scholarly journals Modeling regional aerosol variability over California and its sensitivity to emissions and long-range transport during the 2010 CalNex and CARES campaigns

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.

2014 ◽  
Vol 14 (18) ◽  
pp. 10013-10060 ◽  
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 the extensive meteorological, trace gas, and aerosol 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 overall objective of the field campaigns was to obtain data needed to better understand processes that affect both climate and air quality, including emission assessments, transport and chemical aging of aerosols, aerosol radiative effects. Simulations were performed that examined the sensitivity of 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. 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. 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 quantifying 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 2 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 data sets are an ideal test bed that can be used to evaluate aerosol models in great detail and develop improved treatments for aerosol processes.


2020 ◽  
Vol 20 (16) ◽  
pp. 10047-10062 ◽  
Author(s):  
Samantha J. Kramer ◽  
Claudia Alvarez ◽  
Anne E. Barkley ◽  
Peter R. Colarco ◽  
Lillian Custals ◽  
...  

Abstract. North African dust reaches the southeastern United States every summer. Size-resolved dust mass measurements taken in Miami, Florida, indicate that more than one-half of the surface dust mass concentrations reside in particles with geometric diameters less than 2.1 µm, while vertical profiles of micropulse lidar depolarization ratios show dust reaching above 4 km during pronounced events. These observations are compared to the representation of dust in the Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) aerosol reanalysis and closely related Goddard Earth Observing System model version 5 (GEOS-5) Forward Processing (FP) aerosol product, both of which assimilate satellite-derived aerosol optical depths using a similar protocol and inputs. These capture the day-to-day variability in aerosol optical depth well, in a comparison to an independent sun-photometer-derived aerosol optical depth dataset. Most of the modeled dust mass resides in diameters between 2 and 6 µm, in contrast to the measurements. Model-specified mass extinction efficiencies equate light extinction with approximately 3 times as much aerosol mass, in this size range, compared to the measured dust sizes. GEOS-5 FP surface-layer sea salt mass concentrations greatly exceed observed values, despite realistic winds and relative humidities. In combination, these observations help explain why, despite realistic total aerosol optical depths, (1) free-tropospheric model volume extinction coefficients are lower than those retrieved from the micro-pulse lidar, suggesting too-low model dust loadings in the free troposphere, and (2) model dust mass concentrations near the surface can be higher than those measured. The modeled vertical distribution of dust, when captured, is reasonable. Large, aspherical particles exceeding the modeled dust sizes are also occasionally present, but dust particles with diameters exceeding 10 µm contribute little to the measured total dust mass concentrations after such long-range transport. Remaining uncertainties warrant a further integrated assessment to confirm this study's interpretations.


2020 ◽  
Author(s):  
Samantha J. Kramer ◽  
Claudia Alvarez ◽  
Anne Barkley ◽  
Peter R. Colarco ◽  
Lillian Custals ◽  
...  

Abstract. North African dust reaches the southeast United States every summer. Measurements taken in Miami, Florida indicate that more than one-half of the surface dust mass concentrations reside in particles with diameters less than 2.1 μm, while vertical profiles of micropulse lidar depolarization ratios show dust reaching above four km during pronounced events. These observations are compared to the representation of dust in the MERRA-2 aerosol reanalysis and closely-related GEOS-5 Forward Processing (FP) aerosol product, both of which assimilate satellite-derived aerosol optical depths using a similar protocol and inputs. These capture the day-to-day variability in aerosol optical depth well, in a comparison to an independent sun-photometer-derived aerosol optical depth dataset. Measured near-surface dust mass concentrations slightly exceed model values, with most of the modeled dust mass in diameters between 2–6 μm. Modeled-specified mass extinction efficiencies equate light extinction with approximately three times as much aerosol mass, in this size range, compared to the measured dust sizes. GEOS-5 FP surface-layer sea salt mass concentrations greatly exceed observed values, despite realistic winds and relative humidities. In combination, these observations help explain, why, despite realistic total aerosol optical depths, 1) free-tropospheric model volume extinction coefficients are lower than those retrieved from the micro-pulse lidar, suggesting too low model dust loadings, and 2) model dust mass concentrations near the surface are higher than those measured. The modeled vertical distribution of dust, when captured, is reasonable. Large, aspherical particles exceeding the modeled dust sizes are also occasionally present, but dust particles with diameters exceeding ten μm contribute little to the measured total dust mass concentrations after such long-range transport. A further integrated assessment is needed to confirm this study's interpretations.


