Intercontinental Chemical Transport Experiment Research Articles

Development of the CREATE Inventory in Support of Integrated Climate and Air Quality Modeling for Asia

A bottom-up emissions inventory is one of the most important data sets needed to understand air quality (AQ) and climate change (CC). Several emission inventories have been developed for Asia, including Transport and Chemical Evolution over the Pacific (TRACE-P), Regional Emission Inventory in Asia (REAS), and Inter-Continental Chemical Transport Experiment (INTEX) and, while these have been used successfully for many international studies, they have limitations including restricted amounts of information on pollutant types and low levels of transparency with respect to the polluting sectors or fuel types involved. To address these shortcomings, we developed: (1) a base-year, bottom-up anthropogenic emissions inventory for Asia, using the most current parameters and international frameworks (i.e., the Greenhouse gas—Air pollution INteractions and Synergies (GAINS) model); and (2) a base-year, natural emissions inventory for biogenic and biomass burning. For (1), we focused mainly on China, South Korea, and Japan; however, we also covered emission inventories for other regions in Asia using data covering recent energy/industry statistics, emission factors, and control technology penetration. The emissions inventory (Comprehensive Regional Emissions inventory for Atmospheric Transport Experiment (CREATE)) covers 54 fuel classes, 201 subsectors, and 13 pollutants, namely SO2, NOx, CO, non-methane volatile organic compounds (NMVOC), NH3, OC, BC, PM10, PM2.5, CO2, CH4, N2O, and Hg. For the base-year natural emissions inventory, the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and BlueSky-Asia frameworks were used to estimate biogenic and biomass burning emissions, respectively. Since the CREATE emission inventory was designed/developed using international climate change/air quality (CC/AQ) assessment frameworks, such as GAINS, and has been fully connected with the most comprehensive emissions modeling systems—such as the US Environmental Protection Agency (EPA) Chemical Manufacturing Area Source (CMAS) system—it can be used to support various climate and AQ integrated modeling studies, both now and in the future.

Simulation analysis of atmospheric SO2 contributions from different regions in China

Sulfur dioxide (SO2) is an atmospheric pollution source that poses a threat to the environment and human health. Investigating atmospheric SO2 contributions between different regions will help to reduce SO2 emissions and control pollution. Using the weather research and forecasting (WRF) model and the community multiscale air quality (CMAQ) modeling system, as well as the intercontinental chemical transport experiment phase B (INTEX-B) data, we analyzed the regional contributions of atmospheric SO2 in China. The results showed that SO2 contributions varied significantly between regions and seasons. The atmospheric SO2 levels in Central China (CTR) originated mostly from self-emissions, accounting for as much as 60% of the total emissions in January and April and up to 85% in July and October. The SO2 concentrations in Northeast China (NE) were mainly affected by emissions from CTR, especially in January (39.53%). SO2 concentrations in Northwest China (NW) were mainly affected by external emissions, which exceeded half of the SO2 in this region. SO2 concentrations in Southwest China (SW) were dominated by self-emissions, which accounted for more than 90% of the total SO2. In terms of seasons, SO2 concentrations were significantly affected by external emissions in January and April and were dominated by self-emissions in July and October. Coal use, population, area, and thermal power were found to have the greatest impacts on SO2 concentrations. Among these, coal consumption had the biggest impact on the national SO2 concentration.

Global sensitivity analysis of GEOS-Chem modeled ozone and hydrogen oxides during the INTEX campaigns

Abstract. Making sense of modeled atmospheric composition requires not only comparison to in situ measurements but also knowing and quantifying the sensitivity of the model to its input factors. Using a global sensitivity method involving the simultaneous perturbation of many chemical transport model input factors, we find the model uncertainty for ozone (O3), hydroxyl radical (OH), and hydroperoxyl radical (HO2) mixing ratios, and apportion this uncertainty to specific model inputs for the DC-8 flight tracks corresponding to the NASA Intercontinental Chemical Transport Experiment (INTEX) campaigns of 2004 and 2006. In general, when uncertainties in modeled and measured quantities are accounted for, we find agreement between modeled and measured oxidant mixing ratios with the exception of ozone during the Houston flights of the INTEX-B campaign and HO2 for the flights over the northernmost Pacific Ocean during INTEX-B. For ozone and OH, modeled mixing ratios were most sensitive to a bevy of emissions, notably lightning NOx, various surface NOx sources, and isoprene. HO2 mixing ratios were most sensitive to CO and isoprene emissions as well as the aerosol uptake of HO2. With ozone and OH being generally overpredicted by the model, we find better agreement between modeled and measured vertical profiles when reducing NOx emissions from surface as well as lightning sources.

