Hourly-resolved aerosol chemical speciation data can be a highly powerful tool to determine the source origin of atmospheric pollutants in urban environments. Aerosol mass concentrations of seventeen ...elements (Na, Mg, Al, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Sr and Pb) were obtained by time (1 h) and size (PM2.5 particulate matter < 2.5 μm) resolved aerosol samples analysed by Particle Induced X-ray Emission (PIXE) measurements. In the Marie Curie European Union framework of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies), the approach used is the simultaneous sampling at two monitoring sites in Barcelona (Spain) during September-October 2010: an urban background site (UB) and a street canyon traffic road site (RS). Elements related to primary non-exhaust traffic emission (Fe, Cu), dust resuspension (Ca) and anthropogenic Cl were found enhanced at the RS, whereas industrial related trace metals (Zn, Pb, Mn) were found at higher concentrations at the more ventilated UB site. When receptor modelling was performed with positive matrix factorization (PMF), nine different aerosol sources were identified at both sites: three types of regional aerosols (regional sulphate (S) - 27%, biomass burning (K) - 5%, sea salt (Na-Mg) - 17%), three types of dust aerosols (soil dust (Al-Ti) - 17%, urban crustal dust (Ca) - 6%, and primary traffic non-exhaust brake dust (Fe-Cu) - 7%), and three types of industrial aerosol plumes-like events (shipping oil combustion (V-Ni) - 17%, industrial smelters (Zn-Mn) - 3%, and industrial combustion (Pb-Cl) - 5%, percentages presented are average source contributions to the total elemental mass measured). The validity of the PMF solution of the PIXE data is supported by very good correlations with external single particle mass spectrometry measurements. Some important conclusions can be drawn about the PM2.5 mass fraction simultaneously measured at the UB and RS sites: (1) the regional aerosol sources impact both monitoring sites at similar concentrations regardless their different ventilation conditions; (2) by contrast, local industrial aerosol plumes associated with shipping oil combustion and smelters activities have a higher impact on the more ventilated UB site; (3) a unique source of Pb-Cl (associated with combustion emissions) is found to be the major (82%) source of fine Cl in the urban agglomerate; (4) the mean diurnal variation of PM2.5 primary traffic non-exhaust brake dust (Fe-Cu) suggests that this source is mainly emitted and not resuspended, whereas PM2.5 urban dust (Ca) is found mainly resuspended by both traffic vortex and sea breeze; (5) urban dust (Ca) is found the aerosol source most affected by land wetness, reduced by a factor of eight during rainy days and suggesting that wet roads may be a solution for reducing urban dust concentrations.
The Redundancy Discrimination Analysis (RDA) and Spearman correlation coefficients were used to investigate relationships between airborne bacteria at the phylum and genus level and chemical species ...in winter and spring PM10 samples over Southeastern Italy. The identification of main chemical species/pollution sources that were related to and likely affected the bacterial community structure was the main goal of this work. The 16S rRNA gene metabarcoding approach was used to characterize airborne bacteria. Seventeen phyla and seventy-nine genera contributing each by mean within-sample relative abundance percentage > 0.01% were identified in PM10 samples, which were chemically characterized for 33 species, including ions, metals, OC, and EC (organic and elemental carbon, respectively). Chemical species were associated with six different pollution sources. A shift from winter to spring in both bacterial community structure and chemical species mass concentrations/sources and the relationships between them was observed. RDA triplots pointed out significant correlations for all tested bacterial phyla (genera) with other phyla (genera) and/or with chemical species, in contrast to correlation coefficient results, which showed that few phyla (genera) were significantly correlated with chemical species. More specifically, in winter Bacillus and Chryseobacterium were the only genera significantly correlated with chemical species likely associated with particles from soil-dust and anthropogenic pollution source, respectively. In spring, Enterobacter and Sphingomonas were the only genera significantly correlated with chemical species likely associated with particles from the anthropogenic pollution and the marine and soil-dust sources, respectively. The results of this study also showed that the correlation coefficients were the best tool to obtain unequivocal identifications of the correlations of phyla (genera) with chemical species. The seasonal changes of the PM10 chemical composition, the microbial community structure, and their relationships suggested that the seasonal changes of atmospheric particles may have likely contributed to seasonal changes of bacterial community in the atmosphere.
