Aerosol Source Attributions and Source-Receptor Relationships Across the Northern Hemisphere

Emissions and long-range transport of air pollution pose major concerns on air quality and climate change. To better assess the impact of intercontinental transport of air pollution on regional and global air quality, ecosystems, and near-term climate change, the UN Task Force on Hemispheric Transport of Air Pollution (HTAP) is organizing a phase II activity (HTAP2) that includes global and regional model experiments and data analysis, focusing on ozone and aerosols. This study presents the initial results of HTAP2 global aerosol modeling experiments. We will (a) evaluate the model results with surface and aircraft measurements, (b) examine the relative contributions of regional emission and extra-regional source on surface PM concentrations and column aerosol optical depth (AOD) over several NH pollution and dust source regions and the Arctic, and (c) quantify the source-receptor relationships in the pollution regions that reflect the sensitivity of regional aerosol amount to the regional and extra-regional emission reductions

Observations of convective and dynamical instabilities in tropopause folds and their contribution to stratosphere-troposphere exchange

With aircraft-mounted in situ and remote sensing instruments for dynamical, thermal, and chemical measurements we studied two cases of tropopause folding. In both folds we found Kelvin-Helmholtz billows with horizontal wavelength of ∼900 m and thickness of ∼120 m. In one case the instability was effectively mixing the bottomside of the fold, leading to the transfer of stratospheric air into the troposphere. Also, we discovered in both cases small-scale secondary ozone maxima shortly after the aircraft ascended past the topside of the fold that corresponded to regions of convective instability. We interpreted this phenomenon as convectively breaking gravity waves. Therefore we posit that convectively breaking gravity waves acting on tropopause folds must be added to the list of important irreversible mixing mechanisms leading to stratosphere-troposphere exchange.United States. National Aeronautics and Space Administration (Grant NAG2-1105)United States. National Aeronautics and Space Administration (Grant NAGl-1758)United States. National Aeronautics and Space Administration (Grant NAGl-1901

Observationally constrained analysis of sea salt aerosol in the marine atmosphere

Atmospheric sea salt plays important roles in marine cloud formation and atmospheric chemistry. We performed an integrated analysis of NASA GEOS model simulations run with the GOCART aerosol module, in situ measurements from the PALMS and SAGA instruments obtained during the NASA ATom campaign, and aerosol optical depth (AOD) measurements from the AERONET Marine Aerosol Network (MAN) and from MODIS satellite observations to better constrain sea salt in the marine atmosphere. ATom measurements and GEOS model simulations both show that sea salt concentrations over the Pacific and Atlantic oceans have a strong vertical gradient, varying up to 4 orders of magnitude from the marine boundary layer to free troposphere. The modeled residence times suggest that the lifetime of sea salt particles with a dry diameter of less than 3 µm is largely controlled by wet removal, followed by turbulent process. During both boreal summer and winter, the GEOS-simulated sea salt mass mixing ratios agree with SAGA measurements in the marine boundary layer (MBL) and with PALMS measurements above the MBL. However, comparison of AOD from GEOS with AERONET/MAN and MODIS aerosol retrievals indicated that the model underestimated AOD over the oceans where sea salt dominates. The apparent discrepancy of slightly overpredicted concentration and large underpredicted AOD could not be explained by biases in the model RH affecting the particle hygroscopic growth, as modeled RH was found to be comparable to or larger than the in situ measurements. This conundrum could at least partially be explained by the difference in sea salt size distribution; the GEOS simulation has much less sea salt percentage-wise in the smaller particle size range and thus less efficient light extinction than what was observed by PALMS

Convective and Wave Signatures in Ozone Profiles Over the Equatorial Americas: Views from TC4 (2007) and SHADOZ

During the months of July-August 2007 NASA conducted a research campaign called the Tropical Composition, Clouds and Climate Coupling (TC4) experiment. Vertical profiles of ozone were measured daily using an instrument known as an ozonesonde, which is attached to a weather balloon and launch to altitudes in excess of 30 km. These ozone profiles were measured over coastal Las Tablas, Panama (7.8N, 80W) and several times per week at Alajuela, Costa Rica (ION, 84W). Meteorological systems in the form of waves, detected most prominently in 100- 300 in thick ozone layer in the tropical tropopause layer, occurred in 50% (Las Tablas) and 40% (Alajuela) of the soundings. These layers, associated with vertical displacements and classified as gravity waves ("GW," possibly Kelvin waves), occur with similar stricture and frequency over the Paramaribo (5.8N, 55W) and San Cristobal (0.925, 90W) sites of the Southern Hemisphere Additional Ozonesondes (SHADOZ) network. The gravity wave labeled layers in individual soundings correspond to cloud outflow as indicated by the tracers measured from the NASA DC-8 and other aircraft data, confirming convective initiation of equatorial waves. Layers representing quasi-horizontal displacements, referred to as Rossby waves, are robust features in soundings from 23 July to 5 August. The features associated with Rossby waves correspond to extra-tropical influence, possibly stratospheric, and sometimes to pollution transport. Comparison of Las Tablas and Alajuela ozone budgets with 1999-2007 Paramaribo and San Cristobal soundings shows that TC4 is typical of climatology for the equatorial Americas. Overall during TC4, convection and associated meteorological waves appear to dominate ozone transport in the tropical tropopause layer

