51. Secondary organic aerosol formation from semi- and intermediate-volatility organic compounds and glyoxal : relevance of O/C as a tracer for aqueous multiphase chemistryEleanor M. Waxman, Katja Džepina, Barbara Ervens, Julia Lee-Taylor, Bernard Aumont, Jose L. Jimenez, Sasha Madronich, Rainer Volkamer, 2013, izvirni znanstveni članek Opis: 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.
Ključne besede: secondary organic aerosol, glyoxal, aqueous multiphase chemistry, oxygen-to-carbon ratio, single scattering albedo
Objavljeno v RUNG: 11.04.2021; Ogledov: 2146; Prenosov: 0
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52. Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory : a case study with a long-range transported biomass burning plumeKatja Džepina, Claudio Mazzoleni, Paulo Fialho, Swarup China, Bo Zhang, R. Chris Owen, D. Helmig, J. Hueber, Sumit Kumar, J. A. Perlinger, 2015, izvirni znanstveni članek Opis: Free tropospheric aerosol was sampled at the
Pico Mountain Observatory located at 2225 m above mean
sea level on Pico Island of the Azores archipelago in the
North Atlantic. The observatory is located ∼ 3900 km east
and downwind of North America, which enables studies
of free tropospheric air transported over long distances.
Aerosol samples collected on filters from June to October
2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 µg m−3
. On average, organic aerosol components represent the largest mass fraction of the total measured aerosol (60 ± 51 %), followed by
sulfate (23 ± 28 %), nitrate (13 ± 10 %), chloride (2 ± 3 %),
and elemental carbon (2 ± 2 %). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and
9/25) collected consecutively during a pollution event were
analyzed using ultrahigh-resolution electrospray ionization
Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned
to each of the mass spectra in the range of m/z 100–1000.
The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled
air masses were very aged (average plume age > 12 days).
These aged aerosol WSOM compounds had an average O /C
ratio of ∼ 0.45, which is relatively low compared to O /C
ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to
biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM
and with the morphology and mixing state of particles as
determined by scanning electron microscopy. The presence
of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were
more aged and influenced by marine emissions, as indicated
by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for
the two samples was corroborated by the changes in ethane,
propane, and ozone, morphology of particles, as well as by
the FLEXPART retroplume simulations. This paper presents
the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere
remote location and provides evidence of low oxygenation
after long-range transport. We hypothesize this is a result of
the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a
combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and
fragmentation (e.g., photolysis) of components.
Ključne besede: organic aerosol, ultrahigh-resolution FT-ICR MS, electron microscopy, remote marine atmosphere, Pico Mountain Observatory
Objavljeno v RUNG: 11.04.2021; Ogledov: 2369; Prenosov: 0
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53. Morphology and mixing state of aged soot particles at a remote marine free troposphere site : implications for optical propertiesSwarup China, Barbara Scarnato, Robert C. Owen, Bo Zhang, MarianT. Ampadu, Sumit Kumar, Katja Džepina, Michael P. Dziobak, Paulo Fialho, Judith A. Perlinger, 2015, izvirni znanstveni članek Opis: 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.
Ključne besede: atmospheric aerosol, soot, long-range transport, free troposphere, single scattering albedo
Objavljeno v RUNG: 11.04.2021; Ogledov: 2132; Prenosov: 0
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54. Elucidating local pollution and site representativeness at the Jungfraujoch, Switzerland through parallel aerosol measurements at an adjacent mountain ridgeNicolas Bukowiecki, Benjamin Brem, Günther Wehrle, Griša Močnik, Stéphane Affolter, Markus Christian Leuenberger, Martine Collaud Coen, Maxime Hervo, Urs Baltensperger, Martin Gysel, 2021, izvirni znanstveni članek Opis: Many long-term air pollution and climate monitoring stations face the issue of increasing anthropogenic activities in their vicinity. Furthermore, the spatial representativeness of the sites is often not entirely understood especially in mountainous terrain with complex topographic features. This study presents a 5-year comparison of parallel aerosol measurements (total particle number concentration and equivalent black carbon mass concentration) at the Jungfraujoch in the Swiss Alps (JFJ, 3580 m a.s.l.), and an adjacent mountain ridge, the Jungfrau East Ridge (JER, 3705 m a.s.l.), in 1000 m air-line distance to the main site. The parallel aerosol measurements reveal characteristic differences in the diurnal variations between the two sites under certain specific meteorological conditions. Our analysis estimates that on 20-40% of the days local activities at the Jungfraujoch have a clear influence on the measured time series of the total aerosol number concentration and the equivalent black carbon mass concentration. This influence is mainly seen in form of strong isolated spikes rather than by an increase in the on-site background concentration. They can thus be flagged during the data quality assurance process and filtered from those measurement parameters available at high time resolution. Removing the spikes from the original time series results in daily mean values for the total aerosol number concentration and equivalent black carbon mass concentration that are 5-10 % lower compared to the original signals. During nighttime with hardly any local pollution sources that cause spikes this percentage decreases towards 0%. The signal baselines at the Jungfraujoch and Jungfrau East Ridge correlate well during more than 50% of the days.
