ORCID Profile
0000-0002-6800-154X
Current Organisation
University of Leeds
Does something not look right? The information on this page has been harvested from data sources that may not be up to date. We continue to work with information providers to improve coverage and quality. To report an issue, use the Feedback Form.
Publisher: Copernicus GmbH
Date: 03-2018
Publisher: Springer Science and Business Media LLC
Date: 08-2011
DOI: 10.1038/NATURE10343
Abstract: Atmospheric aerosols exert an important influence on climate through their effects on stratiform cloud albedo and lifetime and the invigoration of convective storms. Model calculations suggest that almost half of the global cloud condensation nuclei in the atmospheric boundary layer may originate from the nucleation of aerosols from trace condensable vapours, although the sensitivity of the number of cloud condensation nuclei to changes of nucleation rate may be small. Despite extensive research, fundamental questions remain about the nucleation rate of sulphuric acid particles and the mechanisms responsible, including the roles of galactic cosmic rays and other chemical species such as ammonia. Here we present the first results from the CLOUD experiment at CERN. We find that atmospherically relevant ammonia mixing ratios of 100 parts per trillion by volume, or less, increase the nucleation rate of sulphuric acid particles more than 100-1,000-fold. Time-resolved molecular measurements reveal that nucleation proceeds by a base-stabilization mechanism involving the stepwise accretion of ammonia molecules. Ions increase the nucleation rate by an additional factor of between two and more than ten at ground-level galactic-cosmic-ray intensities, provided that the nucleation rate lies below the limiting ion-pair production rate. We find that ion-induced binary nucleation of H(2)SO(4)-H(2)O can occur in the mid-troposphere but is negligible in the boundary layer. However, even with the large enhancements in rate due to ammonia and ions, atmospheric concentrations of ammonia and sulphuric acid are insufficient to account for observed boundary-layer nucleation.
Publisher: Copernicus GmbH
Date: 25-03-2020
DOI: 10.5194/GMD-2019-357
Abstract: Abstract. We document and evaluate the aerosol schemes as implemented in the physical and Earth system models, HadGEM3-GC3.1 (GC3.1) and UKESM1, which are contributing to the 6th Coupled Model Intercomparison Project (CMIP6). The simulation of aerosols in the present-day period of the historical ensemble of these models is evaluated against a range of observations. Updates to the aerosol microphysics scheme are documented as well as differences in the aerosol representation between the physical and Earth system configurations. The additional Earth-system interactions included in UKESM1 leads to differences in the emissions of natural aerosol sources such as dimethyl sulfide, mineral dust and organic aerosol and subsequent evolution of these species in the model. UKESM1 also includes a stratospheric-tropospheric chemistry scheme which is fully coupled to the aerosol scheme, while GC3.1 employs a simplified aerosol chemistry mechanism driven by prescribed monthly climatologies of the relevant oxidants. Overall, the simulated speciated aerosol mass concentrations compare reasonably well with observations. Both models capture the negative trend in sulfate aerosol concentrations over Europe and the eastern United States of America (US) although the models tend to underestimate the sulfate concentrations in both regions. Interactive emissions of biogenic volatile organic compounds in UKESM1 lead to an improved agreement of organic aerosol over the US. Simulated dust burdens are similar in both models despite a 2-fold difference in dust emissions. Aerosol optical depth is biased low in dust source and outflow regions but performs well in other regions compared to a number of satellite and ground-based retrievals of aerosol optical depth. Simulated aerosol number concentrations are generally within a factor of 2 of the observations with both models tending to overestimate number concentrations over remote ocean regions, apart from at high latitudes, and underestimate over Northern Hemisphere continents. Finally, UKESM1 includes for the first time a representation of a primary marine organic aerosol source. The impact of this new aerosol source is evaluated. Over the pristine Southern Ocean, it is found to improve the seasonal cycle of organic aerosol mass and cloud droplet number concentrations relative to GC3.1 although underestimations in cloud droplet number concentrations remain. This paper provides a useful characterization of the aerosol climatology in both models facilitating the understanding of the numerous aerosol-climate interaction studies that will be conducted as part of CMIP6 and beyond.
Publisher: Copernicus GmbH
Date: 05-07-2010
Abstract: Abstract. The 1783–1784 AD Laki flood lava eruption commenced on 8 June 1783 and released 122 Tg of sulphur dioxide gas over the course of 8 months into the upper troposphere and lower stratosphere above Iceland. Previous studies have examined the impact of the Laki eruption on sulphate aerosol and climate using general circulation models. Here, we study the impact on aerosol microphysical processes, including the nucleation of new particles and their growth to cloud condensation nuclei (CCN) using a comprehensive Global Model of Aerosol Processes (GLOMAP). Total particle concentrations in the free troposphere increase by a factor ~16 over large parts of the Northern Hemisphere in the 3 months following the onset of the eruption. Particle concentrations in the boundary layer increase by a factor 2 to 5 in regions as far away as North America, the Middle East and Asia due to long-range transport of nucleated particles. CCN concentrations (at 0.22% supersaturation) increase by a factor 65 in the upper troposphere with maximum changes in 3-month zonal mean concentrations of ~1400 cm−3 at high northern latitudes. 3-month zonal mean CCN concentrations in the boundary layer at the latitude of the eruption increase by up to a factor 26, and averaged over the Northern Hemisphere, the eruption caused a factor 4 increase in CCN concentrations at low-level cloud altitude. The simulations show that the Laki eruption would have completely dominated as a source of CCN in the pre-industrial atmosphere. The model also suggests an impact of the eruption in the Southern Hemisphere, where CCN concentrations are increased by up to a factor 1.4 at 20° S. Our model simulations suggest that the impact of an equivalent wintertime eruption on upper tropospheric CCN concentrations is only about one-third of that of a summertime eruption. The simulations show that the microphysical processes leading to the growth of particles to CCN sizes are fundamentally different after an eruption when compared to the unperturbed atmosphere, underlining the importance of using a fully coupled microphysics model when studying long-lasting, high-latitude eruptions.
Publisher: Wiley
Date: 09-10-2014
DOI: 10.1002/ASL2.539
Publisher: American Geophysical Union (AGU)
Date: 09-02-2022
DOI: 10.1029/2021JD035485
Abstract: Atmospheric aerosol size and abundance influence radiative effects and climate change. To date, efforts to constrain global climate models' radiative forcing with in situ aerosol observations have been hamstrung by uncertainty. One source of error, the regional “representation error,” arises when accurate but sparse single‐point measurements of atmospheric aerosol distributions are compared with a model value, assuming that the single‐point measurement is representative of the model domain. The Portable Optical Particle Spectrometer network in the Southern Great Plains (POPSnet‐SGP) c aign has demonstrated that a network of nearly autonomous aerosol instruments operating at ambient temperature and relative humidity (with low measurement error) may be used to quantify measurement representation error and investigate the factors introducing heterogeneity in aerosol distributions across a rural, continental background region. Measurements were made using Portable Optical Particle Spectrometer (POPS) instruments at several sites for five months across the Department of Energy's Aerosol Radiation Measurement Southern Great Plains (ARM‐SGP) User Facility in the central USA. Measurement representation error decreased with longer averaging periods (20%–40% between 1 s and 1 day), varied between sites by 10%–20% for aerosol concentration 140–2,500 nm in diameter (N_140), and was higher for aerosols nm in diameter (N_400). Our measurements also show the influence of local meteorology on aerosol surface area (A_140) and size distributions: A_140 is positively correlated with wind speed and relative humidity, negatively correlated with precipitation, and lower given westerly winds. We conclude that the POPSnet approach provides considerably more insight into the spatial variability in the aerosol population that can be used to constrain climate models than would be available from similar networks of PM 2.5 monitors.
Publisher: Copernicus GmbH
Date: 16-02-2023
Publisher: Copernicus GmbH
Date: 16-08-2010
Abstract: Abstract. The emission of dimethyl-sulphide (DMS) gas by phytoplankton and the subsequent formation of aerosol has long been suggested as an important climate regulation mechanism. The key aerosol quantity is the number concentration of cloud condensation nuclei (CCN), but until recently global models did not include the necessary aerosol physics to quantify CCN. Here we use a global aerosol microphysics model to calculate the sensitivity of CCN to changes in DMS emission using multiple present-day and future sea-surface DMS climatologies. Calculated annual fluxes of DMS to the atmosphere for the five model-derived and one observations based present day climatologies are in the range 15.1 to 32.3 Tg a−1 sulphur. The impact of DMS climatology on surface level CCN concentrations was calculated in terms of summer and winter hemispheric mean values of ΔCCN/ΔFluxDMS, which varied between −43 and +166 cm−3/(mg m−2 day−1 sulphur), with a mean of 63 cm−3/(mg m−2 day−1 sulphur). The range is due to CCN production in the atmosphere being strongly dependent on the spatial distribution of the emitted DMS. The relative sensitivity of CCN to DMS (i.e. fractional change in CCN ided by fractional change in DMS flux) depends on the abundance of non-DMS derived aerosol in each hemisphere. The relative sensitivity averaged over the five present day DMS climatologies is estimated to be 0.02 in the northern hemisphere (i.e. a 0.02% change in CCN for a 1% change in DMS) and 0.07 in the southern hemisphere where aerosol abundance is lower. In a globally warmed scenario in which the DMS flux increases by ~1% relative to present day we estimate a ~0.1% increase in global mean CCN at the surface. The largest CCN response occurs in the Southern Ocean, contributing to a Southern Hemisphere mean annual increase of less than 0.2%. We show that the changes in DMS flux and CCN concentration between the present day and global warming scenario are similar to interannual differences due to variability in windspeed. In summary, although DMS makes a significant contribution to global marine CCN concentrations, the sensitivity of CCN to potential future changes in DMS flux is very low. This finding, together with the predicted small changes in future seawater DMS concentrations, suggests that the role of DMS in climate regulation is very weak.
Publisher: American Geophysical Union (AGU)
Date: 16-02-2016
DOI: 10.1002/2015JD023539
Publisher: Elsevier BV
Date: 09-2020
Publisher: Springer Science and Business Media LLC
Date: 20-05-2016
DOI: 10.1038/NCOMMS11594
Abstract: The growth of freshly formed aerosol particles can be the bottleneck in their survival to cloud condensation nuclei. It is therefore crucial to understand how particles grow in the atmosphere. Insufficient experimental data has impeded a profound understanding of nano-particle growth under atmospheric conditions. Here we study nano-particle growth in the CLOUD (Cosmics Leaving OUtdoors Droplets) chamber, starting from the formation of molecular clusters. We present measured growth rates at sub-3 nm sizes with different atmospherically relevant concentrations of sulphuric acid, water, ammonia and dimethylamine. We find that atmospheric ions and small acid-base clusters, which are not generally accounted for in the measurement of sulphuric acid vapour, can participate in the growth process, leading to enhanced growth rates. The availability of compounds capable of stabilizing sulphuric acid clusters governs the magnitude of these effects and thus the exact growth mechanism. We bring these observations into a coherent framework and discuss their significance in the atmosphere.
