Search

Global multiconstituent concentration and emission fields obtained from the assimilation of the satellite retrievals of ozone, CO, NO2, HNO3, and SO2 from the Ozone Monitoring Instrument (OMI), Global Ozone Monitoring Experiment 2, Measurements of Pollution in the Troposphere, Microwave Limb Sounder, and Atmospheric Infrared Sounder (AIRS)/OMI are used to understand the processes controlling air pollution during the Korea‐United States Air Quality (KORUS‐AQ) campaign. Estimated emissions in South Korea were 0.42 Tg N for NOx and 1.1 Tg CO for CO, which were 40% and 83% higher, respectively, than the a priori bottom‐up inventories, and increased mean ozone concentration by up to 7.5 ± 1.6 ppbv. The observed boundary layer ozone exceeded 90 ppbv over Seoul under stagnant phases, whereas it was approximately 60 ppbv during dynamical conditions given equivalent emissions. Chemical reanalysis showed that mean ozone concentration was persistently higher over Seoul (75.10 ± 7.6 ppbv) than the broader KORUS‐AQ domain (70.5 ± 9.2 ppbv) at 700 hPa. Large bias reductions (>75%) in the free tropospheric OH show that multiple‐species assimilation is critical for balanced tropospheric chemistry analysis and emissions. The assimilation performance was dependent on the particular phase. While the evaluation of data assimilation fields shows an improved agreement with aircraft measurements in ozone (to less than 5 ppbv biases), CO, NO2, SO2, PAN, and OH profiles, lower tropospheric ozone analysis error was largest at stagnant conditions, whereas the model errors were mostly removed by data assimilation under dynamic weather conditions. Assimilation of new AIRS/OMI ozone profiles allowed for additional error reductions, especially under dynamic weather conditions. Our results show the important balance of dynamics and emissions both on pollution and the chemical assimilation system performance. Plain Language Summary: Global multi‐constituent concentration and emission fields obtained from the assimilation of the satellite retrievals are used to understand the processes controlling air pollution during the Korea U.S.‐Air Quality (KORUS‐AQ) campaign. Our results show the important balance of dynamics and emissions both on pollution and the chemical assimilation system performance. Key Points: Multiconstituent data assimilation during KORUS‐AQ showed that emissions in South Korea were 0.42 Tg N for NOx and 1.1 Tg CO for COThese emissions were 40% and 83% higher, respectively, than the a priori bottom‐up inventories and increased ozone by up to 7.5 ± 1.6 ppbvMean ozone concentration was persistently higher over Seoul (75.1 ± 7.6 ppbv) than the broader KORUS‐AQ domain (70.5 ± 9.2 ppbv) at 700 hPa [ABSTRACT FROM AUTHOR]

Abstract: In the Southern Hemisphere and tropics, the main contribution to carbon monoxide (CO) variability is from fire emissions, which are connected to climate through the availability, type, and dryness of fuel. Here we assess the data‐driven relationships between CO and climate, aiming to predict atmospheric loading during fire seasons. Observations of total column CO from the Measurements Of Pollution In The Troposphere satellite instrument are used to build a record of monthly anomalies between 2001 and 2016, focusing on seven biomass burning regions of the Southern Hemisphere and tropics. With the exception of 2015, the range of absolute variability in CO is similar between regions. We model CO anomalies in each of the regions using climate indices for the climate modes: El Niño–Southern Oscillation, Indian Ocean Dipole, Tropical South Atlantic, and Antarctic Oscillation. Stepwise forward and backward variable selection is used to choose from statistical regression models that use combinations of climate indices, at lag times between 1 and 8 months relative to CO anomalies. The Bayesian information criterion selects models with the best predictive power. We find that all climate mode indices are required to model CO in each region, generally explaining over 50% of the variability and over 70% for tropical regions. First‐order interaction terms of the climate modes are necessary, producing greatly improved explanation of CO variability over single terms. Predictive capability is assessed for the Maritime Southeast Asia and the predicted peak CO anomaly in 2015 is within 20% of the measurements. [ABSTRACT FROM AUTHOR]