Seasonal ozone vertical profiles over North America using the AQMEII3 group of air quality models: model inter-comparison and stratospheric intrusions.

This study evaluates simulated vertical ozone profiles produced in the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII3) against ozonesonde observations in North America for the year 2010. Four research groups from the United States (US) and Europe have provided modeled ozone vertical profiles to conduct this analysis. Because some of the modeling systems differ in their meteorological drivers, wind speed and temperature are also included in the analysis. In addition to the seasonal ozone profile evaluation for 2010, we also analyze chemically inert tracers designed to track the influence of lateral boundary conditions on simulated ozone profiles within the modeling domain. Finally, cases of stratospheric ozone intrusions during May–June 2010 are investigated by analyzing ozonesonde measurements and the corresponding model simulations at Intercontinental Chemical Transport Experiment Ozonesonde Network Study (IONS) experiment sites in the western United States. The evaluation of the seasonal ozone profiles reveals that, at a majority of the stations, ozone mixing ratios are underestimated in the 1–6 km range. The seasonal change noted in the errors follows the one seen in the variance of ozone mixing ratios, with the majority of the models exhibiting less variability than the observations. The analysis of chemically inert tracers highlights the importance of lateral boundary conditions up to 250 hPa for the lower-tropospheric ozone mixing ratios (0–2 km). Finally, for the stratospheric intrusions, the models are generally able to reproduce the location and timing of most intrusions but underestimate the magnitude of the maximum mixing ratios in the 2–6 km range and overestimate ozone up to the first kilometer possibly due to marine air influences that are not accurately described by the models. The choice of meteorological driver appears to be a greater predictor of model skill in this altitude range than the choice of air quality model.

WRF-Chem simulated surface ozone over south Asia during the pre-monsoon: effects of emission inventories and chemical mechanisms

Abstract. We evaluate numerical simulations of surface ozone mixing ratios over the south Asian region during the pre-monsoon season, employing three different emission inventories in the Weather Research and Forecasting model with Chemistry (WRF-Chem) with the second-generation Regional Acid Deposition Model (RADM2) chemical mechanism: the Emissions Database for Global Atmospheric Research – Hemispheric Transport of Air Pollution (EDGAR-HTAP), the Intercontinental Chemical Transport Experiment phase B (INTEX-B) and the Southeast Asia Composition, Cloud, Climate Coupling Regional Study (SEAC4RS). Evaluation of diurnal variability in modelled ozone compared to observational data from 15 monitoring stations across south Asia shows the model ability to reproduce the clean, rural and polluted urban conditions over this region. In contrast to the diurnal average, the modelled ozone mixing ratios during noontime, i.e. hours of intense photochemistry (11:30–16:30 IST – Indian Standard Time – UTC +5:30), are found to differ among the three inventories. This suggests that evaluations of the modelled ozone limited to 24 h average are insufficient to assess uncertainties associated with ozone buildup. HTAP generally shows 10–30 ppbv higher noontime ozone mixing ratios than SEAC4RS and INTEX-B, especially over the north-west Indo-Gangetic Plain (IGP), central India and southern India. The HTAP simulation repeated with the alternative Model for Ozone and Related Chemical Tracers (MOZART) chemical mechanism showed even more strongly enhanced surface ozone mixing ratios due to vertical mixing of enhanced ozone that has been produced aloft. Our study indicates the need to also evaluate the O3 precursors across a network of stations and the development of high-resolution regional inventories for the anthropogenic emissions over south Asia accounting for year-to-year changes to further reduce uncertainties in modelled ozone over this region.

