| 21. |
- Angot, H., et al.
(författare)
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Chemical cycling and deposition of atmospheric mercury in polar regions: review of recent measurements and comparison with models
- 2016
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:16, s. 10735-10763
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Tidskriftsartikel (refereegranskat)abstract
- Mercury (Hg) is a worldwide contaminant that can cause adverse health effects to wildlife and humans. While atmospheric modeling traces the link from emissions to deposition of Hg onto environmental surfaces, large uncertainties arise from our incomplete understanding of atmospheric processes (oxidation pathways, deposition, and re-emission). Atmospheric Hg reactivity is exacerbated in high latitudes and there is still much to be learned from polar regions in terms of atmospheric processes. This paper provides a synthesis of the atmospheric Hg monitoring data available in recent years (2011-2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. The cycle of atmospheric Hg in the Arctic and in Antarctica presents both similarities and differences. Coastal sites in the two regions are both influenced by springtime atmospheric Hg depletion events and by summertime snowpack re-emission and oceanic evasion of Hg. The cycle of atmospheric Hg differs between the two regions primarily because of their different geography. While Arctic sites are significantly influenced by northern hemispheric Hg emissions especially in winter, coastal Antarctic sites are significantly influenced by the reactivity observed on the East Antarctic ice sheet due to katabatic winds. Based on the comparison of multi-model simulations with observations, this paper discusses whether the processes that affect atmospheric Hg seasonality and inter-annual variability are appropriately represented in the models and identifies research gaps in our understanding of the atmospheric Hg cycling in high latitudes.
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| 22. |
- Ansmann, A., et al.
(författare)
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Profiling of fine and coarse particle mass : case studies of Saharan dust and Eyjafjallajokull/Grimsvotn volcanic plumes
- 2012
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:20, s. 9399-9415
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Tidskriftsartikel (refereegranskat)abstract
- The polarization lidar photometer networking (POLIPHON) method introduced to separate coarse-mode and fine-mode particle properties of Eyjafjallajokull volcanic aerosols in 2010 is extended to cover Saharan dust events as well. Furthermore, new volcanic dust observations performed after the Grimsvotn volcanic eruptions in 2011 are presented. The retrieval of particle mass concentrations requires mass-specific extinction coefficients. Therefore, a review of recently published mass-specific extinction coefficients for Saharan dust and volcanic dust is given. Case studies of four different scenarios corroborate the applicability of the profiling technique: (a) Saharan dust outbreak to central Europe, (b) Saharan dust plume mixed with biomass-burning smoke over Cape Verde, and volcanic aerosol layers originating from (c) the Eyjafjallajokull eruptions in 2010 and (d) the Grimsvotn eruptions in 2011. Strong differences in the vertical aerosol layering, aerosol mixing, and optical properties are observed for the different volcanic events.
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| 23. |
- Ashworth, Kirsti, et al.
(författare)
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Megacity and local contributions to regional air pollution : an aircraft case study over London
- 2020
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:12, s. 7193-7216
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Tidskriftsartikel (refereegranskat)abstract
- In July 2017 three research flights circumnavigating the megacity of London were conducted as a part of the STANCO training school for students and early career researchers organised by EUFAR (European Facility for Airborne Research). Measurements were made from the UK's Facility for Airborne Atmospheric Measurements (FAAM) BAe-146-301 atmospheric research aircraft with the aim to sample, characterise and quantify the impact of megacity outflow pollution on air quality in the surrounding region. Conditions were extremely favourable for airborne measurements, and all three flights were able to observe clear pollution events along the flight path. A small change in wind direction provided sufficiently different air mass origins over the 2 d such that a distinct pollution plume from London, attributable marine emissions and a double-peaked dispersed area of pollution resulting from a combination of local and transported emissions were measured. We were able to analyse the effect of London emissions on air quality in the wider region and the extent to which local sources contribute to pollution events. The background air upwind of London was relatively clean during both days; concentrations of CO were 88-95 ppbv, total (measured) volatile organic compounds (VOCs) were 1.6-1.8 ppbv and NOx was 0.7-0.8 ppbv. Downwind of London, we encountered elevations in all species with CO>100 ppbv, VOCs 2.8-3.8 ppbv, CH4> 2080 ppbv and NOx >4 ppbv, and peak concentrations in individual pollution events were higher still. Levels of O-3 were inversely correlated with NOx, during the first flight, with O-3 concentrations of 37 ppbv upwind falling to similar to 26 ppbv in the well-defined London plume. Total pollutant fluxes from London were estimated through a vertical plane downwind of the city. Our calculated CO2 fluxes are within the combined uncertainty of those estimated previously, but there was a greater disparity in our estimates of CH4 and CO. On the second day, winds were lighter and downwind O-3 concentrations were elevated to similar to 39-43 ppbv (from similar to 32 to 35 ppbv upwind), reflecting the contribution of more aged pollution to the regional background. Elevations in pollutant concentrations were dispersed over a wider area than the first day, although we also encountered a number of clear transient enhancements from local sources. This series of flights demonstrated that even in a region of megacity outflow, such as the south-east of the UK, local fresh emissions and more distant UK sources of pollution can all contribute substantially to pollution events. In the highly complex atmosphere around a megacity where a high background level of pollution mixes with a variety of local sources at a range of spatial and temporal scales and atmospheric dynamics are further complicated by the urban heat island, the use of pollutant ratios to track and determine the ageing of air masses may not be valid. The individual sources must therefore all be well-characterised and constrained to understand air quality around megacities such as London. Research aircraft offer that capability through targeted sampling of specific sources and longitudinal studies monitoring trends in emission strength and profiles over time.
