Optical and microphysical characterization of biomass- burning and industrial-pollution aerosols from- multiwavelength lidar and aircraft measurements

2002 ◽  
Vol 107 (D21) ◽  
pp. LAC 7-1-LAC 7-20 ◽  
Author(s):  
Ulla Wandinger ◽  
Detlef Müller ◽  
Christine Böckmann ◽  
Dietrich Althausen ◽  
Volker Matthias ◽  
...  
2016 ◽  
Author(s):  
Emily A. Bruns ◽  
Jay G. Slowik ◽  
Imad El Haddad ◽  
Dogushan Kilic ◽  
Felix Klein ◽  
...  

Abstract. Organic gases emitted during the flaming phase of residential wood combustion are characterized individually and by functionality using proton transfer reaction time-of-flight mass spectrometry. The evolution of the organic gases is monitored during photochemical aging. Primary gaseous emissions are dominated by oxygenated species (e.g., acetic acid, acetaldehyde, phenol and methanol), many of which have deleterious health effects and play an important role in atmospheric processes such as secondary organic aerosol formation and ozone production. Residential wood combustion emissions differ considerably from open biomass burning in both absolute magnitude and relative composition. Ratios of acetonitrile, a potential biomass burning marker, to CO are considerably lower (~ 0.09 pptv ppbv−1) than those observed in air masses influenced by open burning (~ 1–2 pptv ppbv−1), which may make differentiation from background levels difficult, even in regions heavily impacted by residential wood burning. Considerable formic acid forms during aging (~ 200–600 mg kg−1 at an OH exposure of (4.5–5.5) × 107 molec  cm−3 h), indicating residential wood combustion can be an important local source for this acid, the quantities of which are currently underestimated in models. Phthalic anhydride, a naphthalene oxidation product, is also formed in considerable quantities with aging (~ 55–75 mg kg−1 at an OH exposure of (4.5–5.5) × 107 molec  cm−3 h). Although total NMOG emissions vary by up to a factor of ~ 9 between burns, SOA formation potential does not scale with total NMOG emissions and is similar in all experiments. This study is the first thorough characterization of both primary and aged organic gases from residential wood combustion and provides a benchmark for comparison of emissions generated under different burn parameters.


2015 ◽  
Vol 15 (7) ◽  
pp. 3831-3850 ◽  
Author(s):  
L. Marelle ◽  
J.-C. Raut ◽  
J. L. Thomas ◽  
K. S. Law ◽  
B. Quennehen ◽  
...  

Abstract. During the POLARCAT-France airborne campaign in April 2008, pollution originating from anthropogenic and biomass burning emissions was measured in the European Arctic. We compare these aircraft measurements with simulations using the WRF-Chem model to investigate model representation of aerosols transported from Europe to the Arctic. Modeled PM2.5 is evaluated using European Monitoring and Evaluation Programme (EMEP) measurements in source regions and POLARCAT aircraft measurements in the Scandinavian Arctic. Total PM2.5 agrees well with the measurements, although the model overestimates nitrate and underestimates organic carbon in source regions. Using WRF-Chem in combination with the Lagrangian model FLEXPART-WRF, we find that during the campaign the research aircraft sampled two different types of European plumes: mixed anthropogenic and fire plumes from eastern Europe and Russia transported below 2 km, and anthropogenic plumes from central Europe uplifted by warm conveyor belt circulations to 5–6 km. Both modeled plume types had undergone significant wet scavenging (> 50% PM10) during transport. Modeled aerosol vertical distributions and optical properties below the aircraft are evaluated in the Arctic using airborne lidar measurements. Model results show that the pollution event transported aerosols into the Arctic (> 66.6° N) for a 4-day period. During this 4-day period, biomass burning emissions have the strongest influence on concentrations between 2.5 and 3 km altitudes, while European anthropogenic emissions influence aerosols at both lower (~ 1.5 km) and higher altitudes (~ 4.5 km). As a proportion of PM2.5, modeled black carbon and SO4= concentrations are more enhanced near the surface in anthropogenic plumes. The European plumes sampled during the POLARCAT-France campaign were transported over the region of springtime snow cover in northern Scandinavia, where they had a significant local atmospheric warming effect. We find that, during this transport event, the average modeled top-of-atmosphere (TOA) shortwave direct and semi-direct radiative effect (DSRE) north of 60° N over snow and ice-covered surfaces reaches +0.58 W m−2, peaking at +3.3 W m−2 at noon over Scandinavia and Finland.


