| 11. |
- Ball, William T., et al.
(författare)
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Reconciling differences in stratospheric ozone composites
- 2017
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:20, s. 12269-12302
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Tidskriftsartikel (refereegranskat)abstract
- Observations of stratospheric ozone from multiple instruments now span three decades; combining these into composite datasets allows long-term ozone trends to be estimated. Recently, several ozone composites have been published, but trends disagree by latitude and altitude, even between composites built upon the same instrument data. We confirm that the main causes of differences in decadal trend estimates lie in (i) steps in the composite time series when the instrument source data changes and (ii) artificial sub-decadal trends in the underlying instrument data. These artefacts introduce features that can alias with regressors in multiple linear regression (MLR) analysis; both can lead to inaccurate trend estimates. Here, we aim to remove these artefacts using Bayesian methods to infer the underlying ozone time series from a set of composites by building a joint-likelihood function using a Gaussian-mixture density to model outliers introduced by data artefacts, together with a data-driven prior on ozone variability that incorporates knowledge of problems during instrument operation. We apply this Bayesian self-calibration approach to stratospheric ozone in 10 degrees bands from 60 degrees S to 60 degrees N and from 46 to 1 hPa (similar to 21-48 km) for 1985-2012. There are two main outcomes: (i) we independently identify and confirm many of the data problems previously identified, but which remain unaccounted for in existing composites; (ii) we construct an ozone composite, with uncertainties, that is free from most of these problems - we call this the BAyeSian Integrated and Consolidated (BASIC) composite. To analyse the new BASIC composite, we use dynamical linear modelling (DLM), which provides a more robust estimate of long-term changes through Bayesian inference than MLR. BASIC and DLM, together, provide a step forward in improving estimates of decadal trends. Our results indicate a significant recovery of ozone since 1998 in the upper stratosphere, of both northern and southern midlatitudes, in all four composites analysed, and particularly in the BASIC composite. The BASIC results also show no hemispheric difference in the recovery at midlatitudes, in contrast to an apparent feature that is present, but not consistent, in the four composites. Our overall conclusion is that it is possible to effectively combine different ozone composites and account for artefacts and drifts, and that this leads to a clear and significant result that upper stratospheric ozone levels have increased since 1998, following an earlier decline.
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| 12. |
- Ball, William T., et al.
(författare)
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Stratospheric ozone trends for 1985-2018 : sensitivity to recent large variability
- 2019
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:19, s. 12731-12748
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Tidskriftsartikel (refereegranskat)abstract
- The Montreal Protocol, and its subsequent amendments, has successfully prevented catastrophic losses of stratospheric ozone, and signs of recovery are now evident. Nevertheless, recent work has suggested that ozone in the lower stratosphere (< 24 km) continued to decline over the 1998-2016 period, offsetting recovery at higher altitudes and preventing a statistically significant increase in quasi-global (60 degrees S-60 degrees N) total column ozone. In 2017, a large lower stratospheric ozone resurgence over less than 12 months was estimated (using a chemistry transport model; CTM) to have offset the long-term decline in the quasi-global integrated lower stratospheric ozone column. Here, we extend the analysis of space-based ozone observations to December 2018 using the BASIC(SG) ozone composite. We find that the observed 2017 resurgence was only around half that modelled by the CTM, was of comparable magnitude to other strong interannual changes in the past, and was restricted to Southern Hemisphere (SH) midlatitudes (60-30 degrees S). In the SH midlatitude lower stratosphere, the data suggest that by the end of 2018 ozone is still likely lower than in 1998 (probability similar to 80 %). In contrast, tropical and Northern Hemisphere (NH) ozone continue to display ongoing decreases, exceeding 90 % probability. Robust tropical (> 95 %, 30 degrees S-30 degrees N) decreases dominate the quasi-global integrated decrease (99 % probability); the integrated tropical stratospheric column (1-100 hPa, 30 degrees S-30 degrees N) displays a significant overall ozone decrease, with 95 % probability. These decreases do not reveal an inefficacy of the Montreal Protocol; rather, they suggest that other effects are at work, mainly dynamical variability on long or short timescales, counteracting the positive effects of the Montreal Protocol on stratospheric ozone recovery. We demonstrate that large interannual midlatitude (30-60 degrees) variations, such as the 2017 resurgence, are driven by non-linear quasi-biennial oscillation (QBO) phase-dependent seasonal variability. However, this variability is not represented in current regression analyses. To understand if observed lower stratospheric ozone decreases are a transient or long-term phenomenon, progress needs to be made in accounting for this dynamically driven variability.
