| 1. |
- Gramlich, Yvette, 1993-, et al.
(författare)
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Impact of Biomass Burning on Arctic Aerosol Composition
- 2024
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Ingår i: ACS Earth and Space Chemistry. - 2472-3452.
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Tidskriftsartikel (refereegranskat)abstract
- Emissions from biomass burning (BB) occurring at midlatitudes can reach the Arctic, where they influence the remote aerosol population. By using measurements of levoglucosan and black carbon, we identify seven BB events reaching Svalbard in 2020. We find that most of the BB events are significantly different to the rest of the year (nonevents) for most of the chemical and physical properties. Aerosol mass and number concentrations are enhanced by up to 1 order of magnitude during the BB events. During BB events, the submicrometer aerosol bulk composition changes from an organic- and sulfate-dominated regime to a clearly organic-dominated regime. This results in a significantly lower hygroscopicity parameter κ for BB aerosol (0.4 ± 0.2) compared to nonevents (0.5 ± 0.2), calculated from the nonrefractory aerosol composition. The organic fraction in the BB aerosol showed no significant difference for the O:C ratios (0.9 ± 0.3) compared to the year (0.9 ± 0.6). Accumulation mode particles were present during all BB events, while in the summer an additional Aitken mode was observed, indicating a mixture of the advected air mass with locally produced particles. BB tracers (vanillic, homovanillic, and hydroxybenzoic acid, nitrophenol, methylnitrophenol, and nitrocatechol) were significantly higher when air mass back trajectories passed over active fire regions in Eastern Europe, indicating agricultural and wildfires as sources. Our results suggest that the impact of BB on the Arctic aerosol depends on the season in which they occur, and agricultural and wildfires from Eastern Europe have the potential to disturb the background conditions the most.
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| 2. |
- Gramlich, Yvette, 1993-, et al.
(författare)
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Revealing the chemical characteristics of Arctic low-level cloud residuals – in situ observations from a mountain site
- 2023
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Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 23:12, s. 6813-6834
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Tidskriftsartikel (refereegranskat)abstract
- The role aerosol chemical composition plays in Arctic low-level cloud formation is still poorly understood. In this study we address this issue by combining in situ observations of the chemical characteristics of cloud residuals (dried liquid cloud droplets or ice crystals) and aerosol particles from the Zeppelin Observatory in Ny-Ålesund, Svalbard (approx. 480 m a.s.l.). These measurements were part of the 1-year-long Ny-Ålesund Aerosol and Cloud Experiment 2019–2020 (NASCENT). To obtain the chemical composition of cloud residuals at molecular level, we deployed a Filter Inlet for Gases and AEROsols coupled to a Chemical Ionization Mass Spectrometer (FIGAERO-CIMS) with iodide as the reagent ion behind a ground-based counterflow virtual impactor (GCVI). The station was enshrouded in clouds roughly 15 % of the time during NASCENT, out of which we analyzed 14 cloud events between December 2019 and December 2020. During the entire year, the composition of the cloud residuals shows contributions from oxygenated organic compounds, including organonitrates, and traces of the biomass burning tracer levoglucosan. In summer, methanesulfonic acid (MSA), an oxidation product of dimethyl sulfide (DMS), shows large contributions to the sampled mass, indicating marine natural sources of cloud condensation nuclei (CCN) and ice nucleating particle (INP) mass during the sunlit part of the year. In addition, we also find contributions of the inorganic acids nitric acid and sulfuric acid, with outstanding high absolute signals of sulfuric acid in one cloud residual sample in spring and one in late summer (21 May and 12 September 2020), probably caused by high anthropogenic sulfur emissions near the Barents Sea and Kara Sea. During one particular cloud event, on 18 May 2020, the air mass origin did not change before, during, or after the cloud. We therefore chose it as a case study to investigate cloud impact on aerosol physicochemical properties. We show that the overall chemical composition of the organic aerosol particles was similar before, during, and after the cloud, indicating that the particles had already undergone one or several cycles of cloud processing before being measured as residuals at the Zeppelin Observatory and/or that, on the timescales of the observed cloud event, cloud processing of the organic fraction can be neglected. Meanwhile, there were on average fewer particles but relatively more in the accumulation mode after the cloud. Comparing the signals of sulfur-containing compounds of cloud residuals with aerosols during cloud-free conditions, we find that sulfuric acid had a higher relative contribution to the cloud residuals than to aerosols during cloud-free conditions, but we did not observe an increase in particulate MSA due to the cloud. Overall, the chemical composition, especially of the organic fraction of the Arctic cloud residuals, reflected the overall composition of the general aerosol population well. Our results thus suggest that most aerosols can serve as seeds for low-level clouds in the Arctic.