2017 ◽  
Vol 17 (21) ◽  
pp. 13233-13263 ◽  
Author(s):  
Uri Dayan ◽  
Philippe Ricaud ◽  
Régina Zbinden ◽  
François Dulac

Abstract. The eastern Mediterranean (EM) is one of the regions in the world where elevated concentrations of primary and secondary gaseous air pollutants have been reported frequently, mainly in summer. This review discusses published studies of the atmospheric dispersion and transport conditions characterizing this region during the summer, followed by a description of some essential studies dealing with the corresponding concentrations of air pollutants such as ozone, carbon monoxide, total reactive nitrogen, methane, and sulfate aerosols observed there. The interlaced relationship between the downward motion of the subsiding air aloft induced by global circulation systems affecting the EM and the depth of the Persian Trough, a low-pressure trough that extends from the Asian monsoon at the surface controlling the spatiotemporal distribution of the mixed boundary layer during summer, is discussed. The strength of the wind flow within the mixed layer and its depth affect much the amount of pollutants transported and determine the potential of the atmosphere to disperse contaminants off their origins in the EM. The reduced mixed layer and the accompanying weak westerlies, characterizing the summer in this region, led to reduced ventilation rates, preventing an effective dilution of the contaminants. Several studies pointing at specific local (e.g., ventilation rates) and regional peculiarities (long-range transport) enhancing the build-up of air pollutant concentrations are presented. Tropospheric ozone (O3) concentrations observed in the summer over the EM are among the highest over the Northern Hemisphere. The three essential processes controlling its formation (i.e., long-range transport of polluted air masses, dynamic subsidence at mid-tropospheric levels, and stratosphere-to-troposphere exchange) are reviewed. Airborne campaigns and satellite-borne initiatives have indicated that the concentration values of reactive nitrogen identified as precursors in the formation of O3 over the EM were found to be 2 to 10 times higher than in the hemispheric background troposphere. Several factors favor sulfate particulate abundance over the EM. Models, aircraft measurements, and satellite-derived data have clearly shown that sulfate has a maximum during spring and summer over the EM. The carbon monoxide (CO) seasonal cycle, as obtained from global background monitoring sites in the EM, is mostly controlled by the tropospheric concentration of the hydroxyl radical (OH) and therefore demonstrates high concentrations over winter months and the lowest concentrations during summer when photochemistry is active. Modeling studies have shown that the diurnal variations in CO concentration during the summer result from long-range CO transport from European anthropogenic sources, contributing 60 to 80 % of the boundary-layer CO over the EM. The values retrieved from satellite data enable us to derive the spatial distribution of methane (CH4), identifying August as the month with the highest levels over the EM. The outcomes of a recent extensive examination of the distribution of methane over the tropospheric Mediterranean Basin, as part of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx) program, using model simulations and satellite measurements, are coherent with other previous studies. Moreover, this methane study provides some insight into the role of the Asian monsoon anticyclone in controlling the variability of CH4 pollutant within mid-to-upper tropospheric levels above the EM in summer.


