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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.

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).

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.

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.

Biogenic organic precursors play an important role in atmospheric new particle formation (NPF). One of the major precursor species is α-pinene, which upon oxidation can form a suite of products covering a wide range of volatilities. Highly oxygenated organic molecules (HOMs) comprise a fraction of the oxidation products formed. While it is known that HOMs contribute to secondary organic aerosol (SOA) formation, including NPF, they have not been well studied in newly formed particles due to their very low mass concentrations. Here we present gas- and particle-phase chemical composition data from experimental studies of α-pinene oxidation, including in the presence of isoprene, at temperatures (−50 and −30 ∘C) and relative humidities (20 % and 60 %) relevant in the upper free troposphere. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber. The particle chemical composition was analyzed by a thermal desorption differential mobility analyzer (TD-DMA) coupled to a nitrate chemical ionization–atmospheric pressure interface–time-of-flight (CI-APi-TOF) mass spectrometer. CI-APi-TOF was used for particle- and gas-phase measurements, applying the same ionization and detection scheme. Our measurements revealed the presence of C8−10 monomers and C18−20 dimers as the major compounds in the particles (diameter up to ∼ 100 nm). Particularly, for the system with isoprene added, C5 (C5H10O5−7) and C15 compounds (C15H24O5−10) were detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C5 and C15 compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene oxidation products enhance the growth of particles larger than 15 nm. Additionally, we report on the nucleation rates measured at 1.7 nm (J1.7 nm) and compared with previous studies, we found lower J1.7 nm values, very likely due to the higher α-pinene and ozone mixing ratios used in the present study.

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 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.

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 PM2.5 samples collected in parallel. From AE31 and AE33 data, the loading-corrected aerosol attenuation coefficients (bATN) were calculated at seven wavelengths (λ, where λ values are 370, 470, 520, 590, 660, 880, and 950 nm). The aerosol absorption coefficient at 637 nm (babs_MAAP) was determined by MAAP measurements. Furthermore, babs was also measured at four wavelengths (405, 532, 635, 780 nm) on the 12 h resolved PM2.5 samples by a polar photometer (PP_UniMI). After comparing PP_UniMI and MAAP results, we exploited PP_UniMI data to evaluate the filter multiple-scattering enhancement parameter at different wavelengths for AE31 and AE33. We obtained instrument- and wavelength-dependent multiple-scattering enhancement parameters by linear regression of the Aethalometer bATN against the babs measured by PP_UniMI. We found significant dependence of the multiple-scattering enhancement parameter on filter material, hence on the instrument, with a difference of up to 30 % between the AE31 and the AE33 tapes. The wavelength dependence and day–night variations were small – the difference between the smallest and largest value was up to 6 %. Data from the different instruments were used as input to the so-called “Aethalometer model” for optical source apportionment, and instrument dependence of the results was investigated. Inconsistencies among the source apportionment were found fixing the AE31 and AE33 multiple-scattering enhancement parameters to their usual values. In contrast, optimised multiple-scattering enhancement parameters led to a 5 % agreement among the approaches. Also, the component apportionment “MWAA model” (Multi-Wavelength Absorption Analyzer model) was applied to the dataset. It was less sensitive to the instrument and the number of wavelengths, whereas significant differences in the determination of the absorption Ångström exponent for brown carbon were found (up to 22 %).

Cryoconite is rich in natural and artificial radioactivity, but a discussion about its ability to accumulate radionuclides is lacking. A characterization of cryoconite from two Alpine glaciers is presented here. Results confirm that cryoconite is significantly more radioactive than the matrices usually adopted for the environmental monitoring of radioactivity, such as lichens and mosses, with activity concentrations exceeding 10 000 Bq kg−1 for single radionuclides. This makes cryoconite an ideal matrix to investigate the deposition and occurrence of radioactive species in glacial environments. In addition, cryoconite can be used to track environmental radioactivity sources. We have exploited atomic and activity ratios of artificial radionuclides to identify the sources of the anthropogenic radioactivity accumulated in our samples. The signature of cryoconite from different Alpine glaciers is compatible with the stratospheric global fallout and Chernobyl accident products. Differences are found when considering other geographic contexts. A comparison with data from literature shows that Alpine cryoconite is strongly influenced by the Chernobyl fallout, while cryoconite from other regions is more impacted by events such as nuclear test explosions and satellite reentries. To explain the accumulation of radionuclides in cryoconite, the glacial environment as a whole must be considered, and particularly the interaction between ice, meltwater, cryoconite and atmospheric deposition. We hypothesize that the impurities originally preserved into ice and mobilized with meltwater during summer, including radionuclides, are accumulated in cryoconite because of their affinity for organic matter, which is abundant in cryoconite. In relation to these processes, we have explored the possibility of exploiting radioactivity to date cryoconite.

