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Optical properties of near-surface urban aerosols and their chemical tracing in a Mediterranean city (Athens)
Dimitris Katsanos, Aikaterini Bougiatioti, Eleni Liakakou, Dimitris G. Kaskaoutis, Iasonas Stavroulas, D. Paraskevopoulou, Maria Lianou, Basil E. Psiloglou, Evangelos Gerasopoulos, Christodoulos Pilinis, 2019, original scientific article

Abstract: One-year measurements (October 2016–September 2017) of aerosol optical properties in the Athens urban environment were analyzed; for closure purposes, the results were supported by data of chemical composition of the non-refractory submicron aerosol fraction acquired with an Aerosol Chemical Speciation Monitor (ACSM). Both the spectral scattering (bsca) and absorption (babs) coefficients exhibit a pronounced annual variability with higher values (63.6 Mm–1 at 550 nm and 41.0 Mm–1 at 520 nm, respectively) in winter, due to domestic heating releasing increased carbonaceous emissions and the shallow mixing layer trapping aerosols near the surface. Much lower values (33.5 Mm–1 and 22.9 Mm–1 for bsca and babs, respectively) are found during summer, indicating rather aged aerosols from regional sources. The estimations of the dry spectral single scattering albedo (SSA), scattering (SAE) and absorption (AAE) Ångström exponents focus on the seasonality of the urban aerosols. The high SAE (~2.0) and low SSA (0.62 ± 0.11) values throughout the year indicate the dominance of fine-absorbing aerosols from fossil-fuel combustion, while the high AAE (~1.5) in winter suggests enhanced presence of biomass-burning aerosols. Pronounced morning and late evening/night peaks are found in both bsca and babs during winter, coinciding with the morning traffic rush hour and increased residential wood burning in the evening, while in the other seasons, the diurnal patterns flatten out. The wind speed strongly affects the aerosol loading and properties in winter, since for winds below 3 m s–1, a high increase in bsca and babs is observed, consistent with low dilution processes and hazy/smoggy conditions. Our closure experiments indicate a good agreement (R2 = 0.91, slope = 1.08) between the reconstructed and measured bsca values and reveal that organic matter contributes about half of the sub-micron mass in winter, followed by sulfate (~40%) and nitrate (10%, only in winter) aerosols.
Keywords: urban aerosols, light scattering, absorption, chemical species, wood burning, Athens
Published in RUNG: 10.05.2024; Views: 200; Downloads: 2
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Assessment of the COVID-19 lockdown effects on spectral aerosol scattering and absorption properties in Athens, Greece
Dimitris G. Kaskaoutis, Georgios Grivas, Eleni Liakakou, Nikos Kalivitis, Giorgos Kouvarakis, Iasonas Stavroulas, Panayiotis Kalkavouras, Pavlos Zarmpas, Umesh Chandra Dumka, Evangelos Gerasopoulos, Nikolaos Mihalopoulos, 2021, original scientific article

