| 1. |
- Cantos, Irene Pardo, et al.
(author)
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Determination and analysis of time series of CFC-11 (CCl3F) from FTIR solar spectra, in situ observations, and model data in the past 20 years above Jungfraujoch (46 degrees N), Lauder (45 degrees S), and Cape Grim (40 degrees S) stations
- 2022
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In: Environmental Science: Atmospheres. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:6, s. 1487-1501
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Journal article (peer-reviewed)abstract
- The atmospheric concentration of CFC-11 (CCl3F) has declined in response to the phase-out of its production by the Montreal Protocol. Nevertheless, this atmospheric concentration decline suffered a slow-down around 2012 due to emissions from non-reported production. Since CFC-11 is one of the most important ozone-depleting chlorofluorocarbons (CFCs), its continuous monitoring is essential. We present the CFC-11 total column time series (2000-2020) retrieved in a consistent way from ground-based high-resolution solar absorption Fourier transform infrared (FTIR) spectra. These observations were recorded at two remote stations of the Network for the Detection of Atmospheric Composition Change (NDACC): the Jungfraujoch station (Northern Hemisphere) and the Lauder station (Southern Hemisphere). These time series are new. They were produced using improved line parameters and merged considering the instrument changes and setup modifications. Afterwards, they were compared with Cape Grim station in situ surface observations conducted within the Advanced Global Atmospheric Gases Experiment (AGAGE) network and with total column datasets calculated by the TOMCAT/SLIMCAT 3-D chemical transport model. Trend analyses were performed, using an advanced statistical tool, in order to identify the timing and magnitude of the trend change in both hemispheres. The observations are consistent with the model results and confirm the slowdown in the CFC-11 atmospheric concentration decay, since approximate to 2011 in the Northern Hemisphere, and since approximate to 2014 in the Southern Hemisphere.
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| 2. |
- Chen, Dean, et al.
(author)
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A modelling study of OH, NO3 and H2SO4 in 2007- 2018 at SMEAR II, Finland : Analysis of long-term trends
- 2021
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In: Environmental Science: Atmospheres. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 1:6, s. 449-472
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Journal article (peer-reviewed)abstract
- Major atmospheric oxidants (OH,O3 and NO3) dominate the atmospheric oxidation capacity, while H2SO4 is considered as a main driver for new particle formation. Although numerous studies have investigated the long-term trend of ozone in Europe, the trends of OH, NO3 and H2SO4 at specific sites are to a large extent unknown. The one-dimensional model SOSAA has been applied in several studies at the SMEAR II station and has been validated by measurements in several projects. Here, we applied the SOSAA model for the years 2007-2018 to simulate the atmospheric chemical components, especially the atmospheric oxidants OH and NO3, as well as H2SO4 at SMEAR II. The simulations were evaluated with observations from several shorter and longer campaigns at SMEAR II. Our results show that daily OH increased by 2.39% per year and NO3 decreased by 3.41% per year, with different trends of these oxidants during day and night. On the contrary, daytime sulfuric acid concentrations decreased by 2.78% per year, which correlated with the observed decreasing concentration of newly formed particles in the size range of 3- 25 nm with 1.4% per year at SMEAR II during the years 1997-2012. Additionally, we compared our simulated OH, NO3 and H2SO4 concentrations with proxies, which are commonly applied in case a limited number of parameters are measured and no detailed model simulations are available.
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| 3. |
- Gopakumar, Geethanjali, et al.
(author)
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The surface composition of amino acid - halide salt solutions is pH-dependent
- 2022
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In: Environmental Science: Atmospheres. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:3, s. 441-448
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Journal article (peer-reviewed)abstract
- In atmospheric aerosol particles, the chemical surface composition governs both heterogenous chemical reactions with gas-phase species and the ability to act as nuclei for cloud droplets. The pH in aerosol particles is expected to affect these properties, but it is very challenging to measure the pH in individual droplets, precluding the investigation of its influence on the particle's surface composition. In this work, we use photoelectron spectroscopy to explore how the surface composition of aqueous solutions containing inorganic salt and amino acids changes as a function of pH. We observe a change by a factor of 4-5 of the relative distribution of inorganic ions at the surface of a liquid water jet, as a function of solution pH and type of amino acid in the solution. The driving forces for the surface enhancement or depletion are ion pairing and the formation of charged layers close to the aqueous surface.
