Atmospheric 14C Activity Research Articles

Forensic Radiocarbon Dating of Human Remains

Radiocarbon dating is a valuable tool for the forensic examination of human remains in answering questions as to whether the remains are of forensic or medico-legal interest or archaeological in date. The technique is also potentially capable of providing the year of birth and/or death of an individual. Atmospheric radiocarbon levels are currently enhanced relative to the natural level due to the release of large quantities of radiocarbon (14C) during the atmospheric nuclear weapons testing of the 1950s and 1960s. This spike, or “bomb-pulse,” can, in some instances, provide precision dates to within 1–2 calendar years. However, atmospheric 14C activity has been declining since the end of atmospheric weapons testing in 1963 and is likely to drop below the natural level by the mid-twenty-first century, with implications for the application of radiocarbon dating to forensic specimens.

Study of isotopes of carbon, thorium, and uranium in travertine and thermal spring samples: implications for effects of changes in geochemical environment and processes

ABSTRACTData on modern radiocarbon activity in the old travertine formations of the Pymvashor hydrothermal system were used, in combination with 230Th/U dating of the travertine, to estimate the 14C contents of the total dissolved inorganic carbon in the ancient thermal water at the time of precipitation of the travertine (14Ccalc). With the known values of 14Ccalc and average age of the thermal water, and under the assumption that the residence time of the water in aquifer was constant over the last 13.9 ± 1.5 ka, the initial 14C contents (14C0) in the ancient thermal water were estimated. The findings in this study are that (1) both 14C0 and δ13С have decreased in young waters compared to the ancient waters; (2) although atmospheric 14C activity (14Catm) has also decreased in the same time, the decrease in 14C0 is faster than the decrease in 14Catm. Under certain assumptions, one could link changes in 14C0 and δ13C to climate change. Decrease in δ13С of soil CO2 and decrease in 14C0 was caused predominantly by warmer and wetter climate, decomposition of fossil organic matter, and decrease in 14Catm. There could be also increased dissolution of solid carbonate and increased carbon exchange between DIC and soil CO2, caused by thawing permafrost.

Determination of biogenic component in liquid fuels by the 14C direct LSC method by using quenching properties of modern liquids for calibration

The fraction of biogenic component within various types of materials that can be used as fuels for energy production and transport can be determined by measuring their 14C activity. The method is based on different 14C signatures of the biogenic and the fossil components: while the biogenic component reflects the modern atmospheric 14C activity, no 14C is present in fossil fuels. A direct measurement of the 14C content in liquid fuel by liquid scintillation counter is a simple and fast technique but has a main disadvantage: different liquid colors cause different quenching properties and affect the measurement efficiency. We propose a new evaluation technique that uses liquids of different colors to construct modern and background calibration curves. Various binary mixtures of biogenic liquids have been used to verify the relation between the count rate and the quenching parameter. Mixtures of a biogenic and a 14C-free liquid demonstrated the potential of the proposed technique for determining the biogenic fraction of a mixture.

The TOCATTA-χ model for assessing 14C transfers to grass: an evaluation for atmospheric operational releases from nuclear facilities

Radioactive 14C is formed as a by-product of nuclear power generation and from the operation of nuclear fuel reprocessing plants like AREVA-NC La Hague (North France), which releases about 15 TBq per year of 14C into the atmosphere. This article evaluates a recently improved radioecology model (TOCATTA-χ) to assess 14C transfers to grassland ecosystems under normal operating conditions. The new version of the TOCATTA model (TOCATTA-χ) includes developments that were derived from PaSiM, a pasture model for simulating grassland carbon and radiocarbon cycling. The TOCATTA-χ model has been tested against observations of 14C activity concentrations in grass samples collected monthly from six plots which are located around the periphery of the reprocessing plant. Simulated 14C activities are consistent with observations on both intensively managed and poorly managed grasslands, but an adaptation of the mean turn-over time for 14C within the plant is necessary in the model to account for different management practices. When atmospheric 14C activity concentrations are directly inferred from observations, TOCATTA-χ performs better than TOCATTA (the root mean square error is decreased by 45%), but when atmospheric 14C activity concentrations are not known and must be calculated, the uncertainty associated with the TOCATTA-χ model outcomes is estimated to be larger than the standard deviation of the observations.

