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Systematic measurements of atmospheric methane (CH4) mole fractions at the northern high latitudes only began in the early 1980s. Although CH4 measurements from Greenland ice cores consistently covered the period before ∼ 1900, no reliable observational record is available for the intermediate period. We newly report a data set of trace gases from the air trapped in firn (an intermediate stage between snow and glacial ice formation) collected at the NGRIP (North Greenland Ice Core Project) site in 2001. We also use a set of published firn air data at the NEEM (North Greenland Eemian ice Drilling) site. The two Arctic firn air data sets are analysed with a firn air transport model, which translates historical variations to depth profiles of trace gases in firn. We examine a variety of possible firn diffusivity profiles, using a suite of measured trace gases, and reconstruct the CH4 mole fraction by an iterative dating method. Although the reconstructions of the Arctic CH4 mole fraction before the mid-1970s still has large uncertainties (> 30 ppb – parts per billion), we find a relatively narrow range of atmospheric CH4 history that is consistent with both depth profiles of NGRIP and NEEM. The atmospheric CH4 history inferred by this study is more consistent with the atmospheric CH4 scenario prepared for the NEEM firn modelling than that for the CMIP6 (Climate Model Intercomparison Project Phase 6) experiments. Our study shows that the atmospheric CH4 scenario used for the NEEM firn modelling is considered to be the current best choice for the Arctic CH4 history, but it should not be used to tune firn air transport models until being verified by further measurements from sources such as the Arctic ice cores. Given the current difficulty in reconstructing the CH4 history with low uncertainty from the firn air data sets from Greenland, future sampling and measurements of ice cores at a high-accumulation site may be the only way to accurately reconstruct the atmospheric CH4 trend over the 20th century.

The variations of δO2/N2 and δAr/N2 in the Dome Fuji ice core were measured from 112 m (bubbly ice) to 2001 m (clathrate hydrate ice). Our method, combined with the low storage temperature of the samples (−50 ∘C), successfully excludes post-coring gas-loss fractionation signals from our data. From the bubbly ice to the middle of the bubble–clathrate transition zone (BCTZ) (112–800 m) and below the BCTZ (>1200 m), the δO2/N2 and δAr/N2 data exhibit orbital-scale variations similar to local summer insolation. The data in the lower BCTZ (800–1200 m) have large scatter, which may be caused by millimeter-scale inhomogeneity of air composition combined with finite sample lengths. The insolation signal originally recorded at the bubble close-off remains through the BCTZ, and the insolation signal may be reconstructed by analyzing long ice samples (more than 50 cm for the Dome Fuji core). In the clathrate hydrate zone, the scatter around the orbital-scale variability decreases with depth, indicating diffusive smoothing of δO2/N2 and δAr/N2. A simple gas diffusion model was used to reproduce the smoothing and thus constrain their permeation coefficients. The relationship between δAr/N2 and δO2/N2 is markedly different for the datasets representing bubble close-off (slope ∼ 0.5), bubble–clathrate hydrate transformation (∼1), and post-coring gas loss (∼0.2), suggesting that the contributions of the mass-independent and mass-dependent fractionation processes are different for those cases. The method and data presented here may be useful for improving the orbital dating of deep ice cores over the multiple glacial cycles and further studying non-insolation-driven signals (e.g., atmospheric composition) of these gases.

The 13th Symposium on Polar Science/Ordinary sessions [OM] Polar meteorology and glaciology, Wed. 16 Nov.