Measurements of aerosol composition and size distributions were taken during the summer of 2013 at the remote island of Lampedusa in the southern central Mediterranean Sea. These measurements were part of the ChArMEx/ADRIMED (Chemistry and Aerosol Mediterranean Experiment/Aerosol Direct Radiative Forcing on the Mediterranean Climate) framework and took place during Special Observation Period 1a (SOP-1a) from 11 June to 5 July 2013. From compact time-of-flight aerosol mass spectrometer (cToF-AMS) measurements in the size range below 1 µm in aerodynamic diameter (PM1), particles were predominately comprised of ammonium and sulfate. On average, ammonium sulfate contributed 63 % to the non-refractory PM1 mass, followed by organics (33 %). The organic aerosol was generally very highly oxidized (f44 values were typically between 0.25 and 0.26). The contribution of ammonium sulfate was generally higher than organic aerosol in comparison to measurements taken in the western Mediterranean but is consistent with studies undertaken in the eastern basin. Source apportionment of organics using a statistical (positive matrix factorization) model revealed four factors: a hydrocarbon-like organic aerosol (HOA), a methanesulfonic-acid-related oxygenated organic aerosol (MSA-OOA), a more oxidized oxygenated organic aerosol (MO-OOA) and a less oxidized oxygenated organic aerosol (LO-OOA). The MO-OOA was the dominant factor for most of the campaign (53 % of the PM1 OA mass). It was well correlated with SO42-, highly oxidized and generally more dominant during easterly air masses originating from the eastern Mediterranean and central Europe. The LO-OOA factor had a very similar composition to the MO-OOA factor but was more prevalent during westerly winds, with air masses originating from the Atlantic Ocean, the western Mediterranean and at high altitudes over France and Spain from mistral winds. The MSA-OOA factor contributed an average 12 % to the PM1 OA and was more dominant during the mistral winds. The HOA, representing observed primary organic aerosol, only contributed 8 % of the average PM1 OA during the campaign. Even though Lampedusa is one of the most remote sites in the Mediterranean, PM1 concentrations (10 ± 5 µg m−3) were comparable to those observed in coastal cities and sites closer to continental Europe. Cleaner conditions corresponded to higher wind speeds. Nucleation and growth of new aerosol particles was observed during periods of north-westerly winds. From a climatology analysis from 1999 to 2012, these periods were much more prevalent during the measurement campaign than during the preceding 13 years. These results support previous findings that highlight the importance of different large-scale synoptic conditions in determining the regional and local aerosol composition and oxidation and also suggest that a non-polluted surface atmosphere over the Mediterranean is rare.

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 Ångström exponent (α) of the sources and mass absorption cross sections (MACs) for fossil fuel emissions at different wavelengths. A multi-time resolution source apportionment study using the Multilinear Engine (ME-2) was performed on a PM10 dataset with different time resolutions (24, 12, and 1 h) collected during two different seasons in Milan (Italy) in 2016. Samples were optically analysed by an in-house polar photometer to retrieve the aerosol absorption coefficient bap (in Mm−1) at four wavelengths (λ=405, 532, 635, and 780 nm) and were chemically characterized for elements, ions, levoglucosan, and carbonaceous components. The dataset joining chemically speciated and optical data was the input for the multi-time resolution receptor model; this approach was proven to strengthen the identification of sources, thus being particularly useful when important chemical markers (e.g. levoglucosan, elemental carbon) are not available. The final solution consisted of eight factors (nitrate, sulfate, resuspended dust, biomass burning, construction works, traffic, industry, aged sea salt); the implemented constraints led to a better physical description of factors and the bootstrap analysis supported the goodness of the solution. As for bap apportionment, consistent with what was expected, biomass burning and traffic were the main contributors to aerosol absorption in the atmosphere. A relevant feature of the approach proposed in this work is the possibility of retrieving a lot of other information about optical parameters; for example, in contrast to the more traditional approach used by optical source apportionment models, here we obtained source-dependent α values without any a priori assumption (α biomass burning =1.83 and α fossil fuels =0.80). In addition, the MACs estimated for fossil fuel emissions were consistent with literature values. It is worth noting that the approach presented here can also be applied using more common receptor models (e.g. EPA PMF instead of multi-time resolution ME-2) if the dataset comprises variables with the same time resolution as well as optical data retrieved by widespread instrumentation (e.g. an Aethalometer instead of in-house instrumentation).

