ALBERT

Description: Although quantitative isotope data from speleothems has been used to evaluate isotope-enabled model simulations, currently no consensus exists regarding the most appropriate methodology through which to achieve this. A number of modelling groups will be running isotope-enabled palaeoclimate simulations in the framework of the Coupled Model Intercomparison Project Phase 6, so it is timely to evaluate different approaches to using the speleothem data for data–model comparisons. Here, we illustrate this using 456 globally distributed speleothem δ18O records from an updated version of the Speleothem Isotopes Synthesis and Analysis (SISAL) database and palaeoclimate simulations generated using the ECHAM5-wiso isotope-enabled atmospheric circulation model. We show that the SISAL records reproduce the first-order spatial patterns of isotopic variability in the modern day, strongly supporting the application of this dataset for evaluating model-derived isotope variability into the past. However, the discontinuous nature of many speleothem records complicates the process of procuring large numbers of records if data–model comparisons are made using the traditional approach of comparing anomalies between a control period and a given palaeoclimate experiment. To circumvent this issue, we illustrate techniques through which the absolute isotope values during any time period could be used for model evaluation. Specifically, we show that speleothem isotope records allow an assessment of a model’s ability to simulate spatial isotopic trends. Our analyses provide a protocol for using speleothem isotope data for model evaluation, including screening the observations to take into account the impact of speleothem mineralogy on δ18O values, the optimum period for the modern observational baseline and the selection of an appropriate time window for creating means of the isotope data for palaeo-time-slices.

Description: Isoprene-derived secondary organic aerosol (iSOA) is a significant contributor to organic carbon (OC) in some forested regions, such as tropical rainforests and the Southeastern US. However, its contribution to organic aerosol in urban areas that have high levels of anthropogenic pollutants is poorly understood. In this study, we examined the formation of anthropogenically influenced iSOA during summer in Beijing, China. Local isoprene emissions and high levels of anthropogenic pollutants, in particular NOx and particulate SO42-, led to the formation of iSOA under both high- and low-NO oxidation conditions, with significant heterogeneous transformations of isoprene-derived oxidation products to particulate organosulfates (OSs) and nitrooxy-organosulfates (NOSs). Ultra-high-performance liquid chromatography coupled to high-resolution mass spectrometry was combined with a rapid automated data processing technique to quantify 31 proposed iSOA tracers in offline PM2.5 filter extracts. The co-elution of the inorganic ions in the extracts caused matrix effects that impacted two authentic standards differently. The average concentration of iSOA OSs and NOSs was 82.5 ng m−3, which was around 3 times higher than the observed concentrations of their oxygenated precursors (2-methyltetrols and 2-methylglyceric acid). OS formation was dependant on both photochemistry and the sulfate available for reactive uptake, as shown by a strong correlation with the product of ozone (O3) and particulate sulfate (SO42-). A greater proportion of high-NO OS products were observed in Beijing compared with previous studies in less polluted environments. The iSOA-derived OSs and NOSs represented 0.62 % of the oxidized organic aerosol measured by aerosol mass spectrometry on average, but this increased to ∼3 % on certain days. These results indicate for the first time that iSOA formation in urban Beijing is strongly controlled by anthropogenic emissions and results in extensive conversion to OS products from heterogenous reactions.

