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Observations of the atmospheric CO2 concentration from a 90-m tower in Berezorechka, western Siberia, that have taken place since October 2001 were used to characterize CO2 variations over a vast boreal forest area. A new CO2 standard gas saving system was developed that reduced the consumption of standard gases and kept the analysis precision to within 0.3 μmol mol−1. The CO2 day-to-day variation correlated well with atmospheric stability. The average amplitudes of the diurnal variation at 80 m were found to be about 17 and 1.5 μmol mol−1 in July and December 2003, respectively. Extremely high daytime CO2 concentrations of greater than 400 μmol mol−1 were occasionally observed during the winter, which were caused by anticyclonic atmospheric conditions lasting more than several days. Afternoon CO2 values observed at the 80-m height agreed to within 0.4 μmol mol−1 with aircraft CO2 measurements taken in the planetary boundary layer; disagreements were found for anticyclonic conditions in the winter. The afternoon CO2 values reached their maximum in mid-January and their minimum late in July, with the seasonal amplitude of 30.9 μmol mol−1. Compared to observations at background stations, this observation tower recorded a larger seasonal amplitude and earlier occurrence of the seasonal minimum.

Simultaneous observations from the Infrared Atmospheric Sounding Interferometer (IASI) and from the Advanced Microwave Sounding Unit (AMSU), launched together onboard the European MetOp platform in October 2006, are used to retrieve an upper tropospheric content of carbon dioxide (CO2) covering the range 11–15 km (100–300 hPa), in clear-sky conditions, in the tropics, over sea, for the first year of operation of MetOp (January 2008–December 2008). With its very high spectral resolution, IASI provides fourteen channels in the 15 μm band highly sensitive to CO2 with reduced sensitivities to other atmospheric variables. IASI observations, sensitive to both CO2 and temperature, are used in conjunction with AMSU observations, only sensitive to temperature, to decorrelate both signals through a non-linear inference scheme based on neural networks. A key point of this approach is that no use is made of prior information in terms of CO2 seasonality, trend, or geographical patterns. The accuracy of the retrieval is estimated to be about 2.0 ppmv (~0.5%) for a 5°×5° spatial resolution on a monthly time scale. Features of the retrieved CO2 space-time distribution include: (1) a strong seasonal cycle of 4 ppmv in the northern tropics with a maximum in June–July and a minimum in September–October. This cycle is characterized by a backward two-months lag as compared to the surface, by a backward one-month lag as compared to measurements performed at 11 km, and by a forward one-month lag as compared to observations performed at the tropopause (16 km). This is likely due to the time-lag of CO2 cycle while transported from the surface to the upper troposphere; (2) a more complex seasonal cycle in the southern tropics, in agreement with in-situ measurements; (3) a latitudinal variation of CO2 shifting from a South-to-North increase of 3.5 ppmv in boreal spring to a South-to-North decrease of 1.5 ppmv in the fall, in excellent agreement with tropospheric aircraft measurements; (4) signatures of CO2 emissions (such as biomass burning) transported to the troposphere. In addition to bringing an improved view of CO2 distribution, these results from IASI should provide an additional means to observe and understand atmospheric transport pathways of CO2 from the surface to the upper troposphere.

By the results of long-term (1997–2007) airborne sounding, the vertical distribution of three greenhouse gases such as CO2, CH4, and N2O above the south of Western Siberia is investigated. The average monthly profiles of the distribution of these components in height and the long-term change in gas concentration at different heights are presented. The climatic characteristics of the vertical distribution of these gases are determined.

Northern Eurasia, the largest land-mass in the northern extratropics, accounts for ∼20% of the global land area. However, little is known about how the biogeochemical cycles, energy and water cycles, and human activities specific to this carbon-rich, cold region interact with global climate. A major concern is that changes in the distribution of land-based life, as well as its interactions with the environment, may lead to a self-reinforcing cycle of accelerated regional and global warming. With this as its motivation, the Northern Eurasian Earth Science Partnership Initiative (NEESPI) was formed in 2004 to better understand and quantify feedbacks between northern Eurasian and global climates. The first group of NEESPI projects has mostly focused on assembling regional databases, organizing improved environmental monitoring of the region, and studying individual environmental processes. That was a starting point to addressing emerging challenges in the region related to rapidly and simultaneously...

2005年12月以降、新しい空気採取装置（ASE）を利用して、オーストラリアと日本を結ぶJALの旅客機によって西部太平洋上の高度約10kmにおける大気中二酸化炭素(CO2)の測定結果を収集した。ASEで観測されたCO2は、同じフライトで観測した二酸化炭素連続測定装置（CME）の結果と非常に良く一致していた。また、ASEのデータは高時間分解能を持つCMEのデータに比べて観測密度が粗いが、両データとも、北緯30度から南緯30度までを5度間隔で分割した緯度帯平均のCO2濃度は、近い値を示した。JAL旅客機による新旧観測において一貫したデータセットを作成するために、気象研究所と国立環境研究所で使用しているCO2標準ガスのスケールを比較した。新観測で得られたCO2のデータには明瞭な季節変化と増加傾向が見られ、それらは、過去12年間の旧観測で得られたCO2変動の気候値の外挿から再現された変動とほぼ一致していた。特に、新観測において、長期的トレンドを除去した季節変動の緯度帯変化は、旧観測の気候値から得られるものと極めて良く類似していた。これらの結果から、JAL旅客機による新旧の観測データが一貫した連続性を保っていることが示された。

New automated observation systems for use in passenger aircraft to measure atmospheric carbon dioxide (CO2) and other trace species have been developed and are described in this paper. The Continuous CO2 Measuring Equipment (CME) is composed mainly of a nondispersive infrared analyzer, a datalogger, and two calibration cylinders for in situ CO2 measurements. The Automatic Air Sampling Equipment (ASE), on the other hand, is designed for flask sampling; the instrument, connected to a metal bellows pump, is made up of a specially designed control board and can accommodate 12 flasks. The CME platform can be used to conduct high-frequency measurements of CO2 for obtaining a detailed spatial observation over a wide area, while ASE, despite the limited flight frequency, can provide useful distributions not only of CO2 but also various trace gas species, as well as their isotopic ratios. ASE and CME are installed on the racks in the forward cargo compartment of the aircraft and the air bypass intake is mounted on the air-conditioning duct upstream of the recirculation fan. Both sets of sampling equipment are automatically controlled through input of relevant flight parameters from the aircraft data system. Their deployment in a Boeing 747-400 aircraft was approved by the aviation regulatory agencies in the United States and Japan through issuance of the supplemental type certificate (STC), while the approval for installation of CME in a Boeing 777-200ER was also obtained via STC. First measurement results of CO2 variations obtained by CME and ASE deployed on Japan Airlines (JAL) aircraft are reported herein.