Air in polar ice cores provides unique information on past climatic and atmospheric changes. We developed a new method combining wet extraction, gas chromatography and mass spectrometry for high-precision, simultaneous measurements of eight air components (CH4, N2O and CO2 concentrations; δ15N, δ18O, δO2∕N2 and δAr∕N2; and total air content) from an ice-core sample of ∼ 60 g. The ice sample is evacuated for ∼ 2 h and melted under vacuum, and the released air is continuously transferred into a sample tube at 10 K within 10 min. The air is homogenized in the sample tube overnight at room temperature and split into two aliquots for mass spectrometric and gas chromatographic measurements. Care is taken to minimize (1) contamination of greenhouse gases by using a long evacuation time, (2) consumption of oxygen during sample storage by a passivation treatment on sample tubes, and (3) fractionation of isotopic ratios with a long homogenization time for splitting. Precision is assessed by analyzing standard gases with artificial ice and duplicate measurements of the Dome Fuji and NEEM ice cores. The overall reproducibility (1 SD) of duplicate ice-core analyses are 3.2 ppb, 2.2 ppb and 2.9 ppm for CH4, N2O and CO2 concentrations; 0.006 ‰, 0.011 ‰, 0.09 ‰ and 0.12 ‰ for δ15N, δ18O, δO2∕N2 and δAr∕N2; and 0.63 mLSTP kg−1 for total air content, respectively. Our new method successfully combines the high-precision, small-sample and multiple-species measurements, with a wide range of applications for ice-core paleoenvironmental studies.

International audience; Precise ice-core chronologies are essential for identifying the timing and duration of polar climatic changes as well as their phasing with the changes in other parts of the globe. However, existing ice-core chronologies beyond the last 60 kyr show relatively large disagreements with each other and with U-Th chronologies of speleothems. Here, we constructed new ice and gas age scales for the Dome Fuji (DF) core (DF2021) over the last 207 kyr by combining a Bayesian dating model and firn densification model, constrained by various types of chronological and glaciological information including new δO2/N2 age markers, precise synchronization to other high-quality chronologies (volcanic, cosmogenic, and CH4 signals), and high-resolution δ15N of N2 (reflecting past firn thickness). The new chronology is tightly constrained by synchronization to other well-dated records for the last 60 kyr, whereas it is independent from other chronologies for the older period. For the last 60 kyr, the DF2021 chronology agrees with the layer-counted ice core chronologies (GICC05 and a part of WD2014) and U-Th chronologies of speleothems within ∼200 years. For the period 60-130 kyr BP, the timing of all Dansgaard-Oeschger warming events on DF2021 agree with those of corresponding events in the U-Th dated Chinese or European speleothems mostly within 1 kyr (well within 2σ uncertainty of DF2021). The excellent agreement suggests high accuracy of our chronology, and supports the assumption of negligible phasing between the past local summer solstice insolation and δO2/N2 fractionation at bubble close-off (the basis for constructing the δO2/N2 age markers). Between 130 and 207 kyr BP (penultimate glacial period), there is a lower degree of similarity between the variations in atmospheric CH4 and speleothem calcite δ18O than in the last glacial period, making the age comparison challenging. The comparison of DF2021 with 9 U-Th dates at 7 abrupt events shows the mean difference of -0.2 ± 0.8 kyr, which is within the DF2021 uncertainty (on the order of 1.5 kyr). The DF2021 chronology agrees with the AICC2012 chronology within 2 kyr except between ∼103 and 128 kyr BP where AICC2012 is likely too young by up to ∼4 kyr. By analyzing the lag between δ18O of O2 (δ18Oatm) on DF2021 and 65°N summer solstice insolation, the relatively large error in AICC2012 is found to originate in three δ18Oatm age markers assuming a constant lag, which are off by more than 3 kyr. The phasing between δ18Οatm and orbital forcing identified in this study may be useful for future ice core dating, especially where other age constraints are weak or lacking.