Publisher: Copernicus GmbH
Date: 21-11-2019
Publisher: Springer Science and Business Media LLC
Date: 22-06-2017
DOI: 10.1038/NATURE22974
Abstract: Aerosols have a potentially large effect on climate, particularly through their interactions with clouds, but the magnitude of this effect is highly uncertain. Large volcanic eruptions produce sulfur dioxide, which in turn produces aerosols these eruptions thus represent a natural experiment through which to quantify aerosol-cloud interactions. Here we show that the massive 2014-2015 fissure eruption in Holuhraun, Iceland, reduced the size of liquid cloud droplets-consistent with expectations-but had no discernible effect on other cloud properties. The reduction in droplet size led to cloud brightening and global-mean radiative forcing of around -0.2 watts per square metre for September to October 2014. Changes in cloud amount or cloud liquid water path, however, were undetectable, indicating that these indirect effects, and cloud systems in general, are well buffered against aerosol changes. This result will reduce uncertainties in future climate projections, because we are now able to reject results from climate models with an excessive liquid-water-path response.
Publisher: American Meteorological Society
Date: 11-2019
Abstract: Uncertainty in radiative forcing caused by aerosol–cloud interactions is about twice as large as for CO 2 and remains the least well understood anthropogenic contribution to climate change. A major cause of uncertainty is the poorly quantified state of aerosols in the pristine preindustrial atmosphere, which defines the baseline against which anthropogenic effects are calculated. The Southern Ocean is one of the few remaining near-pristine aerosol environments on Earth, but there are very few measurements to help evaluate models. The Antarctic Circumnavigation Expedition: Study of Preindustrial-like Aerosols and their Climate Effects (ACE-SPACE) took place between December 2016 and March 2017 and covered the entire Southern Ocean region (Indian, Pacific, and Atlantic Oceans length of ship track ,000 km) including previously unexplored areas. In situ measurements covered aerosol characteristics [e.g., chemical composition, size distributions, and cloud condensation nuclei (CCN) number concentrations], trace gases, and meteorological variables. Remote sensing observations of cloud properties, the physical and microbial ocean state, and back trajectory analyses are used to interpret the in situ data. The contribution of sea spray to CCN in the westerly wind belt can be larger than 50%. The abundance of methanesulfonic acid indicates local and regional microbial influence on CCN abundance in Antarctic coastal waters and in the open ocean. We use the in situ data to evaluate simulated CCN concentrations from a global aerosol model. The extensive, available ACE-SPACE dataset ( ommunities/spi-ace?page=1& size=20 ) provides an unprecedented opportunity to evaluate models and to reduce the uncertainty in radiative forcing associated with the natural processes of aerosol emission, formation, transport, and processing occurring over the pristine Southern Ocean.
Publisher: American Association for the Advancement of Science (AAAS)
Date: 29-05-2020
Abstract: NO x is important for particle growth as it can participate in HOM formation and alter the HOM volatility distribution.
Publisher: Copernicus GmbH
Date: 07-2015
Abstract: Abstract. We present the results of laboratory measurements of the ion–ion recombination coefficient at different temperatures, relative humidities and concentrations of ozone and sulfur dioxide. The experiments were carried out using the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at CERN, the walls of which are made of conductive material, making it possible to measure small ions. We produced ions in the chamber using a 3.5 GeV c−1 beam of positively charged pions (π+) generated by the CERN Proton Synchrotron (PS). When the PS was switched off, galactic cosmic rays were the only ionization source in the chamber. The range of the ion production rate varied from 2 to 100 cm−3 s−1, covering the typical range of ionization throughout the troposphere. The temperature ranged from −55 to 20 °C, the relative humidity (RH) from 0 to 70 %, the SO2 concentration from 0 to 40 ppb, and the ozone concentration from 200 to 700 ppb. The best agreement of the retrieved ion–ion recombination coefficient with the commonly used literature value of 1.6 × 10−6 cm3 s−1 was found at a temperature of 5 °C and a RH of 40 % (1.5 ± 0.6) × 10−6 cm3 s−1. At 20 °C and 40 % RH, the retrieved ion–ion recombination coefficient was instead (2.3 ± 0.7) × 10−6 cm3 s−1. We observed no dependency of the ion–ion recombination coefficient on ozone concentration and a weak variation with sulfur dioxide concentration. However, we observed a more than fourfold increase in the ion–ion recombination coefficient with decreasing temperature. We compared our results with three different models and found an overall agreement for temperatures above 0 °C, but a disagreement at lower temperatures. We observed a strong increase in the recombination coefficient for decreasing relative humidities, which has not been reported previously.
Publisher: Copernicus GmbH
Date: 08-05-2015
DOI: 10.5194/ACPD-15-13457-2015
Abstract: Abstract. Substantial changes in anthropogenic aerosols and precursor gas emissions have occurred over recent decades due to the implementation of air pollution control legislation and economic growth. The response of atmospheric aerosols to these changes and the impact on climate are poorly constrained, particularly in studies using detailed aerosol chemistry climate models. Here we compare the HadGEM3-UKCA coupled chemistry-climate model for the period 1960 to 2009 against extensive ground based observations of sulfate aerosol mass (1978–2009), total suspended particle matter (SPM, 1978–1998), PM10 (1997–2009), aerosol optical depth (AOD, 2000–2009) and surface solar radiation (SSR, 1960–2009) over Europe. The model underestimates observed sulfate aerosol mass (normalised mean bias factor (NMBF) = −0.4), SPM (NMBF = −0.9), PM10 (NMBF = −0.2) and aerosol optical depth (AOD, NMBF = −0.01) but slightly overpredicts SSR (NMBF = 0.02). Trends in aerosol over the observational period are well simulated by the model, with observed (simulated) changes in sulfate of −68% (−78%), SPM of −42% (−20%), PM10 of −9% (−8%) and AOD of −11% (−14%). Discrepancies in the magnitude of simulated aerosol mass do not affect the ability of the model to reproduce the observed SSR trends. The positive change in observed European SSR (5%) during 1990–2009 ("brightening") is better reproduced by the model when aerosol radiative effects (ARE) are included (3%), compared to simulations where ARE are excluded (0.2%). The simulated top-of-the-atmosphere aerosol radiative forcing over Europe under all-sky conditions increased by 3 W m−2 during the period 1970–2009 in response to changes in anthropogenic emissions and aerosol concentrations.
Publisher: Copernicus GmbH
Date: 11-04-2023
Publisher: American Geophysical Union (AGU)
Date: 24-08-2017
DOI: 10.1002/2017JD026844
Publisher: Copernicus GmbH
Date: 04-12-2019
Publisher: American Association for the Advancement of Science (AAAS)
Date: 16-05-2014
Abstract: New-particle formation from gaseous precursors in the atmosphere is a complex and poorly understood process with importance in atmospheric chemistry and climate. Laboratory studies have had trouble reproducing the particle formation rates that must occur in the natural world. Riccobono et al. (p. 717 ) used the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN to recreate a realistic atmospheric environment. Sulfuric acid and oxidized organic vapors in typical natural concentrations caused particle nucleation at similar rates to those observed in the lower atmosphere.
Publisher: Springer Science and Business Media LLC
Date: 23-11-2015
DOI: 10.1038/NGEO2588
Publisher: American Geophysical Union (AGU)
Date: 16-12-2014
DOI: 10.1002/2014GL062029
Publisher: Copernicus GmbH
Date: 03-2018
DOI: 10.5194/ACP-2018-175
Abstract: Abstract. Changes in aerosols cause a change in net top-of-the-atmosphere (ToA) short-wave and long-wave radiative fluxes, rapid adjustments in clouds, water vapour and temperature, and cause an effective radiative forcing (ERF) of the planetary energy budget. The erse sources of model uncertainty and the computational cost of running climate models make it difficult to isolate the main causes of aerosol ERF uncertainty and to understand how observations can be used to constrain it. We explore the aerosol ERF uncertainty by using fast model emulators to generate a very large set of aerosol-climate model variants that span the model uncertainty due to twenty-seven parameters related to atmospheric and aerosol processes. Sensitivity analyses shows that the uncertainty in the ToA flux is dominated (around 80 %) by uncertainties in the physical atmosphere model, particularly parameters that affect cloud reflectivity. However, uncertainty in the change in ToA flux caused by aerosol emissions over the industrial period (the aerosol ERF) is controlled by a combination of uncertainties in aerosol (around 60 %) and physical atmosphere (around 40 %) parameters. Four of the atmospheric and aerosol parameters that cause uncertainty in short-wave ToA flux (mostly parameters that directly scale cloud reflectivity, cloud water content or cloud droplet concentrations) also account for around 60% of the aerosol ERF uncertainty. The common causes of uncertainty mean that constraining the modelled planetary brightness to tightly match satellite observations changes the lower 95 % credible aerosol ERF value from −2.65 Wm−2 to −2.37 Wm−2. This suggests the strongest forcings (below around −2.4 Wm−2) are inconsistent with observations. These results show that, regardless of the fact that the ToA flux is an order of magnitude larger than the aerosol ERF, the observed flux can constrain the uncertainty in ERF because their values are connected by constrainable process parameters. The key to reducing the aerosol ERF uncertainty further will be to identify observations that can additionally constrain in idual parameter ranges and/or combined parameter effects, which can be achieved through sensitivity analysis of perturbed parameter ensembles.
