Light-absorbing aerosols (LAAs) are short-lived climate forcers with a significant impact on Earth's radiative balance. LAAs include dust aerosols, black carbon (BC) and organic light-absorbing ...carbonaceous aerosol (collectively termed brown carbon, BrC), which have also been proven to be highly toxic. In this study, aerosol absorption at five wavelengths (ranging from ultraviolet to infrared) was monitored continuously using filter-based photometers during two winter seasons in 2020 and 2021 in the city of Modena (southern central Po Valley, northern Italy), at two regulatory air quality monitoring sites, along with other pollutants (coarse particulate matter, PM10; fine particulate matter, PM2.5; O3; NO; NO2; and C6H6) and the vehicular traffic rate. The aerosol optical depth (AOD) and other column aerosol optical properties were concurrently monitored at four wavelengths by an AErosol RObotic NETwork (AERONET) sun photometer under urban background conditions within Modena. In situ absorption levels were apportioned to both sources (fossil fuel and biomass burning) and species (BC and BrC), while columnar absorption was apportioned to BC, BrC and mineral dust. The combined analysis of the atmospheric aerosol and gas measurements and of the meteorological conditions (in situ and from the ERA5 reanalysis) identified the location of potential urban sources of BC and BrC, most likely related to traffic and biomass burning. In situ data show different diurnal/weekly patterns for BrC from biomass burning and BC from traffic, with minor differences between the background and the urban traffic conditions. AERONET version 3 absorption aerosol optical depth (AAOD) retrievals at four wavelengths allowed the estimation of the absorptive direct radiative effect due to LAAs over the same period under the reasonable assumption that the AOD signal is concentrated within the mixing layer. AERONET retrievals showed a modest correlation of columnar absorption with planetary boundary layer (PBL)-scaled in situ observations, although the correlation improved significantly during a desert dust transport event that affected both in situ aerosol and columnar absorption, particularly in the blue spectrum range. A low correlation occurred between the contribution of BrC to aerosol absorption for the in situ and the columnar observations, with the BrC contribution being generally larger for in situ observations. Finally, evidence of a highly layered atmosphere during the study period, featuring significant spatial mixing and modest vertical mixing, was shown by ERA5-based atmospheric temperature profiles and by the large correlation of concurrent AERONET AOD retrievals in Modena and in Ispra (on the northwestern side of the Po Valley, ca. 225 km from Modena).
In this paper, a new methodology coupling aerosol optical and chemical parameters in the same source apportionment study is reported. In addition to results on source contributions, this approach ...provides information such as estimates for the atmospheric absorption à ngström exponent (α) of the sources and mass absorption cross sections (MACs) for fossil fuel emissions at different wavelengths.
Instruments measuring aerosol light absorption, such as the Aethalometer and the Multi-Wavelength Absorbance Analyzer (MWAA), have been extensively used to characterize optical absorption of ...atmospheric particulate matter. Data retrieved with such instruments can be analysed with mathematical models to apportion different aerosol sources (Aethalometer model) and components (MWAA model). In this work we present an upgrade to the MWAA optical apportionment model. In addition to the apportionment of the absorption coefficient babs in its components (black carbon and brown carbon) and sources (fossil fuels and wood burning), the extended model allows for the retrieval of the absorption Ångström exponent of each component and source, thereby avoiding initial assumptions regarding these parameters. We also present a new open-source software toolkit, the MWAA model toolkit (MWAA_MT), written in both Python and R, that performs the entire apportionment procedure.
The interplay of bio-aerosol dispersion and impact,
meteorology, and air quality is gaining increasing interest in the wide spectrum
of atmospheric sciences. Experiments conducted inside confined ...artificial
environments, such as atmospheric simulation chambers (ASCs), where
atmospheric conditions and composition are controlled, can provide valuable
information on bio-aerosol viability, dispersion, and impact. We focus here
on the reproducible aerosolization and injection of viable microorganisms
into an ASC, the first and crucial step of any experimental protocol to
expose bio-aerosols to different atmospheric conditions. We compare the
performance of three nebulizers specifically designed for bio-aerosol
applications: the Collison nebulizer, the Blaustein Atomizing Modules (BLAM), and the Sparging Liquid Aerosol Generator (SLAG), all manufactured and commercialized by CH TECHNOLOGIES. The comparison refers to operating
conditions and the concentration of viable bacteria at the nebulizer outlet,
with the final goal being to measure the reproducibility of the nebulization
procedures and assess their application in experiments inside ASCs. A typical
bacterial test model, Escherichia coli (ATCC® 25922™), was
selected for such characterization. Bacteria suspensions with a
concentration around 108 CFU mL−1 were first aerosolized at
different air pressures and collected by a liquid impinger to obtain a
correlation curve between airflow and nebulized bacteria for each
generator. Afterwards, bacteria were aerosolized inside the atmospheric
simulation chamber ChAMBRe (Chamber for Aerosol Modelling and Bio-aerosol
Research) to measure the reproducibility of the whole procedure. An overall
reproducibility of 11 % (i.e., standard deviation of the results obtained with the three nebulizers) was obtained with each nebulizer through a set of
baseline experiments.
