| 321. |
- McCusker, Gillian Young, et al.
(author)
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Evaluating Arctic clouds modelled with the Unified Model and Integrated Forecasting System
- 2023
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In: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 23:8, s. 4819-4847
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Journal article (peer-reviewed)abstract
- By synthesising remote-sensing measurements made in the central Arctic into a model-gridded Cloudnet cloud product, we evaluate how well the Met Office Unified Model (UM) and the European Centre for Medium-Range Weather Forecasting (ECMWF) Integrated Forecasting System (IFS) capture Arctic clouds and their associated interactions with the surface energy balance and the thermodynamic structure of the lower troposphere. This evaluation was conducted using a 4-week observation period from the Arctic Ocean 2018 expedition, where the transition from sea ice melting to freezing conditions was measured. Three different cloud schemes were tested within a nested limited-area model (LAM) configuration of the UM – two regionally operational single-moment schemes (UM_RA2M and UM_RA2T) and one novel double-moment scheme (UM_CASIM-100) – while one global simulation was conducted with the IFS, utilising its default cloud scheme (ECMWF_IFS).Consistent weaknesses were identified across both models, with both the UM and IFS overestimating cloud occurrence below 3 km. This overestimation was also consistent across the three cloud configurations used within the UM framework, with >90 % mean cloud occurrence simulated between 0.15 and 1 km in all the model simulations. However, the cloud microphysical structure, on average, was modelled reasonably well in each simulation, with the cloud liquid water content (LWC) and ice water content (IWC) comparing well with observations over much of the vertical profile. The key microphysical discrepancy between the models and observations was in the LWC between 1 and 3 km, where most simulations (all except UM_RA2T) overestimated the observed LWC.Despite this reasonable performance in cloud physical structure, both models failed to adequately capture cloud-free episodes: this consistency in cloud cover likely contributes to the ever-present near-surface temperature bias in every simulation. Both models also consistently exhibited temperature and moisture biases below 3 km, with particularly strong cold biases coinciding with the overabundant modelled cloud layers. These biases are likely due to too much cloud-top radiative cooling from these persistent modelled cloud layers and were consistent across the three UM configurations tested, despite differences in their parameterisations of cloud on a sub-grid scale. Alarmingly, our findings suggest that these biases in the regional model were inherited from the global model, driving a cause–effect relationship between the excessive low-altitude cloudiness and the coincident cold bias. Using representative cloud condensation nuclei concentrations in our double-moment UM configuration while improving cloud microphysical structure does little to alleviate these biases; therefore, no matter how comprehensive we make the cloud physics in the nested LAM configuration used here, its cloud and thermodynamic structure will continue to be overwhelmingly biased by the meteorological conditions of its driving model.
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| 322. |
- McMeeking, G. R., et al.
(author)
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Black carbon measurements in the boundary layer over western and northern Europe
- 2010
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 10:19, s. 9393-9414
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Journal article (peer-reviewed)abstract
- Europe is a densely populated region that is a significant global source of black carbon (BC) aerosol, but there is a lack of information regarding the physical properties and spatial/vertical distribution of rBC in the region. We present the first aircraft observations of sub-micron refractory BC (rBC) aerosol concentrations and physical properties measured by a single particle soot photometer (SP2) in the lower troposphere over Europe. The observations spanned a region roughly bounded by 50 degrees to 60 degrees N and from 15 degrees W to 30 degrees E. The measurements, made between April and September 2008, showed that average rBC mass concentrations ranged from about 300 ng m(-3) near urban areas to approximately 50 ng m(-3) in remote continental regions, lower than previous surface-based measurements. rBC represented between 0.5 and 3% of the sub-micron aerosol mass. Black carbon mass size distributions were log-normally distributed and peaked at approximately 180 nm, but shifted to smaller diameters (similar to 160 nm) near source regions. rBC was correlated with carbon monoxide (CO) but had different ratios to CO depending on location and air mass. Light absorption coefficients were measured by particle soot absorption photometers on two separate aircraft and showed similar geographic patterns to rBC mass measured by the SP2. We summarize the rBC and light absorption measurements as a function of longitude and air mass age and also provide profiles of rBC mass concentrations and size distribution statistics. Our results will help evaluate model-predicted regional rBC concentrations and properties and determine regional and global climate impacts from rBC due to atmospheric heating and surface dimming.
