Holocene variations in the North Atlantic marine radiocarbon reservoir effect

This thesis aims to examine the spatial and temporal characteristics of the ¹⁴C marine reservoir effect (MRE) in the North Atlantic over the Holocene. The MRE is a time dependant offset in ¹⁴C age between the atmospheric and ocean carbon reservoirs and accurate quantification of MRE correction values is crucial for radiocarbon chronologies. In a specific ocean area the MRE may show a deviation (known as ΔR) from the average value for the global average surface oceans given by the marine calibration curve (currently MARINE04). This occurs as a function of local oceanographic and climatic variables and current research has identified the potential for both spatial and temporal variations in ΔR values. A new and rigorous sample selection protocol was developed for this study to produce a large number of ΔR determinations that have a high degree of accuracy and precision. This involved selection of multiple single entity samples of both marine and terrestrial material from 30 clearly-defined deposits at 20 archaeological sites in Western Ireland, the island belts ofNorthern and Western Scotland, the western and northern Scottish mainland coast and the Faroe Isles. A total of 301 radiocarbon (¹⁴C) measurements were made of sample material and the overall results demonstrate observable spatial and temporal variability in ΔR within the study area over the past c.8000 years. These can be related to climate and oceanographic changes previously identified as potential mechanisms for producing variation in ΔR. The interpretations drawn from this study were as follows:1. At sites selected according to the study protocol a range of marine mollusc species can be used to accurately determine ΔR. || 2. In the Early Holocene (c.6480-1940 BC) ΔR values were greater relative to that of later periods. || 3. During the periods c.400 BC - 60 AD and c. 1000-1200 AD, ΔR values were reduced relative to those of the present day || 4. During the period c.1200-1400 AD, ΔR values were higher compared to the present. || 5. In addition, there is evidence for spatial variation in ΔR within the study area over the Holocene. This is illustrated at c. 1000-1200 AD when a large number of measurements indicate an increase in ΔR value northwards from the west coast of Ireland to the Faroe IslesThe results of this study have important implications for our understanding of the MRE and the effective application of correction values to marine samples for ¹⁴C measurement within both paleoenvironmental and archaeological research

A period of calm in Scottish seas: a comprehensive study of ΔR values for the northern British Isles coast and the consequent implications for archaeology and oceanography

The Marine Radiocarbon Reservoir Effect (MRE) is a 14C age offset between contemporaneous marine- and terrestrially-derived carbon. In Northern Hemisphere surface waters it is of the order of 400 years but temporal and spatial deviations, known as ΔR, occur. This study provides a comprehensive dataset of 21 ΔR and MRE values for the east coast of Scotland and 21 recalculated values for the west coast of Scotland and Ireland, for the period c. 3500 BC to 1450 AD. They are presented as mean, site-specific ΔR and MRE values, together with their associated uncertainties, calculated as standard errors for predicted values. The ΔR values range from -320 ± 35 to +150 ± 28 14C years and show no spatial or temporal trends. The MRE values range from 59 ± 40 to 531 ± 26, show an almost identical distribution pattern to the ΔR values and again show no spatial or temporal trends. Results show that ΔR values calculated for a single site using statistically indistinguishable groups of terrestrial and marine radiocarbon age measurements can produce variability of up to 225 14C years. ΔR is an important factor in the accurate calibration of samples containing marine-derived carbon for archaeological interpretation but is often also used as an indicator of changes in 14C specific activity of the oceans, and therefore a proxy for changes in ocean circulation and/or climate. Using the methods outlined in this paper, it is apparent that ΔR values for the northern part of the British Isles have been relatively stable, within our ability to quantify non-random variation in the data. The fact that significant climatic shifts have been recorded during this time, yet these are not visible in the ΔR data, presents a cautionary tale regarding the use of ΔR to infer large-scale oceanographic or climatic changes. Upon the exclusion of 5 outliers from the 42 values, the remaining ΔR values are statistically indistinguishable from one another and range from -142 ± 61 to +40 ± 47 14C years. 34 of these values are from Scottish archaeological sites and can be combined to produce a mean value for Scotland of -47 ± 52 14C years for the period 3500 BC to 1450 AD, to be used only in the absence of site- and period-specific data

