| 11. |
- Baró Pérez, Alejandro, et al.
(författare)
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Comparing the simulated influence of biomass burning plumes on low-level clouds over the southeastern Atlantic under varying smoke conditions
- 2024
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Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 24:8, s. 4591-4610
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Tidskriftsartikel (refereegranskat)abstract
- Biomass burning plumes are frequently transported over the southeast Atlantic (SEA) stratocumulus deck during the southern African fire season (June-October). The plumes bring large amounts of absorbing aerosols and enhanced moisture, which can trigger a rich set of aerosol-cloud-radiation interactions with climatic consequences that are still poorly understood. We use large-eddy simulation (LES) to explore and disentangle the individual impacts of aerosols and moisture on the underlying stratocumulus clouds, the marine boundary layer (MBL) evolution, and the stratocumulus-to-cumulus transition (SCT) for three different meteorological situations over the southeast Atlantic during August 2017. For all three cases, our LES shows that the SCT is driven by increased sea surface temperatures and cloud-top entrainment as the air is advected towards the Equator. In the LES model, aerosol indirect effects, including impacts on drizzle production, have a small influence on the modeled cloud evolution and SCT, even when aerosol concentrations are lowered to background concentrations. In contrast, local semi-direct effects, i.e., aerosol absorption of solar radiation in the MBL, cause a reduction in cloud cover that can lead to a speed-up of the SCT, in particular during the daytime and during broken cloud conditions, especially in highly polluted situations. The largest impact on the radiative budget comes from aerosol impacts on cloud albedo: the plume with absorbing aerosols produces a total average 3 d of simulations. We find that the moisture accompanying the aerosol plume produces an additional cooling effect that is about as large as the total aerosol radiative effect. Overall, there is still a large uncertainty associated with the radiative and cloud evolution effects of biomass burning aerosols. A comparison between different models in a common framework, combined with constraints from in situ observations, could help to reduce the uncertainty.
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| 12. |
- Baró Pérez, Alejandro, et al.
(författare)
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Impact of smoke and non-smoke aerosols on radiation and low-level clouds over the southeast Atlantic from co-located satellite observations
- 2021
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:8, s. 6053-6077
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Tidskriftsartikel (refereegranskat)abstract
- Data derived from instruments on board the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) and CloudSat satellites as well as meteorological parameters from reanalysis are used to explore situations when moist aerosol layers overlie stratocumulus clouds over the southeast Atlantic during the biomass burning season (June to October). To separate and quantify the impacts of aerosol loading, aerosol type, and humidity on the radiative fluxes (including cloud top cooling), the data are split into different levels of aerosol and moisture loadings. The aerosol classification available from the CALIPSO products is used to compare and contrast situations with pristine air, with smoke, and with other (non-smoke) types of aerosols. A substantial number of cases with non-smoke aerosols above clouds are found to occur under similar meteorological conditions to the smoke cases. In contrast, the meteorology is substantially different for the pristine situations, making a direct comparison with the aerosol cases ambiguous. The moisture content is enhanced within the aerosol layers, but the relative humidity does not always increase monotonously with increasing optical depth. Shortwave (SW) heating rates within the moist aerosol plumes increase with increasing aerosol loading and are higher in the smoke cases compared to the non-smoke cases. However, there is no clear correlation between moisture changes and SW absorption. Cloud top cooling rates do not show a clear correlation with moisture within the overlying aerosol layers due to the strong variability of the cooling rates caused by other meteorological factors (most notably cloud top temperature). No clear influence of aerosol type or loading on cloud top cooling rates is detected. Further, there is no correlation between aerosol loading and the thermodynamic structure of the atmosphere nor the cloud top height.
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| 13. |
- Bell, David M., et al.
