Top-down estimates of global CO sources using MOPITT measurements

We present a synthesis inversion of CO emissions from various geographical regions and for various source categories for the year 2000 using CO retrievals from the MOPITT (Measurements of Pollution in the Troposphere) instrument. We find a large discrepancy between our top‐down estimates and recent bottom‐up estimates of CO emissions from fossil fuel/biofuel (FFBF) use in Asia. A key conclusion of this study is that CO emissions in East Asia (EAS) are about a factor of 1.8–2 higher than recent bottom‐up estimates

Challenges in Developing Better Observational Constraints and Models for Aerosols : Emerging Ideas for Design and Use of Future Observing Systems

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Top-down estimates of global CO sources using MOPITT measurements

We present a synthesis inversion of CO emissions from various geographical regions and for various source categories for the year 2000 using CO retrievals from the MOPITT (Measurements of Pollution in the Troposphere) instrument. We find a large discrepancy between our top‐down estimates and recent bottom‐up estimates of CO emissions from fossil fuel/biofuel (FFBF) use in Asia. A key conclusion of this study is that CO emissions in East Asia (EAS) are about a factor of 1.8–2 higher than recent bottom‐up estimates

Measurement Report: Firework Impacts on Air Quality in Metro Manila, Philippines, during the 2019 New Year Revelry

Fireworks degrade air quality, reduce visibility, alter atmospheric chemistry, and cause short-term adverse health effects. However, there have not been any comprehensive physicochemical and optical measurements of fireworks and their associated impacts in a Southeast Asia megacity, where fireworks are a regular part of the culture. Size-resolved particulate matter (PM) measurements were made before, during, and after New Year 2019 at the Manila Observatory in Quezon City, Philippines, as part of the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex). A high-spectral-resolution lidar (HSRL) recorded a substantial increase in backscattered signal associated with high aerosol loading ∼440 m above the surface during the peak of firework activities around 00:00 (local time). This was accompanied by PM2.5 concentrations peaking at 383.9 µg m−3. During the firework event, water-soluble ions and elements, which affect particle formation, growth, and fate, were mostly in the submicrometer diameter range. Total (\u3e0.056 µm) water-soluble bulk particle mass concentrations were enriched by 5.7 times during the fireworks relative to the background (i.e., average of before and after the firework). The water-soluble mass fraction of PM2.5 increased by 18.5 % above that of background values. This corresponded to increased volume fractions of inorganics which increased bulk particle hygroscopicity, kappa (κ), from 0.11 (background) to 0.18 (fireworks). Potassium and non-sea-salt (nss) SO42- role= presentation style= box-sizing: border-box; border-radius: 0px; display: inline; line-height: normal; word-spacing: normal; overflow-wrap: normal; white-space: nowrap; float: none; direction: ltr; max-width: none; max-height: none; min-width: 0px; min-height: 0px; border: 0px; padding: 0px; margin: 0px; position: relative; \u3e2−4 contributed the most (70.9 %) to the water-soluble mass, with their mass size distributions shifting from a smaller to a larger submicrometer mode during the firework event. On the other hand, mass size distributions for NO3- role= presentation style= box-sizing: border-box; border-radius: 0px; display: inline; line-height: normal; word-spacing: normal; overflow-wrap: normal; white-space: nowrap; float: none; direction: ltr; max-width: none; max-height: none; min-width: 0px; min-height: 0px; border: 0px; padding: 0px; margin: 0px; position: relative; \u3e−3, Cl−, and Mg2+ (21.1 % mass contribution) shifted from a supermicrometer mode to a submicrometer mode. Being both uninfluenced by secondary aerosol formation and constituents of firework materials, a subset of species were identified as the best firework tracer species (Cu, Ba, Sr, K+, Al, and Pb). Although these species (excluding K+) only contributed 2.1 % of the total mass concentration of water-soluble ions and elements, they exhibited the highest enrichments (6.1 to 65.2) during the fireworks. Surface microscopy analysis confirmed the presence of potassium/chloride-rich cubic particles along with capsule-shaped particles in firework samples. The results of this study highlight how firework emissions change the physicochemical and optical properties of water-soluble particles (e.g., mass size distribution, composition, hygroscopicity, and aerosol backscatter), which subsequently alters the background aerosol\u27s respirability, influence on surroundings, ability to uptake gases, and viability as cloud condensation nuclei (CCN)