2014 ◽  
Vol 7 (1) ◽  
pp. 163-172 ◽  
Author(s):  
L. Kuai ◽  
J. Worden ◽  
S. S. Kulawik ◽  
S. A. Montzka ◽  
J. Liu

Abstract. We present a description of the NASA Aura Tropospheric Emission Spectrometer (TES) carbonyl sulfide (OCS) retrieval algorithm for oceanic observations, along with evaluation of the biases and uncertainties using aircraft profiles from the HIPPO (HIAPER Pole-to-Pole Observations) campaign and data from the NOAA Mauna Loa site. In general, the OCS retrievals (1) have less than 1.0 degree of freedom for signals (DOFs), (2) are sensitive in the mid-troposphere with a peak sensitivity typically between 300 and 500 hPa, (3) but have much smaller systematic errors from temperature, CO2 and H2O calibrations relative to random errors from measurement noise. We estimate the monthly means from TES measurements averaged over multiple years so that random errors are reduced and useful information about OCS seasonal and latitudinal variability can be derived. With this averaging, TES OCS data are found to be consistent (within the calculated uncertainties) with NOAA ground observations and HIPPO aircraft measurements. TES OCS data also captures the seasonal and latitudinal variations observed by these in situ data.


2013 ◽  
Vol 6 (4) ◽  
pp. 6975-7003
Author(s):  
L. Kuai ◽  
J. Worden ◽  
S. S. Kulawik ◽  
S. A. Montzka ◽  
J. Liu

Abstract. We present a description of the Tropospheric Emission Spectrometer (TES) carbonyl sulfide (OCS) retrieval algorithm, along with evaluation of the biases and uncertainties against aircraft profiles from the HIPPO campaign and data from the NOAA Mauna Loa site. In general, the OCS retrievals (1) have less than 1.0 degree of freedom for signals (DOFs), (2) are sensitive in the mid-troposphere with a peak sensitivity typically between 300 to 500 hPa, (3) but have much smaller systematic errors from temperature, CO2 and H2O calibrations relative to random errors from measurement noise. Here we estimate the monthly means from TES measurements averaged over multiple years so that random errors are reduced and useful information about OCS seasonal and latitudinal variability can be derived. With this averaging, TES OCS data are found to be consistent (within the calculated uncertainties) with NOAA ground observations and HIPPO aircraft measurements. TES OCS data also captures the seasonal and latitudinal variations observed by these in situ data.


2013 ◽  
Vol 13 (5) ◽  
pp. 2735-2756 ◽  
Author(s):  
T. L. Lathem ◽  
A. J. Beyersdorf ◽  
K. L. Thornhill ◽  
E. L. Winstead ◽  
M. J. Cubison ◽  
...  

Abstract. The NASA DC-8 aircraft characterized the aerosol properties, chemical composition, and cloud condensation nuclei (CCN) concentrations of the summertime Arctic during the 2008 NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. Air masses characteristic of fresh and aged biomass burning, boreal forest, Arctic background, and anthropogenic industrial pollution were sampled. Observations were spatially extensive (50–85° N and 40–130° W) and exhibit significant variability in aerosol and CCN concentrations. The chemical composition was dominated by highly oxidized organics (66–94% by volume), with a water-soluble mass fraction of more than 50%. The aerosol hygroscopicity parameter, κ, ranged between κ = 0.08–0.32 for all air mass types. Industrial pollution had the lowest κ of 0.08 ± 0.01, while the Arctic background had the highest and most variable κ of 0.32 ± 0.21, resulting from a lower and more variable organic fraction. Both fresh and aged (long-range transported) biomass burning air masses exhibited remarkably similar κ (0.18 ± 0.13), consistent with observed rapid chemical and physical aging of smoke emissions in the atmosphere, even in the vicinity of fresh fires. The organic hygroscopicity (κorg) was parameterized by the volume fraction of water-soluble organic matter (εWSOM), with a κ = 0.12, such that κorg = 0.12εWSOM. Assuming bulk (size-independent) composition and including the κorg parameterization enabled CCN predictions to within 30% accuracy for nearly all environments sampled. The only exception was for industrial pollution from Canadian oil sands exploration, where an external mixture and size-dependent composition was required. Aerosol mixing state assumptions (internal vs. external) in all other environments did not significantly affect CCN predictions; however, the external mixing assumption provided the best results, even though the available observations could not determine the true degree of external mixing and therefore may not always be representative of the environments sampled. No correlation was observed between κorg and O : C. A novel correction of the CCN instrument supersaturation for water vapor depletion, resulting from high concentrations of CCN, was also employed. This correction was especially important for fresh biomass burning plumes where concentrations exceeded 1.5×104 cm−3 and introduced supersaturation depletions of ≥25%. Not accounting for supersaturation depletion in these high concentration environments would therefore bias CCN closure up to 25% and inferred κ by up to 50%.


2016 ◽  
Vol 50 (21) ◽  
pp. 11815-11824 ◽  
Author(s):  
Peng Lin ◽  
Paige K. Aiona ◽  
Ying Li ◽  
Manabu Shiraiwa ◽  
Julia Laskin ◽  
...  

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