Description: In recent decades, rapid ice shelf disintegration along the Antarctic Peninsula has had a global impact through enhancing outlet glacier flow and hence sea level rise and the freshening of Antarctic Bottom Water. Ice shelf thinning due to basal melting results from the circulation of relatively warm water in the underlying ocean cavity. However, the effect of sub-shelf circulation on future ice shelf stability cannot be predicted accurately with computer simulations if the geometry of the ice shelf cavity is unknown. To address this deficit for Larsen C Ice Shelf, West Antarctica, we integrate new water column thickness measurements from recent seismic campaigns with existing observations. We present these new data here along with an updated bathymetry grid of the ocean cavity. Key findings include a relatively deep seabed to the southeast of the Kenyon Peninsula, along the grounding line and around the key ice shelf pinning-point of Bawden Ice Rise. In addition, we can confirm that the cavity's southern trough stretches from Mobiloil Inlet to the open ocean. These areas of deep seabed will influence ocean circulation and tidal mixing and will therefore affect the basal-melt distribution. These results will help constrain models of ice shelf cavity circulation with the aim of improving our understanding of sub-shelf processes and their potential influence on ice shelf stability. The datasets are comprised of all the new point measurements of seabed depth. We present the new depth measurements here, as well as a compilation of previously published measurements. To demonstrate the improvements to the sub-shelf bathymetry map that these new data provide we include a gridded data product in the Supplement of this paper, derived using the additional measurements of both offshore seabed depth and the thickness of grounded ice. The underlying seismic datasets that were used to determine bed depth and ice thickness are available at https://doi.org/10.5285/315740B1-A7B9-4CF0-9521-86F046E33E9A (Brisbourne et al., 2019), https://doi.org/10.5285/5D63777D-B375-4791-918F-9A5527093298 (Booth, 2019), https://doi.org/10.5285/FFF8AFEE-4978-495E-9210-120872983A8D (Kulessa and Bevan, 2019) and https://doi.org/10.5285/147BAF64-B9AF-4A97-8091-26AEC0D3C0BB (Booth et al., 2019).

Description: The scientific career of Michael Rycroft (born in 1938) spans the space age, during which significant changes have occurred in how scientists work, experiment, and interact. Here, as part of his 80th birthday celebrations, we review his career to date in terms of the social and structural changes in collaborative international science. His contributions to research, teaching, and management across solar–terrestrial and ionospheric physics as well as atmospheric and space science are also discussed.

Description: We present a new global reconstruction of seasonal climates at the Last Glacial Maximum (LGM, 21 000 years BP) made using 3-D variational data assimilation with pollen-based site reconstructions of six climate variables and the ensemble average of the PMIP3—CMIP5 simulations as a prior (initial estimate of LGM climate). We assume that the correlation matrix of the uncertainties in the prior is both spatially and temporally Gaussian, in order to produce a climate reconstruction that is smoothed both from month to month and from grid cell to grid cell. The pollen-based reconstructions include mean annual temperature (MAT), mean temperature of the coldest month (MTCO), mean temperature of the warmest month (MTWA), growing season warmth as measured by growing degree days above a baseline of 5 ∘C (GDD5), mean annual precipitation (MAP), and a moisture index (MI), which is the ratio of MAP to mean annual potential evapotranspiration. Different variables are reconstructed at different sites, but our approach both preserves seasonal relationships and allows a more complete set of seasonal climate variables to be derived at each location. We further account for the ecophysiological effects of low atmospheric carbon dioxide concentration on vegetation in making reconstructions of MAP and MI. This adjustment results in the reconstruction of wetter climates than might otherwise be inferred from the vegetation composition. Finally, by comparing the uncertainty contribution to the final reconstruction, we provide confidence intervals on these reconstructions and delimit geographical regions for which the palaeodata provide no information to constrain the climate reconstructions. The new reconstructions will provide a benchmark created using clear and defined mathematical procedures that can be used for evaluation of the PMIP4–CMIP6 entry-card LGM simulations and are available at https://doi.org/10.17864/1947.244 (Cleator et al., 2020b).

Description: The Southern Ocean and Antarctic region currently best represent one of the few places left on our planet with conditions similar to the preindustrial age. Currently, climate models have a low ability to simulate conditions forming the aerosol baseline; a major uncertainty comes from the lack of understanding of aerosol size distributions and their dynamics. Contrasting studies stress that primary sea salt aerosol can contribute significantly to the aerosol population, challenging the concept of climate biogenic regulation by new particle formation (NPF) from dimethyl sulfide marine emissions. We present a statistical cluster analysis of the physical characteristics of particle size distributions (PSDs) collected at Halley (Antarctica) for the year 2015 (89 % data coverage; 6–209 nm size range; daily size resolution). By applying the Hartigan–Wong k-mean method we find eight clusters describing the entire aerosol population. Three clusters show pristine average low particle number concentrations (