Atmospheric inversions use measurements of atmospheric CO2 gradients to constrain regional surface fluxes. Current inversions indicate a net terrestrial CO2 sink in China between 0.16 and 0.35 PgC/yr. The uncertainty of these estimates is as large as the mean because the atmospheric network historically contained only one high altitude station in China. Here, we revisit the calculation of the terrestrial CO2 flux in China, excluding emissions from fossil fuel burning and cement production, by using two inversions with three new CO2 monitoring stations in China as well as aircraft observations over Asia. We estimate a net terrestrial CO2 uptake of 0.39–0.51 PgC/yr with a mean of 0.45 PgC/yr in 2006–2009. After considering the lateral transport of carbon in air and water and international trade, the annual mean carbon sink is adjusted to 0.35 PgC/yr. To evaluate this top-down estimate, we constructed an independent bottom-up estimate based on ecosystem data, and giving a net land sink of 0.33 PgC/yr. This demonstrates closure between the top-down and bottom-up estimates. Both top-down and bottom-up estimates give a higher carbon sink than previous estimates made for the 1980s and 1990s, suggesting a trend towards increased uptake by land ecosystems in China.

To investigate the effect of additional CO2 observations in the Siberia region on the Asian and global surface CO2 flux analyses, two experiments using different observation dataset were performed. One experiment was conducted using a data set that includes additional observations of Siberian tower measurements (Japan-Russia Siberian Tall Tower Inland Observation Network: JR-STATION), and the other experiment was conducted using a data set without the above additional observations. The results show that the global balance of the sources and sinks of surface CO2 fluxes was maintained for both experiments with and without the additional observations. While the magnitude of the optimized surface CO2 flux uptake in Siberia decreased, the magnitude of the optimized surface CO2 flux uptake in the other regions (e.g., Europe) of the Northern Hemisphere (NH) increased for the experiment with the additional observations. This change was mostly caused by changes in the magnitudes of surface CO2 flux in June and July. The observation impact measured by uncertainty reduction and self-sensitivity tests shows that additional observations provide useful information on the estimated surface CO2 flux. It is expected that the Siberian observations play an important role in estimating surface CO2 flux in the NH in the future.

Increasing atmospheric carbon dioxide (CO2) is the principal driver of anthropogenic climate change. Asia is an important region for the global carbon budget, with 4 of the world's 10 largest national emitters of CO2. Using an ensemble of seven atmospheric inverse systems, we estimated land biosphere fluxes (natural, land-use change and fires) based on atmospheric observations of CO2 concentration. The Asian land biosphere was a net sink of −0.46 (−0.70–0.24) PgC per year (median and range) for 1996–2012 and was mostly located in East Asia, while in South and Southeast Asia the land biosphere was close to carbon neutral. In East Asia, the annual CO2 sink increased between 1996–2001 and 2008–2012 by 0.56 (0.30–0.81) PgC, accounting for ∼35% of the increase in the global land biosphere sink. Uncertainty in the fossil fuel emissions contributes significantly (32%) to the uncertainty in land biosphere sink change., Land biosphere uptake of carbon is important in mitigating the anthropogenic increase in atmospheric CO2 and its climate forcing. Here, the authors show that land biosphere uptake of carbon in Asia has increased substantially since the mid 1990s, likely owing to reforestation and regional climate change.

Satellite observations of atmospheric CO2 offer the potential to identify regional carbon surface sources and sinks and to investigate carbon cycle processes. The extent to which satellite measurements are useful however, depends on the near surface sensitivity of the chosen sensor. In this paper, the capability of the SCIAMACHY instrument on board ENVISAT, to observe lower tropospheric and surface CO2 variability is examined. To achieve this, atmospheric CO2 retrieved from SCIAMACHY near infrared (NIR) spectral measurements, using the Full Spectral Initiation (FSI) WFM-DOAS algorithm, is compared to in-situ aircraft observations over Siberia and additionally to tower and surface CO2 data over Mongolia, Europe and North America. Preliminary validation of daily averaged SCIAMACHY/FSI CO2 against ground based Fourier Transform Spectrometer (FTS) column measurements made at Park Falls, reveal a negative bias of about −2.0% for collocated measurements within ±1.0° of the site. However, at this spatial threshold SCIAMACHY can only capture the variability of the FTS observations at monthly timescales. To observe day to day variability of the FTS observations, the collocation limits must be increased. Furthermore, comparisons to in-situ CO2 observations demonstrate that SCIAMACHY is capable of observing a seasonal signal that is representative of lower tropospheric variability on (at least) monthly timescales. Out of seventeen time series comparisons, eleven have correlation coefficients of 0.7 or more, and have similar seasonal cycle amplitudes. Additional evidence of the near surface sensitivity of SCIAMACHY, is provided through the significant correlation of FSI derived CO2 with MODIS vegetation indices at over twenty selected locations in the United States. The SCIAMACHY/MODIS comparison reveals that at many of the sites, the amount of CO2 variability is coincident with the amount of vegetation activity. The presented analysis suggests that SCIAMACHY has the potential to detect CO2 variability within the lowermost troposphere arising from the activity of the terrestrial biosphere.

