| 1. |
- Boy, Michael, et al.
(författare)
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Positive feedback mechanism between biogenic volatile organic compounds and the methane lifetime in future climates
- 2022
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Ingår i: npj Climate and Atmospheric Science. - : Springer Science and Business Media LLC. - 2397-3722. ; 5:1
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Tidskriftsartikel (refereegranskat)abstract
- A multitude of biogeochemical feedback mechanisms govern the climate sensitivity of Earth in response to radiation balance perturbations. One feedback mechanism, which remained missing from most current Earth System Models applied to predict future climate change in IPCC AR6, is the impact of higher temperatures on the emissions of biogenic volatile organic compounds (BVOCs), and their subsequent effects on the hydroxyl radical (OH) concentrations. OH, in turn, is the main sink term for many gaseous compounds including methane, which is the second most important human-influenced greenhouse gas in terms of climate forcing. In this study, we investigate the impact of this feedback mechanism by applying two models, a one-dimensional chemistry-transport model, and a global chemistry-transport model. The results indicate that in a 6 K temperature increase scenario, the BVOC-OH-CH4 feedback increases the lifetime of methane by 11.4% locally over the boreal region when the temperature rise only affects chemical reaction rates, and not both, chemistry and BVOC emissions. This would lead to a local increase in radiative forcing through methane (ΔRFCH4) of approximately 0.013 Wm−2 per year, which is 2.1% of the current ΔRFCH4. In the whole Northern hemisphere, we predict an increase in the concentration of methane by 0.024% per year comparing simulations with temperature increase only in the chemistry or temperature increase in chemistry and BVOC emissions. This equals approximately 7% of the annual growth rate of methane during the years 2008–2017 (6.6 ± 0.3 ppb yr−1) and leads to an ΔRFCH4 of 1.9 mWm−2 per year.
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| 2. |
- Chen, Dean, et al.
(författare)
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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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Ingår i: Environmental Science: Atmospheres. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 1:6, s. 449-472
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Tidskriftsartikel (refereegranskat)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. |
- Clusius, Petri, et al.
(författare)
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Atmospherically Relevant Chemistry and Aerosol box model - ARCA box (version 1.2)
- 2022
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Ingår i: Geoscientific Model Development. - : Copernicus GmbH. - 1991-959X .- 1991-9603. ; 15:18, s. 7257-7286
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Tidskriftsartikel (refereegranskat)abstract
- We introduce the Atmospherically Relevant Chemistry and Aerosol box model ARCA box (v.1.2.2). It is a zero-dimensional process model with a focus on atmospheric chemistry and submicron aerosol processes, including cluster formation. A novel feature in the model is its comprehensive graphical user interface, allowing for detailed configuration and documentation of the simulation settings, flexible model input, and output visualization. Additionally, the graphical interface contains tools for module customization and input data acquisition. These properties - customizability, ease of implementation and repeatability - make ARCA an invaluable tool for any atmospheric scientist who needs a view on the complex atmospheric aerosol processes. ARCA is based on previous models (MALTE-BOX, ADiC and ADCHEM), but the code has been fully rewritten and reviewed. The gas-phase chemistry module incorporates the Master Chemical Mechanism (MCMv3.3.1) and Peroxy Radical Autoxidation Mechanism (PRAM) but can use any compatible chemistry scheme. ARCA's aerosol module couples the ACDC (Atmospheric Cluster Dynamics Code) in its particle formation module, and the discrete particle size representation includes the fully stationary and fixed-grid moving average methods. ARCA calculates the gas-particle partitioning of low-volatility organic vapours for any number of compounds included in the chemistry, as well as the Brownian coagulation of the particles. The model has parametrizations for vapour and particle wall losses but accepts user-supplied time- and size-resolved input. ARCA is written in Fortran and Python (user interface and supplementary tools), can be installed on any of the three major operating systems and is licensed under GPLv3.
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| 4. |
- de Jonge, Robin Wollesen, et al.
(författare)
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Natural Marine Precursors Boost Continental New Particle Formation and Production of Cloud Condensation Nuclei
- 2024
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Ingår i: Environmental Science and Technology. - Malmö : IVL Svenska Miljöinstitutet. - 0013-936X .- 1520-5851. ; 58:25, s. 10956-10968
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Tidskriftsartikel (refereegranskat)abstract
- Marine dimethyl sulfide (DMS) emissions are the dominant source of natural sulfur in the atmosphere. DMS oxidizes to produce low-volatility acids that potentially nucleate to form particles that may grow into climatically important cloud condensation nuclei (CCN). In this work, we utilize the chemistry transport model ADCHEM to demonstrate that DMS emissions are likely to contribute to the majority of CCN during the biological active period (May-August) at three different forest stations in the Nordic countries. DMS increases CCN concentrations by forming nucleation and Aitken mode particles over the ocean and land, which eventually grow into the accumulation mode by condensation of low-volatility organic compounds from continental vegetation. Our findings provide a new understanding of the exchange of marine precursors between the ocean and land, highlighting their influence as one of the dominant sources of CCN particles over the boreal forest.
