ALBERT

Description: Carbon–nitrogen (C–N) interactions regulate N availability for plant growth and for emissions of nitrous oxide (N2O) and the uptake of carbon dioxide. Future projections of these terrestrial greenhouse gas fluxes are strikingly divergent, leading to major uncertainties in projected global warming. Here we analyse the large increase in terrestrial N2O emissions over the past 21 000 years as reconstructed from ice-core isotopic data and presented in part 1 of this study. Remarkably, the increase occurred in two steps, each realized over decades and within a maximum of 2 centuries, at the onsets of the major deglacial Northern Hemisphere warming events. The data suggest a highly dynamic and responsive global N cycle. The increase may be explained by an increase in the flux of reactive N entering and leaving ecosystems or by an increase in N2O yield per unit N converted. We applied the LPX-Bern dynamic global vegetation model in deglacial simulations forced with Earth system model climate data to investigate N2O emission patterns, mechanisms, and C–N coupling. The N2O emission changes are mainly attributed to changes in temperature and precipitation and the loss of land due to sea-level rise. LPX-Bern simulates a deglacial increase in N2O emissions but underestimates the reconstructed increase by 47 %. Assuming time-independent N sources in the model to mimic progressive N limitation of plant growth results in a decrease in N2O emissions in contrast to the reconstruction. Our results appear consistent with suggestions of (a) biological controls on ecosystem N acquisition and (b) flexibility in the coupling of the C and N cycles during periods of rapid environmental change. A dominant uncertainty in the explanation of the reconstructed N2O emissions is the poorly known N2O yield per N lost through gaseous pathways and its sensitivity to soil conditions. The deglacial N2O record provides a constraint for future studies.

Description: We report results from a worldwide interlaboratory comparison of samples among laboratories that measure (or measured) stable carbon and hydrogen isotope ratios of atmospheric CH4 (δ13C-CH4 and δD-CH4). The offsets among the laboratories are larger than the measurement reproducibility of individual laboratories. To disentangle plausible measurement offsets, we evaluated and critically assessed a large number of intercomparison results, some of which have been documented previously in the literature. The results indicate significant offsets of δ13C-CH4 and δD-CH4 measurements among data sets reported from different laboratories; the differences among laboratories at modern atmospheric CH4 level spread over ranges of 0.5 ‰ for δ13C-CH4 and 13 ‰ for δD-CH4. The intercomparison results summarized in this study may be of help in future attempts to harmonize δ13C-CH4 and δD-CH4 data sets from different laboratories in order to jointly incorporate them into modelling studies. However, establishing a merged data set, which includes δ13C-CH4 and δD-CH4 data from multiple laboratories with desirable compatibility, is still challenging due to differences among laboratories in instrument settings, correction methods, traceability to reference materials and long-term data management. Further efforts are needed to identify causes of the interlaboratory measurement offsets and to decrease those to move towards the best use of available δ13C-CH4 and δD-CH4 data sets.

Description: Continuous records of the atmospheric greenhouse gases (GHGs) CO2, CH4, and N2O are necessary input data for transient climate simulations, and their associated radiative forcing represents important components in analyses of climate sensitivity and feedbacks. Since the available data from ice cores are discontinuous and partly ambiguous, a well-documented decision process during data compilation followed by some interpolating post-processing is necessary to obtain those desired time series. Here, we document our best possible data compilation of published ice core records and recent measurements on firn air and atmospheric samples spanning the interval from the penultimate glacial maximum ( ∼  156 kyr BP) to the beginning of the year 2016 CE. We use the most recent age scales for the ice core data and apply a smoothing spline method to translate the discrete and irregularly spaced data points into continuous time series. These splines are then used to compute the radiative forcing for each GHG using well-established, simple formulations. We compile only a Southern Hemisphere record of CH4 and discuss how much larger a Northern Hemisphere or global CH4 record might have been due to its interpolar difference. The uncertainties of the individual data points are considered in the spline procedure. Based on the given data resolution, time-dependent cutoff periods of the spline, defining the degree of smoothing, are prescribed, ranging from 5000 years for the less resolved older parts of the records to 4 years for the densely sampled recent years. The computed splines seamlessly describe the GHG evolution on orbital and millennial timescales for glacial and glacial–interglacial variations and on centennial and decadal timescales for anthropogenic times. Data connected with this paper, including raw data and final splines, are available at doi:10.1594/PANGAEA.871273.