The thermal infrared (TIR) band of the Thermal and Near Infrared Sensor for Carbon Observation (TANSO)–Fourier Transform Spectrometer (FTS) on board the Greenhouse Gases Observing Satellite (GOSAT) has been observing carbon dioxide (CO2) concentrations in several atmospheric layers since its launch. This study compared TANSO-FTS TIR V1.0 CO2 data and CO2 data obtained in the Comprehensive Observation Network for TRace gases by AIrLiner (CONTRAIL) project in the upper troposphere and lower stratosphere (UTLS), where the TIR band of TANSO-FTS is most sensitive to CO2 concentrations, to validate the quality of the TIR V1.0 UTLS CO2 data from 287 to 162 hPa. From a comparison made during flights between Tokyo and Sydney, the averages of the TIR upper atmospheric CO2 data agreed well with the averages of the data obtained by the CONTRAIL Continuous CO2 Measuring Experiment (CME) within 0.1 % for all of the seasons in the Southern Hemisphere. The results of a comparison for all of the eight airline routes showed that the agreement between the TIR and CONTRAIL CO2 data was within 0.5 % on average in the Northern Hemisphere, which was better than the agreement between a priori and CONTRAIL CO2 data. The quality of TIR lower stratospheric CO2 data depends largely on the information content, and therefore has a seasonal dependence. In high latitudes, TIR V1.0 lower stratospheric CO2 data are only valid in the summer. The magnitude of bias in the TIR upper atmospheric CO2 data did not have a clear longitudinal dependence. The comparison results for flights in northern low and middle latitudes showed that the agreement between TIR and CONTRAIL CO2 data in the upper troposphere was worse in the spring and summer than in the fall and winter. This could be attributed to a larger negative bias in the upper atmospheric a priori CO2 data in the spring and summer and a seasonal dependence of spectral bias in TANSO-FTS TIR Level 1B (L1B) radiance data. The negative bias in northern middle latitudes made the maximum of TIR CO2 concentrations lower than that of CONTRAIL CO2 concentrations, which leads to underestimate the amplitude of CO2 seasonal variation.

第6回極域科学シンポジウム分野横断セッション：[IA] 急変する北極気候システム及びその全球的な影響の総合的解明―GRENE北極気候変動研究事業研究成果報告2015―11月19日（木） 国立極地研究所１階交流アトリウム

To make the investigation of the temporal and spatial variations of atmospheric CO2 in and above the planetary boundary layer more flexible and economical, a lightweight observation system using a small unmanned aerial vehicle has been developed whose flight path is preset using GPS. The total weight of the CO2 measurement device carried inside the vehicle is about 3.5 kg. The device is equipped with both flow and pressure controllers and can be used to measure atmospheric CO2 from the ground surface to a maximum altitude of about 3000 m. The response time of the instrument is about 20 s, with a precision of about ±0.26 ppm. The observation system is easy to handle and can be easily and quickly deployed at a site to make frequent measurements in and above the boundary layer. Compared to the deployment of a piloted aircraft the system shows distinctive advantages, in addition to being more affordable. To test the system, preliminary measurements over a boreal forest area in Japan in the summer of 2000 have been conducted. The results indicate that the unmanned aerial vehicle measurement system provides an affordable platform that can be used to obtain quantitative understanding of the temporal and vertical variations of atmospheric CO2 in and above the planetary boundary layer.

From 5 to 14 March, 2002, the Arctic Airborne Measurement Program 2002(AAMP02) was conducted on a round-trip flight between Nagoya, Japan, and Longyearbyen, Svalbard, via Anchorage and Barrow, U.S.A. and the North Pole using a chartered twin-jet aircraft, the Gulfstream-II(G-II). On board the G-II, in-situ measurements of the ozone concentration were carried out every 12s in order to obtain information on air mass differences and advection. Vertical profiles of the ozone concentration observed over Longyearbyen agreed well with those observed by ozone sonde launched around the same time from Ny-Ålesund, about 100km north of Longyearbyen. The ozone variations observed in the upper troposphere and lower stratosphere showed negative correlation with the CO_2 concentration, suggesting vertical displacements of air masses. However, it was also observed that the ozone concentration fluctuated considerably with little consistency with the meteorological field.

The Arctic Airborne Measurement Program 2002(AAMP 02) campaign was carried out in March 2002 as one of the sub programs of the project Variations of atmospheric constituents and their climate impact in the Arctic". The main goal of the project was to investigate the transport, transformation and radiative effect of trace gases and aerosols, and their role in the global climate. An instrumented jet plane, Gulfstream II(G-II), was flown from Nagoya, Japan via Barrow, Alaska to Longyearbyen(78°N , 15°E ), Svalbard, crossing the Arctic Ocean in the lower stratospher. Three local flights were made over the Greenland Sea around Svalbard and two profile flights near Barrow. The plane was equipped with CO_2 and ozone analyzers, gas and aerosol sampling systems, aerosol particle counter, nephelometer, absorption photometer, PMS particle probes, sunphotometer, dew point hygrometer and dropsonde system. During the campaign, intensitive surface operations were also conducted at Ny-Ålesund(79°N , 12°E ), Svalbard. Vertical profiles of several trace gases gave information about transport, a new observation by sunphotometer derived an aerosol optical depth in the stratosphere, and another new observation by dropsonde gave information on the polar vortex.

Systematic collections of stratospheric air samples have been conducted over Japan since 1985 using a balloon-borne cryogenic sampler. The collection of stratospheric air samples was also carried out twice over Scandinavia and once over Antarctica. Vertical profiles of CO 2 concentration thus obtained over these locations were quite similar to each other; CO 2 concentration decreased with increasing altitude in the lower stratosphere and reached an almost constant value in the mid-stratosphere. δ 13 C of stratospheric CO 2 observed over these locations enriched with increasing altitude. A negative correlation between δ 13 C and CO 2 concentration with Δδ 13 C/ΔCO 2 of −0.02‰ ppmv −1 was found in the lower stratosphere. Although CO 2 concentration was almost constant in the mid-stratosphere, the δ 13 C enrichment was observed in succession. δ 18 O of stratospheric CO 2 also enriched with increasing altitude. The enrichment was significant; δ 18 O was almost 0‰ at the tropopause and reached a maximum value of about 11‰ at a layer with N 2 O concentration of about 10 ppbv. A compact relation between δ 18 O and N 2 O concentration was consistently observed for these locations. Stratosperic CO 2 over Japan showed a secular increase with an average rate of 1.4 ppmv yr −1 for the period 1985–2000. The secular increase was not constant with time, and temporal stagnation of the CO 2 increase was observed in 1997. DOI: 10.1034/j.1600-0889.2003.00059.x

