scholarly journals The impact of North American anthropogenic emissions and lightning on long-range transport of trace gases and their export from the continent during summers 2002 and 2004

Author(s):  
Matus Martini ◽  
Dale J. Allen ◽  
Kenneth E. Pickering ◽  
Georgiy L. Stenchikov ◽  
Andreas Richter ◽  
...  
2006 ◽  
Vol 6 (8) ◽  
pp. 2057-2072 ◽  
Author(s):  
G. Guerova ◽  
I. Bey ◽  
J.-L. Attié ◽  
R. V. Martin ◽  
J. Cui ◽  
...  

Abstract. This paper reports on the transport of ozone (O3) and related species over the North Atlantic ocean and its impact on Europe. Measurements of nitrogen dioxide (NO2) and carbon monoxide (CO) columns from the GOME and MOPITT satellite instruments, respectively, are used in conjunction with the GEOS-CHEM global model of transport and tropospheric chemistry to identify the major events of long range transport that reach Europe over the course of summer 2000. Sensitivity model simulations are used to analyse observed O3 distributions with respect to the impact of long range transport events. For that purpose, we used in-situ O3 observations taken at the mountain site of Jungfraujoch as well as O3 vertical profiles taken in the vicinity of central European cities. Over the course of summer 2000, we identified 9 major episodes of transatlantic pollution transport; 7 events are associated with transient cyclones while 2 events occur through zonal transport (e.g. by advection in the strong low-level westerly winds established in summer between the Azores anticyclone and transient cyclones). We find that on average three episodes occur per month with the strongest ones being in June. The number and frequency of long range transport events that reach Europe are driven by the position and strength of the Azores anticyclone. Model sensitivity simulations indicate that the summer mean North American O3 contribution ranges from 3 to 5 ppb (7–11%) in the planetary boundary layer and 10 to 13 ppb (18–23%) in the middle and upper troposphere. During particular episodes, North American sources can result in O3 enhancements up to 25–28 ppb in the layer between 800–600 hPa and 10–12 ppb in the boundary layer. The impact of the zonal transport events on O3 distribution over Europe is more clearly seen below 700 hPa as they tend to transport pollution at lower levels while the events associated with transient cyclones are more likely to have an impact on the middle and upper troposphere (i.e. above 600 hPa). The air mass origins found in the GEOS-CHEM model are clearly confirmed by back trajectory analyses. During most of the 9 events, a strong contribution in North American O3 is in general associated with only little European O3 and vice-versa (in particular at the Jungfraujoch). A substantial North American contribution (e.g., 30% or higher) to O3 over Europe does not always result in pronounced O3 enhancements in the observations during our period of study.


2014 ◽  
Vol 14 (6) ◽  
pp. 7187-7303 ◽  
Author(s):  
J. D. Fast ◽  
J. Allan ◽  
R. Bahreini ◽  
J. Craven ◽  
L. Emmons ◽  
...  

