Late summer transition from a free-tropospheric to boundary layer source of Aitken mode aerosol in the high Arctic

Ruth Price; Andrea Baccarini; Julia Schmale; Paul Zieger; Ian M. Brooks; Paul Field; Ken S. Carslaw
2023 | Atmos. Chem. Phys. | 23 (2927-2961)

In the Arctic, the aerosol budget plays a particular role in determining the behaviour of clouds,
which are important for the surface energy balance and thus for the region’s climate. A key question is the extent to which cloud condensation nuclei in the high Arctic summertime boundary layer are controlled by local emission and formation processes as opposed to transport from outside. Each of these sources is likely to respond differently to future changes in ice cover. Here we use a global model and observations from ship and aircraft field campaigns to understand the source of high Arctic aerosol in late summer. We find that particles formed remotely, i.e. at latitudes outside the Arctic, are the dominant source of boundary layer Aitken mode particles during the sea ice melt period up to the end of August. Particles from such remote sources, entrained into the boundary layer from the free troposphere, account for nucleation and Aitken mode particle concentrations that are otherwise underestimated by the model. This source from outside the high Arctic declines as photochemical rates decrease towards the end of summer and is largely replaced by local new particle formation driven by iodic acid created during freeze-up. Such a local source increases the simulated Aitken mode particle concentrations by 2 orders of magnitude during sea ice freeze-up and is consistent with strong fluctuations in nucleation mode concentrations that occur in September. Our results suggest a high-Arctic aerosol regime shift in late summer,
and only after this shift do cloud condensation nuclei become sensitive to local aerosol processes.

The Representation of Sea Salt Aerosols and Their Role in Polar Climate Within CMIP6

Rémy Lapere; Jennie L. Thomas; Louis Marelle; Annica M. L. Ekman; Markus M. Frey; Marianne Tronstad Lund; Risto Makkonen; Ananth Ranjithkumar; Matthew E. Salter; Bjørn Hallvard Samset; Michael Schulz; Larisa Sogacheva; Xin Yang; Paul Zieger
2023 | J. Geophys. Res.-Atmos. | e2022JD038235 (1-36)

Natural aerosols and their interactions with clouds remain an important uncertainty within
climate models, especially at the poles. Here, we study the behavior of sea salt aerosols (SSaer) in the Arctic and Antarctic within 12 climate models from CMIP6. We investigate the driving factors that control SSaer abundances and show large differences based on the choice of the source function, and the representation of aerosol processes in the atmosphere. Close to the poles, the CMIP6 models do not match observed seasonal cycles of surface concentrations, likely due to the absence of wintertime SSaer sources such as blowing snow. Further away from the poles, simulated concentrations have the correct seasonality, but have a positive mean bias of up to one order of magnitude. SSaer optical depth is derived from the MODIS data and compared to modeled values, revealing good agreement, except for winter months. Better agreement for aerosol optical depth than surface concentration may indicate a need for improving the vertical distribution, the size distribution and/or hygroscopicity of modeled polar SSaer. Source functions used in CMIP6 emit very different numbers of small SSaer, potentially exacerbating cloud-aerosol interaction uncertainties in these remote regions. For future climate scenarios SSP126 and SSP585, we show that SSaer concentrations increase at both poles at the end of the 21st century, with more than two times mid-20th century values in the Arctic. The pre-industrial climate CMIP6 experiments suggest there is a large uncertainty in the polar radiative budget due to SSaer.

The Ny-Ålesund Aerosol Cloud Experiment (NASCENT): Overview and First Results

J. T. Pasquier; R. O. David; G. Freitas; R. Gierens; Y. Gramlich; S. Haslett; G. Li; B. Schäfer; K. Siegel; J. Wieder; K. Adachi; F. Belosi; T. Carlsen; S. Decesari; K. Ebell; S. Gilardoni; M. Gysel-Beer; J. Henneberger; J. Inoue; Z. A. Kanji; M. Koike; Y. Kondo; R. Krejci; U. Lohmann; M. Maturilli; M. Mazzolla; R. Modini; C. Mohr; G. Motos; A. Nenes; A. Nicosia; S. Ohata; M. Paglione; S. Park; R. E. Pileci; F. Ramelli; M. Rinaldi; C. Ritter; K. Sato; T. Storelvmo; Y. Tobo; R. Traversi; A. Viola; P. Zieger
2022 | Bull. Amer. Meteor. Soc. (E2533-E2558)

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.