Systematic measurements of atmospheric methane (CH4) mole fractions at the northern high latitudes only began in the early 1980s, and whilst CH4 measurements from Greenland ice cores covered the period before ~1900, no reliable observational record is available for the intermediate period. In this study, we reconstruct the atmospheric CH4 for that period, when the mole fraction started to increase rapidly. We use a set of trace gas data measured from firn (an intermediate stage between snow and glacial ice formation) air samples collected at the NGRIP (North Greenland Ice Core Project) site in 2001, in combination with a firn air transport model whose performance is validated by using a set of published firn air data at the NEEM (North Greenland Eemian ice Drilling) site. We examine a variety of possible firn diffusivity profiles using a suite of measured trace gases, and reconstruct the CH4 mole fraction by an iterative dating method. We find that, given the currently available firn air data sets from Greenland, reliable reconstruction of the Arctic CH4 mole fraction is possible only back to the mid 1970s. For the earlier period, it is difficult to identify the atmospheric CH4 history that consistently reproduce the depth profiles of CH4 in firn at both NGRIP and NEEM sites. Therefore, the currently proposed Arctic CH4 history should still be considered preliminary and uncertain, and should not be treated as the known history for constraining firn-air transport models.

The variations of δO2/N2 and δAr/N2 in the Dome Fuji ice core were measured from 112 m (bubbly ice) to 2001 m (clathrate hydrate ice) at high precision. Our method, combined with the low storage temperature of the samples (−50 °C), successfully excludes post-coring gas-loss fractionation signals from our data. From the bubbly ice to the middle of the bubble-clathrate transition zone (BCTZ) (112–800 m) and below the BCTZ (> 1200 m), the δO2/N2 and δAr/N2 data exhibit orbital-scale variations similar to local summer insolation. The data in the lower BCTZ (800–1200 m) have large scatters, which may be caused by mm-scale inhomogeneity of air composition combined with finite sample lengths. The insolation signal originally recorded at the bubble close-off remains through the BCTZ, and the insolation signal may be reconstructed by analyzing long ice samples. In the clathrate hydrate zone, the scatters around the orbital-scale variability decrease with depth, indicating diffusive smoothing of δO2/N2 and δAr/N2. A simple gas diffusion model was used to reproduce the smoothing and thus constrain their permeation coefficients. The relationship between δAr/Ν2 and δO2/N2 is markedly different for the datasets representing bubble close-off (slope ~0.5), bubble-clathrate hydrate transformation (~1), and post-coring gas-loss (~0.2), suggesting that the contribution of the mass-independent and mass-dependent fractionation processes are different for those cases. The method and data presented here may be useful for improving the orbital dating of deep ice cores over the multiple glacial cycles and further studying non-insolation-driven signals (e.g., atmospheric composition) of these gases.

Antarctic paleotemperatures It has been widely thought that East Antarctica was ∼9°C cooler during the Last Glacial Maximum, close to the ∼10°C difference between then and now determined independently for West Antarctica. Buizert et al. used borehole thermometry, firn density reconstructions, and climate modeling to show that the temperature in East Antarctica was actually only ∼4° to 7°C cooler during the Last Glacial Maximum. This result has important consequences for our understanding of Antarctic climate, polar amplification, and global climate change. Science , abd2897, this issue p. 1097

The 11th Symposium on Polar Science/Interdisciplinary sessions: [IW] Whole atmosphere, Poster presentations, Mon. 16 Nov. - Fri. 18 Dec.

The 11th Symposium on Polar Science/Special session: [S] Accelerating Arctic research: Recent progress and future prospect of Arctic research, Poster presentations, Mon. 16 Nov. - Fri. 18 Dec.

Air in polar ice cores provides various information on past climatic and atmospheric changes. We developed a new method combining wet extraction, gas chromatography and mass spectrometry, for high-precision, simultaneous measurements of eight air components (CH4, N2O and CO2 concentrations, δ15N, δ18O, δO2/N2, δAr/N2 and total air content) from an ice core sample of ~60 g. The ice sample is evacuated for ~2 hours and melted under vacuum, and the released air is continuously transferred into a sample tube at 10 K within 10 minutes. The air is homogenized in the sample tube overnight at room temperature, and split into two aliquots for mass spectrometric and gas chromatographic measurements. Cares are taken to minimize contamination of greenhouse gases with long evacuation time, consumption of oxygen during sample storage by passivation treatment on sample tubes, and fractionation of isotopic ratios with long homogenization time for splitting. Precisions are assessed by analysing standard gases with artificial ice, and by duplicate measurements of the Dome Fuji and NEEM ice cores. The overall reproducibility (one standard deviation) from duplicate ice-core analyses are 3.2 ppb, 2.2 ppb and 3.1 ppm for CH4, N2O and CO2 concentrations, 0.006, 0.010, 0.09 and 0.12 ‰ for δ15N, δ18O, δO2/N2 and δAr/N2, and 0.67 mlSTP kg-1 for total air content, respectively. Our new method successfully combines the high-precision, small-sample and multiple-species measurements, with a wide range of applications for ice-core paleoenvironmental studies.

