scholarly journals Airborne observations and modeling of springtime stratosphere-to-troposphere transport over California

2013 ◽  
Vol 13 (24) ◽  
pp. 12481-12494 ◽  
Author(s):  
E. L. Yates ◽  
L. T. Iraci ◽  
M. C. Roby ◽  
R. B. Pierce ◽  
M. S. Johnson ◽  
...  

Abstract. Stratosphere-to-troposphere transport (STT) results in air masses of stratospheric origin intruding into the free troposphere. Once in the free troposphere, ozone (O3)-rich stratospheric air can be transported and mixed with tropospheric air masses, contributing to the tropospheric O3 budget. Evidence of STT can be identified based on the differences in the trace gas composition of the two regions. Because O3 is present in such large quantities in the stratosphere compared to the troposphere, it is frequently used as a tracer for STT events. This work reports on airborne in situ measurements of O3 and other trace gases during two STT events observed over California, USA. The first, on 14 May 2012, was associated with a cutoff low, and the second, on 5 June 2012, occurred during a post-trough, building ridge event. In each STT event, airborne measurements identified high O3 within the stratospheric intrusion, which were observed as low as 3 km above sea level. During both events the stratospheric air mass was characterized by elevated O3 mixing ratios and reduced carbon dioxide (CO2) and water vapor. The reproducible observation of reduced CO2 within the stratospheric air mass supports the use of non-conventional tracers as an additional method for detecting STT. A detailed meteorological analysis of each STT event is presented, and observations are interpreted with the Realtime Air Quality Modeling System (RAQMS). The implications of the two STT events are discussed in terms of the impact on the total tropospheric O3 budget and the impact on air quality and policy-making.

2013 ◽  
Vol 13 (4) ◽  
pp. 10157-10192 ◽  
Author(s):  
E. L. Yates ◽  
L. T. Iraci ◽  
M. C. Roby ◽  
R. B. Pierce ◽  
M. S. Johnson ◽  
...  

Abstract. Stratosphere-to-troposphere transport (STT) results in air masses of stratospheric origin intruding into the free troposphere. Once in the free troposphere, O3-rich stratospheric air can be transported and mixed with tropospheric air masses, contributing to the tropospheric O3 budget. Evidence of STT can be identified based on the differences in the trace gas composition of the two regions. Because ozone (O3) is present in such large quantities in the stratosphere compared to the troposphere, it is frequently used as a tracer for STT events. This work reports on airborne in situ measurements of O3 and other trace gases during two STT events observed over California, USA. The first, on 14 May 2012, was associated with a cut-off low, and the second, on 5 June 2012, occurred during a post-trough, building ridge event. In each STT event, airborne measurements identified high O3 within a stratospheric intrusion which was observed as low as 3 km above sea level. During both events the stratospheric air mass was characterized by elevated O3 mixing ratios and reduced carbon dioxide (CO2) and water vapor. The reproducible observation of reduced CO2 within the stratospheric air mass supports the use of non-conventional tracers as an additional method for detecting STT. A detailed meteorological analysis of each STT event is presented and observations are interpreted with the Realtime Air Quality Modeling System (RAQMS). The implications of the two STT events are discussed in terms of the impact on the total tropospheric O3 budget and the impact on air quality and policy-making.


2013 ◽  
Vol 13 (24) ◽  
pp. 12451-12467 ◽  
Author(s):  
S. J. O'Shea ◽  
G. Allen ◽  
M. W. Gallagher ◽  
S. J.-B. Bauguitte ◽  
S. M. Illingworth ◽  
...  