Publisher: Springer Science and Business Media LLC
Date: 03-2017
Publisher: Copernicus GmbH
Date: 07-03-2018
DOI: 10.5194/ACP-2018-174
Abstract: Abstract. Observational constraint of simulated aerosol and cloud properties is an essential part of building trustworthy climate models for calculating aerosol radiative forcing. Models are usually tuned to achieve good agreement with observations, but tuning produces just one of many potential variants of a model, so the model uncertainty cannot be determined. Here we estimate the uncertainty in aerosol effective radiative forcing (ERF) in a tuned climate model by constraining 4 million variants of the HadGEM3-UKCA aerosol-climate model to match nine common observations (top-of-atmosphere shortwave flux, aerosol optical depth, PM2.5, cloud condensation nuclei, concentrations of sulphate, black carbon and organic carbon, as well as decadal trends in aerosol optical depth and surface shortwave radiation.) The model uncertainty is calculated by using a perturbed parameter ensemble that s les twenty-seven uncertainties in both the aerosol model and the physical climate model. Focusing over Europe, we show that the aerosol ERF uncertainty can be reduced by about 30 % by constraining it to the nine observations, demonstrating that producing climate models with an observationally plausible base state can contribute to narrowing the uncertainty in aerosol ERF. However, the uncertainty in the aerosol ERF after observational constraint is large compared to the typical spread of a multi-model ensemble. Our results therefore raise questions about whether the underlying multi-model uncertainty would be larger if similar approaches as adopted here were applied more widely. It is hoped that aerosol ERF uncertainty can be further reduced by introducing process-related constraints, however, any such results will be robust only if the enormous number of potential model variants is explored.
Publisher: Copernicus GmbH
Date: 27-09-2021
DOI: 10.5194/ACP-21-14275-2021
Abstract: Abstract. New particle formation (NPF) is a significant source of atmospheric particles, affecting climate and air quality. Understanding the mechanisms involved in urban aerosols is important to develop effective mitigation strategies. However, NPF rates reported in the polluted boundary layer span more than 4 orders of magnitude, and the reasons behind this variability are the subject of intense scientific debate. Multiple atmospheric vapours have been postulated to participate in NPF, including sulfuric acid, ammonia, amines and organics, but their relative roles remain unclear. We investigated NPF in the CLOUD chamber using mixtures of anthropogenic vapours that simulate polluted boundary layer conditions. We demonstrate that NPF in polluted environments is largely driven by the formation of sulfuric acid–base clusters, stabilized by the presence of amines, high ammonia concentrations and lower temperatures. Aromatic oxidation products, despite their extremely low volatility, play a minor role in NPF in the chosen urban environment but can be important for particle growth and hence for the survival of newly formed particles. Our measurements quantitatively account for NPF in highly erse urban environments and explain its large observed variability. Such quantitative information obtained under controlled laboratory conditions will help the interpretation of future ambient observations of NPF rates in polluted atmospheres.
Publisher: American Meteorological Society
Date: 09-2015
Abstract: Regional patterns of aerosol radiative forcing are important for understanding climate change on decadal time scales. Uncertainty in aerosol forcing is likely to vary regionally and seasonally because of the short aerosol lifetime and heterogeneous emissions. Here the sensitivity of regional aerosol cloud albedo effect (CAE) forcing to 31 aerosol process parameters and emission fluxes is quantified between 1978 and 2008. The effects of parametric uncertainties on calculations of the balance of incoming and outgoing radiation are found to be spatially and temporally dependent. Regional uncertainty contributions of opposite sign cancel in global-mean forcing calculations, masking the regional importance of some parameters. Parameters that contribute little to uncertainty in Earth’s global energy balance during recent decades make significant contributions to regional forcing variance. Aerosol forcing sensitivities are quantified within 11 climatically important regions, where surface temperatures are thought to influence large-scale climate effects. Substantial simulated uncertainty in CAE forcing in the eastern Pacific leaves open the possibility that apparent shifts in the mean ENSO state may result from a forced aerosol signal on multidecadal time scales. A likely negative aerosol CAE forcing in the tropical North Atlantic calls into question the relationship between Northern Hemisphere aerosol emission reductions and CAE forcing of sea surface temperatures in the main Atlantic hurricane development region on decadal time scales. Simulated CAE forcing uncertainty is large in the North Pacific, suggesting that the role of the CAE in altering Pacific tropical storm frequency and intensity is also highly uncertain.
Publisher: Copernicus GmbH
Date: 24-10-2014
DOI: 10.5194/ACP-14-11221-2014
Abstract: Abstract. We use a stratosphere–troposphere composition–climate model with interactive sulfur chemistry and aerosol microphysics, to investigate the effect of the 1991 Mount Pinatubo eruption on stratospheric aerosol properties. Satellite measurements indicate that shortly after the eruption, between 14 and 23 Tg of SO2 (7 to 11.5 Tg of sulfur) was present in the tropical stratosphere. Best estimates of the peak global stratospheric aerosol burden are in the range 19 to 26 Tg, or 3.7 to 6.7 Tg of sulfur assuming a composition of between 59 and 77 % H2SO4. In light of this large uncertainty range, we performed two main simulations with 10 and 20 Tg of SO2 injected into the tropical lower stratosphere. Simulated stratospheric aerosol properties through the 1991 to 1995 period are compared against a range of available satellite and in situ measurements. Stratospheric aerosol optical depth (sAOD) and effective radius from both simulations show good qualitative agreement with the observations, with the timing of peak sAOD and decay timescale matching well with the observations in the tropics and mid-latitudes. However, injecting 20 Tg gives a factor of 2 too high stratospheric aerosol mass burden compared to the satellite data, with consequent strong high biases in simulated sAOD and surface area density, with the 10 Tg injection in much better agreement. Our model cannot explain the large fraction of the injected sulfur that the satellite-derived SO2 and aerosol burdens indicate was removed within the first few months after the eruption. We suggest that either there is an additional alternative loss pathway for the SO2 not included in our model (e.g. via accommodation into ash or ice in the volcanic cloud) or that a larger proportion of the injected sulfur was removed via cross-tropopause transport than in our simulations. We also critically evaluate the simulated evolution of the particle size distribution, comparing in detail to balloon-borne optical particle counter (OPC) measurements from Laramie, Wyoming, USA (41° N). Overall, the model captures remarkably well the complex variations in particle concentration profiles across the different OPC size channels. However, for the 19 to 27 km injection height-range used here, both runs have a modest high bias in the lowermost stratosphere for the finest particles (radii less than 250 nm), and the decay timescale is longer in the model for these particles, with a much later return to background conditions. Also, whereas the 10 Tg run compared best to the satellite measurements, a significant low bias is apparent in the coarser size channels in the volcanically perturbed lower stratosphere. Overall, our results suggest that, with appropriate calibration, aerosol microphysics models are capable of capturing the observed variation in particle size distribution in the stratosphere across both volcanically perturbed and quiescent conditions. Furthermore, additional sensitivity simulations suggest that predictions with the models are robust to uncertainties in sub-grid particle formation and nucleation rates in the stratosphere.
Publisher: Copernicus GmbH
Date: 20-01-2021
Publisher: Copernicus GmbH
Date: 28-03-2022
DOI: 10.5194/EGUSPHERE-EGU22-13286
Abstract: & & Increasing anthropogenic aerosol emissions have been attributed as the main driver of an observed southward shift in tropical precipitation between the 1950s and 1980s. In the near-term future, anthropogenic aerosol emissions will decline which could drive a northward shift in tropical precipitation over the coming decades. We use a perturbed parameter ensemble (PPE) of transient coupled-ocean atmosphere simulations that span a range of aerosol radiative forcing to investigate the role of aerosol radiative forcing uncertainty on tropical precipitation shifts in the 20& sup& th& /sup& and 21& sup& st& /sup& centuries. We find no relationship between the strength of the hemispheric contrast in pre-industrial to 1975 anthropogenic aerosol radiative forcing and tropical precipitation shifts during the 20& sup& th& /sup& century. This result is in contrary to that from CMIP5, and we suspect internal variability plays a large role in why we do not see the expected relationship in our PPE. Tropical precipitation shifts are associated with major volcanic eruptions over the 20& sup& th& /sup& century. However, we do find a relationship between the hemispheric contrast in pre-industrial to 2005 anthropogenic aerosol radiative forcing and the magnitude of future tropical precipitation shifts over 2006 to 2060 under scenario RCP8.5. Overall, our results suggest that reduction in aerosol radiative forcing uncertainty would improve projections of future precipitation shifts, but any predictive gains would be offset if future major volcanic eruptions temporarily shift tropical precipitation.& &
Publisher: Copernicus GmbH
Date: 13-05-2014
Abstract: Abstract. Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model ersity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multi-model-mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the in idual global aerosol microphysics models are performing well, although the large model ersity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation and growth (e.g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.
Publisher: IOP Publishing
Date: 07-09-2020
Publisher: Copernicus GmbH
Date: 20-01-2021
Abstract: Abstract. New-particle formation (NPF) is a significant source of atmospheric particles, affecting climate and air quality. Understanding the mechanisms involved in urban aerosols is important to develop effective mitigation strategies. However, NPF rates reported in the polluted boundary layer span more than four orders of magnitude and the reasons behind this variability subject of intense scientific debate. Multiple atmospheric vapours have been postulated to participate in NPF, including sulfuric acid, ammonia, amines and organics, but their relative roles remain unclear. We investigated NPF in the CLOUD chamber using mixtures of anthropogenic vapours that simulate polluted boundary layer conditions. We demonstrate that NPF in polluted environments are largely driven by the formation of sulfuric acid-base clusters, stabilized by the presence of amines, high ammonia concentrations and lower temperatures. Aromatic oxidation products, despite their extremely low volatility, play a minor role in NPF in the chosen urban environment but can be important for particle growth and hence for the survival of newly formed particles. Our measurements quantitatively account for NPF in highly erse urban environments and explain its large observed variability. Such quantitative information obtained under controlled laboratory conditions will help the interpretation of future ambient observations of NPF rates in polluted atmospheres.
Publisher: Copernicus GmbH
Date: 13-08-2020
Abstract: Abstract. The effect of observational constraint on the ranges of uncertain physical and chemical process parameters was explored in a global aerosol–climate model. The study uses 1 million variants of the Hadley Centre General Environment Model version 3 (HadGEM3) that s le 26 sources of uncertainty, together with over 9000 monthly aggregated grid-box measurements of aerosol optical depth, PM2.5, particle number concentrations, sulfate and organic mass concentrations. Despite many compensating effects in the model, the procedure constrains the probability distributions of parameters related to secondary organic aerosol, anthropogenic SO2 emissions, residential emissions, sea spray emissions, dry deposition rates of SO2 and aerosols, new particle formation, cloud droplet pH and the diameter of primary combustion particles. Observational constraint rules out nearly 98 % of the model variants. On constraint, the ±1σ (standard deviation) range of global annual mean direct radiative forcing (RFari) is reduced by 33 % to −0.14 to −0.26 W m−2, and the 95 % credible interval (CI) is reduced by 34 % to −0.1 to −0.32 W m−2. For the global annual mean aerosol–cloud radiative forcing, RFaci, the ±1σ range is reduced by 7 % to −1.66 to −2.48 W m−2, and the 95 % CI by 6 % to −1.28 to −2.88 W m−2. The tightness of the constraint is limited by parameter cancellation effects (model equifinality) as well as the large and poorly defined “representativeness error” associated with comparing point measurements with a global model. The constraint could also be narrowed if model structural errors that prevent simultaneous agreement with different measurement types in multiple locations and seasons could be improved. For ex le, constraints using either sulfate or PM2.5 measurements in idually result in RFari±1σ ranges that only just overlap, which shows that emergent constraints based on one measurement type may be overconfident.