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| 3. |
- Kommula, S. M., et al.
(författare)
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Effect of Long-Range Transported Fire Aerosols on Cloud Condensation Nuclei Concentrations and Cloud Properties at High Latitudes
- 2024
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Ingår i: Geophysical Research Letters. - 0094-8276 .- 1944-8007. ; 51:6
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Tidskriftsartikel (refereegranskat)abstract
- Active vegetation fires in south-eastern (SE) Europe resulted in a notable increase in the number concentration of aerosols and cloud condensation nuclei (CCN) particles at two high latitude locations—the SMEAR IV station in Kuopio, Finland, and the Zeppelin Observatory in Svalbard, high Arctic. During the fire episode aerosol hygroscopicity κ slightly increased at SMEAR IV and at the Zeppelin Observatory κ decreased. Despite increased κ in high CCN conditions at SMEAR IV, the aerosol activation diameter increased due to the decreased supersaturation with an increase in aerosol loading. In addition, at SMEAR IV during the fire episode, in situ measured cloud droplet number concentration (CDNC) increased by a factor of ∼7 as compared to non-fire periods which was in good agreement with the satellite observations (MODIS, Terra). Results from this study show the importance of SE European fires for cloud properties and radiative forcing in high latitudes.
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| 4. |
- Siegel, Karolina, 1990-, et al.
(författare)
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Arctic observations of hydroperoxymethyl thioformate (HPMTF) – seasonal behavior and relationship to other oxidation products of dimethyl sulfide at the Zeppelin Observatory, Svalbard
- 2023
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Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 23:13, s. 7569-7587
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Tidskriftsartikel (refereegranskat)abstract
- Dimethyl sulfide (DMS), a gas produced by phytoplankton, is the largest source of atmospheric sulfur over marine areas. DMS undergoes oxidation in the atmosphere to form a range of oxidation products, out of which sulfuric acid (SA) is well known for participating in the formation and growth of atmospheric aerosol particles, and the same is also presumed for methanesulfonic acid (MSA). Recently, a new oxidation product of DMS, hydroperoxymethyl thioformate (HPMTF), was discovered and later also measured in the atmosphere. Little is still known about the fate of this compound and its potential to partition into the particle phase. In this study, we present a full year (2020) of concurrent gas- and particle-phase observations of HPMTF, MSA, SA and other DMS oxidation products at the Zeppelin Observatory (Ny-Ålesund, Svalbard) located in the Arctic. This is the first time HPMTF has been measured in Svalbard and attempted to be observed in atmospheric particles. The results show that gas-phase HPMTF concentrations largely follow the same pattern as MSA during the sunlit months (April–September), indicating production of HPMTF around Svalbard. However, HPMTF was not observed in significant amounts in the particle phase, despite high gas-phase levels. Particulate MSA and SA were observed during the sunlit months, although the highest median levels of particulate SA were measured in February, coinciding with the highest gaseous SA levels with assumed anthropogenic origin. We further show that gas- and particle-phase MSA and SA are coupled in May–July, whereas HPMTF lies outside of this correlation due to the low particulate concentrations. These results provide more information about the relationship between HPMTF and other DMS oxidation products, in a part of the world where these have not been explored yet, and about HPMTF's ability to contribute to particle growth and cloud formation.