Influence of Different Foreign Emissions Inventories on Simulated, Ground-Level Ozone in the Seoul Metropolitan Area during May 2014

ABSTRACTThis study examines the effects of different foreign anthropogenic emissions inventories on predicted ozone concentrations in the Seoul Metropolitan Area (SMA), South Korea, and estimates changes in ozone due to emissions reductions. We ran the Community Multi-Scale Air Quality (CMAQ) model using the High-Order Decoupled Direct Method with three inventories of foreign anthropogenic emissions: (1) the Intercontinental Chemical Transport Experiment, Phase B (INTEX-B) 2006; (2) the Comprehensive Regional Emissions inventory for Atmospheric Transport Experiment (CREATE) 2010; and (3) the Model Inter-Comparison Study (MICS)-Asia 2010. All three inventories have different spatial distributions of emissions, yielding different modeled ozone concentrations. However, the ozone concentrations modeled for the SMA differ less than those modeled for large, foreign cities in the modeling domain. The simulations using INTEX-B 2006 and CREATE 2010 suggested greater reduction in ozone with NOx control than with VOCs control. All simulations show that (1) simultaneous reduction in NOx and VOCs leads to less ozone reduction than the sum of ozone reductions for individual NOx and VOCs controls and (2) ozone reductions are stronger for high ozone days than for low ozone days. Comparing the modeled reductions in the relative sense yields smaller differences between high and low ozone days than comparing the modeled reductions in the absolute sense. With a 20% reduction in only NOx emissions, the differences in MDA1O3 among the three inventories were between 0.3 and 0.7 ppb. Because air-quality planning often leads to defined tonnage reductions, we examined the model’s response to such a defined emissions reduction. Using the NOx reduction in China estimated by Zhao et al. (2013), we estimated that the differences in MDA1O3 among the three inventories were between 1.50 and 1.78 ppb. Based on these results, we recommend using different foreign anthropogenic emissions inventories to test future scenarios for air-quality control

Human-model hybrid Korean air quality forecasting system

ABSTRACTThe Korean national air quality forecasting system, consisting of the Weather Research and Forecasting, the Sparse Matrix Operator Kernel Emissions, and the Community Modeling and Analysis (CMAQ), commenced from August 31, 2013 with target pollutants of particulate matters (PM) and ozone. Factors contributing to PM forecasting accuracy include CMAQ inputs of meteorological field and emissions, forecasters’ capacity, and inherent CMAQ limit. Four numerical experiments were conducted including two global meteorological inputs from the Global Forecast System (GFS) and the Unified Model (UM), two emissions from the Model Intercomparison Study Asia (MICS-Asia) and the Intercontinental Chemical Transport Experiment (INTEX-B) for the Northeast Asia with Clear Air Policy Support System (CAPSS) for South Korea, and data assimilation of the Monitoring Atmospheric Composition and Climate (MACC). Significant PM underpredictions by using both emissions were found for PM mass and major components (sulfate and organic carbon). CMAQ predicts PM2.5 much better than PM10 (NMB of PM2.5: -20~-25%, PM10: -43~-47%). Forecasters’ error usually occurred at the next day of high PM event. Once CMAQ fails to predict high PM event the day before, forecasters are likely to dismiss the model predictions on the next day which turns out to be true. The best combination of CMAQ inputs is the set of UM global meteorological field, MICS-Asia and CAPSS 2010 emissions with the NMB of -12.3%, the RMSE of 16.6μ/m3 and the R2 of 0.68. By using MACC data as an initial and boundary condition, the performance skill of CMAQ would be improved, especially in the case of undefined coarse emission. A variety of methods such as ensemble and data assimilation are considered to improve further the accuracy of air quality forecasting, especially for high PM events to be comparable to for all cases.Implications: The growing utilization of the air quality forecast induced the public strongly to demand that the accuracy of the national forecasting be improved. In this study, we investigated the problems in the current forecasting as well as various alternatives to solve the problems. Such efforts to improve the accuracy of the forecast are expected to contribute to the protection of public health by increasing the availability of the forecast system.