Abstract. In situ airborne measurements were made over eastern Canada in summer 2011 as part of the BORTAS experiment (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites). In this paper we present observations of greenhouse gases (CO2 and CH4) and other biomass burning tracers (CO, HCN and CH3CN), both climatologically and through case studies, as recorded on board the FAAM BAe-146 research aircraft. Vertical profiles of CO2 were generally characterised by depleted boundary layer concentrations relative to the free troposphere, consistent with terrestrial biospheric uptake. In contrast, CH4 concentrations were found to rise with decreasing altitude due to strong local and regional surface sources. BORTAS observations were found to be broadly comparable with both previous measurements in the region during the regional burning season and with reanalysed composition fields from the EU Monitoring Atmospheric Composition and Change (MACC) project. We use coincident tracer–tracer correlations and a Lagrangian trajectory model to characterise and differentiate air mass history of intercepted plumes. In particular, CO, HCN and CH3CN were used to identify air masses that have been recently influenced by biomass burning. Examining individual cases we were able to quantify emissions from biomass burning. Using both near-field (< 1 day) and far-field (> 1 day) sampling, boreal forest fire plumes were identified throughout the troposphere. Fresh plumes from fires in northwestern Ontario yield emission factors for CH4 and CO2 of 8.5 ± 0.9 g (kg dry matter)−1 and 1512 ± 185 g (kg dry matter)−1, respectively. We have also investigated the efficacy of calculating emission factors from far-field sampling, in which there might be expected to be limited mixing with background and other characteristic air masses, and we provide guidance on best practice and limitations in such analysis. We have found that for measurements within plumes that originated from fires in northwestern Ontario 2–4 days upwind, emission factors can be calculated that range between 1618 ± 216 and 1702 ± 173 g (kg dry matter)−1 for CO2 and 1.8 ± 0.2 and 6.1 ± 1 g (kg dry matter)−1 for CH4.


2021 ◽  
Vol 21 (17) ◽  
pp. 12965-12988
Author(s):  
Bert Verreyken ◽  
Crist Amelynck ◽  
Niels Schoon ◽  
Jean-François Müller ◽  
Jérôme Brioude ◽  
...  

Abstract. We present a source apportionment study of a near-continuous 2-year dataset of volatile organic compounds (VOCs), recorded between October 2017 and November 2019 with a quadrupole-based high-sensitivity proton-transfer-reaction mass-spectrometry (hs-PTR-MS) instrument deployed at the Maïdo observatory (21.1∘ S, 55.4∘ E, 2160 m altitude). The observatory is located on La Réunion island in the southwest Indian Ocean. We discuss seasonal and diel profiles of six key VOC species unequivocally linked to specific sources – acetonitrile (CH3CN), isoprene (C5H8), isoprene oxidation products (Iox), benzene (C6H6), C8-aromatic compounds (C8H10), and dimethyl sulfide (DMS). The data are analyzed using the positive matrix factorization (PMF) method and back-trajectory calculations based on the Lagrangian mesoscale transport model FLEXPART-AROME to identify the impact of different sources on air masses sampled at the observatory. As opposed to the biomass burning tracer CH3CN, which does not exhibit a typical diel pattern consistently throughout the dataset, we identify pronounced diel profiles with a daytime maximum for the biogenic (C5H8 and Iox) and anthropogenic (C6H6, C8H10) tracers. The marine tracer DMS generally displays a daytime maximum except for the austral winter when the difference between daytime and nighttime mixing ratios vanishes. Four factors were identified by the PMF: background/biomass burning, anthropogenic, primary biogenic, and secondary biogenic. Despite human activity being concentrated in a few coastal areas, the PMF results indicate that the anthropogenic source factor is the dominant contributor to the VOC load (38 %), followed by the background/biomass burning source factor originating in the free troposphere (33 %), and by the primary (15 %) and secondary biogenic (14 %) source factors. FLEXPART-AROME simulations showed that the observatory was most sensitive to anthropogenic emissions west of Maïdo while the strongest biogenic contributions coincided with air masses passing over the northeastern part of La Réunion. At night, the observatory is often located in the free troposphere, while during the day, the measurements are influenced by mesoscale sources. Interquartile ranges of nighttime 30 min average mixing ratios of methanol (CH3OH), CH3CN, acetaldehyde (CH3CHO), formic acid (HCOOH), acetone (CH3COCH3), acetic acid (CH3COOH), and methyl ethyl ketone (MEK), representative for the atmospheric composition of the free troposphere, were found to be 525–887, 79–110, 61–101, 172–335, 259–379, 64–164, and 11–21 pptv, respectively.


