Search

A study was conducted to compare the δ(O2/N2) scales used by four laboratories engaged in atmospheric δ(O2/N2) measurements. These laboratories are the Research Institute for Environmental Management Technology, Advanced Industrial Science and Technology (EMRI/AIST); the National Institute for Environmental Studies (NIES); Tohoku University (TU); and Scripps Institution of Oceanography (SIO). Therefore, five high-precision standard mixtures for the O2 molar fraction gravimetrically prepared by the National Metrology Institute of Japan, AIST (NMIJ/AIST) with a standard uncertainty of less than 5 per meg (0.001 ‰) were used as round-robin standard mixtures. EMRI/AIST, NIES, TU, and SIO reported the analyzed values of the standard mixtures on their own δ(O2/N2) scales, and the values were compared with the δ(O2/N2) values gravimetrically determined by NMIJ/AIST (the NMIJ/AIST scale). The δ(O2/N2) temporal drift in the five standard mixtures during the intercomparison experiment from May 2017 to March 2020 was corrected based on the δ(O2/N2) values analyzed before and after the laboratory measurements by EMRI/AIST. The scales are compared based on offsets in zero and span. The relative span offsets of EMRI/AIST, TU, NIES, and SIO scales against the NMIJ/AIST scale were -0.11%±0.10%, -0.10%±0.13%, 3.39 %±0.13 %, and 0.93 %±0.10 %, respectively. The largest offset corresponded to a 0.30 Pg yr−1 decrease and increase in global estimates for land biospheric and oceanic CO2 uptakes based on trends in atmospheric CO2 and δ(O2/N2). The deviations in the measured δ(O2/N2) values on the laboratory scales from the NMIJ/AIST scale are 65.8±2.2, 425.7±3.1, 404.5±3.0, and 596.4±2.4 per meg for EMRI/AIST, TU, NIES, and SIO, respectively. The difference between atmospheric δ(O2/N2) values observed at Hateruma Island (HAT; 24.05∘ N, 123.81∘ E), Japan, by EMRI/AIST and NIES were reduced from -329.3±6.9 to -6.6±6.8 per meg by converting their scales to the NMIJ/AIST scale.

The island of Hateruma is the southernmost inhabited island of Japan. Here we interpret observations of carbon monoxide (CO), ethane (C2H6), propane (C3H8), nitrogen oxides (NOx and NOy) and ozone (O3) made from the island in 2018 with the GEOS-Chem atmospheric chemistry transport model. We simulated the concentrations of these species within a nested grid centered over the site, with a model resolution of 0.5°×0.625°. We use the Community Emissions Data System (CEDS) emissions dataset for anthropogenic emissions and add a geological source of C2H6 and C3H8. The model captured the seasonality of primary pollutants (CO, C2H6, C3H8) at the site - high concentrations in the winter months when oxidation rates are low and flow is from the north, and low concentrations in the summer months when oxidation rates are higher and flow is from the south. It also simulates many of the synoptic scale events with Pearson’s correlation coefficients (r) of 0.74, 0.88 and 0.89 for CO, C2H6 and C3H8, respectively. Concentrations of CO are well simulated by the model (with a gradient of best fit between model and measurements of 0.91) but simulated concentrations of C2H6 and C3H8 are significantly lower than the observations (gradients of best fit between model and measurement of 0.57 and 0.41, respectively), most noticeably in the winter months. Simulated NOx concentrations were underestimated but NOy appear to be overestimated. The concentration of O3 is moderately well simulated (gradient of best fit line of 0.76, with an r of 0.87) but there is a tendency to underestimate concentrations in the winter months. By switching off the model’s biomass burning emissions we show that during winter biomass burning has limited influence on the concentration of compounds in the winter but can represent a sizeable fraction in the summer. We also show that increasing the anthropogenic emissions of C2H6 and C3H8 in Asia by factors of 2.22 and 3.17, respectively, significantly increases the model’s ability to simulate these species in the winter months, consistent with previous studies.