(författare)
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Particle-phase processing of α-pinene NO3 secondary organic aerosol in the dark
- 2022
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Ingår i: Atmospheric Chemistry and Physics. - 1680-7316 .- 1680-7324. ; 22, s. 13167-13182
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Tidskriftsartikel (refereegranskat)abstract
- The NO3 radical represents a significant nighttime oxidant which is present downstream of polluted environments. Existing studies have investigated the formation of secondary organic aerosol (SOA) from NO3 radicals, focusing on the yields, general composition, and hydrolysis of organonitrates; however, there is limited knowledge about how the composition of NO3-derived SOA evolves as a result of particle-phase reactions. Here, SOA was formed from the reaction of α-pinene with NO3 radicals generated from N2O5, and the resulting SOA was aged in the dark. The initial composition of NO3-derived α-pinene SOA was slightly dependent upon the concentration of N2O5 injected (excess of NO3 or excess of α-pinene) but was largely dominated by dimer dinitrates (C20H32N2O8-13). Oxidation reactions (e.g., C20H32N2O8 → C20H32N2O9 → C20H32N2O10) accounted for 60 %-70 % of the particle-phase reactions observed. Fragmentation reactions and dimer degradation pathways made up the remainder of the particle-phase processes occurring. The exact oxidant is not known, although suggestions are offered (e.g., N2O5, organic peroxides, or peroxynitrates). Hydrolysis of -ONO2 functional groups was not an important loss term during dark aging under the relative humidity conditions of our experiments (58 %-62 %), and changes in the bulk organonitrate composition were likely driven by evaporation of highly nitrogenated molecules. Overall, 25 %-30 % of the particle-phase composition changes as a function of particle-phase reactions during dark aging, representing an important atmospheric aging pathway.
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| 14. |
- Bell, David M., et al.
(författare)
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Particle-phase processing of α-pinene NO3 secondary organic aerosol in the dark
- 2022
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:19, s. 13167-13182
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Tidskriftsartikel (refereegranskat)abstract
- The NO3 radical represents a significant night-time oxidant present in or downstream of polluted environments. There are studies that investigated the formation of secondary organic aerosol (SOA) from NO3 radicals focusing on yields, general composition, and hydrolysis of organonitrates. However, there is limited knowledge about how the composition of NO3-derived SOA evolves as a result of particle phase reactions. Here, SOA was formed from the reaction of α-pinene with NO3 radicals generated from N2O5, and the resulting SOA aged in the absence of external stimuli. The initial composition of NO3-derived α-pinene SOA was slightly dependent upon the concentration of N2O5 injected (excess of NO3 or excess of α-pinene), but was largely dominated by dimer dinitrates (C20H32N2O8-13). Oxidation reactions (e.g. C20H32N2O8 → C20H32N2O9 → C20H32N2O10 etc...) accounted for 60–70 % of the particle phase reactions observed. Fragmentation reactions and dimer degradation pathways made up the remainder of the particle-phase processes occurring. The exact oxidant is not known, though suggestions are offered (e.g. N2O5, organic peroxides, or peroxy-nitrates). Hydrolysis of −ONO2 functional groups was not an important loss term during dark aging under the relative humidity conditions of our experiments (58–62 %), and changes in the bulk organonitrate composition were likely driven by evaporation of highly nitrogenated molecules. Overall, 25–30 % of the particle-phase composition changes as a function of particle-phase reactions during dark aging representing an important atmospheric aging pathway.
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| 15. |
- Berchet, Antoine, et al.
(författare)
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Using ship-borne observations of methane isotopic ratio in the Arctic Ocean to understand methane sources in the Arctic
- 2020
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:6, s. 3987-3998
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Tidskriftsartikel (refereegranskat)abstract
- Characterizing methane sources in the Arctic remains challenging due to the remoteness, heterogeneity and variety of such emissions. In situ campaigns provide valuable datasets to reduce these uncertainties. Here we analyse data from the summer 2014 SWERUS-C3 campaign in the eastern Arctic Ocean, off the shore of Siberia and Alaska. Total concentrations of methane, as well as relative concentrations of (CH4)-C-12 and (CH4)-C-13, were measured continuously during this campaign for 35 d in July and August. Using a chemistry-transport model, we link observed concentrations and isotopic ratios to regional emissions and hemispheric transport structures. A simple inversion system helped constrain source signatures from wetlands in Siberia and Alaska, and oceanic sources, as well as the isotopic composition of lower-stratosphere air masses. The variation in the signature of lower-stratosphere air masses, due to strongly fractionating chemical reactions in the stratosphere, was suggested to explain a large share of the observed variability in isotopic ratios. These results point towards necessary efforts to better simulate large-scale transport and chemistry patterns to make relevant use of isotopic data in remote areas. It is also found that constant and homogeneous source signatures for each type of emission in a given region (mostly wetlands and oil and gas industry in our case at high latitudes) are not compatible with the strong synoptic isotopic signal observed in the Arctic. A regional gradient in source signatures is highlighted between Siberian and Alaskan wetlands, the latter having lighter signatures (more depleted in C-13). Finally, our results suggest that marine emissions of methane from Arctic continental-shelf sources are dominated by thermogenicorigin methane, with a secondary biogenic source as well.