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| 323. |
- Megner, Linda, et al.
(author)
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Comparison of retrieved noctilucent cloud particle properties from Odin tomography scans and model simulations
- 2016
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:23, s. 15135-15146
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Journal article (peer-reviewed)abstract
- Mesospheric ice particles, known as noctilucent clouds or polar mesospheric clouds, have long been observed by rocket instruments, satellites and ground-based remote sensing, while models have been used to simulate ice particle growth and cloud properties. However, the fact that different measurement techniques are sensitive to different parts of the ice particle distribution makes it difficult to compare retrieved parameters such as ice particle radius or ice concentration from different experiments. In this work we investigate the accuracy of satellite retrieval based on scattered light and how this affects derived cloud properties. We apply the retrieval algorithm on spectral signals calculated from modelled cloud distributions and compare the results to the properties of the original distributions. We find that ice mass density is accurately retrieved whereas mean radius is often overestimated and high ice concentrations are generally underestimated. The reason is partly that measurements based on scattered light are insensitive to the smaller particles and partly that the retrieval algorithm assumes a Gaussian size distribution. Once we know the limits of the satellite retrieval we proceed to compare the properties retrieved from the modelled cloud distributions to those observed by the Optical, Spectroscopic, and Infrared Remote Imaging System (OSIRIS) instrument on the Odin satellite. We find that a model with a stationary atmosphere, as given by average atmospheric conditions, does not yield cloud properties that are in agreement with the observations, whereas a model with realistic temperature and vertical wind variations does. This indicates that average atmospheric conditions are insufficient to understand the process of noctilucent cloud growth and that a realistic atmospheric variability is crucial for cloud formation and growth. Further, the agreement between results from the model, when set up with a realistically variable atmosphere, and the observations suggests that our understanding of the growth process itself is reasonable.
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| 324. |
- Mehra, Archit, et al.
(author)
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Evaluation of the chemical composition of gas- and particle-phase products of aromatic oxidation
- 2020
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In: ATMOSPHERIC CHEMISTRY AND PHYSICS. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:16, s. 9783-9803
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Journal article (peer-reviewed)abstract
- Aromatic volatile organic compounds (VOCs) are key anthropogenic pollutants emitted to the atmosphere and are important for both ozone and secondary organic aerosol (SOA) formation in urban areas. Recent studies have indicated that aromatic hydrocarbons may follow previously unknown oxidation chemistry pathways, including autoxidation that can lead to the formation of highly oxidised products. In this study we evaluate the gas- and particle-phase ions measured by online mass spectrometry during the hydroxyl radical oxidation of substituted C-9-aromatic isomers (1,3,5-trimethylbenzene, 1,2,4-trimethylbenzene, propylbenzene and isopropylbenzene) and a substituted polyaromatic hydrocarbon (1-methylnaphthalene) under low- and medium-NO x conditions. A time-of-flight chemical ionisation mass spectrometer (ToF-CIMS) with iodide-anion ionisation was used with a filter inlet for gases and aerosols (FIGAERO) for the detection of products in the particle phase, while a Vocus protontransfer-reaction mass spectrometer (Vocus-PTR-MS) was used for the detection of products in the gas phase. The signal of product ions observed in the mass spectra were compared for the different precursors and experimental conditions. The majority of mass spectral product signal in both the gas and particle phases comes from ions which are common to all precursors, though signal distributions are distinct for different VOCs. Gas- and particle-phase composition are distinct from one another. Ions corresponding to products contained in the near-explicit gas phase Master Chemical Mechanism (MCM version 3.3.1) are utilised as a benchmark of current scientific understanding, and a comparison of these with observations shows that the MCM is missing a range of highly oxidised products from its mechanism. In the particle phase, the bulk of the product signal from all precursors comes from ring scission ions, a large proportion of which are more oxidised than previously reported and have undergone further oxidation to form highly oxygenated organic molecules (HOMs). Under the perturbation of OH oxidation with increased NOx, the contribution of HOM-ion signals to the particle-phase signal remains elevated for more substituted aromatic precursors. Up to 43% of product signal comes from ring-retaining ions including HOMs; this is most important for the more substituted aromatics. Unique products are a minor component in these systems, and many of the dominant ions have ion formulae concurrent with other systems, highlighting the challenges in utilising marker ions for SOA.