Accepted: 2018-04-09, 資料番号: SA1180010000

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.

An in situ measurement system was developed for continuous observations of the mole fractions of atmospheric oxygen (defined as δ(O2/N2)) and carbon dioxide (CO2) and the continuous observation was conducted onboard the research vessel SHIRASE 5003 during its voyage between Australia and Syowa Station, Antarctica, in 2017–2018. The CO2 variation was low with respect to that of δ(O2/N2) in the Southern Ocean, suggesting that the land biospheric and fossil-fuel derived CO2 and O2 emissions negligibly influenced the observations. Therefore, the observed significant variations in the atmospheric O2/N2 can be attributed to the atmosphere-ocean gas exchange. During the southbound voyage in December 2017, we observed large spatial variations in δ(O2/N2) due to marine biological production on the western side of the cruise track. Oceanic O2 fluxes based on a simple model and atmospheric δ(O2/N2) variability were consistent with past oceanic observations. No clear longitudinal gradient in δ(O2/N2) was observed at latitudes toward south of 60° S in December 2017 and February–March 2018. However, local δ(O2/N2) maxima were observed in regions with active marine biological production in December 2017. These observations indicate that local O2 fluxes can also modify the spatial distribution of atmospheric δ(O2/N2) in the Southern Ocean.

Systematic observations of CO2 mole fraction, the isotopic ratio δ13C of CO2 and oxygen to nitrogen ratio (δ(O2/N2)) in the atmosphere have been carried out at Ny-Alesund, Svalbard since 1991, 1996 and 2001, respectively. The CO2 mole fraction shows a clear seasonal cycle superimposed on a secular increase with an average rate of 2.0 ppm yr−1 for the period 1996–2013. On the other hand, δ13C and δ(O2/N2) decrease secularly at an average rate of −0.020 ‰ yr−1 for 1996–2013, and −19.9 per meg yr−1 for 2001–2013, respectively. Based on the observed secular trends of the CO2 mole fraction and δ(O2/N2), the average CO2 uptake during 2001–2013 was estimated to be 1.6 ± 0.8 and 2.3 ± 0.5 GtC yr−1 for the terrestrial biosphere and the ocean, respectively. By using the observed CO2 and δ13C, the corresponding CO2 uptake of 1.3 ± 0.6 and 2.6 ± 0.5 GtC yr−1 were obtained for the same period. The estimates from the two methods are in good agreement with each other. The terrestrial biospheric CO2 uptake derived by the latter method showed large inter-annual variability in association with El Nino events. On the other hand, the oceanic uptake increased secularly with less inter-annual variability during 1996–2013.

The Total Carbon Column Observing Network (TCCON) is a network of ground-based Fourier transform spectrometers (FTSs) that record near-infrared (NIR) spectra of the sun. From these spectra, accurate and precise observations of CO2 column-averaged dry-air mole fractions (denoted XCO2) are retrieved. TCCON FTS observations have previously been used to validate satellite estimations of XCO2; however, our knowledge of the short-term spatial and temporal variations in XCO2 surrounding the TCCON sites is limited. In this work, we use the National Institute for Environmental Studies (NIES) Eulerian three-dimensional transport model and the FLEXPART (FLEXible PARTicle dispersion model) Lagrangian particle dispersion model (LPDM) to determine the footprints of short-term variations in XCO2 observed by operational, past, future and possible TCCON sites. We propose a footprint-based method for the collocation of satellite and TCCON XCO2 observations and estimate the performance of the method using the NIES model and five GOSAT (Greenhouse Gases Observing Satellite) XCO2 product data sets. Comparison of the proposed approach with a standard geographic method shows a higher number of collocation points and an average bias reduction up to 0.15 ppm for a subset of 16 stations for the period from January 2010 to January 2014. Case studies of the Darwin and Reunion Island sites reveal that when the footprint area is rather curved, non-uniform and significantly different from a geographical rectangular area, the differences between these approaches are more noticeable. This emphasises that the collocation is sensitive to local meteorological conditions and flux distributions.