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. We introduce here a modified Sunset Lab Inc. EC–OC analyzer. Starting from a standard commercial instrument, the unit has been modified at the physics department of the University of Genoa (Italy), making possible the alternative use of the standard laser diode at λ=635 nm and of a new laser diode at λ=405 nm. In this way, the optical transmittance through the sample can be monitored at both wavelengths. Since at shorter wavelengths the BrC absorbance is higher, a better sensitivity to this species is gained. The modified instrument also gives the possibility to quantify the BrC concentration in the sample at both wavelengths. The new unit has been thoroughly tested, with both artificial and real-world aerosol samples: the first experiment, in conjunction with the multi-wavelength absorbance analyzer (MWAA; Massabò et al., 2013, 2015), resulted in the first direct determination of the BrC mass absorption coefficient (MAC) at λ=405 nm: MAC =23±1 m2 g−1.

Atmospheric simulation chambers are exploratory platforms used to study various atmospheric processes at realistic but controlled conditions. We describe here a new facility specifically designed for the research on atmospheric bio-aerosol as well as the protocols to produce, inject, expose and collect bio-aerosols. ChAMBRe (Chamber for Aerosol Modelling and Bio-aerosol Research) is installed at the Physics Department of the University of Genoa, Italy, and it is a node of the EUROCHAMP-2020 consortium. The chamber is made of stainless steel with a total volume of about 2.2 m3. The lifetime of aerosol particle with dimension from a few hundreds of nanometres to a few microns varies from about 2 to 10 h. Characteristic parts of the facility are the equipment and the procedures to grow, inject, and extract bacterial strains in the chamber volume while preserving their viability. Bacteria are part of the atmospheric ecosystem and have impact on several levels as: health related issues, cloud formation, and geochemistry. ChAMBRe will host experiments to study the bacterial viability vs. the air quality level, i.e. the atmospheric concentration of gaseous and aerosol pollutants. In this article, we report the results of the characterization tests as well as of the first experiments performed on two bacterial strains belonging to the Gram-positive and Gram-negative groups. A reproducibility at the 10 % level has been obtained in repeated injections and collection runs with a clean atmosphere, assessing this way the chamber sensitivity for systematic studies on bacterial viability vs. environmental conditions.

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.

Deriving absorption coefficients from Aethalometer attenuation data requires different corrections to compensate for artifacts related to filter-loading effects, scattering by filter fibers, and scattering by aerosol particles. In this study, two different correction schemes were applied to seven-wavelength Aethalometer data, using multi-angle absorption photometer (MAAP) data as a reference absorption measurement at 637 nm. The compensation algorithms were compared to five-wavelength offline absorption measurements obtained with a multi-wavelength absorbance analyzer (MWAA), which serves as a multiple-wavelength reference measurement. The online measurements took place in the Amazon rainforest, from the wet-to-dry transition season to the dry season (June–September 2014). The mean absorption coefficient (at 637 nm) during this period was 1.8 ± 2.1 Mm−1, with a maximum of 15.9 Mm−1. Under these conditions, the filter-loading compensation was negligible. One of the correction schemes was found to artificially increase the short-wavelength absorption coefficients. It was found that accounting for the aerosol optical properties in the scattering compensation significantly affects the absorption Ångström exponent (åABS) retrievals. Proper Aethalometer data compensation schemes are crucial to retrieve the correct åABS, which is commonly implemented in brown carbon contribution calculations. Additionally, we found that the wavelength dependence of uncompensated Aethalometer attenuation data significantly correlates with the åABS retrieved from offline MWAA measurements.