Composition and mixing state of Arctic aerosol and cloud residual particles from long-term single-particle observations at Zeppelin Observatory, Svalbard

Kouji Adachi; Yutaka Tobo; Makoto Koike; Gabriel Freitas; Paul Zieger; Radovan Krejci
2022 | Atmos. Chem. Phys. | 22 (14421-14439)

The Arctic region is sensitive to climate change and is warming faster than the global average. Aerosol particles change cloud properties by acting as cloud condensation nuclei and ice-nucleating particles, thus influencing the Arctic climate system. Therefore, understanding the aerosol particle properties in the Arctic is needed to interpret and simulate their influences on climate. In this study, we collected ambient aerosol particles using whole-air and PM10 inlets and residual particles of cloud droplets and ice crystals from Arctic low-level clouds (typically, all-liquid or mixed-phase clouds) using a counterflow virtual impactor inlet at the Zeppelin Observatory near Ny-Ålesund, Svalbard, within a time frame of 4 years. We measured the composition and mixing state of individual fine-mode particles in 239 samples using transmission electron microscopy. On the basis of their composition, the aerosol and cloud residual particles were classified as mineral dust, sea salt, K-bearing, sulfate, and carbonaceous particles. The number fraction of aerosol particles showed seasonal changes, with sulfate dominating in summer and sea salt increasing in winter. There was no measurable difference in the fractions between ambient aerosol and cloud residual particles collected at ambient temperatures above 0 ∘C. On the other hand, cloud residual samples collected at ambient temperatures below 0 ∘C had several times more sea salt and mineral dust particles and fewer sulfates than ambient aerosol samples, suggesting that sea spray and mineral dust particles may influence the formation of cloud particles in Arctic mixed-phase clouds. We also found that 43 % of mineral dust particles from cloud residual samples were mixed with sea salt, whereas only 18 % of mineral dust particles in ambient aerosol samples were mixed with sea salt. This study highlights the variety in aerosol compositions and mixing states that influence or are influenced by aerosol–cloud interactions in Arctic low-level clouds.

Using Novel Molecular-Level Chemical Composition Observations of High Arctic Organic Aerosol for Predictions of Cloud Condensation Nuclei

Siegel, K.; Neuberger, A.; Karlsson, L.; Zieger, P.; Mattsson, F.; Duplessis, P.; Dada, L.; Daellenbach, K.; Schmale, J.; Baccarini, A.; Krejci, R.; Svenningsson, B.; Chang, R.; Ekman, A.; Riipinen, I.; Mohr, C.
2022 | Environ. Sci. Technol. | 56 (19) (13888-13899)
aerosol chemistry , aerosol−cloud interactions , atmospheric aerosol , CCN closure , chemical ionization mass spectrometry (CIMS) , cloud droplet activation , High Arctic

Predictions of cloud droplet activation in the late summertime (September) central Arctic Ocean are made using κ-Köhler theory with novel observations of the aerosol chemical composition from a high-resolution time-of-flight chemical ionization mass spectrometer with a filter inlet for gases and aerosols (FIGAERO-CIMS) and an aerosol mass spectrometer (AMS), deployed during the Arctic Ocean 2018 expedition onboard the Swedish icebreaker Oden. We find that the hygroscopicity parameter κ of the total aerosol is 0.39 ± 0.19 (mean ± std). The predicted activation diameter of ∼25 to 130 nm particles is overestimated by 5%, leading to an underestimation of the cloud condensation nuclei (CCN) number concentration by 4–8%. From this, we conclude that the aerosol in the High Arctic late summer is acidic and therefore highly cloud active, with a substantial CCN contribution from Aitken mode particles. Variability in the predicted activation diameter is addressed mainly as a result of uncertainties in the aerosol size distribution measurements. The organic κ was on average 0.13, close to the commonly assumed κ of 0.1, and therefore did not significantly influence the predictions. These conclusions are supported by laboratory experiments of the activation potential of seven organic compounds selected as representative of the measured aerosol.