The Tenth Symposium on Polar Science/Ordinary sessions: [OM] Polar Meteorology and Glaciology, Wed. 4 Dec. / Entrance Hall (1st floor) , National Institute of Polar Research

The Ninth Symposium on Polar Science/Ordinary sessions: [OM] Polar meteorology and glaciology, Wed. 5 Dec. / Entrance Hall (1st floor), National Institute of Polar Research

To investigate the seasonal characteristics of chemical tracer distributions in the extratropical upper troposphere and lower stratosphere (ExUTLS) as well as stratosphere–troposphere exchange processes, mixing fractions of air masses originating in the stratosphere, tropical troposphere, mid-latitude lower troposphere (LT), and high-latitude LT in the ExUTLS are estimated using 90-day backward trajectories calculated with European Centre For Medium-Range Weather Forecasts (ECMWF) ERA-Interim data as the meteorological input. Time-series of chemical tracers obtained from ground-based and airborne observations are incorporated into the estimated mixing fractions, thus reconstructing spatiotemporal distributions of chemical tracers in the ExUTLS. The reconstructed tracer distributions are analysed with the mixing fractions and the stratospheric age of air (AoA) estimated using a 10-year backward trajectory. The reconstructed distributions of CO and CO2 in the ExUTLS are affected primarily by tropospheric air masses because of the short chemical lifetime of the former and large seasonal variations in the troposphere of the latter. Distributions of CH4, N2O, and SF6 are controlled primarily by seasonally varying air masses transported from the stratosphere. For CH4 and N2O distributions, air masses transported via the deep branch of the Brewer–Dobson circulation are particularly important. This interpretation is qualitatively and quantitatively supported by the estimated spatiotemporal distributions of AoA.

著者人数: 13名, Accepted: 2018-09-04, 資料番号: SA1180168000

The seasonal variations of greenhouse gases at about 11 km altitude were analyzed from monthly air samples collected aboard a commercial airliner flying between Europe and Japan from April 2012 to March 2014. Compared to lower latitudes, the upper troposphere between 50 and 70°N showed higher CH4 and SF6 and an earlier seasonal phase of CO2. However, N2O values were similar to those in the subtropics. CH4, N2O, and SF6 in the lower stratosphere with potential temperature of up to 50 K above the tropopause showed seasonal variations with maxima in November/December and minima in April/May. At potential temperatures of 37.5–50 K above the tropopause, SF6 age was estimated to be about 22 months in May and 9 months in November. This strong seasonal variation is explained by the subsidence of high-stratospheric air in spring and the effective flushing of the lowermost stratospheric air with tropospheric air in autumn.

