scholarly journals Unexpected long-range transport of glyoxal and formaldehyde observed from the Copernicus Sentinel-5 Precursor satellite during the 2018 Canadian wildfires

2019 ◽  
Author(s):  
Leonardo M. A. Alvarado ◽  
Andreas Richter ◽  
Mihalis Vrekoussis ◽  
Andreas Hilboll ◽  
Anna B. Kalisz Hedegaard ◽  
...  

Abstract. Glyoxal (CHO.CHO) and formaldehyde (HCHO) are intermediate products in the oxidation of the majority of volatile organic compounds (VOC). CHO.CHO is also a precursor of secondary organic aerosol (SOA) formation in the atmosphere. These VOCs are released from biogenic, anthropogenic, and pyrogenic sources. CHO.CHO and HCHO tropospheric lifetimes are short during the daytime and at mid-latitudes (few hours), as they are rapidly removed from the atmosphere by their photolysis, oxidation by OH, and uptake on particles/deposition. During nighttime or at high latitudes, lifetime can be prolonged to many hours or even days. Previous studies demonstrated that CHO.CHO and HCHO can be retrieved from space-borne observations using the DOAS method. In this study, we present CHO.CHO and HCHO columns retrieved from measurements of the TROPOMI instrument, launched recently on the Sentinel-5 Precursor (S5P) platform in October 2017. Strongly elevated amounts of CHO.CHO and HCHO are observed during the fire season in British Columbia Canada, where a large number of fires occurred in August 2018. CHO.CHO and HCHO plumes from individual fire hot-spots are observed in air masses travelling over distances of up to 1500 km, i.e. much longer than expected for the short atmospheric lifetime of CHO.CHO and HCHO. However, the temporal evolution of the plume differs for both species. Comparison with Lagrangian-based FLEXPART simulations for particles with different lifetimes shows that effective lifetimes of 20 hours and more are needed to explain the observations, indicating that CHO.CHO and HCHO are either efficiently recycled during transport or, continuously formed from the oxidation of longer-lived precursors present in the plume.

2020 ◽  
Vol 20 (4) ◽  
pp. 2057-2072 ◽  
Author(s):  
Leonardo M. A. Alvarado ◽  
Andreas Richter ◽  
Mihalis Vrekoussis ◽  
Andreas Hilboll ◽  
Anna B. Kalisz Hedegaard ◽  
...  

Abstract. Glyoxal (CHOCHO) and formaldehyde (HCHO) are intermediate products in the tropospheric oxidation of the majority of volatile organic compounds (VOCs). CHOCHO is also a precursor of secondary organic aerosol (SOA) in the atmosphere. CHOCHO and HCHO are released from biogenic, anthropogenic, and pyrogenic sources. CHOCHO and HCHO tropospheric lifetimes are typically considered to be short during the daytime at mid-latitudes (e.g. several hours), as they are rapidly removed from the atmosphere by their photolysis, oxidation by OH, and uptake on particles or deposition. At night and at high latitudes, tropospheric lifetimes increase to many hours or even days. Previous studies demonstrated that CHOCHO and HCHO vertical column densities (VCDs) are well retrieved from space-borne observations using differential optical absorption spectroscopy (DOAS). In this study, we present CHOCHO and HCHO VCDs retrieved from measurements by TROPOMI (TROPOspheric Monitoring Instrument), launched on the Sentinel-5 Precursor (S5P) platform in October 2017. We observe strongly elevated amounts of CHOCHO and HCHO during the 2018 fire season in British Columbia, Canada, where a large number of fires occurred in August. CHOCHO and HCHO plumes from individual fire hot spots are observed in air masses travelling over distances of up to 1500 km, i.e. much longer than expected for the relatively short tropospheric lifetime expected for CHOCHO and HCHO. Comparison with simulations by the particle dispersion model FLEXPART (FLEXible PARTicle dispersion model) indicates that effective lifetimes of 20 h and more are needed to explain the observations of CHOCHO and HCHO if they decay in an effective first-order process. FLEXPART used in the study calculates accurately the transport. In addition an exponential decay, in our case assumed to be photochemical, of a species along the trajectory is added. We have used this simple approach to test our assumption that CHOCHO and HCHO are created in the fires and then decay at a constant rate in the plume as it is transported. This is clearly not the case and we infer that CHOCHO and HCHO are either efficiently recycled during transport or continuously formed from the oxidation of longer-lived precursors present in the plume, or possibly a mixture of both. We consider the best explanation of the observed CHOCHO and HCHO VCD in the plumes of the fire is that they are produced by oxidation of longer-lived precursors, which were also released by the fire and present in the plume.


