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Radiocarbon analyses are commonly used in a broad range of fields, including earth science, archaeology, forgery detection, isotope forensics, and physiology. Many applications are sensitive to the radiocarbon (14C) content of atmospheric CO₂, which has varied since 1890 as a result of nuclear weapons testing, fossil fuel emissions, and CO₂ cycling between atmospheric, oceanic, and terrestrial carbon reservoirs. Over this century, the ratio14C/C in atmospheric CO₂ (Δ14CO₂) will be determined by the amount of fossil fuel combustion, which decreases Δ14CO₂ because fossil fuels have lost all14C from radioactive decay. Simulations of Δ14CO₂ using the emission scenarios from the Intergovernmental Panel on Climate Change Fifth Assessment Report, the Representative Concentration Pathways, indicate that ambitious emission reductions could sustain Δ14CO₂ near the preindustrial level of 0‰ through 2100, whereas “business-as-usual” emissions will reduce Δ14CO₂ to −250‰, equivalent to the depletion expected from over 2,000 y of radioactive decay. Given current emissions trends, fossil fuel emission-driven artificial “aging” of the atmosphere is likely to occur much faster and with a larger magnitude than previously expected. This finding has strong and as yet unrecognized implications for many applications of radiocarbon in various fields, and it implies that radiocarbon dating may no longer provide definitive ages for samples up to 2,000 y old.

A decrease in the 13C/12C ratio of atmospheric CO₂ has been documented by direct observations since 1978 and from ice core measurements since the industrial revolution. This decrease, known as the 13C-Suess effect, is driven primarily by the input of fossil fuel-derived CO₂ but is also sensitive to land and ocean carbon cycling and uptake. Using updated records, we show that no plausible combination of sources and sinks of CO₂ from fossil fuel, land, and oceans can explain the observed 13C-Suess effect unless an increase has occurred in the 13C/12C isotopic discrimination of land photosynthesis. A trend toward greater discrimination under higher CO₂ levels is broadly consistent with tree ring studies over the past century, with field and chamber experiments, and with geological records of C₃ plants at times of altered atmospheric CO₂, but increasing discrimination has not previously been included in studies of long-term atmospheric 13C/12C measurements. We further show that the inferred discrimination increase of 0.014 ± 0.007‰ ppm−1 is largely explained by photorespiratory and mesophyll effects. This result implies that, at the global scale, land plants have regulated their stomatal conductance so as to allow the CO₂ partial pressure within stomatal cavities and their intrinsic water use efficiency to increase in nearly constant proportion to the rise in atmospheric CO₂ concentration.

Radiocarbon (14C) is a powerful tracer of fossil emissions because fossil fuels are entirely depleted in 14C, but observations of 14CO2 and especially 14CH4 in urban regions are sparse. We present the first observations of 14C in both methane (CH4) and carbon dioxide (CO2) in an urban area (London) using a recently developed sampling system. We find that the fossil fraction of CH4 and the atmospheric concentration of fossil CO2 are consistently higher than simulated values using the atmospheric dispersion model NAME coupled with emission inventories. Observed net biospheric uptake in June–July is not well correlated with simulations using the SMURF model with NAME. The results show the partitioning of fossil and biospheric CO2 and CH4 in cities can be evaluated and improved with 14C observations when the nuclear power plants influence is negligible. Plain Language Summary Radiocarbon (14C) is an ideal tracer of fossil emissions, as fossil fuels have lost all 14C during millions of years of burial underground. When fossil carbon is re‐introduced into the atmosphere, it exerts a strong dilution of the radiocarbon to total carbon ratio. By measuring this ratio in the atmosphere, we can quantify fossil methane and carbon dioxide emissions. This is the first combined study of 14C in both atmospheric methane and carbon dioxide at regional scale. Key Points Atmospheric radiocarbon measurements in central London reveal higher fossil CH4 and CO2 present, compared to simulations Radiocarbon measurements show biospheric uptake of CO2 in July that is stronger than simulations Nuclear power plants interfere with radiocarbon measurements in London when air is coming from Europe