Publisher: Copernicus GmbH
Date: 28-08-2020
DOI: 10.5194/ACP-20-10063-2020
Abstract: Abstract. Aerosol measurements over the Southern Ocean are used to constrain aerosol–cloud interaction radiative forcing (RFaci) uncertainty in a global climate model. Forcing uncertainty is quantified using 1 million climate model variants that s le the uncertainty in nearly 30 model parameters. Measurements of cloud condensation nuclei and other aerosol properties from an Antarctic circumnavigation expedition strongly constrain natural aerosol emissions: default sea spray emissions need to be increased by around a factor of 3 to be consistent with measurements. Forcing uncertainty is reduced by around 7 % using this set of several hundred measurements, which is comparable to the 8 % reduction achieved using a erse and extensive set of over 9000 predominantly Northern Hemisphere measurements. When Southern Ocean and Northern Hemisphere measurements are combined, uncertainty in RFaci is reduced by 21 %, and the strongest 20 % of forcing values are ruled out as implausible. In this combined constraint, observationally plausible RFaci is around 0.17 W m−2 weaker (less negative) with 95 % credible values ranging from −2.51 to −1.17 W m−2 (standard deviation of −2.18 to −1.46 W m−2). The Southern Ocean and Northern Hemisphere measurement datasets are complementary because they constrain different processes. These results highlight the value of remote marine aerosol measurements.
Publisher: American Meteorological Society
Date: 09-2017
DOI: 10.1175/BAMS-D-15-00317.1
Abstract: The largest uncertainty in the historical radiative forcing of climate is caused by changes in aerosol particles due to anthropogenic activity. Sophisticated aerosol microphysics processes have been included in many climate models in an effort to reduce the uncertainty. However, the models are very challenging to evaluate and constrain because they require extensive in situ measurements of the particle size distribution, number concentration, and chemical composition that are not available from global satellite observations. The Global Aerosol Synthesis and Science Project (GASSP) aims to improve the robustness of global aerosol models by combining new methodologies for quantifying model uncertainty, to create an extensive global dataset of aerosol in situ microphysical and chemical measurements, and to develop new ways to assess the uncertainty associated with comparing sparse point measurements with low-resolution models. GASSP has assembled over 45,000 hours of measurements from ships and aircraft as well as data from over 350 ground stations. The measurements have been harmonized into a standardized format that is easily used by modelers and nonspecialist users. Available measurements are extensive, but they are biased to polluted regions of the Northern Hemisphere, leaving large pristine regions and many continental areas poorly s led. The aerosol radiative forcing uncertainty can be reduced using a rigorous model–data synthesis approach. Nevertheless, our research highlights significant remaining challenges because of the difficulty of constraining many interwoven model uncertainties simultaneously. Although the physical realism of global aerosol models still needs to be improved, the uncertainty in aerosol radiative forcing will be reduced most effectively by systematically and rigorously constraining the models using extensive syntheses of measurements.
Publisher: Proceedings of the National Academy of Sciences
Date: 06-10-2014
Abstract: A significant fraction of atmospheric aerosols is formed from the condensation of low-volatility vapors. These newly formed particles can grow, become seeds for cloud particles, and influence climate. New particle formation in the planetary boundary layer generally proceeds via the neutral channel. However, unambiguous identification of neutral nucleating clusters has so far not been possible under atmospherically relevant conditions. We explored the system of sulfuric acid, water, and dimethylamine in a well-controlled laboratory experiment and measured the time-resolved concentrations of neutral clusters. Clusters containing up to 14 sulfuric acid and 16 dimethylamine molecules were observed. Our results demonstrate that a cluster containing as few as two sulfuric acid and one or two dimethylamine molecules is already stable against evaporation.
Publisher: Proceedings of the National Academy of Sciences
Date: 27-07-2020
Abstract: Enhancement of aerosol that can nucleate cloud droplets increases the droplet number concentration and albedo of clouds. This increases the amount of sunlight reflected to space. Uncertainty in how aerosol−cloud interactions over the industrial period have increased planetary albedo by this mechanism leads to significant uncertainty in climate projections. Our work presents a method for observationally constraining the change in albedo due to anthropogenic aerosol emissions: a hemispheric difference in remotely sensed cloud droplet number between the pristine Southern Ocean (a preindustrial proxy) and the polluted Northern Hemisphere. Application of this constraint to climate models reduces the range of estimated albedo change since industrialization and suggests current models underpredict cloud droplet number concentration in the preindustrial era.
Publisher: Copernicus GmbH
Date: 26-08-2022
Abstract: Abstract. An observed southward shift in tropical rainfall over land between 1950 and 1985, followed by a weaker recovery post-1985, has been attributed to anthropogenic aerosol radiative forcing and cooling of the Northern Hemisphere relative to the Southern Hemisphere. We might therefore expect models that have a strong historic hemispheric contrast in aerosol forcing to simulate a further northward tropical rainfall shift in the near-term future when anthropogenic aerosol emission reductions will predominantly warm the Northern Hemisphere. We investigate this paradigm using a perturbed parameter ensemble (PPE) of transient coupled ocean–atmosphere climate simulations that span a range of aerosol radiative forcing comparable to multi-model studies. In the 20th century, in our single-model ensemble, we find no relationship between the magnitude of pre-industrial to 1975 inter-hemispheric anthropogenic aerosol radiative forcing and tropical precipitation shifts. Instead, tropical precipitation shifts are associated with major volcanic eruptions and are strongly affected by internal variability. However, we do find a relationship between the magnitude of pre-industrial to 2005 inter-hemispheric anthropogenic aerosol radiative forcing and future tropical precipitation shifts over 2006 to 2060 under scenario RCP8.5. Our results suggest that projections of tropical precipitation shifts will be improved by reducing aerosol radiative forcing uncertainty, but predictive gains may be offset by temporary shifts in tropical precipitation caused by future major volcanic eruptions.
Publisher: Springer Science and Business Media LLC
Date: 25-05-2016
DOI: 10.1038/NATURE18271
Abstract: About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday 1 . Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres 2,3 . In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles 4 , thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth 5,6 , leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer 7,8,9,10 . Although recent studies 11,12,13 predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon 2 , and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Köhler theory) 2,14 , has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absence of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown 15 that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10 −4.5 micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10 −4.5 to 10 −0.5 micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations.
Publisher: Proceedings of the National Academy of Sciences
Date: 07-10-2013
Abstract: The formation of nanoparticles by condensable vapors in the atmosphere influences radiative forcing and therefore climate. We explored the detailed mechanism of particle formation, in particular the role of oxidized organic molecules that arise from the oxidation of monoterpenes, a class of volatile organic compounds emitted from plants. We mimicked atmospheric conditions in a well-controlled laboratory setup and found that these oxidized organics form initial clusters directly with single sulfuric acid molecules. The clusters then grow by the further addition of both sulfuric acid and organic molecules. Some of the organics are remarkably highly oxidized, a critical feature that enables them to participate in forming initial stable molecular clusters and to facilitate the first steps of atmospheric nanoparticle formation.
Publisher: American Geophysical Union (AGU)
Date: 27-10-2016
DOI: 10.1002/2015JD023908
Publisher: Elsevier BV
Date: 12-2020
Publisher: American Geophysical Union (AGU)
Date: 09-04-2019
DOI: 10.1029/2019GL082067
Publisher: American Geophysical Union (AGU)
Date: 07-08-2008
DOI: 10.1029/2007JD009718
Publisher: Copernicus GmbH
Date: 25-06-2020
Abstract: Abstract. In the present-day atmosphere, sulfuric acid is the most important vapour for aerosol particle formation and initial growth. However, the growth rates of nanoparticles ( nm) from sulfuric acid remain poorly measured. Therefore, the effect of stabilizing bases, the contribution of ions and the impact of attractive forces on molecular collisions are under debate. Here, we present precise growth rate measurements of uncharged sulfuric acid particles from 1.8 to 10 nm, performed under atmospheric conditions in the CERN (European Organization for Nuclear Research) CLOUD chamber. Our results show that the evaporation of sulfuric acid particles above 2 nm is negligible, and growth proceeds kinetically even at low ammonia concentrations. The experimental growth rates exceed the hard-sphere kinetic limit for the condensation of sulfuric acid. We demonstrate that this results from van der Waals forces between the vapour molecules and particles and disentangle it from charge–dipole interactions. The magnitude of the enhancement depends on the assumed particle hydration and collision kinetics but is increasingly important at smaller sizes, resulting in a steep rise in the observed growth rates with decreasing size. Including the experimental results in a global model, we find that the enhanced growth rate of sulfuric acid particles increases the predicted particle number concentrations in the upper free troposphere by more than 50 %.