Using observations from aircraft, surface stations and a satellite instrument, we comprehensively evaluate multi-model simulations of carbon monoxide (CO) and ozone (O3) in the Arctic and over lower latitude emission regions, as part of the POLARCAT Model Intercomparison Project (POLMIP). Evaluation of 11-atmospheric models with chemistry shows that they generally underestimate CO throughout the Arctic troposphere, with the largest biases found during winter and spring. Negative CO biases are also found throughout the Northern Hemisphere, with multi-model mean gross errors (9-12%) suggesting models perform similarly over Asia, North America and Europe. A multi-model annual mean tropospheric OH (10.8 ± 0.6 × 105 molec cm-3) is found to be slightly higher than previous estimates of OH constrained by methyl chloroform, suggesting negative CO biases in models may be improved through better constraints on OH. Models that have lower Arctic OH do not always show a substantial improvement in their negative CO biases, suggesting that Arctic OH is not the dominant factor controlling the Arctic CO burden in these models. In addition to these general biases, models do not capture the magnitude of CO enhancements observed in the Arctic free troposphere in summer, suggesting model errors in the simulation of plumes that are transported from anthropogenic and biomass burning sources at lower latitudes. O3 in the Arctic is also generally underestimated, particularly at the surface and in the upper troposphere. Summer O3 comparisons over lower latitudes show several models overestimate upper tropospheric concentrations. Simulated CO, O3 and OH all demonstrate a substantial degree of inter-model variability. Idealised CO-like tracers are used to quantitatively compare the impact of inter-model differences in transport and OH on CO in the Arctic troposphere. The tracers show that model differences in transport from Europe in winter and from Asia throughout the year are important sources of model variability at Barrow. Unlike transport, inter-model variability in OH similarly affects all regional tracers at Barrow. Comparisons of fixed-lifetime and OH-loss idealised CO-like tracers throughout the Arctic troposphere show that OH differences are a much larger source of inter-model variability than transport differences. Model OH concentrations are correlated with H2O concentrations, suggesting water vapour concentrations are linked to differences in simulated concentrations of CO and OH at high latitudes in these simulations. Despite inter-model differences in transport and OH, the relative contributions from the different source regions (North America, Europe and Asia) and different source types (anthropogenic and biomass burning) are comparable across the models. Fire emissions from the boreal regions in 2008 contribute 33, 43 and 19 % to the total Arctic CO-like tracer in spring, summer and autumn, respectively, highlighting the importance of boreal fire emissions in controlling pollutant burdens in the Arctic. [ABSTRACT FROM AUTHOR]

We investigate Arctic tropospheric composition using ground-based Fourier transform infrared (FTIR) solar absorption spectra, recorded at the Polar Environment Atmospheric Research Laboratory (PEARL, Eureka, Nunavut, Canada, 80°05' N, 86°42' W) and at Thule (Greenland, 76°53' N, -68°74' W) from 2008 to 2012. The target species, carbon monoxide (CO), hydrogen cyanide (HCN), ethane (C2H6), acetylene (C2H2), formic acid (HCOOH), and formaldehyde (H2CO) are emitted by biomass burning and can be transported from mid-latitudes to the Arctic. By detecting simultaneous enhancements of three biomass burning tracers (HCN, CO, and C2H6), ten and eight fire events are identified at Eureka and Thule, respectively, within the 5-year FTIR time series. Analyses of Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model back-trajectories coupled with Moderate Resolution Imaging Spectroradiometer (MODIS) fire hotspot data, Stochastic Time-Inverted Lagrangian Transport (STILT) model footprints, and Ozone Monitoring Instrument (OMI) UV aerosol index maps, are used to attribute burning source regions and travel time durations of the plumes. By taking into account the effect of aging of the smoke plumes, measured FTIR enhancement ratios were corrected to obtain emission ratios and equivalent emission factors. The means of emission factors for extratropical forest estimated with the two FTIR data sets are 0.40 ± 0.21 g kg-1 for HCN, 1.24 ± 0.71 g kg-1 for C2H6, 0.34 ± 0.21 g kg-1 for C2H2, and 2.92 ± 1.30 g kg-1 for HCOOH. The emission factor for CH3OH estimated at Eureka is 3.44 ± 1.68 g kg-1. To improve our knowledge concerning the dynamical and chemical processes associated with Arctic pollution from fires, the two sets of FTIR measurements were compared to the Model for OZone And Related chemical Tracers, version 4 (MOZART-4). Seasonal cycles and day-to-day variabilities were compared to assess the ability of the model to reproduce emissions from fires and their transport. Good agreement in winter confirms that transport is well implemented in the model. For C2H6, however, the lower wintertime concentration estimated by the model as compared to the FTIR observations highlights an underestimation of its emission. Results show that modeled and measured total columns are correlated (linear correlation coefficient r > 0.6 for all gases except for H2CO at Eureka and HCOOH at Thule), but suggest a general underestimation of the concentrations in the model for all seven tropospheric species in the high Arctic. [ABSTRACT FROM AUTHOR]