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| 4. |
- Hemming, Joanna M., et al.
(author)
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Changes to lung surfactant monolayers upon exposure to gas phase ozone observed using X-ray and neutron reflectivity
- 2022
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In: Environmental Science. - : Royal Society of Chemistry. - 2634-3606. ; 2:4, s. 753-760
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Journal article (peer-reviewed)abstract
- Exposure to the secondary pollutant ozone in ambient air is associated with adverse health effects when inhaled. In this work we use surface pressure measurements, combined with X-ray and neutron reflection, to observe changes in a layer of lung surfactant at the air water interface when exposed to gas phase ozone. The results demonstrate that the layer reacts with ozone changing its physical characteristics. A slight loss of material, a significant thinning of the layer and increased hydration of the surfactant material is observed. The results support the hypothesis that unsaturated lipids present in lung surfactant are still susceptible to rapid reaction with ozone and the reaction changes the properties of the interfacial layer.
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| 5. |
- Hjelm, Rikard, et al.
(author)
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Ultrafine particle emissions from dry clutches : number concentration, size distribution and chemical composition
- 2024
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In: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 4:1, s. 35-42
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Journal article (peer-reviewed)abstract
- Non-exhaust sources, such as brakes, tyres, roads, and clutches, emit a large portion of airborne particles in road transportation, from ultrafine to coarse sizes. While airborne wear particle emissions from brakes and road-tyre contacts have been studied extensively, emissions from clutches have been overlooked. A preliminary study using a novel test rig has indicated that dry clutches also emit airborne wear particles. This paper presents a multi-method for the assessment of ultrafine particles from dry clutches regarding the number concentration, size distribution and chemical composition. The results show that ultrafine particles are emitted both during run-in and at the steady state, featuring a bi-modal size distribution. Elementary analysis shows that the particles consist of several elements, predominately iron, silicon, and sulfur. It can be concluded from this study that ultrafine particles are always generated when the clutch is operated. Clutches in automobiles are shown to produce ultrafine particles, consisting of several metallic elements, which become airborne.
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| 6. |
- Koenig, Alkuin M., et al.
(author)
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Observed in-plume gaseous elemental mercury depletion suggests significant mercury scavenging by volcanic aerosols
- 2023
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In: Environmental Science: Atmospheres. - 2634-3606. ; 3:10, s. 1418-1438
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Journal article (peer-reviewed)abstract
- Terrestrial volcanism is known to emit mercury (Hg) into the atmosphere. However, despite many years of investigation, its net impact on the atmospheric Hg budget remains insufficiently constrained, in part because the transformations of Hg in volcanic plumes as they age and mix with background air are poorly understood. Here we report the observation of complete gaseous elemental mercury (GEM) depletion events in dilute and moderately aged (& SIM;3-7 hours) volcanic plumes from Piton de la Fournaise on Reunion Island. While it has been suggested that co-emitted bromine could, once photochemically activated, deplete GEM in a volcanic plume, we measured low bromine concentrations in both the gas- and particle-phase and observed complete GEM depletion even before sunrise, ruling out a leading role of bromine chemistry here. Instead, we hypothesize that the GEM depletions were mainly caused by gas-particle interactions with sulfate-rich volcanic particles (mostly of submicron size), abundantly present in the dilute plume. We consider heterogeneous GEM oxidation and GEM uptake by particles as plausible manifestations of such a process and derive empirical rate constants. By extrapolation, we estimate that volcanic aerosols may scavenge 210 Mg y(-1) (67-480 Mg y(-1)) of Hg from the atmosphere globally, acting effectively as atmospheric mercury sink. While this estimate is subject to large uncertainties, it highlights that Hg transformations in aging volcanic plumes must be better understood to determine the net impact of volcanism on the atmospheric Hg budget and Hg deposition pathways.
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| 7. |
- Kong, Xiangrui, et al.