2020 ◽  
Vol 20 (6) ◽  
pp. 3397-3413 ◽  
Author(s):  
Syuichi Itahashi ◽  
Rohit Mathur ◽  
Christian Hogrefe ◽  
Sergey L. Napelenok ◽  
Yang Zhang

Abstract. The state-of-the-science Community Multiscale Air Quality (CMAQ) modeling system, which has recently been extended for hemispheric-scale modeling applications (referred to as H-CMAQ), is applied to study the trans-Pacific transport, a phenomenon recognized as a potential source of air pollution in the US, during April 2010. The results of this analysis are presented in two parts. In the previous paper (Part 1), model evaluation for tropospheric ozone (O3) was presented and an air mass characterization method was developed. Results from applying this newly established method pointed to the importance of emissions as the factor to enhance the surface O3 mixing ratio over the US. In this subsequent paper (Part 2), emission impacts are examined based on mathematically rigorous sensitivity analysis using the higher-order decoupled direct method (HDDM) implemented in H-CMAQ. The HDDM sensitivity coefficients indicate the presence of a NOx-sensitive regime during April 2010 over most of the Northern Hemisphere. By defining emission source regions over the US and east Asia, impacts from these emission sources are examined. At the surface, during April 2010, the emission impacts of the US and east Asia are comparable over the western US with a magnitude of about 3 ppbv impacts on monthly mean O3 all-hour basis, whereas the impact of domestic emissions dominates over the eastern US with a magnitude of about 10 ppbv impacts on monthly mean O3. The positive correlation (r=0.63) between surface O3 mixing ratios and domestic emission impacts is confirmed. In contrast, the relationship between surface O3 mixing ratios and emission impacts from east Asia exhibits a flat slope when considering the entire US. However, this relationship has strong regional differences between the western and eastern US; the western region exhibits a positive correlation (r=0.36–0.38), whereas the latter exhibits a flat slope (r < 0.1). Based on the comprehensive evaluation of H-CMAQ, we extend the sensitivity analysis for O3 aloft. The results reveal the significant impacts of emissions from east Asia on the free troposphere (defined as 750 to 250 hPa) over the US (impacts of more than 5 ppbv) and the dominance of stratospheric air mass on upper model layer (defined as 250 to 50 hPa) over the US (impacts greater than 10 ppbv). Finally, we estimate changes of trans-Pacific transport by taking into account recent emission trends from 2010 to 2015 assuming the same meteorological condition. The analysis suggests that the impact of recent emission changes on changes in the contribution of trans-Pacific transport to US O3 levels was insignificant at the surface level and was small (less than 1 ppbv) over the free troposphere.


2009 ◽  
Vol 9 (11) ◽  
pp. 3731-3743 ◽  
Author(s):  
M. Mena-Carrasco ◽  
G. R. Carmichael ◽  
J. E. Campbell ◽  
D. Zimmerman ◽  
Y. Tang ◽  
...  

Abstract. The impact of Mexico City (MCMA) emissions is examined by studying its effects on air quality, photochemistry, and on ozone production regimes by combining model products and aircraft observations from the MILAGRO experiment during March 2006. The modeled influence of MCMA emissions to enhancements in surface level NOx, CO, and O3 concentrations (10–30% increase) are confined to distances <200 km, near surface. However, the extent of the influence is significantly larger at higher altitudes. Broader MCMA impacts (some 900 km Northeast of the city) are shown for specific outflow conditions in which enhanced ozone, NOy, and MTBE mixing ratios over the Gulf of Mexico are linked to MCMA by source tagged tracers and sensitivity runs. This study shows that the "footprint" of MCMA on average is fairly local, with exception to reactive nitrogen, which can be transported long range in the form of PAN, acting as a reservoir and source of NOx with important regional ozone formation implications. The simulated effect of MCMA emissions of anthropogenic aerosol on photochemistry showed a maximum regional decrease of 40% in J[NO2→NO+O], and resulting in the reduction of ozone production by 5–10%. Observed ozone production efficiencies are evaluated as a function of distance from MCMA, and by modeled influence from MCMA. These tend to be much lower closer to MCMA, or in those points where modeled contribution from MCMA is large. This research shows that MCMA emissions do effect on regional air quality and photochemistry, both contributing large amounts of ozone and its precursors, but with caveat that aerosol concentrations hinder formation of ozone to its potential due to its reduction in photolysis rates.