Description: Continuous records of the atmospheric greenhouse gases (GHGs) CO2, CH4, and N2O are necessary input data for transient climate simulations and their related radiative forcing important components in analyses of climate sensitivity and feedbacks. Since the available data from ice cores are discontinuous and partly ambiguous a well-documented decision process during data compilation followed by some interpolating post-processing are necessary to obtain those desired time series. Here we document our best-guess data compilation of published ice core records and recent measurements on firn air and atmospheric samples covering the time window from the penultimate glacial maximum (∼ 156 kyr BP) to the beginning of year 2016 CE. A smoothing spline method is applied to translate the discrete and irregularly spaced data points into continuous time series. These splines are assumed to represent the evolution of the atmospheric mixing ratios for the three GHGs. Global- mean radiative forcing for each GHG is computed using well-established, simple formulations. Newest published age scales are used for the ice core data. While CO2 is representing an integrated global signal, we compile only a southern hemisphere record of CH4 and identify how much larger a northern hemisphere or global CH4 record might have been due to its interhemispheric gradient. Data resolution and uncertainties are considered in the spline procedure and typical cutoff periods, defining the degree of smoothing, range from 5000 years for the less resolved older parts of the records to 4 years for the densely-sampled recent years. The data sets describe seamlessly the GHG evolution on orbital and millennial time scales for glacial and glacial-interglacial variations and on centennial and decadal time scales for anthropogenic times. Data connected with this paper, including raw data and final splines, are available at https://doi.pangaea.de/10.1594/PANGAEA.871273.

Description: Using high-precision and centennial-resolution ice core information on atmospheric nitrous oxide concentrations and its stable nitrogen and oxygen isotopic composition, we quantitatively reconstruct changes in the terrestrial and marine N2O emissions over the last 21 000 years. Our reconstruction indicates that N2O emissions from land and ocean increased over the deglaciation largely in parallel by 1.7±0.3 and 0.7±0.3 TgN yr−1, respectively, relative to the Last Glacial Maximum level. However, during the abrupt Northern Hemisphere warmings at the onset of the Bølling–Allerød warming and the end of the Younger Dryas, terrestrial emissions respond more rapidly to the northward shift in the Intertropical Convergence Zone connected to the resumption of the Atlantic Meridional Overturning Circulation. About 90 % of these large step increases were realized within 2 centuries at maximum. In contrast, marine emissions start to slowly increase already many centuries before the rapid warmings, possibly connected to a re-equilibration of subsurface oxygen in response to previous changes. Marine emissions decreased, concomitantly with changes in atmospheric CO2 and δ13C(CO2), at the onset of the termination and remained minimal during the early phase of Heinrich Stadial 1. During the early Holocene a slow decline in marine N2O emission of 0.4 TgN yr−1 is reconstructed, which suggests an improvement of subsurface water ventilation in line with slowly increasing Atlantic overturning circulation. In the second half of the Holocene total emissions remain on a relatively constant level, but with significant millennial variability. The latter is still difficult to attribute to marine or terrestrial sources. Our N2O emission records provide important quantitative benchmarks for ocean and terrestrial nitrogen cycle models to study the influence of climate on nitrogen turnover on timescales from several decades to glacial–interglacial changes.

Description: Because the total air content (TAC) of polar ice is directly affected by the atmospheric pressure and temperature, its record in polar ice cores was initially considered as a proxy for past ice sheet elevation changes. However, the Antarctic ice core TAC record is known to also contain an insolation signature, although the underlying physical mechanisms are still a matter of debate. Here we present a high-resolution TAC record over the whole North Greenland Ice Core Project ice core, covering the last 120 000 years, which independently supports an insolation signature in Greenland. Wavelet analysis reveals a clear precession and obliquity signal similar to previous findings on Antarctic TAC, with a different insolation history. In our high-resolution record we also find a decrease of 4–6 % (4–5 mL kg−1) in TAC as a response to Dansgaard–Oeschger events (DO events). TAC starts to decrease in parallel to increasing Greenland surface temperature and slightly before CH4 reacts to the warming but also shows a two-step decline that lasts for several centuries into the warm interstadial. The TAC response is larger than expected considering only changes in air density by local temperature and atmospheric pressure as a driver, pointing to a transient firnification response caused by the accumulation-induced increase in the load on the firn at bubble close-off, while temperature changes deeper in the firn are still small.

Description: We report results from intercomparison exercises between laboratories that conduct measurements of stable carbon and hydrogen isotope ratios of atmospheric CH4 (δ13C-CH4 and δD-CH4). The offsets between the laboratories are larger than the measurement reproducibility of individual laboratories. To disentangle plausible offsets between worldwide laboratories, we evaluated and critically assessed a large number of intercomparison results documented previously in the literature. The results indicate significant offsets of δ13C-CH4 and δD-CH4 measurements among datasets reported from different laboratories; the data spread over ranges of 0.5 ‰ for δ13C-CH4 and 13 ‰ for δD-CH4. The intercomparison results summarized in this study may be of help when combining isotope datasets from different laboratories in future studies.