Concentrations of carbonyl sulfide (COS) were measured in whole air samples collected between East Asia (Japan) and the Arctic (Spitsbergen) up to an altitude of 12 km during the Arctic Airborne Measurement Program 98 (AAMP98). Continuously measured O3 and CO2 concentrations were used to interpret the distribution of COS concentrations. A latitudinal gradient to lower concentrations of COS was observed poleward of 70°N; concentrations of COS were 421±27 pptv poleward of 70°N and 461±30 pptv at 60-70°N. The relationship between COS concentration and the O3/CO2 ratio indicates that the concentrations of COS near the ozonopause were almost equal to those in the troposphere, and then decreased as the O3/CO2 ratio increased. Tropospheric influence was observed up to potential temperatures of 350 K in this study. According to the AAMP98 observations, on the basis of the trajectory analysis and the O3/O2 ratio, distribution of COS in the Arctic lowermost stratosphere is certainly effected by the downward transport of an arctic stratospheric air mass and by the horizontal transport of a tropospheric air mass across the tropopause over midlatitudes. The sulfate aerosol produced by COS oxidation is estimated to be very small at the observed altitudes between East Asia and the Arctic in late winter.

Eight surface observation sites providing quasi-continuous measurements of atmospheric methane mixing ratios have been operated since the mid-2000's in Siberia. For the first time in a single work, we assimilate 1 year of these in situ observations in an atmospheric inversion. Our objective is to quantify methane surface fluxes from anthropogenic and wetland sources at the mesoscale in the Siberian lowlands for the year 2010. To do so, we first inquire about the way the inversion uses the observations and the way the fluxes are constrained by the observation sites. As atmospheric inversions at the mesoscale suffer from mis-quantified sources of uncertainties, we follow recent innovations in inversion techniques and use a new inversion approach which quantifies the uncertainties more objectively than the previous inversion systems. We find that, due to errors in the representation of the atmospheric transport and redundant pieces of information, only one observation every few days is found valuable by the inversion. The remaining high-resolution quasi-continuous signal is representative of very local emission patterns difficult to analyse with a mesoscale system. An analysis of the use of information by the inversion also reveals that the observation sites constrain methane emissions within a radius of 500 km. More observation sites than the ones currently in operation are then necessary to constrain the whole Siberian lowlands. Still, the fluxes within the constrained areas are quantified with objectified uncertainties. Finally, the tolerance intervals for posterior methane fluxes are of roughly 20 % (resp. 50 %) of the fluxes for anthropogenic (resp. wetland) sources. About 50–70 % of Siberian lowlands emissions are constrained by the inversion on average on an annual basis. Extrapolating the figures on the constrained areas to the whole Siberian lowlands, we find a regional methane budget of 5–28 TgCH4 for the year 2010, i.e. 1–5 % of the global methane emissions. As very few in situ observations are available in the region of interest, observations of methane total columns from the Greenhouse Gas Observing SATellite (GOSAT) are tentatively used for the evaluation of the inversion results, but they exhibit only a marginal signal from the fluxes within the region of interest.

1998年の3月に実施された北極圏航空機観測計画（Arctic Airborne Measurement Program 1998; AAMP 98）において航空機にCO2濃度連続観測装置を搭載し，北極域対流圏及び下部成層圏におけるCO2濃度の空間分布を観測した. CO2濃度は下部成層圏において高度と共に急激に減少する鉛直勾配が存在しているが対流圏においては鉛直方向の濃度勾配は非常に小さかった． 下部成層圏における水平分布においては緯度方向にCO2濃度の系統的な勾配は見られなかったが，78°-80°Nにおいて水平飛行中に極めて高濃度のCO2が観測された． このことから，等圧面上であってもCO2濃度の分布が水平方向に大きく異なる場合のあることが明らかになった． 本観測で得られたCO2濃度とO3 濃度は非常に良い負の相関を示す． これは濃度の空間分布が主に空気塊の混合に支配されていることを表している．, Tropospheric and lower stratospheric CO2 mixing ratios were measured onboard an aircraft in the Arctic Airborne Measurement Program 1998. Steep vertical gradients in CO2 mixing ratio were observed in the lower stratosphere. Small gradients were seen in the troposphere, reflecting weak sources and sinks for CO2 in winter. A significant increase in CO2 mixing ratio was found during level flight in the lower stratosphere. Back trajectory analysis indicated that rapid upward transport brought high CO2 to the observation area. Spatial variations of CO2 mixing ratio were highly correlated with O3 mixing ratio. It is suggested that CO2 distribution was produced mainly by air transport and mixing.

Regional net carbon fluxes of terrestrial ecosystems could be estimated with either biogeochemistry models by assimilating surface carbon flux measurements or atmospheric CO2 inversions by assimilating observations of atmospheric CO2 concentrations. Here we combine the ecosystem biogeochemistry modeling and atmospheric CO2 inverse modeling to investigate the magnitude and spatial distribution of the terrestrial ecosystem CO2 sources and sinks. First, we constrain a terrestrial ecosystem model (TEM) at site level by assimilating the observed net ecosystem production (NEP) for various plant functional types. We find that the uncertainties of model parameters are reduced up to 90% and model predictability is greatly improved for all the plant functional types (coefficients of determination are enhanced up to 0.73). We then extrapolate the model to a global scale at a 0.5° × 0.5° resolution to estimate the large-scale terrestrial ecosystem CO2 fluxes, which serve as prior for atmospheric CO2 inversion. Second, we constrain the large-scale terrestrial CO2 fluxes by assimilating the GLOBALVIEW-CO2 and mid-tropospheric CO2 retrievals from the Atmospheric Infrared Sounder (AIRS) into an atmospheric transport model (GEOS-Chem). The transport inversion estimates that: (1) the annual terrestrial ecosystem carbon sink in 2003 is −2.47 Pg C yr−1, which agrees reasonably well with the most recent inter-comparison studies of CO2 inversions (−2.82 Pg C yr−1); (2) North America temperate, Europe and Eurasia temperate regions act as major terrestrial carbon sinks; and (3) The posterior transport model is able to reasonably reproduce the atmospheric CO2 concentrations, which are validated against Comprehensive Observation Network for TRace gases by AIrLiner (CONTRAIL) CO2 concentration data. This study indicates that biogeochemistry modeling or atmospheric transport and inverse modeling alone might not be able to well quantify regional terrestrial carbon fluxes. However, combining the two modeling approaches and assimilating data of surface carbon flux as well as atmospheric CO2 mixing ratios might significantly improve the quantification of terrestrial carbon fluxes.