We investigate the optical properties of light-absorbing organic carbon (brown carbon) from domestic wood combustion as a function of simulated atmospheric aging. At shorter wavelengths (370–470 nm), light absorption by brown carbon from primary organic aerosol (POA) and secondary organic aerosol (SOA) formed during aging was around 10 % and 20 %, respectively, of the total aerosol absorption (brown carbon plus black carbon). The mass absorption cross section (MAC) determined for black carbon (BC, 13.7 m2 g−1 at 370 nm, with geometric standard deviation GSD =1.1) was consistent with that recommended by Bond et al. (2006). The corresponding MAC of POA (5.5 m2 g−1; GSD =1.2) was higher than that of SOA (2.4 m2 g−1; GSD =1.3) at 370 nm. However, SOA presents a substantial mass fraction, with a measured average SOA ∕ POA mass ratio after aging of ∼5 and therefore contributes significantly to the overall light absorption, highlighting the importance of wood-combustion SOA as a source of atmospheric brown carbon. The wavelength dependence of POA and SOA light absorption between 370 and 660 nm is well described with absorption Ångström exponents of 4.6 and 5.6, respectively. UV-visible absorbance measurements of water and methanol-extracted OA were also performed, showing that the majority of the light-absorbing OA is water insoluble even after aging.

This paper presents new laboratory measurements of the mass absorption efficiency (MAE) between 375 and 850 nm for 12 individual samples of mineral dust from different source areas worldwide and in two size classes: PM10. 6 (mass fraction of particles of aerodynamic diameter lower than 10.6 µm) and PM2. 5 (mass fraction of particles of aerodynamic diameter lower than 2.5 µm). The experiments were performed in the CESAM simulation chamber using mineral dust generated from natural parent soils and included optical and gravimetric analyses. The results show that the MAE values are lower for the PM10. 6 mass fraction (range 37–135 × 10−3 m2 g−1 at 375 nm) than for the PM2. 5 (range 95–711 × 10−3 m2 g−1 at 375 nm) and decrease with increasing wavelength as λ−AAE, where the Ångström absorption exponent (AAE) averages between 3.3 and 3.5, regardless of size. The size independence of AAE suggests that, for a given size distribution, the dust composition did not vary with size for this set of samples. Because of its high atmospheric concentration, light absorption by mineral dust can be competitive with black and brown carbon even during atmospheric transport over heavy polluted regions, when dust concentrations are significantly lower than at emission. The AAE values of mineral dust are higher than for black carbon (∼ 1) but in the same range as light-absorbing organic (brown) carbon. As a result, depending on the environment, there can be some ambiguity in apportioning the aerosol absorption optical depth (AAOD) based on spectral dependence, which is relevant to the development of remote sensing of light-absorbing aerosols and their assimilation in climate models. We suggest that the sample-to-sample variability in our dataset of MAE values is related to regional differences in the mineralogical composition of the parent soils. Particularly in the PM2. 5 fraction, we found a strong linear correlation between the dust light-absorption properties and elemental iron rather than the iron oxide fraction, which could ease the application and the validation of climate models that now start to include the representation of the dust composition, as well as for remote sensing of dust absorption in the UV–vis spectral region.

The airborne transmission of bacterial pathogens poses a significant challenge to public health, especially with the emergence of antibiotic-resistant strains. This study investigated environmental factors influencing the survival of airborne bacteria, focusing on the effects of different carbon dioxide (CO 2 ) and dust concentrations. The experiments were conducted in an atmospheric simulation chamber using the non-resistant wild-type E. coli K12 (JM109) and a multi-resistant variant (JM109-pEC958). Different CO 2 (100 ppm, 800 ppm, 3000 ppm) and dust concentrations (250 µg m -3 , 500 µg m -3 , 2000 µg m -3 ) were tested to encompass a wide range of CO 2 and dust levels. The results revealed that JM109-pEC958 exhibited greater resilience to high CO 2 and dust concentrations compared to its non-resistant counterpart. At 3000 ppm CO 2 , the survival rate of JM109 was significantly reduced, while the survival rate of JM109-pEC958 remained unaffected. At the dust concentration of 250 µg m -3 , JM109 exhibited significantly reduced survival, whereas JM109-pEC958 did not. When the dust concentration was increased to 500 and 2000 µg m -3 , even the JM109-pEC958 experienced substantially reduced survival rates, which were still significantly higher than those of its non-resistant counterpart at these concentrations. These findings suggest that multi-resistant E. coli strains possess mechanisms enabling them to endure extreme environmental conditions better than non-resistant strains, potentially involving regulatory genes or efflux pumps. The study underscores the importance of understanding bacterial adaptation strategies to develop effective mitigation approaches against antibiotic-resistant bacteria in atmospheric environments. Overall, this study provides valuable insights into the interplay between environmental stressors and bacterial survival, serving as a foundational step towards elucidating the adaptation mechanisms of multi-resistant bacteria and informing strategies for combating antibiotic resistance in the atmosphere.