The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. Both configurations are well suited as tools for atmospheric-chemistry modeling studies in the troposphere and lower stratosphere, whether with internally derived "free running" (FR) meteorology, or "specified dynamics" (SD). The main focus of this paper is to compare the performance of these configurations against observations from surface, aircraft, and satellite, as well as understand the origin of the identified differences. We partic ularly focus on comparing present-day methane lifetime estimates within the different model configurations, which range between 7.8 years in the SD configuration of CAM5- chem and 8.8 years in the FR configuration of CAM4-chem. We find that tropospheric surface area density is an important factor in controlling the burden of the hydroxyl radical (OH), which causes differences in tropical methane lifetime of about half a year between CAM4-chem and CAM5-chem. In addition, different distributions of nitrogen oxides (NOx) produced from lightning production explain about half of the difference between SD and FR model versions in both CAM4-chem and CAM5-chem. Remaining differences in the tropical OH burden are due to enhanced tropical ozone burden in SD configurations compared to the FR versions, which are not only caused by differences in chemical production or loss, but also by transport and mixing. For future studies, we recommend the use of CAM5-chem, due to improved aerosol description and inclusion of aerosol-cloud interactions. However, smaller tropospheric surface area density in the current version of CAM5-chem compared to CAM4-chem results in larger oxidizing capacity in the troposphere and therefore a shorter methane lifetime. [ABSTRACT FROM AUTHOR]

Observations of a comprehensive suite of inorganic and organic trace gases, including non-methane hydrocarbons (NMHCs), halogenated organics and oxygenated volatile organic compounds (OVOCs), obtained from the NASA DC-8 over Canada during the ARCTAS aircraft campaign in July 2008 illustrate that convection is important for redistributing both long- and short-lived species throughout the troposphere. Convective outflow events were identified by the elevated mixing ratios of organic species in the upper troposphere relative to background conditions. Several dramatic events were observed in which isoprene and its oxidation products were detected at hundreds of pptv at altitudes higher than 8 km. Two events are studied in detail using detailed experimental data and the NASA Langley Research Center (LaRC) box model. One event had no lightning NOx (NO + NO2) associated with it and the other had substantial lightning NOx (LNOx >1 ppbv). When convective storms transport isoprene from the boundary layer to the upper troposphere and no LNOx is present, OH is reduced due to scavenging by isoprene, which serves to slow the chemistry, resulting in longer lifetimes for species that react with OH. Ozone and PAN production is minimal in this case. In the case where isoprene is convected and LNOx is present, there is a large effect on the expected ensuing chemistry: isoprene exerts a dominant impact on HOx and nitrogen-containing species; the relative contribution from other species to HOx, such as peroxides, is insignificant. The isoprene reacts quickly, resulting in primary and secondary products, including formaldehyde and methyl glyoxal. The model predicts enhanced production of alkyl nitrates (ANs) and peroxyacyl nitrate compounds (PANs). PANs persist because of the cold temperatures of the upper troposphere resulting in a large change in the NOx mixing ratios which, in turn, has a large impact on the HO chemistry. Ozone production is substantial during the first few hours following the convection to the UT, resulting in a net gain of approximately 10 ppbv compared to the modeled scenario in which LNOx is present but no isoprene is present aloft. [ABSTRACT FROM AUTHOR]

The NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission was conducted in two 3-week deployments based in Alaska (April 2008) and western Canada (June-July 2008). Its goal was to better understand the factors driving current changes in Arctic atmospheric composition and climate, including (1) influx of mid-latitude pollution, (2) boreal forest fires, (3) aerosol radiative forcing, and (4) chemical processes. The June-July deployment was preceded by one week of flights over California (ARCTAS-CARB) focused on (1) improving state emission inventories for greenhouse gases and aerosols, (2) providing observations to test and improve models of ozone and aerosol pollution. ARCTAS involved three aircraft: a DC-8 with a detailed chemical payload, a P-3 with an extensive aerosol and radiometric payload, and a B-200 with aerosol remote sensing instrumentation. The aircraft data augmented satellite observations of Arctic atmospheric composition, in particular from the NASA A-Train. The spring phase (ARCTAS-A) revealed pervasive Asian pollution throughout the Arctic as well as significant European pollution below 2 km. Unusually large Siberian fires in April 2008 caused high concentrations of carbonaceous aerosols and also affected ozone. Satellite observations of BrO column hotspots were found not to be related to Arctic boundary layer events but instead to tropopause depressions, suggesting the presence of elevated inorganic bromine (5-10 pptv) in the lower stratosphere. Fresh fire plumes from Canada and California sampled during the summer phase (ARCTAS-B) indicated low NOx emission factors from the fires, rapid conversion of NOx to PAN, no significant secondary aerosol production, and no significant ozone enhancements except when mixed with urban pollution. [ABSTRACT FROM AUTHOR]

The article describes and evaluates the Model for Zone and Related chemical Tracers, version 4 (MOZART-4). It says that the MOZART-4 is an offline worldwide chemical transport model specifically fitted for researches of the troposphere. It also describes the updates of MOZART-4 from its last version MOZART-2, which include online calculations of several processes, such as emissions of isoprene and monoterpenes, dry deposition, and photolysis frequencies are also included in the model.

Comparisons of aircraft measurements of carbon monoxide (CO) to the retrievals of CO using observations from the Measurements of Pollution in The Troposphere (MOPITT) instrument onboard the Terra satellite are presented. Observations made as part of the NASA INTEX-B and NSF MIRAGE field campaigns during March-May 2006 are used to validate the MOPITT CO retrievals, along with routine samples from 2001 through 2006 from NOAA and the MOZAIC measurements from commercial aircraft. A significant positive bias, around 20% for total column CO, in MOPITT CO was found in the comparison to in situ measurements during 2006. Comparisons to the long-term records of measurements from NOAA and MOZAIC revealed an increasing bias in the V3 MOPITT CO retrievals over time. The impact of an instrumental drift is illustrated through retrieval simulations. [ABSTRACT FROM AUTHOR]

We present a global chemical data assimilation system using a global atmosphere model, the Community Atmosphere Model (CAM3) with simplified chemistry and the Data Assimilation Research Testbed (DART) assimilation package. DART is a community software facility for assimilation studies using the ensemble Kalman filter approach. Here, we apply the assimilation system to constrain global tropospheric carbon monoxide (CO) by assimilating meteorological observations of temperature and horizontal wind velocity and satellite CO retrievals from the Measurement of Pollution in the Troposphere (MOPITT) satellite instrument. We verify the system performance using independent CO observations taken on board the NSF/NCAR C-130 and NASA DC-8 aircrafts during the April 2006 part of the Intercontinental Chemical Transport Experiment (INTEX-B). Our evaluations show that MOPITT data assimilation provides significant improvements in terms of capturing the observed CO variability relative to no MOPITT assimilation (i.e. the correlation improves from 0.62 to 0.71, significant at 99% confidence). The assimilation provides evidence of median CO loading of about 150 ppbv at 700 hPa over the NE Pacific during April 2006. This is marginally higher than the modeled CO with no MOPITT assimilation (~140 ppbv). Our ensemble-based estimates of model uncertainty also show model overprediction over the source region (i.e. China) and underprediction over the NE Pacific, suggesting model errors that cannot be readily explained by emissions alone. These results have important implications for improving regional chemical forecasts and for inverse modeling of CO sources and further demonstrate the utility of the assimilation system in comparing non-coincident measurements, e.g. comparing satellite retrievals of CO with in-situ aircraft measurements. [ABSTRACT FROM AUTHOR]