We developed a near-real-time estimation method for temporal changes in fossil fuel CO2 (FFCO2) emissions from China for three months (January, February, March, (JFM)) based on atmospheric CO2 and CH4 observations on Hateruma Island (HAT, 24.06°N, 123.81°E) and Yonaguni Island (YON, 24.47°N, 123.01°E), Japan. These two remote islands are in the downwind region of continental East Asia during winter because of the East Asian monsoon. Previous studies have revealed that monthly averages of synoptic-scale variability ratios of atmospheric CO2 and CH4 (ΔCO2/ΔCH4) observed at HAT and YON in JFM are sensitive to changes in continental emissions. From the analysis based on an atmospheric transport model with all components of CO2 and CH4 fluxes, we found that the ΔCO2/ΔCH4 ratio was linearly related to the FFCO2/CH4 emission ratio in China because calculating the variability ratio canceled out the transport influences. Using the simulated linear relationship, we converted the observed ΔCO2/ΔCH4 ratios into FFCO2/CH4 emission ratios in China. The change rates of the emission ratios were calculated relative to those for the preceding 9-year period (2011–2019), during which relatively stable ΔCO2/ΔCH4 ratios were observed. These changes in the emission ratios can be read as FFCO2 emission changes under the assumption of no interannual variations in CH4 emissions and biospheric CO2 fluxes for JFM. The resulting average changes in the FFCO2 emissions in January, February, and March 2020 were 17 ± 8%, − 36 ± 7%, and − 12 ± 8%, respectively, (− 10 ± 9% for JFM overall) relative to 2011–2019. These results were generally consistent with previous estimates. The emission changes for the two most recent JFM were 18 ± 8%, − 2 ± 10%, 29 ± 12%, respectively, in 2021 (15 ± 10% for JFM overall) and 20 ± 9%, − 3 ± 10%, − 10 ± 9%, respectively, in 2022 (2 ± 9% for JFM overall). These results suggest that the FFCO2 emissions from China rebounded to the normal level or set a new high in early 2021 after the COVID-19 lockdown. In addition, the estimated reduction in March 2022 might be attributed to the influence of a new wave of COVID-19 infections in Shanghai.

Systematic measurements of the atmospheric Ar∕N2 ratio have been made at ground-based stations in Japan and Antarctica since 2012. Clear seasonal cycles of the Ar∕N2 ratio with summertime maxima were found at middle- to high-latitude stations, with seasonal amplitudes increasing with increasing latitude. Eight years of the observed Ar∕N2 ratio at Tsukuba (TKB) and Hateruma (HAT), Japan, showed interannual variations in phase with the observed variations in the global ocean heat content (OHC). We calculated secularly increasing trends of 0.75 ± 0.30 and 0.89 ± 0.60 per meg per year from the Ar∕N2 ratio observed at TKB and HAT, respectively, although these trend values are influenced by large interannual variations. In order to examine the possibility of the secular trend in the surface Ar∕N2 ratio being modified significantly by the gravitational separation in the stratosphere, two-dimensional model simulations were carried out by arbitrarily modifying the mass stream function in the model to simulate either a weakening or an enhancement of the Brewer–Dobson circulation (BDC). The secular trend of the Ar∕N2 ratio at TKB, corrected for gravitational separation under the assumption of weakening (enhancement) of BDC simulated by the 2-D model, was 0.60 ± 0.30 (0.88 ± 0.30) per meg per year. By using a conversion factor of 3.5 × 10−23 per meg per joule by assuming a one-box ocean with a temperature of 3.5 ∘C, average OHC increase rates of 17.1 ± 8.6 ZJ yr−1 and 25.1 ± 8.6 ZJ yr−1 for the period 2012–2019 were estimated from the corrected secular trends of the Ar∕N2 ratio for the weakened- and enhanced-BDC conditions, respectively. Both OHC increase rates from the uncorrected- and weakened-BDC secular trends of the Ar∕N2 ratio are consistent with 12.2 ± 1.2 ZJ yr−1 reported by ocean temperature measurements, while that from the enhanced-BDC is outside of the range of the uncertainties. Although the effect of the actual atmospheric circulation on the Ar∕N2 ratio is still unclear and longer-term observations are needed to reduce uncertainty of the secular trend of the surface Ar∕N2 ratio, the analytical results obtained in the present study imply that the surface Ar∕N2 ratio is an important tracer for detecting spatiotemporally integrated changes in OHC and BDC.

We conducted ship-based measurements of marine aerosol particles (number concentration, size distribution, black carbon (BC), autofluorescence property, and PM

The regional budget of methane (CH4) emissions for East Asia, a crucial region in the global greenhouse gas budget, was quantified for 1990–2015 with a bottom-up method based on inventories and emission model simulations. Anthropogenic emissions associated with fossil fuel extraction, industrial activities, waste management, and agricultural activities were derived from the Emission Database for Global Atmospheric Research version 4.3.2 and compared with other inventories. Emissions from natural wetlands and CH4 uptake by upland soil oxidation were estimated using the Vegetation Integrative SImulator for Trace gases (VISIT), a biogeochemical model that considers historical land use and climatic conditions. Emissions from biomass burning and termites were calculated using satellite and land-use data combined with empirical emission factors. The resulting average annual estimated CH4 budget for 2000–2012 indicated that East Asia was a net source of 67.3 Tg CH4 yr−1, of which 88.8% was associated with anthropogenic emissions. The uncertainty (±standard deviation) of this estimate, ±14 Tg CH4 yr−1, stemmed from data and model inconsistencies. The increase of the net flux from 60.2 Tg CH4 yr−1 in 1990 to 78.0 Tg CH4 yr−1 in 2012 was due mainly to increased emissions by the fossil fuel extraction and livestock sectors. Our results showed that CH4 was a crucial component of the regional greenhouse gas budget. A spatial analysis using 0.25° × 0.25° grid cells revealed emission hotspots in urban areas, agricultural areas, and wetlands. These hotspots were surrounded by weak sinks in upland areas. The estimated natural and anthropogenic emissions fell within the range of independent estimates, including top-down estimates from atmospheric inversion models. Such a regional accounting is an effective way to elucidate climatic forcings and to develop mitigation policies. Further studies, however, are required to reduce the uncertainties in the budget.

