| 1. |
- Ahlberg, Erik, et al.
(författare)
-
Effect of salt seed particle surface area, composition and phase on secondary organic aerosol mass yields in oxidation flow reactors
- 2019
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:4, s. 2701-2712
-
Tidskriftsartikel (refereegranskat)abstract
- Atmospheric particulate water is ubiquitous, affecting particle transport and uptake of gases. Yet, research on the effect of water on secondary organic aerosol (SOA) mass yields is not consistent. In this study, the SOA mass yields of an α-pinene and m-xylene mixture, at a concentration of 60 μgm-3, were examined using an oxidation flow reactor operated at a relative humidity (RH) of 60% and a residence time of 160 s. Wet or dried ammonium sulfate and ammonium nitrate seed particles were used. By varying the amount of seed particle surface area, the underestimation of SOA formation induced by the short residence time in flow reactors was confirmed. Starting at a SOA mass concentration of 5 μgm-3, the maximum yield increased by a factor of 2 with dry seed particles and on average a factor of 3.2 with wet seed particles. Hence, wet particles increased the SOA mass yield by 60% compared to the dry experiment. Maximum yield in the reactor was achieved using a surface area concentration of 1600 μm2 cm-3. This corresponded to a condensational lifetime of 20 s for low-volatility organics. The O V C ratio of SOA on wet ammonium sulfate was significantly higher than when using ammonium nitrate or dry ammonium sulfate seed particles, probably due to differences in heterogeneous chemistry.
|
|
| 2. |
- Ahlberg, Erik, et al.
(författare)
-
Measurement report : Black carbon properties and concentrations in southern Sweden urban and rural air-the importance of long-range transport
- 2023
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 23:5, s. 3051-3064
-
Tidskriftsartikel (refereegranskat)abstract
- Soot, or black carbon (BC), aerosol is a major climate forcer with severe health effects. The impacts depend strongly on particle number concentration, size and mixing state. This work reports on two field campaigns at nearby urban and rural sites, 65gkm apart, in southern Sweden during late summer 2018. BC was measured using a single-particle soot photometer (SP2) and Aethalometers (AE33). Differences in BC concentrations between the sites are driven primarily by local traffic emissions. Equivalent and refractory BC mass concentrations at the urban site were on average a factor 2.2 and 2.5, with peaks during rush hour up to a factor g1/44, higher than the rural background levels. The number fraction of particles containing a soot core was significantly higher in the city. BC particles at the urban site were on average smaller by mass and had less coating owing to fresh traffic emissions. The organic components of the fresh traffic plumes were similar in mass spectral signature to hydrocarbon-like organic aerosol (HOA), commonly associated with traffic. Despite the intense local traffic (g1/4g30g000 vehicles passing per day), PM1, including organic aerosol, was dominated by aged continental air masses even at the curbside site. The fraction of thickly coated particles at the urban site was highly correlated with the mass concentrations of all measured chemical species of PM1, consistent with aged, internally mixed aerosol. Trajectory analysis for the whole year showed that air masses arriving at the rural site from eastern Europe contained approximately double the amount of BC compared to air masses from western Europe. Furthermore, the largest regional emissions of BC transported to the rural site, from the Malmö-Copenhagen urban area, are discernible above background levels only when precipitation events are excluded. We show that continental Europe and not the Malmö-Copenhagen region is the major contributor to the background BC mass concentrations in southern Sweden.
|
|
| 3. |
- Ahlberg, Erik, et al.
(författare)
-
No particle mass enhancement from induced atmospheric ageing at a rural site in northern Europe
- 2019
-
Ingår i: Atmosphere. - : MDPI AG. - 2073-4433. ; 10:7
-
Tidskriftsartikel (refereegranskat)abstract
- A large portion of atmospheric aerosol particles consists of secondary material produced by oxidation reactions. The relative importance of secondary organic aerosol (SOA) can increase with improved emission regulations. A relatively simple way to study potential particle formation in the atmosphere is by using oxidation flow reactors (OFRs) which simulate atmospheric ageing. Here we report on the first ambient OFR ageing experiment in Europe, coupled with scanning mobility particle sizer (SMPS), aerosol mass spectrometer (AMS) and proton transfer reaction (PTR)-MS measurements. We found that the simulated ageing did not produce any measurable increases in particle mass or number concentrations during the two months of the campaign due to low concentrations of precursors. Losses in the reactor increased with hydroxyl radical (OH) exposure and with increasing difference between ambient and reactor temperatures, indicating fragmentation and evaporation of semivolatile material.
|
|
| 4. |
- Ahlberg, Erik, et al.
