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1.
A European aerosol phenomenology - 7 : high-time resolution chemical characteristics of submicron particulate matter across Europe
M. Bressi, F. Cavalli, Jean-Philippe Putaud, R. Fröhlich, J. -E. Petit, W. Aas, M. Äijälä, A. Alastuey, J. D. Allan, M. Aurela, Iasonas Stavroulas, Marta Via, 2021, izvirni znanstveni članek

Opis: Similarities and differences in the submicron atmospheric aerosol chemical composition are analyzed from a unique set of measurements performed at 21 sites across Europe for at least one year. These sites are located between 35 and 62°N and 10° W – 26°E, and represent various types of settings (remote, coastal, rural, industrial, urban). Measurements were all carried out on-line with a 30-min time resolution using mass spectroscopy based instruments known as Aerosol Chemical Speciation Monitors (ACSM) and Aerosol Mass Spectrometers (AMS) and following common measurement guidelines. Data regarding organics, sulfate, nitrate and ammonium concentrations, as well as the sum of them called non-refractory submicron aerosol mass concentration ([NR-PM1]) are discussed. NR-PM1 concentrations generally increase from remote to urban sites. They are mostly larger in the mid-latitude band than in southern and northern Europe. On average, organics account for the major part (36–64%) of NR-PM1 followed by sulfate (12–44%) and nitrate (6–35%). The annual mean chemical composition of NR-PM1 at rural (or regional background) sites and urban background sites are very similar. Considering rural and regional background sites only, nitrate contribution is higher and sulfate contribution is lower in mid-latitude Europe compared to northern and southern Europe. Large seasonal variations in concentrations (μg/m³) of one or more components of NR-PM1 can be observed at all sites, as well as in the chemical composition of NR-PM1 (%) at most sites. Significant diel cycles in the contribution to [NR-PM1] of organics, sulfate, and nitrate can be observed at a majority of sites both in winter and summer. Early morning minima in organics in concomitance with maxima in nitrate are common features at regional and urban background sites. Daily variations are much smaller at a number of coastal and rural sites. Looking at NR-PM1 chemical composition as a function of NR-PM1 mass concentration reveals that although organics account for the major fraction of NR-PM1 at all concentration levels at most sites, nitrate contribution generally increases with NR-PM1 mass concentration and predominates when NR-PM1 mass concentrations exceed 40 μg/m³ at half of the sites.
Ključne besede: aerosol, chemical composition, mass spectrometry, phenomenology
Objavljeno v RUNG: 10.05.2024; Ogledov: 167; Prenosov: 2
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2.
Molekularna karakterizacija lebdećih čestica slobodne troposfere sa Opservatorija Pico planine
Katja Džepina, Claudio Mazzoleni, Paulo Fialho, Swarup China, B. Zhang, R. Chris Owen, D. Helmig, J. Hueber, Sumit Kumar, J. A. Perlinger, 2017, objavljeni povzetek znanstvenega prispevka na konferenci