Time series of the atmospheric O2∕N2 ratio and CO2 mole fraction of flask samples obtained from the National Institute for Environmental Studies' (NIES's) flask sampling network are presented. The network includes two ground sites, Hateruma island (HAT; 24.05 ∘ N, 123.81 ∘ E) and Cape Ochiishi (COI; 43.17 ∘ N, 145.50 ∘ E), and cargo ships regularly sailing in the western Pacific. Based on temporal changes in fossil-fuel-derived CO2 emissions, global atmospheric CO2 burden and atmospheric potential oxygen (APO), which were calculated from the observed O2∕N2 ratio and CO2 mole fraction according to APO = O2 + 1.1 × CO 2 , we estimated the global carbon sinks of the ocean and land biosphere for a period of more than 15 years. In this carbon budget calculation, we adopted a correction for the time-varying ocean O2 outgassing effect with an average of 0.54 PgC yr −1 for 2000–2016. The outgassing effect, attributed mainly to global ocean warming, was evaluated under the assumption that the net ocean gas flux is proportional to the change in the ocean heat content for the 0–2000 m layer. The resulting oceanic and land biotic carbon sinks were 2.6±0.7 and 1.5±0.9 PgC yr −1 , respectively, for a 17-year period (2000–2016) and 2.4±0.7 and 1.9±0.9 PgC yr −1 , respectively, for a 14-year period (2003–2016). Despite the independent approaches, the sink values of this study agreed with those estimated by the Global Carbon Project (GCP) within a difference of about ±0.4 PgC yr −1 . We examined the carbon sinks for an interval of 5 years to assess the temporal trends. The pentad (5-year) ocean sinks showed an increasing trend at a rate of 0.08±0.02 PgC yr −2 during 2001–2014, while the pentad land sinks showed an increasing trend at a rate of 0.23±0.04 PgC yr −2 for 2001–2009 and a decreasing trend at a rate of - 0.22 ± 0.04 PgC yr −2 during 2009–2014. Although there is good agreement in the trends of the pentad sinks between this study and that of GCP, the increasing rate of the pentad ocean sinks of this study was about 2 times larger than that of GCP.

In Asia, much effort is put into reducing methane (CH4) emissions due to the region’s contribution to the recent rapid global atmospheric CH4 concentration growth. Accurate quantification of Asia’s CH4 budgets is critical for conducting global stocktake and achieving the long-term temperature goal of the Paris Agreement. In this study, we present top-down estimates of CH4 emissions from 2009 to 2018 deduced from atmospheric observations from surface network and GOSAT satellite with the high-resolution global inverse model NIES-TM-FLEXPART-VAR. The optimized average CH4 budgets are 63.40 ± 10.52 Tg y−1 from East Asia (EA), 45.20 ± 6.22 Tg y−1 from Southeast Asia (SEA), and 64.35 ± 9.28 Tg y−1 from South Asia (SA) within the 10 years. We analyzed two 5 years CH4 emission budgets for three subregions and 13 top-emitting countries with an emission budget larger than 1 Tg y−1, and interannual variabilities for these subregions. Statistically significant increasing trends in emissions are found in EA with a lower emission growth rate during 2014–2018 compared to that during 2009–2013, while trends in SEA are not significant. In contrast to the prior emission, the posterior emission shows a significant decreasing trend in SA. The flux decrease is associated with the transition from strong La Ninña (2010–2011) to strong El Ninño (2015–2016) events, which modulate the surface air temperature and rainfall patterns. The interannual variability in CH4 flux anomalies was larger in SA compared to EA and SEA. The Southern Oscillation Index correlates strongly with interannual CH4 flux anomalies for SA. Our findings suggest that the interannual variability in the total CH4 flux is dominated by climate variability in SA. The contribution of climate variability driving interannual variability in natural and anthropogenic CH4 emissions should be further quantified, especially for tropical countries. Accounting for climate variability may be necessary to improve anthropogenic emission inventories.