Atmospheric methane (CH4) increased from ~900 ppb (parts per billion, or nanomoles per mole of dry air) in 1900 to ~1800 ppb in 2010 at a rate unprecedented in any observational records. However, the contributions of the various methane sources and sinks to the CH4 increase are poorly understood. Here we use initial emissions from bottom-up inventories for anthropogenic sources, emissions from wetlands and rice paddies simulated by a~terrestrial biogeochemical model, and an atmospheric general circulation model (AGCM)-based chemistry-transport model (i.e. ACTM) to simulate atmospheric CH4 concentrations for 1910–2010. The ACTM simulations are compared with the CH4 concentration records reconstructed from Antarctic and Arctic ice cores and firn air samples, and from direct measurements since the 1980s at multiple sites around the globe. The differences between ACTM simulations and observed CH4 concentrations are minimized to optimize the global total emissions using a mass balance calculation. During 1910–2010, the global total CH4 emission doubled from ~290 to ~580 Tg yr−1. Compared to optimized emission, the bottom-up emission data set underestimates the rate of change of global total CH4 emissions by ~30% during the high growth period of 1940–1990, while it overestimates by ~380% during the low growth period of 1990–2010. Further, using the CH4 stable carbon isotopic data (δ13C), we attribute the emission increase during 1940–1990 primarily to enhancement of biomass burning. The total lifetime of CH4 shortened from 9.4 yr during 1910–1919 to 9 yr during 2000–2009 by the combined effect of the increasing abundance of atomic chlorine radicals (Cl) and increases in average air temperature. We show that changes of CH4 loss rate due to increased tropospheric air temperature and CH4 loss due to Cl in the stratosphere are important sources of uncertainty to more accurately estimate the global CH4 budget from δ13C observations.

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.

Stratospheric air samples were collected over Biak, Indonesia in February 2015 using four large plastic balloons, each loaded with two compact cryogenic samplers. With a vertical resolution of better than 2 km, air samples from seven different altitudes were analyzed for CO2 and SF6 mole fractions, δ15N of N2, δ18O of O2, and δ(Ar/N2), to examine vertically dependent age and gravitational separation of air in the Tropical Tropopause Layer (TTL) and the equatorial stratosphere. By comparing their measured mole fractions with aircraft observation in the upper tropical troposphere, we have found that CO2 and SF6 age increases gradually with increasing altitude from the TTL to 22 km, and then rapidly from there up to 25 km. The CO2 and SF6 age agrees well with each other in the TTL and in the lower stratosphere, but shows a significant difference above 24 km. The average values of δ15N of N2, δ18O of O2, and δ(Ar/N2) all show small but distinct upward decrease due to the gravitational separation effect. Simulations with a two-dimensional atmospheric transport model indicate that the gravitational separation effect decreases as tropical upwelling is enhanced. From the model calculations with enhanced eddy mixing, it is also found that the upward increase in air age is magnified by horizontal mixing. These model simulations also show that the gravitational separation effect remains relatively constant in the lower stratosphere. The results of this study strongly suggest that the gravitational separation, combined with the age of air, can be used to diagnose air transport processes in the stratosphere.

Oxygen in the atmosphere undergoes variations and changes in response to biospheric activities, ocean–atmosphere exchange and fossil fuel combustion. Continuous in situ measurements of atmospheric δ(O2/N2) and CO2 mole fraction were started at Ny-Ålesund, Svalbard (78.93°N, 11.83°E, 40 m a.s.l.) in November 2012. Atmospheric potential oxygen (APO) calculated from the measured O2 and CO2 values during November 2012–January 2015 show a clear seasonal cycle with a peak-to-peak amplitude of approximately 50 per meg. The seasonal cycle of APO simulated using an atmospheric transport model, with prescribed oceanic O2, N2 and CO2 fluxes at monthly time intervals, is in excellent agreement with the observed APO. However, in spring and early summer, high values of APO are observed irregularly on a timescale of hours to days. By comparing backward trajectories of air parcels released from the site with distributions of marine net primary production (NPP), and tagged tracer experiments made using the atmospheric transport model for APO, it is found that these high APO fluctuations are primarily attributable to O2 emissions from the Greenland Sea, the Norwegian Sea and the Barents Sea, due to marine biological productivity. Marine net community production, estimated based on the sea-to-air O2 flux derived from observed APO fluctuations, agrees with NPP obtained from satellite observations within an order of magnitude. The results obtained in this study have still some uncertainties, but our continuous observations of atmospheric δ(O2/N2) and CO2 mole fraction at Ny-Ålesund can play an important role in detecting possible changes in the carbon cycle in the near future.