Aerosol-cloud associations over Gangetic Basin during a typical monsoon depression event using WRF-Chem simulation

To study aerosol-cloud interactions over the Gangetic Basin of India, the Weather Research and Forecasting model coupled with chemistry (WRF-Chem) has been applied to a typical monsoon depression event prevalent between the 23 and 29 August 2009. This event was sampled during the Cloud Aerosol Interaction and Precipitation Enhancement EXperiment (CAIPEEX) aircraft campaign, providing measurements of aerosol and cloud microphysical properties from two sorties. Comparison of the simulated meteorological, thermodynamical, and aerosol fields against satellite and in situ aircraft measurements illustrated that the westward propagation of the monsoon depression and the cloud, aerosol, and rainfall spatial distribution was simulated reasonably well using anthropogenic emission rates from Monitoring Atmospheric Composition and Climate project along with cityZEN projects (MACCity)+Intercontinental Chemical Transport Experiment Phase B anthropogenic emission rates. However,the magnitude of aerosol optical depth was underestimated by up to 50%. A simulation with aerosol emissions increased by a factor of 6 over the CAIPEEX campaign domain increased the simulated aerosol concentrations to values close to the observations, mainly within boundary layer. Comparison of the low-aerosol simulation and high-aerosol simulation for the two sorties illustrated that more anthropogenic aerosols increased the cloud condensing nuclei (CCN) and cloud droplet mass concentrations. The number of simulated cloud droplets increased while the cloud droplet effective radii decreased, highlighting the importance of CCN-cloud feedbacks over this region. The increase in simulated anthropogenic aerosols (including absorbing aerosols) also increased the temperature of air parcels below clouds and thus the convective available potential energy (CAPE). The increase in CAPE intensified the updraft and invigorated the cloud, inducing formation of deeper clouds with more ice-phase hydrometeors for both cases. These case studies provide evidence of aerosol-induced cloud invigoration over the Gangetic Basin.

Uncertainties in anthropogenic aerosol concentrations and direct radiative forcing induced by emission inventories in eastern China

This study quantified the uncertainties in concentrations and direct radiative forcing of anthropogenic aerosols due to emissions in eastern China using a global chemistry–aerosol–climate model. The emission inventories included three global inventories, ACCMIP (Atmospheric Chemistry & Climate Model Intercomparison Project), EDGAR-HTAP (Emission Database for Global Atmospheric Research for Hemispheric Transport of Air Pollution), and EDGAR Version 4.2, and one regional INTEX-B (Intercontinental Chemical Transport Experiment—Phase B) inventory. The uncertainties (a percentage of the standard deviation divided by the mean value across the four inventories) in the regional surface-layer aerosol concentrations due to emissions were 3.9% in sulfate, 40.0% in nitrate, 18.4% in ammonium, 11.1% in POA, 16.7% in SOA and 15.4% in BC. Compared with the ACCMIP model results based on a uniform emission inventory, the impacts of emissions were smaller. One exception is the regional surface-layer nitrate concentration, which had comparable uncertainties due to the emissions (40.0%) and the models (43.8%) because of the complex nitrate chemistry and the highly uncertain NH3 emission. The mean regional aerosol direct forcing at the top of the atmosphere between 1850 and 2006 was −3.6Wm−2 under all-sky conditions and was enhanced up to −3.83Wm−2 after the model assimilated the MODIS find-mode aerosol optical depth (AOD). The impact of the assimilation of absorption AOD is discussed. The uncertainties in aerosol direct forcing were smaller than those of the ACCMIP inter-model results, but still significant. An accurate emission inventory is essential for quantifying the role of aerosols in regional climate.

Evaluation of updated nitric acid chemistry on ozone precursors and radiative effects

Abstract. This study shows that revising the reaction rate of NO2 + HO· → HNO3 improves simulated nitrogen partitioning and changes the simulated radiative effects of several short-lived climate forcers (SLCF). Both laboratory and field study analyses have found that the reaction rate should be reduced by 13–30% from current recommendations. We evaluate the GEOS-Chem model over North America with and without the recommended update using observations from the Intercontinental Chemical Transport Experiment – North America (INTEX-NA) Phase A campaign. Revising the NO2 + HO· → HNO3 rate coefficient improves model performance of oxidized nitrogen partitioning by increasing NOx concentrations in the upper troposphere and decreasing HNO3 throughout the troposphere. The increase in NOx concentrations has a corresponding global increase in O3 concentrations and local increases in sulfate aerosols, causing a perturbation in simulated radiative effects. These findings demonstrate the positive influence the mechanism update has on the partitioning of oxidized nitrogen species, the benefits it provides when compared to aircraft observations, and the simulated radiative effects that the reduction induces.