A study was conducted to compare the δ(O2/N2) scales used by four laboratories engaged in atmospheric δ(O2/N2) measurements. These laboratories are the Research Institute for Environmental Management Technology, Advanced Industrial Science and Technology (EMRI/AIST), the National Institute for Environmental Studies (NIES), Tohoku University (TU), and Scripps Institution of Oceanography (SIO). Therefore, five high-precision standard mixtures for O2 molar fraction gravimetrically prepared by the National Metrology Institute of Japan (NMIJ), AIST (NMIJ/AIST) with a standard uncertainty of less than 5 per meg were used as round-robin standard mixtures. EMRI/AIST, NIES, TU, and SIO reported the analysed values of the standard mixtures on their own δ(O2/N2) scales, and the values were compared with the δ(O2/N2) values gravimetrically determined by NMIJ/AIST (the NMIJ/AIST scale). The δ(O2/N2) temporal drift in the five standard mixtures during the inter-comparison experiment was corrected based on the δ(O2/N2) values analysed before and after the experiments by EMRI/AIST. The scales are compared based on offsets in zero and span. The span offsets from the NMIJ/AIST scale ranged from −0.17 % to 3.3 %, corresponding with the difference of 0.29 Pg yr−1 in the estimates for land biospheric and oceanic CO2 uptakes. The zero offsets from the NMIJ/AIST scale are −581.0 ± 2.2, −221.4 ± 3.1, −243.0 ± 3.0, and −50.7 ± 2.4 per meg for EMRI/AIST, TU, NIES, and SIO, respectively. The atmospheric δ(O2/N2) values observed at Hateruma Island (HAT; 24.05° N, 123.81° E), Japan, by EMRI/AIST and NIES became comparable by converting their scales to the NMIJ/AIST scale.

The inverse analysis was used to estimate the fire carbon emission in Equatorial Asia induced by the big El Niño in 2015. This inverse analysis is unique because it extensively used high-precision atmospheric mole fraction data of carbon dioxide (CO2) from the commercial aircraft observation project. By comparisons with independent shipboard observations, especially carbon monoxide (CO) data, the validity of the estimated fire-induced carbon emission was elucidated. The best estimate, which used both aircraft and shipboard CO2 observations, indicated 273 Tg C for fire emission during September–October 2015. This two-month-long emission accounts for 75 % of the annual total fire emission and 45 % of the annual total net carbon flux within the region, indicating that fire emission is a dominant driving force of interannual variations of carbon fluxes in Equatorial Asia. Several sensitivity experiments demonstrated that aircraft observations could measure fire signals, though they showed a certain degree of sensitivity to prior fire-emission data. The inversions coherently estimated smaller fire emissions than the priors, partially because of the small contribution of peatland fires, indicated by enhancement ratios of CO and CO2 observed by the ship. In the future warmer climate condition, Equatorial Asia would experience more severe droughts and have risks for releasing a large amount of carbon into the atmosphere. Therefore, the continuation of aircraft and shipboard observations is fruitful for reliable monitoring of carbon fluxes in Equatorial Asia.

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.

Carbonaceous aerosol particles emitted from biomass burning (BB) have a large impact on the global climate. In particular, tarball particles (TBs), which are spherical organic aerosol particles, account for a large proportion of aerosol particles from BB. In this study, we collected aerosol particles over the western North Pacific and analyzed them using transmission electron microscopy with energy-dispersive X-ray spectroscopy (TEM-EDX) to reveal their shape and composition. We detected TBs and organic carbon particles originating from Siberian forest fires. To the best of our knowledge, this is the first case in which a large number of TBs have been found over the Pacific Ocean far from the BB source. The spherical shapes of the TBs were maintained even after long-range transport. In addition, our individual analysis of TBs showed that the size and composition of TBs differ depending on the air mass origin. The occurrence and microphysical properties of TBs are important to accurately evaluate the impact of TBs on climate. Our results imply that TBs can be transported to the Arctic and have an influence on radiative forcing over the ocean and in the Arctic.

The COVID-19 pandemic caused drastic reductions in carbon dioxide (CO2) emissions, but due to its large atmospheric reservoir and long lifetime, no detectable signal has been observed in the atmospheric CO2 growth rate. Using the variabilities in CO2 (ΔCO2) and methane (ΔCH4) observed at Hateruma Island, Japan during 1997–2020, we show a traceable CO2 emission reduction in China during February–March 2020. The monitoring station at Hateruma Island observes the outflow of Chinese emissions during winter and spring. A systematic increase in the ΔCO2/ΔCH4 ratio, governed by synoptic wind variability, well corroborated the increase in China’s fossil-fuel CO2 (FFCO2) emissions during 1997–2019. However, the ΔCO2/ΔCH4 ratios showed significant decreases of 29 ± 11 and 16 ± 11 mol mol−1 in February and March 2020, respectively, relative to the 2011–2019 average of 131 ± 11 mol mol−1. By projecting these observed ΔCO2/ΔCH4 ratios on transport model simulations, we estimated reductions of 32 ± 12% and 19 ± 15% in the FFCO2 emissions in China for February and March 2020, respectively, compared to the expected emissions. Our data are consistent with the abrupt decrease in the economic activity in February, a slight recovery in March, and return to normal in April, which was calculated based on the COVID-19 lockdowns and mobility restriction datasets.