Abstract. The performance of the Weather Research and Forecasting regional model with chemistry (WRF-Chem) in simulating the spatial and temporal variations in aerosol mass, composition, and size over California is quantified using measurements collected during the California Nexus of Air Quality and Climate Experiment (CalNex) and the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted during May and June of 2010. The extensive meteorological, trace gas, and aerosol measurements collected at surface sites and along aircraft and ship transects during CalNex and CARES were combined with operational monitoring network measurements to create a single dataset that was used to evaluate the one configuration of the model. Simulations were performed that examined the sensitivity of regional variations in aerosol concentrations to anthropogenic emissions and to long-range transport of aerosols into the domain obtained from a global model. The configuration of WRF-Chem used in this study is shown to reproduce the overall synoptic conditions, thermally-driven circulations, and boundary layer structure observed in region that controls the transport and mixing of trace gases and aerosols. However, sub-grid scale variability in the meteorology and emissions as well as uncertainties in the treatment of secondary organic aerosol chemistry likely contribute to errors at a primary surface sampling site located at the edge of the Los Angeles basin. Differences among the sensitivity simulations demonstrate that the aerosol layers over the central valley detected by lidar measurements likely resulted from lofting and recirculation of local anthropogenic emissions along the Sierra Nevada. Reducing the default emissions inventory by 50% led to an overall improvement in many simulated trace gases and black carbon aerosol at most sites and along most aircraft flight paths; however, simulated organic aerosol was closer to observed when there were no adjustments to the primary organic aerosol emissions. The model performance for some aerosol species was not uniform over the region, and we found that sulfate was better simulated over northern California whereas nitrate was better simulated over southern California. While the overall spatial and temporal variability of aerosols and their precursors were simulated reasonably well, we show cases where the local transport of some aerosol plumes were either too slow or too fast, which adversely affects the statistics regarding the differences between observed and simulated quantities. Comparisons with lidar and in-situ measurements indicate that long-range transport of aerosols from the global model was likely too high in the free troposphere even though their concentrations were relatively low. This bias led to an over-prediction in aerosol optical depth by as much as a factor of two that offset the under-predictions of boundary-layer extinction resulting primarily from local emissions. Lowering the boundary conditions of aerosol concentrations by 50% greatly reduced the bias in simulated aerosol optical depth for all regions of California. This study shows that quantifying regional-scale variations in aerosol radiative forcing and determining the relative role of emissions from local and distant sources is challenging during "clean" conditions and that a wide array of measurements are needed to ensure model predictions are correct for the right reasons. In this regard, the combined CalNex and CARES datasets are an ideal testbed that can be used to evaluate aerosol models in great detail and develop improved treatments for aerosol processes.


2009 ◽  
Vol 9 (4) ◽  
pp. 16381-16439 ◽  
Author(s):  
B. Adhikary ◽  
G. R. Carmichael ◽  
S. Kulkarni ◽  
C. Wei ◽  
Y. Tang ◽  
...  

Abstract. The Sulfur Transport and dEposition Model (STEM) developed at the University of Iowa is applied to the analysis of observations obtained during the Intercontinental Chemical Transport Experiment-Phase B (INTEX-B), conducted over the Pacific Ocean during the 2006 North American spring season. This paper reports on the model performance of meteorological parameters, trace gases, aerosols and photolysis rate (J-values) predictions with the NASA DC-8 and NSF/NCAR C-130 airborne measurements along with observations from three surface sites Mt. Bachelor, Trinidad Head and Kathmandu, Nepal. In general the model shows appreciable skill in predicting many of the important aspects of the observed distributions. The major meteorological parameters driving long range transport are accurately predicted by the WRF simulations used in this study. Furthermore, the STEM model predicts aerosols and trace gases concentrations within a standard deviation of most of the observed mean values. The results also point towards areas where model improvements are needed; e.g., the STEM model underestimates CO (15% for the DC8 and 6% for the C-130), whereas it overpredicts PAN (by a factor of two for both aircraft). The errors in the model calculations are attributed to uncertainty in emissions estimates and uncertainty in the top and lateral boundary conditions. Results from a series of sensitivity simulations examining the impact of the growth of emissions in Asia from 2000 to 2006, the importance of biomass burning, the effect of using boundary conditions from different global models, and the role of heterogeneous chemistry on the predictions are also presented. The impacts of heterogeneous reactions at specific times during dust transport episodes can be significant, and in the presence of dust both sulfate and nitrate aerosol production is increased and gas phase nitric acid levels are reduced appreciably (~50%). The aging of the air masses during the long range transport over the Pacific and the impact of various sources (source regions as well as energy and biomass burning) on targeted observations are analyzed using back-trajectories and tagged CO-tracer analysis.


Author(s):  
Hervé Petetin ◽  
Bastien Sauvage ◽  
Mark Parrington ◽  
Hannah Clark ◽  
Alain Fontaine ◽  
...  