Methane is a substantial contributor to climate change. It also contributes to maintaining the background levels of tropospheric ozone. Among a variety of CH4 sources, current estimates suggest that CH4 emissions from oil and gas processes account for approximately 20% of worldwide anthropogenic emissions. Here, we report on observational evidence of CH4 emissions from offshore oil and gas platforms in Southeast Asia, detected by a highly time-resolved spectroscopic monitoring technique deployed onboard cargo ships of opportunity. We often encountered CH4 plumes originating from operational flaring/venting and fugitive emissions off the coast of the Malay Peninsula and Borneo. Using night-light imagery from satellites, we discovered more offshore platforms in this region than are accounted for in the emission inventory. Our results demonstrate that current knowledge regarding CH4 emissions from offshore platforms in Southeast Asia has considerable uncertainty and therefore, emission inventories used for modeling and assessment need to be re-examined.

In order to characterize airborne lead in eastern and central Russian cities in terms of lead isotope ratios, aerosol samples were collected at six selected cities and Moscow, and their lead concentrations and isotope ratios were studied by comparing them to the data of ore lead used in Russia. All eastern Russian cities (Vladivostok, Khabarovsk and Yakutsk) were found to have isotope ratios similar to those of ore leads in Kazakhstan, the major lead producer for Russia. Samples collected in Moscow also showed isotope ratios similar to those of eastern Russian cities. The contribution from coal combustion to airborne lead was considered to be small even in winter, in these cities. This observation suggested that the origin of lead in these Russian atmosphere regions is closely related to the lead products (e.g. leaded gasoline). The lead isotope ratios in three eastern Russian cities were very close to the value for Russian air mass reported previously in Japan, which were also in good agreement with the same observation in Sweden. However, considerably different lead isotope ratios were observed in central Russian cities, Kemerovo and Nizhnevartovsk, indicating that specific lead emissions, such as industrial activities using Precambrian-age ores or unique leaded gasoline, might contribute to the atmospheric lead.

Variations of δ^C in atmospheric CO_2 were reconstructed for the period of 1724 to 1961 by analyzing a high-accumulation ice core drilled at H15,Antarctica. Measured values of δ^C were corrected for the gravitational enrichment which occurred in the firn, on the basis of the analytical results of δ^N in N_2 in the core. From the vertical profile of δ^N calculated using a diffusion model for the firn, it was suggested that the air in the layer shallower than 17m depth was mixed well with the atmosphere over the firn surface. The average value of δ^C during the period 1724-1775 was found to be -6.67±0.11‰. δ^C decreased secularly from this value to -7.33‰ in 1961,and its trend was enhanced especially after the late 19th century, corresponding to the long-term increase of the CO_2 concentration. CO_2 fluxes estimated by deconvolution analysis of the reconstructed CO_2 concentrations with the box-diffusion model accounted for the observed variations of δ^C fairly well. It was also suggested that a dip of δ^C found at the end of the 18th century was attributable to terrestrial biospheric CO_2 emissions enhanced under high air temperatures.

In situ measurement of atmospheric nitrous oxide (N 2 O) has been carried out at Hateruma monitoring station (lat 24°03 ′ N, long 123°48 ′ E) since March 1996 by the National Institute for Environmental Studies (NIES). A fully automated gas chromatograph equipped with an electron capture detector (ECD) measures the N 2 O concentrations at a frequency of 3 air samples per hour. Details of the experimental methods and procedures are presented in this paper. The N 2 O concentrations observed from March 1996 to February 1999 increased at an average rate of 0.64 ppb/yr. The observed data also suggest that there is a weak annual cycle of N 2 O concentration, increasing in autumn and winter and decreasing in spring and summer, with a peak-to-peak amplitude of at most 0.3 ppb. The N 2 O mixing ratios, smoothed with the 24-h running average, clearly showed short-term variability with synoptic timescales and had peak-to-peak amplitudes of about 1 ppb or less. These short-term variations correlated positively with the short-term variations of CO 2 during the period from winter to early spring when the air masses arriving at Hateruma are dominantly transported from the Asian continent. The ΔN 2 O/ΔCO 2 ratios could be used to constrain the relative strengths of these fluxes on a regional scale.

The global distribution of atmospheric methyl bromide (CH 3 Br) obtained from extensive new measurements of atmospheric CH 3 Br from latitude 82.5°N to 69.1°S, showed a small decrease from mid- to high-latitudes, a gradient between the northern and southern hemispheres with a ratio of 1.2 to 1.3, and occasional high concentrations in the tropics. The observed data and modeled distributions of industrial CH 3 Br were used to apportion CH 3 Br between natural and industrial components for both hemisphere. We obtained an estimated man-made contribution of 4.3 pptv and 2.3 pptv in the northern and southern hemispheres, respectively and a natural (non-industrial) background concentration in both hemispheres of 6 pptv with a slight increase in the tropics.

Methyl chloride (CH3Cl), the most abundant halocarbon in the atmosphere, has received much attention as a natural source of chlorine atoms in the stratosphere1,2. The annual global flux of CH3Cl has been estimated to be around 3.5 Tg on the grounds that this must balance the loss through reaction with OH radicals (which gives a lifetime for atmospheric CH3Cl of 1.5 yr)3,4,5. The most likely main source of methyl chloride has been thought to be oceanic emission2,6,7,8, with biomass burning the second largest source9. But recent seawater measurements10 indicate that oceanic fluxes cannot account for more than 12% of the estimated global flux of CH3Cl, raising the question of where the remainder comes from. Here we report evidence of significant CH3Cl emission from warm coastal land, particularly from tropical islands. This conclusion is based on a global monitoring study and spot measurements, which show enhancement of atmospheric CH3Cl in the tropics, a close correlation between CH3Cl concentrations and those of biogenic compounds emitted by terrestrial plants, and OH-linked seasonality of CH3Cl concentrations in middle and high latitudes. A strong, equatorially located source of this nature would explain why the distribution of CH3Cl is uniform between the Northern and Southern hemispheres, despite their differences in ocean and land area.