First estimates of global free-tropospheric NO<sub>2</sub> abundances derived using a cloud-slicing technique applied to satellite observations from the Aura Ozone Monitoring Instrument (OMI)

Abstract. We derive free-tropospheric NO2 volume mixing ratios (VMRs) by applying a cloud-slicing technique to data from the Ozone Monitoring Instrument (OMI) on the Aura satellite. In the cloud-slicing approach, the slope of the above-cloud NO2 column versus the cloud scene pressure is proportional to the NO2 VMR. In this work, we use a sample of nearby OMI pixel data from a single orbit for the linear fit. The OMI data include cloud scene pressures from the rotational-Raman algorithm and above-cloud NO2 vertical column density (VCD) (defined as the NO2 column from the cloud scene pressure to the top of the atmosphere) from a differential optical absorption spectroscopy (DOAS) algorithm. We compare OMI-derived NO2 VMRs with in situ aircraft profiles measured during the NASA Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign in 2006. The agreement is generally within the estimated uncertainties when appropriate data screening is applied. We then derive a global seasonal climatology of free-tropospheric NO2 VMR in cloudy conditions. Enhanced NO2 in the free troposphere commonly appears near polluted urban locations where NO2 produced in the boundary layer may be transported vertically out of the boundary layer and then horizontally away from the source. Signatures of lightning NO2 are also shown throughout low and middle latitude regions in summer months. A profile analysis of our cloud-slicing data indicates signatures of lightning-generated NO2 in the upper troposphere. Comparison of the climatology with simulations from the global modeling initiative (GMI) for cloudy conditions (cloud optical depth > 10) shows similarities in the spatial patterns of continental pollution outflow. However, there are also some differences in the seasonal variation of free-tropospheric NO2 VMRs near highly populated regions and in areas affected by lightning-generated NOx.

Global carbon monoxide products from combined AIRS, TES and MLS measurements on A-train satellites

Abstract. This study tests a novel methodology to add value to satellite data sets. This methodology, data fusion, is similar to data assimilation, except that the background model-based field is replaced by a satellite data set, in this case AIRS (Atmospheric Infrared Sounder) carbon monoxide (CO) measurements. The observational information comes from CO measurements with lower spatial coverage than AIRS, namely, from TES (Tropospheric Emission Spectrometer) and MLS (Microwave Limb Sounder). We show that combining these data sets with data fusion uses the higher spectral resolution of TES to extend AIRS CO observational sensitivity to the lower troposphere, a region especially important for air quality studies. We also show that combined CO measurements from AIRS and MLS provide enhanced information in the UTLS (upper troposphere/lower stratosphere) region compared to each product individually. The combined AIRS–TES and AIRS–MLS CO products are validated against DACOM (differential absorption mid-IR diode laser spectrometer) in situ CO measurements from the INTEX-B (Intercontinental Chemical Transport Experiment: MILAGRO and Pacific phases) field campaign and in situ data from HIPPO (HIAPER Pole-to-Pole Observations) flights. The data fusion results show improved sensitivities in the lower and upper troposphere (20–30% and above 20%, respectively) as compared with AIRS-only version 5 CO retrievals, and improved daily coverage compared with TES and MLS CO data.

Understanding the impact of recent advances in isoprene photooxidation on simulations of regional air quality

Abstract. The CMAQ (Community Multiscale Air Quality) us model in combination with observations for INTEX-NA/ICARTT (Intercontinental Chemical Transport Experiment–North America/International Consortium for Atmospheric Research on Transport and Transformation) 2004 are used to evaluate recent advances in isoprene oxidation chemistry and provide constraints on isoprene nitrate yields, isoprene nitrate lifetimes, and NOx recycling rates. We incorporate recent advances in isoprene oxidation chemistry into the SAPRC-07 chemical mechanism within the US EPA (United States Environmental Protection Agency) CMAQ model. The results show improved model performance for a range of species compared against aircraft observations from the INTEX-NA/ICARTT 2004 field campaign. We further investigate the key processes in isoprene nitrate chemistry and evaluate the impact of uncertainties in the isoprene nitrate yield, NOx (NOx = NO + NO2) recycling efficiency, dry deposition velocity, and RO2 + HO2 reaction rates. We focus our examination on the southeastern United States, which is impacted by both abundant isoprene emissions and high levels of anthropogenic pollutants. We find that NOx concentrations increase by 4–9% as a result of reduced removal by isoprene nitrate chemistry. O3 increases by 2 ppbv as a result of changes in NOx. OH concentrations increase by 30%, which can be primarily attributed to greater HOx production. We find that the model can capture observed total alkyl and multifunctional nitrates (∑ANs) and their relationship with O3 by assuming either an isoprene nitrate yield of 6% and daytime lifetime of 6 hours or a yield of 12% and lifetime of 4 h. Uncertainties in the isoprene nitrates can impact ozone production by 10% and OH concentrations by 6%. The uncertainties in NOx recycling efficiency appear to have larger effects than uncertainties in isoprene nitrate yield and dry deposition velocity. Further progress depends on improved understanding of isoprene oxidation pathways, the rate of NOx recycling from isoprene nitrates, and the fate of the secondary, tertiary, and further oxidation products of isoprene.