<p><strong>Abstract.</strong> This study investigates the role of biomass burning and long-range transport in the anomalies of carbon monoxide (CO) regularly observed along the tropospheric vertical profiles measured in the framework of IAGOS. Considering the high interannual variability of biomass burning emissions and the episodic nature of pollution long-range transport, one strength of this study is the amount of data taken into account, namely 30,000 vertical profiles at 9 clusters of airports in Europe, North America, Asia, India and southern Africa over the period 2002&amp;ndash;2017. </p> <p> As a preliminary, a brief overview of the spatio-temporal variability, latitudinal distribution, interannual variability and trends of biomass burning CO emissions from 14 regions is provided. The distribution of CO mixing ratios at different levels of the troposphere is also provided based on the entire IAGOS database (125 million CO observations). </p> <p> This study focuses on the free troposphere (altitudes above 2<span class="thinspace"></span>km) where the long-range transport of pollution is favoured. Anomalies at a given airport cluster are here defined as departures from the local seasonally-averaged climatological vertical profile. The intensity of these anomalies varies significantly depending on the airport, with maximum (minimum) CO anomalies of 110&amp;ndash;150 (48)<span class="thinspace"></span>ppbv in Asia (Europe). Looking at the seasonal variation of the frequency of occurrence, the 25<span class="thinspace"></span>% strongest CO anomalies appears reasonably well distributed along the year, in contrast to the 5<span class="thinspace"></span>% or 1<span class="thinspace"></span>% strongest anomalies that exhibit a strong seasonality with for instance more frequent anomalies during summertime in northern United-States, during winter/spring in Japan, during spring in South-east China, during the non-monsoon seasons in south-east Asia and south India, and during summer/fall at Windhoek, Namibia. Depending on the location, these strong anomalies are observed in different parts of the free troposphere. </p> <p> In order to investigate the role of biomass burning emissions in these anomalies, we used the SOFT-IO v1.0 IAGOS added-value products that consist of FLEXPART 20-days backward simulations along all IAGOS aircraft trajectories, coupled with anthropogenic (MACCity) and biomass burning (GFAS) CO emission inventories and vertical injections. SOFT-IO estimates the contribution (in ppbv) of the recent (less than 20 days) primary worldwide CO emissions, tagged per source region. Biomass burning emissions are found to play an important role in the strongest CO anomalies observed at most airport clusters. The regional tags indicate a large contribution from boreal regions at airport clusters in Europe and North America during summer season. In both Japan and south India, the anthropogenic emissions dominate all along the year, except for the strongest summertime anomalies observed in Japan that are due to Siberian fires. The strongest CO anomalies at airport clusters located in south-east Asia are induced by fires burning during spring in south-east Asia and during fall in equatorial Asia. In southern Africa, the Windhoek airport was mainly impacted by fires in southern hemisphere Africa and South America. </p> <p> To our knowledge, no other studies have used such a large dataset of in situ vertical profiles for deriving a climatology of the impact of biomass burning versus anthropogenic emissions on the strongest CO anomalies observed in the troposphere, in combination with information on the source regions. This study therefore provides both qualitative and quantitative information for interpreting the highly variable CO vertical distribution in several regions of interest.</p>


2015 ◽  
Vol 15 (22) ◽  
pp. 32323-32365 ◽  
Author(s):  
G. Ancellet ◽  
J. Pelon ◽  
J. Totems ◽  
P. Chazette ◽  
A. Bazureau ◽  
...  