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| 16. |
- Bergamaschi, Peter, et al.
(författare)
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High-resolution inverse modelling of European CH4emissions using the novel FLEXPART-COSMO TM5 4DVAR inverse modelling system
- 2022
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:20, s. 13243-13268
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Tidskriftsartikel (refereegranskat)abstract
- We present a novel high-resolution inverse modelling system ("FLEXVAR") based on FLEXPARTCOSMO back trajectories driven by COSMO meteorological fields at 7 km×7 km resolution over the European COSMO-7 domain and the four-dimensional variational (4DVAR) data assimilation technique. FLEXVAR is coupled offline with the global inverse modelling system TM5-4DVAR to provide background mole fractions ("baselines") consistent with the global observations assimilated in TM5-4DVAR. We have applied the FLEXVAR system for the inverse modelling of European CH4 emissions in 2018 using 24 stations with in situ measurements, complemented with data from five stations with discrete air sampling (and additional stations outside the European COSMO-7 domain used for the global TM5-4DVAR inversions). The sensitivity of the FLEXVAR inversions to different approaches to calculate the baselines, different parameterizations of the model representation error, different settings of the prior error covariance parameters, different prior inventories, and different observation data sets are investigated in detail. Furthermore, the FLEXVAR inversions are compared to inversions with the FLEXPART extended Kalman filter ("FLExKF") system and with TM5-4DVAR inversions at 1° × 1° resolution over Europe. The three inverse modelling systems show overall good consistency of the major spatial patterns of the derived inversion increments and in general only relatively small differences in the derived annual total emissions of larger country regions. At the same time, the FLEXVAR inversions at 7 km × 7 km resolution allow the observations to be better reproduced than the TM5-4DVAR simulations at 1° × 1°. The three inverse models derive higher annual total CH4 emissions in 2018 for Germany, France, and BENELUX compared to the sum of anthropogenic emissions reported to UNFCCC and natural emissions estimated from the Global Carbon Project CH4 inventory, but the uncertainty ranges of top-down and bottom-up total emission estimates overlap for all three country regions. In contrast, the top-down estimates for the sum of emissions from the UK and Ireland agree relatively well with the total of anthropogenic and natural bottom-up inventories.
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| 17. |
- Bibi, Z., et al.
(författare)
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Technical note: A new approach to discriminate different black carbon sources by utilising fullerene and metals in positive matrix factorisation analysis of high-resolution soot particle aerosol mass spectrometer data
- 2021
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:13, s. 10763-10777
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Tidskriftsartikel (refereegranskat)abstract
- Atmospheric aerosol particles are known to have detrimental effects on human health and climate. Black carbon is an important constituent of atmospheric aerosol particulate matter (PM), emitted from incomplete combustion. Source apportionment of BC is very important, to evaluate the influence of different sources. The high-resolution soot particle aerosol mass spectrometer (HR-SP-AMS) instrument uses a laser vaporiser, which allows the real-time detection and characterisation of refractory black carbon (rBC) and its internally mixed particles such as metals, coating species, and rBC subcomponents in the form of HOAĝ€¯+ĝ€¯fullerene. In this case study, the soot data were collected by using HR-SP-AMS during Guy Fawkes Night on 5 November 2014. Positive matrix factorisation was applied to positively discriminate between different wood-burning and bonfire sources for the first time, which no existing black carbon source apportionment technique is currently able to do. Along with this, the use of the fullerene signals in differentiating between soot sources and the use of metals as a tracer for fireworks has also been investigated, which did not significantly contribute to the rBC concentrations. The addition of fullerene signals and successful positive matrix factorisation (PMF) application to HR-SP-AMS data apportioned rBC into more than two sources. These bonfire sources are HOAĝ€¯+ĝ€¯fullerene, biomass burning organic aerosol, more oxidised oxygenated organic aerosol (MO-OOA), and non-bonfire sources such as hydrocarbon-like OA and domestic burning. The result of correlation analysis between HR-SP-AMS data and previously published Aethalometer, MAAP, and CIMS data provides an effective way of gaining insights into the relationships between the variables and provide a quantitative estimate of the source contributions to the BC budget during this period. This research study is an important demonstration of using HR-SP-AMS for the purpose of BC source apportionment. © 2021 Zainab Bibi et al.
