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As part of the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), we evaluate the historical black carbon (BC) aerosols simulated by 8 ACCMIP models against observations including 12 ice core records, long-term surface mass concentrations, and recent Arctic BC snowpack measurements. We also estimate BC albedo forcing by performing additional simulations using offline models with prescribed meteorology from 1996–2000. We evaluate the vertical profile of BC snow concentrations from these offline simulations using the recent BC snowpack measurements. <br><br> Despite using the same BC emissions, the global BC burden differs by approximately a factor of 3 among models due to differences in aerosol removal parameterizations and simulated meteorology: 34 Gg to 103 Gg in 1850 and 82 Gg to 315 Gg in 2000. However, the global BC burden from preindustrial to present-day increases by 2.5–3 times with little variation among models, roughly matching the 2.5-fold increase in total BC emissions during the same period. We find a large divergence among models at both Northern Hemisphere (NH) and Southern Hemisphere (SH) high latitude regions for BC burden and at SH high latitude regions for deposition fluxes. The ACCMIP simulations match the observed BC surface mass concentrations well in Europe and North America except at Ispra. However, the models fail to predict the Arctic BC seasonality due to severe underestimations during winter and spring. The simulated vertically resolved BC snow concentrations are, on average, within a factor of 2–3 of the BC snowpack measurements except for Greenland and the Arctic Ocean. <br><br> For the ice core evaluation, models tend to adequately capture both the observed temporal trends and the magnitudes at Greenland sites. However, models fail to predict the decreasing trend of BC depositions/ice core concentrations from the 1950s to the 1970s in most Tibetan Plateau ice cores. The distinct temporal trend at the Tibetan Plateau ice cores indicates a strong influence from Western Europe, but the modeled BC increases in that period are consistent with the emission changes in Eastern Europe, the Middle East, South and East Asia. At the Alps site, the simulated BC suggests a strong influence from Europe, which agrees with the Alps ice core observations. At Zuoqiupu on the Tibetan Plateau, models successfully simulate the higher BC concentrations observed during the non-monsoon season compared to the monsoon season but overpredict BC in both seasons. Despite a large divergence in BC deposition at two Antarctic ice core sites, some models with a BC lifetime of less than 7 days are able to capture the observed concentrations. <br><br> In 2000 relative to 1850, globally and annually averaged BC surface albedo forcing from the offline simulations ranges from 0.014 to 0.019 W m<sup>−2</sup> among the ACCMIP models. Comparing offline and online BC albedo forcings computed by some of the same models, we find that the global annual mean can vary by up to a factor of two because of different aerosol models or different BC-snow parameterizations and snow cover. The spatial distributions of the offline BC albedo forcing in 2000 show especially high BC forcing (i.e., over 0.1 W m<sup>−2</sup>) over Manchuria, Karakoram, and most of the Former USSR. Models predict the highest global annual mean BC forcing in 1980 rather than 2000, mostly driven by the high fossil fuel and biofuel emissions in the Former USSR in 1980.
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Characterizing chemical and physical aerosol properties is important to understand their sources, effects, and feedback mechanisms in the atmosphere. This study proposes a scheme to classify aerosol populations based on their spectral optical properties (absorption and scattering). The scheme is obtained thanks to the outstanding set of information on particle size and composition these properties contain. The spectral variability of the aerosol single scattering albedo (dSSA), and the extinction, scattering and absorption Angstrom exponents (EAE, SAE and AAE, respectively) were observed on the basis of two-year measurements of aerosol optical properties (scattering and absorption coefficients at blue, green and red wavelengths) performed in the suburbs of Rome (Italy). Optical measurements of various aerosol types were coupled to measurements of particle number size distributions and relevant optical properties simulations (Mie theory). These latter allowed the investigation of the role of the particle size and composition in the bulk aerosol properties observed. The combination of simulations and measurements suggested a general "paradigm" built on dSSA, SAE and AAE to optically classify aerosols. The paradigm proved suitable to identify the presence of key aerosol populations, including soot, biomass burning, organics, dust and marine particles. The work highlights that (i) aerosol populations show distinctive combinations of SAE and dSSA times AAE, these variables being linked by a linear inverse relation varying with varying SSA; (ii) fine particles show EAE > 1.5, whilst EAE < 2 is found for both coarse particles and ultrafine soot-rich aerosols; (iii) fine and coarse particles both show SSA > 0.8, whilst ultrafine urban Aitken mode and soot particles show SSA < 0.8. The proposed paradigm agrees with aerosol observations performed during past major field campaigns, this indicating that relations concerning the paradigm have a general validity.