Mechanical Engineering

Black carbon (BC) emissions play an important role in regional climate change in the Arctic. It is necessary to pay attention to the impact of long-range transport from regions outside the Arctic as BC emissions from local sources in the Arctic were relatively small. The task force Hemispheric Transport of Air Pollution Phase 2 (HTAP2) set up a series of simulation scenarios to investigate the response of BC in a given region to different source regions. This study investigated the responses of Arctic BC concentrations and surface temperature to 20&thinsp;% anthropogenic emission reductions from six regions in 2010 within the framework of HTAP2 based on ensemble modeling results. Emission reductions from East Asia (EAS) had the most (monthly contributions: 0.2&ndash;1.5&thinsp;ng&thinsp;m&minus;3) significant impact on the Arctic near-surface BC concentrations, while the monthly contributions from Europe (EUR), Middle East (MDE), North America (NAM), Russia&ndash;Belarus&ndash;Ukraine (RBU), and South Asia (SAS) were 0.2&ndash;1.0, 0.001&ndash;0.01, 0.1&ndash;0.3, 0.1&ndash;0.7, and 0.0&ndash;0.2&thinsp;ng&thinsp;m&minus;3, respectively. The responses of the vertical profiles of the Arctic BC to the six regions were found to be different due to multiple transport pathways. Emission reductions from NAM, RBU, EUR, and EAS mainly influenced the BC concentrations in the low troposphere of the Arctic, while most of the BC in the upper troposphere of the Arctic derived from SAS. The response of the Arctic BC to emission reductions in six source regions became less significant with the increase in the latitude. The benefit of BC emission reductions in terms of slowing down surface warming in the Arctic was evaluated by using absolute regional temperature change potential (ARTP). Compared to the response of global temperature to BC emission reductions, the response of Arctic temperature was substantially more sensitive, highlighting the need for curbing global BC emissions. &nbsp;</p

OMI Tropospheric NO2 from Lightning in Observed Convective Events

Lightning is responsible for an estimated 15 percent of total NO emissions, and is one of the most prominent sources in the upper troposphere. In this study, we present evidence of lightning-generated NO2 (LNO2) using data from the Ozone Monitoring Instrument (OMI), which has observed tropospheric NO2 since its launch in 2004. Although LNO2 has been also reported in previous satellite studies from the Global Ozone Monitoring Experiment (GOME) and SCIAMACHY, OMI is better suited for such measurements by virtue of its higher spatial resolution and daily global coverage. We will present data clearly showing the LNO2 signal in the OMI tropospheric NO2 product on two days over and downwind of specific convective systems in the US Midwest. Gridded monthly mean tropospheric NO 2 data are subtracted from the daily gridded data to obtain the presumed LNO2 signal. Observed cloud-to-ground (CG) lightning flashes from the National Lightning Detection Network (NLDN) were counted along middle and upper tropospheric back trajectories that were run from the regions containing the LNO2 signal. A vertically-weighted average number of upwind CG flashes was obtained using a profile of LNO(x) mass obtained from a series of midlatitude cloud-resolved storm chemistry simulations. The number of CG flashes was scaled up to total flashes (intracloud (IC) flashes plus CG) using a climatological IC/CG ratio. The number of moles of LNO(x) in the region considered was estimated by assuming that LNO2 is 30 percent of LNO(x). This value was divided by the number of upwind flashes to obtain an average estimate of the number of moles produced per flash. Results yield values in the range obtained through other estimation techniques (e.g., aircraft measurements, models). We will also present a similar analysis over northern Australia during the SCOUT-O3/ACTIVE field campaigns in November and December 2005, in which we will compare the OMI LNOx signals with aircraft observations from the storm anvils

Regional and Global Aspects of Aerosols in Western Africa: From Air Quality to Climate