Abstract. Long range transport of biomass burning (BB) aerosols between North America and the Mediterranean region took place in June 2013. A large number of ground based and airborne lidar measurements were deployed in the Western Mediterranean during the Chemistry-AeRosol Mediterranean EXperiment (ChArMEx) intensive observation period. A detailed analysis of the potential North American aerosol sources is conducted including the assessment of their transport to Europe using forward simulations of the FLEXPART Lagrangian particle dispersion model initialized using satellite observations by MODIS and CALIOP. The three dimensional structure of the aerosol distribution in the ChArMEx domain observed by the ground-based lidars (Menorca, Barcelona and Lampedusa), a Falcon-20 aircraft flight and three CALIOP tracks, agree very well with the model simulation of the three major sources considered in this work: Canadian and Colorado fires, a dust storm from Western US and the contribution of Saharan dust streamers advected from the North Atlantic trade wind region into the Westerlies region. Four aerosol types were identified using the optical properties of the observed aerosol layers (aerosol depolarization ratio, lidar ratio) and the transport model analysis of the contribution of each aerosol source: (I) pure BB layer, (II) weakly dusty BB, (III) significant mixture of BB and dust transported from the trade wind region (IV) the outflow of Saharan dust by the subtropical jet and not mixed with BB aerosol. The contribution of the Canadian fires is the major aerosol source during this episode while mixing of dust and BB is only significant at altitude above 5 km. The mixing corresponds to a 20–30 % dust contribution in the total aerosol backscatter. The comparison with the MODIS AOD horizontal distribution during this episode over the Western Mediterranean sea shows that the Canadian fires contribution were as large as the direct northward dust outflow from Sahara.


2018 ◽  
Author(s):  
Xinyi Dong ◽  
Joshua S. Fu ◽  
Qingzhao Zhu ◽  
Jian Sun ◽  
Jiani Tan ◽  
...  

Abstract. Haze has been severely affecting the densely populated areas in China during recent years. While many of the pilot studies have been devoted to investigate the contributions from local anthropogenic emission, limited attention has been paid to the influence from long-range transport. In this study, we use simulations from 6 participating models supplied through the Task Force on Hemispheric Transport of Air Pollution Phase 2 (HTAP2) exercise to investigate the long-range transport impact of Europe and Russia/Belarussia/Ukraine on the surface air quality in East Asia, with special focus on their contributions during the haze episodes over China. The impact of 20 % anthropogenic emission perturbation from the source region is extrapolated by a factor of 5 to estimate the full impact. We find that the full impacts from EUR and RBU are 0.99 µg/m3 (3.1 %) and 1.32 µg/m3 (4.1 %) respectively during haze episodes, while the annual averaged full impacts are only 0.35 µg m3 (1.7 %) and 0.53 µg/m3 (2.6 %) respectively. By estimating the aerosol response within and above the planetary boundary layer (PBL), we find that long-range transport within the PBL contributes to 22–38 % of the total column density of aerosol response. Comparison with the HTAP Phase 1 (HTAP1) assessment reveals that from 2000 to 2010, the long-range transport from Europe to East Asia has decreased significantly by a factor of 2–10 for surface aerosol mass concentration due to the simultaneous emission reduction in source region and emission increase in the receptor region. By investigating the visibility response, we find that the long-range transport from the Europe and RBU region increases the number of haze events in China by 0.15 % and 0.11 % respectively, and the North China Plain and southeast China receives 1–3 extra haze days. This study is the first investigation into the contribution of long-range transport to haze in China with multiple model experiments.


Atmosphere ◽  
2019 ◽  
Vol 11 (1) ◽  
pp. 48 ◽  
Author(s):  
Changhan Bae ◽  
Byeong-Uk Kim ◽  
Hyun Cheol Kim ◽  
Chul Yoo ◽  
Soontae Kim

This study identified the key chemical components based on an analysis of the seasonal variations of ground level PM2.5 concentrations and its major chemical constituents (sulfate, nitrate, ammonium, organic carbon, and elemental carbon) in the Seoul Metropolitan Area (SMA), over a period of five years, ranging from 2012 to 2016. It was found that the mean PM2.5 concentration in the SMA was 33.7 μg/m3, while inorganic ions accounted for 53% of the total mass concentration. The component ratio of inorganic ions increased by up to 61%–63% as the daily mean PM2.5 concentration increased. In spring, nitrate was the dominant component of PM2.5, accounting for 17%–32% of the monthly mean PM2.5 concentrations. In order to quantify the impact of long-range transport on the SMA PM2.5, a set of sensitivity simulations with the community multiscale air-quality model was performed. Results show that the annual averaged impact of Chinese emissions on SMA PM2.5 concentrations ranged from 41% to 44% during the five years. Chinese emissions’ impact on SMA nitrate ranged from 50% (winter) to 67% (spring). This result exhibits that reductions in SO2 and NOX emissions are crucial to alleviate the PM2.5 concentration. It is expected that NOX emission reduction efforts in China will help decrease PM2.5 concentrations in the SMA.