Opis: Long-range transported free tropospheric aerosol was sampled at the PMO (38°28’15’’N, 28°24’14’’W; 2225 m amsl) on Pico Island of the Azores in the North Atlantic. Filter-collected aerosol during summer 2012 was analysed for organic and elemental carbon, and inorganic ions. The average aerosol ambient concentration was 0.9 µg m-3. Organic aerosol contributed the majority of mass (57%), followed by sulphate (21%) and nitrate (17%). Filter-collected aerosol was positively correlated with on-line aerosol measurements of black carbon, light scattering and number concentration. Water-soluble organic compounds (WSOC) from 9/24 and 9/25 samples collected during a pollution event were analysed with ultrahigh-resolution FT-ICR MS. FLEXPART analysis showed the air masses were very aged (>12 days). ~4000 molecular formulas were assigned to each of the mass spectra between m/z 100-1000. The majority of the assigned molecular formulas have unsaturated structures with CHO and CHNO elemental compositions. WSOC have an average O/C of ~0.45, relatively low compared to O/C of other aged aerosol, which might be the result of evaporation and fragmentation during long-range transport. The increase in aerosol loading during 9/24 was linked to biomass burning emissions from North America by FLEXPART and MODIS fire counts. This was confirmed with WSOC biomass burning markers and with the morphology and mixing state of particles as determined by SEM. The presence of markers characteristic of aqueous-phase reactions of biomass burning phenolic species suggests that the aerosol collected at Pico had undergone cloud processing. The air masses on 9/25 were more aged (~15 days) and influenced by marine emissions, as indicated by organosulphates and species characteristic for marine aerosol (e.g. fatty acids). The change in air masses for the two samples was corroborated by the changes in ozone, ethane, propane, morphology of particles, as well as by FLEXPART. In this presentation we will presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at the PMO.
Ključne besede: Atmospheric aerosol, Free troposphere, Mass spectrometry, Pico mountain observatory
Objavljeno v RUNG: 26.05.2021; Ogledov: 2813; Prenosov: 0
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3.
Characterization of ambient aerosols in Mexico City during the MCMA-2003 campaign with aerosol mass spectrometry : results from the CENICA Supersite
Dara Salcedo, T. B. Onasch, Katja Džepina, M. R. Canagaratna, Qi Zhang, J. A. Huffman, P. F. DeCarlo, J. Jayne, P. Mortimer, D. Worsnop, 2006, izvirni znanstveni članek

Opis: An Aerodyne Aerosol Mass Spectrometer (AMS) was deployed at the CENICA Supersite, during the Mexico City Metropolitan Area field study (MCMA-2003) from 31 March-4 May 2003 to investigate particle concentrations, sources, and processes. The AMS provides real time information on mass concentration and composition of the non-refractory species in particulate matter less than 1 mu m (NR-PM1) with high time and size-resolution. In order to account for the refractory material in the aerosol, we also present estimates of Black Carbon (BC) using an aethalometer and an estimate of the aerosol soil component obtained from Proton-Induced X-ray Emission Spectrometry (PIXE) analysis of impactor substrates. Comparisons of AMS + BC + soil mass concentration with other collocated particle instruments (a LASAIR Optical Particle Counter, a PM2.5 Tapered Element Oscillating Microbalance (TEOM), and a PM2.5 DustTrak Aerosol Monitor) show that the AMS + BC + soil mass concentration is consistent with the total PM2.5 mass concentration during MCMA-2003 within the combined uncertainties. In Mexico City, the organic fraction of the estimated PM2.5 at CENICA represents, on average, 54.6% (standard deviation sigma=10%) of the mass, with the rest consisting of inorganic compounds ( mainly ammonium nitrate and sulfate/ammonium salts), BC, and soil. Inorganic compounds represent 27.5% of PM2.5 (sigma=10%); BC mass concentration is about 11% (sigma=4%); while soil represents about 6.9% (sigma=4%). Size distributions are presented for the AMS species; they show an accumulation mode that contains mainly oxygenated organic and secondary inorganic compounds. The organic size distributions also contain a small organic particle mode that is likely indicative of fresh traffic emissions; small particle modes exist for the inorganic species as well. Evidence suggests that the organic and inorganic species are not always internally mixed, especially in the small modes. The aerosol seems to be neutralized most of the time; however, there were some periods when there was not enough ammonium to completely neutralize the nitrate, chloride and sulfate present. The diurnal cycle and size distributions of nitrate suggest local photochemical production. On the other hand, sulfate appears to be produced on a regional scale. There are indications of new particle formation and growth events when concentrations of SO2 were high. Although the sources of chloride are not clear, this species seems to condense as ammonium chloride early in the morning and to evaporate as the temperature increases and RH decreases. The total and speciated mass concentrations and diurnal cycles measured during MCMA-2003 are similar to measurements during a previous field campaign at a nearby location.
Ključne besede: aerosol mass-spectrometer, atmospheric aerosol, atmospheric chemistry, atmospheric physics
Objavljeno v RUNG: 12.04.2021; Ogledov: 2285; Prenosov: 0
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4.
Sources and transformations of particle-bound polycyclic aromatic hydrocarbons in Mexico City
L. C. Marr, Katja Džepina, Jose L. Jimenez, F. Reisen, H. L. Bethel, Janet Arey, J. S. Gaffney, N. A. Marley, Luisa T. Molina, Mario J. Molina, 2006, izvirni znanstveni članek