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| 13. |
- Beecken, Jörg, 1982, et al.
(författare)
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Emission factors of SO2, NOx and particles from ships in Neva Bay from ground-based and helicopter-borne measurements and AIS-based modeling
- 2015
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:9, s. 5229-5241
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Tidskriftsartikel (refereegranskat)abstract
- Emission factors of SO2, NOx and size-distributed particle numbers were measured for approximately 300 different ships in the Gulf of Finland and Neva Bay area during two campaigns in August/September 2011 and June/July 2012. The measurements were carried out from a harbor vessel and from an Mi-8 helicopter downwind of passing ships. Other measurements were carried out from shore sites near the island of Kronstadt and along the Neva River in the urban area of Saint Petersburg. Most ships were running at reduced speed (10 kn), i.e., not at their optimal load. Vessels for domestic and international shipping were monitored. It was seen that the distribution of the SO2 emission factors is bi-modal, with averages of 4.6 and 18.2 gSO(2) kg(fuel)(-1) for the lower and the higher mode, respectively. The emission factors show compliance with the 1% fuel sulfur content Sulfur Emission Control Areas (SECA) limit for 90% of the vessels in 2011 and 97% in 2012. The distribution of the NOx emission factor is mono-modal, with an average of 58 gNO(x) kg(fuel)(-1). The corresponding emission related to the generated power yields an average of 12.1 gNO(x) kWh(-1). The distribution of the emission factors for particulate number shows that nearly 90% of all particles in the 5.6 nm to 10 mu m size range were below 70 nm in diameter. The distribution of the corresponding emission factors for the mass indicates two separated main modes, one for particles between 30 and 300 nm and the other for above 2 mu m. The average particle emission factors were found to be in the range from 0.7 to 2.7 x 10(16) particles kg(fuel)(-1) and 0.2 to 3.4 gPM kg(fuel)(-1), respectively. The NOx and particulate emissions are comparable with other studies. The measured emission factors were compared, for individual ships, to modeled ones using the Ship Traffic Emission Assessment Model (STEAM) of the Finnish Meteorological Institute. A reasonably good agreement for gaseous sulfur and nitrogen emissions can be seen for ships in international traffic, but significant deviations are found for inland vessels. Regarding particulate mass, the values of the modeled data are about 2-3 times higher than the measured results, which probably reflects the assumptions made in the modeled fuel sulfur content. The sulfur contents in the fuel retrieved from the measurements were lower than the previously used assumptions by the City of Saint Petersburg when carrying out atmospheric modeling, and using these measurements it was possible to better assess the impact of shipping on air quality.
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| 14. |
- Berthet, Gwenaël, et al.