Simulation and validation of the aerosol optical thickness over China in 2006

The Model of Atmospheric Transport and Chemistry (MATCH) developed by the US National Center for Atmospheric Research (NCAR) was used to calculate the aerosol optical thickness (AOT) over China in 2006, with emission source data of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) and NCEP/NCAR reanalysis data as inputs. The simulation results of AOT were then validated with observational data from the Moderate Resolution Imaging Spectroradiometer (MODIS), Chinese Sun Hazemeter Network (CSHNET), Aerosol Robotics Network (AERONET), and China Aerosol Remote Sensing Network (CARSNET) at more than 30 stations over China. The comparison results indicated that the high values of AOT in the areas such as the Sichuan basin and East and South China and the low values of AOT over the Tibetan Plateau and Northwest and Northeast China were reasonably simulated by the MATCH. This model tended to underestimate the AOT values in high-aerosol-loading areas but overestimate the AOT values in less polluted areas because there are still large uncertainties in the expression of emission sources, the description of the optical properties of aerosols, the treatment of cloud and precipitation, and the selection of grid resolution. The modeling results were consistent with the CSHNET, CARSNET, AERONET, and MODIS data in most parts of China, and the correlation coefficient of the monthly mean AOT between the model and the observation was 0.79 with CSHNET data at 23 stations, 0.51 with MODIS data, and 0.88 with data at 3 CARSNET stations and 2 other stations. All of them passed the significance test with α < 0.0001. The results demonstrated that the MATCH has the ability to simulate the characteristics of the AOT distribution and its seasonal variation over China.

Impact of lightning-NO on eastern United States photochemistry during the summer of 2006 as determined using the CMAQ model

Abstract. A lightning-nitrogen oxide (NO) algorithm is implemented in the Community Multiscale Air Quality Model (CMAQ) and used to evaluate the impact of lightning-NO emissions (LNOx) on tropospheric photochemistry over the United States during the summer of 2006. For a 500 mole per flash lightning-NO source, the mean summertime tropospheric NO2 column agrees with satellite-retrieved columns to within −5 to +13%. Temporal fluctuations in the column are moderately well simulated; however, the addition of LNOx does not lead to a better simulation of day-to-day variability. The contribution of lightning-NO to the model column ranges from ∼10% in the northern US to &gt;45% in the south-central and southeastern US. Lightning-NO adds up to 20 ppbv to upper tropospheric model ozone and 1.5–4.5 ppbv to 8-h maximum surface layer ozone, although, on average, the contribution of LNOx to model surface ozone is 1–2 ppbv less on poor air quality days. LNOx increases wet deposition of oxidized nitrogen by 43% and total deposition of nitrogen by 10%. This additional deposition reduces the mean magnitude of the CMAQ low-bias in nitrate wet deposition with respect to National Atmospheric Deposition monitors to near zero. Differences in urban/rural biases between model and satellite-retrieved NO2 columns were examined to identify possible problems in model chemistry and/or transport. CMAQ columns were too large over urban areas. Biases at other locations were minor after accounting for the impacts of lightning-NO emissions and the averaging kernel on model columns. In order to obtain an upper bound on the contribution of uncertainties in NOy chemistry to upper tropospheric NOx low biases, sensitivity calculations with updated chemistry were run for the time period of the Intercontinental Chemical Transport Experiment (INTEX-A) field campaign (summer 2004). After adjusting for possible interferences in NO2 measurements and averaging over the entire campaign, these updates reduced 7–9 km biases from 32 to 17% and 9–12 km biases from 57 to 46%. While these changes lead to better agreement, a considerable unexplained NO2 low-bias remains in the uppermost troposphere.