Source Contributions to Carbon Monoxide Concentrations During KORUS‐AQ Based on CAM‐chem Model Applications

We investigate regional sources contributing to CO during the Korea United States Air Quality (KORUS-AQ) campaign conducted over Korea (1 May to 10 June 2016) using 17 tagged CO simulations from the Community Atmosphere Model with chemistry (CAM-chem). The simulations use three spatial resolutions, three anthropogenic emission inventories, two meteorological fields, and nine emission scenarios. These simulations are evaluated against measurements from the DC-8 aircraft and Measurements Of Pollution In The Troposphere (MOPITT). Results show that simulations using bottom-up emissions are consistently lower (bias: -34 to -39%) and poorer performing (Taylor skill: 0.38-0.61) than simulations using alternative anthropogenic emissions (bias: -6 to -33%; Taylor skill: 0.48-0.86), particularly for enhanced Asian CO and volatile organic compound (VOC) emission scenarios, suggesting underestimation in modeled CO background and emissions in the region. The ranges of source contributions to modeled CO along DC-8 aircraft from Korea and southern (90 degrees E to 123 degrees E, 20 degrees N to 29 degrees N), middle (90 degrees E to 123 degrees E, 29 degrees N to 38.5 degrees N), and northern (90 degrees E to 131.5 degrees E, 38.5 degrees N to 45 degrees N) East Asia (EA) are 6-13%, similar to 5%, 16-28%, and 9-18%, respectively. CO emissions from middle and northern EA can reach Korea via transport within the boundary layer, whereas those from southern EA are transported to Korea mainly through the free troposphere. Emission contributions from middle EA dominate during continental outflow events (29-51%), while Korean emissions play an overall more important role for ground sites (up to 25-49%) and plumes within the boundary layer (up to 25-44%) in Korea. Finally, comparisons with four other source contribution approaches (FLEXPART 9.1 back trajectory calculations driven by Weather Research and Forecasting (WRF) WRF inert tracer, China signature VOCs, and CO to CO2 enhancement ratios) show general consistency with CAM-chem.National Science Foundation (NSF); U.S. Department of Energy (DOE); National Aeronautics and Space Administration (NASA) Earth Observing System (EOS) Program; NCAR Advanced Study Program Postdoctoral Fellowship; Environment Research and Technology Development Fund of the Ministry of the Environment, Japan [2-1505, 2-1803]; National Science Foundation; NASA [NNX16AD96G, NNX16AE16G, NNX17AG39G]6 month embargo; published online: 1 February 2019This item from the UA Faculty Publications collection is made available by the University of Arizona with support from the University of Arizona Libraries. If you have questions, please contact us at [email protected]

The Multi-Scale Infrastructure for Chemistry and Aerosols (MUSICA)

To explore the various couplings across space and time and between ecosystems in a consistent manner, atmospheric modeling is moving away from the fractured limited-scale modeling strategy of the past toward a unification of the range of scales inherent in the Earth system. This paper describes the forward-looking Multi-Scale Infrastructure for Chemistry and Aerosols (MUSICA), which is intended to become the next-generation community infrastructure for research involving atmospheric chemistry and aerosols. MUSICA will be developed collaboratively by the National Center for Atmospheric Research (NCAR) and university and government researchers, with the goal of serving the international research and applications communities. The capability of unifying various spatiotemporal scales, coupling to other Earth system components, and process-level modularization will allow advances in both fundamental and applied research in atmospheric composition, air quality, and climate and is also envisioned to become a platform that addresses the needs of policy makers and stakeholders