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During four aircraft field experiments with the DLR research aircraft Falcon in 1998 (LACE), 2006 (SAMUM-1) and 2008 (SAMUM-2 and EUCAARI), airborne High Spectral Resolution Lidar (HSRL) and in situ measurements of aerosol microphysical and optical properties were performed. Altogether, the properties of six different aerosol types and aerosol mixtures – Saharan mineral dust, Saharan dust mixtures, Canadian biomass burning aerosol, African biomass burning mixture, anthropogenic pollution aerosol, and marine aerosol have been studied. On the basis of this extensive HSRL data set, we present an aerosol classification scheme which is also capable to identify mixtures of different aerosol types. We calculated mixing lines that allowed us to determine the contributing aerosol types. The aerosol classification scheme was supported by backward trajectory analysis and validated with in-situ measurements. Our results demonstrate that the developed aerosol mask is capable to identify complex stratifications with different aerosol types throughout the atmosphere.
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The impact of changes in aerosol and cloud droplet concentration (<i>N</i><sub>a</sub> and <i>N</i><sub>d</sub>) on the radiative forcing of stratocumulus-topped boundary layers (STBLs) has been widely studied. How these impacts compare to those due to variations in meteorological context has not been investigated in a systematic fashion for non-drizzling overcast stratocumulus. In this study we examine the impact of observed variations in meteorological context and aerosol state on daytime, non-drizzling overcast stratiform evolution, and determine how resulting changes in cloud properties compare. <br><br> Using large-eddy simulation (LES) we create a model base case of daytime southeast Pacific coastal stratocumulus, spanning a portion of the diurnal cycle (early morning to near noon) and constrained by observations taken during the VOCALS (VAMOS Ocean-Atmosphere-Land Study) field campaign. We perturb aerosol and meteorological properties around this base case to investigate the stratocumulus response. We determine perturbations in the cloud top jumps in potential temperature θ and total water mixing ratio <i>q</i><sub>t</sub> from ECMWF Re-analysis Interim data, and use a set of <i>N</i><sub>d</sub> values spanning the observable range. To determine the cloud response to these meteorological and aerosol perturbations, we compute changes in liquid water path (LWP), bulk optical depth (τ) and cloud radiative forcing (CRF). <br><br> We find that realistic variations in the thermodynamic jump properties can elicit a response in the cloud properties of τ and shortwave (SW) CRF that are on the same order of magnitude as the response found due to realistic changes in aerosol state (i.e <i>N</i><sub>d</sub>). In response to increases in <i>N</i><sub>d</sub>, the cloud layer in the base case thinned due to increases in evaporative cooling and entrainment rate. This cloud thinning somewhat mitigates the increase in τ resulting from increases in <i>N</i><sub>d</sub>. On the other hand, variations in θ and <i>q</i><sub>t</sub> jumps did not substantially modify <i>N</i><sub>d</sub>. The cloud layer thickens in response to an increase in the θ jump and thins in response to an increase in the <i>q</i><sub>t</sub> jump, both resulting in a τ and SW CRF response comparable to those found from perturbations in <i>N</i><sub>d</sub>. Longwave CRF was not substantially altered by the perturbations we tested. <br><br> We find that realistic variations in meteorological context can elicit a response in CRF and τ on the same order of magnitude as, and at times larger than, that response found due to realistic changes in aerosol state. We estimate the limits on variability of cloud top jump properties required for accurate observation of aerosol SW radiative impacts on stratocumulus, and find strict constraints: less than 1 K and 1 g kg<sup>−1</sup> in the early morning hours, and order 0.1 K and 0.1 g kg<sup>−1</sup> close to solar noon. These constraints suggest that accurately observing aerosol radiative impacts in stratocumulus may be challenging as co-variation of meteorological properties may obfuscate aerosol-cloud interactions.