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| 325. |
- Miao, J., et al.
(author)
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The potential of polarization measurements from space at mm and sub-mm wavelengths for determining cirrus cloud parameters
- 2003
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 3:1, s. 39-48
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Journal article (peer-reviewed)abstract
- The millimeter and sub-millimeter waves have been attracting a lot of attention recently in the cloud remote sensing community. This is largely because of their potential use in measuring cirrus cloud parameters with airborne or space-borne radiometers. In this study, we examine the possibility of using polarization measurements in this frequency range to get information on the microphysical properties of cirrus clouds. By using a simple radiative transfer model, we calculated the brightness temperature differences at the vertical and horizontal polarization channels for the following seven frequencies: 90, 157, 220, 340, 463, 683, and 874 GHz. The ice crystals in cirrus clouds are modeled with nearly spherical particles, circular cylinder, and circular plate, as well as with mixtures of these types. We found that the polarization difference signal shows a unique "resonance'' feature with the change of ice particle characteristic size: it has a strong response only in a certain range of ice particle size, beyond that range it approaches zero. The size range where this resonance happens depends to a large extent on particle shape and aspect ratio, but to a much less extent on particle orientation. This resonance feature appears even when ice clouds are composed of a mixture of ice crystals in different shapes, although the magnitude and the position of the resonance peak may change, depending on how the mixture is made. Oriented particles generally show larger polarization difference than randomly oriented ones, and plates have larger polarization difference than cylinders. However, the state of particle orientation has a significantly stronger effect on the polarization difference than the particle shape (cylinder or plate). This makes it difficult to distinguish particle shapes using millimeter and sub-millimeter radiometric measurements, if there is no information available on particle orientations. However, if the state of particle shape mixture can be predetermined by other approaches, polarization measurements can help to determine ice particle characteristic size and orientation. This information, in turn, will benefit our retrieval of the ice water path of cirrus clouds.
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| 326. |
- Mihalikova, Maria, et al.
(author)
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Vertical mixing in the lower troposphere by mountain waves over Arctic Scandinavia
- 2011
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11, s. 31475-31493
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Journal article (peer-reviewed)abstract
- Measurements made by ozonesondes and by a 52 MHz wind-profiling radar during February and March 1997 are studied. The radar is located at Esrange, near Kiruna in Arctic Sweden, on the eastern flank of the Scandinavian mountains. Daily ozonesondes were launched from the same site. The radar vertical and horizontal wind measurements are used to identify times when mountain waves were present. Mean vertical gradients in ozone mixing ratio in the lower troposphere are determined in conditions with mountain waves present and when they were absent. Back-trajectories were calculated so that only air-masses with their origin to the west of the mountains were included in the final averages. The vertical gradient in ozone mixing ratio is found to be about twice as steep outside wave conditions as it is during mountain waves. This suggests a very high rate of vertical mixing, with an average eddy diffusivity of order 5000 m2 s−1. This is consistent with an earlier estimate of the occurrence rate of complete mixing by wave breaking over the mountain range.
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| 327. |
- Modak, Angshuman, 1987-, et al.