On January 3rd, 1998, a cryogenic air sampling experiment was carried out at Syowa Station (69S, 40E), which is the first successful trial in the world for collection of large amount of stratospheric air over the Antarctic. The samples are analyzed for CO 2 , CH 4 , CFCs, and C and O isotope ratios in CO 2 in the laboratories. As the meteorological conditions for launching and payload recovery are both critical, feasibility on wind conditions over Syowa Station was studied in detail. The balloon launching operations had to be performed without a specialist. Facilities for balloon launching, tracking, and other support systems were newly designed for ready-to- and easy-to-use. Realtime remote support from Japan for the balloon launching and flight control operations was applied using a computer network linked by INMARSAT.

The Arctic Airborne Measurement Program (AAMP) was planned to investigate the transport, exchange and chemical processes of gas and aerosol in the Arctic atmosphere in early spring, and further to understand their roles in global change. An instrumented aircraft, Gulfstream II (G-II) twin-jet plane, was used for airborne measurements in the troposphere and lower stratosphere of the Arctic. For the AAMP 1998 campaign, G-II was equipped with CO_2 and O_3 concentration monitor systems, gas and aerosol sampling systems, aerosol particle counters, and the PMS 1D and 2D airborne particle probes. The aircraft was flown from Alaska, USA to Svalbard, Norway passing over the North Pole, and on the reverse route, in the first half of March 1998. The approximate cruising altitude was 12km for long-range flights. Vertical profiles of gas and aerosol concentrations were obtained over Spitsbergen, Svalbard and Barrow, Alaska. A convective cloud system associated with a polar low was observed over the Norwegian Sea. Another cloud observation was made for marine boundary layer clouds over the open sea off Spitsbergen. Most of the instruments on-board G-II worked well, and measurements were successfully acquired during the AAMP 1998 campaign.

On January 3, 1998, a large balloon (30000 m^3) was successfully launched at Syowa Station for the cryo-sampling of the stratospheric atmosphere. The sampling system splashed down in the Liitzow-Holm Bay and recovered by icebreaker SHIRASE. The cryo-sampling at Antarctica was the first trial in the world and the recovery of a heavy payload was also the first challenge at Syowa Station. A lot of new ballooning technologies were applied to this operation, such as compact balloon launching equipments, a reliable recovery system, a handy ground radio station for the balloon tracking and data acquisition and so forth. The realtime flight data could be received at National Institute of Polar Research (NIPR) in Tokyo by using the computer network via INMARSAT. At NIPR the collaboration members could monitor the entire process of the experiment at Syowa Station in detail and send some instructions and advice. This balloon experiment showed an extended possibility of a large scale scientific ballooning at Syowa Station. This paper deals with those newly developed balloon engineering technologies.

Sampling for atmospheric isoprene and some other volatile organic compounds was conducted during two cruises in the austral summer, covering the western Pacific, eastern Indian Ocean, Southeast Asian Sea, and Southern Ocean. High isoprene levels were observed in the marine air masses over the southern Indian Ocean (up to 280 parts per trillion by volume (pptv)) and over the Southern Ocean (up to 60 pptv), as well as high levels of dimethyl sulfide and bromoform, both of which are mainly emitted by marine biota. It is highly probable that the high phytoplankton activity in the Southern Ocean during the austral summer was responsible for the high oceanic isoprene levels. The findings suggest a possible significant influence of oceanic isoprene on marine atmospheric chemistry.

We estimate the CO2 flux over Tropical Asia in 2009, 2010, and 2011 using Greenhouse Gases Observing Satellite (GOSAT) total column CO2(XCO2) and in situ measurements of CO2. Compared to flux estimates from assimilating surface measurements of CO2, GOSAT XCO2 estimates a more dynamic seasonal cycle and a large source in March–May 2010. The more dynamic seasonal cycle is consistent with earlier work by Patra et al. (2011), and the enhanced 2010 source is supported by independent upper air CO2 measurements from the Comprehensive Observation Network for Trace gases by Airliner (CONTRAIL) project. Using Infrared Atmospheric Sounding Interferometer (IASI) measurements of total column CO (XCO), we show that biomass burning CO2 can explain neither the dynamic seasonal cycle nor the 2010 source. We conclude that both features must come from the terrestrial biosphere. In particular, the 2010 source points to biosphere response to above-average temperatures that year.

About 370 air samples were collected using aircraft in the troposphere over Russia in the summers of 1992, 1993, and 1994. These were then analyzed for the CO2, CH4, N2O and CO concentrations, as well as for δ13C and δ18O of CO2. Measured vertical profiles of tropospheric CO2 showed that the concentration increased with height over all locations. In the lower troposphere over the wetland and taiga regions, extremely low CO2 concentrations of 335–345 parts per million by volume (ppmv) were often observed. Measured values of δ13C and the CO2 concentration were negatively correlated with each other, the rate of change in δ13C with respect to the CO2 concentration being about −0.05‰/ppmv. This implies that the variations in the CO2 concentration observed over Russia in the summer are primarily caused by terrestrial biospheric activities. In the middle and upper troposphere, the CO2 concentration and δ13C showed systematic differences between each other in 1992, 1993, and 1994, probably due to their secular changes. The δ18O and CO2 observed in the lowest part of the troposphere over east and west Siberia were also negatively correlated with each other, with the rate of change in δ18O with respect to CO2 estimated to be about −0.1 l‰/ppmv. This relation may be caused by isotopic equilibrium of oxygen in CO2 with soil water through respiration of living plants and decomposition of organic matter and with chloroplast water in leaves through photosynthesis of living plants. In contrast to CO2, the CH4 concentration decreased with height. Extremely high CH4 concentrations were observed over the west Siberian lowland, owing to a large amount of CH4 emitted from wetlands. The N2O concentrations were fairly constant through the troposphere over all locations covered by this study, with an average value of about 311 parts per billion by volume (ppbv). The CO concentrations also showed vertical profiles, with a small gradient over natural wetlands, taiga, and tundra. High values of the CH4, CO, and CO2 concentrations were observed over Moscow, owing to emissions of the respective gases by human activities in an urban area. It was also found that over natural wetlands and tundra the CO2 and CH4 concentrations were negatively correlated with each other, reflecting a strong biospheric CO2 uptake and CH4 emissions from wetlands. The relationship between the CH4 and CO concentrations was strongly positive over areas with their anthropogenic and natural sources; the relationship was only slightly positive over wetlands, possibly due to CO emissions from wetlands and/or photochemically produced CO.