Spatial variability of 14C reservoir effects in Tibetan Plateau lakes

Radiocarbon dating of lake sediments is often hampered by the presence of a lake reservoir effect (LRE, also ‘dead carbon’ or ‘old carbon’ effect) especially in dry and cold regions with a sparse plant cover in the catchment. The Tibetan Plateau became a hotspot of the palaeoenvironmental and climate research community in recent years and the assessment of present-day LREs is a crucial prerequisite for the establishment of reliable radiocarbon age–depth relationships for lake sediment cores. This paper examines the spatial variability of LREs within individual lakes, through a discussion of new data for Lake Donggi Cona and a compilation of previously published data for five additional lakes where LRE data are available for different sites. Lake reservoir effects for Lake Donggi Cona on the northeastern Tibetan Plateau were determined for shells of aquatic snails collected alive close to the lake's shore. The largest determined LRE of 20,000 14C years is significantly larger than previously reported LREs from the central part of the lake, and larger than any previously published LRE for the Tibetan Plateau. Relatively low LREs in the central regions of lakes, higher LREs towards the margins, and high LREs in tributaries and spring waters are apparently a common pattern of Tibetan Plateau lakes. The differences in LREs within individual lakes or catchment areas are attributed to the more prolonged exchange of the lake water's dissolved inorganic carbon with the atmospheric CO2 in central lake regions on the one hand and the increasing influence of 14C free or poor stream and groundwater due to the dissolution of carbonaceous basement rocks towards its margins. Generally higher LREs were recorded in the three tectonically active lake regions of the six examined catchments, and it is speculated that rising crustal CO2 further contributes to the LREs in these catchments. In addition to these observations and inferences, elevated 14C levels of the atmosphere as a result of nuclear bomb testing are often ignored if LREs for modern materials are reported by convention relative to the atmospheric 14C activity of the year 1950. LRE data reported in this way represent unrealistic minimum estimates.

Radiocarbon Impact on a Nearby Tree of a Light-Water VVER-Type Nuclear Power Plant, Paks, Hungary

Tree-ring series were collected for radiocarbon analyses from the vicinity of Paks nuclear power plant (NPP) and a background area (Dunaföldvár) for a 10-yr period (2000–2009). Samples of holocellulose were prepared from the wood and converted to graphite for accelerator mass spectrometry (AMS) 14C measurement using the MICADAS at ETH Zürich. The 14C concentration data from these tree rings was compared to the background tree rings for each year. The global decreasing trend of atmospheric 14C activity concentration was observed in the annual tree rings both in the background area and in the area of the NPP. As an average of the past 10 yr, the excess 14C emitted by the pressurized-water reactor (PWR) NPP to the atmosphere shows only a slight systematic excess (∼6′) 14C in the annual rings. The highest 14C excess was 13′ (in 2006); however, years with the same 14C level as the background were quite frequent in the tree-ring series.

The Influence of Soil Organic Matter Age Spectrum on the Reconstruction of Atmospheric 14C Levels Via Stalagmites

The imprint of the radiocarbon bomb peak was detected in the top of stalagmite ER-77 from Grotta di Ernesto (NE Italy). This recently grown stalagmite reveals a reservoir age, also known as dead carbon fraction (dcf), of ≃1050 14C yr, or 12%. By applying a 14C soil-karst model, the age spectrum of soil organic matter (SOM) as well as the CO2 contribution of the single SOM reservoirs to the total soil CO2 can be derived. Under the assumption of constant vegetation, meaning both vegetation density and the age spectrum of SOM, it is possible to derive the soil-air 14C activity of the past using the 14C calibration curve (IntCal04). Hence, it is also possible to calculate an artificial stalagmite 14C data set covering the last 25,000 yr with parameters determined for stalagmite ER-77. With this artificially constructed data set, we derived the hypothetical atmospheric 14C activity by using the common method of applying a constant dcf on the modeled 14C data set of the stalagmite. This theoretical approach allows to analyze the impact of a constant and variable SOM age spectrum on atmospheric 14C reconstructions performed with real stalagmite 14C measurements. We observe deviations between IntCal04 and the atmospheric 14C activity as derived with our modeled 14C data set, which are larger for older SOM than for younger SOM and vary in time up to 2 pMC, depending on the strength of the variations in the atmospheric 14C level. This value is comparable with the 1-σ uncertainty given by IntCal04 for the last glacial. For a varying SOM age spectrum, the deviations between the calibration curve and 14C level of the atmosphere reconstructed with a stalagmite exceed 3 pMC, which is larger than the 1-σ uncertainty of IntCal04. In general, the SOM has smoothing, shifting, and 14C-depleting effects on the stalagmite 14C record and, therefore, on the stalagmite-derived atmospheric 14C activity. In this study, changes in soil-air pCO2 and carbonate dissolution conditions, which have also an important impact on the 14C record of a stalagmite, are not accounted for.