Stable polycyclic aromatic carbon (SPAC) content as an improved parameter for determining biochar stability

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Advances in the radiocarbon analysis of carbon dioxide at the NERC radiocarbon facility (East Kilbride) using molecular sieve cartridges

Radiocarbon (14C) analysis of carbon dioxide (CO2) provides unique information on the age, turnover and source of this important greenhouse gas, raising the prospect of novel scientific investigations into a range of natural and anthropogenic processes. To achieve these measurements, cartridges containing zeolite molecular sieves are a reliable and convenient method for collecting CO2 samples. At the NERC Radiocarbon Facility (East Kilbride) we have been refining our molecular sieve methods for over twenty years to achieve high-quality, reproducible and precise measurements. At the same time, we have been developing novel field sampling methods to expand the possibilities in collecting gas from the atmosphere, soil respiration and aquatic environments. Here, we present our latest improvements to cartridge design and procedures. We provide the results of tests used to verify the methods using known 14C content standards, demonstrating reliability for sample volumes of 3 mL CO2 (STP; 1.6 mg C) collected in cartridges that had been prepared at least three months earlier. We also report the results of quality assurance standards processed over the last two years, with results for 22 out of 23 international 14C standards being within measurement uncertainty of consensus values. We describe our latest automated procedures for the preparation of cartridges prior to use

Holocene variations in the Scottish marine radiocarbon reservoir effect

We assessed the evidence for variations in the marine radiocarbon reservoir effect (MRE) at coastal, archaeological Iron Age sites in north and west Scotland by comparing AMS measurements of paired marine and terrestrial materials (4 pairs per context). DeltaR values were calculated from measurements on material from 3 sites using 6 sets of samples, all of which were deposited around 2000 BP. The weighted mean of the DeltaR determinations was -79 +/- 17 C-14 yr, which indicates a consistent, reduced offset between atmospheric and surface ocean C-14 specific activity for these sites during this period, relative to the present day (DeltaR = similar to0 C-14 yr). We discuss the significance of this revised AR correction by using the example of wheelhouse chronologies at Hornish Point and their development in relation to brochs. In addition, we assess the importance of using the concepts of MRE correction and AR variations when constructing chronologies using C-14 measurements made on materials that contain marine- derived carbon

Wood-Based Carbon Storage in the Mackenzie River Delta: The World\u27s Largest Mapped Riverine Wood Deposit

The Mackenzie River Delta (MRD) has been recognized as an important host of river-derived wood deposits, and Mackenzie River wood has been found across the Arctic Ocean. Nevertheless, we lack estimates of the amount of carbon stored as wood and its age in the delta, representing a gap in carbon cycle estimates. Here, we use very high-resolution satellite imagery and deep learning to map wood deposits in the MRD, combining this with field data to measure the stock and age of wood-based carbon. We find \u3e400,000 individual large wood deposits, collectively storing 3.1 × 1012 g-C, equating to 2 × 106 g-C ha−1 across the delta. Sampled wood pieces date from 690 AD to 2015 AD but are mostly young with ∼40% of the wood samples formed after 1955 AD. These estimates represent a minimum bound on an important surficial, potentially reactive, carbon pool compared to other deeper carbon stocks in permafrost zones

Performance of the rebuilt SUERC single-stage accelerator mass spectrometer

The SUERC bipolar single-stage accelerator mass spectrometer (SSAMS) has been dismantled and rebuilt to accommodate an additional rotatable pre-accelerator electrostatic spherical analyser (ESA) and a second ion source injector. This is for the attachment of an experimental positive-ion electron cyclotron resonance (ECR) ion source in addition to a Cs-sputter source. The ESA significantly suppresses oxygen interference to radiocarbon detection, and remaining measurement interference is now thought to be from 13C injected as 13CH molecule scattering off the plates of a second original pre-detector ESA

