| 1. |
- Blichner, Sara M., 1989-, et al.
(författare)
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Process-evaluation of forest aerosol-cloud-climate feedback shows clear evidence from observations and large uncertainty in models
- 2024
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Ingår i: Nature Communications. - 2041-1723. ; 15
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Tidskriftsartikel (refereegranskat)abstract
- Natural aerosol feedbacks are expected to become more important in the future, as anthropogenic aerosol emissions decrease due to air quality policy. One such feedback is initiated by the increase in biogenic volatile organic compound (BVOC) emissions with higher temperatures, leading to higher secondary organic aerosol (SOA) production and a cooling of the surface via impacts on cloud radiative properties. Motivated by the considerable spread in feedback strength in Earth System Models (ESMs), we here use two long-term observational datasets from boreal and tropical forests, together with satellite data, for a process-based evaluation of the BVOC-aerosol-cloud feedback in four ESMs. The model evaluation shows that the weakest modelled feedback estimates can likely be excluded, but highlights compensating errors making it difficult to draw conclusions of the strongest estimates. Overall, the method of evaluating along process chains shows promise in pin-pointing sources of uncertainty and constraining modelled aerosol feedbacks.
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| 2. |
- Heikkinen, Liine, 1990-, et al.
(författare)
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Cloud response to co-condensation of water and organic vapors over the boreal forest
- 2024
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Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 24:8, s. 5117-5147
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Tidskriftsartikel (refereegranskat)abstract
- Accounting for the condensation of organic vapors along with water vapor (co-condensation) has been shown in adiabatic cloud parcel model (CPM) simulations to enhance the number of aerosol particles that activate to form cloud droplets. The boreal forest is an important source of biogenic organic vapors, but the role of these vapors in co-condensation has not been systematically investigated. In this work, the environmental conditions under which strong co-condensation-driven cloud droplet number enhancements would be expected over the boreal biome are identified. Recent measurement technology, specifically the Filter Inlet for Gases and AEROsols (FIGAERO) coupled to an iodide-adduct chemical ionization mass spectrometer (I-CIMS), is utilized to construct volatility distributions of the boreal atmospheric organics. Then, a suite of CPM simulations initialized with a comprehensive set of concurrent aerosol observations collected in the boreal forest of Finland during spring 2014 is performed. The degree to which co-condensation impacts droplet formation in the model is shown to be dependent on the initialization of temperature, relative humidity, updraft velocity, aerosol size distribution, organic vapor concentration, and the volatility distribution. The predicted median enhancements in cloud droplet number concentration (CDNC) due to accounting for the co-condensation of water and organics fall on average between 16 % and 22 %. This corresponds to activating particles 10–16 nm smaller in dry diameter that would otherwise remain as interstitial aerosol. The highest CDNC enhancements (ΔCDNC) are predicted in the presence of a nascent ultrafine aerosol mode with a geometric mean diameter of ∼ 40 nm and no clear Hoppel minimum, indicative of pristine environments with a source of ultrafine particles (e.g., via new particle formation processes). Such aerosol size distributions are observed 30 %–40 % of the time in the studied boreal forest environment in spring and fall when new particle formation frequency is the highest. To evaluate the frequencies with which such distributions are experienced by an Earth system model over the whole boreal biome, 5 years of UK Earth System Model (UKESM1) simulations are further used. The frequencies are substantially lower than those observed at the boreal forest measurement site (< 6 % of the time), and the positive values, peaking in spring, are modeled only over Fennoscandia and the western parts of Siberia. Overall, the similarities in the size distributions between observed and modeled (UKESM1) are limited, which would limit the ability of this model, or any model with a similar aerosol representation, to project the climate relevance of co-condensation over the boreal forest. For the critical aerosol size distribution regime, ΔCDNC is shown to be sensitive to the concentrations of semi-volatile and some intermediate-volatility organic compounds (SVOCs and IVOCs), especially when the overall particle surface area is low. The magnitudes of ΔCDNC remain less affected by the more volatile vapors such as formic acid and extremely low- and low-volatility organic compounds (ELVOCs and LVOCs). The reasons for this are that most volatile organic vapors condense inefficiently due to their high volatility below the cloud base, and the concentrations of LVOCs and ELVOCs are too low to gain significant concentrations of soluble mass to reduce the critical supersaturations enough for droplet activation to occur. A reduction in the critical supersaturation caused by organic condensation emerges as the main driver of the modeled ΔCDNC. The results highlight the potential significance of co-condensation in pristine boreal environments close to sources of fresh ultrafine particles. For accurate predictions of co-condensation effects on CDNC, also in larger-scale models, an accurate representation of the aerosol size distribution is critical. Further studies targeted at finding observational evidence and constraints for co-condensation in the field are encouraged.