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>


2021 ◽  
Vol 21 (1) ◽  
pp. 357-392
Author(s):  
Igor B. Konovalov ◽  
Nikolai A. Golovushkin ◽  
Matthias Beekmann ◽  
Meinrat O. Andreae

Abstract. Long-range transport of biomass burning (BB) aerosol from regions affected by wildfires is known to have a significant impact on the radiative balance and air quality in receptor regions. However, the changes that occur in the optical properties of BB aerosol during long-range transport events are insufficiently understood, limiting the adequacy of representations of the aerosol processes in chemistry transport and climate models. Here we introduce a framework to infer and interpret changes in the optical properties of BB aerosol from satellite observations of multiple BB plumes. Our framework includes (1) a procedure for analysis of available satellite retrievals of the absorption and extinction aerosol optical depths (AAOD and AOD) and single-scattering albedo (SSA) as a function of the BB aerosol photochemical age and (2) a representation of the AAOD and AOD evolution with a chemistry transport model (CTM) involving a simplified volatility basis set (VBS) scheme with a few adjustable parameters. We apply this framework to analyze a large-scale outflow of BB smoke plumes from Siberia toward Europe that occurred in July 2016. We use AAOD and SSA data derived from OMI (Ozone Monitoring Instrument) satellite measurements in the near-UV range along with 550 nm AOD and carbon monoxide (CO) columns retrieved from MODIS (Moderate Resolution Imaging Spectroradiometer) and IASI (Infrared Atmospheric Sounding Interferometer) satellite observations, respectively, to infer changes in the optical properties of Siberian BB aerosol due to its atmospheric aging and to get insights into the processes underlying these changes. Using the satellite data in combination with simulated data from the CHIMERE CTM, we evaluate the enhancement ratios (EnRs) that allow isolating AAOD and AOD changes due to oxidation and gas–particle partitioning processes from those due to other processes, including transport, deposition, and wet scavenging. The behavior of EnRs for AAOD and AOD is then characterized using nonlinear trend analysis. It is found that the EnR for AOD strongly increases (by about a factor of 2) during the first 20–30 h of the analyzed evolution period, whereas the EnR for AAOD does not exhibit a statistically significant increase during this period. The increase in AOD is accompanied by a statistically significant enhancement of SSA. Further BB aerosol aging (up to several days) is associated with a strong decrease in EnRs for both AAOD and AOD. Our VBS simulations constrained by the observations are found to be more consistent with satellite observations of strongly aged BB plumes than “tracer” simulations in which atmospheric transformations of BB organic aerosol were disregarded. The simulation results indicate that the upward trends in EnR for AOD and in SSA are mainly due to atmospheric processing of secondary organic aerosol (SOA), leading to an increase in the mass scattering efficiency of BB aerosol. Evaporation and chemical fragmentation of the SOA species, part of which is assumed to be absorptive (to contain brown carbon), are identified as likely reasons for the subsequent decrease in the EnR for both AAOD and AOD. Hence, our analysis reveals that the long-range transport of smoke plumes from Siberian fires is associated with major changes in BB aerosol optical properties and chemical composition. Overall, this study demonstrates the feasibility of using available satellite observations for evaluating and improving representations in atmospheric models of the BB aerosol aging processes in different regions of the world at much larger temporal scales than those typically addressed in aerosol chamber experiments.


2019 ◽  
Author(s):  
Rachel A. Braun ◽  
Mojtaba Azadi Aghdam ◽  
Paola Angela Bañaga ◽  
Grace Betito ◽  
Maria Obiminda Cambaliza ◽  
...  