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•Chemical species and airborne bacteria abundance relationships are season-dependent•Correlation coefficients and RDA are used to study bacterium-chemical relations•Spearman coefficients show good evidence of relations between bacteria and chemicals•Proteobacteria phylum does not show significant correlations with chemical species•Chemical species/pollution sources likely affect the bacterial community structure
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
The present study aimed at performing PM10 source apportionment, using positive matrix factorization (PMF), based on filter samples collected every 4h at a sub-urban station in the Paris region ...(France) during a PM pollution event in March 2015 (PM10>50μgm−3 for several consecutive days). The PMF model allowed to deconvolve 11 source factors. The use of specific primary and secondary organic molecular markers favoured the determination of common sources such as biomass burning and primary traffic emissions, as well as 2 specific biogenic SOA (marine+isoprene) and 3 anthropogenic SOA (nitro-PAHs+oxy-PAHs+phenolic compounds oxidation) factors. This study is probably the first one to report the use of methylnitrocatechol isomers as well as 1-nitropyrene to apportion secondary OA linked to biomass burning emissions and primary traffic emissions, respectively. Secondary organic carbon (SOC) fractions were found to account for 47% of the total OC. The use of organic molecular markers allowed the identification of 41% of the total SOC composed of anthropogenic SOA (namely, oxy-PAHs, nitro-PAHs and phenolic compounds oxidation, representing 15%, 9%, 11% of the total OC, respectively) and biogenic SOA (marine+isoprene) (6% in total). Results obtained also showed that 35% of the total SOC originated from anthropogenic sources and especially PAH SOA (oxy-PAHs+nitro-PAHs), accounting for 24% of the total SOC, highlighting its significant contribution in urban influenced environments. Anthropogenic SOA related to nitro-PAHs and phenolic compounds exhibited a clear diurnal pattern with high concentrations during the night indicating the prominent role of night-time chemistry but with different chemical processes involved.
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•Source apportionment using key primary and secondary organic molecular markers•High resolution filter data allowed the understanding of the atmospheric processes.•7 SOA factors identified including 2 specific biogenic SOA and 3 anthropogenic SOA•Traffic and biomass burning SOA resolved using 1-nitropyrene and methylnitrocatechols•Role of night-time chemistry for SOA related to nitro-PAHs and phenolic compounds
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
In this paper, a new way to apportion the absorption coefficient (babs) of carbonaceous atmospheric aerosols starting from a multi-wavelength optical analysis is shown. This methodology can ...disentangle and quantify the contribution to total absorption of equivalent black carbon (EBC) emitted by wood burning (EBCWB) and fossil fuel (EBCFF) as well as brown carbon (BrC) due to incomplete combustion. The method uses the information gathered at five different wavelengths in a renewed and upgraded version of the approach usually referred to as Aethalometer model. Moreover, we present the results of an apportionment study of carbonaceous aerosol sources performed in a rural area and in a coastal city, both located in the North-West of Italy. Results obtained by the proposed approach are validated against independent measurements of levoglucosan and radiocarbon. At the rural site the EBCWB and EBCFF relative contributions are about 40% and 60% in winter and 15% and 85% in summer, respectively. At the coastal urban site, EBCWB and EBCFF are about 15% and 85% during fall. The OC contribution to the wood burning source at the rural site results approximately 50% in winter and 10% in summer and about 15% at the coastal urban site in fall. The new methodology also provides a direct measurement of the absorption Ångström exponent of BrC (αBrC) which resulted αBrC = 3.95 ± 0.20.
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•Aerosol light absorption at several λs due to Black and Brown Carbon is measured.•The value of Ångström exponent of Brown Carbon is directly extracted by raw data.•The new apportionment procedure disentangles fossil and wood burning contributions.•Equivalent Black Carbon and Organic Carbon are separately apportioned.•The procedure is validated against independent Levoglucosan and 14C determination.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
At the 3MV Tandetron accelerator of the LABEC laboratory of INFN (Florence, Italy) an external beam facility is fully dedicated to PIXE-PIGE measurements of the elemental composition of atmospheric ...aerosols. All the elements with Z>10 are simultaneously detected by PIXE typically in one minute. This setup allows us an easy automatic positioning, changing and scanning of samples collected by different kinds of devices: long series of daily PM (Particulate Matter) samples can be analysed in short times, as well as size-segregated and high time-resolution aerosol samples.