Thermal-optical analysis is widely adopted for the quantitative determination of total (TC), organic (OC), and elemental (EC) carbon in atmospheric aerosol sampled by suitable filters. Nevertheless, ...the methodology suffers from several uncertainties and artifacts such as the well-known issue of charring affecting the OC-EC separation. In the standard approach, the effect of the possible presence of brown carbon, BrC, in the sample is neglected. BrC is a fraction of OC, usually produced by biomass burning with a thermic behavior intermediate between OC and EC. BrC is optically active: it shows an increasing absorbance when the wavelength moves to the blue-UV region of the electromagnetic spectrum. Definitively, the thermal-optical characterization of carbonaceous aerosol should be reconsidered to address the possible BrC content in the sample under analysis.
Understanding the sources of light-absorbing organic (brown) carbon (BrC) and its interaction with black carbon (BC) and other non-refractory particulate matter (NR-PM) fractions is important for ...reducing uncertainties in the aerosol direct radiative forcing. In this study, we combine multiple filter-based techniques to achieve long-term, spectrally resolved, source- and species-specific atmospheric absorption closure. We determine the mass absorption efficiency (MAE) in dilute bulk solutions at 370 nm to be equal to 1.4 m2 g−1 for fresh biomass smoke, 0.7 m2 g−1 for winter-oxygenated organic aerosol (OA), and 0.13 m2 g−1 for other less absorbing OA. We apply Mie calculations to estimate the contributions of these fractions to total aerosol absorption. While enhanced absorption in the near-UV has been traditionally attributed to primary biomass smoke, here we show that anthropogenic oxygenated OA may be equally important for BrC absorption during winter, especially at an urban background site. We demonstrate that insoluble tar balls are negligible in residential biomass burning atmospheric samples of this study and thus could attribute the totality of the NR-PM absorption at shorter wavelengths to methanol-extractable BrC. As for BC, we show that the mass absorption cross-section (MAC) of this fraction is independent of its source, while we observe evidence for a filter-based lensing effect associated with the presence of NR-PM components. We find that bare BC has a MAC of 6.3 m2 g−1 at 660 nm and an absorption Ångström exponent of 0.93 ± 0.16, while in the presence of coatings its absorption is enhanced by a factor of ∼ 1.4. Based on Mie calculations of closure between observed and predicted total light absorption, we provide an indication for a suppression of the filter-based lensing effect by BrC. The total absorption reduction remains modest, ∼ 10 %–20 % at 370 nm, and is restricted to shorter wavelengths, where BrC absorption is significant. Overall, our results allow an assessment of the relative importance of the different aerosol fractions to the total absorption for aerosols from a wide range of sources and atmospheric ages. When integrated with the solar spectrum at 300–900 nm, bare BC is found to contribute around two-thirds of the solar radiation absorption by total carbonaceous aerosols, amplified by the filter-based lensing effect (with an interquartile range, IQR, of 8 %–27 %), while the IQR of the contributions by particulate BrC is 6 %–13 % (13 %–20 % at the rural site during winter). Future studies that will directly benefit from these results include (a) optical modelling aiming at understanding the absorption profiles of a complex aerosol composed of BrC, BC and lensing-inducing coatings; (b) source apportionment aiming at understanding the sources of BC and BrC from the aerosol absorption profiles; (c) global modelling aiming at quantifying the most important aerosol absorbers.