Abstract. This study analyzes mechanisms of long-range transport of aerosol and aerosol chemical characteristics in and around East and Southeast Asia. Ground-based size-resolved aerosol measurements collected at the Manila Observatory in Metro Manila, Philippines from July–October 2018 were used to identify and contrast high and low aerosol loading events. Multiple data sources, including models, remote-sensing, and in situ measurements, are used to analyze the impacts of long-range aerosol transport on Metro Manila and the conditions at the local and synoptic scales facilitating this transport. Evidence of long-range transport of biomass burning aerosol from the Maritime Continent was identified through model results and the presence of biomass burning tracers (e.g. K, Rb) in the ground-based measurements. The impacts of emissions transported from continental East Asia are also identified; for one of the events analyzed, this transport was facilitated by the nearby passage of a typhoon. Changes in the aerosol size distributions, water-soluble chemical composition, and contributions of various organic aerosol species to the total water-soluble organic aerosol were examined for the different cases. The events impacted by biomass burning transport had the overall highest concentration of water-soluble organic acids, while the events impacted by long-range transport from continental East Asia, showed high percent contributions from shorter chain dicarboxylic acids (i.e. oxalate) that are often representative of photochemical and aqueous processing in the atmosphere. The low aerosol loading event was subject to a larger precipitation accumulation than the high aerosol events, indicative of wet scavenging as an aerosol sink in the study region. This low aerosol event was characterized by a larger relative contribution from supermicrometer aerosols and had a higher percent contribution from longer-chain dicarboxylic acids (i.e. maleate) to the water-soluble organic aerosol fraction. Results of this study have implications for better understanding of the transport and chemical characteristics of aerosol in a highly-populated region that has thus far been difficult to measure through remote-sensing methods. Furthermore, findings associated with the effects of air mass mixing on aerosol physiochemical properties are applicable to other global regions impacted by both natural and anthropogenic sources.


2017 ◽  
Author(s):  
Uri Dayan ◽  
Philippe Ricaud ◽  
Regina Zbinden ◽  
Francois Dulac

Abstract. The Eastern Mediterranean (EM) is one of the regions in the world where elevated concentrations of primary and secondary gaseous air pollutants have been reported frequently, mainly in summer. This review discusses published studies of the atmospheric dispersion and transport conditions characterizing this region during the summer, followed by a description of some essential studies dealing with the corresponding concentrations of air pollutants such as ozone, carbon monoxide, total reactive nitrogen, methane and sulfate aerosols observed there. The interlaced relationship between the downward motion of the subsiding air aloft induced by global circulation systems affecting the EM and the depth of the Persian Trough, a low-pressure trough that extends from the Asian monsoon at the surface controlling the spatio-temporal distribution of the mixed boundary layer during summer is discussed. The strength of the wind flow within the mixed layer and its depth affect much the amount of pollutants transported and determine the potential of the atmosphere to disperse contaminants off their origins in the EM. The reduced mixed layer and the accompanying weak westerlies, characterizing the summer in this region, lead to reduced ventilation rates, preventing an effective dilution of the contaminants. Several studies pointing at specific local (e.g. ventilation rates) and regional peculiarities (long-range transport) enhancing the building up of pollutant concentrations are presented. Tropospheric ozone concentrations observed in the summer over the EM are among the highest over the Northern Hemisphere. The three essential processes controlling its formation (i.e., long- range transport of polluted air masses, dynamic subsidence at mid-tropospheric levels, and stratosphere-to-troposphere exchange) are reviewed. Airborne campaigns and satellite-borne initiatives have indicated that the concentration values of reactive nitrogen identified as precursors in the formation of ozone over the EM were found to be 2 to 10 times higher than in the hemispheric background troposphere. Several factors favor sulfate particulate abundance over the EM. Models, aircraft measurements, and satellite derived data, have clearly shown that sulfate has a maximum during spring and summer over the EM. The carbon monoxide (CO) seasonal cycle, as obtained from global background monitoring sites in the EM is mostly controlled by the tropospheric concentration of the hydroxyl radical (OH), and therefore demonstrates high concentrations over winter months and the lowest during summer when photochemistry is active. Modeling studies have shown that the diurnal variations in CO concentration during the summer result from long-range CO transport from European anthropogenic sources, contributing 60 to 80 % of the boundary-layer CO over the EM. The values retrieved from satellite data enable us to derive the spatial distribution of methane (CH4), identifying August as the month with the highest levels over the EM. The outcomes of a recent extensive examination of the distribution of methane over the tropospheric Mediterranean Basin, as part of the Chemical and Aerosol Mediterranean Experiment (ChArMEx) program, using model simulations and satellite measurements is coherent with other previous studies. Moreover, this methane study provides some insights on the role of the Asian monsoon anticyclone in controlling the variability of CH4 pollutant within mid-to-upper tropospheric levels above the EM in summer.


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

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