(författare)
-
Secondary organic aerosol from VOC mixtures in an oxidation flow reactor
- 2017
-
Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310. ; 161, s. 210-220
-
Tidskriftsartikel (refereegranskat)abstract
- The atmospheric organic aerosol is a tremendously complex system in terms of chemical content. Models generally treat the mixtures as ideal, something which has been questioned owing to model-measurement discrepancies. We used an oxidation flow reactor to produce secondary organic aerosol (SOA) mixtures containing oxidation products of biogenic (α-pinene, myrcene and isoprene) and anthropogenic (m-xylene) volatile organic compounds (VOCs). The resulting volume concentration and chemical composition was measured using a scanning mobility particle sizer (SMPS) and a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), respectively. The SOA mass yield of the mixtures was compared to a partitioning model constructed from single VOC experiments. The single VOC SOA mass yields with no wall-loss correction applied are comparable to previous experiments. In the mixtures containing myrcene a higher yield than expected was produced. We attribute this to an increased condensation sink, arising from myrcene producing a significantly higher number of nucleation particles compared to the other precursors. Isoprene did not produce much mass in single VOC experiments but contributed to the mass of the mixtures. The effect of high concentrations of isoprene on the OH exposure was found to be small, even at OH reactivities that previously have been reported to significantly suppress OH exposures in oxidation flow reactors. Furthermore, isoprene shifted the particle size distribution of mixtures towards larger sizes, which could be due to a change in oxidant dynamics inside the reactor.
|
|
| 5. |
- Ahlberg, Erik, et al.
(författare)
-
"Vi klimatforskare stödjer Greta och skolungdomarna"
- 2019
-
Ingår i: Dagens nyheter (DN debatt). - 1101-2447.
-
Tidskriftsartikel (populärvet., debatt m.m.)abstract
- DN DEBATT 15/3. Sedan industrialiseringens början har vi använt omkring fyra femtedelar av den mängd fossilt kol som får förbrännas för att vi ska klara Parisavtalet. Vi har bara en femtedel kvar och det är bråttom att kraftigt reducera utsläppen. Det har Greta Thunberg och de strejkande ungdomarna förstått. Därför stödjer vi deras krav, skriver 270 klimatforskare.
|
|
| 6. |
|
|
| 7. |
- Bianchi, Federico, et al.
(författare)
-
Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals : A Key Contributor to Atmospheric Aerosol
- 2019
-
Ingår i: Chemical Reviews. - : American Chemical Society (ACS). - 0009-2665 .- 1520-6890. ; 119:6, s. 3472-3509
-
Forskningsöversikt (refereegranskat)abstract
- Highly oxygenated organic molecules (HOM) are formed in the atmosphere via autoxidation involving peroxy radicals arising from volatile organic compounds (VOC). HOM condense on pre-existing particles and can be involved in new particle formation. HOM thus contribute to the formation of secondary organic aerosol (SOA), a significant and ubiquitous component of atmospheric aerosol known to affect the Earths radiation balance. HOM were discovered only very recently, but the interest in these compounds has grown rapidly. In this Review, we define HOM and describe the currently available techniques for their identification/quantification, followed by a summary of the current knowledge on their formation mechanisms and physicochemical properties. A main aim is to provide a common frame for the currently quite fragmented literature on HOM studies. Finally, we highlight the existing gaps in our understanding and suggest directions for future HOM research.
|
|
| 8. |
- Boy, M., et al.