8.2 ka event North Sea hydrography determined by bivalve shell stable isotope geochemistry

The abrupt 8.2 ka cold event has been widely described from Greenland and North Atlantic records. However, its expression in shelf seas is poorly documented, and the temporal resolution of most marine records is inadequate to precisely determine the chronology of major events. A robust hydrographical reconstruction can provide an insight on climatic reaction times to perturbations to the Atlantic Meridional Overturning Circulation. Here we present an annually-resolved temperature and water column stratification reconstruction based on stable isotope geochemistry of Arctica islandica shells from the Fladen Ground (northern North Sea) temporally coherent with Greenland ice core records. Our age model is based on a growth increment chronology obtained from four radiometrically-dated shells covering the 8290–8100 cal BP interval. Our results indicate that a sudden sea level rise (SSLR) event-driven column stratification occurred between ages 8320–8220 cal BP. Thirty years later, cold conditions inhibited water column stratification but an eventual incursion of sub-Arctic waters into the North Sea re-established density-driven stratification. The water temperatures reached their minimum of ~3.7 °C 55 years after the SSLR. Intermittently-mixed conditions were later established when the sub-Arctic waters receded

Assessing the Effect of Sterilization on the Radiocarbon Signature of Freshwater Dissolved Organic Carbon

Radiocarbon analysis of freshwater dissolved organic carbon (DOC) involves substantial sample pretreatment, including an initial rotary evaporation stage necessary to concentrate large volumes of freshwater sample. This may lead to a health risk from the exposure to pathogens, and there is the additional concern that the warm conditions during the rotary evaporation stage may provide ideal growing conditions for some pathogens. To remove any pathogen risk in water samples, boiling or autoclaving can be undertaken. However, to date, no studies have been undertaken to investigate whether boiling will alter the 14C signature of dissolved organic carbon. Here, we analyze the effect of sterilization on 9 contrasting river water samples. Comparing filtered, filtered and boiled, and filtered and sterilized dissolved organic matter, we observe that both boiling and autoclaving increases the uncertainty associated with the 14C and 13C of DOC, that the 14C and 13C changes are not unidirectional, and that they are not related to original DOC composition. Neither sterilization method is recommended unless essential, in which instance we recommend a 3 uncertainty on 14C and that the 13C is not considered representative of the original sample.The Radiocarbon archives are made available by Radiocarbon and the University of Arizona Libraries. Contact [email protected] for further information.Migrated from OJS platform February 202

Chemical characteristics of macroscopic pyrogenic carbon following millennial-scale environmental exposure

Pyrogenic Carbon (PyC) is ubiquitous in global environments, and is now known to form a significant, and dynamic component of the global carbon cycle, with at least some forms of PyC persisting in their depositional environment for many millennia. Despite this, the factors that determine the turnover of PyC remain poorly understood, as do the physical and chemical changes that this material undergoes when exposed to the environment over tens of thousands of years. Here, we present the results of an investigation to address these knowledge gaps through chemical and physical analysis of a suite of wood PyC samples exposed to the environment for varying time periods, to a maximum of >90,000 years. This includes an assessment of the quantity of resistant carbon, known as Stable Polyaromatic Carbon (SPAC) versus more chemically labile carbon in the samples. We find that, although production temperature is likely to determine the initial ‘degradation potential’ of PyC, an extended exposure to environmental conditions does not necessarily mean that remaining PyC always progresses to a ‘SPAC-dominant’ state. Instead, some ancient PyC can be composed largely of chemical components typically thought of as environmentally labile, and it is likely that the depositional environment drives the trajectory of preservation versus loss of PyC over time. This has important implications for the size of global PyC stocks, which may have been underestimated, and also for the potential loss of previously stored PyC, when its depositional environment alters through environmental or climatic changes