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| 18. |
- Blichner, Sara Marie, et al.
(författare)
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Reduced effective radiative forcing from cloud-aerosol interactions (ERFaci) with improved treatment of early aerosol growth in an Earth system model
- 2021
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:23, s. 17243-17265
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Tidskriftsartikel (refereegranskat)abstract
- Historically, aerosols of anthropogenic origin have offset some of the warming from increased atmospheric greenhouse gas concentrations. The strength of this negative aerosol forcing, however, is highly uncertain-especially the part originating from cloud-aerosol interactions. An important part of this uncertainty originates from our lack of knowledge about pre-industrial aerosols and how many of these would have acted as cloud condensation nuclei (CCN). In order to simulate CCN concentrations in models, we must adequately model secondary aerosols, including new particle formation (NPF) and early growth, which contributes a large part of atmospheric CCN. In this study, we investigate the effective radiative forcing (ERF) from cloud-aerosol interactions (ERFaci) with an improved treatment of early particle growth, as presented in . We compare the improved scheme to the default scheme, OsloAero, which are both embedded in the atmospheric component of the Norwegian Earth System Model v2 (NorESM2). The improved scheme, OsloAeroSec, includes a sectional scheme that treats the growth of particles from 5-39.6ĝ€¯nm in diameter, which thereafter inputs the particles to the smallest mode in the pre-existing modal aerosol scheme. The default scheme parameterizes the growth of particles from nucleation up to the smallest mode, a process that can take several hours. The explicit treatment of early growth in OsloAeroSec, on the other hand, captures the changes in atmospheric conditions during this growth time in terms of air mass mixing, transport, and condensation and coagulation. We find that the ERFaci with the sectional scheme is-1.16ĝ€¯Wm-2, which is 0.13ĝ€¯Wm-2 weaker compared to the default scheme. This reduction originates from OsloAeroSec producing more particles than the default scheme in pristine, low-aerosol-concentration areas and fewer NPF particles in high-aerosol areas. We find, perhaps surprisingly, that NPF inhibits cloud droplet activation in polluted and/or high-aerosol-concentration regions because the NPF particles increase the condensation sink and reduce the growth of the larger particles which may otherwise activate. This means that in these high-aerosol regions, the model with the lowest NPF-OsloAeroSec-will have the highest cloud droplet activation and thus more reflective clouds. In pristine and/or low-aerosol regions, however, NPF enhances cloud droplet activation because the NPF particles themselves tend to activate. Lastly, we find that sulfate emissions in the present-day simulations increase the hygroscopicity of secondary aerosols compared to pre-industrial simulations. This makes NPF particles more relevant for cloud droplet activation in the present day than the pre-industrial atmosphere because increased hygroscopicity means they can activate at smaller sizes.
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| 19. |
- Boyer, Matthew, et al.