Description: Atmospheric aerosols contribute some of the greatest uncertainties to estimates of global radiative forcing and have significant effects on human health. New particle formation (NPF) is the process by which new aerosols of sub-2 nm diameter form from gas-phase precursors and contributes significantly to particle numbers in the atmosphere, accounting for approximately 50 % of cloud condensation nuclei globally. Here, we study summertime NPF in urban Barcelona in north-eastern Spain utilising particle counting instruments down to 1.9 nm and a Nitrate Chemical Ionisation Atmospheric Pressure interface Time of Flight Mass Spectrometer (CI-APi-ToF). The rate of formation of new particles is seen to increase linearly with sulfuric acid concentration, although particle formation rates fall short of chamber studies of H2SO4–DMA–H2O while exceeding those of H2SO4–BioOxOrg–H2O nucleation, although a role of highly oxygenated molecules (HOMs) cannot be ruled out. The sulfuric acid dimer : monomer ratio is significantly lower than that seen in experiments involving sulfuric acid and dimethylamine (DMA) in chambers, indicating that stabilisation of sulfuric acid clusters by bases is weaker in this dataset than in chambers, either due to rapid evaporation due to high summertime temperatures or limited pools of stabilising amines. Such a mechanism cannot be verified in these data, as no higher-order H2SO4–amine clusters nor H2SO4–HOM clusters were measured. The high concentrations of HOMs arise from isoprene, alkylbenzene, monoterpene and polycyclic aromatic hydrocarbon (PAH) oxidation, with alkylbenzenes providing greater concentrations of HOMs due to significant local sources. The concentration of these HOMs shows a dependence on temperature. The organic compounds measured primarily fall into the semivolatile organic compound (SVOC) volatility class arising from alkylbenzene and isoprene oxidation. Low-volatility organic compounds (LVOCs) largely arise from oxidation of alkylbenzenes, PAHs and monoterpenes, whereas extremely low-volatility organic compounds (ELVOCs) arise from primarily PAH and monoterpene oxidation. New particle formation without growth past 10 nm is also observed, and on these days oxygenated organic concentrations are lower than on days with growth by a factor of 1.6, and thus high concentrations of low-volatility oxygenated organics which primarily derive from traffic-emitted volatile organic compounds (VOCs) appear to be a necessary condition for the growth of newly formed particles in Barcelona. These results are consistent with prior observations of new particle formation from sulfuric acid–amine reactions in both chambers and the real atmosphere and are likely representative of the urban background of many European Mediterranean cities. A role for HOMs in the nucleation process cannot be confirmed or ruled out, and there is strong circumstantial evidence of the participation of HOMs across multiple volatility classes in particle growth.

Description: Global fire-vegetation models are widely used to assess impacts of environmental change on fire regimes and the carbon cycle and to infer relationships between climate, land use and fire. However, differences in model structure and parameterizations, in both the vegetation and fire components of these models, could influence overall model performance, and to date there has been limited evaluation of how well different models represent various aspects of fire regimes. The Fire Model Intercomparison Project (FireMIP) is coordinating the evaluation of state-of-the-art global fire models, in order to improve projections of fire characteristics and fire impacts on ecosystems and human societies in the context of global environmental change. Here we perform a systematic evaluation of historical simulations made by nine FireMIP models to quantify their ability to reproduce a range of fire and vegetation benchmarks. The FireMIP models simulate a wide range in global annual total burnt area (39–536 Mha) and global annual fire carbon emission (0.91–4.75 Pg C yr−1) for modern conditions (2002–2012), but most of the range in burnt area is within observational uncertainty (345–468 Mha). Benchmarking scores indicate that seven out of nine FireMIP models are able to represent the spatial pattern in burnt area. The models also reproduce the seasonality in burnt area reasonably well but struggle to simulate fire season length and are largely unable to represent interannual variations in burnt area. However, models that represent cropland fires see improved simulation of fire seasonality in the Northern Hemisphere. The three FireMIP models which explicitly simulate individual fires are able to reproduce the spatial pattern in number of fires, but fire sizes are too small in key regions, and this results in an underestimation of burnt area. The correct representation of spatial and seasonal patterns in vegetation appears to correlate with a better representation of burnt area. The two older fire models included in the FireMIP ensemble (LPJ–GUESS–GlobFIRM, MC2) clearly perform less well globally than other models, but it is difficult to distinguish between the remaining ensemble members; some of these models are better at representing certain aspects of the fire regime; none clearly outperforms all other models across the full range of variables assessed.

