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Abstract: Accurate measurements of the horizontal and vertical distribution of atmospheric aerosol particle optical properties are key for a better understanding of their impact on the climate. Here we present the results of a measurement campaign based on instrumented flights over north-eastern Spain. We measured vertical profiles of size-segregated atmospheric particulate matter (PM) mass concentrations and multi-wavelength scattering and absorption coefficients in the western Mediterranean basin (WMB). The campaign took place during typical summer conditions, characterized by the development of a vertical multi-layer structure, under both summer regional pollution episodes (REGs) and Saharan dust events (SDEs). REG patterns in the region form under high insolation and scarce precipitation in summer, favouring layering of highly aged fine-PM strata in the lower few kma.s.l. The REG scenario prevailed during the entire measurement campaign. Additionally, African dust outbreaks and plumes from northern African wildfires influenced the study area. The vertical profiles of climate-relevant intensive optical parameters such as single-scattering albedo (SSA); the asymmetry parameter (g); scattering, absorption and SSA Ångström exponents (SAE, AAE and SSAAE); and PM mass scattering and absorption cross sections (MSC and MAC) were derived from the measurements. Moreover, we compared the aircraft measurements with those performed at two GAW–ACTRIS (Global Atmosphere Watch–Aerosol, Clouds and Trace Gases) surface measurement stations located in north-eastern Spain, namely Montseny (MSY; regional background) and Montsec d'Ares (MSA; remote site). Airborne in situ measurements and ceilometer ground-based remote measurements identified aerosol air masses at altitudes up to more than 3.5 kma.s.l. The vertical profiles of the optical properties markedly changed according to the prevailing atmospheric scenarios. During SDE the SAE was low along the profiles, reaching values < 1.0 in the dust layers. Correspondingly, SSAAE was negative, and AAE reached values up to 2.0–2.5, as a consequence of the UV absorption increased by the presence of the coarse dust particles. During REG, the SAE increased to > 2.0, and the asymmetry parameter g was rather low (0.5–0.6) due to the prevalence of fine PM, which was characterized by an AAE close to 1.0, suggesting a fossil fuel combustion origin. During REG, some of the layers featured larger AAE (> 1.5), relatively low SSA at 525 nm (< 0.85) and high MSC (> 9 m2 g−1) and were associated with the influence of PM from wildfires. Overall, the SSA and MSC near the ground ranged around 0.85 and 3 m2 g−1, respectively, and increased at higher altitudes, reaching values above 0.95 and up to 9 m2 g−1. The PM, MSC and MAC were on average larger during REG compared to SDE due to the larger scattering and absorption efficiency of fine PM compared with dust. The SSA and MSC had quite similar vertical profiles and often both increased with height indicating the progressive shift toward PM with a larger scattering efficiency with altitude. This study contributes to our understanding of regional-aerosol vertical distribution and optical properties in the WMB, and the results will be useful for improving future climate projections and remote sensing or satellite retrieval algorithms.
Keywords: aerosol, climate change, Saharan dust, black carbon, aerosol absorption, aerosol scattering
Published in RUNG: 14.01.2021; Views: 2429; Downloads: 0
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Abstract: We have developed a novel single-beam photothermal interferometer and present here its application for the measurement of aerosol light absorption. The use of only a single laser beam allows for a compact optical set-up and significantly easier alignment compared to standard dual-beam photothermal interferometers, making it ideal for field measurements. Due to a unique configuration of the reference interferometer arm, light absorption by aerosols can be determined directly – even in the presence of light-absorbing gases. The instrument can be calibrated directly with light-absorbing gases, such as NO2, and can be used to calibrate other light absorption instruments. The detection limits (1σ) for absorption for 10 and 60 s averaging times were determined to be 14.6 and 7.4 Mm−1, respectively, which for a mass absorption cross section of 10 m2 g−1 leads to equivalent black carbon concentration detection limits of 1460 and 740 ng m−3, respectively. The detection limit could be reduced further by improvements to the isolation of the instrument and the signal detection and processing schemes employed.
Keywords: aerosol, aerosol absorption, black carbon, photo-thermal interferometer, climate change
Published in RUNG: 29.12.2020; Views: 2595; Downloads: 74
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Abstract: Small aethalometers are frequently used to measure equivalent black carbon (eBC) mass concentrations in the context of personal exposure and air pollution mapping through mobile measurements (MM). The most widely used is the microAethalometer (AE51). Its performance in the laboratory and field is well documented, however, there is not sufficient data in the context of its performance in different environments. In this investigation, we present the characterization of the performance of the AE51 through field unit-to-unit intercomparisons (IC), and against a reference absorption photometer from three MM campaigns conducted in drastically different environments. Five IC parameters were considered: i) study area, ii) location of IC, iii) time of day, iv) duration of IC, and v) correction for the filter-loading effect. We can conclude that it is crucial where and how long the IC have been performed in terms of the correlation between the mobile and reference instruments. Better correlations (R2 > 0.8, slope = 0.8) are achieved for IC performed in rural, and background areas for more than 10 minutes. In locations with more homogenous atmosphere, the correction of the loading effect improved the correlation between the mobile and reference instruments. In addition, a newer microAethalometer model (MA200) was characterized in the field under extreme cold conditions and correlated against another MA200 (R2 > 0.8, slope ≈ 1.0), AE51(R2 > 0.9, slope ≈ 0.9), and a stationary Aethalometer (AE33) across all wavelengths (R2 > 0.8, slope ≈ 0.7). For MA200, the loading effect was more pronounced, especially at the lower wavelengths, hence the correction of the loading effect is essential to improve the correlation against the AE33. The MA200 and AE51 proved to be robust and dependable portable instruments for MM applications. Real-world quality assurance of these instruments should be performed through field IC against reference instruments with longer durations in areas of slowly changing eBC concentration.
Keywords: Portable instruments, Mobile monitoring, Black carbon, Instrument intercomparisons
Published in RUNG: 15.09.2020; Views: 2662; Downloads: 184
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Abstract: What starts as an air quality problem in urban areas, ends up as a climate change problem globally. Emissions from cities and the power generating facilities powering the cities have local, regional and global effects. We show examples spanning these scales with very practical advice on how to start abatement locally.
Keywords: air quality, climate change, black carbon, aerosol, co2, smart city
Published in RUNG: 11.09.2020; Views: 3197; Downloads: 0
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Abstract: Brown carbon (BrC) is known to absorb light at subvisible wavelengths but its optical properties and sources are still poorly documented, leading to large uncertainties in climate studies. Here, we show its major wintertime contribution to total aerosol absorption at 370 nm (18–42%) at 9 different French sites. Moreover, an excellent correlation with levoglucosan (r2 = 0.9 and slope = 22.2 at 370 nm), suggesting important contribution of wood burning emissions to ambient BrC aerosols in France. At all sites, BrC peaks were mainly observed during late evening, linking to local intense residential wood burning during this time period. Furthermore, the geographic origin analysis also highlighted the high potential contribution of local and/or small-regional emissions to BrC. Focusing on the Paris region, twice higher BrC mass absorption efficiency value was obtained for less oxidized biomass burning organic aerosols (BBOA) compared to more oxidized BBOA (e.g., about 4.9 ± 0.2 vs. 2.0 ± 0.1 m2 g−1, respectively, at 370 nm). Finally, the BBOA direct radiative effect was found to be 40% higher when these two BBOA fractions are treated as light-absorbing species, compared to the non-absorbing BBOA scenario.
Keywords: Brown carbon, Multi sites, Residential wood burning, Mass absorption efficiency, France
Published in RUNG: 20.07.2020; Views: 3070; Downloads: 0
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