Sub-Saharan Africa is a hotspot for biomass burning (BB)-derived carbonaceous aerosols, including light-absorbing organic (brown) carbon (BrC). However, the chemically complex nature of BrC in BB aerosols from this region is not fully understood. We generated smoke in a chamber through smoldering combustion of common sub-Saharan African biomass fuels (hardwoods, cow dung, savanna grass, and leaves). We quantified aethalometer-based, real-time light-absorption properties of BrC-containing organic-rich BB aerosols, accounting for variations in wavelength, fuel type, relative humidity, and photochemical aging conditions. In filter samples collected from the chamber and Botswana in the winter, we identified 182 BrC species, classified into lignin pyrolysis products, nitroaromatics, coumarins, stilbenes, and flavonoids. Using an extensive set of standards, we determined species-specific mass and emission factors. Our analysis revealed a linear relationship between the combined BrC species contribution to chamber-measured BB aerosol mass (0.4-14%) and the mass-absorption cross-section at 370 nm (0.2-2.2 m 2 g -1 ). Hierarchical clustering resolved key molecular-level components from the BrC matrix, with photochemically aged emissions from leaf and cow-dung burning showing BrC fingerprints similar to those found in Botswana aerosols. These quantitative findings could potentially help refine climate model predictions, aid in source apportionment, and inform effective air quality management policies for human health and the global climate.

Urban textures of the Italian cities are peculiarly shaped by the local geography generating similarities among cities placed in different regions but comparable topographical districts. This suggested the following scientific question: can different topographies generate significant differences on the PM 10 chemical composition at Italian urban sites that share similar geography despite being in different regions? To investigate whether such communalities can be found and are applicable at Country-scale, we propose here a novel methodological approach. A dataset comprising season-averages of PM 10 mass concentration and chemical composition data was built, covering the decade 2005-2016 and referring to urban sites only (21 cities). Statistical analyses, estimation of missing data, identification of latent clusters and source apportionment modeling by Positive Matrix Factorization (PMF) were performed on this unique dataset. The first original result is the demonstration that a dataset with atypical time resolution can be successfully exploited as an input matrix for PMF obtaining Country-scale representative chemical profiles, whose physical consistency has been assessed by different tests of modeling performance. Secondly, this dataset can be considered a reference repository of season averages of chemical species over the Italian territory and the chemical profiles obtained by PMF for urban Italian agglomerations could contribute to emission repositories. These findings indicate that our approach is powerful, and it could be further employed with datasets typically available in the air pollution monitoring networks., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 The Authors. Published by Elsevier B.V. All rights reserved.)

The main nucleating vapor in the atmosphere is thought to be sulfuric acid (H 2 SO 4 ), stabilized by ammonia (NH 3 ). However, in marine and polar regions, NH 3 is generally low, and H 2 SO 4 is frequently found together with iodine oxoacids [HIO x , i.e., iodic acid (HIO 3 ) and iodous acid (HIO 2 )]. In experiments performed with the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we investigated the interplay of H 2 SO 4 and HIO x during atmospheric particle nucleation. We found that HIO x greatly enhances H 2 SO 4 (-NH 3 ) nucleation through two different interactions. First, HIO 3 strongly binds with H 2 SO 4 in charged clusters so they drive particle nucleation synergistically. Second, HIO 2 substitutes for NH 3 , forming strongly bound H 2 SO 4 -HIO 2 acid-base pairs in molecular clusters. Global observations imply that HIO x is enhancing H 2 SO 4 (-NH 3 ) nucleation rates 10- to 10,000-fold in marine and polar regions.