We have conducted systematic observations of the CH4 mole fraction and its carbon isotope ratio (δ13C) at Ny-Ålesund, Svalbard (78°55′N, 11°56′E) using air samples collected weekly since 1991 and 1996, respectively. The CH4 mole fraction showed long-term increase until 1999, stagnation between 2000 and 2006, followed by an increase after 2006. On the other hand, δ13C showed monotonous increase until 2006 and decrease after 2006. By comparing the rates of change in the CH4 mole fraction and δ13C under the assumption that the atmospheric CH4 lifetime is constant, it is suggested that the temporal pause of the CH4 mole fraction observed at Ny-Ålesund is attributed to reductions of CH4 release from the microbial and fossil fuel sectors. On the other hand, the increase in CH4 after 2006 could be ascribed to an increase in microbial CH4 release. The CH4 and δ13C data presented in this paper would be useful for clarifying their temporal variations in the Arctic atmosphere, as well as providing additional constraints on the global CH4 budget.

In this study we reexamine nearly four decades of in situ balloon-based stratospheric observations of SF6 and CO2 with an idealized model and reanalysis products. We use new techniques to account for the spatial and temporal inhomogeneity of the sparse balloon profiles and to calculate stratospheric mean ages of air more consistently from the observations with the idealized model. By doing so we are able to more clearly show and account for the variability of mean age of air throughout the bulk of the depth of the stratosphere. From an idealized model guided by the observations, we identify variability in the mean age due to the seasonal cycle of stratospheric transport, the quasi-biennial oscillation in tropical zonal winds, major volcanic eruptions, and linear trends that vary significantly with altitude. We calculate a negative mean age trend in the lowest 5 km of the stratosphere that agrees within uncertainties with a trend calculated from a set of chemistry climate model mean ages in this layer. The mean age trends reverse sign in the middle and upper stratosphere and are in agreement with a previous positive trend estimate using the same observational data set, although we have substantially reduced the uncertainty on the trend. Our analysis shows that a long time series of in situ profile measurements of trace gases such as SF6 and CO2 can be a unique and useful indicator of stratospheric circulation variability on a range of time scales and an important contributor to help validate the stratospheric portion of global chemistry climate models. However, with only SF6 and CO2 measurements, the competing effects on mean age between mean circulation and mixing (tropical entrainment) are not uniquely separable.

著者人数: 12名, 資料番号: SA1140112000

We present a comprehensive estimate of nitrous oxide (N2O) emissions using observations and models from 1995 to 2008. High-frequency records of tropospheric N2O are available from measurements at Cape Grim, Tasmania; Cape Matatula, American Samoa; Ragged Point, Barbados; Mace Head, Ireland; and at Trinidad Head, California using the Advanced Global Atmospheric Gases Experiment (AGAGE) instrumentation and calibrations. The Global Monitoring Division of the National Oceanic and Atmospheric Administration/Earth System Research Laboratory (NOAA/ESRL) has also collected discrete air samples in flasks and in situ measurements from remote sites across the globe and analyzed them for a suite of species including N2O. In addition to these major networks, we include in situ and aircraft measurements from the National Institute of Environmental Studies (NIES) and flask measurements from the Tohoku University and Commonwealth Scientific and Industrial Research Organization (CSIRO) networks. All measurements show increasing atmospheric mole fractions of N2O, with a varying growth rate of 0.1–0.7% per year, resulting in a 7.4% increase in the background atmospheric mole fraction between 1979 and 2011. Using existing emission inventories as well as bottom-up process modeling results, we first create globally gridded a priori N2O emissions over the 37 years since 1975. We then use the three-dimensional chemical transport model, Model for Ozone and Related Chemical Tracers version 4 (MOZART v4), and a Bayesian inverse method to estimate global as well as regional annual emissions for five source sectors from 13 regions in the world. This is the first time that all of these measurements from multiple networks have been combined to determine emissions. Our inversion indicates that global and regional N2O emissions have an increasing trend between 1995 and 2008. Despite large uncertainties, a significant increase is seen from the Asian agricultural sector in recent years, most likely due to an increase in the use of nitrogenous fertilizers, as has been suggested by previous studies.