Ključne besede: aerosol long-term monitoring, equivalent black carbon, aerosol number concentration, spatial variation
Objavljeno v RUNG: 15.03.2021; Ogledov: 1978; Prenosov: 71
 Povezava na celotno besedilo
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55. Aircraft vertical profiles during summertime regional and Saharan dust scenarios over the north-western Mediterranean basin: aerosol optical and physical propertiesJesús Yus-Díez, Marina Ealo, Marco Pandolfi, Noemi Perez, Gloria Titos, Griša Močnik, Xavier Querol, A. Alastuey, 2021, izvirni znanstveni članek Opis: 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.
Ključne besede: aerosol, climate change, Saharan dust, black carbon, aerosol absorption, aerosol scattering
Objavljeno v RUNG: 14.01.2021; Ogledov: 2456; Prenosov: 0
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57. A single-beam photothermal interferometer for in situ measurements of aerosol light absorptionBradley Visser, Jannis Röhrbein, Peter Steigmeier, Luka Drinovec, Griša Močnik, Ernest Weingartner, 2020, izvirni znanstveni članek Opis: We have developed a novel single-beam photothermal interferometer and present here its application for the measurement of aerosol light absorption. The use of only a single laser beam allows for a compact optical set-up and significantly easier alignment compared to standard dual-beam photothermal interferometers, making it ideal for field measurements. Due to a unique configuration of the reference interferometer arm, light absorption by aerosols can be determined directly – even in the presence of light-absorbing gases. The instrument can be calibrated directly with light-absorbing gases, such as NO2, and can be used to calibrate other light absorption instruments. The detection limits (1σ) for absorption for 10 and 60 s averaging times were determined to be 14.6 and 7.4 Mm−1, respectively, which for a mass absorption cross section of 10 m2 g−1 leads to equivalent black carbon concentration detection limits of 1460 and 740 ng m−3, respectively. The detection limit could be reduced further by improvements to the isolation of the instrument and the signal detection and processing schemes employed.
Ključne besede: aerosol, aerosol absorption, black carbon, photo-thermal interferometer, climate change
Objavljeno v RUNG: 29.12.2020; Ogledov: 2650; Prenosov: 74
 Celotno besedilo (2,44 MB) |
58. Photo-thermal interferometerLuka Drinovec, Griša Močnik, 2020, patent Opis: A photo-thermal interferometer for measuring the light absorption of an aerosol or gas comprises a first laser source emitting a laser beam and a beam splitter adapted to divide the laser beam into a probe beam and a reference beam. The interferometer further comprises first optical elements which are adapted to direct the probe beam such that it passes through the aerosol and interferes with the reference beam thereafter thereby causing interference patterns. A detector detects the interference patterns. The interferometer further comprises a second laser source configured to emit a pump beam for transferring energy to the aerosol. Second optical elements are adapted to direct the pump beam such that it overlaps with the probe beam at least partially in the aerosol or gas. At least one of the second optical elements modifying the pump beam is an axicon.
Ključne besede: aerosol, absorption, black carbon
Objavljeno v RUNG: 15.09.2020; Ogledov: 2968; Prenosov: 0
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59. Air quality and climate change - how smart can the cities be?Griša Močnik, Matevž Lenarčič, 2020, vabljeno predavanje na konferenci brez natisa Opis: What starts as an air quality problem in urban areas, ends up as a climate change problem globally. Emissions from cities and the power generating facilities powering the cities have local, regional and global effects. We show examples spanning these scales with very practical advice on how to start abatement locally.
Ključne besede: air quality, climate change, black carbon, aerosol, co2, smart city
Objavljeno v RUNG: 11.09.2020; Ogledov: 3271; Prenosov: 0
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60. A new optical-based technique for real-time measurements of mineral dust concentration in PM10 using a virtual impactorLuka Drinovec, Jean Sciare, Iasonas Stavroulas, Spiros Bezantakos, Michael Pikridas, FLORIN UNGA, Chrysanthos Savvides, Bojana Višnjić, Maja Remškar, Griša Močnik, 2020, izvirni znanstveni članek Opis: Atmospheric mineral dust influences Earth’s radiative
budget, cloud formation, and lifetime; has adverse
health effects; and affects air quality through the increase of
regulatory PM10 concentrations, making its real-time quantification
in the atmosphere of strategic importance. Only
few near-real-time techniques can discriminate dust aerosol
in PM10 samples and they are based on the dust chemical
composition. The online determination of mineral dust using
aerosol absorption photometers offers an interesting and
competitive alternative but remains a difficult task to achieve.
This is particularly challenging when dust is mixed with
black carbon, which features a much higher mass absorption
cross section. We build on previous work using filter photometers
and present here for the first time a highly timeresolved
online technique for quantification of mineral dust
concentration by coupling a high-flow virtual impactor (VI)
sampler that concentrates coarse particles with an aerosol absorption
photometer (Aethalometer, model AE33). The absorption
of concentrated dust particles is obtained by subtracting
the absorption of the submicron (PM1) aerosol fraction
from the absorption of the virtual impactor sample (VIPM1
method). This real-time method for detecting desert
dust was tested in the field for a period of 2 months (April and
May 2016) at a regional background site of Cyprus, in the
Eastern Mediterranean. Several intense desert mineral dust
events were observed during the field campaign with dust
concentration in PM10 up to 45 μgm
Ključne besede: aerosol absorption, mineral dust, on-line detection, air quality
Objavljeno v RUNG: 20.07.2020; Ogledov: 2794; Prenosov: 0
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