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| 3. |
- Huang, Wei, et al.
(författare)
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Potential pre-industrial–like new particle formation induced by pure biogenic organic vapors in Finnish peatland
- 2024
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Ingår i: Science Advances. - 2375-2548. ; 10:14
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Tidskriftsartikel (refereegranskat)abstract
- Pure biogenic new particle formation (NPF) induced by highly oxygenated organic molecules (HOMs) could be an important mechanism for pre-industrial aerosol formation. However, it has not been unambiguously confirmed in the ambient due to the scarcity of truly pristine continental locations in the present-day atmosphere or the lack of chemical characterization of NPF precursors. Here, we report ambient observations of pure biogenic HOM-driven NPF over a peatland in southern Finland. Meteorological decoupling processes formed an “air pocket” (i.e., a very shallow surface layer) at night and favored NPF initiated entirely by biogenic HOM from this peatland, whose atmospheric environment closely resembles that of the pre-industrial era. Our study sheds light on pre-industrial aerosol formation, which represents the baseline for estimating the impact of present and future aerosol on climate, as well as on future NPF, the features of which may revert toward pre-industrial–like conditions due to air pollution mitigation.
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| 4. |
- Stolzenburg, Dominik, et al.
(författare)
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Atmospheric nanoparticle growth
- 2023
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Ingår i: Reviews of Modern Physics. - 0034-6861 .- 1539-0756. ; 95:4
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Forskningsöversikt (refereegranskat)abstract
- New particle formation of liquid or solid nanoparticles from gas-phase precursors is a decisive process in Earth’s atmosphere and is considered one of the largest uncertainties in climate change predictions. Key for the climate relevance of new particle formation is the growth of freshly formed molecular clusters, as it determines the survival of these particles to cloud condensation nuclei sizes, where they can contribute to the aerosol-indirect effect. This review lays out the fundamental definitions of nanoparticle growth and addresses the rapidly emerging field of new particle formation studies with a focus on the diverse processes contributing to nanoparticle growth, explicitly comparing the latest experimental findings and their implementation in large-scale models. Atmospheric nanoparticle growth is a complex phenomenon including condensational and reactive vapor uptake, aerosol coagulation, and sink processes. It is linked to thermodynamics, cluster- and phase-transition physics. Nanoparticle growth rates measured from the evolution of the particle-size distribution describe growth as a collective phenomenon, while models often interpret them on a single-particle level and incorporate it into highly simplified size-distribution representations. Recent atmospheric observations show that sulfuric acid together with ammonia and amines, iodic acid, and oxidized organic species can contribute to nanoparticle growth, whereas most models describe the growth effects from a limited subset of this variety of condensable vapors. Atmospheric simulation chamber experiments have clarified the role of ions, intermolecular forces, the interplay of acids and bases, and the contribution of different types of organic vapors. Especially in the complex thermodynamics of organic vapor condensation, the field has had noteworthy advances over the last decade. While the experimental field has achieved significant progress in methodology and process level understanding, this has not led to a similar improvement in the description of the climate impact of nanoparticle formation in large-scale models. This review sets the basis to better align experimental and modeling studies on nanoparticle growth, giving specific guidance for future studies aiming to resolve the questions as to why the climate response in large-scale models seems to be buffered against high survival probabilities and why the global growth observations herein show surprisingly low variation.
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