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The new generation GISS climate model includes fully interactive chemistry related to ozone in historical and future simulations, and interactive methane in future simulations. Evaluation of ozone, its tropospheric precursors, and methane shows that the model captures much of the large-scale spatial structure seen in recent observations. While the model is much improved compared with the previous chemistry-climate model, especially for ozone seasonality in the stratosphere, there is still slightly too rapid stratospheric circulation, too little stratosphere-to-troposphere ozone flux in the Southern Hemisphere and an Antarctic ozone hole that is too large and persists too long. Quantitative metrics of spatial and temporal correlations with satellite datasets as well as spatial autocorrelation to examine transport and mixing are presented to document improvements in model skill and provide a benchmark for future evaluations. The difference in radiative forcing (RF) calculated using modeled tropospheric ozone versus tropospheric ozone observed by TES is only 0.016 W m<sup>−2</sup>. Historical 20th Century simulations show a steady increase in whole atmosphere ozone RF through 1970 after which there is a decrease through 2000 due to stratospheric ozone depletion. Ozone forcing increases throughout the 21st century under RCP8.5 owing to a projected recovery of stratospheric ozone depletion and increases in methane, but decreases under RCP4.5 and 2.6 due to reductions in emissions of other ozone precursors. RF from methane is 0.05 to 0.18 W m<sup>−2</sup> higher in our model calculations than in the RCP RF estimates. The surface temperature response to ozone through 1970 follows the increase in forcing due to tropospheric ozone. After that time, surface temperatures decrease as ozone RF declines due to stratospheric depletion. The stratospheric ozone depletion also induces substantial changes in surface winds and the Southern Ocean circulation, which may play a role in a slightly stronger response per unit forcing during later decades. Tropical precipitation shifts south during boreal summer from 1850 to 1970, but then shifts northward from 1970 to 2000, following upper tropospheric temperature gradients more strongly than those at the surface.
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Volcanic ash cloud-top height (ACTH) can be monitored on the global level using satellite remote sensing. Here we propose a photogrammetric method based on the parallax between data retrieved from geostationary and polar orbiting satellites to overcome some limitations of the existing methods of ACTH retrieval. SEVIRI HRV band and MODIS band 1 are a good choice because of their high resolution. The procedure works well if the data from both satellites are retrieved nearly simultaneously. MODIS does not retrieve the data at exactly the same time as SEVIRI. To compensate for advection we use two sequential SEVIRI images (one before and one after the MODIS retrieval) and interpolate the cloud position from SEVIRI data to the time of MODIS retrieval. The proposed method was tested for the case of the Eyjafjallajökull eruption in April 2010. The parallax between MODIS and SEVIRI data can reach 30 km, which implies an ACTH of approximately 12 km at the beginning of the eruption. At the end of April eruption an ACTH of 3–4 km is observed. The accuracy of ACTH was estimated to be 0.6 km.
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The objectives of this study were to characterize polycyclic aromatic hydrocarbons from particulate matter emitted during wood combustion and to determine, for the first time, the isotopic signature of PAHs from nine wood species and Moroccan coal from the Mediterranean Basin. In order to differentiate sources of particulate-PAHs, molecular and isotopic measurements of PAHs were performed on the set of wood samples for a large panel of compounds. Molecular profiles and diagnostic ratios were measured by gas chromatography/mass spectrometry (GC/MS) and molecular isotopic compositions (<i>δ</i><sup>13</sup>C) of particulate-PAHs were determined by gas chromatography/combustion/isotope ratio mass spectrometry (GC/C/IRMS). Wood species present similar molecular profiles with benz(a)anthracene and chrysene as dominant PAHs, whereas levels of concentrations range from 1.8 to 11.4 mg g<sup>−1</sup> OC (sum of PAHs). Diagnostic ratios are consistent with reference ratios from literature but are not sufficient to differentiate the species of woods. Concerning isotopic methodology, PAH molecular isotopic compositions are specific for each species and contrary to molecular fingerprints, significant variations of <i>δ</i><sup>13</sup>C are observed for the panel of PAHs. This work allows differentiating wood combustion (with <i>δ</i><sup>13</sup>C<sub>PAH</sub> = −28.7 to −26.6‰) from others origins of particulate matter (like vehicular exhaust) using isotopic measurements but also confirms the necessity to investigate source characterisation at the emission in order to help and complete source assessment models. These first results on woodburnings will be useful for the isotopic approach to source tracking.