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| 5. |
- Gramlich, Yvette, 1993-
(författare)
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Chemical composition of Arctic aerosols and their link to clouds
- 2023
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The Arctic is a place particularly vulnerable to climate change, warming at an accelerated rate compared to the rest of the Earth. In this remote environment, the atmosphere, the ocean, the ice, and the land are all interlinked and are shaping a very complex system. This is why the interplay between aerosols and clouds and their role in the warming Arctic is still not fully understood.To address this issue, a better understanding of the sources, properties, and fate of aerosol particles in the Arctic is needed. By means of in situ observations of aerosols and clouds at the Zeppelin Observatory on Svalbard, this thesis aims to shed light on aerosol-cloud interactions in the Arctic. These measurements were conducted within the framework of the one-year long Ny-Ålesund Aerosol Cloud Experiment (2019-2020). A special focus of this thesis is on the chemical composition of aerosol particles from a molecular-level perspective, where measurements from a filter inlet for gases and aerosols coupled to a chemical ionization mass spectrometer were used.To identify the properties of the aerosol particles serving as cloud condensation nuclei (CCN) or ice nucleating particles (INP), cloud droplets and ice crystals were sampled with a ground-based counterflow virtual impactor inlet. The measured particles are called cloud residuals. The observations show that the cloud residuals have sizes in the Aitken and accumulation mode (as small as 10 nm in diameter). The chemical composition of these cloud residuals followed largely the expected annual cycle of aerosol particles in the Arctic, suggesting that most of the aerosol particles can act as CCN or INP in the Arctic. Anthropogenic signatures were present in the cloud residuals in the winter and spring, whereas in the summer a large contribution from methanesulfonic acid (MSA) was present, indicating natural source regions.The thesis also investigated how the oxidation products of dimethyl sulfide, MSA, sulfuric acid, and hydroperoxymethyl thioformate (HPMTF) are related to each other in the gaseous and particulate phase. HPMTF was observed to be present mainly in the gas phase, where it followed the gas phase signal of MSA in the summer. However, it was not present in significant amounts in the particle phase. In the presence of clouds, the gas phase levels of HPMTF decreased, indicating the uptake by cloud droplets.Another source of aerosol particles investigated are those from biomass burning (BB) emissions. The BB aerosol showed a largely similar molecular-level chemical composition of the organic aerosol compared to the rest of the year; however, a clear change to a largely organic dominated bulk aerosol composition was observed. Back trajectories suggested mainly Eastern Europe and Siberia as the source regions for the BB events. Using BB tracer compounds in combination with the back trajectories suggested that agricultural fires from Eastern Europe have a larger impact on the Arctic aerosol population, where mass and number enhancements compared to times not influenced by BB were found to reach up to one order of magnitude.The results from this thesis show that aerosol particles from natural emissions are an important source for Arctic aerosol particles. Especially, emissions from marine biological activity are relevant for the growth of aerosol particles to sizes in the CCN active regime in the summer.
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| 6. |
- Huang, Wei, et al.
(författare)
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Variation in chemical composition and volatility of oxygenated organic aerosol in different rural, urban, and mountain environments
- 2024
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Ingår i: Atmospheric Chemistry and Physics. - 1680-7316 .- 1680-7324. ; 24:4, s. 2607-2624
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Tidskriftsartikel (refereegranskat)abstract
- The apparent volatility of atmospheric organic aerosol (OA) particles is determined by their chemical composition and environmental conditions (e.g., ambient temperature). A quantitative, experimental assessment of volatility and the respective importance of these two factors remains challenging, especially in ambient measurements. We present molecular composition and volatility of oxygenated OA (OOA) particles in different rural, urban, and mountain environments (including Chacaltaya, Bolivia; Alabama, US; Hyytiälä, Finland; Stuttgart and Karlsruhe, Germany; and Delhi, India) based on deployments of a filter inlet for gases and aerosols coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (FIGAERO-CIMS). We find on average larger carbon numbers (nC) and lower oxygen-To-carbon (O:C) ratios at the urban sites (nC: 9.8±0.7; O:C: 0.76±0.03; average ±1 standard deviation) compared to the rural (nC: 8.8±0.6; O:C: 0.80±0.05) and mountain stations (nC: 8.1±0.8; O:C: 0.91±0.07), indicative of different emission sources and chemistry. Compounds containing only carbon, hydrogen, and oxygen atoms (CHO) contribute the most to the total OOA mass at the rural sites (79.9±5.2%), in accordance with their proximity to forested areas (66.2±5.5% at the mountain sites and 72.6±4.3% at the urban sites). The largest contribution of nitrogen-containing compounds (CHON) is found at the urban stations (27.1±4.3%), consistent with their higher NOx levels. Moreover, we parametrize OOA volatility (saturation mass concentrations, Csat) using molecular composition information and compare it with the bulk apparent volatility derived from thermal desorption of the OOA particles within the FIGAERO. We find differences in Csat values of up to 1/43 orders of magnitude and variation in thermal desorption profiles (thermograms) across different locations and systems. From our study, we draw the general conclusion that environmental conditions (e.g., ambient temperature) do not directly affect OOA apparent volatility but rather indirectly by influencing the sources and chemistry of the environment and thus the chemical composition. The comprehensive dataset provides results that show the complex thermodynamics and chemistry of OOA and their changes during its lifetime in the atmosphere. We conclude that generally the chemical description of OOA suffices to predict its apparent volatility, at least qualitatively. Our study thus provides new insights that will help guide choices of, e.g., descriptions of OOA volatility in different model frameworks such as air quality models and cloud parcel models.