(author)
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Better-constrained climate sensitivity when accounting for dataset dependency on pattern effect estimates
- 2023
-
In: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 23:13, s. 7535-7549
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Journal article (peer-reviewed)abstract
- The best estimate of equilibrium climate sensitivity (ECS) constrained based on the instrumental record of historical warming becomes coherent with other lines of evidence when the dependence of radiative feedback on the pattern of surface temperature change (pattern effect) is incorporated. Pattern effect strength is usually estimated with atmosphere-only model simulations forced with observed historical sea-surface temperature (SST) and sea-ice change and constant pre-industrial forcing. However, recent studies indicate that pattern effect estimates depend on the choice of SST boundary condition dataset, due to differences in the measurement sources and the techniques used to merge and construct them. Here, we systematically explore this dataset dependency by applying seven different observed SST datasets to the MPI-ESM1.2-LR model covering 1871–2017. We find that the pattern effect ranges from -0.01±0.09 to 0.42±0.10 W m−2 K−1 (standard error), whereby the commonly used Atmospheric Model Intercomparison Project II (AMIPII) dataset produces by far the largest estimate. When accounting for the generally weaker pattern effect in MPI-ESM1.2-LR compared to other models, as well as dataset dependency and intermodel spread, we obtain a combined pattern effect estimate of 0.37 W m−2 K−1 [−0.14 to 0.88 W m−2 K−1] (5th–95th percentiles) and a resulting instrumental record ECS estimate of 3.2 K [1.8 to 11.0 K], which as a result of the weaker pattern effect is slightly lower and better constrained than in previous studies.
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| 328. |
- Moldanova, Jana, et al.
(author)
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Resonance-Enhanced Detection of Metals in Aerosols using Single Particle Mass Spectrometry
- 2020
-
In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:12, s. 7139-7152
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Journal article (peer-reviewed)abstract
- We describe resonance effects in laser desorption–ionization (LDI) of particles that substantially increase the sensitivity and selectivity to metals in single-particle mass spectrometry (SPMS). Within the proposed scenario, resonant light absorption by ablated metal atoms increases their ionization rate within a single laser pulse. By choosing the appropriate laser wavelength, the key micronutrients Fe, Zn and Mn can be detected on individual aerosol particles with considerably improved efficiency. These ionization enhancements for metals apply to natural dust and anthropogenic aerosols, both important sources of bioavailable metals to marine environments. Transferring the results into applications, we show that the spectrum of our KrF-excimer laser is in resonance with a major absorption line of iron atoms. To estimate the impact of resonant LDI on the metal detection efficiency in SPMS applications, we performed a field experiment on ambient air with two alternately firing excimer lasers of different wavelengths. Herein, resonant LDI with the KrF-excimer laser (248.3 nm) revealed iron signatures for many more particles of the same aerosol ensemble compared to the more common ArF-excimer laser line of 193.3 nm (nonresonant LDI of iron). Many of the particles that showed iron contents upon resonant LDI were mixtures of sea salt and organic carbon. For nonresonant ionization, iron was exclusively detected in particles with a soot contribution. This suggests that resonant LDI allows a more universal and secure metal detection in SPMS. Moreover, our field study indicates relevant atmospheric iron transport by mixed organic particles, a pathway that might be underestimated in SPMS measurements based on nonresonant LDI. Our findings show a way to improve the detection and source attribution capabilities of SPMS for particle-bound metals, a health-relevant aerosol component and an important source of micronutrients to the surface oceans affecting marine primary productivity.
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| 329. |
- Moldanova, Jana, et al.
(author)
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The impact of ship emissions on air quality and human health in the Gothenburg area – Part I: 2012 emissions
- 2020
-
In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20, s. 7509 – 7530-
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Journal article (peer-reviewed)abstract
- Ship emissions in and around ports are of interest for urban air quality management in many harbour cities. We investigated the impact of regional and local ship emissions on urban air quality for 2012 conditions in the city of Gothenburg, Sweden, the largest cargo port in Scandinavia. In order to assess the effects of ship emissions, a coupled regional- and local-scale model system has been set up using ship emissions in the Baltic Sea and the North Sea as well as in and around the port of Gothenburg. Ship emissions were calculated with the Ship Traffic Emission Assessment Model (STEAM), taking into account individual vessel characteristics and vessel activity data. The calculated contributions from local and regional shipping to local air pollution in Gothenburg were found to be substantial, especially in areas around the city ports. The relative