Emission of primary bioaerosol particles from Baltic seawater

Gabriel P. Freitas; Christian Stolle; Paul H. Kaye; Warren Stanley; Daniel P. R. Herlemann; Matthew Salter; Paul Zieger
2022 | Environ. Sci. Atmos.

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.

The Effect of Seawater Salinity and Seawater Temperature on Sea Salt Aerosol Production

2022 | J. Geophys. Res.-Atmos. | 127

To improve our understanding of the impact of sea salt aerosols (SSA) on the Earth's climate, it is critical to understand the physical mechanisms which determine the size-resolved SSA production flux. Of the factors affecting SSA emissions, seawater salinity has perhaps received the least attention in the literature and previous studies have produced conflicting results. Here, we present a series of laboratory experiments designed to investigate the role of salinity on aerosol production from artificial seawater using a continuous plunging jet. During these experiments, the aerosol and surface bubble size distributions were monitored while the salinity was decreased from 35 to 0 g kg−1. Three distinct salinity regimes were identified: (a) A high salinity regime, 10–35 g kg−1, where lower salinity resulted in only minor reductions in particle number flux but notable reductions in particle volume flux; (b) an intermediate salinity regime, 5–10 g kg−1, with a local maximum in particle number flux; (c) a low salinity regime, <5 g kg−1, characterized by a rapid decrease in particle number flux at lower salinities and dominated by small particles and larger bubbles. We discuss the implications of our results through comparison of the size-resolved aerosol flux and the surface bubble population at different salinities. Finally, by varying the seawater temperature at three specific salinities we have also developed a simple parameterization of the particle production flux as a function of seawater temperature and salinity. The range of seawater salinity and temperature studied is representative of the global oceans and lower salinity water bodies such as the Baltic Sea.

Surface composition of size-selected sea salt particles under the influence of organic acids studied in situ using synchrotron radiation X-ray photoelectron spectroscopy

Minna Patanen; Isaak Unger; Clara-Magdalena Saak; Geethanjali Gopakumar; Rebecka Lexelius; Olle Björneholm; Matthew Salter; Paul Zieger
2022 | Environ. Sci. Atmos.

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.

Physical and Chemical Properties of Cloud Droplet Residuals and Aerosol Particles During the Arctic Ocean 2018 Expedition

Linn Karlsson; Andrea Baccarini; Patrick Duplessis; Darrel Baumgardner; Ian M. Brooks; Rachel Y.-W. Chang; Lubna Dada; Kaspar R. Dällenbach; Liine Heikkinen; Radovan Krejci; W. Richard Leaitch; Caroline Leck; Daniel G. Partridge; Matthew E. Salter; Heini Wernli; Michael J. Wheeler; Julia Schmale; Paul Zieger
2022 | J. Geophys. Res.-Atmos. | 127 (e2021JD036383)

Detailed knowledge of the physical and chemical properties and sources of particles that form clouds is especially important in pristine areas like the Arctic, where particle concentrations are often low and observations are sparse. Here, we present in situ cloud and aerosol measurements from the central Arctic Ocean in August–September 2018 combined with air parcel source analysis. We provide direct experimental evidence that Aitken mode particles (particles with diameters ≲70 nm) significantly contribute to cloud condensation nuclei (CCN) or cloud droplet residuals, especially after the freeze-up of the sea ice in the transition toward fall. These Aitken mode particles were associated with air that spent more time over the pack ice, while size distributions dominated by accumulation mode particles (particles with diameters ≳70 nm) showed a stronger contribution of oceanic air and slightly different source regions. This was accompanied by changes in the average chemical composition of the accumulation mode aerosol with an increased relative contribution of organic material toward fall. Addition of aerosol mass due to aqueous-phase chemistry during in-cloud processing was probably small over the pack ice given the fact that we observed very similar particle size distributions in both the whole-air and cloud droplet residual data. These aerosol–cloud interaction observations provide valuable insight into the origin and physical and chemical properties of CCN over the pristine central Arctic Ocean.