(author)
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Surface solvation of Martian salt analogues at low relative humidities
- 2022
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In: Environmental Science: Atmospheres. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:2, s. 137-145
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Journal article (peer-reviewed)abstract
- Salt aerosols play important roles in many processes related to atmospheric chemistry and the climate systems on both Earth and Mars. Complicated and still poorly understood processes occur on the salt surfaces when interacting with water vapor. In this study, ambient pressure X-ray photoelectron spectroscopy (APXPS) is used to characterize the surface chemical environment of Martian salt analogues originating from saline lakes and playas, as well as their responses to varying relative humidities. Generally, APXPS shows similar ionic compositions to those observed by ion chromatography (IC). However, XPS is a surface-sensitive method while IC is bulk-sensitive and differences are observed for species that preferentially partition to the surface or the bulk. Element-selective surface enhancement of Cl− is observed, likely caused by the presence of SO42−. In addition, Mg2+ is concentrated on the surface while Na+ is relatively depleted in the surface layer. Hence, the cations (Na+ and Mg2+) and the anions (Cl− and SO42−) show competitive correlations. At elevated relative humidity (RH), no major spectral changes were observed in the XPS results, except for the growth of an oxygen component originating from condensed H2O. Near-edge X-ray absorption fine structure (NEXAFS) measurements show that the magnesium and sodium spectra are sensitive to the presence of water, and the results imply that the surface is fully solvated already at RH = 5%. The surface solvation is also fully reversible as the RH is reduced. No major differences are observed between sample types and sample locations, indicating that the salts originated from saline lakes commonly have solvated surfaces under the environmental conditions on Earth.
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| 8. |
- Kontkanen, Jenni, et al.
(author)
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What controls the observed size-dependency of the growth rates of sub-10 nm atmospheric particles?
- 2022
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In: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; :2, s. 449-468
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Journal article (peer-reviewed)abstract
- The formation and growth of atmospheric particles involving sulfuric acid and organic vapors is estimated to have significant climate effects. To accurately represent this process in large-scale models, the correct interpretation of the observations on particle growth, especially below 10 nm, is essential. Here, we disentangle the factors governing the growth of sub-10 nm particles in the presence of sulfuric acid and organic vapors, using molecular-resolution cluster population simulations and chamber experiments. We find that observed particle growth rates are determined by the combined effects of (1) the concentrations and evaporation rates of the condensing vapors, (2) particle population dynamics, and (3) stochastic fluctuations, characteristic to initial nucleation. This leads to a different size-dependency of growth rate in the presence of sulfuric acid and/or organic vapors at different concentrations. Specifically, the activation type behavior, resulting in growth rate increasing with the particle size, is observed only at certain vapor concentrations. In our model simulations, cluster-cluster collisions enhance growth rate at high vapor concentrations and their importance is dictated by the cluster evaporation rates, which demonstrates the need for accurate evaporation rate data. Finally, we show that at sizes below ∼2.5-3.5 nm, stochastic effects can importantly contribute to particle population growth. Overall, our results suggest that interpreting particle growth observations with approaches neglecting population dynamics and stochastics, such as with single particle growth models, can lead to the wrong conclusions on the properties of condensing vapors and particle growth mechanisms.
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| 9. |
- Ladd-Parada, Marjorie, et al.
(author)
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Using coherent X-rays to follow dynamics in amorphous ices
- 2022
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In: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:6, s. 1314-1323
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Journal article (peer-reviewed)abstract
- Amorphous solid water plays an important role in our overall understanding of water's phase diagram. X-ray scattering is an important tool for characterising the different states of water, and modern storage ring and XFEL facilities have opened up new pathways to simultaneously study structure and dynamics. Here, X-ray photon correlation spectroscopy (XPCS) was used to study the dynamics of high-density amorphous (HDA) ice upon heating. We follow the structural transition from HDA to low-density amorphous (LDA) ice, by using wide-angle X-ray scattering (WAXS), for different heating rates. We used a new type of sample preparation, which allowed us to study μm-sized ice layers rather than powdered bulk samples. The study focuses on the non-equilibrium dynamics during fast heating, spontaneous transformation and crystallization. Performing the XPCS study at ultra-small angle (USAXS) geometry allows us to characterize the transition dynamics at length scales ranging from 60 nm–800 nm. For the HDA-LDA transition we observe a clear separation in three dynamical regimes, which show different dynamical crossovers at different length scales. The crystallization from LDA, instead, is observed to appear homogenously throughout the studied length scales.