2018 ◽  
Author(s):  
Steven Turnock ◽  
Oliver Wild ◽  
Frank Dentener ◽  
Yanko Davila ◽  
Louisa Emmons ◽  
...  

Abstract. This study quantifies future changes in tropospheric ozone (O3) using a simple parameterisation of source-receptor relationships based on simulations from a range of models participating in the Task Force on Hemispheric Transport of Air Pollutants (TF-HTAP) experiments. Surface and tropospheric O3 changes are calculated globally and across 16 regions from perturbations in precursor emissions (NOx, CO, VOCs) and methane (CH4) abundance. A source attribution is provided for each source region along with an estimate of uncertainty based on the spread of the results from the models. Tests against model simulations using HadGEM2-ES confirm that the approaches used within the parameterisation are valid. The O3 response to changes in CH4 abundance is slightly larger in TF-HTAP Phase 2 than in the TF-HTAP Phase 1 assessment (2010) and provides further evidence that controlling CH4 is important for limiting future O3 concentrations. Different treatments of chemistry and meteorology in models remains one of the largest uncertainties in calculating the O3 response to perturbations in CH4 abundance and precursor emissions, particularly over the Middle East and South Asian regions. Emission changes for the future ECLIPSE scenarios and a subset of preliminary Shared Socio-economic Pathways (SSPs) indicate that surface O3 concentrations will increase by 1 to 8 ppbv in 2050 across different regions. Source attribution analysis highlights the growing importance of CH4 in the future under current legislation. A global tropospheric O3 radiative forcing of +0.07 W m−2 from 2010 to 2050 is predicted using the ECLIPSE scenarios and SSPs, based solely on changes in CH4 abundance and tropospheric O3 precursor emissions and neglecting any influence of climate change. Current legislation is shown to be inadequate in limiting the future degradation of surface ozone air quality and enhancement of near-term climate warming. More stringent future emission controls provide a large reduction in both surface O3 concentrations and O3 radiative forcing. The parameterisation provides a simple tool to highlight the different impacts and associated uncertainties of local and hemispheric emission control strategies on both surface air quality and the near-term climate forcing by tropospheric O3.


2010 ◽  
Vol 10 (6) ◽  
pp. 3001-3025 ◽  
Author(s):  
S. Yu ◽  
R. Mathur ◽  
G. Sarwar ◽  
D. Kang ◽  
D. Tong ◽  
...  

Abstract. A critical module of air quality models is the photochemical mechanism. In this study, the impact of the three photochemical mechanisms (CB4, CB05, SAPRC-99) on the Eta-Community Multiscale Air Quality (CMAQ) model's forecast performance for O3, and its related precursors has been assessed over the eastern United States with observations obtained by aircraft (NOAA P-3 and NASA DC-8) flights, ship and two surface networks (AIRNow and AIRMAP) during the 2004 International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) study. The results show that overall none of the mechanisms performs systematically better than the others. On the other hand, at the AIRNow surface sites, CB05 has the best performance with the normalized mean bias (NMB) of 3.9%, followed by CB4 (NMB=−5.7%) and SAPRC-99 (NMB=10.6%) for observed O3≥75 ppb, whereas CB4 has the best performance with the least overestimation for observed O3<75 ppb. On the basis of comparisons with aircraft P-3 measurements, there were consistent overestimations of O3, NOz, PAN and NOy and consistent underestimations of CO, HNO3, NO2, NO, SO2 and terpenes for all three mechanisms although the NMB values for each species and mechanisms were different. The results of aircraft DC-8 show that CB05 predicts the H2O2 mixing ratios most closely to the observations (NMB=10.8%), whereas CB4 and SAPRC-99 overestimated (NMB=74.7%) and underestimated (NMB=−25.5%) H2O2 mixing ratios significantly, respectively. For different air mass flows over the Gulf of Maine on the basis of the ship data, the three mechanisms have relatively better performance for O3, isoprene and SO2 for the clean marine or continental flows but relatively better performance for CO, NO2 and NO for southwesterly/westerly offshore flows. The results of the O3-NOz slopes over the ocean indicate that SAPRC-99 has the highest upper limits of the ozone production efficiency (εN) (5.8), followed by CB05 (4.5) and CB4 (4.0) although they are much lower than that inferred from the observation (11.8), being consistent with the fact that on average, SAPRC-99 produces the highest O3, followed by CB05 and CB4, across all O3 mixing ratio ranges