Description: A new set of stratospheric aerosol geoengineering (SAG) model experiments has been performed with Community Earth System Model version 2 (CESM2) with the Whole Atmosphere Community Climate Model (WACCM6) that are based on the Coupled Model Intercomparison Project phase 6 (CMIP6) overshoot scenario (SSP5-34-OS) as a baseline scenario to limit global warming to 1.5 or 2.0 ∘C above 1850–1900 conditions. The overshoot scenario allows us to applying a peak-shaving scenario that reduces the needed duration and amount of SAG application compared to a high forcing scenario. In addition, a feedback algorithm identifies the needed amount of sulfur dioxide injections in the stratosphere at four pre-defined latitudes, 30∘ N, 15∘ N, 15∘ S, and 30∘ S, to reach three surface temperature targets: global mean temperature, and interhemispheric and pole-to-Equator temperature gradients. These targets further help to reduce side effects, including overcooling in the tropics, warming of high latitudes, and large shifts in precipitation patterns. These experiments are therefore relevant for investigating the impacts on society and ecosystems. Comparisons to SAG simulations based on a high emission pathway baseline scenario (SSP5-85) are also performed to investigate the dependency of impacts using different injection amounts to offset surface warming by SAG. We find that changes from present-day conditions around 2020 in some variables depend strongly on the defined temperature target (1.5 ∘C vs. 2.0 ∘C). These include surface air temperature and related impacts, the Atlantic Meridional Overturning Circulation, which impacts ocean net primary productivity, and changes in ice sheet surface mass balance, which impacts sea level rise. Others, including global precipitation changes and the recovery of the Antarctic ozone hole, depend strongly on the amount of SAG application. Furthermore, land net primary productivity as well as ocean acidification depend mostly on the global atmospheric CO2 concentration and therefore the baseline scenario. Multi-model comparisons of experiments that include strong mitigation and carbon dioxide removal with some SAG application are proposed to assess the robustness of impacts on societies and ecosystems.

Description: Ice-nucleating particles (INPs) affect cloud development, lifetime, and radiative properties, hence it is important to know the abundance of INPs throughout the atmosphere. A critical factor in determining the lifetime and transport of INPs is their size; however very little size-resolved atmospheric INP concentration information exists. Here we present the development and application of a radio-controlled payload capable of collecting size-resolved aerosol from a tethered balloon for the primary purpose of offline INP analysis. This payload, known as the SHARK (Selective Height Aerosol Research Kit), consists of two complementary cascade impactors for aerosol size-segregation from 0.25 to 10 µm, with an after-filter and top stage to collect particles below and above this range at flow rates of up to 100 L min−1. The SHARK also contains an optical particle counter to quantify aerosol size distribution between 0.38 and 10 µm, and a radiosonde for the measurement of temperature, pressure, GPS altitude, and relative humidity. This is all housed within a weatherproof box, can be run from batteries for up to 11 h, and has a total weight of 9 kg. The radio control and live data link with the radiosonde allow the user to start and stop sampling depending on meteorological conditions and height, which can, for example, allow the user to avoid sampling in very humid or cloudy air, even when the SHARK is out of sight. While the collected aerosol could, in principle, be studied with an array of analytical techniques, this study demonstrates that the collected aerosol can be analysed with an offline droplet freezing instrument to determine size-resolved INP concentrations, activated fractions, and active site densities, producing similar results to those obtained using a standard PM10 aerosol sampler when summed over the appropriate size range. Test data, where the SHARK was sampling near ground level or suspended from a tethered balloon at 20 m altitude, are presented from four contrasting locations having very different size-resolved INP spectra: Hyytiälä (southern Finland), Leeds (northern England), Longyearbyen (Svalbard), and Cardington (southern England).