Search

MAX-DOAS and direct sun NO2 vertical column network data are used to investigate the accuracy of tropospheric NO2 column measurements of the GOME-2 instrument on the MetOP-A satellite platform and the OMI instrument on Aura. The study is based on 23 MAX-DOAS and 16 direct sun instruments at stations distributed worldwide. A method to quantify and correct for horizontal dilution effects in heterogeneous NO2 field conditions is proposed. After systematic application of this correction to urban sites, satellite measurements are found to present smaller biases compared to ground-based reference data in almost all cases. We investigate the seasonal dependence of the validation results, as well as the impact of using different approaches to select satellite ground pixels in coincidence with ground-based data. In optimal comparison conditions (satellite pixels containing the station) the median bias between satellite tropospheric NO2 column measurements and the ensemble of MAX-DOAS and direct sun measurements is found to be significant and equal to −36 % for GOME-2A and −20 % for OMI. These biases are further reduced to −24 % and −8 % respectively, after application of the dilution correction. Comparisons with the QA4ECV satellite product for both GOME-2A and OMI is also performed, showing less scatter but also a slightly larger median tropospheric NO2 column bias with respect to the ensemble of MAX-DOAS and direct sun measurements.

Constraints from ozone (O3) observations over oceans are needed in addition to those from terrestrial regions to fully understand global tropospheric chemistry and its impact on the climate. Here, we provide a large data set of ozone and carbon monoxide (CO) levels observed (for 11 666 and 10 681 h, respectively) over oceans. The data set is derived from observations made during 24 research cruise legs of R/V Mirai during 2012 to 2017, in the Southern, Indian, Pacific, and Arctic Oceans, covering the region from 67° S to 75° N. The data are suitable for critical evaluation of the over-ocean distribution of ozone derived from chemical transport models. We first give an overview of the statistics in the data set and highlight key features in terms of geographical distribution and air mass type. We then use the data set to evaluate ozone concentration fields from Tropospheric Chemistry Reanalysis version 2 (TCR-2), produced by assimilating a suite of satellite observations of multiple species into a chemical transport model, namely CHASER. For long-range transport of polluted air masses from continents to the oceans, during which the effects of forest fires and fossil fuel combustion were recognized, TCR-2 gave an excellent performance in reproducing the observed temporal variations and photochemical buildup of O3 when assessed from ΔO3 / ΔCO ratios. For clean marine conditions with low and stable CO concentrations, two focused analyses were performed. The first was in the Arctic (> 70° N) in September every year from 2013 to 2016; TCR-2 underpredicted O3 levels by 6.7 ppb (21 %) on average. The observed vertical profiles from O3 soundings from R/V Mirai during September 2014 had less steep vertical gradients at low altitudes (> 850 hPa) than those obtained TCR-2. This suggests the possibilities of more efficient descent of the O3-rich air from above or less efficient dry deposition on the surface than were assumed in the model. In the second analysis, over the western Pacific equatorial region (125–165° E, 10° S to 25° N), the observed O3 level frequently decreased to less than 10 ppb in comparison to that obtained with TCR-2, and also those obtained in most of the Atmospheric Chemistry Climate Model Intercomparison Project (ACCMIP) model runs for the decade from 2000. These results imply loss processes that are unaccounted for in the models. We found that the model’s positive bias positively correlated with the daytime residence times of air masses over a particular grid, namely 165–180° E and 15–30° N; an additional loss rate of 0.25 ppb h−1 in the grid best explained the gap. Halogen chemistry, which is commonly omitted from currently used models, might be active in this region and could have contributed to additional losses. Our open data set covering wide ocean regions is complementary to the Tropospheric Ozone Assessment Report data set, which basically comprises ground-based observations, and enables a fully global study of the behavior of O3.