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| 10. |
- Patanen, Minna, et al.
(author)
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Surface composition of size-selected sea salt particles under the influence of organic acids studied in situ using synchrotron radiation X-ray photoelectron spectroscopy
- 2022
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In: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:5, s. 1032-1040
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Journal article (peer-reviewed)abstract
- Sea spray aerosols play a key role in the climate system by scattering solar radiation and by serving as cloud condensation nuclei. Despite their importance, the impact of sea spray aerosols on global climate remains highly uncertain. One of the key knowledge gaps in our understanding of sea spray aerosol is the chemical composition of the particle surface, important for various atmospheric chemical processes, as a function of size and bulk composition. Here, we have applied X-ray photoelectron spectroscopy (XPS) to determine the surface composition of both pure inorganic sea salt aerosols and sea salt aerosols spiked with an amino acid (phenylalanine) and a straight chain fatty acid (octanoic acid). Importantly, the use of a differential mobility analyser allowed size-selection of 150, 250 and 350 nm monodisperse aerosol particles for comparison to polydisperse aerosol particles. We observed enrichment of magnesium at the particle surfaces relative to chloride in all aerosols tested, across all particle sizes. Interestingly, the magnitude of this enrichment was dependent on the type of organic present in the solution as well as the particle size. Our results suggest that the observed enrichment in magnesium is an inorganic effect which can be either enhanced or diminished by the addition of organic substances.
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| 11. |
- Pereira Freitas, Gabriel, 1993-, et al.
(author)
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Emission of primary bioaerosol particles from Baltic seawater
- 2022
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In: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:5, s. 1170-1182
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Journal article (peer-reviewed)abstract
- Bioaerosols are particles of biological origin with various important atmospheric implications, for example, within cloud formation where bioaerosols can act as cloud condensation or ice nuclei. Their sources and properties, however, are poorly understood. We conducted a controlled sea spray experiment to determine the properties and emission of primary biological aerosol particles (PBAP) originating from Baltic seawater. Using a single-particle fluorescence and light-scattering instrument, the Multiparameter Bioaerosol Spectrometer (MBS), we differentiated PBAP within sea spray aerosol (SSA). Overall, approximately 1 in 104 particles larger than 0.8 μm in diameter were classified as PBAP. The optically-determined morphology of the nascent and fluorescent SSA particles showed a clear transition in symmetry and elongation most likely due to changes in the biogeochemical properties of the surface water. These shifts were also reflected in a clear change of the bacterial community composition of the aerosol and seawater as determined by 16S rRNA-gene analysis, which were significantly distinct from each other, suggesting a preferential emission of specific bacteria to the atmosphere. Our results demonstrate the capability of the MBS to identify and count PBAP within SSA on a single-particle basis and will help to better constrain the emission of marine PBAP and their dependence on the seawater's biogeochemical properties.
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| 12. |
- Prakash, Jai, et al.