High precision measurements of Δ14C were conducted for monthly samples of CO2from seven global stations over 2‐ to 16‐year periods ending in 2007. Mean Δ14C over 2005–07 in the Northern Hemisphere was 5 ‰ lower than Δ14C in the Southern Hemisphere, similar to recent observations from I. Levin. This is a significant shift from 1988–89 when Δ14C in the Northern Hemisphere was slightly higher than the South. The influence of fossil fuel CO2 emission and transport was simulated for each of the observation sites by the TM3 atmospheric transport model and compared to other models that participated in the Transcom 3 Experiment. The simulated interhemispheric gradient caused by fossil fuel CO2 emissions was nearly the same in both 1988–89 and 2005–07, due to compensating effects from rising emissions and decreasing sensitivity of Δ14C to fossil fuel CO2. The observed 5 ‰ shift must therefore have been caused by non‐fossil influences, most likely due to changes in the air‐sea14C flux in the Southern Ocean. Seasonal cycles with higher Δ14C in summer or fall were evident at most stations, with largest amplitudes observed at Point Barrow (71°N) and La Jolla (32°N). Fossil fuel emissions do not account for the seasonal cycles of Δ14C in either hemisphere, indicating strong contributions from non‐fossil influences, most likely from stratosphere‐troposphere exchange. Key Points Observations of 14CO2 were conducted at 7 sites Delta‐14C is now lower in the Northern Hemisphere, a shift from 1980s Gradients and seasonal cycles have substantial fossil and non‐fossil components

The isotopic composition of carbon (Δ14C and δ13C) in atmospheric CO2 and in oceanic and terrestrial carbon reservoirs is influenced by anthropogenic emissions and by natural carbon exchanges, which can respond to and drive changes in climate. Simulations of 14C and13C in the ocean and terrestrial components of Earth system models (ESMs) present opportunities for model evaluation and for investigation of carbon cycling, including anthropogenic CO2 emissions and uptake. The use of carbon isotopes in novel evaluation of the ESMs' component ocean and terrestrial biosphere models and in new analyses of historical changes may improve predictions of future changes in the carbon cycle and climate system. We compile existing data to produce records of Δ14C andδ13C in atmospheric CO2 for the historical period 1850–2015. The primary motivation for this compilation is to provide the atmospheric boundary condition for historical simulations in the Coupled Model Intercomparison Project 6 (CMIP6) for models simulating carbon isotopes in the ocean or terrestrial biosphere. The data may also be useful for other carbon cycle modelling activities.

Radiocarbon observations (Δ14C) in dissolved inorganic carbon (DIC) of seawater provide useful information about ocean carbon cycling and ocean circulation. To deliver high-quality observations, the Laboratory of Ion Beam Physics (LIP) at ETH-Zurich developed a new simplified method allowing the rapid analysis of radiocarbon in DIC of small seawater samples, which is continually assessed by following internal quality controls. However, a comparison with externally produced 14C measurements to better establish an equivalency between methods was still missing. Here, we make the first intercomparison with the National Ocean Sciences Accelerator Mass Spectrometry (NOSAMS) facility based on 14 duplicate seawater samples collected in 2020. We also compare with prior deep-water observations from the 1970s to 1990s. The results show a very good agreement in both comparisons. The mean Δ14C of 12 duplicate samples measured by LIP and NOSAMS were statistically identical within one sigma uncertainty while two other duplicate samples agreed within two sigma. Based on this small number of duplicate samples, LIP values appear to be slightly lower than the NOSAMS values, but more measurements will be needed for confirmation. We also comment on storage and preservation techniques used in this study, including the freezing of samples collected in foil bags.

Coordinated experimental design and implementation has become a cornerstone of global climate modelling. Model Intercomparison Projects (MIPs) enable systematic and robust analysis of results across many models, by reducing the influence of ad hoc differences in model set-up or experimental boundary conditions. As it enters its 6th phase, the Coupled Model Intercomparison Project (CMIP6) has grown significantly in scope with the design and documentation of individual simulations delegated to individual climate science communities. The Coupled Climate-Carbon Cycle Model Intercomparison Project (C4MIP) takes responsibility for design, documentation, and analysis of carbon cycle feedbacks and interactions in climate simulations. These feedbacks are potentially large and play a leading-order contribution in determining the atmospheric composition in response to human emissions of CO2 and in the setting of emissions targets to stabilize climate or avoid dangerous climate change. For over a decade, C4MIP has coordinated coupled climate-carbon cycle simulations, and in this paper we describe the C4MIP simulations that will be formally part of CMIP6. While the climate-carbon cycle community has created this experimental design, the simulations also fit within the wider CMIP activity, conform to some common standards including documentation and diagnostic requests, and are designed to complement the CMIP core experiments known as the Diagnostic, Evaluation and Characterization of Klima (DECK). C4MIP has three key strands of scientific motivation and the requested simulations are designed to satisfy their needs: (1) pre-industrial and historical simulations (formally part of the common set of CMIP6 experiments) to enable model evaluation, (2) idealized coupled and partially coupled simulations with 1 % per year increases in CO2 to enable diagnosis of feedback strength and its components, (3) future scenario simulations to project how the Earth system will respond to anthropogenic activity over the 21st century and beyond. This paper documents in detail these simulations, explains their rationale and planned analysis, and describes how to set up and run the simulations. Particular attention is paid to boundary conditions, input data, and requested output diagnostics. It is important that modelling groups participating in C4MIP adhere as closely as possible to this experimental design.