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| 5. |
- de Jonge, Robin Wollesen, et al.
(författare)
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Natural Marine Precursors Boost Continental New Particle Formation and Production of Cloud Condensation Nuclei
- 2024
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Ingår i: Environmental Science and Technology. - Malmö : IVL Svenska Miljöinstitutet. - 0013-936X .- 1520-5851. ; 58:25, s. 10956-10968
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Tidskriftsartikel (refereegranskat)abstract
- Marine dimethyl sulfide (DMS) emissions are the dominant source of natural sulfur in the atmosphere. DMS oxidizes to produce low-volatility acids that potentially nucleate to form particles that may grow into climatically important cloud condensation nuclei (CCN). In this work, we utilize the chemistry transport model ADCHEM to demonstrate that DMS emissions are likely to contribute to the majority of CCN during the biological active period (May-August) at three different forest stations in the Nordic countries. DMS increases CCN concentrations by forming nucleation and Aitken mode particles over the ocean and land, which eventually grow into the accumulation mode by condensation of low-volatility organic compounds from continental vegetation. Our findings provide a new understanding of the exchange of marine precursors between the ocean and land, highlighting their influence as one of the dominant sources of CCN particles over the boreal forest.
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| 6. |
- Foreback, Benjamin, et al.
(författare)
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A new implementation of FLEXPART with Enviro-HIRLAM meteorological input, and a case study during a heavy air pollution event
- 2024
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Ingår i: Big Earth Data. - 2096-4471 .- 2574-5417.
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Tidskriftsartikel (refereegranskat)abstract
- We integrated Enviro-HIRLAM (Environment-High Resolution Limited Area Model) meteorological output into FLEXPART (FLEXible PARTicle dispersion model). A FLEXPART simulation requires meteorological input from a numerical weather prediction (NWP) model. The publicly available version of FLEXPART can utilize either ECMWF (European Centre for Medium-range Weather Forecasts) Integrated Forecast System (IFS) forecast or reanalysis NWP data, or NCEP (U.S. National Center for Environmental Prediction) Global Forecast System (GFS) forecast or reanalysis NWP data. The primary benefits of using Enviro-HIRLAM are that it runs at a higher resolution and accounts for aerosol effects in meteorological fields. We compared backward trajectories generated with FLEXPART using Enviro-HIRLAM (both with and without aerosol effects) to trajectories generated using NCEP GFS and ECMWF IFS meteorological inputs, for a case study of a heavy haze event which occurred in Beijing, China in November 2018. We found that results from FLEXPART were considerably different when using different meteorological inputs. When aerosol effects were included in the NWP, there was a small but noticeable difference in calculated trajectories. Moreover, when looking at potential emission sensitivity instead of simply expressing trajectories as lines, additional information, which may have been missed when looking only at trajectories as lines, can be inferred.
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| 7. |
- Pichelstorfer, Lukas, et al.
(författare)
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Towards automated inclusion of autoxidation chemistry in models: from precursors to atmospheric implications
- 2024
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Ingår i: Environmental Science. - Malmö : IVL Svenska Miljöinstitutet. - 2634-3606. ; 4:8, s. 879-896
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Tidskriftsartikel (refereegranskat)abstract
- In the last few decades, atmospheric formation of secondary organic aerosols (SOA) has gained increasing attention due to their impact on air quality and climate. However, methods to predict their abundance are mainly empirical and may fail under real atmospheric conditions. In this work, a close-to-mechanistic approach allowing SOA quantification is presented, with a focus on a chainlike chemical reaction called “autoxidation”. A novel framework is employed to (a) describe the gasphase chemistry, (b) predict the products' molecular structures and (c) explore the contribution of autoxidation chemistry on SOA formation under various conditions. As a proof of concept, the method is applied to benzene, an important anthropogenic SOA precursor. Our results suggest autoxidation to explain up to 100% of the benzene-SOA formed under low-NOx laboratory conditions. Under atmospheric-like day-time conditions, the calculated benzene-aerosol mass continuously forms, as expected based on prior work. Additionally, a prompt increase, driven by the NO3 radical, is predicted by the model at dawn. This increase has not yet been explored experimentally and stresses the potential for atmospheric SOA formation via secondary oxidation of benzene by O3 and NO3.
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| 8. |
- Roldin, Pontus, et al.