(författare)
-
Interactions between the atmosphere, cryosphere, and ecosystems at northern high latitudes
- 2019
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:3, s. 2015-2061
-
Tidskriftsartikel (refereegranskat)abstract
- The Nordic Centre of Excellence CRAICC (Cryosphere-Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011-2016, is the largest joint Nordic research and innovation initiative to date, aiming to strengthen research and innovation regarding climate change issues in the Nordic region. CRAICC gathered more than 100 scientists from all Nordic countries in a virtual centre with the objectives of identifying and quantifying the major processes controlling Arctic warming and related feedback mechanisms, outlining strategies to mitigate Arctic warming, and developing Nordic Earth system modelling with a focus on short-lived climate forcers (SLCFs), including natural and anthropogenic aerosols. The outcome of CRAICC is reflected in more than 150 peer-reviewed scientific publications, most of which are in the CRAICC special issue of the journal Atmospheric Chemistry and Physics. This paper presents an overview of the main scientific topics investigated in the centre and provides the reader with a state-of-the-art comprehensive summary of what has been achieved in CRAICC with links to the particular publications for further detail. Faced with a vast amount of scientific discovery, we do not claim to completely summarize the results from CRAICC within this paper, but rather concentrate here on the main results which are related to feedback loops in climate change-cryosphere interactions that affect Arctic amplification.
|
|
| 9. |
- Boy, Michael, et al.
(författare)
-
Positive feedback mechanism between biogenic volatile organic compounds and the methane lifetime in future climates
- 2022
-
Ingår i: npj Climate and Atmospheric Science. - : Springer Science and Business Media LLC. - 2397-3722. ; 5:1
-
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.
|
|
| 10. |
|
|
| 11. |
- Chen, Dean, et al.
(författare)
-
A modelling study of OH, NO3 and H2SO4 in 2007- 2018 at SMEAR II, Finland : Analysis of long-term trends
- 2021
-
Ingår i: Environmental Science: Atmospheres. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 1:6, s. 449-472
-
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.
|
|
| 12. |
- Clusius, Petri, et al.
(författare)
-
Atmospherically Relevant Chemistry and Aerosol box model - ARCA box (version 1.2)
- 2022
-
Ingår i: Geoscientific Model Development. - : Copernicus GmbH. - 1991-959X .- 1991-9603. ; 15:18, s. 7257-7286
-
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.
|
|
| 13. |
- de Jonge, Robin Wollesen, et al.
(författare)
-
Natural Marine Precursors Boost Continental New Particle Formation and Production of Cloud Condensation Nuclei
- 2024
-
Ingår i: Environmental Science and Technology. - Malmö : IVL Svenska Miljöinstitutet. - 0013-936X .- 1520-5851. ; 58:25, s. 10956-10968
-
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.
|
|
| 14. |
- de Jonge, Robin Wollesen, et al.
(författare)
-
Natural Marine Precursors Boost Continental New Particle Formation and Production of Cloud Condensation Nuclei
- 2024
-
Ingår i: Environmental Science and Technology. - Malmö : IVL Svenska Miljöinstitutet. - 0013-936X .- 1520-5851. ; 58:25, s. 10956-10968
-
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.
|
|
| 15. |
- Du, Yaxing, et al.
(författare)
-
Large-eddy simulation of aerosol concentrations in a realistic urban environment : Model validation and transport mechanism
- 2024
-
Ingår i: Environmental Pollution. - Malmö : IVL Svenska Miljöinstitutet. - 0269-7491 .- 1873-6424. ; 358
-
Tidskriftsartikel (refereegranskat)abstract
- Air pollution in urban environments exhibits large spatial and temporal variations due to high heterogeneous air flow and emissions. To address the complexity of local air pollutant dynamics, a comprehensive large-eddy simulation using the PALM model system v6.0 was conducted. The distribution of flow and vehicle emitted aerosol particles in a realistic urban environment in Malmö, Sweden, was studied and evaluated against on-site measurements made using portable instrumentation on a spring morning in 2021. The canyon transport mechanisms were investigated, and the convective and turbulent mass-transport rates compared to clarify their role in aerosol transport. The horizontal distribution of aerosols showed acceptable evaluation metrics for both mass and number. Flow and pollutant concentrations were more complex than those in idealized street canyon networks. Vertical turbulent mass-transport rate was found to dominate the mass transport process compared with the convective transport rate, contributing more than 70% of the pollutant transport process. Our findings highlight the necessity of examining various aerosol metric due their distinct dispersion behaviour. This study introduces a comprehensive high-resolution modelling framework that accounts for dynamic meteorological and aerosol background boundary conditions, real-time traffic emission, and detailed building features, offering a robust toll for local urban air quality assessment.
|
|
| 16. |
- Eriksson, Axel, et al.