Late Holocene climate oscillations and solar fluctuations from speleothem STAL‐AH‐1, Sauerland, Germany: A numerical perspective

Initial 14C activity in a late Holocene stalagmite (a14Cstal) from Attahöhle (Sauerland, Germany) varies synchronously with atmospheric 14C activity (a14Catm). This observation provides independent chronological support for the correlation between a solar forcing proxy (atmospheric 14C production rate, a14Cprod) and a climate proxy (δ18Ostal) in this stalagmite, and eliminates the need to ‘tune’ the chronology. Monte Carlo randomizations in which 100,000 synthetic δ18Ostal datasets were generated indicate that the correlation between a14Cprod and δ18Ostal is statistically robust. The absence of a significant time lag between a14Cprod and δ18Ostal implies rapid climate response at this site to variations in solar output. Positively correlated a14Cprod‐δ18Ostal indicates drier winter conditions during late Holocene solar minima. This supports atmospheric amplification models that predict reduced NAO indices during solar minima if kinetic enrichment of δ18O during dry phases outweighs the reduction of δ18O in rainfall that results from lower air temperatures during negative NAO phases.

Monitoring of atmospheric 14CO2 in central European countries

Carbon-14 is a radionuclide with global occurrence and partly natural origin. The main anthropogenic sources of the 14C were the nuclear weapon tests, namely at the beginning of the 1960s, nowadays the nuclear energy facilities are the main sources. Maximum in the atmospheric 14C activity was observed in 1963. In the following years the considerable 14C activity decrease was due to intensive carbon deposition into oceanic water and sediments particularly. At present the 14C activity approximates the level before nuclear age, corresponding to ∼0 ‰ Δ 14C. Another actual type of anthropogenic influence is the Suess effect, i.e., the dilution of 14C by fossil carbon (fuel combustion). This effect causes a decrease of the 14C activity on a global, regional and local scale. Thus, monitoring of actual reference level of 14C activity gives a possibility to indicate local or global anthropogenic influences. This paper reporting data from the atmospheric 14CO2 monitoring in the Czech Republic and Hungary compares the actual results with other European countries. The observed effects connected with local and regional CO2 releases from fossil fuel combustion are discussed.

Monitoring of atmospheric 14CO2 in central European countries

Carbon-14 is a radionuclide with global occurrence and partly natural origin. The main anthropogenic sources of the 14C were the nuclear weapon tests, namely at the beginning of the 1960s, nowadays the nuclear energy facilities are the main sources. Maximum in the atmospheric 14C activity was observed in 1963. In the following years the considerable 14C activity decrease was due to intensive carbon deposition into oceanic water and sediments particularly. At present the 14C activity approximates the level before nuclear age, corresponding to ∼0 ‰ Δ 14C. Another actual type of anthropogenic influence is the Suess effect, i.e., the dilution of 14C by fossil carbon (fuel combustion). This effect causes a decrease of the 14C activity on a global, regional and local scale. Thus, monitoring of actual reference level of 14C activity gives a possibility to indicate local or global anthropogenic influences. This paper reporting data from the atmospheric 14CO2 monitoring in the Czech Republic and Hungary compares the actual results with other European countries. The observed effects connected with local and regional CO2 releases from fossil fuel combustion are discussed.

Recharge mechanism and hydrochemistry evaluation of groundwater in the Nuaimeh area, Jordan, using environmental isotope techniques