(author)
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Characterization, sources, and atmospheric transformation of a few key short-lived climate pollutants (SLCPs) at a rural super-site in the Indo-Gangetic Plain (IGP) of India
- 2022
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In: Environmental Science: Atmospheres. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2, s. 517-538
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Journal article (peer-reviewed)abstract
- The Indo-Gangetic Plain (IGP) region of India faces some of the most severe air pollution problems on Earth that threaten human health, food security, ecosystems, environmental sustainability, and the climate. The aim of this study is to identify and characterize the sources of key short-lived climate pollutants (SLCPs) - black carbon (BC), brown carbon (BrC), and ozone (O3) - as well as other pollutants [carbon monoxide (CO) and nitrogen oxides NOX = NO and NO2], and interlinked atmospheric processes of their formation and transformation at our long-term air pollution monitoring station in a remote rural IGP site, the Indo-Gangetic Plains Centre for Air Research and Education (IGP-CARE). Because of its location, measurements acquired at IGP-CARE provide otherwise new information on the key SLCPs in the IGP region at a remote and rural location. The year-long measurement data at this remote site provided new insights into the variability of SLCP concentration and interlinked atmospheric processes that affect air quality in the rural IGP region. Thirteen episodic events (E1-E13) of elevated BC and BrC concentrations were identified, which can largely be attributed to the local biomass burning activities in the neighboring rural communities. It is suggested that high concentrations of BrC were mostly primary in nature and thought to be co-emitted with BC from biomass burning. Also, secondary pollutant tropospheric O3 showed elevated concentration. O3 peaks were mostly attributed to local ozone formation. Nevertheless, on several occasions, O3 emission was also attributed to regional urban areas. This study's most important finding is that BrC concentrations were relatively high throughout the year with very pronounced diurnal variation with distinct morning and evening peaks in general and a minimum at around noon time; this is hypothesized to be associated with daytime photochemical processes. Analyses using a conditional bivariate probability function (CBPF) and potential source contribution function (PSCF) suggest that regional sources likely affected the local concentrations of SLCPs. These results partly explain the high concentrations and spatial distributions of SLCPs at the local and regional scales at the IGP-CARE site in winter and autumn. In contrast, in the summer and monsoon seasons, strong convection likely favored the dilution of pollutants.
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| 13. |
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| 14. |
- Radoman, Nikola, et al.
(author)
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Probing the impact of a phytoplankton bloom on the chemistry of nascent sea spray aerosol using high-resolution mass spectrometry
- 2022
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In: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:5, s. 1152-1169
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Journal article (peer-reviewed)abstract
- Sea spray aerosol is the largest natural source of aerosol to Earth's atmosphere with significant impacts on climate. Despite this, estimates of the impact of sea spray aerosol on Earth's radiation budget are highly uncertain due to an overall lack of understanding of the physical and chemical factors controlling its composition. Critically, results from studies probing the importance of oceanic biological activity on the amount and type of organic matter present in nascent sea spray aerosol have been ambiguous. Some field studies have shown a relationship between the organic fraction of sea spray aerosol and oceanic primary productivity while others have reported no such relationships. Given this, we have probed the composition of seawater and nascent sea spray aerosol during a phytoplankton bloom in the North Atlantic using a novel liquid chromatography-mass spectrometry method. We observed that the composition of dissolved organic matter present in seawater changed as the phytoplankton bloom progressed over an 18 day period. Further, we observed changes to both the chemical composition of the organic matter present in seawater and the chemical composition of the organic matter present in the sea spray aerosol despite the organic matter mass fraction of the aerosol remaining unchanged. More specifically, we observed that the nascent sea spray aerosol became progressively more enriched in surface-active organic substances as the bloom progressed and that the sea spray aerosol had a distinct organic matter composition compared to the seawater. Thus, our work provides additional insight into the biological dependence of nascent sea spray aerosol composition.
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| 15. |
- Santos, Luis F.E.d., et al.
(author)
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Changes in CCN activity of ship exhaust particles induced by fuel sulfur content reduction and wet scrubbing
- 2022
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In: Environmental Science: Atmospheres. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 3:1, s. 182-195
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Journal article (peer-reviewed)abstract
- Maritime transport remains a large source of airborne pollutants, including exhaust particles that can act as cloud condensation nuclei (CCN). While primary diesel engine exhaust particles are generally considered hydrophobic, international regulations targeting a reduction of particulate emissions from ships may have secondary effects, and therefore influence how exhaust interacts within the atmosphere. The effect of international fuel sulfur content (FSC) regulations on the cloud forming abilities of exhaust particles was investigated using a marine test engine operating on compliant low FSC fuels, non-compliant high FSC distillate fuels and in conjunction with a marine wet scrubber (fresh- and seawater). Particle sizing and liquid droplet activation measurements reveal that compliance measures can have opposing effects on the CCN activity of exhaust particles. For a non-compliant, high FSC fuel, wet scrubbing leads to an increase in CCN activity but not to significant increases in CCN emission factors. However, switching to low FSC fuels resulted in emissions of highly hydrophobic particles, causing a significant reduction in CCN activity resulting in smaller CCN emission factors by at least one order of magnitude. Our observations are supported by chemical analysis of exhaust particles using scanning transmission X-ray microscopy and near edge X-ray absorption fine structure (STXM/NEXAFS) spectra. Potential implications of effects on ship exhaust particles for cloud and climate interactions due to different compliance measures are discussed.