(författare)
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A full year of aerosol size distribution data from the central Arctic under an extreme positive Arctic Oscillation : insights from the Multidisciplinarydrifting Observatory for the Study of Arctic Climate (MOSAiC) expedition
- 2023
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 23:1, s. 389-415
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Tidskriftsartikel (refereegranskat)abstract
- The Arctic environment is rapidly changing due to accelerated warming in the region. The warming trend is driving a decline in sea ice extent, which thereby enhances feedback loops in the surface energy budget in the Arctic. Arctic aerosols play an important role in the radiative balance and hence the climate response in the region, yet direct observations of aerosols over the Arctic Ocean are limited. In this study, we investigate the annual cycle in the aerosol particle number size distribution (PNSD), particle number concentration (PNC), and black carbon (BC) mass concentration in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. This is the first continuous, year-long data set of aerosol PNSD ever collected over the sea ice in the central Arctic Ocean. We use a k-means cluster analysis, FLEXPART simulations, and inverse modeling to evaluate seasonal patterns and the influence of different source regions on the Arctic aerosol population. Furthermore, we compare the aerosol observations to land-based sites across the Arctic, using both long-term measurements and observations during the year of the MOSAiC expedition (2019–2020), to investigate interannual variability and to give context to the aerosol characteristics from within the central Arctic. Our analysis identifies that, overall, the central Arctic exhibits typical seasonal patterns of aerosols, including anthropogenic influence from Arctic haze in winter and secondary aerosol processes in summer. The seasonal pattern corresponds to the global radiation, surface air temperature, and timing of sea ice melting/freezing, which drive changes in transport patterns and secondary aerosol processes. In winter, the Norilsk region in Russia/Siberia was the dominant source of Arctic haze signals in the PNSD and BC observations, which contributed to higher accumulation-mode PNC and BC mass concentrations in the central Arctic than at land-based observatories. We also show that the wintertime Arctic Oscillation (AO) phenomenon, which was reported to achieve a record-breaking positive phase during January–March 2020, explains the unusual timing and magnitude of Arctic haze across the Arctic region compared to longer-term observations. In summer, the aerosol PNCs of the nucleation and Aitken modes are enhanced; however, concentrations were notably lower in the central Arctic over the ice pack than at land-based sites further south. The analysis presented herein provides a current snapshot of Arctic aerosol processes in an environment that is characterized by rapid changes, which will be crucial for improving climate model predictions, understanding linkages between different environmental processes, and investigating the impacts of climate change in future Arctic aerosol studies.
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| 20. |
- Brasseur, Z., et al.
(författare)
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Measurement report: Introduction to the HyICE-2018 campaign for measurements of ice-nucleating particles and instrument inter-comparison in the Hyytiala boreal forest
- 2022
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:8, s. 5117-5145
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Tidskriftsartikel (refereegranskat)abstract
- The formation of ice particles in Earth's atmosphere strongly influences the dynamics and optical properties of clouds and their impacts on the climate system. Ice formation in clouds is often triggered heterogeneously by ice-nucleating particles (INPs) that represent a very low number of particles in the atmosphere. To date, many sources of INPs, such as mineral and soil dust, have been investigated and identified in the low and mid latitudes. Although less is known about the sources of ice nucleation at high latitudes, efforts have been made to identify the sources of INPs in the Arctic and boreal environments. In this study, we investigate the INP emission potential from high-latitude boreal forests in the mixed-phase cloud regime. We introduce the HyICE-2018 measurement campaign conducted in the boreal forest of Hyytiala, Finland, between February and June 2018. The campaign utilized the infrastructure of the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR) II, with additional INP instruments, including the Portable Ice Nucleation Chamber I and II (PINC and PINCii), the SPectrometer for Ice Nuclei (SPIN), the Portable Ice Nucleation Experiment (PINE), the Ice Nucleation SpEctrometer of the Karlsruhe Institute of Technology (INSEKT) and the Microlitre Nucleation by Immersed Particle Instrument (mu L-NIPI), used to quantify the INP concentrations and sources in the boreal environment. In this contribution, we describe the measurement infrastructure and operating procedures during HyICE-2018, and we report results from specific time periods where INP instruments were run in parallel for inter-comparison purposes. Our results show that the suite of instruments deployed during HyICE-2018 reports consistent results and therefore lays the foundation for forthcoming results to be considered holistically. In addition, we compare measured INP concentrations to INP parameterizations, and we observe good agreement with the Tobo et al. (2013) parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA.
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