Abstract: COVID-19 is evolving into one of the worst pandemics in recent history, claiming a death toll of over 1.5 million as of December 2020. In an attempt to limit the expansion of the pandemic in its initial phase, nearly all countries imposed restriction measures, which resulted in an unprecedented reduction of air pollution. This study aims to assess the impact of the lockdown effects due to COVID-19 on in situ measured aerosol properties, namely spectral-scattering (bsca) and absorption (babs) coefficients, black carbon (BC) concentrations, single-scattering albedo (SSA), scattering and absorption Ångström exponents (SAE, AAE) in Athens, Greece. Moreover, a comparison is performed with the regional background site of Finokalia, Crete, for a better assessment of the urban impact on observed differences. The study examines pre-lockdown (1–22 March 2020), lockdown (23 March–3 May 2020) and post-lockdown (4–31 May 2020) periods, while the aerosol properties are also compared with a 3–4 year preceding period (2016/2017–2019). Comparison of meteorological parameters in Athens, between the lockdown period and respective days in previous years, showed only marginal variation, which is not deemed sufficient in order to justify the notable changes in aerosol concentrations and optical properties. The largest reduction during the lockdown period was observed for babs compared to the pre-lockdown (−39%) and to the same period in previous years (−36%). This was intensified during the morning traffic hours (−60%), reflecting the large decrease in vehicular emissions. Furthermore, AAE increased during the lockdown period due to reduced emissions from fossil-fuel combustion, while a smaller (−21%) decrease was observed for bsca along with slight increases (6%) in SAE and SSA values, indicating that scattering aerosol properties were less affected by the decrease in vehicular emissions, as they are more dependent on regional sources and atmospheric processing. Nighttime BC emissions related to residential wood-burning were slightly increased during the lockdown period, with respect to previous-year means. On the contrary, aerosol and pollution changes during the lockdown period at Finokalia were low and highly sensitive to natural sources and processes.
Keywords: COVID-19, traffic, aerosol scattering, absorption, SSA, Greece
Published in RUNG: 10.05.2024; Views: 145; Downloads: 3
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Secondary organic aerosol formation from semi- and intermediate-volatility organic compounds and glyoxal : relevance of O/C as a tracer for aqueous multiphase chemistry
Eleanor M. Waxman, Katja Džepina, Barbara Ervens, Julia Lee-Taylor, Bernard Aumont, Jose L. Jimenez, Sasha Madronich, Rainer Volkamer, 2013, original scientific article

Abstract: The role of aqueous multiphase chemistry in the formation of secondary organic aerosol (SOA) remains difficult to quantify. We investigate it here by testing the rapid formation of moderate oxygen-to-carbon (O/C) SOA during a case study in Mexico City. A novel laboratory-based glyoxal-SOA mechanism is applied to the field data, and explains why less gas-phase glyoxal mass is observed than predicted. Furthermore, we compare an explicit gas-phase chemical mechanism for SOA formation from semi- and intermediate-volatility organic compounds (S/IVOCs) with empirical parameterizations of S/IVOC aging. The mechanism representing our current understanding of chemical kinetics of S/IVOC oxidation combined with traditional SOA sources and mixing of background SOA underestimates the observed O/C by a factor of two at noon. Inclusion of glyoxal-SOA with O/C of 1.5 brings O/C predictions within measurement uncertainty, suggesting that field observations can be reconciled on reasonable time scales using laboratory-based empirical relationships for aqueous chemistry.
Keywords: secondary organic aerosol, glyoxal, aqueous multiphase chemistry, oxygen-to-carbon ratio, single scattering albedo
Published in RUNG: 11.04.2021; Views: 2215; Downloads: 0
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Morphology and mixing state of aged soot particles at a remote marine free troposphere site : implications for optical properties
Swarup China, Barbara Scarnato, Robert C. Owen, Bo Zhang, MarianT. Ampadu, Sumit Kumar, Katja Džepina, Michael P. Dziobak, Paulo Fialho, Judith A. Perlinger, 2015, original scientific article

Abstract: The radiative properties of soot particles depend on their morphology and mixing state, but their evolution during transport is still elusive. Here we report observations from an electron microscopy analysis of individual particles transported in the free troposphere over long distances to the remote Pico Mountain Observatory in the Azores in the North Atlantic. Approximately 70% of the soot particles were highly compact and of those 26% were thinly coated. Discrete dipole approximation simulations indicate that this compaction results in an increase in soot single scattering albedo by a factor of <= 2.17. The top of the atmosphere direct radiative forcing is typically smaller for highly compact than mass-equivalent lacy soot. The forcing estimated using Mie theory is within 12% of the forcing estimated using the discrete dipole approximation for a high surface albedo, implying that Mie calculations may provide a reasonable approximation for compact soot above remote marine clouds.
Keywords: atmospheric aerosol, soot, long-range transport, free troposphere, single scattering albedo
Published in RUNG: 11.04.2021; Views: 2208; Downloads: 0
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Aircraft vertical profiles during summertime regional and Saharan dust scenarios over the north-western Mediterranean basin: aerosol optical and physical properties
Jesús Yus-Díez, Marina Ealo, Marco Pandolfi, Noemi Perez, Gloria Titos, Griša Močnik, Xavier Querol, A. Alastuey, 2021, original scientific article