To reconstruct variations of atmospheric greenhouse gases in the glacial period, air in an ice core recovered from a bare ice field in the southern part of the Yamato Mountains, Antarctica was extracted and then the CO_2,CH_4 and N_2O concentrations and δ^C of CO_2 were analyzed. The CO_2,CH_4 and N_2O concentrations were obviously lower than the pre-industrial Holocene values, suggesting that this ice core was formed in the glacial period. The variations of the CO_2,CH_4 and N_2O concentrations during the glacial period showed a good correlation with that of δ^O of ice from the core. The CO_2 concentrations varied almost opposite in phase with δ^C, which implies that CO_2 with isotopically light carbon was added to or subtracted from the atmosphere in the glacial period.

Air samples collected using aircraft during the Siberian Terrestrial Ecosystem-Atmosphere-Cryosphere Experiments (STEACE) in the summer of 1993 and 1994 were analyzed for the carbon isotopic ratio, δ13C, of atmospheric CH4 as well as for the CH4 concentration. The CH4 concentrations and δ13C values observed in the lower troposphere over wetlands in the West Siberian Lowland varied considerably, showing a clear negative correlation between the two components. From the relationships between measured values of the CH4 concentration and δ13C, values of δ13C of CH4 released from wetlands into the atmosphere were estimated to be −75 to −67‰. The results observed over oil wells and pipelines showed isotopic evidence for leakage of natural gas. Mean values of δ13C measured in the middle and upper troposphere over Siberia in the summer season were −47.9±0.3 and −47.8±0.2‰ for 1993 and 1994, respectively, which are quite similar to each other.

Since July 2007, monthly averages of mid-tropospheric methane have been retrieved in the tropics over land and sea, by day and night, from IASI onboard MetOp-A, yielding a complete view of the geographical distribution, seasonality and long-term tendency of methane in the mid-troposphere. Retrieved methane displays a clear seasonal cycle of ~25 ppbv in the northern tropics, with a maximum in November and a minimum in April–May, a more complex cycle of ~15 ppbv in the southern tropics, and a south-to-north latitudinal variation of ~30 ppbv – in good agreement with regular aircraft measurements of the CONTRAIL program. Comparisons with CARIBIC aircraft measurements made at ~11 km yield an averaged difference between collocated IASI estimates and CARIBIC measurements of 7.2 ppbv with a standard deviation of 13.1 ppbv. Comparisons with aircraft measurements made above 6 km during five HIPPO campaigns give an averaged difference between collocated IASI estimates and HIPPO measurements of 5.1 ppbv with a standard deviation of 16.3 ppbv. These comparisons show that IASI captures well the evolution of mid-tropospheric methane. In particular, in 2007 and 2008, IASI shows an increase of mid-tropospheric methane in the tropical region of 9.5 ± 2.8 and 6.3 ± 1.7 ppbv yr−1, respectively – in excellent agreement with the rate of increase measured at the surface after almost a decade of near-zero growth. IASI also indicates a slowing down of this increase in the following years to ~2 ppbv yr−1, with the highest increase in 2010. Assuming that the recent evolution of methane is mostly due to an increase in surface emissions, IASI might indicate a decrease in tropical wetland emissions for the period 2009–2011 compared to 2007–2008, in agreement with decreasing tropical precipitation over this period, together with an increase in biomass burning emissions in 2010 in the southern tropics.

In order to estimate the concentrations of atmospheric nitrous oxide (N 2 O) during the last 250 years, air samples were extracted from an Antarctic ice core, H15, using a dry extraction system and were then analyzed with a precision of ±2 ppbv. The results obtained were clearly less scattered and much tighter than those of the previous studies. Our data showed that the concentrations of atmospheric N 2 O in the 18th century were about 276 ppbv on average. It was also obvious that the N 2 O concentration began to increase in the mid-19th century and reached approximately 293 ppbv around 1965, the trend of the concentration increase correlating quite well with the direct atmospheric measurements at the South Pole. Such an increase in the atmospheric N 2 O concentration is thought to be of anthropogenic origin.

Stratospheric air samples have been collected once per year since 1985 over Japan using a balloon-borne cryogenic sampler and then analyzed for their CO2 concentrations. The measurements showed high values of CO2 in the lowest part of the stratosphere, then a decrease with height to 20.0–25.0 km, and almost constant values above this level. From the comparison with the results of our aircraft measurements in the upper troposphere and lower stratosphere, it is suggested that the vertical profile of stratospheric CO2 over Japan is strongly related to transport processes that are associated with tropospheric air being introduced into the stratosphere in the tropical region and then moving poleward with different speeds at different heights. The average rate of the CO2 increase from 1985 to 1991 was estimated to be 1.4 ppmv/year; this is similar to the rate found for the troposphere over the same period.

We have been measuring stable isotopic ratios of carbon (delta-C-13) and oxygen (delta-O-18) of carbon dioxide in the stratosphere (18-35 km altitudes) over Japan since 1985, presenting here the first temporal delta-C-13 and delta-O-18 records between 1985 and 1991. The stratospheric delta-C-13 is gradually decreasing due to anthropogenic effects with a rate of approximately -0.03%/y, which is similar to the tropospheric value. The previously found O-18 enrichment is stratospheric CO2 has been maintained almost steadily during the 6 years, with a monotonous delta-O-18 increase with increasing altitude up to 35 km over Japan.