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| 16. |
- Sebastiani, Federica, et al.
(author)
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Night-time oxidation at the air-water interface : co-surfactant effects in binary mixtures
- 2022
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In: Environmental Science. - : Royal Society of Chemistry. - 2634-3606. ; :6, s. 1324-1337
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Journal article (peer-reviewed)abstract
- The ageing of organic-coated aqueous aerosols at night is investigated by reacting NO3 with binary surfactant mixtures floating on water. The surfactants are oleic acid (OA), methyl oleate (MO) and stearic acid (SA). Deuterated surfactants mixed with hydrogenous surfactants were studied using neutron reflectometry to determine the reaction kinetics of organic two-component monolayers with NO3 at the air-water interface for the first time. We measured the rate coefficients for OA monolayers, mixed with hydrogenous co-surfactant MO or SA to be (3 +/- 1) x 10-8 cm2 per molecule per s or (3.6 +/- 0.9) x 10-8 cm2 per molecule per s and MO monolayers mixed with hydrogenous co-surfactant OA or SA to be (0.7 +/- 0.4) x 10-8 cm2 per molecule per s or (3 +/- 1) x 10-8 cm2 per molecule per s. The initial desorption lifetimes of NO3, taud,NO3,1, were 8 +/- 3 ns, 14 +/- 4 ns, 12 +/- 3 ns and 21 +/- 10 ns. The approximately doubled desorption lifetime for MO-SA compared to the other mixtures is consistent with a more accessible double bond associated with the larger area per molecule of MO in the presence of SA facilitating NO3 attack. The significantly slower reactive loss of MO-OA compared to a MO monolayer demonstrates that multi-component surfactant mixtures need to be studied in addition to single-component monolayers. Such a retarded decay would cause the residence time to change from ca. 4 to 22 minutes associated with increased transport distances of surfactant species together with any other pollutants that may be protected underneath the surfactant film.
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| 17. |
- Shepherd, Rosalie H., et al.
(author)
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Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air-water interface using material extracted from urban, remote and wood smoke aerosol
- 2022
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In: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:4, s. 574-590
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Journal article (peer-reviewed)abstract
- The presence of an organic film on a cloud droplet or aqueous aerosol particle has the potential to alter the chemical, optical and physical properties of the droplet or particle. In the study presented, water insoluble organic materials extracted from urban, remote (Antarctica) and wood burning atmospheric aerosol were found to have stable, compressible, films at the air-water interface that were typically similar to 6-18 angstrom thick. These films are reactive towards gas-phase OH radicals and decay exponentially, with bimolecular rate constants for reaction with gas-phase OH radicals of typically 0.08-1.5 x 10(-10) cm(3) molecule(-1) s(-1). These bimolecular rate constants equate to initial OH radical uptake coefficients estimated to be similar to 0.6-1 except woodsmoke (similar to 0.05). The film thickness and the neutron scattering length density of the extracted atmosphere aerosol material (from urban, remote and wood burning) were measured by neutron reflection as they were exposed to OH radicals. For the first time neutron reflection has been demonstrated as an excellent technique for studying the thin films formed at air-water interfaces from materials extracted from atmospheric aerosol samples. Additionally, the kinetics of gas-phase OH radicals with a proxy compound, the lipid 1,2-distearoyl-sn-glycero-3-phosphocholine (DSPC) was studied displaying significantly different behaviour, thus demonstrating it is not a good proxy for atmospheric materials that may form films at the air-water interface. The atmospheric lifetimes, with respect to OH radical oxidation, of the insoluble organic materials extracted from atmospheric aerosol at the air-water interface were a few hours. Relative to a possible physical atmospheric lifetime of 4 days, the oxidation of these films is important and needs inclusion in atmospheric models. The optical properties of these films were previously reported [Shepherd et al., Atmos. Chem. Phys., 2018, 18, 5235-5252] and there is a significant change in top of the atmosphere albedo for these thin films on core-shell atmospheric aerosol using the film thickness data and confirmation of stable film formation at the air-water interface presented here.