Publisher: Copernicus GmbH
Date: 04-03-2021
DOI: 10.5194/EGUSPHERE-EGU21-8499
Abstract: & & & & The change in planetary albedo due to aerosol-cloud interactions (aci) during the industrial era is the leading source of uncertainty in inferring& Earth's& climate sensitivity to increased greenhouse gases from the historical record. Examining pristine environments such as the Southern Ocean (SO) helps us to understand the pre-industrial state and constrain the change in cloud brightness over the industrial period associated with aci. This study presents two methods of utilizing observations of pristine environments to examine climate models and our understanding of the pre-industrial state.& & & / & & & & & First, cloud droplet number concentration (& em& N& sub& d& /sub& & /em& ) is used as an indicator of aci. Global climate models (GCMs) show that the& hemispheric contrast& in liquid cloud & em& N& sub& d& /sub& & /em& between the& ristine SO& and the polluted& Northern Hemisphere observed in the present-day can be used& strong& & /strong& as& a proxy for the increase& in & em& N& sub& d& /sub& & /em& from& the pre-industrial. A hemispheric difference constraint& developed from MODIS satellite observations indicates that pre-industrial& & em& N& sub& d& /sub& & /em& may have been higher than previously thought and provides an estimate of radiative forcing associated with aci between -1.2 and -0.6 Wm& sup& -2& /sup& . Comparisons with MODIS & em& N& sub& d & & /sub& & /em& highlight significant GCM discrepancies in pristine, biologically active regions.& & & / & & & & & Second, aerosol and cloud microphysical observations from a recent SO aircraft c aign are used to identify two potentially important mechanisms that are incomplete or missing in GCMs: i) production of new aerosol particles through synoptic uplift, and ii) buffering of & em& N& sub& d& /sub& & /em& against precipitation removal by small, Aitken mode aerosols entrained from the free troposphere. The latter may significantly contribute to the high, summertime SO & em& N& sub& d& /sub& & /em& levels which persist despite precipitation depletion associated with mid-latitude storm systems. Observational comparisons with nudged Community Atmosphere Model version 6 (CAM6) hindcasts show low-biased SO & em& N& sub& d & & /sub& & /em& is linked to under-production of free-tropospheric Aitken aerosol which drives low-biases in cloud condensation nuclei number and likely discrepancies in composition. These results have important implications for the ability of current GCMs to capture aci in pristine environments.& & & / &
Publisher: Copernicus GmbH
Date: 15-03-2013
Abstract: Abstract. The Hadley Centre Global Environmental Model (HadGEM) includes two aerosol schemes: the Coupled Large-scale Aerosol Simulator for Studies in Climate (CLASSIC), and the new Global Model of Aerosol Processes (GLOMAP-mode). GLOMAP-mode is a modal aerosol microphysics scheme that simulates not only aerosol mass but also aerosol number, represents internally-mixed particles, and includes aerosol microphysical processes such as nucleation. In this study, both schemes provide hindcast simulations of natural and anthropogenic aerosol species for the period 2000–2006. HadGEM simulations of the aerosol optical depth using GLOMAP-mode compare better than CLASSIC against a data-assimilated aerosol re-analysis and aerosol ground-based observations. Because of differences in wet deposition rates, GLOMAP-mode sulphate aerosol residence time is two days longer than CLASSIC sulphate aerosols, whereas black carbon residence time is much shorter. As a result, CLASSIC underestimates aerosol optical depths in continental regions of the Northern Hemisphere and likely overestimates absorption in remote regions. Aerosol direct and first indirect radiative forcings are computed from simulations of aerosols with emissions for the year 1850 and 2000. In 1850, GLOMAP-mode predicts lower aerosol optical depths and higher cloud droplet number concentrations than CLASSIC. Consequently, simulated clouds are much less susceptible to natural and anthropogenic aerosol changes when the microphysical scheme is used. In particular, the response of cloud condensation nuclei to an increase in dimethyl sulphide emissions becomes a factor of four smaller. The combined effect of different 1850 baselines, residence times, and abilities to affect cloud droplet number, leads to substantial differences in the aerosol forcings simulated by the two schemes. GLOMAP-mode finds a present-day direct aerosol forcing of −0.49 W m−2 on a global average, 72% stronger than the corresponding forcing from CLASSIC. This difference is compensated by changes in first indirect aerosol forcing: the forcing of −1.17 W m−2 obtained with GLOMAP-mode is 20% weaker than with CLASSIC. Results suggest that mass-based schemes such as CLASSIC lack the necessary sophistication to provide realistic input to aerosol-cloud interaction schemes. Furthermore, the importance of the 1850 baseline highlights how model skill in predicting present-day aerosol does not guarantee reliable forcing estimates. Those findings suggest that the more complex representation of aerosol processes in microphysical schemes improves the fidelity of simulated aerosol forcings.
Publisher: Copernicus GmbH
Date: 04-12-2019
Abstract: Abstract. Aerosol measurements over the Southern Ocean are used to constrain aerosol-cloud interaction radiative forcing uncertainty in a global climate model. Aerosol forcing uncertainty is quantified using one million climate model variants that s le the uncertainty in nearly 30 model parameters. Ship-based measurements of cloud condensation nuclei, particle number concentrations and sulfate mass concentrations from the Antarctic Circumnavigation Expedition: Study of Preindustrial-like Aerosols and Their Climate Effects (ACE-SPACE) are used to identify observationally implausible variants and thereby reduce the spread in the simulated forcing. Southern Ocean measurements strongly constrain natural aerosol emissions: default sea spray emissions in the model need to be increased by around a factor of 3 to be consistent with measurements. Aerosol forcing uncertainty is reduced by around 7 % using these measurements, which is comparable to the 8 % reduction achieved using an extensive set of over 9000 predominantly Northern Hemisphere measurements. The radiative forcing due to aerosol–cloud interactions (RFaci) is constrained to −2.61 to −1.10 W m−2 (95 % confidence) and the effective radiative forcing from aerosol-cloud interactions (ERFaci) is constrained to −2.43 to −0.54 W m−2. When Southern Ocean and Northern Hemisphere measurements are combined, the uncertainty in RFaci is reduced by 21 % and the strongest 20 % of forcing values are ruled out as implausible. In this combined constraint the observationally plausible RFaci is around 0.17 W m−2 weaker (less negative) with credible values ranging from −2.51 to −1.17 W m−2 and from −2.18 to −1.46 W m−2 when using one standard deviation to quantify the uncertainty. The Southern Ocean and Northern Hemisphere measurement datasets are complementary because they constrain different processes. These results highlight the value of remote marine aerosol measurements.
Publisher: American Association for the Advancement of Science (AAAS)
Date: 02-12-2016
Abstract: Observations made in the CLOUD chamber at CERN illuminate atmospheric particle formation.
Publisher: Copernicus GmbH
Date: 15-05-2023
DOI: 10.5194/EGUSPHERE-EGU23-15360
Abstract: Evidence from model simulations has suggested that anthropogenic aerosols may have forced multidecadal variability in a range of North Atlantic variables including sea surface temperatures, ocean circulation, and sea ice. However, many questions remain concerning the importance of anthropogenic aerosols in driving past changes in the North Atlantic climate system. The pathways via which changes in aerosol and aerosol precursor emissions, and oxidant levels, influence climate are complex. They involve both chemical and physical processes, and likely include changes in clouds, radiation, surface temperatures, atmospheric and oceanic circulation, and Arctic sea ice. This complexity is an important factor in the large uncertainty surrounding the role of anthropogenic aerosol in North Atlantic climate change, and was one of the major motivations for the UK& #8217 s North Atlantic Climate System Integrated Study (ACSIS). ACSIS was a multidisciplinary research programme conducted over the period 2016-2022, delivered by a consortium of seven UK institutions. This presentation draws together findings from the programme to provide an overall synthesis of what was learned in ACSIS about the role of anthropogenic aerosol in North Atlantic climate change. Remaining uncertainties, the potential for observational constraints, and opportunities for future work will also be discussed.& ACSIS made extensive use of simulations conducted for CMIP6, particularly historical simulations, and attribution experiments included in AerChemMIP and DAMIP. Additional sensitivity experiments with HadGEM3-GC3.1 and UKESM1 were used to quantify the effects of uncertainty in aerosol forcing in the absence of the additional uncertainty associated with model differences, to decompose the aerosol forcing, and to better illustrate the role of aerosol in recent changes.& As aerosol emissions increased (1850-1985), North Atlantic CDNC increased. Emissions of ozone precursors, and resulting changes in OH, contributed to this trend. This led to downwelling surface shortwave decreases across the North Atlantic, which drove colder surface temperatures, increased sea ice extent, and increased mean sea level pressure. In contrast, the eastern subpolar gyre warmed, likely due to increased ocean heat convergence due to the increase in the AMOC.& As local aerosol emissions fell (1986-2014) much of the reverse occurred. Downwelling surface shortwave increased across the North Atlantic, predominantly over land, driving warmer surface temperatures and reduced sea ice extent. The eastern subpolar gyre cooled. However, the role of aerosol in this later period is less clear due to a dominance of temperature-mediated cloud feedbacks over aerosol forcing, AMOC related feedbacks, and a changing aerosol forcing pattern.
Publisher: Copernicus GmbH
Date: 11-09-2018
DOI: 10.5194/ACP-18-13031-2018
Abstract: Abstract. Observational constraint of simulated aerosol and cloud properties is an essential part of building trustworthy climate models for calculating aerosol radiative forcing. Models are usually tuned to achieve good agreement with observations, but tuning produces just one of many potential variants of a model, so the model uncertainty cannot be determined. Here we estimate the uncertainty in aerosol effective radiative forcing (ERF) in a tuned climate model by constraining 4 million variants of the HadGEM3-UKCA aerosol–climate model to match nine common observations (top-of-atmosphere shortwave flux, aerosol optical depth, PM2.5, cloud condensation nuclei at 0.2 % supersaturation (CCN0.2), and concentrations of sulfate, black carbon and organic carbon, as well as decadal trends in aerosol optical depth and surface shortwave radiation.) The model uncertainty is calculated by using a perturbed parameter ensemble that s les 27 uncertainties in both the aerosol model and the physical climate model, and we use synthetic observations generated from the model itself to determine the potential of each observational type to constrain this uncertainty. Focusing over Europe in July, we show that the aerosol ERF uncertainty can be reduced by about 30 % by constraining it to the nine observations, demonstrating that producing climate models with an observationally plausible “base state” can contribute to narrowing the uncertainty in aerosol ERF. However, the uncertainty in the aerosol ERF after observational constraint is large compared to the typical spread of a multi-model ensemble. Our results therefore raise questions about whether the underlying multi-model uncertainty would be larger if similar approaches as adopted here were applied more widely. The approach presented in this study could be used to identify the most effective observations for model constraint. It is hoped that aerosol ERF uncertainty can be further reduced by introducing process-related constraints however, any such results will be robust only if the enormous number of potential model variants is explored.
Publisher: Proceedings of the National Academy of Sciences
Date: 19-01-2010
Abstract: New particle formation in the atmosphere is an important parameter in governing the radiative forcing of atmospheric aerosols. However, detailed nucleation mechanisms remain ambiguous, as laboratory data have so far not been successful in explaining atmospheric nucleation. We investigated the formation of new particles in a smog chamber simulating the photochemical formation of H 2 SO 4 and organic condensable species. Nucleation occurs at H 2 SO 4 concentrations similar to those found in the ambient atmosphere during nucleation events. The measured particle formation rates are proportional to the product of the concentrations of H 2 SO 4 and an organic molecule. This suggests that only one H 2 SO 4 molecule and one organic molecule are involved in the rate-limiting step of the observed nucleation process. Parameterizing this process in a global aerosol model results in substantially better agreement with ambient observations compared to control runs.
Publisher: Proceedings of the National Academy of Sciences
Date: 10-10-2016
Abstract: A mechanism for the formation of atmospheric aerosols via the gas to particle conversion of highly oxidized organic molecules is found to be the dominant aerosol formation process in the preindustrial boundary layer over land. The inclusion of this process in a global aerosol model raises baseline preindustrial aerosol concentrations and could lead to a reduction of 27% in estimates of anthropogenic aerosol radiative forcing.