Carbon monoxide (CO) is an atmospheric pollutant with a positive net warming effect on the climate. The magnitude of CO sources and the fraction of fossil vs biogenic sources are still uncertain and vary across emissions inventories. Measurements of radiocarbon (14C) in CO could potentially be used to investigate the sources of CO on a regional scale because fossil sources lack 14C and reduce the 14C/C ratio (Δ14C) of atmospheric CO more than biogenic sources. We use regional Lagrangian model simulations to investigate the utility of Δ14CO measurements for estimating the fossil fraction of CO emissions and evaluating bottom-up emissions estimates (United Kingdom Greenhouse Gas, UKGHG, and TNO Copernicus Atmosphere Monitoring Service, TNO) in London, UK. Due to the high Δ14CO in atmospheric CO from cosmogenic production, both fossil and biogenic CO emissions cause large reductions in Δ14CO regionally, with larger reductions for fossil than biogenic CO per ppb added. There is a strong seasonal variation in Δ14CO in background air and in the sensitivity of Δ14CO to fossil and biogenic emissions of CO. In the UK, the CO emissions estimate from TNO has a higher fraction from fossil fuels than UKGHG (72% vs 67%). This results in larger simulated decreases in Δ14C per ppb CO for TNO emissions. The simulated differences between UKGHG and TNO are likely to be easily detectable by current measurement precision, suggesting that Δ14CO measurements could be an effective tool to understand regional CO sources and assess bottom-up emissions estimates.

Reflecting recent advances in our understanding of soil organic carbon (SOC) turnover and persistence, a new generation of models increasingly makes the distinction between the more labile soil particulate organic matter (POM) and the more persistent mineral-associated organic matter (MAOM). Unlike the typically poorly defined conceptual pools of traditional SOC models, the POM and MAOM soil fractions can be directly measured for their carbon content and isotopic composition, allowing for fraction-specific data assimilation. However, the new-generation model predictions of POM and MAOM dynamics have not yet been validated with fraction-specific carbon and 14C observations. In this study, we evaluate five influential and actively developed new-generation models (CORPSE, MEND, Millennial, MIMICS, SOMic) with fraction-specific and bulk soil 14C measurements of 77 mineral topsoil profiles in the International Soil Radiocarbon Database (ISRaD). We find that all five models consistently overestimate the 14C content (Δ14C) of POM by 69 ‰ on average, and two out of the five models also strongly overestimate the Δ14C of MAOM by more than 80 ‰ on average, indicating that the models generally overestimate the turnover rates of SOC and do not adequately represent the long-term stabilization of carbon in soils. These results call for more widespread usage of fraction-specific carbon and 14C measurements for parameter calibration and may even suggest that some new-generation models might need to restructure or further subdivide their simulated carbon pools in order to accurately reproduce SOC dynamics.

High precision measurements of Δ 14 C were performed on CO 2 sampled at La Jolla, California, USA over 1992–2007. A decreasing trend in Δ 14 C was observed, which averaged −5.5 ‰ yr −1 yet showed significant interannual variability. Contributions to the trend in global tropospheric Δ 14 C by exchanges with the ocean, terrestrial biosphere and stratosphere, by natural and anthropogenic 14 C production and by 14 C‐free fossil fuel CO 2 emissions were estimated using simple models. Dilution by fossil fuel emissions made the strongest contribution to the Δ 14 C trend while oceanic 14 C uptake showed the most significant change between 1992 and 2007, weakening by 70%. Relatively steady positive influences from the stratosphere, terrestrial biosphere and 14 C production moderated the decreasing trend. The most prominent excursion from the average trend occurred when Δ 14 C decreased rapidly in 2000. The rapid decline in Δ 14 C was concurrent with a rapid decline in atmospheric O 2 , suggesting a possible cause may be the anomalous ventilation of deep 14 C‐poor water in the North Pacific Ocean. We additionally find the presence of a 28‐month period of oscillation in the Δ 14 C record at La Jolla. Observations of 14CO2 were conducted over 16 yrs Fossil fuel emissions are the strongest influence on the decreasing trend Ocean uptake may now be weaker than preindustrial, may vary interannually