMS) facility at the University of California, Irvine, USA. Recent spectrometer upgrades and repairs are discussed. Modifications to preparation laboratory procedures designed to improve sample throughput efficiency while maintaining precision of 2–3‰ for 1-mg samples (Santos et al. 2007c) are presented.

A preliminary determination of the absolute 14C/12C ratio of the oxalic acid I standard (NBS SRM 4990B) has been made. Using an accelerator mass spectrometry (AMS) system, a known number of radiocarbon ions were implanted in a thin copper foil. The foil was then combusted with the addition of 14C-free carrier material. This resulting gas (which had a known 14C/12C ratio) was graphitized and compared to OX-I material. This comparison yielded an absolute 14C/12C ratio of OX-I. The absolute 14C/12C ratio of OX-I, coupled with knowledge of the specific activity of OX-1, provides an alternative determination of the 14C half-life.

Author Posting. © Elsevier B.V., 2006. This is the author's version of the work. It is posted here by permission of Elsevier B.V. for personal use, not for redistribution. The definitive version was published in Quaternary Science Reviews 25 (2006): 855-862, doi:10.1016/j.quascirev.2005.09.009., A recently published radiocarbon calibration curve extending to 50,000 cal BP (Fairbanks et al. 2005) is purportedly superior to that generated by the IntCal working group beyond the end of the tree-ring data at 12,400 cal BP (Reimer et al. 2004). This claim is based, in part, on different diagenetic screening criteria and pretreatment for coral samples (Fairbanks et al. 2005; Chiu et al. 2005) which do not stand up under careful scrutiny. Also at issue is the conversion of the coral-based calibration curve to an atmospheric curve where large inter-annual variability in the sea-surface age reservoir age has been observed in the southwest Pacific where one of two sets of corals used were sampled. In addition we comment on the seemingly ad hoc statistical methods utilized by Fairbanks et al. (2005) to construct their curve. We recognize the value of the Fairbanks et al. (2005) coral radiocarbon data set, but reassert the need for multiple, independently derived data to provide confirmation and validation to all radiocarbon calibration data. This is especially important before 26,000 cal BP when lower sea-levels of the last glacial maximum exposed most coral samples to alteration by fresh water.