(författare)
-
Diesel soot aging in urban plumes within hours under cold dark and humid conditions
- 2017
-
Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322.
-
Tidskriftsartikel (refereegranskat)abstract
- Fresh and aged diesel soot particles have different impacts on climate and human health. While fresh diesel soot particles are highly aspherical and non-hygroscopic, aged particles are spherical and hygroscopic. Aging and its effect on water uptake also controls the dispersion of diesel soot in the atmosphere. Understanding the timescales on which diesel soot ages in the atmosphere is thus important, yet knowledge thereof is lacking. We show that under cold, dark and humid conditions the atmospheric transformation from fresh to aged soot occurs on a timescale of less than five hours. Under dry conditions in the laboratory, diesel soot transformation is much less efficient. While photochemistry drives soot aging, our data show it is not always a limiting factor. Field observations together with aerosol process model simulations show that the rapid ambient diesel soot aging in urban plumes is caused by coupled ammonium nitrate formation and water uptake.
|
|
| 17. |
|
|
| 18. |
|
|
| 19. |
- Gunthe, S. S., et al.
(författare)
-
Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity
- 2009
-
Ingår i: Atmospheric Chemistry and Physics. - 1680-7324. ; 9:19, s. 7551-7575
-
Tidskriftsartikel (refereegranskat)abstract
- Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. We have measured and characterized CCN at water vapor supersaturations in the range of S=0.10-0.82% in pristine tropical rainforest air during the AMAZE-08 campaign in central Amazonia. The effective hygroscopicity parameters describing the influence of chemical composition on the CCN activity of aerosol particles varied in the range of kappa approximate to 0.1-0.4 (0.16+/-0.06 arithmetic mean and standard deviation). The overall median value of kappa approximate to 0.15 was by a factor of two lower than the values typically observed for continental aerosols in other regions of the world. Aitken mode particles were less hygroscopic than accumulation mode particles (kappa approximate to 0.1 at D approximate to 50 nm; kappa approximate to 0.2 at D approximate to 200 nm), which is in agreement with earlier hygroscopicity tandem differential mobility analyzer (H-TDMA) studies. The CCN measurement results are consistent with aerosol mass spectrometry (AMS) data, showing that the organic mass fraction (f(org)) was on average as high as similar to 90% in the Aitken mode (D <= 100 nm) and decreased with increasing particle diameter in the accumulation mode (similar to 80% at D approximate to 200 nm). The kappa values exhibited a negative linear correlation with f(org) (R-2=0.81), and extrapolation yielded the following effective hygroscopicity parameters for organic and inorganic particle components: kappa(org)approximate to 0.1 which can be regarded as the effective hygroscopicity of biogenic secondary organic aerosol (SOA) and kappa(inorg)approximate to 0.6 which is characteristic for ammonium sulfate and related salts. Both the size dependence and the temporal variability of effective particle hygroscopicity could be parameterized as a function of AMS-based organic and inorganic mass fractions (kappa(p)=kappa(org) x f(org)+kappa(inorg) x f(inorg)). The CCN number concentrations predicted with kappa(p) were in fair agreement with the measurement results (similar to 20% average deviation). The median CCN number concentrations at S=0.1-0.82% ranged from N-CCN,N-0.10 approximate to 35 cm(-3) to N-CCN,N-0.82 approximate to 160 cm(-3), the median concentration of aerosol particles larger than 30 nm was N-CN,N-30 approximate to 200 cm(-3), and the corresponding integral CCN efficiencies were in the range of N-CCN,N-0.10/NCN,N-30 approximate to 0.1 to N-CCN,N-0.82/NCN,N-30 approximate to 0.8. Although the number concentrations and hygroscopicity parameters were much lower in pristine rainforest air, the integral CCN efficiencies observed were similar to those in highly polluted megacity air. Moreover, model calculations of N-CCN,N-S assuming an approximate global average value of kappa approximate to 0.3 for continental aerosols led to systematic overpredictions, but the average deviations exceeded similar to 50% only at low water vapor supersaturation (0.1%) and low particle number concentrations (<= 100 cm(-3)). Model calculations assuming aconstant aerosol size distribution led to higher average deviations at all investigated levels of supersaturation: similar to 60% for the campaign average distribution and similar to 1600% for a generic remote continental size distribution. These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators. Depending on the required and applicable level of detail, the information and parameterizations presented in this paper should enable efficient description of the CCN properties of pristine tropical rainforest aerosols of Amazonia in detailed process models as well as in large-scale atmospheric and climate models.