Description: Using high precision and centennial resolution ice core information on atmospheric nitrous oxide concentrations and its stable nitrogen and oxygen isotopic composition, we quantitatively reconstruct changes in the terrestrial and marine N2O emissions over the last 21,000 years. We show that N2O emissions from land and ocean increased largely in parallel by 1.7 ± 0.3 TgN yr−1 and 0.7 ± 0.3 TgN yr−1 over the deglaciation, respectively. However, during the abrupt Northern Hemisphere warmings at the onset of the Bølling/Allerød and the end of the Younger Dryas, terrestrial emissions respond more rapidly to the northward shift in the Intertropical Convergence Zone connected to the resumption of the Atlantic Meridional Overturning Circulation. 90 % of these large step increases were realized within maximum two centuries. In contrast, marine emissions start to slowly increase already many centuries before the rapid warmings, possibly connected to a re-equilibration of subsurface oxygen in response to previous changes. Marine emissions decreased, concomitantly with changes in atmospheric CO2 and δ13C(CO2), at the onset of the termination and remained minimal during the early phase of Heinrich Stadial 1. During the early Holocene a slow decline in marine N2O emission of 0.4 TgN yr−1 is reconstructed, suggesting an improvement of subsurface water ventilation in line with slowly increasing Atlantic overturning circulation. In the second half of the Holocene total emissions remain on a relatively constant level, however with significant millennial variability which is currently still difficult to attribute to marine or terrestrial sources. Our N2O emission records provide important quantitative benchmarks for ocean and terrestrial nitrogen cycle models to study the influence of climate on nitrogen turnover on time scales from several decades to glacial/interglacial changes.

Description: Atmospheric methane concentration shows a well-known decrease over the first half of the Holocene following the northern hemisphere summer insolation before it started to increase again to preindustrial values. There is a debate about what caused this change in the methane concentration trend, in particular, whether an early anthropogenic influence or natural emissions led to the reversal of the atmospheric CH4 concentration. Here, we present new methane concentration and stable hydrogen and carbon isotope data measured on ice core samples from both Greenland and Antarctica over the Holocene. With the help of a two-box model and the full suite of CH4 parameters, the new data allow us to quantify the total methane emissions in the northern and southern hemispheres separately as well as their isotopic signatures, while interpretation of isotopic records of only one hemisphere may lead to erroneous conclusions. For the first half of the Holocene our results indicate a decrease in northern and southern hemisphere CH4 emissions by more than 30 Tg CH4/yr in total accompanied by a drop in the northern carbon isotopic source signature of about −3 ‰. This cannot be explained by a change in the source mix alone, but requires shifts in the isotopic signature of the sources themselves caused by changes in the precursor material for the methane production. In the second half of the Holocene global CH4 emissions increased by about 30 Tg CH4/yr, while preindustrial isotopic emission signatures remained more a less constant. However, our results show that the increase of methane emissions starting in the mid-Holocene took place in the southern hemisphere, while northern hemisphere emissions started to increase only about 2000 years ago. Accordingly, natural emissions in the southern tropics appear to be the main cause of the CH4 increase starting 5000 years ago in contradiction to an early anthropogenic influence on the global methane budget by East Asian land use changes.

Description: Atmospheric methane concentration shows a well-known decrease over the first half of the Holocene following the Northern Hemisphere summer insolation before it started to increase again to preindustrial values. There is a debate about what caused this change in the methane concentration evolution, in particular, whether an early anthropogenic influence or natural emissions led to the reversal of the atmospheric CH4 concentration evolution. Here, we present new methane concentration and stable hydrogen and carbon isotope data measured on ice core samples from both Greenland and Antarctica over the Holocene. With the help of a two-box model and the full suite of CH4 parameters, the new data allow us to quantify the total methane emissions in the Northern Hemisphere and Southern Hemisphere separately as well as their stable isotopic signatures, while interpretation of isotopic records of only one hemisphere may lead to erroneous conclusions. For the first half of the Holocene our results indicate an asynchronous decrease in Northern Hemisphere and Southern Hemisphere CH4 emissions by more than 30 Tg CH4 yr−1 in total, accompanied by a drop in the northern carbon isotopic source signature of about −3 ‰. This cannot be explained by a change in the source mix alone but requires shifts in the isotopic signature of the sources themselves caused by changes in the precursor material for the methane production. In the second half of the Holocene, global CH4 emissions increased by about 30 Tg CH4 yr−1, while preindustrial isotopic emission signatures remained more or less constant. However, our results show that this early increase in methane emissions took place in the Southern Hemisphere, while Northern Hemisphere emissions started to increase only about 2000 years ago. Accordingly, natural emissions in the southern tropics appear to be the main cause of the CH4 increase starting 5000 years before present, not supporting an early anthropogenic influence on the global methane budget by East Asian land use changes.