Thanks to the capability of detecting all the crustal elements, PIXE-PIGE analyses are unrivalled in the study of mineral dust: consequently, they are very effective in the study of natural aerosols, like, for example, Saharan dust intrusions. Among the detectable elements there are also important markers of anthropogenic sources, which allow effective source apportionment studies in polluted urban environments using a multivariate method like Positive Matrix Factorization (PMF).
Examples regarding recent monitoring campaigns, performed in urban and remote areas, both daily and with high time resolution (hourly samples), as well as with size selection, are presented. The importance of the combined use of the Particle Induced Gamma Ray emission technique (PIGE) and of other complementary (non-nuclear) techniques is highlighted.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
Daily time series measurements of elements or compounds are widely used to apportion the contribution of specific sources of particulate matter concentration in the atmosphere. We present results ...obtained for the urban area of Genoa (Italy) based on several hundred of PM10, PM2.5 and PM1 daily samples collected in sites with different geo-morphological and urbanization characteristics. Elemental concentrations of Na to Pb were obtained through Energy Dispersive X-Ray Fluorescence (ED-XRF), and the contributions of specific sources of particulate matter (PM) concentration were apportioned through Positive Matrix Factorization (PMF). By sampling at different sites we were able to obtain, in each PM fraction, the average and stable values for the tracers of specific sources, in particular traffic (Cu, Zn, Pb) and heavy oil combustion (V, Ni). We could also identify and quote the contamination of anthropogenic PM in “natural” sources (sea, soil dust). Sampling at several sites in the same urban area allowed us to resolve local characteristics as well as to quote average values.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
On 2016 July 31 the ICECUBE collaboration reported the detection of a high-energy starting event induced by an astrophysical neutrino. Here, we report on a search for a gamma-ray counterpart to the ...ICECUBE-160731 event, made with the AGILE satellite. No detection was found spanning the time interval of 1 ks around the neutrino event time T0 using the AGILE "burst search" system. Looking for a possible gamma-ray precursor in the results of the AGILE-GRID automatic Quick Look procedure over predefined 48-hr time bins, we found an excess above 100 MeV between 1 and 2 days before T0, which is positionally consistent with the ICECUBE error circle, that has a post-trial significance of about . A refined data analysis of this excess confirms, a posteriori, the automatic detection. The new AGILE transient source, named AGL J1418+0008, thus stands as a possible ICECUBE-160731 gamma-ray precursor. No other space missions nor ground observatories have reported any detection of transient emission consistent with the ICECUBE event. We show that Fermi-LAT had a low exposure for the ICECUBE region during the AGILE gamma-ray transient. Based on an extensive search for cataloged sources within the error regions of ICECUBE-160731 and AGL J1418+0008, we find a possible common counterpart showing some of the key features associated with the high-energy peaked BL Lac (HBL) class of blazars. Further investigations on the nature of this source using dedicated SWIFT ToO data are presented.
Abstract
We present the results of a systematic search and analysis of GRBs detected by the Astrorivelatore Gamma ad Immagini LEggero (AGILE) MiniCALorimeter (MCAL; 0.4–100 MeV) over a time frame of ...13 yr, from 2007 to 2020 November. The MCAL GRB sample consists of 503 bursts triggered by MCAL, 394 of which were fully detected onboard with high time resolution. The sample consists of about 44% short GRBs and 56% long GRBs. In addition, 109 bursts triggered partial MCAL onboard data acquisitions, providing further detections that can be used for joint analyses or triangulations. More than 90% of these GRBs were also detected by the AGILE Scientific RateMeters (RMs), providing simultaneous observations between 20 keV and 100 MeV. We performed spectral analysis of these events in the 0.4–50 MeV energy range. We could fit the time-integrated spectrum of 258 GRBs with a single power-law model, resulting in a mean photon index 〈
β
〉of−2.3. Among them, 43 bursts could also be fitted with a Band model, with peak energy above 400 keV, resulting in a mean low-energy photon index 〈
α
〉 = −0.6, a mean high-energy photon index 〈
β
〉 = −2.5, and a mean peak energy 〈
E
p
〉 = 640 keV. The AGILE MCAL GRB sample mostly consists of hard-spectrum GRBs, with a large fraction of short-duration events. We discuss properties and features of the MCAL bursts, whose detections can be used to perform joint broad-band analysis with other missions, and to provide insights on the high-energy component of the prompt emission in the tens of mega electron volt energy range.