For the intercomparison of tropospheric nitrogen dioxide (NO2) vertical column density (VCD) data from three different satellite sensors (SCIAMACHY, OMI, and GOME-2), we use a common standard to quantitatively evaluate the biases for the respective data sets. As the standard, a regression analysis using a single set of collocated ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations at several sites in Japan and China from 2006–2011 is adopted. Examinations of various spatial coincidence criteria indicates that the slope of the regression line can be influenced by the spatial distribution of NO2 over the area considered. While the slope varies systematically with the distance between the MAX-DOAS and satellite observation points around Tokyo in Japan, such a systematic dependence is not clearly seen and correlation coefficients are generally higher in comparisons at sites in China. On the basis of these results, we focus mainly on comparisons over China and estimate the biases in SCIAMACHY, OMI, and GOME-2 data (TM4NO2A and DOMINO version 2 products) against the MAX-DOAS observations to be −5 ± 14%, −10 ± 14%, and +1 ± 14%, respectively, which are all small and insignificant. We suggest that these small biases now allow for analyses combining these satellite data for air quality studies, which are more systematic and quantitative than previously possible.

大気球シンポジウム 平成27年度（2015年11月5-6日. 宇宙航空研究開発機構宇宙科学研究所 (JAXA)(ISAS)）, 相模原市, 神奈川県, Balloon Symposium 2015 (November 5-6, 2015. Institute of Space and Astronautical Science, Japan Aerospace Exploration Agency (JAXA)(ISAS)), Sagamihara, Kanagawa Japan, 著者人数: 16名, 資料番号: SA6000044017, レポート番号: isas15-sbs-017

資料番号: AA0046920062

大気球シンポジウム 平成26年度（2014年11月6-7日. 宇宙航空研究開発機構宇宙科学研究所 (JAXA)(ISAS)）, 相模原市, 神奈川県, Balloon Symposium 2014 (November 6-7, 2014. Institute of Space and Astronautical Science, Japan Aerospace Exploration Agency (JAXA)(ISAS)), Sagamihara, Kanagawa Japan, 著者人数: 15名, 資料番号: SA6000021032, レポート番号: isas14-sbs-032

第23回大気圏シンポジウム（2009年2月26日-27日. 宇宙航空研究開発機構宇宙科学研究本部（JAXA)(ISAS)）, 相模原市, 神奈川県, 23rd Atmospheric Science Symposium (February 26-27, 2009. Institute of Space and Astronautical Science, Japan Aerospace Exploration Agency (JAXA)(ISAS)), Sagamihara, Kanagawa Japan, 資料番号: SA6000074005, レポート番号: Ⅰ-5

14 pags., 7 figs., 4 tabs., Iodine compounds destroy ozone (O3) in the global troposphere and form new aerosols, thereby affecting the global radiative balance. However, few reports have described the latitudinal distribution of atmospheric iodine compounds. This work reports iodine monoxide (IO) measurements taken over unprecedented sampling areas from the Arctic to the Southern Hemisphere and spanning sea surface temperatures (SSTs) of approximately 0 to 31.5°C. The highest IO concentrations were observed over the Western Pacific warm pool (WPWP), where O3 minima were also measured. There, a negative correlation was found between O3 and IO mixing ratios at extremely low O3 concentrations. This correlation is not explained readily by the O3-dependent oceanic fluxes of photolabile inorganic iodine compounds, which is the dominant source in recent global-scale chemistry transport models representing iodine chemistry. Actually, the correlation rather implies that O3-independent pathways can be similarly important in the WPWP. The O3-independent fluxes result in a 15% greater O3 loss than that estimated for O3-dependent processes alone. The daily O3 loss rate related to iodine over the WPWP is as high as approximately 2ppbv (parts per billion by volume) despite low O3 concentrations of approximately 10ppbv, with the loss being up to 100% greater than that without iodine. This finding suggests that warming SST driven by climate change might affect the marine atmospheric chemical balance through iodine-ozone chemistry. Copyright, This study was supported by the KAKENHI (grant nos. 16KK0017 and 21H04933), and by the ArCS (Arctic Challenge for Sustainability; grant no. JPMXD1300000000) of the Ministry of Education, Culture, Sports, Science, and Technology of Japan. This study has also received funding from the European Research Council Executive Agency under the European Union’s Horizon 2020 Research and Innovation programme (grant no. ERC2016-COG 726349; CLIMAHAL). This study was also supported, in part, by funding from Fukuoka University (grant no. 197103).