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| 18. |
- Siegel, Karolina, et al.
(author)
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Insights into the molecular composition of semi-volatile aerosols in the summertime central Arctic Ocean using FIGAERO-CIMS
- 2021
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In: Environmental Science. - 2634-3606. ; 1:4, s. 161-175
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Journal article (peer-reviewed)abstract
- The remote central Arctic during summertime has a pristine atmosphere with very low aerosol particle concentrations. As the region becomes increasingly ice-free during summer, enhanced ocean-atmosphere fluxes of aerosol particles and precursor gases may therefore have impacts on the climate. However, large knowledge gaps remain regarding the sources and physicochemical properties of aerosols in this region. Here, we present insights into the molecular composition of semi-volatile aerosol components collected in September 2018 during the MOCCHA (Microbiology-Ocean-Cloud-Coupling in the High Arctic) campaign as part of the Arctic Ocean 2018 expedition with the Swedish Icebreaker Oden. Analysis was performed offline in the laboratory using an iodide High Resolution Time-of-Flight Chemical Ionization Mass Spectrometer with a Filter Inlet for Gases and AEROsols (FIGAERO-HRToF-CIMS). Our analysis revealed significant signal from organic and sulfur-containing compounds, indicative of marine aerosol sources, with a wide range of carbon numbers and O : C ratios. Several of the sulfur-containing compounds are oxidation products of dimethyl sulfide (DMS), a gas released by phytoplankton and ice algae. Comparison of the time series of particulate and gas-phase DMS oxidation products did not reveal a significant correlation, indicative of the different lifetimes of precursor and oxidation products in the different phases. This is the first time the FIGAERO-HRToF-CIMS was used to investigate the composition of aerosols in the central Arctic. The detailed information on the molecular composition of Arctic aerosols presented here can be used for the assessment of aerosol solubility and volatility, which is relevant for understanding aerosol-cloud interactions.
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| 19. |
- Thomsen, Ditte, et al.
(author)
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The effect of temperature and relative humidity on secondary organic aerosol formation from ozonolysis of Δ3-carene
- 2024
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In: Environmental Science: Atmospheres. - 2634-3606. ; 4:1, s. 88-103
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Journal article (peer-reviewed)abstract
- This study investigates the effects of temperature and relative humidity (RH) on the formation of secondary organic aerosol (SOA) from Δ3-carene, a prevalent monoterpene in boreal forests. Dark ozonolysis experiments of 10 ppb Δ3-carene were conducted in the Aarhus University Research on Aerosol (AURA) atmospheric simulation chamber at temperatures of 0, 10, and 20 °C. Under dry conditions (RH < 2%), the SOA formation in terms of both particle number and mass concentration shows minimal temperature dependence. This is in contrast to previous findings at higher initial concentrations and suggests an effect of VOC loading for Δ3-carene. Interestingly, the mass fraction of key oxidation products (cis-3-caric acid, cis-3-caronic acid) exhibit a temperature dependence suggesting continuous condensation at lower temperatures, while evaporation and further reactions over time become more favourable at higher temperatures. The oxygen-to-carbon ratios in the particle phase and the occurrence of highly oxygenated organic molecules (HOM) in the gas phase show modest increases with higher temperatures. Predictions from the Aerosol Dynamics and Gas- and Particle-Phase Chemistry Kinetic Multilayer Model (ADCHAM) agrees with the experimental results regarding both physical particle properties and aerosol composition considering the experimental uncertainties. At high RH (∼80%, 10 °C), a considerable increase in the particle nucleation rate and particle number concentration is observed compared to experiments under dry conditions. This is likely due to enhanced particle nucleation resulting from more stable cluster formation of water and inorganics at increased RH. However, RH does not affect the particle mass concentration.
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