2012 ◽  
Vol 12 (11) ◽  
pp. 29475-29533 ◽  
Author(s):  
Q. J. Zhang ◽  
M. Beekmann ◽  
F. Drewnick ◽  
F. Freutel ◽  
J. Schneider ◽  
...  

Abstract. Results of the chemistry transport model CHIMERE are compared with the measurements performed during the MEGAPOLI summer campaign in the Greater Paris Region in July, 2009. The Volatility-Basis-Set approach (VBS) is implemented into this model, taking into account the volatility of primary organic aerosol (POA) and the chemical aging of semi-volatile organic species. Organic aerosol is the main focus and is simulated with three different configurations related to the volatility of POA and the scheme of secondary organic aerosol (SOA) formation. In addition, two types of emission inventories are used as model input in order to test the uncertainty related to the emissions. Predictions of basic meteorological parameters and primary and secondary pollutant concentrations are evaluated and four pollution regimes according to the air mass origin are defined. Primary pollutants are generally overestimated, while ozone is consistent with observations. Sulfate is generally overestimated, while ammonium and nitrate levels are well simulated with the refined emission data set. As expected, the simulation with non-volatile POA and a single-step SOA formation mechanism largely overestimates POA and underestimates SOA. Simulation of organic aerosol with the VBS approach taking into account the aging of semi-volatile organic compounds (SVOC) shows the best correlation with measurements. All observed high concentration events are reproduced by the model mostly after long range transport, indicating that long range transport of SOA to Paris is well reproduced. Depending on the emission inventory used, simulated POA levels are either reasonable or underestimated, while SOA levels tend to be overestimated. Several uncertainties related to the VBS scheme (POA volatility, SOA yields, the aging parameterization), to emission input data, and to simulated OH levels can be responsible for this behavior. Despite these uncertainties, the implementation of the VBS scheme into the CHIMERE model allowed for much more realistic organic aerosol simulations for Paris during summer time. The advection of SOA from outside Paris is mostly responsible for the highest OA concentration levels. During advection of polluted air masses from north-east (Benelux and Central Europe), simulations indicate high levels of both anthropogenic and biogenic SOA fractions, while biogenic SOA dominates during days with advection from Southern France and Spain.


2017 ◽  
Author(s):  
Xiaobin Xu ◽  
Hualong Zhang ◽  
Weili Lin ◽  
Ying Wang ◽  
Shihui Jia

Abstract. Both peroxyacetyl nitrate (PAN) and ozone (O3) are key photochemical products in the atmosphere. Most of the previous in-situ observations of both gases have been made in polluted regions and at low altitude sites. Here we present first simultaneous measurements of PAN and O3 at Nam Co (NMC, 90°57′ E, 30°46′ N, 4745 m  a.s.l.), a remote site in the central Tibetan Plateau (TP). The observations were made during summer periods in 2011 and 2012. The PAN concentrations averaged 0.36 ppb (range: 0.11–0.76 ppb) and 0.44 ppb (range: 0.21–0.99 ppb) during 16–25 August 2011 and 15 May to 13 July 2012, respectively. The O3 concentration varied from 27.9 ppb to 96.4 ppb, with an average of 60.0 ppb. Profound diurnal cycles of PAN and O3 were observed, with minimum values around 05:00 LT, steep rises in the early morning, and broader platforms of high values during 09:00–20:00 LT. We find that the evolution of planetary boundary layer (PBL) played a key role in shaping the diurnal patterns of both gases, particularly the rapid increases of PAN and O3 in the early morning. Air entrainment from the free troposphere into the PBL seemed to cause the early morning increase and be a key factor of sustaining the daytime high concentrations of both gases. The days with higher daytime PBL (about 3 km) showed stronger diurnal variations of both gases and were mainly distributed in the drier pre-monsoon period, while those with shallower daytime PBL (about 2 km) showed minor diurnal variations of both gases and were mainly distributed in the humid monsoon period. Episodes of higher PAN levels were observed occasionally at NMC. These PAN episodes were caused either by rapid downward transport of air masses from the middle/upper troposphere or by long-range transport of PAN plumes from North India. The PAN level in the downward transport cases ranged from 0.5 ppb to 0.7 ppb and may indicate the PAN abundance in the middle/upper troposphere. In the long-range transport case, the PAN level varied in the range of 0.6–1.0 ppb. This long-range transport process influenced most of the western and central TP region for about a week in early June 2012. Our results suggest that polluted air masses from South Asia can significantly enhance the PAN level over the TP. As PAN act as a reservoir of NOx, the impacts of pollution transport from South Asia on tropospheric photochemistry over the TP region deserve further studies.