[1] Aircraft measurements of carbon and hydrogen isotopic ratios of atmospheric CH4 (δ13CH4 and δD-CH4), with the respective precisions of 0.08‰ and 2.2‰, as well as CH4 concentration were made at 1 and 2 km altitudes over western Siberia during 2006–2009. δ13CH4 and δD-CH4 were almost always lower at lower altitudes, while the CH4 concentration was higher, implying strong sources on the ground with low isotopic values. δ13CH4 showed a clear seasonal minimum in the late summer, while seasonality of CH4 and δD-CH4 was ambiguous due to the local disturbances. By inspecting the relationships between the CH4 concentration and isotopes, we found that isotopic source signatures in the winter (December–April) are −41.2 ± 1.8 and −187 ± 18‰ for δ13CH4 and δD-CH4, respectively, and the corresponding values in the summer (June–October) are −65.0 ± 2.5 and −282 ± 25‰. These values indicate predominant CH4emissions from fossil fuel facilities in the winter and wetlands in the summer. It was also found that the shorter-term CH4 variations are more influenced by fossil CH4 than that from wetlands. The finding presumably reflects the fact that the former is released from limited areas such as leakage from fossil fuel facilities, while the latter is released from a vast expanse of wetland. By employing a CH4 emission data set used in an atmospheric chemistry transport model, we calculated seasonal isotopic changes of CH4 sources in western Siberia and compared them to the estimates obtained in this study. The results indicated that the seasonal change in the CH4 emission data set is reasonable, at least in terms of a ratio of fossil to biogenic emissions.

[1] We present a data set of atmospheric potential oxygen (APO = O2 + 1.1 × CO2) based on the atmospheric O2/N2 and CO2measurements of flask samples collected at two monitoring stations in Japan and on commercial cargo ships sailing between Japan and U.S./Canada and Australia/New Zealand. Since APO is invariant with respect to the terrestrial biotic exchange, its variation mainly reflects the spatiotemporal distribution in the air-to-sea gas exchange. From the observed APO for the years 2002–2008, we find: (1) elevated annual mean values near the equator, (2) elevated annual mean values and large seasonal amplitudes in the northwestern North Pacific, and (3) a deep trough of low annual mean values at latitudes 20–40°N in the Western Pacific. In addition, latitudinal distributions in the timing of the observed seasonal maximum and minimum show asymmetric patterns across the equator. Comparing these observations with a series of simulated APO generated in the NIES99 atmospheric transport model driven by a set of climatological oceanic O2 and CO2 flux fields, we find a good agreement except for the observed deep trough at the midlatitude. Simulations with different transport mechanisms and fluxes reveal that the seasonal covariation between oceanic O2 flux and atmospheric transport contribute significantly to the observed APO variations in the northern North Pacific; also the seasonal variation in the meridional transport affects the latitudinal difference in the seasonal cycle. The observed latitudinal gradient of the annual mean APO in the Southern Hemisphere is better reproduced by the model based on the recently revised ocean CO2 flux distribution than that based on the previous CO2 flux distribution. The observed APO trough at 36°N in the Western Pacific is about 10 per meg lower than the simulation with the more recent pCO2 data, suggesting the existence of additional APO sinks in that latitudinal region. Indeed, a model simulation performed with an additional ocean O2 sink flux of about 30 Tmol yr−1 within the region (30–50°N, 120–180°E) reproduces considerably well the observed APO trough.

Received 29 May 2012; revised 8 August 2012; accepted 16 August 2012; published 4 October 2012. [1] We investigate the upper tropospheric distribution of methane (CH4) at low latitudes based on the analysis of air samples collected from aboard passenger aircraft. The distribution of CH4 exhibits spatial and seasonal differences, such as the pronounced seasonal cycles over tropical Asia and elevated mixing ratios over central Africa. Over Africa, the correlations of methane, ethane, and acetylene with carbon monoxide indicate that these high mixing ratios originate from biomass burning as well as from biogenic sources. Upper tropospheric mixing ratios of CH4were modeled using a chemistry transport model. The simulation captures the large-scale features of the distributions along different flight routes, but discrepancies occur in some regions. Over Africa, where emissions are not well constrained, the model predicts a too steep interhemispheric gradient. During summer, efficient convective vertical transport and enhanced emissions give rise to a large-scale CH4 maximum in the upper troposphere over subtropical Asia. This seasonal (monsoonal) cycle is analyzed with a tagged tracer simulation. The model confirms that in this region convection links upper tropospheric mixing ratios to regional sources on the Indian subcontinent, subtropical East Asia, and Southeast Asia. This type of aircraft data can therefore provide information about surface fluxes.

In order to use high resolution in-situ measurements to constrain regional emissions of carbon dioxide (CO2), we use a Lagrangian methodology based on diffusive backward trajectory tracer reconstructions. We use aircraft, tall tower and ground sites for CO2 data collected nearby the CO2 emission hot spot of the Tokyo Bay Area during the CONTRAIL campaign, from the MRI/JMA Tsukuba tall tower and from the World Data Centre for Greenhouse Gases (WDCGG). We calculated Bayesian inversions based on EDGAR 4 and CDIAC a priori fluxes. Estimated fluxes for the Tokyo Bay Area for the analyzed period between 2005 and 2009 range between 4.80×10−7 and 3.45×10−6 kgCO2 m2 s−1 with significant time variations. Significant differences in retrieved fluxes of up to 21% were found when CONTRAIL measurements were added to the dataset. No significant trend was found in the time series of spatially averaged retrieved fluxes.

[1] A large number of in situ carbon dioxide (CO2) measurements from 5224 flights were taken by commercial airliners from 2005 to 2010. We analyzed the seasonal cycles in tropospheric CO2 in wide areas of the world over the Eurasian continent, the North Pacific, Southeast Asia, and Oceania. In the Northern Hemisphere, large seasonal changes of CO2 in the upper troposphere are found from spring through summer at northern midlatitudes to high latitudes with significant longitudinal differences; seasonally low CO2 mixing ratios are vertically transported from the surface over the Eurasian continent and then transported eastward to the North Pacific. In the Southern Hemisphere, the CO2 in the upper troposphere increases rapidly from April to June, indicating clearly the interhemispheric transport of high CO2 from the Northern Hemisphere winter. The rapid increase in the upper southern lower latitudes is equivalent to about 0.2 Pg increase in carbon. This interhemispheric transport should be adequately represented in general circulation models for source/sink estimates by inverse methods, because it is comparable to the seasonal or net fluxes estimated for a current inversion area size or a typical subcontinental domain. Estimation for transport of CO2 through the high altitudes will be more important than ever with increasing data from aircraft observations.