Source contributions to carbonaceous aerosol concentrations in Korea

We estimated the source contributions to carbonaceous aerosol concentration in Korea on the basis of Intercontinental Chemical Transport Experiment Phase B (INTEX-B) anthropogenic emissions and satellite-derived biomass burning emissions by using a nested version of GEOS-Chem with a spatial resolution of 0.5 � � 0.667 � for the period March 2006eFebruary 2007. First, we evaluated the model by comparing the simulated and observed aerosol concentrations at East Asia Network (EANET) sites and at a site in Korea. The results indicate that the model reproduces the variability and magnitudes of the observed SO4 2� ,N O 3 � , and NH 4 þ concentrations in Korea and those of the observed PM 10 concentrations in East Asia. However, the organic carbon (OC) and black carbon (BC) aerosol concentrations estimated by the model are lower than those observed in Korea by a factor of 2, especially in winter. This underestimation is likely due to extremely low domestic anthropogenic emissions and lack in seasonal variation. Source adjustments using a simple fitting and the Emission Database for Global Atmospheric Research (EDGAR) monthly allocation factors for seasonal variation yield significantly improved model results (R 2

Impact of lightning NO emissions on North American photochemistry as determined using the Global Modeling Initiative (GMI) model

The impact of nitric oxide (NO) emissions by lightning on summertime North American nitrogen oxides (NOx) and ozone is studied using the Global Modeling Initiative (GMI) CTM and an improved lightning NO algorithm. The spatial distributions of modeled and National Lightning Detection Network‐based flash rates during the summers of 2004–2006 agree well (R2 = 0.49, 18% low bias). Despite this reasonable agreement, 9–12 km model NOx during the Intercontinental Chemical Transport Experiment (INTEX‐A) campaign is a factor of 2.2–3.6 too low for a simulation that includes a 480 mol per flash midlatitude lightning NO source, the source that provides the best agreement with measurements. Possible causes of this low bias include biases in model convection and/or too rapid NOx chemistry in the upper troposphere. Model tropospheric NO2 columns over the southeastern United States during these summers show a 7% high bias with respect to the OMI DOMINO/GEOS‐Chem tropospheric column NO2 product. Observed changes between 2004 and 2006 in upper tropospheric ozone at southeastern U. S. INTEX Ozonesonde Network Study sites are captured by the model and appear to be caused by a stronger upper tropospheric anticyclone in 2006 that led to an increase from 21 to 30 ppbv between 2004 and 2006 in the amount of ozone with a lightning NO source; lightning NO emissions were 15%–20% larger in 2004. The contribution of lightning NO to monthly average summertime 300 hPa NOx over the eastern United States during 2004–2006 varies from 61%–73% (0.09–0.16 ppbv), while the contribution to ozone varies from 19%–31% (15–24 ppbv).

Improved agreement of AIRS tropospheric carbon monoxide products with other EOS sensors using optimal estimation retrievals

Abstract. We present in this paper an alternative retrieval algorithm for the Atmospheric Infrared Sounder (AIRS) tropospheric Carbon Monoxide (CO) products using the Optimal Estimation (OE) technique, which is different from the AIRS operational algorithm. The primary objective for this study was to compare AIRS CO, as well as the other retrieval properties such as the Averaging Kernels (AKs), the Degrees of Freedom for Signal (DOFS), and the error covariance matrix, against the Tropospheric Emission Spectrometer (TES) and the Measurement of Pollution in the Troposphere (MOPITT) CO, which were also derived using the OE technique. We also demonstrate that AIRS OE CO results are much more realistic than AIRS V5 operational CO, especially in the lower troposphere and in the Southern Hemisphere (SH). These products are validated with in situ profiles obtained by the Differential Absorption Carbon Monoxide Measurements (DACOM), which took place as part of NASA's Intercontinental Chemical Transport Experiment (INTEX-B) field mission that was conducted over the northern Pacific in Spring 2006. To demonstrate the differences existing in the current operational products we first show a detailed direct comparison between AIRS V5 and TES operational V3 CO for the global datasets from December 2005 to July 2008. We then present global CO comparisons between AIRS OE, TES V3, and MOPITT V4 at selected pressure levels as well as for the total column amounts. We conclude that the tropospheric CO retrievals from AIRS OE and TES V3 agree to within 5–10 ppbv or 5% on average globally and throughout the free troposphere. The agreements in total column CO amounts between AIRS OE and MOPITT V4 have improved significantly compared to AIRS V5 with global relative RMS differences now being 12.7%.