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| 7. |
- Pasquier, J. T., et al.
(författare)
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The Ny-Ålesund Aerosol Cloud Experiment (NASCENT) : Overview and First Results
- 2022
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Ingår i: Bulletin of The American Meteorological Society - (BAMS). - 0003-0007 .- 1520-0477. ; 103:11, s. e2533-E2558
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Tidskriftsartikel (refereegranskat)abstract
- The Arctic is warming at more than twice the rate of the global average. This warming is influenced by clouds, which modulate the solar and terrestrial radiative fluxes and, thus, determine the surface energy budget. However, the interactions among clouds, aerosols, and radiative fluxes in the Arctic are still poorly understood. To address these uncertainties, the Ny-Ålesund Aerosol Cloud Experiment (NASCENT) study was conducted from September 2019 to August 2020 in Ny-Ålesund, Svalbard. The campaign’s primary goal was to elucidate the life cycle of aerosols in the Arctic and to determine how they modulate cloud properties throughout the year. In situ and remote sensing observations were taken on the ground at sea level, at a mountaintop station, and with a tethered balloon system. An overview of the meteorological and the main aerosol seasonality encountered during the NASCENT year is introduced, followed by a presentation of first scientific highlights. In particular, we present new findings on aerosol physicochemical and molecular properties. Further, the role of cloud droplet activation and ice crystal nucleation in the formation and persistence of mixed-phase clouds, and the occurrence of secondary ice processes, are discussed and compared to the representation of cloud processes within the regional Weather Research and Forecasting Model. The paper concludes with research questions that are to be addressed in upcoming NASCENT publications.
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| 8. |
- Zha, Qiaozhi, et al.
(författare)
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Oxidized organic molecules in the tropical free troposphere over Amazonia
- 2024
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Ingår i: National Science Review. - 2095-5138 .- 2053-714X. ; 11:1
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Tidskriftsartikel (refereegranskat)abstract
- New particle formation (NPF) in the tropical free troposphere (FT) is a globally important source of cloud condensation nuclei, affecting cloud properties and climate. Oxidized organic molecules (OOMs) produced from biogenic volatile organic compounds are believed to contribute to aerosol formation in the tropical FT, but without direct chemical observations. We performed in situ molecular-level OOMs measurements at the Bolivian station Chacaltaya at 5240 m above sea level, on the western edge of Amazonia. For the first time, we demonstrate the presence of OOMs, mainly with 4-5 carbon atoms, in both gas-phase and particle-phase (in terms of mass contribution) measurements in tropical FT air from Amazonia. These observations, combined with air mass history analyses, indicate that the observed OOMs are linked to isoprene emitted from the rainforests hundreds of kilometers away. Based on particle-phase measurements, we find that these compounds can contribute to NPF, at least the growth of newly formed nanoparticles, in the tropical FT on a continental scale. Thus, our study is a fundamental and significant step in understanding the aerosol formation process in the tropical FT. In-situ molecular-level measurements demonstrate the presence of oxidized organic molecules, mainly with 4-5 carbon atoms, in both gas-phase and particle-phase in tropical free troposphere air from Amazonia. These molecules are linked to isoprene emitted from the rainforests hundreds of kilometers away, and can contribute to new particle formation.
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