The mechanistic pathway by which high relative humidity (RH) affects gas-particle partitioning remains poorly understood, although many studies report increased secondary organic aerosol (SOA) yields at high RH. Here, we use real-time, molecular measurements of both the gas and particle phase to provide a mechanistic understanding of the effect of RH on the partitioning of biogenic oxidized organic molecules (from α-pinene and isoprene) at low temperatures (243 and 263 K) at the CLOUD chamber at CERN. We observe increases in SOA mass of 45 and 85% with increasing RH from 10-20 to 60-80% at 243 and 263 K, respectively, and attribute it to the increased partitioning of semi-volatile compounds. At 263 K, we measure an increase of a factor 2-4 in the concentration of C 10 H 16 O 2-3 , while the particle-phase concentrations of low-volatility species, such as C 10 H 16 O 6-8 , remain almost constant. This results in a substantial shift in the chemical composition and volatility distribution toward less oxygenated and more volatile species at higher RH (e.g., at 263 K, O/C ratio = 0.55 and 0.40, at RH = 10 and 80%, respectively). By modeling particle growth using an aerosol growth model, which accounts for kinetic limitations, we can explain the enhancement in the semi-volatile fraction through the complementary effect of decreased compound activity and increased bulk-phase diffusivity. Our results highlight the importance of particle water content as a diluting agent and a plasticizer for organic aerosol growth.

It is a well - established fact that road traffic is one of the main contributors to ambient levels of airborne particulate matter (APM). This study was carried out at a traffic site in which the PM 10 levels are monitored all year round. A trend analysis of these levels revealed that over a decade there was no discernible trend, with the PM 10 concentrations normally hovering around the EU limit values. In 2018, one of these limit values was exceeded. The contribution of traffic at the site was therefore investigated through a chemical speciation of 209 PM 10 samples collected throughout this year. The speciation data were used in a source apportionment exercise in which the output of the PMF model was further refined using the lesser-known, constraint weighted non - negative matrix factorization (CW - NMF) model. This technique enabled the isolation of two factors clearly related to traffic, which were labelled as "exhaust contribution" (responsible for 3.4% of the PM 10 ), "tire/brake wear contribution" (contributing 17% of the PM 10 ). Additionally, a factor including both traffic resuspended dust and crustal material was also isolated and labelled "road dust/crustal" factor. The two contributors to the factor jointly contribute 18% to the PM 10 and the contribution of the traffic resuspended dust was estimated at 7.3%. The traffic resuspended component of this factor together with the "tire/brake wear contribution" jointly make up the non-exhaust contribution of traffic - derived dust. Consonant with what has been known for quite some time, the exhaust fraction is the minor component of traffic PM 10 . It is therefore, clear that policies aimed at controlling traffic derived PM 10 pollution at the receptor will have a minimal effect unless the non - exhaust emissions are adequately controlled., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Dimethyl sulfide (DMS) influences climate via cloud condensation nuclei (CCN) formation resulting from its oxidation products (mainly methanesulfonic acid, MSA, and sulfuric acid, H 2 SO 4 ). Despite their importance, accurate prediction of MSA and H 2 SO 4 from DMS oxidation remains challenging. With comprehensive experiments carried out in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at CERN, we show that decreasing the temperature from +25 to -10 °C enhances the gas-phase MSA production by an order of magnitude from OH-initiated DMS oxidation, while H 2 SO 4 production is modestly affected. This leads to a gas-phase H 2 SO 4 -to-MSA ratio (H 2 SO 4 /MSA) smaller than one at low temperatures, consistent with field observations in polar regions. With an updated DMS oxidation mechanism, we find that methanesulfinic acid, CH 3 S(O)OH, MSIA, forms large amounts of MSA. Overall, our results reveal that MSA yields are a factor of 2-10 higher than those predicted by the widely used Master Chemical Mechanism (MCMv3.3.1), and the NO x effect is less significant than that of temperature. Our updated mechanism explains the high MSA production rates observed in field observations, especially at low temperatures, thus, substantiating the greater importance of MSA in the natural sulfur cycle and natural CCN formation. Our mechanism will improve the interpretation of present-day and historical gas-phase H 2 SO 4 /MSA measurements.