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| 24. |
- Asmi, A., et al.
(författare)
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Number size distributions and seasonality of submicron particles in = rope 2008-2009
- 2011
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:11, s. 5505-5538
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Tidskriftsartikel (refereegranskat)abstract
- Two years of harmonized aerosol number size distribution data from 24 = ropean field monitoring sites have been analysed. The results give a = mprehensive overview of the European near surface aerosol particle = mber concentrations and number size distributions between 30 and 500 = of dry particle diameter. Spatial and temporal distribution of = rosols in the particle sizes most important for climate applications = e presented. We also analyse the annual, weekly and diurnal cycles of = e aerosol number concentrations, provide log-normal fitting parameters = r median number size distributions, and give guidance notes for data = ers. Emphasis is placed on the usability of results within the aerosol = delling community.
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| 25. |
- Baars, Holger, et al.
(författare)
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An overview of the first decade of Polly(NET) : an emerging network of automated Raman-polarization lidars for continuous aerosol profiling
- 2016
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:8, s. 5111-5137
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Tidskriftsartikel (refereegranskat)abstract
- A global vertically resolved aerosol data set covering more than 10 years of observations at more than 20 measurement sites distributed from 63 degrees N to 52 degrees S and 72 degrees W to 124 degrees E has been achieved within the Raman and polarization lidar network Polly(NET). This network consists of portable, remote-controlled multiwavelength-polarization-Raman lidars (Polly) for automated and continuous 24/7 observations of clouds and aerosols. Polly(NET) is an independent, voluntary, and scientific network. All Polly lidars feature a standardized instrument design with different capabilities ranging from single wavelength to multiwavelength systems, and now apply unified calibration, quality control, and data analysis. The observations are processed in near-real time without manual intervention, and are presented online at polly.tropos.de. The paper gives an overview of the observations on four continents and two research vessels obtained with eight Polly systems. The specific aerosol types at these locations (mineral dust, smoke, dust-smoke and other dusty mixtures, urban haze, and volcanic ash) are identified by their Angstrom exponent, lidar ratio, and depolarization ratio. The vertical aerosol distribution at the Polly(NET) locations is discussed on the basis of more than 55 000 automatically retrieved 30 min particle backscatter coefficient profiles at 532 nm as this operating wavelength is available for all Polly lidar systems. A seasonal analysis of measurements at selected sites revealed typical and extraordinary aerosol conditions as well as seasonal differences. These studies show the potential of Polly(NET) to support the establishment of a global aerosol climatology that covers the entire troposphere.
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| 26. |
- Babkovskaia, Natalia, et al.
(författare)
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A DNS study of aerosol and small-scale cloud turbulence interaction
- 2016
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:12, s. 7889-7898
-
Tidskriftsartikel (refereegranskat)abstract
- The purpose of this study is to investigate the interaction between small-scale turbulence and aerosol and cloud microphysical properties using direct numerical simulations (DNS). We consider the domain located at the height of about 2000 m from the sea level, experiencing transient high supersaturation due to atmospheric fluctuations of temperature and humidity. To study the effect of total number of particles (Ntot) on air temperature, activation and supersaturation, we vary Ntot. To investigate the effect of aerosol dynamics on small-scale turbulence and vertical air motion, we vary the intensity of turbulent fluctuations and the buoyant force. We find that even a small number of aerosol particles (55.5 cm-3), and therefore a small droplet number concentration, strongly affects the air temperature due to release of latent heat. The system comes to an equilibrium faster and the relative number of activated particles appears to be smaller for larger Ntot. We conclude that aerosol particles strongly affect the air motion. In a case of updraught coursed by buoyant force, the presence of aerosol particles results in acceleration of air motion in vertical direction and increase of turbulent fluctuations.