contribution from local shipping to annual mean NO2 concentrations was 14 % as the model domain average, while the relative contribution from regional shipping in the North Sea and the Baltic Sea was 26 %. In an area close to the city terminals, the contribution of NO2 from local shipping (33 %) was higher than that of road traffic (28 %), which indicates the importance of controlling local shipping emissions. Local shipping emissions of NOx led to a decrease in the summer mean O3 levels in the city by 0.5 ppb (∼2 %) on average. Regional shipping led to a slight increase in O3 concentrations; however, the overall effect of regional and the local shipping together was a small decrease in the summer mean O3 concentrations in the city. In addition, volatile organic compound (VOC) emissions from local shipping compensate up to 4 ppb of the decrease in summer O3 concentrations due to the NO titration effect. For particulate matter with a median aerodynamic diameter less than or equal to 2.5 µm (PM2.5), local ship emissions contributed only 3 % to the annual mean in the model domain, while regional shipping under 2012 conditions was a larger contributor, with an annual mean contribution of 11 % of the city domain average. Based on the modelled local and regional shipping contributions, the health effects of PM2.5, NO2 and ozone were assessed using the ALPHA-RiskPoll (ARP) model. An effect of the shipping-associated PM2.5 exposure in the modelled area was a mean decrease in the life expectancy by 0.015 years per person. The relative contribution of local shipping to the impact of total PM2.5 was 2.2 %, which can be compared to the 5.3 % contribution from local road traffic. The relative contribution of the regional shipping was 10.3 %. The mortalities due to the exposure to NO2 associated with shipping were calculated to be 2.6 premature deaths yr−1. The relative contribution of local and regional shipping to the total exposure to NO2 in the reference simulation was 14 % and 21 %, respectively. The shipping-related ozone exposures were due to the NO titration effect leading to a negative number of premature deaths. Our study shows that overall health impacts of regional shipping can be more significant than those of local shipping, emphasizing that abatement policy options on city-scale air pollution require close cooperation across governance levels. Our findings indicate that the strengthened Sulphur Emission Control Areas (SECAs) fuel sulphur limit from 1 % to 0.1 % in 2015, leading to a strong decrease in the formation of secondary particulate matter on a regional scale was an important step in improving the air quality in the city.
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| 330. |
- Moldanova, Jana, et al.
(author)
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The impact of ship emissions on air quality and human health in the Gothenburg area – Part II: Scenarios for 2040
- 2020
-
In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:10, s. 667-10686
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Journal article (peer-reviewed)abstract
- Shipping is an important source of air pollutants, from the global to the local scale. Ships emit substantial amounts of sulfur dioxides, nitrogen dioxides, and particulate matter in the vicinity of coasts, threatening the health of the coastal population, especially in harbour cities. Reductions in emissions due to shipping have been targeted by several regulations. Nevertheless, effects of these regulations come into force with temporal delays, global ship traffic is expected to grow in the future, and other land-based anthropogenic emissions might decrease. Thus, it is necessary to investigate combined impacts to identify the impact of shipping activities on air quality, population exposure, and health effects in the future. We investigated the future effect of shipping emissions on air quality and related health effects considering different scenarios of the development of shipping under current regional trends of economic growth and already decided regulations in the Gothenburg urban area in 2040. Additionally, we investigated the impact of a large-scale implementation of shore electricity in the Port of Gothenburg. For this purpose, we established a one-way nested chemistry transport modelling (CTM) system from the global to the urban scale, to calculate pollutant concentrations, population-weighted concentrations, and health effects related to NO2, PM2.5, and O3. The simulated concentrations of NO2 and PM2.5 in future scenarios for the year 2040 are in general very low with up to 4 ppb for NO2 and up to 3.5 µg m−3 PM2.5 in the urban areas which are not close to the port area. From 2012 the simulated overall exposure to PM2.5 decreased by approximately 30 % in simulated future scenarios; for NO2 the decrease was over 60 %. The simulated concentrations of O3 increased from the year 2012 to 2040 by about 20 %. In general, the contributions of local shipping emissions in 2040 focus on the harbour area but to some extent also influence the rest of the city domain. The simulated impact of onshore electricity implementation for shipping in 2040 shows reductions for NO2 in the port of up to 30 %, while increasing O3 of up to 3 %. Implementation of onshore electricity for ships at berth leads to additional local reduction potentials of up to 3 % for PM2.5 and 12 % for SO2 in the port area. All future scenarios show substantial decreases in population-weighted exposure and health-effect impacts.
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