The COVID-19 pandemic caused drastic reductions in carbon dioxide (CO2) emissions, but due to its large atmospheric reservoir and long lifetime, no detectable signal has been observed in the atmospheric CO2 growth rate. Using the variabilities in CO2 (ΔCO2) and methane (ΔCH4) observed at Hateruma Island, Japan during 1997–2020, we show a traceable CO2 emission reduction in China during February–March 2020. The monitoring station at Hateruma Island observes the outflow of Chinese emissions during winter and spring. A systematic increase in the ΔCO2/ΔCH4 ratio, governed by synoptic wind variability, well corroborated the increase in China’s fossil-fuel CO2 (FFCO2) emissions during 1997–2019. However, the ΔCO2/ΔCH4 ratios showed significant decreases of 29 ± 11 and 16 ± 11 mol mol−1 in February and March 2020, respectively, relative to the 2011–2019 average of 131 ± 11 mol mol−1. By projecting these observed ΔCO2/ΔCH4 ratios on transport model simulations, we estimated reductions of 32 ± 12% and 19 ± 15% in the FFCO2 emissions in China for February and March 2020, respectively, compared to the expected emissions. Our data are consistent with the abrupt decrease in the economic activity in February, a slight recovery in March, and return to normal in April, which was calculated based on the COVID-19 lockdowns and mobility restriction datasets.

Systematic measurements of the atmospheric Ar/N2 ratio have been made at ground-based stations in Japan and Antarctica since 2012. Clear seasonal cycles of the Ar/N2 ratio with summertime maxima were found at middle to high latitude stations, with seasonal amplitudes increasing with increasing latitude. Eight years of the observed Ar/N2 ratio at Tsukuba and Hateruma, Japan showed not only secular increasing trends, but also interannual variations in phase with the observed variations in the global ocean heat content (OHC). The observed secular trend of the Ar/N2 ratio was 0.75±0.30 per meg yr-1. Sensitivity test by using a 2-dimensional model with the Brewer-Dobson circulation (BDC) scenarios indicated the possibility of the secular trend in the surface Ar/N2 ratio being modified significantly by the gravitational separation in the stratosphere. The secular trend of the Ar/N2 ratio, corrected for gravitational separation under the assumption of weakening of BDC simulated by the 2D model, was 0.60±0.30 per meg yr-1. By using a conversion factor of 3.5x10-23 per meg J-1 by assuming a 1-box ocean with a temperature of 3.5 °C, then an average OHC increase rate of 17.1±8.6 ZJ yr-1 for the period 2012–2019 was estimated from the corrected secular trend of the Ar/N2 ratio. This value is consistent with 12.2±1.2 ZJ yr-1 reported by ocean temperature measurements. The effect of the actual atmospheric circulation on the Ar/N2 ratio is still unclear, however the analytical results obtained in the present study imply that the surface Ar/N2 ratio is an important tracer for detecting spatiotemporally-integrated changes in OHC and BDC.

The Grater Tokyo Area is the most populated (38 million) metropolitan area in the world. To capture fossil fuel carbon dioxide (CO2) emissions from the Grater Tokyo Area, we performed ground-based atmospheric observations for measuring concentrations of CO2, radiocarbon in CO2 (14CO2), oxygen (O2) and carbon monoxide (CO) at Tokyo Skytree (TST, with high altitude (250m) inlet) and Yoyogi (YYG, turbulentCO2 flux measurement site located in resident area) in Tokyo and at National Institute for Environmental Studies (NIES, suburb/rural area) in Ibaraki, Japan. The 14CO2 measurement was used for separating the fossil fuel CO2 emissions from the biotic emissions. Results from 14CO2 measurements showed that a ratio of fossil fuel-derived CO2 to the variation of CO2 concentrations was 71% in average for winter both at TST and YYG but varied from 44% to 92%, indicating significant contribution of biotic CO2 in Tokyo. The O2:CO2 exchange ratio (oxidation ratio, OR) was used for the partitioning of CO2 into emissions from gas fuels and gasoline. We observed larger OR in winter than in summer (due to both wintertime increases of fossil fuel combustion and summertime terrestrial biospheric activities) at TST and YYG and larger OR in the morning and late evening in winter due to increase of gas fuel combustion at YYG. We showed that the O2 concentrations might be also used as a proxy for continuous monitoring of fossil fuel CO2 content by assuming typical ratio of gas fuels and gasoline combustions. The presenter will introduce the related projects including development of building/road-scale dynamic CO2 mapping and grid-based CO2 emission inventory with high special resolution in Tokyo.