|
|
| 20. |
- Hao, Liqing, et al.
(författare)
-
Combined effects of boundary layer dynamics and atmospheric chemistry on aerosol composition during new particle formation periods
- 2018
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:23, s. 17705-17716
-
Tidskriftsartikel (refereegranskat)abstract
- Characterizing aerosol chemical composition in response to meteorological changes and atmospheric chemistry is important to gain insights into new particle formation mechanisms. A BAECC (Biogenic Aerosols - Effects on Clouds and Climate) campaign was conducted during the spring 2014 at the SMEAR II station (Station for Measuring Forest Ecosystem-Aerosol Relations) in Finland. The particles were characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). A PBL (planetary boundary layer) dilution model was developed to assist interpreting the measurement results. Right before nucleation events, the mass concentrations of organic and sulfate aerosol species were both decreased rapidly along with the growth of PBL heights. However, the mass fraction of sulfate aerosol of the total aerosol mass was increased, in contrast to a decrease for the organic mass fraction. Meanwhile, an increase in LVOOA (low-volatility oxygenated organic aerosol) mass fraction of the total organic mass was observed, in distinct comparison to a reduction of SVOOA (semi-volatile OOA) mass fraction. Our results demonstrate that, at the beginning of nucleation events, the observed sulfate aerosol mass was mainly driven by vertical turbulent mixing of sulfate-rich aerosols between the residual layer and the newly formed boundary layer, while the condensation of sulfuric acid (SA) played a minor role in interpreting the measured sulfate mass concentration. For the measured organic aerosols, their temporal profiles were mainly driven by dilution from PBL development, organic aerosol mixing in different boundary layers and/or partitioning of organic vapors, but accurate measurements of organic vapor concentrations and characterization on the spatial aerosol chemical composition are required. In general, the observed aerosol particles by AMS are subjected to joint effects of PBL dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During aerosol growth periods in the nighttime, the mass concentrations of organic aerosols and organic nitrate aerosols were both increased. The increase in SVOOA mass correlated well with the calculated increase in condensed HOMs' (highly oxygenated organic molecules) mass. To our knowledge, our results are the first atmospheric observations showing a connection between increase in SVOOA and condensed HOMs during the nighttime.
|
|
| 21. |
|
|
| 22. |
- Kalivitis, Nikos, et al.