Tropical and Boreal Forest – Atmosphere Interactions: A Review

Paulo Artaxo; Hans-Christen Hansson; Meinrat O. Andreae; Jaana Bäck; Eliane Gomes Alves; Henrique M. J. Barbosa; Frida Bender; Efstratios Bourtsoukidis; Samara Carbone; Jinshu Chi; Stefano Decesari; Viviane R. Després; Florian Ditas; Ekaterina Ezhova; Sandro Fuzzi; Niles J. Hasselquist; Jost Heintzenberg; Bruna A. Holanda; Alex Guenther; Hannele Hakola; Liine Heikkinen; Veli-Matti Kerminen; Jenni Kontkanen; Radovan Krejci; Markku Kulmala; Jost V. Lavric; Gerrit de Leeuw; Katrianne Lehtipalo; Luiz Augusto T. Machado; Gordon McFiggans; arco Aurelio M. Franco; Bruno Backes Meller; Fernando G. Morais; Claudia Mohr; William Morgan; Mats B. Nilsson; Matthias Peichl; Tuukka Petäjä; Maria Praß; Christopher Pöhlker; Mira L. Pöhlker; Ulrich Pöschl; Celso Von Randow; Ilona Riipinen; Janne Rinne; Luciana V. Rizzo; Daniel Rosenfeld; Maria A. F. Silva Dias; Larisa Sogacheva; Philip Stier; Erik Swietlicki; Matthias Sörgel; Peter Tunved; Aki Virkkula; Jian Wang; Bettina Weber; Ana Maria Yáñez-Serrano; Paul Zieger; Eugene Mikhailov; James N. Smith; Jürgen Kesselmeier
2022 | TELLUS B | 74 (24-163)

This review presents how the boreal and the tropical forests affect the atmosphere, its chemical composition, its function, and further how that affects the climate and, in return, the ecosystems through feedback processes. Observations from key tower sites standing out due to their long-term comprehensive observations: The Amazon Tall Tower Observatory in Central Amazonia, the Zotino Tall Tower Observatory in Siberia, and the Station to Measure Ecosystem-Atmosphere Relations at Hyytiäla in Finland. The review is complemented by short-term observations from networks and large experiments.

The review discusses atmospheric chemistry observations, aerosol formation and processing, physiochemical aerosol, and cloud condensation nuclei properties and finds surprising similarities and important differences in the two ecosystems. The aerosol concentrations and chemistry are similar, particularly concerning the main chemical components, both dominated by an organic fraction, while the boreal ecosystem has generally higher concentrations of inorganics, due to higher influence of long-range transported air pollution. The emissions of biogenic volatile organic compounds are dominated by isoprene and monoterpene in the tropical and boreal regions, respectively, being the main precursors of the organic aerosol fraction.

Observations and modeling studies show that climate change and deforestation affect the ecosystems such that the carbon and hydrological cycles in Amazonia are changing to carbon neutrality and affect precipitation downwind. In Africa, the tropical forests are so far maintaining their carbon sink.

It is urgent to better understand the interaction between these major ecosystems, the atmosphere, and climate, which calls for more observation sites, providing long-term data on water, carbon, and other biogeochemical cycles. This is essential in finding a sustainable balance between forest preservation and reforestation versus a potential increase in food production and biofuels, which are critical in maintaining ecosystem services and global climate stability. Reducing global warming and deforestation is vital for tropical forests.