We employed a global high-resolution inverse model to optimize the CH4 emission using Greenhouse gas Observing Satellite (GOSAT) and surface observation data for a period from 2011−2017 for the two main source categories of anthropogenic and natural emissions. We used the Emission Database for Global Atmospheric Research (EDGAR v4.3.2) for anthropogenic methane emission and scaled them by country to match the national inventories reported to the United Nations Framework Convention on Climate Change (UNFCCC). Wetland and soil sink prior fluxes were simulated using the Vegetation Integrative Simulator of Trace gases (VISIT) model. Biomass burning prior fluxes were provided by the Global Fire Assimilation System (GFAS). We estimated a global total anthropogenic and natural methane emissions of 340.9 Tg CH4 yr−1 and 232.5 Tg CH4 yr−1, respectively. Country-scale analysis of the estimated anthropogenic emissions showed that all the top-emitting countries showed differences with their respective inventories to be within the uncertainty range of the inventories, confirming that the posterior anthropogenic emissions did not deviate from nationally reported values. Large countries, such as China, Russia, and the United States, had the mean estimated emission of 45.7 ± 8.6, 31.9 ± 7.8, and 29.8 ± 7.8 Tg CH4 yr−1, respectively. For natural wetland emissions, we estimated large emissions for Brazil (39.8 ± 12.4 Tg CH4 yr−1), the United States (25.9 ± 8.3 Tg CH4 yr−1), Russia (13.2 ± 9.3 Tg CH4 yr−1), India (12.3 ± 6.4 Tg CH4 yr−1), and Canada (12.2 ± 5.1 Tg CH4 yr−1). In both emission categories, the major emitting countries all had the model corrections to emissions within the uncertainty range of inventories. The advantages of the approach used in this study were: (1) use of high-resolution transport, useful for simulations near emission hotspots, (2) prior anthropogenic emissions adjusted to the UNFCCC reports, (3) combining surface and satellite observations, which improves the estimation of both natural and anthropogenic methane emissions over spatial scale of countries.

Atmospheric CH4 mole fractions were observed aboard the R/V Mirai sailing in waters off Alaska in the Arctic Ocean in September 2012–2017 to investigate the CH4 emissions from the surrounding region, especially from the East Siberian Arctic Shelf (ESAS). The synoptic-scale increases of CH4 were compared with simulated increases based on a Lagrangian Particle Dispersion Model and monthly CH4 flux maps determined by a global atmospheric inversion system. There were good agreements between the observed and simulated CH4 increases, suggesting the validity of CH4 fluxes from the surrounding areas of the cruise experiments. The CH4 emissions from the ESAS in September were further optimized in order to minimize the root mean square of the differences between the observed and simulated CH4 increases. The average (±1σ) of the resulting emission rates was 0.58 ± 0.47 TgCH4 yr−1, which was much smaller than previously reported estimates. The individual optimized CH4 emissions varied from −0.1 ± 0.3 to 1.3 ± 0.4 TgCH4 yr−1, showing a positive correlation with the sea surface temperature and a negative correlation with the ice concentration of the ESAS area in September. These results suggest a possible enhancement of the CH4 emissions from the ESAS in a warmer future.

Extremely high levels of column-averaged dry-air mole fractions of atmospheric methane (XCH4) were detected in August and September 2013 over northeast Asia (∼ 20 ppb above the averaged summertime XCH4 over 2009–2012, after removing a long-term trend), as being retrieved from the Short-Wavelength InfraRed (SWIR) spectral data observed with the Thermal And Near-infrared Sensor for carbon Observation – Fourier Transform Spectrometer (TANSO-FTS) onboard Greenhouse Gases Observing Satellite (GOSAT). Similar enhancements of XCH4 were also observed by the ground-based measurements at two Total Carbon Column Observing Network (TCCON) sites in Japan. The analysis of surface CH4 concentrations observed at three monitoring sites around the Japan archipelago suggest that the extreme increase of XCH4 has occurred in a limited area. The model analysis was conducted to investigate this anomalously high XCH4 event, using an atmospheric transport model. The results indicate that the extreme increase of XCH4 is attributed to the anomalous atmospheric pressure pattern over East Asia during the summer of 2013, which effectively transported the CH4-rich air to Japan from the strong CH4 source areas in east China. The two Japanese TCCON sites, ∼ 1000 km east–west apart each other, coincidentally located along the substantially CH4-rich air flow from east China. This analysis demonstrates the capability of GOSAT to monitor an XCH4 event on a synoptic scale. We anticipate that the synoptic information of XCH4 from GOSAT data contributes to improve our understanding of regional carbon cycle and the regional flux estimation.

A field study was conducted to clarify sources of atmospheric black carbon and related carbonaceous components at Rishiri Island, Japan. We quantified equivalent black carbon (eBC) particle mass and the absorption Angstrom exponent (AAE), atmospheric CO and CH4, in addition to levoglucosan in total suspended particles, a typical tracer of biomass burning. Sixteen high eBC events were identified attributable to either anthropogenic sources or biomass burning in Siberia/China. These events were often accompanied by increases of co-emitted gases such as CH4 and CO. Specifically, we observed pollution events with elevated eBC, AAE, levoglucosan, and CH4 CO slope in late July 2014, which were attributed to forest fires in Siberia by reference to the FLEXPART model footprint and fire hotspots. In autumn, drastic increases of eBC, AAE, and levoglucosan were observed, accompanied by an eBC–CO slope of >15 ng m−3/ppb, resulting from long-range transport of emissions from extensive burning of crop residue on the Northeast China Plain. Other than the sources of fossil fuel combustion in China and forest fires in Siberia, we report for the first time that pollution events in northern Japan are caused by crop residue burning in China. This study elucidated valuable information that will improve understanding of the effects of biomass burning in East Asia on atmospheric carbonaceous components.