Publisher: American Geophysical Union (AGU)
Date: 25-04-2020
DOI: 10.1029/2020GL087141
Publisher: Elsevier BV
Date: 07-2008
Publisher: Proceedings of the National Academy of Sciences
Date: 12-09-2011
Abstract: Historical records show that the A.D. 1783–1784 Laki eruption in Iceland caused severe environmental stress and posed a health hazard far beyond the borders of Iceland. Given the reasonable likelihood of such an event recurring, it is important to assess the scale on which a future eruption could impact society. We quantify the potential health effects caused by an increase in air pollution during a future Laki-style eruption using a global aerosol model together with concentration-response functions derived from current epidemiological studies. The concentration of particulate matter with diameters smaller than 2.5 µm is predicted to double across central, western, and northern Europe during the first 3 mo of the eruption. Over land areas of Europe, the current World Health Organization 24-h air quality guideline for particulate matter with diameters smaller than 2.5 µm is exceeded an additional 36 d on average over the course of the eruption. Based on the changes in particulate air pollution, we estimate that approximately 142,000 additional cardiopulmonary fatalities (with a 95% confidence interval of 52,000–228,000) could occur in Europe. In terms of air pollution, such a volcanic eruption would therefore be a severe health hazard, increasing excess mortality in Europe on a scale that likely exceeds excess mortality due to seasonal influenza.
Publisher: American Geophysical Union (AGU)
Date: 18-01-2019
DOI: 10.1029/2018JD028675
Publisher: Copernicus GmbH
Date: 16-02-2023
DOI: 10.5194/EGUSPHERE-2023-77
Abstract: Abstract. Aerosol radiative forcing uncertainty affects estimates of climate sensitivity and limits model skill at making climate projections. Efforts to improve the representations of physical processes in climate models, including extensive comparisons with observations, have not significantly constrained the range of possible aerosol forcing values. A far stronger constraint, in particular for the lower (most-negative) bound, can be achieved using global mean energy-balance arguments based on observed changes in historical temperature. Here, we show that structural deficiencies in a climate model, revealed as inconsistencies among observationally constrained cloud properties in the model, limit the effectiveness of observational constraint of the uncertain physical processes. We s le uncertainty in 37 model parameters related to aerosols, clouds and radiation in a perturbed parameter ensemble of the UK Earth System Model and evaluate 1 million model variants (different parameter settings from Gaussian Process emulators) against satellite-derived observations over several cloudy regions. We show that it is possible to reduce the parametric uncertainty in global mean aerosol forcing by more than 50 %, constraining it to a range in close agreement with energy-balance constraints (around −1.3 to −0.1 W m−2). However, our analysis of a very large set of model variants exposes model internal inconsistencies that would not be apparent in a small set of model simulations. Incorporating observations associated with these inconsistencies weakens the forcing constraint because they require a wider range of parameter values to accommodate conflicting information. Our estimated aerosol forcing range is the maximum feasible constraint using our structurally imperfect model and the chosen observations. Structural model developments targeted at the identified inconsistencies would enable a larger set of observations to be used for constraint, which would then narrow the uncertainty further. Such an approach provides a rigorous pathway to improved model realism and reduced uncertainty that has so far not been achieved through the normal model development approach.
Publisher: Copernicus GmbH
Date: 08-08-2023
Abstract: Abstract. Aerosol radiative forcing uncertainty affects estimates of climate sensitivity and limits model skill in terms of making climate projections. Efforts to improve the representations of physical processes in climate models, including extensive comparisons with observations, have not significantly constrained the range of possible aerosol forcing values. A far stronger constraint, in particular for the lower (most-negative) bound, can be achieved using global mean energy balance arguments based on observed changes in historical temperature. Here, we show that structural deficiencies in a climate model, revealed as inconsistencies among observationally constrained cloud properties in the model, limit the effectiveness of observational constraint of the uncertain physical processes. We s le the uncertainty in 37 model parameters related to aerosols, clouds, and radiation in a perturbed parameter ensemble of the UK Earth System Model and evaluate 1 million model variants (different parameter settings from Gaussian process emulators) against satellite-derived observations over several cloudy regions. Our analysis of a very large set of model variants exposes model internal inconsistencies that would not be apparent in a small set of model simulations, of an order that may be evaluated during model-tuning efforts. Incorporating observations associated with these inconsistencies weakens any forcing constraint because they require a wider range of parameter values to accommodate conflicting information. We show that, by neglecting variables associated with these inconsistencies, it is possible to reduce the parametric uncertainty in global mean aerosol forcing by more than 50 %, constraining it to a range (around −1.3 to −0.1 W m−2) in close agreement with energy balance constraints. Our estimated aerosol forcing range is the maximum feasible constraint using our structurally imperfect model and the chosen observations. Structural model developments targeted at the identified inconsistencies would enable a larger set of observations to be used for constraint, which would then very likely narrow the uncertainty further and possibly alter the central estimate. Such an approach provides a rigorous pathway to improved model realism and reduced uncertainty that has so far not been achieved through the normal model development approach.
Publisher: Copernicus GmbH
Date: 23-03-2022
DOI: 10.5194/ESD-2022-11
Abstract: Abstract. An observed southward shift in tropical rainfall over land between 1950 and 1985, followed by a weaker recovery post 1985, has been attributed to anthropogenic aerosol radiative forcing and cooling of the Northern Hemisphere relative to the Southern Hemisphere. We might therefore expect models that have a strong historic hemispheric contrast in aerosol forcing to simulate a further northward tropical rainfall shift in the near-term future when anthropogenic aerosol emission reductions will predominantly warm the Northern Hemisphere. We investigate this paradigm using a perturbed parameter ensemble (PPE) of transient coupled ocean-atmosphere climate simulations that span a range of aerosol radiative forcing comparable to multi-model studies. In the 20th century, in our single-model ensemble, we find no relationship between the magnitude of pre-industrial to 1975 inter-hemispheric anthropogenic aerosol radiative forcing and tropical precipitation shifts. Instead, tropical precipitation shifts are associated with major volcanic eruptions and are strongly affected by internal variability. However, we do find a relationship between the magnitude of pre-industrial to 2005 inter-hemispheric anthropogenic aerosol radiative forcing and future tropical precipitation shifts over 2006 to 2060 under scenario RCP8.5. Our results suggest that projections of tropical precipitation shifts will be improved by reducing aerosol radiative forcing uncertainty, but predictive gains may be offset by temporary shifts in tropical precipitation caused by future major volcanic eruptions.
Publisher: Springer Science and Business Media LLC
Date: 25-05-2016
DOI: 10.1038/NATURE17953
Abstract: Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood 1 . Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours 2 . It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere 3,4 , and that ions have a relatively minor role 5 . Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded 6,7 . Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.
Publisher: Copernicus GmbH
Date: 25-03-2020
Publisher: Springer Science and Business Media LLC
Date: 06-10-2013
DOI: 10.1038/NATURE12663
Publisher: American Geophysical Union (AGU)
Date: 11-2019
DOI: 10.1029/2019MS001628
Abstract: Tropospheric aerosol radiative forcing has persisted for many years as one of the major causes of uncertainty in global climate model simulations. To s le the range of plausible aerosol and atmospheric states and perform robust statistical analyses of the radiative forcing, it is important to account for the combined effects of many sources of model uncertainty, which is rarely done due to the high computational cost. This paper describes the designs of two ensembles of the Met Office Hadley Centre Global Environment Model‐U.K. Chemistry and Aerosol global climate model and provides the first analyses of the uncertainties in aerosol radiative forcing and their causes. The first ensemble was designed to comprehensively s le uncertainty in the aerosol state, while the other s les additional uncertainties in the physical model related to clouds, humidity, and radiation, thereby allowing an analysis of uncertainty in the aerosol effective radiative forcing. Each ensemble consists of around 200 simulations of the preindustrial and present‐day atmospheres. The uncertainty in aerosol radiative forcing in our ensembles is comparable to the range of estimates from multimodel intercomparison projects. The mean aerosol effective radiative forcing is −1.45 W/m 2 (credible interval of −2.07 to −0.81 W/m 2 ), which encompasses but is more negative than the −1.17 W/m 2 in the 2013 Atmospheric Chemistry and Climate Model Intercomparison Project and −0.90 W/m 2 in the Intergovernmental Panel on Climate Change Fifth Assessment Report. The ensembles can be used to reduce aerosol radiative forcing uncertainty by challenging them with multiple measurements as well as to isolate potential causes of multimodel differences.
Publisher: Copernicus GmbH
Date: 11-04-2023
DOI: 10.5194/EGUSPHERE-2023-604
Abstract: Abstract. Anthropogenic emissions of aerosols and precursor compounds are known to significantly affect the energy balance of the Earth-atmosphere system, alter the formation of clouds and precipitation, and have substantial impact on human health and the environment. Global models are an essential tool for examining the impacts of these emissions. In this study, we examine the sensitivity of model results to the assumed height of SO2 injection, seasonality of SO2 and BC emissions, and the assumed fraction of SO2 emissions that is injected into the atmosphere as SO4 in 11 climate and chemistry models, including both chemical transport models and the atmospheric component of Earth system models. We find a large variation in atmospheric lifetime across models for SO2, SO4, and BC, with a particularly large relative variation for SO2, which indicates that fundamental aspects of atmospheric sulfur chemistry remain uncertain. Of the perturbations examined in this study, the assumed height of SO2 injection had the largest overall impacts, particularly on global mean net radiative flux (maximum difference of -0.35 W m-2), SO2 lifetime over northern hemisphere land (maximum difference of 0.8 days), surface SO2 concentration (up to 59 % decrease), and surface sulfate concentration (up to 23 % increase). Emitting SO2 at height consistently increased SO2 and SO4 column burdens and shortwave cooling, with varying magnitudes, but had inconsistent effects across models on the sign of the change in implied cloud forcing. The assumed SO4 emission fraction also had a significant impact on net radiative flux and surface sulfate concentration. Because these properties are not standardized across models this is a source of inter-model ersity typically neglected in model intercomparisons. These results imply a need to assure that anthropogenic emission injection height and SO4 emission fraction are accurately and consistently represented in global models.