The relationship between the stable isotopic and chemical composition of precipitation and groundwater was studied in the Nuaimeh area of the Ajloun Highlands in Jordan. The isotopic composition values of precipitation and groundwater are almost identical. The spatial variation of stable isotopes in precipitation is mainly due to the effect of seasonal temperature, altitude and amount. The groundwater reveals identical variation in isotopic composition to the precipitation due to direct recharge and the karstic nature of the outcropping Turonian aquifer. Tritium levels in wells are high and their content is similar to the weighted mean value of tritium content in precipitation, indicating local recharge and low residence time. The 14C activity in the tritiated groundwater is found to be about half of the 14C activity of precipitation in the region. A geochemical evolution through dissolution of carbonate by water–carbonate rock interactions reduced the atmospheric 14C activity from 114 to 61 pmc in the groundwater. A 14C of around 61 pmc and 7.6 TU values are considered the initial concentration for the recharge in the shallow carbonate aquifer in the Yarmouk Basin. The large fluctuation of water level in observation wells during the rainy season indicates the sensitivity and direct response of the aquifer to the recharge. The chemical composition of the groundwater (Ca2+–HCO3−) gives emphasis to the short duration of water–rock interaction and indicates dissolution of the carbonate aquifer. The elevated concentrations of Cl− and NO3− in groundwater are attributed to anthropogenic sources.

Calculation of Past Dead Carbon Proportion and Variability by the Comparison of AMS 14C and Tims U/TH Ages on Two Holocene Stalagmites

Twenty-two radiocarbon activity measurements were made by accelerator mass spectrometry (AMS) on 2 Holocene stalagmites from Belgium (Han-stm1b) and from southwest France (Vil-stm1b). Sixteen thermal ionization mass spectrometric (TIMS) U/Th measurements were performed parallel to AMS analyses. The past dead carbon proportion (dcp) due to limestone dissolution and old soil organic matter (SOM) degradation is calculated with U/Th ages, measured calcite 14C activity and atmospheric 14C activity from the dendrochronological calibration curves. Results show that the dcp is different for the 2 stalagmites: between 10,800 and 4780 yr from present dcp=17.5% (σ=2.4; n=10) for Han-stm1b and dcp=9.4% (σ=1.6; n=6) between 3070 and 520 yr for Vil-stm1b. Despite a broad stability of the dcp during the time ranges covered by each sample, a slight dcp increase of about 5.0% is observed in the Han-stm1b sample between 8500 and 5200 yr. This change is synchronous with a calcite δ13C increase, which could be due to variation in limestone dissolution processes possibly linked with a vegetation change. The dcp and δ13C of the 2 studied samples are compared with 5 other modern stalagmites from Europe. Results show that several factors intervene, among them: the vegetation type, and the soil saturation leading to variable dissolution process systems (open/closed). The good correlation (R2=0.98) between the U/Th ages and the calibrated 14C ages corrected with a constant dcp validates the 14C method. However, the dcp error leads to large 14C age errors (i.e. 250–500 yr for the period studied), which is an obstacle for both a high-resolution chronology and the improvement of the 14C calibration curves, at least for the Holocene.

The Reliability of AMS Radiocarbon Dating of Shells from China

We tested the feasibility of dating freshwater and terrestrial molluscs from the semiarid and arid zone in China, since these types of shell material deposit only aragonite to form their shell structure, and shell integrity can be easily observed using X-ray diffraction. We also tested the possibility of estimating microenvironmental changes from shell δ13C values, but variations within shell populations preclude the use of these values as a reliable indicator. Reservoir ages were calculated for living shells of the same species as fossil shells by using their measured 14C ages, which were recalculated using an average value of atmospheric 14C activity for the years spanning their time of collection as the modern standard. The results indicate that freshwater and terrestrial shells are potentially useful as dating material, provided extreme care is taken in their collection and other datable material (in this case wood and pollen) is within the profile to act as a comparison.

Two Decades of Environmental Isotope Records in Croatia: Reconstruction of the Past and Prediction of Future Levels

A two-decade-long record of environmental isotopes (2H, 3H, 14C, 18O) in Croatia is presented and the data are statistically analyzed. The atmospheric 14C activity for the period before the actual measurements started is reconstructed by measuring tree rings from the clean-air sites, and the past tritium activity in precipitation is estimated by the correlation of our data with the Vienna station record. The long-term 3H record helped to determine a locally contaminated sampling site, and new clean sites are put into operation. The 14C data were fitted by an analytical function and the prediction of future levels is given assuming that the rate of the 14C releases remains constant. From the long-term stable isotope data record, the local meteoric water line and the temperature gradient of δ18O in precipitation are determined.