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| 27. |
- Ball, William T., et al.
(författare)
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Evidence for a continuous decline in lower stratospheric ozone offsetting ozone layer recovery
- 2018
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:2, s. 1379-1394
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Tidskriftsartikel (refereegranskat)abstract
- Ozone forms in the Earth's atmosphere from the photodissociation of molecular oxygen, primarily in the tropical stratosphere. It is then transported to the extratropics by the Brewer-Dobson circulation (BDC), forming a protective ozone layer around the globe. Human emissions of halogen-containing ozone-depleting substances (hODSs) led to a decline in stratospheric ozone until they were banned by the Montreal Protocol, and since 1998 ozone in the upper stratosphere is rising again, likely the recovery from halogen-induced losses. Total column measurements of ozone between the Earth's surface and the top of the atmosphere indicate that the ozone layer has stopped declining across the globe, but no clear increase has been observed at latitudes between 60 degrees S and 60 degrees N outside the polar regions (60-90 degrees). Here we report evidence from multiple satellite measurements that ozone in the lower stratosphere between 60 degrees S and 60 degrees N has indeed continued to decline since 1998. We find that, even though upper stratospheric ozone is recovering, the continuing downward trend in the lower stratosphere prevails, resulting in a downward trend in stratospheric column ozone between 60 degrees S and 60 degrees N. We find that total column ozone between 60 degrees S and 60 degrees N appears not to have decreased only because of increases in tropospheric column ozone that compensate for the stratospheric decreases. The reasons for the continued reduction of lower stratospheric ozone are not clear; models do not reproduce these trends, and thus the causes now urgently need to be established.
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| 28. |
- Ball, William T., et al.
(författare)
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Inconsistencies between chemistry-climate models and observed lower stratospheric ozone trends since 1998
- 2020
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:16, s. 9737-9752
-
Tidskriftsartikel (refereegranskat)abstract
- The stratospheric ozone layer shields surface life from harmful ultraviolet radiation. Following the Montreal Protocol ban on long-lived ozone-depleting substances (ODSs), rapid depletion of total column ozone (TCO) ceased in the late 1990s, and ozone above 32 km is now clearly recovering. However, there is still no confirmation of TCO recovery, and evidence has emerged that ongoing quasiglobal (60 degrees S-60 degrees N) lower stratospheric ozone decreases may be responsible, dominated by low latitudes (30 degrees S-30 degrees N). Chemistry-climate models (CCMs) used to project future changes predict that lower stratospheric ozone will decrease in the tropics by 2100 but not at mid-latitudes (30-60 degrees). Here, we show that CCMs display an ozone decline similar to that observed in the tropics over 1998-2016, likely driven by an increase in tropical upwelling. On the other hand, mid-latitude lower stratospheric ozone is observed to decrease, while CCMs that specify real-world historical meteorological fields instead show an increase up to present day. However, these cannot be used to simulate future changes; we demonstrate here that free-running CCMs used for projections also show increases. Despite opposing lower stratospheric ozone changes, which should induce opposite temperature trends, CCMs and observed temperature trends agree; we demonstrate that opposing model- observation stratospheric water vapour (SWV) trends, and their associated radiative effects, explain why temperature changes agree in spite of opposing ozone trends. We provide new evidence that the observed mid-latitude trends can be explained by enhanced mixing between the tropics and extratropics. We further show that the temperature trends are consistent with the observed mid-latitude ozone decrease. Together, our results suggest that large-scale circulation changes expected in the future from increased greenhouse gases (GHGs) may now already be underway but that most CCMs do not simulate mid-latitude ozone layer changes well. However, it is important to emphasise that the periods considered here are short, and internal variability that is both intrinsic to each CCM and different to observed historical variability is not well-characterised and can influence trend estimates. Nevertheless, the reason CCMs do not exhibit the observed changes needs to be identified to allow models to be improved in order to build confidence in future projections of the ozone layer.
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| 29. |
- 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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| 30. |
- 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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