(författare)
-
Formation and growth of atmospheric nanoparticles in the eastern Mediterranean : Results from long-term measurements and process simulations
- 2019
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:4, s. 2671-2686
-
Tidskriftsartikel (refereegranskat)abstract
- Atmospheric new particle formation (NPF) is a common phenomenon all over the world. In this study we present the longest time series of NPF records in the eastern Mediterranean region by analyzing 10 years of aerosol number size distribution data obtained with a mobility particle sizer. The measurements were performed at the Finokalia environmental research station on Crete, Greece, during the period June 2008-June 2018. We found that NPF took place on 27 % of the available days, undefined days were 23 % and non-event days 50 %. NPF is more frequent in April and May probably due to the terrestrial biogenic activity and is less frequent in August. Throughout the period under study, nucleation was observed also during the night. Nucleation mode particles had the highest concentration in winter and early spring, mainly because of the minimum sinks, and their average contribution to the total particle number concentration was 8 %. Nucleation mode particle concentrations were low outside periods of active NPF and growth, so there are hardly any other local sources of sub-25 nm particles. Additional atmospheric ion size distribution data simultaneously collected for more than 2 years were also analyzed. Classification of NPF events based on ion spectrometer measurements differed from the corresponding classification based on a mobility spectrometer, possibly indicating a different representation of local and regional NPF events between these two measurement data sets. We used the MALTE-Box model for simulating a case study of NPF in the eastern Mediterranean region. Monoterpenes contributing to NPF can explain a large fraction of the observed NPF events according to our model simulations. However the adjusted parameterization resulting from our sensitivity tests was significantly different from the initial one that had been determined for the boreal environment.
|
|
| 23. |
- Kivekäs, Niku, et al.
(författare)
-
Coupling an aerosol box model with one-dimensional flow : A tool for understanding observations of new particle formation events
- 2016
-
Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 1600-0889 .- 0280-6509. ; 68:1
-
Tidskriftsartikel (refereegranskat)abstract
- Field observations of new particle formation and the subsequent particle growth are typically only possible at a fixed measurement location, and hence do not follow the temporal evolution of an air parcel in a Lagrangian sense. Standard analysis for determining formation and growth rates requires that the time-dependent formation rate and growth rate of the particles are spatially invariant; air parcel advection means that the observed temporal evolution of the particle size distribution at a fixed measurement location may not represent the true evolution if there are spatial variations in the formation and growth rates. Here we present a zerodimensional aerosol box model coupled with one-dimensional atmospheric flow to describe the impact of advection on the evolution of simulated new particle formation events. Wind speed, particle formation rates and growth rates are input parameters that can vary as a function of time and location, using wind speed to connect location to time. The output simulates measurements at a fixed location; formation and growth rates of the particle mode can then be calculated from the simulated observations at a stationary point for different scenarios and be compared with the 'true' input parameters. Hence, we can investigate how spatial variations in the formation and growth rates of new particles would appear in observations of particle number size distributions at a fixed measurement site. We show that the particle size distribution and growth rate at a fixed location is dependent on the formation and growth parameters upwind, even if local conditions do not vary. We also show that different input parameters used may result in very similar simulated measurements. Erroneous interpretation of observations in terms of particle formation and growth rates, and the time span and areal extent of new particle formation, is possible if the spatial effects are not accounted for.
|
|
| 24. |
|
|
| 25. |
- Kurppa, Mona, et al.
(författare)
-
Implementation of the sectional aerosol module SALSA2.0 into the PALM model system 6.0 : Model development and first evaluation
- 2019
-
Ingår i: Geoscientific Model Development. - : Copernicus GmbH. - 1991-959X .- 1991-9603. ; 12:4, s. 1403-1422
-
Tidskriftsartikel (refereegranskat)abstract
- Urban pedestrian-level air quality is a result of an interplay between turbulent dispersion conditions, background concentrations, and heterogeneous local emissions of air pollutants and their transformation processes. Still, the complexity of these interactions cannot be resolved by the commonly used air quality models. By embedding the sectional aerosol module SALSA2.0 into the large-eddy simulation model PALM, a novel, high-resolution, urban aerosol modelling framework has been developed. The first model evaluation study on the vertical variation of aerosol number concentration and size distribution in a simple street canyon without vegetation in Cambridge, UK, shows good agreement with measurements, with simulated values mainly within a factor of 2 of observations. Dispersion conditions and local emissions govern the pedestrian-level aerosol number concentrations. Out of different aerosol processes, dry deposition is shown to decrease the total number concentration by over 20 %, while condensation and dissolutional increase the total mass by over 10 %. Following the model development, the application of PALM can be extended to local- and neighbourhood-scale air pollution and aerosol studies that require a detailed solution of the ambient flow field.
|
|