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Mercury (Hg) is a neurotoxin that bioaccumulates in the food chain. Mercury is emitted to the atmosphere primarily in its elemental form, which has a long lifetime allowing global transport. It is known that atmospheric oxidation of gaseous elemental mercury (GEM) generates reactive gaseous mercury (RGM) which plays an important role in the atmospheric mercury cycle by enhancing the rate of mercury deposition to ecosystems. However, the primary GEM oxidants, and the chemical composition of RGM are poorly known. Using speciated mercury measurements conducted at the Mt. Bachelor Observatory since 2005 we present two previously unidentified sources of RGM to the free troposphere (FT). Firstly, we observed elevated RGM concentrations, large RGM/GEM-ratios, and anti-correlation between RGM and GEM during Asian long-rang transport events, demonstrating that RGM is formed from GEM by in-situ oxidation in some anthropogenic pollution plumes in the FT. During the Asian pollution events the measured RGM/GEM-enhancement ratios reached peak values, up to ~0.20, which are significantly larger than ratios typically measured (RGM/GEM < 0.03) in the Asian source region. Secondly, we observed very high RGM levels – the highest reported in the FT – in clean air masses that were processed upwind of Mt. Bachelor Observatory over the Pacific Ocean. The high RGM concentrations (up to 700 pg m<sup>−3</sup>), high RGM/GEM-ratios (up to 1), and very low ozone levels during these events provide observational evidence indicating significant GEM oxidation in the lower FT in some conditions.
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Cloud chemistry simulations were performed for a Hector thunderstorm observed on 16 November 2005 during the SCOUT-O3/ACTIVE campaigns based in Darwin, Australia, with the primary objective of estimating the average NO production per lightning flash in this unique storm type which occurred in a tropical island environment. The 3-D WRF-Aqueous Chemistry (WRF-AqChem) model is used for these calculations and contains the WRF nonhydrostatic cloud-resolving model with online gas- and aqueous-phase chemistry and a lightning-NO<sub>x</sub> (LNO<sub>x</sub>) production algorithm. The model was initialized by inducing convection with an idealized morning sounding and sensible heat source, and initial condition chemical profiles from merged aircraft observations in undisturbed air. Many features of the idealized model storm, such as storm size and peak radar reflectivity, were similar to the observed storm. Tracer species, such as CO, used to evaluate convective transport in the simulated storm found vertical motion from the boundary layer to the anvil region was well represented in the model, with a small overestimate of enhanced CO at anvil altitudes. The lightning detection network (LINET) provided lightning flash data for the model and a lightning placement scheme injected the resulting NO into the simulated cloud. A lightning NO production scenario of 500 moles flash<sup>−1</sup> for both CG and IC flashes yielded anvil NO<sub>x</sub> mixing ratios that compared well with aircraft observations and were also similar to those deduced for several convective modeling analyses in the midlatitudes and subtropics. However, these NO production values were larger than most estimates for tropical thunderstorms and given several uncertainties, LNO<sub>x</sub> production may have been as large as 600 moles flash<sup>−1</sup>. Approximately 85% of the simulated LNO<sub>x</sub> mass was located above 7 km in the later stages of the storm, which was greater than amounts found for subtropical and midlatitude convection. Modeled upper tropospheric NO<sub>2</sub> partial columns were also considerably greater than most satellite observations of tropical marine convective events, as tropical island convection, such as Hector, is more vigorous and more productive of LNO<sub>x</sub>. Additional research is needed to investigate whether LNO<sub>x</sub> production per flash increases in storms with greater wind shear, such as this Hector storm, which showed significant variation in wind direction with altitude.