Decreasing Aerosol Loading in the North American Monsoon Region

We examine the spatio-temporal variability of aerosol loading in the recent decade (2005–2014) over the North American Monsoon (NAM) region. Emerging patterns are characterized using aerosol optical depth (AOD) retrievals from the NASA Terra/Moderate Resolution Imaging Spectroradiometer (MODIS) instrument along with a suite of satellite retrievals of atmospheric and land-surface properties. We selected 20 aerosol hotspots and classified them into fire, anthropogenic, dust, and NAM alley clusters based on the dominant driver influencing aerosol variability. We then analyzed multivariate statistics of associated anomalies during pre-, monsoon, and post-monsoon periods. Our results show a decrease in aerosol loading for the entire NAM region, confirming previous reports of a declining AOD trend over the continental United States. This is evident during pre-monsoon and monsoon for fire and anthropogenic clusters, which are associated with a decrease in the lower and upper quartile of fire counts and carbon monoxide, respectively. The overall pattern is obfuscated in the NAM alley, especially during monsoon and post-monsoon seasons. While the NAM alley is mostly affected by monsoon precipitation, the frequent occurrence of dust storms in the area modulates this trend. We find that aerosol loading in the dust cluster is associated with observed vegetation index and has only slightly decreased in the recent decade

Spatial and Temporal Variations in Characteristic Ratios of Elemental Carbon to Carbon Monoxide and Nitrogen Oxides across the United States

A ratio-based method is used to characterize anthropogenic elemental carbon (EC_a) using in situ measurements and emissions of carbon monoxide (CO) and nitrogen oxides (NO_<i>x</i>). We use long-term records of ground-based measurements from the U.S. Environmental Protection Agency (EPA) Air Quality System and Interagency Monitoring of Protected Visual Environments to assess the patterns in anthropogenic combustion ratios (ΔEC_a/ΔCO and ΔEC_a/ΔNO_<i>x</i>) across the U.S. Petroleum Administration for Defense Districts (PADD) regions for the years 2000–2015. We investigate the change in these ratios between the periods 2000–2007 and 2008–2015. Overall, ΔEC_a/ΔCO ratios increase by 0.7–82% and ΔEC_a/ΔNO_<i>x</i> by 6.8–104% across the East and West PADD regions. The urban West showed the largest increase relative to other regions. This is mainly attributed to a 13–23% increase in ΔEC_a during the winter and fall seasons and significant reductions in urban ΔNO_<i>x</i> (except in winter). We also find that emission ratios derived from the EPA’s National Emission Inventory (NEI) overestimate (underestimate) the increase in the observed enhancement ratios in the East (West). Analyses of changes in NEI emissions in the West reveal (a) smaller reductions in NEI emissions for NO_<i>x</i> from the off-road sector and (b) an increase in PM_2.5 (particulate matter 2.5 μm or less in diameter) emissions from commercial/residential combustion and smaller reductions in nonroad emissions

Decreasing Aerosol Loading in the North American Monsoon Region.

We examine the spatio-temporal variability of aerosol loading in the recent decade (2005-2014) over the North American Monsoon (NAM) region. Emerging patterns are characterized using aerosol optical depth (AOD) retrievals from the NASA Terra/Moderate Resolution Imaging Spectroradiometer (MODIS) instrument along with a suite of satellite retrievals of atmospheric and land-surface properties. We selected 20 aerosol hotspots and classified them into fire, anthropogenic, dust, and NAM alley clusters based on the dominant driver influencing aerosol variability. We then analyzed multivariate statistics of associated anomalies during pre-, monsoon, and post-monsoon periods. Our results show a decrease in aerosol loading for the entire NAM region, confirming previous reports of a declining AOD trend over the continental United States. This is evident during pre-monsoon and monsoon for fire and anthropogenic clusters, which are associated with a decrease in the lower and upper quartile of fire counts and carbon monoxide, respectively. The overall pattern is obfuscated in the NAM alley, especially during monsoon and post-monsoon seasons. While the NAM alley is mostly affected by monsoon precipitation, the frequent occurrence of dust storms in the area modulates this trend. We find that aerosol loading in the dust cluster is associated with observed vegetation index and has only slightly decreased in the recent decade