The performance of a mini inverted soot generator (MISG) has been investigated at ChAMBRe (Chamber for Aerosol Modelling and Bio-aerosol Research) by studying the properties of soot particles ...generated by ethylene and propane combustion. This work deepens and expands the existing characterization of the MISG, which also exploits an atmospheric simulation chamber (ASC). Different from previous works, MISG performance has been also tested at different fuel flows and higher global equivalence ratios. MISG exhausts were investigated after their injection inside the atmospheric
simulation chamber, which is another novelty of this work. Starting from an extensive classification of combustion conditions and resulting flame shapes, the MISG exhaust was characterized in terms of concentration of emitted particles and gases, particle size distribution, and optical properties. Soot particles were also collected on quartz fibre filters and
then analysed by optical and thermal–optical techniques to measure the spectral dependence of the absorption coefficient babs and their composition in terms of elemental carbon and organic carbon (EC and OC). Significant differences could be observed when the MISG was fuelled with ethylene and propane in terms of particle size. In particular, the production of super-micrometric aggregates was observed for ethylene combustion. With equal combustion conditions, ethylene produced a higher number concentration of particles and smaller mode diameters. Soot particles produced by propane combustion resulted in higher EC : TC (total carbon) ratios and they were more light absorbing than particles generated by ethylene combustion. Values of the mass absorption cross section (MAC) and of the Ångström absorption exponent (AAE) turned out to be compatible with the literature, even if there were some specific differences. The comprehensive characterization of the MISG soot particles is an important piece of information to design and perform experiments in atmospheric simulation chambers. Particles with well-known
properties can be used, for example, to investigate the possible interactions between soot and other atmospheric pollutants, the effects of meteorological variables on soot properties, and the oxidative and toxicological potential of soot particles.
The amount of reflected energy by snow and ice plays a fundamental role in their melting processes. Different non-ice materials (carbonaceous particles, mineral dust (MD), microorganisms, algae, ...etc.) can decrease the reflectance of snow and ice promoting the melt. The object of this paper is to assess the capability of field and satellite (EO-1 Hyperion) hyperspectral data to characterize the impact of light-absorbing impurities (LAIs) on the surface reflectance of ice and snow of the Vadret da Morteratsch, a large valley glacier in the Swiss Alps. The spatial distribution of both narrow-band and broad-band indices derived from Hyperion was analyzed in relation to ice and snow impurities. In situ and laboratory reflectance spectra were acquired to characterize the optical properties of ice and cryoconite samples. The concentrations of elemental carbon (EC), organic carbon (OC) and levoglucosan were also determined to characterize the impurities found in cryoconite. Multi-wavelength absorbance spectra were measured to compare the optical properties of cryoconite samples and local moraine sediments. In situ reflectance spectra showed that the presence of impurities reduced ice reflectance in visible wavelengths by 80–90 %. Satellite data also showed the outcropping of dust during the melting season in the upper parts of the glacier, revealing that seasonal input of atmospheric dust can decrease the reflectance also in the accumulation zone of the glacier. The presence of EC and OC in cryoconite samples suggests a relevant role of carbonaceous and organic material in the darkening of the ablation zone. This darkening effect is added to that caused by fine debris from lateral moraines, which is assumed to represent a large fraction of cryoconite. Possible input of anthropogenic activity cannot be excluded and further research is needed to assess the role of human activities in the darkening process of glaciers observed in recent years.
Biological particulate matter or bioaerosol are a subset of atmospheric aerosol. They influence climate, air quality, and health via several mechanisms which often are poorly understood. In ...particular, the quantitative study of possible relationship between bioaerosol viability and air quality or meteorological conditions is an open and relevant issue. The difficulty of retrieving such possible correlations by analyses of data collected during in-field campaigns can benefit of targeted experiments conducted in well-controlled conditions inside atmospheric simulation chambers (ASCs). ChAMBRe (Chamber for Aerosol Modelling and Bio-aerosol Research) is an ASC in Genoa (Italy) designed and built to perform experimental research on bioaerosol. In this article, we focus on bacteria viability. A multi-step protocol was developed and thoroughly tested to cultivate a suitable bacteria population (E. coli), nebulize and inject in a chamber of viable cells, expose and monitor the viability variation inside ChAMBRe, hold at selected conditions, and finally incubate and count the concentration of viable bacteria. The whole procedure showed an estimated lifetime of total (T) and viable (V) E. coli of about 153 and 32 min, respectively and a V : T lifetime ratio of 40±5 min when ChAMBRe is held in a reference baseline condition. The coefficient of variation of 13 % shows how sensitive the protocol is also to changes in viability when the bacteria are exposed to other (e.g. polluted) conditions. First results showing a viability reduction observed exposing the E. coli strain to NOx concentrations and solar irradiation are presented and discussed. The present results pave the way for systematic studies aimed at the definition of dose–effect relationship for several bacteria strains under different conditions of atmospheric pollutants.
In the frame of the EMEP/ACTRIS/COLOSSAL campaign in Milan during winter 2018, equivalent black carbon measurements using the Aethalometer 31 (AE31), the Aethalometer 33 (AE33), and a Multi-Angle ...Absorption Photometer (MAAP) were carried out together with levoglucosan analyses on 12 h resolved PM.sub.2.5 samples collected in parallel.
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