2017 ◽  
Author(s):  
Zhe Jiang ◽  
Helen Worden ◽  
John R. Worden ◽  
Daven K. Henze ◽  
Dylan B. A. Jones ◽  
...  

Abstract. Decreases in surface emissions of nitrogen oxides (NOx = NO + NO2) in North America have led to substantial improvements in air-quality over the last several decades. Here we show that satellite observations of tropospheric nitrogen dioxide (NO2) columns over the contiguous United States (US) do not decrease after about 2009, while surface NO2 concentrations continue to decline through to the present. This divergence, if it continues, could have a substantial impact on surface air quality due to mixing of free-tropospheric air into the boundary layer. Our results show only limited contributions from local effects such as fossil fuel emissions, lightning, or instrument artifacts, but we do find a possible relationship of NO2 changes to decadal climate variability. Our analysis demonstrates that the intensity of transpacific transport is stronger in El Niño years and weaker in La Niña years, and consequently, that decadal-scale climate variability impacts the contribution of Asian emissions on North American atmospheric composition. Because of the short lifetime, it is usually believed that the direct contribution of long-range transport to tropospheric NOx distribution is limited. If our hypothesis about transported Asian emissions is correct, then this observed divergence between satellite and surface NOx could indicate mechanisms that allow for either NOx or its reservoir species to have a larger than expected effect on North American tropospheric composition. These results therefore suggest more aircraft and satellite studies to determine the possible missing processes in our understanding of the long-range transport of tropospheric NOx.


1997 ◽  
Vol 102 (D23) ◽  
pp. 28637-28649 ◽  
Author(s):  
Yoshizumi Kajii ◽  
Hajime Akimoto ◽  
Yuichi Komazaki ◽  
Shigeru Tanaka ◽  
Hitoshi Mukai ◽  
...  

2007 ◽  
Vol 7 (7) ◽  
pp. 1707-1718 ◽  
Author(s):  
S. Matthes ◽  
V. Grewe ◽  
R. Sausen ◽  
G.-J. Roelofs

Abstract. Road traffic is one of the major anthropogenic emission sectors for NOx, CO and NMHCs (non-methane hydrocarbons). We applied ECHAM4/CBM, a general circulation model coupled to a chemistry module, which includes higher hydrocarbons, to investigate the global impact of 1990 road traffic emissions on the atmosphere. Improving over previous global modelling studies, which concentrated on road traffic NOx and CO emissions only, we assess the impact of NMHC emissions from road traffic. It is revealed that NMHC emissions from road traffic play a key role for the impact on ozone. They are responsible for (indirect) long-range transport of NOx from road traffic via the formation of PAN, which is not found in a simulation without NMHC emissions from road traffic. Long-range transport of NMHC-induced PAN impacts on the ozone distribution in Northern Hemisphere regions far away from the sources, especially in arctic and remote maritime regions. In July total road traffic emissions (NOx, CO and NMHCs) contribute to the zonally averaged ozone distribution by more than 12% near the surface in the Northern Hemisphere midlatitudes and arctic latitudes. In January road traffic emissions contribute near the surface in northern and southern extratropics more than 8%. Sensitivity studies for regional emission show that effective transport of road traffic emissions occurs mainly in the free troposphere. In tropical latitudes of America up to an altitude of 200 hPa, global road traffic emissions contribute about 8% to the ozone concentration. In arctic latitudes NMHC emissions from road transport are responsible for about 90% of PAN increase from road transport, leading to a contribution to ozone concentrations of up to 15%.


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