A multi-analytical approach to chemical analysis of inhalable urban atmospheric particulate matter (PM), integrating particle induced X-ray emission, inductively coupled plasma mass ...spectrometry/atomic emission spectroscopy, chromatography and thermal–optical transmission methods, allows comparison between hourly (Streaker) and 24-h (High volume sampler) data and consequently improved PM chemical characterization and source identification. In a traffic hot spot monitoring site in Madrid (Spain) the hourly data reveal metallic emissions (Zn, Cu, Cr, Fe) and resuspended mineral dust (Ca, Al, Si) to be closely associated with traffic flow. These pollutants build up during the day, emphasizing evening rush hour peaks, but decrease (especially their coarser fraction PM2.5–10) after nocturnal road washing. Positive matrix factorization (PMF) analysis of a large Streaker database additionally reveals two other mineral dust components (siliceous and sodic), marine aerosol, and minor, transient events which we attribute to biomass burning (K-rich) and industrial (incinerator?) Zn, Pb plumes. Chemical data on 24-h filters allows the measurement of secondary inorganic compounds and carbon concentrations and offers PMF analysis based on a limited number of samples but using fuller range of trace elements which, in the case of Madrid, identifies the continuing minor presence of a coal combustion source traced by As, Se, Ge and Organic Carbon. This coal component is more evident in the city air after the change to the winter heating season in November. Trace element data also allow use of discrimination diagrams such as V/Rb vs. La/Ce and ternary plots to illustrate variations in atmospheric chemistry (such as the effect of Ce-emissions from catalytic converters), with Madrid being an example of a city with little industrial pollution, recently reduced coal emissions, but serious atmospheric contamination by traffic emissions.
► We apply a multi-analytical approach to the chemical characterization of urban air. ► City traffic controls hourly variations in metallic emissions and mineral dust. ► Winter coal combustion is traced by atmospheric As, Se, Ge and Organic Carbon. ► Traffic exhaust enriches city air in Cerium. ► Applying PMF to both hourly (PIXE) and daily (ICP) data improves source apportionment.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
Measurements of aerosol chemical composition made on the island of Lampedusa, south of the Sicily channel, during years 2004–2008, are used to identify the influence of heavy fuel oil (HFO) ...combustion emissions on aerosol particles in the Central Mediterranean. Aerosol samples influenced by HFO are characterized by elevated Ni and V soluble fraction (about 80% for aerosol from HFO combustion, versus about 40% for crustal particles), high V and Ni to Si ratios, and values of Vsol>6 ng m−3. Evidence of HFO combustion influence is found in 17% of the daily samples. Back trajectories analysis on the selected events show that air masses prevalently come from the Sicily channel region, where an intense ship traffic occurs. This behavior suggests that single fixed sources like refineries are not the main responsible for the elevated V and Ni events, which are probably mainly due to ships emissions. Vsol, Nisol, and non-sea salt SO42− (nssSO42−) show a marked seasonal behaviour, with an evident summer maximum. Such a pattern can be explained by several processes: (i) increased photochemical activity in summer, leading to a faster production of secondary aerosols, mainly nssSO42−, from the oxidation of SO2 (ii) stronger marine boundary layer (MBL) stability in summer, leading to higher concentration of emitted compounds in the lowest atmospheric layers. A very intense event in spring 2008 was studied in detail, also using size segregated chemical measurements. These data show that elements arising from heavy oil combustion (V, Ni, Al, Fe) are distributed in the sub-micrometric fraction of the aerosol, and the metals are present as free metals, carbonates, oxides hydrates or labile complex with organic ligands, so that they are dissolved in mild condition (HNO3, pH1.5). Data suggest a characteristic nssSO42−/V ratio in the range 200–400 for HFO combustion aerosols in summer at Lampedusa. By using the value of 200 a lower limit for the HFO contribution to total sulphates is estimated. HFO combustion emissions account, as a summer average, at least for 1.2 μg m−3, representing about 30% of the total nssSO42−, 3.9% of PM10, 8% of PM2.5, and 11% of PM1. Within the used dataset, sulphate from HFO combustion emissions reached the peak value of 6.1 μg m−3 on 26 June 2008, when it contributed by 47% to nssSO42−, and by 15% to PM10.
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