(författare)
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Impact of a moderate volcanic eruption on chemistry in the lower stratosphere : balloon-borne observations and model calculations
- 2017
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:3, s. 2229-2253
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Tidskriftsartikel (refereegranskat)abstract
- The major volcanic eruption of Mount Pinatubo in 1991 has been shown to have significant effects on stratospheric chemistry and ozone depletion even at midlatitudes. Since then, only moderate but recurrent volcanic eruptions have modulated the stratospheric aerosol loading and are assumed to be one cause for the reported increase in the global aerosol content over the past 15 years. This particularly enhanced aerosol context raises questions about the effects on stratospheric chemistry which depend on the latitude, altitude and season of injection. In this study, we focus on the midlatitude Sarychev volcano eruption in June 2009, which injected 0.9 Tg of sulfur dioxide (about 20 times less than Pinatubo) into a lower stratosphere mainly governed by high-stratospheric temperatures. Together with in situ measurements of aerosol amounts, we analyse high-resolution in situ and/or remote-sensing observations of NO2, HNO3 and BrO from balloon-borne infrared and UV-visible spectrometers launched in Sweden in August-September 2009. It is shown that differences between observations and three-dimensional (3-D) chemistry-transport model (CTM) outputs are not due to transport calculation issues but rather reflect the chemical impact of the volcanic plume below 19 km altitude. Good measurement-model agreement is obtained when the CTM is driven by volcanic aerosol loadings derived from in situ or space-borne data. As a result of enhanced N2O5 hydrolysis in the Sarychev volcanic aerosol conditions, the model calculates reductions of similar to 45% and increases of similar to 11% in NO2 and HNO3 amounts respectively over the August-September 2009 period. The decrease in NOx abundances is limited due to the expected saturation effect for high aerosol loadings. The links between the various chemical catalytic cycles involving chlorine, bromine, nitrogen and HOx compounds in the lower stratosphere are discussed. The increased BrO amounts (similar to 22 %) compare rather well with the balloon-borne observations when volcanic aerosol levels are accounted for in the CTM and appear to be mainly controlled by the coupling with nitrogen chemistry rather than by enhanced BrONO2 hydrolysis. We show that the chlorine partitioning is significantly controlled by enhanced BrONO2 hydrolysis. However, simulated effects of the Sarychev eruption on chlorine activation are very limited in the high-temperature conditions in the stratosphere in the period considered, inhibiting the effect of ClONO2 hydrolysis. As a consequence, the simulated chemical ozone loss due to the Sarychev aerosols is low with a reduction of -22 ppbv (-1.5 %) of the ozone budget around 16 km. This is at least 10 times lower than the maximum ozone depletion from chemical processes (up to -20 %) reported in the Northern Hemisphere lower stratosphere over the first year following the Pinatubo eruption. This study suggests that moderate volcanic eruptions have limited chemical effects when occurring at midlatitudes (restricted residence times) and outside winter periods (high-temperature conditions). However, it would be of interest to investigate longer-lasting tropical volcanic plumes or sulfur injections in the wintertime low-temperature conditions.
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| 15. |
- Bidleman, Terry Frank, et al.
(författare)
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Annual cycles of organochlorine pesticide enantiomers in Arctic air suggest changing sources and pathways
- 2015
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:3, s. 1411-1420
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Tidskriftsartikel (refereegranskat)abstract
- Air samples collected during 1994-2000 at the Canadian Arctic air monitoring station Alert (82 degrees 30'N, 62 degrees 20'W) were analysed by enantiospecific gas chromatography-mass spectrometry for alpha-hexachlorocyclohexane (alpha-HCH), trans-chlordane (TC) and cis-chlordane (CC). Results were expressed as enantiomer fractions (EF = peak areas of (+)/[(+) + (-)] enantiomers), where EFs = 0.5, <0.5 and >0.5 indicate racemic composition, and preferential depletion of (+) and (-) enantiomers, respectively. Long-term average EFs were close to racemic values for alpha-HCH (0.504 +/- 0.004, n = 197) and CC (0.505 +/- 0.004, n = 162), and deviated farther from racemic for TC (0.470 +/- 0.013, n = 165). Digital filtration analysis revealed annual cycles of lower alpha-HCH EFs in summer-fall and higher EFs in winter-spring. These cycles suggest volatilization of partially degraded alpha-HCH with EF < 0.5 from open water and advection to Alert during the warm season, and background transport of alpha-HCH with EF > 0.5 during the cold season. The contribution of sea-volatilized alpha-HCH was only 11% at Alert, vs. 32% at Resolute Bay (74.68 degrees N, 94.90 degrees W) in 1999. EFs of TC also followed annual cycles of lower and higher values in the warm and cold seasons. These were in phase with low and high cycles of the TC / CC ratio (expressed as F-TC = TC/(TC + CC)), which suggests greater contribution of microbially "weathered" TC in summer-fall versus winter-spring. CC was closer to racemic than TC and displayed seasonal cycles only in 1997-1998. EF profiles are likely to change with rising contribution of secondary emission sources, weathering of residues in the environment, and loss of ice cover in the Arctic. Enantiomer-specific analysis could provide added forensic capability to air monitoring programs.