Descent of deep stratospheric intrusions during the IONS August 2006 campaign

Deep stratosphere‐to‐troposphere transport (STT) conveying ozone‐rich stratospheric air to the lower troposphere in the extratropics can episodically increase ozone concentrations in the lower troposphere. However, dynamical aspects of the descent, including dispersion and mixing with the surrounding tropospheric air and necessary conditions for reaching the lower troposphere, are not clearly understood yet. This study focuses on August 2006, as daily balloon sonde measurements were made from many sites covering North America within the Intercontinental Chemical Transport Experiment Ozonesonde Network Study campaign. During this period, four profiles were found with clear signs of deep STT. A mesoscale model was used together with trajectory calculation to represent these events. Over 10 days, 20 distinct clusters of trajectories were identified as significant deep STT events, including three observed. The four largest clusters carried 41, 35, 25, and 16 × 1012 kg of mass of air, respectively. A dynamical analysis was performed on the three observed events that were captured numerically. The descents showed three distinct phases: (1) crossing of the tropopause, (2) free descent, and (3) quasi‐horizontal dispersion in the lower troposphere. Clusters are rapidly sliding down sloping isentropes while being slowly diabatically cooled (approximately −1 K d−1). The tilt in the isentropes along the descent is due to an approximately equal combination of a negative potential temperature anomaly at the tropopause during phase 1 and a nearby baroclinic zone at the ground. The combination of these two conditions appears to be necessary for reaching the lower troposphere. In the three cases, the clusters stayed compact until they reach the lower troposphere, and it is estimated that approximately 80% of the ozone of stratospheric origin is released directly in the lower troposphere.

Trans-Pacific transport of reactive nitrogen and ozone to Canada during spring

Abstract. We interpret observations from the Intercontinental Chemical Transport Experiment, Phase B (INTEX-B) in spring 2006 using a global chemical transport model (GEOS-Chem) to evaluate sensitivities of the free troposphere above the North Pacific Ocean and North America to Asian anthropogenic emissions. We develop a method to use satellite observations of tropospheric NO2 columns to provide timely estimates of trends in NOx emissions. NOx emissions increased by 33% for China and 29% for East Asia from 2003 to 2006. We examine measurements from three aircraft platforms from the INTEX-B campaign, including a Canadian Cessna taking vertical profiles of ozone near Whistler Peak. The contribution to the mean simulated ozone profiles over Whistler below 5.5 km is at least 7.2 ppbv for Asian anthropogenic emissions and at least 3.5 ppbv for global lightning NOx emissions. Tropospheric ozone columns from OMI exhibit a broad Asian outflow plume across the Pacific, which is reproduced by simulation. Mean modelled sensitivities of Pacific (30° N–60° N) tropospheric ozone columns are at least 4.6 DU for Asian anthropogenic emissions and at least 3.3 DU for lightning, as determined by simulations excluding either source. Enhancements of ozone over Canada from Asian anthropogenic emissions reflect a combination of trans-Pacific transport of ozone produced over Asia, and ozone produced in the eastern Pacific through decomposition of peroxyacetyl nitrates (PANs). A sensitivity study decoupling PANs globally from the model's chemical mechanism establishes that PANs increase ozone production by removing NOx from regions of low ozone production efficiency (OPE) and injecting it into regions with higher OPE, resulting in a global increase in ozone production by 2% in spring 2006. PANs contribute up to 4 ppbv to surface springtime ozone concentrations in western Canada. Ozone production due to PAN transport is greatest in the eastern Pacific; commonly occurring transport patterns advect this ozone northeastward into Canada. Transport events observed by the aircraft confirm that polluted airmasses were advected in this way.