Western Africa is one of the most important aerosol source regions in the world. Major aerosol sources include dust from the world's largest desert Sahara, biomass burning from the Sahel, pollution aerosols from local sources and long-range transport from Europe, and biogenic sources from vegetation. Because these sources have large seasonal variations, the aerosol composition over the western Africa changes significantly with time. These aerosols exert large influences on local air quality and regional climate. In this study, we use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to analyze satellite lidar data from the GLAS instrument on the ICESat and the sunphotometer data from the ground-based network AERONET taken in both the wet (September - October 2003) and dry (February - March 2004) seasons over western Africa. We will quantify the seasonal variations of aerosol sources and compositions and aerosol spatial (horizontal and vertical) distributions over western Africa. We will also assess the climate impact of western African aerosols. Such studies will be applied to support the international project, Africa Monsoon Multidisciplinary Analysis (AMMA) and to analyze the AMMA data

Responses of Arctic black carbon and surface temperature to multi-region emission reductions: A Hemispheric Transport of Air Pollution Phase 2 (HTAP2) ensemble modeling study

Black carbon (BC) emissions play an important role in regional climate change in the Arctic. It is necessary to pay attention to the impact of long-range transport from regions outside the Arctic as BC emissions from local sources in the Arctic were relatively small. The task force Hemispheric Transport of Air Pollution Phase 2 (HTAP2) set up a series of simulation scenarios to investigate the response of BC in a given region to different source regions. This study investigated the responses of Arctic BC concentrations and surface temperature to 20 % anthropogenic emission reductions from six regions in 2010 within the framework of HTAP2 based on ensemble modeling results. Emission reductions from East Asia (EAS) had the most (monthly contributions: 0.2–1.5 ng m−3) significant impact on the Arctic near-surface BC concentrations, while the monthly contributions from Europe (EUR), Middle East (MDE), North America (NAM), Russia–Belarus–Ukraine (RBU), and South Asia (SAS) were 0.2–1.0, 0.001–0.01, 0.1–0.3, 0.1–0.7, and 0.0–0.2 ng m−3, respectively. The responses of the vertical profiles of the Arctic BC to the six regions were found to be different due to multiple transport pathways. Emission reductions from NAM, RBU, EUR, and EAS mainly influenced the BC concentrations in the low troposphere of the Arctic, while most of the BC in the upper troposphere of the Arctic derived from SAS. The response of the Arctic BC to emission reductions in six source regions became less significant with the increase in the latitude. The benefit of BC emission reductions in terms of slowing down surface warming in the Arctic was evaluated by using absolute regional temperature change potential (ARTP). Compared to the response of global temperature to BC emission reductions, the response of Arctic temperature was substantially more sensitive, highlighting the need for curbing global BC emissions

Multi-model study of HTAP II on sulfur and nitrogen deposition

This study uses multi-model ensemble results of 11 models from the second phase of Task Force Hemispheric Transport of Air Pollution (HTAP II) to calculate the global sulfur (S) and nitrogen (N) deposition in 2010. Modeled wet deposition is evaluated with observation networks in North America, Europe and East Asia. The modeled results agree well with observations, with 76–83% of stations being edicted within 50% of observations. The models underestimate SO24 , NO3 and NHC 4 wet depositions in some European and East Asian stations but overestimate NO3 wet deposition in the eastern United States. Intercomparison with previous projects (PhotoComp, ACCMIP and HTAP I) shows that HTPA II has considerably improved the estimation of deposition at European and East Asian stations. Modeled dry deposition is generally higher than the “inferential” data calculated by observed concentration and modeled velocity in North America, but the inferential data have high uncertainty, too. The global S deposition is 84 Tg(S) in 2010, with 49% in continental regions and 51% in the ocean (19% of which coastal). The global N deposition consists of 59 Tg(N) oxidized nitrogen (NOy / deposition and 64 Tg(N) reduced nitrogen (NHx / deposition in 2010. About 65% of N is deposited in continental regions, and 35% in the ocean (15% of which coastal). The estimated outflow of pollution from land to ocean is about 4 Tg(S) for S deposition and 18 Tg(N) for N deposition. Comparing our results to the results in 2001 from HTAP I, we find that the global distributions of S and N deposition have changed considerably during the last 10 years. The global S deposition decreases 2 Tg(S) (3 %) from 2001 to 2010, with significant decreases in Europe (5 Tg(S) and 55 %), North America (3 Tg(S) and 29 %) and Russia (2 Tg(S) and 26 %), and increases in South Asia (2 Tg(S) and 42 %) and the Middle East (1 Tg(S) and 44 %). The global N deposition increases by 7 Tg(N) (6 %), mainly contributed by South Asia (5 Tg(N) and 39 %), East Asia (4 Tg(N) and 21 %) and Southeast Asia (2 Tg(N) and 21 %). The NHx deposition increases with no control policy on NH3 emission in North America. On the other hand, NOy deposition has started to dominate in East Asia (especially China) due to boosted NOx emission.JRC.D.5-Food Securit