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| 16. |
- Bolinius, Damien Johann, et al.
(författare)
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Comparison of eddy covariance and modified Bowen ratio methods for measuring gas fluxes and implications for measuring fluxes of persistent organic pollutants
- 2016
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:8, s. 5315-5322
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Tidskriftsartikel (refereegranskat)abstract
- Semi-volatile persistent organic pollutants (POPs) cycle between the atmosphere and terrestrial surfaces; however measuring fluxes of POPs between the atmosphere and other media is challenging. Sampling times of hours to days are required to accurately measure trace concentrations of POPs in the atmosphere, which rules out the use of eddy covariance techniques that are used to measure gas fluxes of major air pollutants. An alternative, the modified Bowen ratio (MBR) method, has been used instead. In this study we used data from FLUXNET for CO2 and water vapor (H2O) to compare fluxes measured by eddy covariance to fluxes measured with the MBR method using vertical concentration gradients in air derived from averaged data that simulate the long sampling times typically required to measure POPs. When concentration gradients are strong and fluxes are unidirectional, the MBR method and the eddy covariance method agree within a factor of 3 for CO2, and within a factor of 10 for H2O. To remain within the range of applicability of the MBR method, field studies should be carried out under conditions such that the direction of net flux does not change during the sampling period. If that condition is met, then the performance of the MBR method is neither strongly affected by the length of sample duration nor the use of a fixed value for the transfer coefficient.
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| 17. |
- Bourgeois, Quentin, et al.
(författare)
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How much of the global aerosol optical depth is found in the boundary layer and free troposphere?
- 2018
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:10, s. 7709-7720
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Tidskriftsartikel (refereegranskat)abstract
- The global aerosol extinction from the CALIOP space lidar was used to compute aerosol optical depth (AOD) over a 9-year period (2007-2015) and partitioned between the boundary layer (BL) and the free troposphere (FT) using BL heights obtained from the ERA-Interim archive. The results show that the vertical distribution of AOD does not follow the diurnal cycle of the BL but remains similar between day and night highlighting the presence of a residual layer during night. The BL and FT contribute 69 and 31 %, respectively, to the global tropospheric AOD during daytime in line with observations obtained in Aire sur l'Adour (France) using the Light Optical Aerosol Counter (LOAC) instrument. The FT AOD contribution is larger in the tropics than at mid-latitudes which indicates that convective transport largely controls the vertical profile of aerosols. Over oceans, the FT AOD contribution is mainly governed by long-range transport of aerosols from emission sources located within neighboring continents. According to the CALIOP aerosol classification, dust and smoke particles are the main aerosol types transported into the FT. Overall, the study shows that the fraction of AOD in the FT - and thus potentially located above low-level clouds - is substantial and deserves more attention when evaluating the radiative effect of aerosols in climate models. More generally, the results have implications for processes determining the overall budgets, sources, sinks and transport of aerosol particles and their description in atmospheric models.
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| 18. |
- Boy, M., et al.
(författare)
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Interactions between the atmosphere, cryosphere, and ecosystems at northern high latitudes
- 2019
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:3, s. 2015-2061
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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.
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| 19. |
- Broman, Lina, et al.