New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN) 1-4 . However, the precursor vapours that drive the process are not well understood. With experiments performed under upper tropospheric conditions in the CERN CLOUD chamber, we show that nitric acid, sulfuric acid and ammonia form particles synergistically, at rates that are orders of magnitude faster than those from any two of the three components. The importance of this mechanism depends on the availability of ammonia, which was previously thought to be efficiently scavenged by cloud droplets during convection. However, surprisingly high concentrations of ammonia and ammonium nitrate have recently been observed in the upper troposphere over the Asian monsoon region 5,6 . Once particles have formed, co-condensation of ammonia and abundant nitric acid alone is sufficient to drive rapid growth to CCN sizes with only trace sulfate. Moreover, our measurements show that these CCN are also highly efficient ice nucleating particles-comparable to desert dust. Our model simulations confirm that ammonia is efficiently convected aloft during the Asian monsoon, driving rapid, multi-acid HNO 3 -H 2 SO 4 -NH 3 nucleation in the upper troposphere and producing ice nucleating particles that spread across the mid-latitude Northern Hemisphere., (© 2022. The Author(s).)

Accurate and temporally consistent measurements of light absorbing aerosol (LAA) heating rate (HR) and of its source apportionment (fossil-fuel, FF; biomass-burning, BB) and speciation (black and brown Carbon; BC, BrC) are needed to evaluate LAA short-term climate forcing. For this purpose, wavelength- and time-dependent accurate LAA absorption coefficients are required. HR was experimentally determined and apportioned (sources/species) in the EMEP/ACTRIS/COLOSSAL-2018 winter campaign in Milan (urban-background site). Two Aethalometers (AE31/AE33) were installed together with a MAAP, CPC, OPC, a low volume sampler (PM 2.5 ) and radiation instruments. AE31/AE33 multiple-scattering correction factors (C) were determined using two reference systems for the absorption coefficient: 1) 5-wavelength PP_UniMI with low time resolution (12 h, applied to PM 2.5 samples); 2) timely-resolved MAAP data at a single wavelength. Using wavelength- and time-independent C values for the AE31 and AE33 obtained with the same reference device, the total HR showed a consistency (i.e. reproducibility) with average values comparable at 95% probability. However, if different reference devices/approaches are used, i.e. MAAP is chosen as reference instead of a PP_UniMI, the HR can be overestimated by 23-30% factor (by both AE31/AE33). This became more evident focusing on HR apportionment: AE33 data (corrected by a wavelength- and time-independent C) showed higher HR FF (+24 ± 1%) and higher HR BC (+10 ± 1%) than that of AE31. Conversely, HR BB and HR BrC were -28 ± 1% and -29 ± 1% lower for AE33 compared to AE31. These inconsistencies were overcome by introducing a wavelength-dependent C λ for both AE31 and AE33, or using multi-wavelength apportionment methods, highlighting the need for further studies on the influence of wavelength corrections for HR determination. Finally, the temporally-resolved determination of C resulted in a diurnal cycle of the HR not statistically different whatever the source- speciation- apportionment used., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Background: During the COVID-19 pandemic, the number of individuals needing hospital admission has sometimes exceeded the availability of hospital beds. Since hospitalization can have detrimental effects on older individuals, preference has been given to younger patients. The aim of this study was to assess the utility of hospitalization for elderly affected by COVID-19. We hypothesized that their mortality decreases when there is greater access to hospitals., Methods: This study examined 1902 COVID-19 patients consecutively admitted to three large hospitals in Milan, Italy. Overall mortality data for Milan from the same period was retrieved. Based on emergency department (ED) data, both peak and off-peak phases were identified. The percentage of elderly patients admitted to EDs during these two phases were compared by calculating the standardized mortality ratio (SMR) of the individuals younger than, versus older than, 80 years., Results: The median age of the patients hospitalized during the peak phase was lower than the median age during the off-peak phase (64 vs. 75 years, respectively; p <0.001). However, while the SMR for the younger patients was lower during the off-peak phase (1.98, 95% CI: 1.72-2.29 versus 1.40, 95% CI: 1.25-1.58, respectively), the SMR was similar between both phases for the elderly patients (2.28, 95% CI: 2.07-2.52 versus 2.48, 95% CI: 2.32-2.65, respectively)., Conclusions: Greater access to hospitals during an off-peak phase did not affect the mortality rate of COVID-19-positive elderly patients in Milan. This finding, if confirmed in other settings, should influence future decisions regarding resource management of health care organizations., Competing Interests: The authors have declared that no competing interests exist.