Long-term environmental monitoring of 14C levels in the Ottawa region

Ambient levels of 14C have been monitored near Ottawa, Canada by the Radiocarbon Dating Laboratory, Geological Survey of Canada, since 1961. The 32 y of data on maple leaves documents the rapid increase of bomb-generated 14C in the mid-1960s and its exponential decline to the present. This bio-generated data set indicates that the half-life of bomb-generated 14C is 12 y as a result of dilution with prebomb 14C from the decay of organic matter and exchange with the oceanic reservoir, and, of course, a dilution from fossil fuel combustion. Atmospheric 14C activity will approach 10% of prebomb levels by the turn of the century, but it will be another century before the prebomb levels of atmospheric 14C are approached.

A possible paleoclimatic ENSO indicator in the spatial variation of annual tree‐ring 14C

Preliminary investigations show regional differences in atmospheric 14C activity archived in tree‐ring cellulose may reflect oceanic and atmospheric shifts associated with ENSO (El Niño‐Southern Oscillation) events. Much of the shared variation between sites in Washington and Arizona can be attributed to global forcings such as anthropogenic 14C‐depleted CO2 emissions and modulation of 14C production. The contrasted residual variation between the Washington and Arizona data sets correlates with the annual Southern Oscillation Index (SOI) of the previous year. The spatial differences between Δ14C data sets may provide a proxy indicator of ENSO phenomenon.

Experimental Determination of the 14C Initial Activity of Calcareous Deposits

We have reconstructed the initial activity of calcareous sediments by 1) measuring the 14C activity of recent pre-bomb-test calcareous deposits, 2) calculating the ratio of the 14C activity of the calcareous sediment to that of the adjacent coeval wood, and 3) extrapolating 14C activity of the deep lacustrine sediment layers to the surface, assuming a constant sedimentation rate. We show here that the uppermost sediment is affected by the global increase of atmospheric 14C activity due to thermonuclear bomb tests in the early 1960s. 14C activity of submerged aquatic plants showed values similar to 14C activity of DIC. Thus, organic residue of the sediment cannot be used for reliable 14C dating because of the unknown fraction of aquatic plant detritus. The initial activity, A0, obtained in a case study of the geochronology of carbonates in the Plitvice Lakes area, ranged from 70.5 to 72.2 pMC for Lake Prošće sediment, and from 75.9 to 76.7 pMC for Lake Kozjak sediment. These values also agree with calculated values based on the downstream increase of 14C activity of DIC in freshwater open to the atmosphere.

Modeling of Atmospheric Radiocarbon Fluctuations for the Past Three Centuries

Relatively precise quantitative observations of geophysical parameters are available to evaluate the fluctuations of atmospheric 14C activity during the past three centuries. As reviewed by Damon, Lerman, and Long (1978), these fluctuations seem to result from three factors: 1) changes in the earth's dipole magnetic field intensity, which has been decreasing since the first measurements by Gauss (McDonald and Gunst, 1968); 2) solar modulation of the cosmic-ray production, which has been correlated with the sunspot record of Waldmeier (1961), and more recently, to the Aa geomagnetic index by Stuiver and Quay (1980); and 3) the combustion of fossil fuels (Suess, 1955). A relationship between the climatic time series and the 14C-derived record of solar change has not yet been demonstrated (Stuiver, 1980).

Atmospheric Radiocarbon: Implications for the Geomagnetic Dipole Moment

The geomagnetic field is one of the major physical fields of the earth. Because its source is fluid motion in the outer core, it exhibits temporal changes, called secular variation, which are quite rapid compared to most geologic phenomena. The prehistoric secular variation is usually inferred from paleomagnetic data. We will discuss here how changes in the atmospheric 14C content can be used to gain additional insight into the behavior of the dipole moment over the past 8500 years. By rewriting the differential equations representing the 14C geochemical cycle in finite-difference form, we are able to convert the atmospheric 14C activity record into an equivalent radiocarbon dipole moment.

Tree Ring, Varve and Carbon-14 Chronologies

CARBON-14 dating has become of great importance and it is therefore necessary to determine the possible deviations between radiocarbon and actual ages. A radiocarbon age, given in radiocarbon years elapsed since the origin of the sample, is based on 14C decay and is calculated from the ratio of the present 14C activity of the sample to the 14C activity of the standard (95 per cent of the 14C activity of NBS oxalic acid). The standard 14C activity is assumed to be identical to the atmospheric 14C activity over the whole time interval over which 14C dating is used. Thus the conventional radiocarbon age does not allow for deviations in atmospheric 14C content during the past. As a result, radiocarbon years need not always be equal to solar years.