Atmospheric composition in the European Arctic and 30 years of the Zeppelin Observatory, Ny-Ålesund

Platt, S. M.; Hov, Ø.; Berg, T.; Breivik, K.; Eckhardt, S.; Eleftheriadis, K.; Evangeliou, N.; Fiebig, M.; Fisher, R.; Hansen, G.; Hansson, H.-C.; Heintzenberg, J.; Hermansen, O.; Heslin-Rees, D.; Holmén, K.; Hudson, S.; Kallenborn, R.; Krejci, R.: Krognes, T.; Larssen, S.; Lowry, D.; Lund Myhre, C.; Lunder, C.; Nisbet, E.; Nizzetto, P. B.; Park, K.-T.; Pedersen, C. A.; Aspmo Pfaffhuber, K.; Röckmann, T.; Schmidbauer, N.; Solberg, S.; Stohl, A.; Ström, J.; Svendby, T.; Tunved, P.; Tørnkvist, K.; van der Veen, C.; Vratolis, S.; Yoon, Y. J.; Yttri, K. E.; Zieger, P.; Aas, W.; Tørseth, K.
2022 | Atmos. Chem. Phys. | 22 (3321-3369)

The Zeppelin Observatory (78.90∘ N, 11.88∘ E) is located on Zeppelin Mountain at 472 m a.s.l. on Spitsbergen, the largest island of the Svalbard archipelago. Established in 1989, the observatory is part of Ny-Ålesund Research Station and an important atmospheric measurement site, one of only a few in the high Arctic, and a part of several European and global monitoring programmes and research infrastructures, notably the European Monitoring and Evaluation Programme (EMEP); the Arctic Monitoring and Assessment Programme (AMAP); the Global Atmosphere Watch (GAW); the Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS); the Advanced Global Atmospheric Gases Experiment (AGAGE) network; and the Integrated Carbon Observation System (ICOS). The observatory is jointly operated by the Norwegian Polar Institute (NPI), Stockholm University, and the Norwegian Institute for Air Research (NILU). Here we detail the establishment of the Zeppelin Observatory including historical measurements of atmospheric composition in the European Arctic leading to its construction. We present a history of the measurements at the observatory and review the current state of the European Arctic atmosphere, including results from trends in greenhouse gases, chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs), other traces gases, persistent organic pollutants (POPs) and heavy metals, aerosols and Arctic haze, and atmospheric transport phenomena, and provide an outline of future research directions.

Highly Active Ice-Nucleating Particles at the Summer North Pole

Grace C. E. Porter; Michael P. Adams; Ian M. Brooks; Luisa Ickes; Linn Karlsson; Caroline Leck; Matthew E. Salter; Julia Schmale; Karolina Siegel; Sebastien N. F. Sikora; Mark D. Tarn; Jutta Vüllers; Heini Wernli; Paul Zieger; Julika Zinke; Benjamin J. Murray
2022 | J. Geophys. Res.-Atmos. | e2021JD036059

The amount of ice versus supercooled water in clouds is important for their radiative properties and role in climate feedbacks. Hence, knowledge of the concentration of ice-nucleating particles (INPs) is needed. Generally, the concentrations of INPs are found to be very low in remote marine locations allowing cloud water to persist in a supercooled state. We had expected the concentrations of INPs at the North Pole to be very low given the distance from open ocean and terrestrial sources coupled with effective wet scavenging processes. Here we show that during summer 2018 (August and September) high concentrations of biological INPs (active at >−20°C) were sporadically present at the North Pole. In fact, INP concentrations were sometimes as high as those recorded at mid-latitude locations strongly impacted by highly active biological INPs, in strong contrast to the Southern Ocean. Furthermore, using a balloon borne sampler we demonstrated that INP concentrations were often different at the surface versus higher in the boundary layer where clouds form. Back trajectory analysis suggests strong sources of INPs near the Russian coast, possibly associated with wind-driven sea spray production, whereas the pack ice, open leads, and the marginal ice zone were not sources of highly active INPs. These findings suggest that primary ice production, and therefore Arctic climate, is sensitive to transport from locations such as the Russian coast that are already experiencing marked climate change.

Contact information

Visiting addresses:

Geovetenskapens Hus,
Svante Arrhenius väg 8, Stockholm

Arrheniuslaboratoriet, Svante Arrhenius väg 16, Stockholm (Unit for Toxicological Chemistry)

Mailing address:
Department of Environmental Science
Stockholm University
106 91 Stockholm

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