2019 ◽  
Vol 19 (19) ◽  
pp. 12477-12494 ◽  
Author(s):  
Armin Sigmund ◽  
Korbinian Freier ◽  
Till Rehm ◽  
Ludwig Ries ◽  
Christian Schunk ◽  
...  

Abstract. To assist atmospheric monitoring at high-alpine sites, a statistical approach for distinguishing between the dominant air masses was developed. This approach was based on a principal component analysis using five gas-phase and two meteorological variables. The analysis focused on the Schneefernerhaus site at Zugspitze Mountain, Germany. The investigated year was divided into 2-month periods, for which the analysis was repeated. Using the 33.3 % and 66.6 % percentiles of the first two principal components, nine air mass regimes were defined. These regimes were interpreted with respect to vertical transport and assigned to the BL (recent contact with the boundary layer), UFT/SIN (undisturbed free troposphere or stratospheric intrusion), and HYBRID (influences of both the boundary layer and the free troposphere or ambiguous) air mass classes. The input data were available for 78 % of the investigated year. BL accounted for 31 % of the cases with similar frequencies in all seasons. UFT/SIN comprised 14 % of the cases but was not found from April to July. HYBRID (55 %) mostly exhibited intermediate characteristics, whereby 17 % of the HYBRID class suggested an influence from the marine boundary layer or the lower free troposphere. The statistical approach was compared to a mechanistic approach using the ceilometer-based mixing layer height from a nearby valley site and a detection scheme for thermally induced mountain winds. Due to data gaps, only 25 % of the cases could be classified using the mechanistic approach. Both approaches agreed well, except in the rare cases of thermally induced uplift. The statistical approach is a promising step towards a real-time classification of air masses. Future work is necessary to assess the uncertainty arising from the standardization of real-time data.


2021 ◽  
Author(s):  
Simone M. Pieber ◽  
Dac-Loc Nguyen ◽  
Hendryk Czech ◽  
Stephan Henne ◽  
Nicolas Bukowiecki ◽  
...  