Atmospheric oxygen (O2) and carbon dioxide (CO2) variations in the North Pacific were measured aboard a cargo ship, the New Century 2 (NC2), while it cruised between Japan and the United States between December 2015 and November 2016. A fuel cell analyzer and a nondispersive infrared analyzer were used for the measurement of O2 and CO2, respectively. To achieve parts-per-million precision for the O2 measurements, we precisely controlled the flow rates of the sample and reference air introduced into the analyzers and the outlet pressure. A relatively low airflow rate (10 cm3 min−1) was adopted to reduce the consumption rate of the reference gases. In the laboratory, the system achieved measurement precisions of 3.8 per meg for δ(O2 ∕ N2), which is commonly used to express atmospheric O2 variation, and 0.1 ppm for the CO2 mole fraction. After the in situ observation started aboard NC2, we found that the ship's motion caused false wavy variations in the O2 signal with an amplitude of more than several tens of ppm and a period of about 20 s. Although we have not resolved the problem at this stage, hourly averaging considerably suppressed the variation associated with ship motion. Comparison between the in situ observation and flask sampling of air samples aboard NC2 showed that the averaged differences (in situ–flask) and the standard deviations (±1σ) are −2.8 ± 9.4 per meg for δ(O2 ∕ N2) and −0.02 ± 0.33 ppm for the CO2 mole fraction. We compared 1 year of in situ data for atmospheric potential oxygen (APO; O2 +1.1 × CO2) obtained from the broad middle-latitude region (140° E–130° W, 29° N–45° N) with previous flask sampling data from the North Pacific. This comparison showed that longitudinal differences in the seasonal amplitude of APO, ranging from 51 to 73 per meg, were smaller than the latitudinal differences.

Long-term monitoring of carbon monoxide (CO) mixing ratios in the atmosphere over the Pacific Ocean is being carried out on commercial cargo vessels participating in the National Institute for Environmental Studies Voluntary Observing Ships program. The program provides a regular platform for measurement of atmospheric CO along four cruise routes: from Japan to Oceania, the United States, Canada, and Southeast Asia. Flask samples are collected during every cruise for subsequent analysis in the laboratory, and in 2005, continuous shipboard CO measurements were initiated on three of the routes. Here, we describe the system we developed for onboard measurement of CO mixing ratios with a commercially available gas filter correlation CO analyzer. The fully automated system measures CO in ambient air, and the detector sensitivity and background signals are calibrated by referencing the measurements to a CO-in-air standard gas (~1 ppmv) and to CO-free air scrubbed with a catalyst, respectively. We examined the artificial production of CO in the high-pressure working gas standards during storage by referencing the measurements to CO standard gases maintained as our primary scale before and after use on the ships. The onboard performance of the continuous CO measurement system was evaluated by comparing its data with data from laboratory analyses of flask samples using gas chromatography with a reduction gas detector. The reasonably good consistency between the two independent measurement methods demonstrated the good performance of both methods over the course of 3–5 years. The continuous measurement system was more useful than the flask sampling method for regionally polluted air masses, which were often encountered on Southeast Asian cruises.

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.

In situ observation of the atmospheric CO2, CH4, and CO mixing ratios at Hateruma Island (HAT, 24.05° N, 123.80° E) often show synoptic-scale variations with correlative elevations during winter, associated with air transport from the East Asian countries. We examine winter (November– March) trends in ΔCH4 / ΔCO2, ΔCO / ΔCO2, and ΔCO / ΔCH4 observed at Hateruma over the period 1999 to 2010. To investigate the relationship between the East Asian emissions and the short-term variations in the atmospheric mixing ratios, we use the FLEXPART Lagrangian particle dispersion model (LPDM). The observed ratios ΔCH4 / ΔCO2 and ΔCO / ΔCO2 both show an overall gradual decrease over the study period due to a recent rapid increase in fossil fuel consumption in China. We note, however, that the decreasing rates of ΔCH4 / ΔCO2 and ΔCO / ΔCO2 show gradual decrease and increase, respectively, during the entire observation periods used in this study. The ΔCO / ΔCH4 slope, on the other hand, shows an increasing trend during 1999–2004 but a decrease during 2005–2010. Calculation of the concentration footprint for the atmospheric observation at HAT by using the FLEXPART LPDM indicates that most of the short-term variations are caused by emission variations from northern and eastern China. Combined with a set of reported emission maps, we have estimated the temporal changes in the annual CH4 and CO emissions from China under the assumption that the estimate of the fossil-fuel-derived CO2 emissions based on the energy statistics are accurate. The estimated annual CH4 emissions, corresponding to nonseasonal sources or anthropogenic sources without rice fields, show a nearly constant value of 39 ± 7 TgCH4 yr−1 during 1998–2002, and then gradually increase to 46 ± 8 TgCH4 yr−1 in 2009/2010. The estimated annual CO emissions increase from 134 ± 32 TgCO yr−1 in 1998/1999 to 182 ± 42 TgCO yr−1 in 2004/2005, level off after 2005, and then slightly decrease to less than 160 TgCO yr−1 in 2008–2010.