Opis: Understanding sources, concentrations, and transformations of polycyclic aromatic hydrocarbons (PAHs) in the atmosphere is important because of their potent mutagenicity and carcinogenicity. The measurement of particle-bound PAHs by three different methods during the Mexico City Metropolitan Area field campaign in April 2003 presents a unique opportunity for characterization of these compounds and intercomparison of the methods. The three methods are ( 1) collection and analysis of bulk samples for time-integrated gas- and particle-phase speciation by gas chromatography/ mass spectrometry; ( 2) aerosol photoionization for fast detection of PAHs on particles' surfaces; and ( 3) aerosol mass spectrometry for fast analysis of size and chemical composition. This research represents the first time aerosol mass spectrometry has been used to measure ambient PAH concentrations and the first time that fast, real-time methods have been used to quantify PAHs alongside traditional filter-based measurements in an extended field campaign. Speciated PAH measurements suggest that motor vehicles and garbage and wood burning are important sources in Mexico City. The diurnal concentration patterns captured by aerosol photoionization and aerosol mass spectrometry are generally consistent. Ambient concentrations of particle-phase PAHs typically peak at similar to 110 ng m(-3) during the morning rush hour and rapidly decay due to changes in source activity patterns and dilution as the boundary layer rises, although surface-bound PAH concentrations decay faster. The more rapid decrease in surface versus bulk PAH concentrations during the late morning suggests that freshly emitted combustion-related particles are quickly coated by secondary aerosol material in Mexico City's atmosphere and may also be transformed by heterogeneous reactions.
Ključne besede: aerosol mass-spectrometer, aerodynamic diameter measurements, oxygenated organic aerosols, relative rate constants
Objavljeno v RUNG: 12.04.2021; Ogledov: 2327; Prenosov: 0
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5.
Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes
Q. Zhang, Jose L. Jimenez, M. R. Canagaratna, J. David Allan, H. Coe, I. M. Ulbrich, M. R. Alfarra, A. Takami, A. M. Middlebrook, Katja Džepina, 2007, izvirni znanstveni članek

Opis: Organic aerosol (OA) data acquired by the Aerosol Mass Spectrometer (AMS) in 37 field campaigns were deconvolved into hydrocarbon-like OA (HOA) and several types of oxygenated OA (OOA) components. HOA has been linked to primary combustion emissions (mainly from fossil fuel) and other primary sources such as meat cooking. OOA is ubiquitous in various atmospheric environments, on average accounting for 64%, 83% and 95% of the total OA in urban, urban downwind, and rural/remote sites, respectively. A case study analysis of a rural site shows that the OOA concentration is much greater than the advected HOA, indicating that HOA oxidation is not an important source of OOA, and that OOA increases are mainly due to SOA. Most global models lack an explicit representation of SOA which may lead to significant biases in the magnitude, spatial and temporal distributions of OA, and in aerosol hygroscopic properties.
Ključne besede: atmospheric aerosol, secondary organic aerosols, primary organic aerosols, aerodyne aerosol mass spectrometer
Objavljeno v RUNG: 11.04.2021; Ogledov: 2171; Prenosov: 0
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6.
Evolution of organic aerosols in the atmosphere
Jose L. Jimenez, M. R. Canagaratna, N. M. Donahue, A. S. H. Prevot, Q. Zhang, J. H. Kroll, P. F. DeCarlo, J. David Allan, H. Coe, Katja Džepina, 2009, izvirni znanstveni članek

Opis: Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework describing the atmospheric evolution of OA that is constrained by high–time-resolution measurements of its composition, volatility, and oxidation state. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.
Ključne besede: secondary organic aerosol, source apportionment, aerodyne aerosol mass spectrometer, global field measurements, laboratory experiments
Objavljeno v RUNG: 11.04.2021; Ogledov: 2320; Prenosov: 0
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