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.


2021 ◽  
Author(s):  
Ivana Tucaković ◽  
Sarah Mateša ◽  
Ivana Coha ◽  
Marija Marguš ◽  
Milan Čanković ◽  
...  

<p>Croatian Science Foundation MARRES project (MARine lake (Rogoznica) as a model for EcoSystem functioning in a changing environment) aims to investigate the unique environment (slow exchange of seawater with the sea; atmospheric input is the only source of freshwater) of the marine lake which is an example of highly stratified (permanent anoxia bellow 9 m depth), and by climate changes affected marine system in the middle of the eastern Adriatic coast (43.53° N, 15.95° E). The area of the lake is characterized by the extensive tourism and mariculture, and the low impact of local industrial activities. It is also affected by the combined influence of long-range transport of air masses and local emissions (open-fire events).</p><p>An important part of the project is focused on the exchange and interaction between atmosphere, water column and sediment by measuring the atmospheric input (wet and dry deposition) of sulphur compounds, organic carbon, trace metals and radionuclides (Be-7, Pb-210).</p><p>This work for the first time will present the current state of the measurements of radioactivity in the Rogoznica lake area, including samples of aerosol particulate matter, PM2.5 < 2.5 um, rainwater and lake water column. Namely, the concentrations of Be-7 and Pb-210 in PM2.5 are measured to determine and correlate the dynamics of particle transport, meteorological information, especially origin of air masses and seasonal variation of PM2.5. While presence of Be-7 indicates the recent wet or dry deposition from the upper parts of the atmosphere, Pb-210 may be used as a tracer for continental air masses. Therefore, it can also indicate the influence of the pollution induced by human activity. Regarding that, special attention will be paid to compare results before and during the Covid-19 lockdown periods.</p><p>So far, preliminary results do not show significant difference in PM2.5 masses and measured radionuclide activity concentrations for the lockdown period. Be-7 and Pb-210 were regularly detected in aerosols collected on a glass fiber filters during a one-week sampling periods with the air flow rate of 2.3 m<sup>3</sup>/h. Their activity concentrations are determined by gamma spectrometry using High Purity Germanium detectors. The results are found to be correlated with PM2.5 masses, ranging from 2.9 to 12.2 Bq/m<sup>3</sup> for Be-7 and from 0.5 to 2.5 Bq/m<sup>3</sup> for Pb-210. First analyses show that the highest values can be related to the long-range transport of air masses and to the recorded near open-fire event. As expected, Be-7 is also detected in almost every rainwater sample (event), with the activity concentration up to 5.6 Bq/L, while low activities of Pb-210 are detected only sporadically. Related to that, Be-7 is detected in lake water column as well, but only in the surface layer and in samples collected during, or immediately after the rain events. </p><p>Dynamics and seasonal variation of radionuclide activity concentrations in here studied samples will be discussed, and the relationships with some meteorological parameters (temperature, wind speed, relative humidity, precipitation level) as well as local and long-range transport and physico-chemical conditions in the lake water column will be established.</p>


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.


2006 ◽  
Vol 14 (3) ◽  
pp. 169-186 ◽  
Author(s):  
Eiliv Steinnes ◽  
Andrew J Friedland