&lt;p&gt;Open biomass burning (BB) is a globally widespread phenomenon. The fires release pollutants, which are harmful for human and ecosystem health and alter the Earth's radiative balance. Yet, the impact of various types of BB on the global radiative forcing remains poorly constrained concerning greenhouse gas emissions, BB organic aerosol (OA) chemical composition and related light absorbing properties. Fire emissions composition is influenced by multiple factors (e.g., fuel and thereby vegetation-type, fuel moisture, fire temperature, available oxygen). Due to regional variations in these parameters, studies in different world regions are needed. Here we investigate the influence of seasonally recurring BB on trace gas concentration and air quality at the regional Global Atmosphere Watch (GAW) station Pha Din (PDI) in rural Northwestern Vietnam. PDI is located in a sparsely populated area on the top of a hill (1466 m a.s.l.) and is well suited to study the large-scale fires on the Indochinese Peninsula, whose pollution plumes are frequently transported towards the site [1]. We present continuous trace gas observations of CO&lt;sub&gt;2&lt;/sub&gt;, CH&lt;sub&gt;4&lt;/sub&gt;, CO, and O&lt;sub&gt;3&lt;/sub&gt; conducted at PDI since 2014 and interpret the data with atmospheric transport simulations. Annually recurrent large scale BB leads to hourly time-scale peaks CO mixing ratios at PDI of 1000 to 1500 ppb around every April since the start of data collection in 2014. We complement this analysis with carbonaceous PM&lt;sub&gt;2.5 &lt;/sub&gt;chemical composition analyzed during an intensive campaign in March-April 2015. This includes measurements of elemental and organic carbon (EC/OC) and more than 50 organic markers, such as sugars, PAHs, fatty acids and nitro-aromatics [2]. For the intensive campaign, we linked CO, CO&lt;sub&gt;2&lt;/sub&gt;, CH&lt;sub&gt;4&lt;/sub&gt; and O&lt;sub&gt;3&lt;/sub&gt; mixing ratios to a statistical classification of BB events, which is based on OA composition. We found increased CO and O&lt;sub&gt;3&lt;/sub&gt; levels during medium and high BB influence during the intensive campaign. A backward trajectory analysis confirmed different source regions for the identified periods based on the OA cluster. Typically, cleaner air masses arrived from northeast, i.e., mainland China and Yellow sea during the intensive campaign. The more polluted periods were characterized by trajectories from southwest, with more continental recirculation of the medium cluster, and more westerly advection for the high cluster. These findings highlight that BB activities in Northern Southeast Asia significantly enhances the regional OA loading, chemical PM&lt;sub&gt;2.5 &lt;/sub&gt;composition and the trace gases in northwestern Vietnam. The presented analysis adds valuable data on air quality in a region of scarce data availability.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;&lt;strong&gt;REFERENCES&lt;/strong&gt;&lt;/p&gt;&lt;p&gt;[1] Bukowiecki, N. et al. Effect of Large-scale Biomass Burning on Aerosol Optical Properties at the GAW Regional Station Pha Din, Vietnam. AAQR. 19, 1172&amp;#8211;1187 (2019).&lt;/p&gt;&lt;p&gt;[2] Nguyen, D. L, et al. Carbonaceous aerosol composition in air masses influenced by large-scale biomass burning: a case-study in Northwestern Vietnam. ACPD., https://doi.org/10.5194/acp-2020-1027, in review, 2020.&lt;/p&gt;


2018 ◽  
Vol 18 (4) ◽  
pp. 2973-2983 ◽  
Author(s):  
Christian Rolf ◽  
Bärbel Vogel ◽  
Peter Hoor ◽  
Armin Afchine ◽  
Gebhard Günther ◽  
...  

Abstract. The impact of air masses originating in Asia and influenced by the Asian monsoon anticyclone on the Northern Hemisphere stratosphere is investigated based on in situ measurements. A statistically significant increase in water vapor (H2O) of about 0.5 ppmv (11 %) and methane (CH4) of up to 20 ppbv (1.2 %) in the extratropical stratosphere above a potential temperature of 380 K was detected between August and September 2012 during the HALO aircraft missions Transport and Composition in the UT/LMS (TACTS) and Earth System Model Validation (ESMVal). We investigate the origin of the increased water vapor and methane using the three-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS). We assign the source of the moist air masses in the Asian region (northern and southern India, eastern China, southeast Asia, and the tropical Pacific) based on tracers of air mass origin used in CLaMS. The water vapor increase is correlated with an increase of the simulated Asian monsoon air mass contribution from about 10 % in August to about 20 % in September, which corresponds to a doubling of the influence from the Asian monsoon region. Additionally, back trajectories starting at the aircraft flight paths are used to differentiate transport from the Asian monsoon anticyclone and other source regions by calculating the Lagrangian cold point (LCP). The geographic location of the LCPs, which indicates the region where the set point of water vapor mixing ratio along these trajectories occurs, can be predominantly attributed to the Asian monsoon region.


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