(författare)
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The role of highly oxygenated organic molecules in the Boreal aerosol-cloud-climate system
- 2019
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 10, s. 1-15
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Tidskriftsartikel (refereegranskat)abstract
- Over Boreal regions, monoterpenes emitted from the forest are the main precursors for secondary organic aerosol (SOA) formation and the primary driver of the growth of new aerosol particles to climatically important cloud condensation nuclei (CCN). Autoxidation of monoterpenes leads to rapid formation of Highly Oxygenated organic Molecules (HOM). We have developed the first model with near-explicit representation of atmospheric new particle formation (NPF) and HOM formation. The model can reproduce the observed NPF, HOM gas-phase composition and SOA formation over the Boreal forest. During the spring, HOM SOA formation increases the CCN concentration by ~10 % and causes a direct aerosol radiative forcing of −0.10 W/m2. In contrast, NPF reduces the number of CCN at updraft velocities < 0.2 m/s, and causes a direct aerosol radiative forcing of +0.15 W/m2. Hence, while HOM SOA contributes to climate cooling, NPF can result in climate warming over the Boreal forest.
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| 9. |
- Thakur, Roseline C., et al.
(författare)
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An evaluation of new particle formation events in Helsinki during a Baltic Sea cyanobacterial summer bloom
- 2022
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:9, s. 6365-6391
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Tidskriftsartikel (refereegranskat)abstract
- Several studies have investigated new particle formation (NPF) events from various sites ranging from pristine locations, including forest sites, to urban areas. However, there is still a dearth of studies investigating NPF processes and subsequent aerosol growth in coastal yet semi-urban sites, where the tropospheric layer is a concoction of biogenic and anthropogenic gases and particles. The investigation of factors leading to NPF becomes extremely complex due to the highly dynamic meteorological conditions at the coastline especially when combined with both continental and oceanic weather conditions. Herein, we engage in a comprehensive study of particle number size distributions and aerosol-forming precursor vapors at the coastal semi-urban site in Helsinki, Finland. The measurement period, 25 June-18 August 2019, was timed with the recurring cyanobacterial summer bloom in the Baltic Sea region and coastal regions of Finland. Our study recorded several regional/local NPF and aerosol burst events during this period. Although the overall anthropogenic influence on sulfuric acid (SA) concentrations was low during the measurement period, we observed that the regional or local NPF events, characterized by SA concentrations on the order of 10(7) molec. cm(-3), occurred mostly when the air mass traveled over the land areas. Interestingly, when the air mass traveled over the Baltic Sea, an area enriched with algae and cyanobacterial blooms, high iodic acid (IA) concentration coincided with an aerosol burst or a spike event at the measurement site. Further, SA-rich bursts were seen when the air mass traveled over the Gulf of Bothnia, enriched with cyanobacterial blooms. The two most important factors affecting aerosol precursor vapor concentrations, and thus the aerosol formation, were speculated to be (1) the type of phytoplankton species and intensity of bloom present in the coastal regions of Finland and the Baltic Sea and (2) the wind direction. During the events, most of the growth of sub-3 nm particles was probably due to SA, rather than IA or methane sulfonic acid (MSA); however much of the particle growth remained unexplained indicative of the strong role of organics in the growth of particles, especially in the 3-7 nm particle size range. Further studies are needed to explore the role of organics in NPF events and the potential influence of cyanobacterial blooms in coastal locations.
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| 10. |
- Xavier, Carlton, et al.
(författare)
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Aerosol mass yields of selected biogenic volatile organic compounds - A theoretical study with nearly explicit gas-phase chemistry
- 2019
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:22, s. 13741-13758
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Tidskriftsartikel (refereegranskat)abstract
- In this study we modeled secondary organic aerosol (SOA) mass loadings from the oxidation (by O3, OH and NO3) of five representative biogenic volatile organic compounds (BVOCs): isoprene, endocyclic bond-containing monoterpenes (α-pinene and limonene), exocyclic double-bond compound (β-pinene) and a sesquiterpene (β-caryophyllene). The simulations were designed to replicate an idealized smog chamber and oxidative flow reactors (OFRs). The Master Chemical Mechanism (MCM) together with the peroxy radical autoxidation mechanism (PRAM) were used to simulate the gas-phase chemistry. The aim of this study was to compare the potency of MCM and MCM + PRAM in predicting SOA formation. SOA yields were in good agreement with experimental values for chamber simulations when MCM + PRAM was applied, while a stand-alone MCM underpredicted the SOA yields. Compared to experimental yields, the OFR simulations using MCM + PRAM yields were in good agreement for BVOCs oxidized by both O3 and OH. On the other hand, a stand-alone MCM underpredicted the SOA mass yields. SOA yields increased with decreasing temperatures and NO concentrations and vice versa. This highlights the limitations posed when using fixed SOA yields in a majority of global and regional models. Few compounds that play a crucial role (>95 % of mass load) in contributing to SOA mass increase (using MCM + PRAM) are identified. The results further emphasized that incorporating PRAM in conjunction with MCM does improve SOA mass yield estimation..
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