This review focuses on the long-range atmospheric transport of metals to organic-rich surface soils (mostly 50–90% organic matter) in the temperate, coniferous, and boreal zones of North America and Europe. From various air-pollution related measurements (air, precipitation, moss, peat cores) Pb and Zn are known to be transported long distances in the air in large amounts. Arsenic, Cd, Hg, Sb, and Se are also typical representatives of long-range transported air masses, and there is evidence that Ag, Bi, In, Mo, Tl, and W belong to this group of elements. Through the use of “environmental archives” such as ice and peat cores it has become evident that long-range transport of pollutants and associated contamination of natural surfaces is not just a recent phenomenon. There is compelling evidence for widespread enrichment of surface soil horizons in Pb from long-range transport, and many studies support enrichment of Zn. Mercury is also generally elevated by anthropogenic emissions over natural levels in organic-rich surface soils, whereas results for Cd are less conclusive. There is evidence that As, Se, Ag, Mo, In, Sb, W, Tl, and Bi all are subject to some enrichment in organic-rich surface soils from long-range atmospheric transport, but studies are still few for most of these elements. With the exception of Pb, little is known about residence times of the elements in the organic-rich surface horizon, and more research is needed on this topic. Further studies are desirable on the temporal and spatial trends in supply of the above elements, which are poorly known in large parts of the northern temperate zone.Key words: natural soils, metals, long-range atmospheric transport, organic matter, lead, zinc, cadmium, mercury.


2016 ◽  
Vol 16 (5) ◽  
pp. 3013-3032 ◽  
Author(s):  
Narendra Ojha ◽  
Andrea Pozzer ◽  
Armin Rauthe-Schöch ◽  
Angela K. Baker ◽  
Jongmin Yoon ◽  
...  

Abstract. We compare in situ measurements of ozone (O3) and carbon monoxide (CO) profiles from the CARIBIC program with the results from the regional chemistry transport model (WRF-Chem) to investigate the role of local and regional emissions and long-range transport over southern India during the summer monsoon of 2008. WRF-Chem successfully reproduces the general features of O3 and CO distributions over the South Asian region. However, absolute CO concentrations in the lower troposphere are typically underestimated. Here we investigate the influence of local relative to remote emissions through sensitivity simulations. The influence of 50 % increased CO emissions over South Asia leads to a significant enhancement (upto 20 % in July) in upper tropospheric CO in the northern and central Indian regions. Over Chennai in southern India, this causes a 33 % increase in surface CO during June. However, the influence of enhanced local and regional emissions is found to be smaller (5 %) in the free troposphere over Chennai, except during September. Local to regional emissions are therefore suggested to play a minor role in the underestimation of CO by WRF-Chem during June–August. In the lower troposphere, a high pollution (O3: 146.4 ± 12.8, CO: 136.4 ± 12.2 nmol mol−1) event (15 July 2008), not reproduced by the model, is shown to be due to transport of photochemically processed air masses from the boundary layer in southern India. A sensitivity simulation combined with backward trajectories indicates that long-range transport of CO to southern India is significantly underestimated, particularly in air masses from the west, i.e., from Central Africa. This study highlights the need for more aircraft-based measurements over India and adjacent regions and the improvement of global emission inventories.


2020 ◽  
Author(s):  
Arman Pouyaei ◽  
Yunsoo Choi ◽  
Jia Jung ◽  
Bavand Sadeghi ◽  
Chul Han Song

Abstract. This paper introduces a reliable and comprehensive Lagrangian output (Concentration Trajectory Route of Air pollution with Integrated Lagrangian model, C-TRAIL version 1.0) from an Eulerian air quality model for validating the source-receptor link by following real polluted air masses. To investigate the concentrations and trajectories of air masses simultaneously, we implement the trajectory-grid (TG) Lagrangian advection scheme in the CMAQ (Community Multiscale Air Quality) Eulerian model version 5.2. The TG algorithm follows the concentrations of representative air packets of species along trajectories determined by the wind field. The generated output from C-TRAIL accurately identifies the origins of pollutants. For validation, we analyzed the results of C-TRAIL during the KORUS-AQ campaign over South Korea. Initially, we implemented C-TRAIL in a simulation of CO concentrations with an emphasis on the long- and short-range transport effect. The output from C-TRAIL reveals that local trajectories were responsible for CO concentrations over Seoul during the stagnant period (May 17–22, 2016) and during the extreme pollution period (May 25–28, 2016), highly polluted air masses from China were distinguished as sources of CO transported to the Seoul Metropolitan Area (SMA). We conclude that long-range transport played a crucial role in high CO concentrations over the receptor area during this period. Furthermore, for May 2016, we find that the potential sources of CO over that SMA were the result of either local transport or long-range transport from the Shandong Peninsula and, in some cases, from north of the SMA. By identifying the trajectories of CO concentrations, one can use the results from C-TRAIL to directly link strong potential sources of pollutants to a receptor in specific regions during various time frames.


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