Publisher: Copernicus GmbH
Date: 25-08-2015
Abstract: Abstract. Substantial changes in anthropogenic aerosols and precursor gas emissions have occurred over recent decades due to the implementation of air pollution control legislation and economic growth. The response of atmospheric aerosols to these changes and the impact on climate are poorly constrained, particularly in studies using detailed aerosol chemistry–climate models. Here we compare the HadGEM3-UKCA (Hadley Centre Global Environment Model-United Kingdom Chemistry and Aerosols) coupled chemistry–climate model for the period 1960–2009 against extensive ground-based observations of sulfate aerosol mass (1978–2009), total suspended particle matter (SPM, 1978–1998), PM10 (1997–2009), aerosol optical depth (AOD, 2000–2009), aerosol size distributions (2008–2009) and surface solar radiation (SSR, 1960–2009) over Europe. The model underestimates observed sulfate aerosol mass (normalised mean bias factor (NMBF) = −0.4), SPM (NMBF = −0.9), PM10 (NMBF = −0.2), aerosol number concentrations (N30 NMBF = −0.85 N50 NMBF = −0.65 and N100 NMBF = −0.96) and AOD (NMBF = −0.01) but slightly overpredicts SSR (NMBF = 0.02). Trends in aerosol over the observational period are well simulated by the model, with observed (simulated) changes in sulfate of −68 % (−78 %), SPM of −42 % (−20 %), PM10 of −9 % (−8 %) and AOD of −11 % (−14 %). Discrepancies in the magnitude of simulated aerosol mass do not affect the ability of the model to reproduce the observed SSR trends. The positive change in observed European SSR (5 %) during 1990–2009 ("brightening") is better reproduced by the model when aerosol radiative effects (ARE) are included (3 %), compared to simulations where ARE are excluded (0.2 %). The simulated top-of-the-atmosphere aerosol radiative forcing over Europe under all-sky conditions increased by 3.0 W m−2 during the period 1970–2009 in response to changes in anthropogenic emissions and aerosol concentrations.
Publisher: Copernicus GmbH
Date: 21-11-2019
DOI: 10.5194/ACP-2019-834
Abstract: Abstract. The effect of observational constraint on the ranges of uncertain physical and chemical process parameters was explored in a global aerosol–climate model. The study uses 1 million variants of the HadGEM3-UKCA climate model that s le 26 sources of uncertainty, together with over 9000 monthly aggregated grid-box measurements of aerosol optical depth, PM2.5, particle number concentrations, sulphate and organic mass concentrations. Despite many compensating effects in the model, the procedure constrains the probability distributions of parameters related to secondary organic aerosol, anthropogenic SO2 emissions, residential emissions, sea spray emissions, dry deposition rates of SO2 and aerosols, new particle formation, cloud droplet pH and the diameter of primary combustion particles. Observational constraint rules out nearly 98 % of the model variants. On constraint, the ± 1σ (standard deviation) range of global annual mean direct radiative forcing, RFari, is reduced by 33 % to −0.14 to −0.26 W m−2, and the 95 % credible interval (CI) is reduced by 34 % to −0.1 to −0.32 W m−2. For the global annual mean aerosol–cloud radiative forcing, RFaci, the ± 1σ range is reduced by 7 % to −1.66 to −2.48 W m−2, and the 95 % CI by 6 % to −1.28 to −2.88 W m−2. The tightness of the constraint is limited by parameter cancellation effects (model equifinality) as well as the large and poorly defined representativeness error associated with comparing point measurements with a global model. The constraint could also be narrowed if model structural errors that prevent simultaneous agreement with different measurement types in multiple locations and seasons could be improved. For ex le, constraints using either sulphate or PM2.5 measurements in idually result in RFari ± 1σ ranges that only just overlap, which shows that emergent constraints based on one measurement type may be over-confident.
Publisher: Copernicus GmbH
Date: 15-11-2019
DOI: 10.5194/ACP-2019-755
Abstract: Abstract. In the present-day atmosphere, sulfuric acid is the most important vapour for aerosol particle formation and initial growth. However, the growth rates of nanoparticles (
Publisher: Copernicus GmbH
Date: 22-05-2012
Abstract: Abstract. In the most advanced aerosol-climate models it is common to represent the aerosol particle size distribution in terms of several log-normal modes. This approach, motivated by computational efficiency, makes assumptions about the shape of the particle distribution that may not always capture the properties of global aerosol. Here, a global modal aerosol microphysics module (GLOMAP-mode) is evaluated and improved by comparing against a sectional version (GLOMAP-bin) and observations in the same 3-D global offline chemistry transport model. With both schemes, the model captures the main features of the global particle size distribution, with sub-micron aerosol approximately unimodal in continental regions and bi-modal in marine regions. Initial bin-mode comparisons showed that the current values for two size distribution parameter settings in the modal scheme (mode widths and inter-modal separation sizes) resulted in clear biases compared to the sectional scheme. By adjusting these parameters in the modal scheme, much better agreement is achieved against the bin scheme and observations. Annual mean surface-level mass of sulphate, sea-salt, black carbon (BC) and organic carbon (OC) are within 25% in the two schemes in nearly all regions. Surface level concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), surface area density and condensation sink also compare within 25% in most regions. However, marine CCN concentrations between 30° N and 30° S are systematically 25–60% higher in the modal model, which we attribute to differences in size-resolved particle growth or cloud-processing. Larger differences also exist in regions or seasons dominated by biomass burning and in free-troposphere and high-latitude regions. Indeed, in the free-troposphere, GLOMAP-mode BC is a factor 2–4 higher than GLOMAP-bin, likely due to differences in size-resolved scavenging. Nevertheless, in most parts of the atmosphere, we conclude that bin-mode differences are much less than model-observation differences, although some processes are missing in these runs which may pose a bigger challenge to modal schemes (e.g., boundary layer nucleation and ultra-fine sea-spray). The findings here underline the need for a spectrum of complexity in global models, with size-resolved aerosol properties predicted by modal schemes needing to be continually benchmarked and improved against freely evolving sectional schemes and observations.
Publisher: American Geophysical Union (AGU)
Date: 08-2006
DOI: 10.1029/2006GL025986
Publisher: Copernicus GmbH
Date: 13-07-2018
Abstract: Abstract. Changes in aerosols cause a change in net top-of-the-atmosphere (ToA) short-wave and long-wave radiative fluxes rapid adjustments in clouds, water vapour and temperature and an effective radiative forcing (ERF) of the planetary energy budget. The erse sources of model uncertainty and the computational cost of running climate models make it difficult to isolate the main causes of aerosol ERF uncertainty and to understand how observations can be used to constrain it. We explore the aerosol ERF uncertainty by using fast model emulators to generate a very large set of aerosol–climate model variants that span the model uncertainty due to 27 parameters related to atmospheric and aerosol processes. Sensitivity analyses shows that the uncertainty in the ToA flux is dominated (around 80 %) by uncertainties in the physical atmosphere model, particularly parameters that affect cloud reflectivity. However, uncertainty in the change in ToA flux caused by aerosol emissions over the industrial period (the aerosol ERF) is controlled by a combination of uncertainties in aerosol (around 60 %) and physical atmosphere (around 40 %) parameters. Four atmospheric and aerosol parameters account for around 80 % of the uncertainty in short-wave ToA flux (mostly parameters that directly scale cloud reflectivity, cloud water content or cloud droplet concentrations), and these parameters also account for around 60 % of the aerosol ERF uncertainty. The common causes of uncertainty mean that constraining the modelled planetary brightness to tightly match satellite observations changes the lower 95 % credible aerosol ERF value from −2.65 to −2.37 W m−2. This suggests the strongest forcings (below around −2.4 W m−2) are inconsistent with observations. These results show that, regardless of the fact that the ToA flux is 2 orders of magnitude larger than the aerosol ERF, the observed flux can constrain the uncertainty in ERF because their values are connected by constrainable process parameters. The key to reducing the aerosol ERF uncertainty further will be to identify observations that can additionally constrain in idual parameter ranges and/or combined parameter effects, which can be achieved through sensitivity analysis of perturbed parameter ensembles.
Publisher: Wiley
Date: 30-01-2020
Publisher: Copernicus GmbH
Date: 23-03-2022
Publisher: Copernicus GmbH
Date: 28-03-2022
DOI: 10.5194/EGUSPHERE-EGU22-12007
Abstract: & & & span xml:lang=& quot EN-US& quot data-contrast=& quot auto& quot & & span data-ccp-parastyle-defn='{& quot ObjectId& quot :& quot c112871-d111-4339-b713-ce16d1de72eb124& quot ,& quot ClassId& quot :1073872969,& quot Properties& quot :[469775450,& quot Text body& quot ,201340122,& quot & quot ,134233614,& quot true& quot ,469778129,& quot Textbody& quot ,335559740,& quot & quot ,201341983,& quot & quot ,335559739,& quot & quot ,469778324,& quot Normal& quot ]}'& The transition from stratocumulus& /span& & span& to& /span& & span& cumulus clouds that takes place & /span& & span& as air is advected from the subtropics towards the equator causes a decrease in cloud radiative effect& /span& & span& , with cloud fraction halving from start to finish. & /span& & span& The transition is initiated by & /span& & span& increas& /span& & span& ing sea surface temperatures& /span& & span& , and & /span& & span& it is widely agreed that & /span& & span& the lower tropospheric stability plays a key role in the tim& /span& & span& ing of the transition.& /span& & span& In this work, we study the relative importance of five atmospheric initial cond& /span& & span& itions& /span& & span& :& /span& & span& specific humidity in the boundary layer and free troposphere, free tropospheric potential temperature, inversion height and initial aerosol distribution. & /span& & span& We& /span& & span& simulate& /span& & span& a & /span& & span& Lagrangian& /span& & span& trajectory of a stratocumulus-to-cumulus transition, & /span& & /span& & span xml:lang=& quot EN-GB& quot data-contrast=& quot none& quot & & span& using the Met Office/NERC cloud model coupled with a & /span& & span& bulk microphysics scheme and a radiation scheme. & /span& & span& From this base simulation we & /span& & span& make 60 perturbations to simulate the transition under different combinations of & /span& & span& the & /span& & span& atmospheric & /span& & span& initial & /span& & span& conditions& /span& & span& mentioned& /span& & span& . & /span& & /span& & span xml:lang=& quot EN-US& quot data-contrast=& quot auto& quot & & span& Additionally, we include a model parameter from the & /span& & span& Khairoutdinov& /span& & span& and Kogan & /span& & span& autoconversion& /span& & span& arameterisation& /span& & span& from 2000.& /span& & /span& & span xml:lang=& quot EN-GB& quot data-contrast=& quot none& quot & & span& We discuss here the relative importance of these so-called parameters, in particular the role of aerosol, and we explore whether a much faster transition by drizzle takes place in simulations with lower aerosol concentrations.& /span& & /span& & span& & & /span& & &
Publisher: Copernicus GmbH
Date: 21-12-2020
Abstract: Abstract. We document and evaluate the aerosol schemes as implemented in the physical and Earth system models, the Global Coupled 3.1 configuration of the Hadley Centre Global Environment Model version 3 (HadGEM3-GC3.1) and the United Kingdom Earth System Model (UKESM1), which are contributing to the sixth Coupled Model Intercomparison Project (CMIP6). The simulation of aerosols in the present-day period of the historical ensemble of these models is evaluated against a range of observations. Updates to the aerosol microphysics scheme are documented as well as differences in the aerosol representation between the physical and Earth system configurations. The additional Earth system interactions included in UKESM1 lead to differences in the emissions of natural aerosol sources such as dimethyl sulfide, mineral dust and organic aerosol and subsequent evolution of these species in the model. UKESM1 also includes a stratospheric–tropospheric chemistry scheme which is fully coupled to the aerosol scheme, while GC3.1 employs a simplified aerosol chemistry mechanism driven by prescribed monthly climatologies of the relevant oxidants. Overall, the simulated speciated aerosol mass concentrations compare reasonably well with observations. Both models capture the negative trend in sulfate aerosol concentrations over Europe and the eastern United States of America (US) although the models tend to underestimate sulfate concentrations in both regions. Interactive emissions of biogenic volatile organic compounds in UKESM1 lead to an improved agreement of organic aerosol over the US. Simulated dust burdens are similar in both models despite a 2-fold difference in dust emissions. Aerosol optical depth is biased low in dust source and outflow regions but performs well in other regions compared to a number of satellite and ground-based retrievals of aerosol optical depth. Simulated aerosol number concentrations are generally within a factor of 2 of the observations, with both models tending to overestimate number concentrations over remote ocean regions, apart from at high latitudes, and underestimate over Northern Hemisphere continents. Finally, a new primary marine organic aerosol source is implemented in UKESM1 for the first time. The impact of this new aerosol source is evaluated. Over the pristine Southern Ocean, it is found to improve the seasonal cycle of organic aerosol mass and cloud droplet number concentrations relative to GC3.1 although underestimations in cloud droplet number concentrations remain. This paper provides a useful characterisation of the aerosol climatology in both models and will facilitate understanding in the numerous aerosol–climate interaction studies that will be conducted as part of CMIP6 and beyond.
