Abstract
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.
Highlights
Atmospheric aerosol particles play an important role in Earth’s radiative balance directly by scattering and absorbing solar radiation and indirectly by acting as cloud condensation nuclei (Myhre et al, 2013)
The time evolution of PM1, PM10 concentrations, PM1/10 ratios, black carbon (BC), particulate matter (PM) components, σap, σsp, scattering Ångström exponent (SAE), AAE, g and single-scattering albedo (SSA) measured at MSY and Montsec d’Ares (MSA) during the first 3 weeks of July 2015 is presented in Fig. 5 together with the concentrations of major species (NO−3, SO24−, NH+4, EC, OM, mineral matter (MM; calculated as the sum of typical mineral oxides) and sea salt (SS; Na + Cl)) from offline analysis of 24 h filters collected at MSY and MSA during the days of the instrumented flights
The dust event had a larger impact at MSA, where the PM10 levels increased sharply and were higher compared to MSY
Summary
Atmospheric aerosol particles play an important role in Earth’s radiative balance directly by scattering and absorbing solar radiation and indirectly by acting as cloud condensation nuclei (Myhre et al, 2013). The in situ surface distribution of atmospheric particles and their physical and chemical properties is determined through an array of networks across the US and Europe and to a lesser extent in Asia and Africa (Laj et al, 2020), such as the Global Atmosphere Watch (GAW, World Meteorological Organization); the European Research Infrastructure for the observation of Aerosol, Clouds and Trace Gases (ACTRIS; http://www.actris.eu, last access: 7 January 2021); the Interagency Monitoring of Protected Visual Environments (IMPROVE; http://vista.cira.colostate.edu/Improve/, last access: 7 January 2021); the European Monitoring and Evaluation Programme (EMEP, http://www.Emep.int, last access: 7 January 2021); and the NOAA Federated Aerosol Network (NFAN; Andrews et al, 2019). These networks provide detailed optical, physical and chemical properties of atmospheric aerosol particles at the surface (Putaud et al, 2004; Putaud et al, 2010; Andrews et al, 2011; Asmi et al, 2013; Collaud Coen et al, 2013; Collaud Coen et al, 2020; Cavalli et al, 2016; Zanatta et al, 2016; Pandolfi et al, 2018; Laj et al, 2020)
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