(författare)
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Common volume satellite studies of polar mesospheric clouds with Odin/OSIRIS tomography and AIM/CIPS nadir imaging
- 2019
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:19, s. 12455-12475
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Tidskriftsartikel (refereegranskat)abstract
- Two important approaches for satellite studies of polar mesospheric clouds (PMCs) are nadir measurements adapting phase function analysis and limb measurements adapting spectroscopic analysis. Combining both approaches enables new studies of cloud structures and microphysical processes but is complicated by differences in scattering conditions, observation geometry and sensitivity. In this study, we compare common volume PMC observations from the nadir-viewing Cloud Imaging and Particle Size (CIPS) instrument on the Aeronomy of Ice in the Mesosphere (AIM) satellite and a special set of tomographic limb observations from the Optical Spectrograph and InfraRed Imager System (OSIRIS) on the Odin satellite performed over 18 d for the years 2010 and 2011 and the latitude range 78 to 80 degrees N. While CIPS provides preeminent horizontal resolution, the OSIRIS tomographic analysis provides combined horizontal and vertical PMC information. This first direct comparison is an important step towards co-analysing CIPS and OSIRIS data, aiming at unprecedented insights into horizontal and vertical cloud processes. Important scientific questions on how the PMC life cycle is affected by changes in humidity and temperature due to atmospheric gravity waves, planetary waves and tides can be addressed by combining PMC observations in multiple dimensions. Two- and three-dimensional cloud structures simultaneously observed by CIPS and tomographic OSIRIS provide a useful tool for studies of cloud growth and sublimation Moreover, the combined CIPS/tomographic OSIRIS dataset can be used for studies of even more fundamental character, such as the question of the assumption of the PMC particle size distribution. We perform the first thorough error characterization of OSIRIS tomographic cloud brightness and cloud ice water content (IWC). We establish a consistent method for comparing cloud properties from limb tomography and nadir observations, accounting for differences in scattering conditions, resolution and sensitivity. Based on an extensive common volume and a temporal coincidence criterion of only 5 min, our method enables a detailed comparison of PMC regions of varying brightness and IWC. However, since the dataset is limited to 18 d of observations this study does not include a comparison of cloud frequency. The cloud properties of the OSIRIS tomographic dataset are vertically resolved, while the cloud properties of the CIPS dataset is vertically integrated. To make these different quantities comparable, the OSIRIS tomographic cloud properties cloud scattering coefficient and ice mass density (IMD) have been integrated over the vertical extent of the cloud to form cloud albedo and IWC of the same quantity as CIPS cloud products. We find that the OSIRIS albedo (obtained from the vertical integration of the primary OSIRIS tomography product, cloud scattering coefficient) shows very good agreement with the primary CIPS product, cloud albedo, with a correlation coefficient of 0.96. However, OSIRIS systematically reports brighter clouds than CIPS and the bias between the instruments (OSIRIS -CIPS) is 3.4 x 10(-6) sr(-1) (+/- 2.9x 10(-6) sr(-1)) on average. The OSIRIS tomography IWC (obtained from the vertical integration of IMD) agrees well with the CIPS IWC, with a correlation coefficient of 0.91. However, the IWC reported by OSIRIS is lower than CIPS, and we quantify the bias to -22 g km(-2) (+/- 14 g km(-2)) on average.
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| 20. |
- Buchholz, Angela, et al.
(författare)
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Insights into the O : C-dependent mechanisms controlling the evaporation of alpha-pinene secondary organic aerosol particles
- 2019
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:6, s. 4061-4073
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Tidskriftsartikel (refereegranskat)abstract
- The volatility of oxidation products of volatile organic compounds (VOCs) in the atmosphere is a key factor to determine if they partition into the particle phase contributing to secondary organic aerosol (SOA) mass. Thus, linking volatility and measured particle composition will provide insights into SOA formation and its fate in the atmosphere. We produced alpha-pinene SOA with three different oxidation levels (characterized by average oxygen-to-carbon ratio; (O:C) over bar = 0.53, 0.69, and 0.96) in an oxidation flow reactor. We investigated the particle volatility by isothermal evaporation in clean air as a function of relative humidity (RH < 2 %, 40 %, and 80 %) and used a filter-based thermal desorption method to gain volatility and chemical composition information. We observed reduced particle evaporation for particles with increasing <(O:C )over bar> ratio, indicating that particles become more resilient to evaporation with oxidative aging. Particle evaporation was increased in the presence of water vapour and presumably particulate water; at the same time the resistance of the residual particles to thermal desorption was increased as well. For SOA with (O:C ) over bar = 0.96, the unexpectedly large increase in mean thermal desorption temperature and changes in the thermogram shapes under wet conditions (80 % RH) were an indication of aqueous phase chemistry. For the lower (O:C ) over bar cases, some water-induced composition changes were observed. However, the enhanced evaporation under wet conditions could be explained by the reduction in particle viscosity from the semi-solid to liquid-like range, and the observed higher desorption temperature of the residual particles is a direct consequence of the increased removal of high-volatility and the continued presence of low-volatility compounds.
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