Abstract: Accurate measurements of the horizontal and vertical distribution of atmospheric aerosol particle optical properties are key for a better understanding of their impact on the climate. Here we present the results of a measurement campaign based on instrumented flights over north-eastern Spain. We measured vertical profiles of size-segregated atmospheric particulate matter (PM) mass concentrations and multi-wavelength scattering and absorption coefficients in the western Mediterranean basin (WMB). The campaign took place during typical summer conditions, characterized by the development of a vertical multi-layer structure, under both summer regional pollution episodes (REGs) and Saharan dust events (SDEs). REG patterns in the region form under high insolation and scarce precipitation in summer, favouring layering of highly aged fine-PM strata in the lower few kma.s.l. The REG scenario prevailed during the entire measurement campaign. Additionally, African dust outbreaks and plumes from northern African wildfires influenced the study area. The vertical profiles of climate-relevant intensive optical parameters such as single-scattering albedo (SSA); the asymmetry parameter (g); scattering, absorption and SSA Ångström exponents (SAE, AAE and SSAAE); and PM mass scattering and absorption cross sections (MSC and MAC) were derived from the measurements. Moreover, we compared the aircraft measurements with those performed at two GAW–ACTRIS (Global Atmosphere Watch–Aerosol, Clouds and Trace Gases) surface measurement stations located in north-eastern Spain, namely Montseny (MSY; regional background) and Montsec d'Ares (MSA; remote site). Airborne in situ measurements and ceilometer ground-based remote measurements identified aerosol air masses at altitudes up to more than 3.5 kma.s.l. The vertical profiles of the optical properties markedly changed according to the prevailing atmospheric scenarios. During SDE the SAE was low along the profiles, reaching values < 1.0 in the dust layers. Correspondingly, SSAAE was negative, and AAE reached values up to 2.0–2.5, as a consequence of the UV absorption increased by the presence of the coarse dust particles. During REG, the SAE increased to > 2.0, and the asymmetry parameter g was rather low (0.5–0.6) due to the prevalence of fine PM, which was characterized by an AAE close to 1.0, suggesting a fossil fuel combustion origin. During REG, some of the layers featured larger AAE (> 1.5), relatively low SSA at 525 nm (< 0.85) and high MSC (> 9 m2 g−1) and were associated with the influence of PM from wildfires. Overall, the SSA and MSC near the ground ranged around 0.85 and 3 m2 g−1, respectively, and increased at higher altitudes, reaching values above 0.95 and up to 9 m2 g−1. The PM, MSC and MAC were on average larger during REG compared to SDE due to the larger scattering and absorption efficiency of fine PM compared with dust. The SSA and MSC had quite similar vertical profiles and often both increased with height indicating the progressive shift toward PM with a larger scattering efficiency with altitude. This study contributes to our understanding of regional-aerosol vertical distribution and optical properties in the WMB, and the results will be useful for improving future climate projections and remote sensing or satellite retrieval algorithms.
Keywords: aerosol, climate change, Saharan dust, black carbon, aerosol absorption, aerosol scattering
Published in RUNG: 14.01.2021; Views: 2536; Downloads: 0
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Amorphous nanocomposite of polycarbosilanes and aluminum oxide
Andraž Mavrič, 2018, doctoral dissertation