Receptor modelling techniques are widely used in order to identify the main natural and anthropogenic processes driving aerosol levels at a receptor. In this work, Positive Matrix Factorization (PMF) was used to apportion PM 2.5 levels at a traffic site (Msida) located in a coastal town. 180 filters collected throughout a yearly sampling campaign conducted in 2016, were chemically characterized by light absorbance analysis, x-ray fluorescence and ion chromatography in order to determine the concentrations of black carbon, 17 elements and 5 ions, respectively. The resulting chemical data base was used in conjunction with PMF in order to identify the 7 components affecting the PM 2.5 levels at the receptor site. Six of these sources are considered to be typical of the atmospheric composition of coastal traffic sites: traffic (27.3%), ammonium sulfate (23.6%), Saharan dust (15%), aged sea salt (12.7%), shipping (5%) and fresh sea salt (4.6%). This is the first time that such a study was carried out in Malta and helps in understanding the aerosol pollution climate of the Central Mediterranean, which is still relatively understudied when compared to the Eastern and Western Mediterranean. Furthermore, we have isolated a factor exclusive to Malta: the fireworks component, which is responsible for 2.9% of the PM 2.5 and which has health implications due to its chemical composition. The results of this work should also serve to guide the policy makers in achieving the necessary emission reductions in order to achieve the WHO guideline for PM 2.5 by 2020., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Heavy fuel oil (HFO) particulate matter (PM) emitted by marine engines is known to contain toxic heavy metals, including vanadium (V) and nickel (Ni). The toxicity of such metals will depend on the their chemical state, size distribution, and mixing state. Using online soot-particle aerosol mass spectrometry (SP-AMS), we quantified the mass of five metals (V, Ni, Fe, Na, and Ba) in HFO-PM soot particles produced by a marine diesel research engine. The in-soot metal concentrations were compared to in-PM 2.5 measurements by inductively coupled plasma-optical emission spectroscopy (ICP-OES). We found that <3% of total PM 2.5 metals was associated with soot particles, which may still be sufficient to influence in-cylinder soot burnout rates. Since these metals were most likely present as oxides, whereas studies on lower-temperature boilers report a predominance of sulfates, this result implies that the toxicity of HFO PM depends on its combustion conditions. Finally, we observed a 4-to-25-fold enhancement in the ratio V:Ni in soot particles versus PM 2.5 , indicating an enrichment of V in soot due to its lower nucleation/condensation temperature. As this enrichment mechanism is not dependent on soot formation, V is expected to be generally enriched within smaller HFO-PM particles from marine engines, enhancing its toxicity.

An interlaboratory comparison was performed to evaluate the analytical methods for quantification of anhydrosugars - levoglucosan, mannosan, galactosan - and biosugars - arabitol, glucose and mannitol - in atmospheric aerosol. The performance of 10 laboratories in Italy currently involved in such analyses was investigated on twenty-six PM (particulate matter) ambient filters, three synthetic PM filters and three aqueous standard solutions. An acceptable interlaboratory variability was found, determined as the mean relative standard deviation (RSD%) of the results from the participating laboratories, with the mean RSD% values ranging from 25% to 46% and decreasing with increasing sugar concentration. The investigated methods show good accuracy, evaluated as the percentage error (ε%) related to mean values, since method biases ranged within ±20% for most of the analytes measured in the different laboratories. The detailed investigation (ANOVA analysis at p < 0.05) of the contribution of each laboratory to the total variability and the measurement accuracy shows that comparable results are generated by the different methods, despite the great diversity in terms of extraction conditions, chromatographic separation - more recent LC (liquid chromatography) and EC (exchange chromatography) methods compared to more widespread GC (gas chromatography) - and detection systems, namely PAD (pulsed amperometric detection) or mass spectrometry., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

Cryoconite, the typical sediment found on the surface of glaciers, is mainly known in relation to its role in glacial microbiology and in altering the glacier albedo. But if these aspects are relatively well addressed, the same cannot be said about the geochemical properties of cryoconite and the possible interactions with glacial and peri-glacial environment. Current glacier retreat is responsible for the secondary emission of species deposited in high-altitude regions in the last decades. The role played by cryoconite in relation to such novel geochemical fluxes is largely unknown. Few and scarce observations suggest that it could interact with these processes, accumulating specific substances, but why, how and to what extent remain open questions. Through a multi-disciplinary approach we tried to shed lights. Results reveal that the peculiar composition of cryoconite is responsible for an extreme accumulation capability of this sediment, in particular for some, specific, anthropogenic substances.