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (similar to biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003-2012 decade, global methane emissions are estimated by top-down inversions at 558 TgCH(4) yr(-1), range 540-568. About 60% of global emissions are anthropogenic (range 50-65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bottom-up approaches suggest larger global emissions (736 TgCH(4) yr(-1), range 596-884) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources. Considering the atmospheric constraints on the top-down budget, it is likely that some of the individual emissions reported by the bottom-up approaches are overestimated, leading to too large global emissions. Latitudinal data from top-down emissions indicate a predominance of tropical emissions (similar to 64% of the global budget, amp;lt;30 degrees N) as compared to mid (similar to 32 %, 30-60 degrees N) and high northern latitudes (similar to 4 %, 60-90 degrees N). Top-down inversions consistently infer lower emissions in China (similar to 58 TgCH(4) yr(-1), range 51-72, -14 %) and higher emissions in Africa (86 TgCH(4) yr(-1), range 73-108, + 19 %) than bottom-up values used as prior estimates. Overall, uncertainties for anthropogenic emissions appear smaller than those from natural sources, and the uncertainties on source categories appear larger for top-down inversions than for bottom-up inventories and models. The most important source of uncertainty on the methane budget is attributable to emissions from wetland and other inland waters. We show that the wetland extent could contribute 30-40% on the estimated range for wetland emissions. Other priorities for improving the methane budget include the following: (i) the development of process-based models for inland-water emissions, (ii) the intensification of methane observations at local scale (flux measurements) to constrain bottom-up land surface models, and at regional scale (surface networks and satellites) to constrain top-down inversions, (iii) improvements in the estimation of atmospheric loss by OH, and (iv) improvements of the transport models integrated in top-down inversions. The data presented here can be downloaded from the Carbon Dioxide Information Analysis Center (http://doi.org/10.3334/CDIAC/GLOBAL_METHANE_BUDGET_2016_V1.1) and the Global Carbon Project. Funding Agencies|Swiss National Science Foundation; NASA [NNX14AF93G, NNX14AO73G]; National Environmental Science Program - Earth Systems and Climate Change Hub; European Commission [283576, 633080]; ESA Climate Change Initiative Greenhouse Gases Phase 2 project; US Department of Energy, BER [DE-AC02-05CH11231]; FAO member countries; Environment Research and Technology Development Fund of the Ministry of the Environment, Japan [2-1502]; ERC [322998]; NERC [NE/J00748X/1]; Swedish Research Council VR; Research Council of Norway [244074]; NSF [1243232, 1243220]; National Science and Engineering Research Council of Canada (NSERC); Chinas QianRen Program; CSIRO Australia; Australian Bureau of Meteorology; Australian Institute of Marine Science; Australian Antarctic Division; NOAA USA; Meteorological Service of Canada; National Aeronautic and Space Administration (NASA) [NAG5-12669, NNX07AE89G, NNX11AF17G, NNX07AE87G, NNX07AF09G, NNX11AF15G, NNX11AF16G]; Department of Energy and Climate Change (DECC, UK) [GA01081]; Commonwealth Scientific and Industrial Research Organization (CSIRO Australia); Bureau of Meteorology (Australia); Joint DECC/Defra Met Office Hadley Centre Climate Programme [GA01101]

[1] Observations of tropospheric N2O mixing ratio show significant variability on interannual timescales (0.2 ppb, 1 standard deviation). We found that interannual variability in N2O is weakly correlated with that in CFC-12 and SF6 for the northern extratropics and more strongly correlated for the southern extratropics, suggesting that interannual variability in all these species is influenced by large-scale atmospheric circulation changes and, for SF6 in particular, interhemispheric transport. N2O interannual variability was not, however, correlated with polar lower stratospheric temperature, which is used as a proxy for stratosphere-to-troposphere transport in the extratropics. This suggests that stratosphere-to-troposphere transport is not a dominant factor in year-to-year variations in N2O growth rate. Instead, we found strong correlations of N2O interannual variability with the Multivariate ENSO Index. The climate variables, precipitation, soil moisture, and temperature were also found to be significantly correlated with N2O interannual variability, suggesting that climate-driven changes in soil N2O flux may be important for variations in N2O growth rate.