Abstract: This work presents a paradigm for high temperature stabilization of bulk amorphous aluminium oxide. The thermodynamic stabilization is achieved by preparing a nanocomposite, where polymethylsilane dendritic molecules are dispersed in an aluminium hydroxide gel. Upon heat-treatment the gel transforms to the amorphous aluminium oxide that is stable up to 900°C. The dispersion of the macromolecules and their covalent bonding to the alumina matrix induce homogeneously distributed strain fields that keep the alumina amorphous. The first part of the thesis focuses on the synthesis, characterization and solubility properties of the dendritic polymethylsilane. The polymethylsilane is synthetized by electrochemical polymerization from trichloromethylsilane monomer. The polymerization mechanism, involving a single polymerization pathway, is identified. The polymer growth proceeds through reduction of the monomers to the silyl anions and their addition to the growing polymer. The solubility of three chemically related but topologically different polysilanes (linear, dendritic and network) were studied by dynamic light scattering. At room temperature the agglomerates in a range from 500 to 1300 nm are present. They undergo de-agglomeration at slightly elevated temperatures of around 40°C. The de-agglomeration results in formation of stable solutions, where a hydrodynamic diameter of the individual polymer molecules was measured to be in a range from 20 to 40 nm. The obtained diameters of two dendritic polymethylsilane macromolecules, synthesized under different electrolysis conditions, are much larger than the theoretical size estimated for an ideal dendrimer. We determined by 29Si NMR that the reason for this is in a large number of branching irregularities (defects) contained in the molecular structure. Combining the experimental values obtained by DLS and density measurements with a structural model that considers the branching irregularities, it is shown that the inclusion of the defects allows the dendritic polymer to exceed the sterical limitations and form the hyperbranched dendritic structure. The final size depends on a relative amount of the branching defects. In the second part, the synthetized polymethylsilane molecules were successfully used for the nanocomposite formation. The aluminium hydroxide gel with the dispersed polymethylsilane molecules was prepared as a precursor. Upon heat-treatment it gives the amorphous aluminium oxide stable up to 900°C. The dispersed macromolecules induce homogeneously distributed strain fields that keep the aluminium oxide amorphous during the thermal treatment the dispersed macromolecules covalently bind to the matrix, inducing the interface strain. The amorphous state was confirmed by the presence of penta-coordinated aluminium detected by 27Al NMR and a low bandgap measured by UV-vis absorption spectroscopy.
Keywords: amorphous aluminium oxide, polymethylsilane, nanocomposite, electropolymerization, solubility, agglomeration, de-agglomeration, dendrimer, hyperbranched dendritic structure, dynamic light scattering, thermal analysis, transmission electron microscopy, scanning electron microscopy, X-ray diffraction, infrared spectroscopy, UV-Vis spectroscopy
Published in RUNG: 19.07.2018; Views: 6298; Downloads: 212
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Polymer Nanoparticle Sizes from Dynamic Light Scattering and Size Exclusion Chromatography: The Case Study of Polysilanes.
Artem Badasyan, Andraž Mavrič, Irena Kralj Cigić, Tim Bencik, Matjaž Valant, 2018, original scientific article

Abstract: Dynamic Light Scattering (DLS) and Size Exclusion Chromatography (SEC) are among the most popular methods for determining polymer sizes in solution. Taking dendritic and network polysilanes as a group of least soluble polymer substances, we critically compare and discuss the difference between nanoparticle sizes, obtained by DLS and SEC. Polymer nanoparticles are typically in poor solution conditions below the theta point and are in globular conformation therefore. Determination of particle sizes in presence of attractive interactions is not a trivial task. The only possibility to measure aggregation-free, a true molecular size of polymer nanoparticles in such regime of solution, is to operate with the dilute solution of globules (below theta point and above the miscibility line). Basing on results of our polysilane measurements, we come to a conclusion that DLS provides more reliable results than SEC for the dilute solution of globules. General implications for the size measurements of polymer nanoparticles in solutions are discussed.
Keywords: Polymer Nanoparticle, Dynamic Light Scattering, Size Exclusion Chromatography, Polysilanes
Published in RUNG: 16.05.2018; Views: 4397; Downloads: 16
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