Publisher: Copernicus GmbH
Date: 08-03-2013
Abstract: Abstract. The atmospheric oxidation of dimethyl-sulphide (DMS) derived from marine phytoplankton is a significant source of marine sulphate aerosol. DMS has been proposed to regulate climate via changes in cloud properties, though recent studies have shown that present-day global cloud condensation nuclei (CCN) concentrations have only a weak dependence on the total emission flux of DMS. Here, we use a global aerosol microphysics model to examine how efficiently CCN are produced when DMS emissions are changed in different marine regions. We find that global CCN production per unit mass of sulphur emitted varies by more than a factor of 20 depending on where the change in oceanic DMS emission flux is applied. The variation in CCN production efficiency depends upon where CCN production processes (DMS oxidation, SO2 oxidation, nucleation and growth) are most efficient and removal processes (deposition) least efficient. The analysis shows that the production of aerosol sulphate through aqueous-phase oxidation of SO2 limits the amount of H2SO4 available for nucleation and condensational growth and therefore suppresses CCN formation, leading to the weak response of CCN to changes in DMS emission. Our results show that past and future changes in the spatial distribution of DMS emissions (through changes in the phytoplankton population or wind speed patterns) could exert a stronger control on climate than net increases in biological productivity.
Publisher: Springer Science and Business Media LLC
Date: 12-06-2013
DOI: 10.1038/NATURE12278
Abstract: The amount of ice present in mixed-phase clouds, which contain both supercooled liquid water droplets and ice particles, affects cloud extent, lifetime, particle size and radiative properties. The freezing of cloud droplets can be catalysed by the presence of aerosol particles known as ice nuclei. One of the most important ice nuclei is thought to be mineral dust aerosol from arid regions. It is generally assumed that clay minerals, which contribute approximately two-thirds of the dust mass, dominate ice nucleation by mineral dust, and many experimental studies have therefore focused on these materials. Here we use an established droplet-freezing technique to show that feldspar minerals dominate ice nucleation by mineral dusts under mixed-phase cloud conditions, despite feldspar being a minor component of dust emitted from arid regions. We also find that clay minerals are relatively unimportant ice nuclei. Our results from a global aerosol model study suggest that feldspar ice nuclei are globally distributed and that feldspar particles may account for a large proportion of the ice nuclei in Earth's atmosphere that contribute to freezing at temperatures below about -15 °C.
Publisher: Springer Science and Business Media LLC
Date: 11-2013
DOI: 10.1038/NATURE12674
Abstract: The effect of anthropogenic aerosols on cloud droplet concentrations and radiative properties is the source of one of the largest uncertainties in the radiative forcing of climate over the industrial period. This uncertainty affects our ability to estimate how sensitive the climate is to greenhouse gas emissions. Here we perform a sensitivity analysis on a global model to quantify the uncertainty in cloud radiative forcing over the industrial period caused by uncertainties in aerosol emissions and processes. Our results show that 45 per cent of the variance of aerosol forcing since about 1750 arises from uncertainties in natural emissions of volcanic sulphur dioxide, marine dimethylsulphide, biogenic volatile organic carbon, biomass burning and sea spray. Only 34 per cent of the variance is associated with anthropogenic emissions. The results point to the importance of understanding pristine pre-industrial-like environments, with natural aerosols only, and suggest that improved measurements and evaluation of simulated aerosols in polluted present-day conditions will not necessarily result in commensurate reductions in the uncertainty of forcing estimates.
Publisher: Copernicus GmbH
Date: 23-03-2020
DOI: 10.5194/EGUSPHERE-EGU2020-10202
Abstract: & & Anthropogenic aerosol emissions over the industrial period have caused a negative but highly uncertain radiative forcing. This negative radiative forcing has had a cooling effect mainly over the northern hemisphere, affecting the atmospheric interhemispheric energy balance. Consequently aerosols have been linked to observed dynamical responses over the industrial period that depend on the atmospheric interhemispheric energy balance, such as changes in the position of the Intertropical Convergence Zone (ITCZ) and resultant tropical precipitation shifts. However, over the course of the 21& sup& st& /sup& century anthropogenic aerosol emissions are predicted to decline. The reduction in anthropogenic aerosol emissions will cause a positive radiative forcing relative to present day, creating a warming effect in the northern hemisphere. Hence, if the strength of aerosol radiative forcing modulates the magnitude of shifts in the ITCZ, then the large uncertainty in aerosol radiative forcing will limit our understanding of how tropical precipitation will shift in the near-term future.& & & & We use a perturbed parameter ensemble (PPE) of a global coupled climate model to investigate the link between aerosol radiative forcing and ITCZ and tropical rainfall shifts in the near-term future. The PPE consists of 20 simulations of the UK Met Office& #8217 s GC3.05 model with parameters perturbed from a range of model schemes. The ensemble was designed to s le uncertainties in future changes, and as a result spans a range of aerosol radiative forcings.& & & & The PPE reveals both northward and southwards shifts in the ITCZ position across the ensemble in the latter half of the 20& sup& th& /sup& century and first half of the 21& sup& st& /sup& century, as well as changes in width and intensity of the ITCZ. We find a correlation between the shift in the ITCZ position and the magnitude of aerosol radiative forcing and AOD trends. However, the correlations in our ensemble are not as strong as those cited in previous studies that use multi-model ensembles. The potential causes of this difference are investigated. We also compare our model output to aerosol, cloud and radiation observations in attempt to identify the most plausible future aerosol-driven climate responses.& &
Publisher: Copernicus GmbH
Date: 15-11-2019
Publisher: Copernicus GmbH
Date: 19-08-2011
Abstract: Abstract. Observations show that the fractional solubility of Fe (FS-Fe, percentage of dissolved to total Fe) in dust aerosol increases considerably from 0.1 % in regions of high dust mass concentration to 80 % in remote regions where concentrations are low. Here, we combined laboratory geochemical measurements with global aerosol model simulations to test the hypothesis that the increase in FS-Fe is due to physical size sorting during transport. We determined the FS-Fe and fractional solubility of Al (FS-Al) in size-fractionated dust generated from two representative soil s les collected from known Saharan dust source regions using a customized dust re-suspension and collection system. The results show that the FS-Fe is size-dependent and ranges from 0.1–0.3 % in the coarse size fractions ( μm) to ~0.2–0.8 % in the fine size fractions ( μm). The FS-Al shows a similar size distribution to that of the FS-Fe. The size-resolved FS-Fe data were then combined with simulated dust mass concentration and size distribution data from a global aerosol model, GLOMAP, to calculate the FS-Fe of dust aerosol over the tropical and subtropical North Atlantic Ocean. We find that the calculated FS-Fe in the dust aerosol increases systematically from ~0.1 % at high dust mass concentrations (e.g., μg m−3) to ~0.2 % at low concentrations ( μg m–3) due to physical size sorting (i.e., particle gravitational settling). These values are one to two orders of magnitude smaller than those observed on cruises across the tropical and sub-tropical North Atlantic Ocean under an important pathway of Saharan dust plumes for similar dust mass concentrations. Even when the FS-Fe of sub-micrometer size fractions (0.18–0.32 μm, 0.32–0.56 μm, and 0.56–1.0 μm) in the model is increased by a factor of 10 over the measured values, the calculated FS-Fe of the dust is still more than an order of magnitude lower than that measured in the field. Therefore, the physical sorting of dust particles alone is unlikely to be an important factor in the observed inverse relationship between the FS-Fe and FS-Al and the atmospheric mineral dust mass concentrations. The results suggest that processes such as chemical reactions and/or mixing with combustion particles are the main mechanisms to cause the increased FS-Fe in long-range transported dust aerosols.
Publisher: American Association for the Advancement of Science (AAAS)
Date: 07-12-2018
Abstract: Atmospheric aerosol formation from biogenic vapors is strongly affected by air pollutants, like NO x , SO 2 , and NH 3 .
Publisher: American Geophysical Union (AGU)
Date: 12-2019
DOI: 10.1029/2019MS001739
Location: United Kingdom of Great Britain and Northern Ireland
Location: United Kingdom of Great Britain and Northern Ireland
Location: United Kingdom of Great Britain and Northern Ireland
No related grants have been discovered for Ken Carslaw.