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A comprehensive inventory of ship traffic exhaust emissions in the European sea areas in 2011

Emissions originating from ship traffic in European sea areas were modelled using the Ship Traffic Emission Assessment Model (STEAM), which uses Automatic Identification System data to describe ship traffic activity. We have estimated the emissions from ship traffic in the whole of Europe in 2011. We report the emission totals, the seasonal variation, the geographical distribution of emissions, and their disaggregation between various ship types and flag states. The total ship emissions of CO2, NOx, SOx, CO, and PM2.5 in Europe for year 2011 were estimated to be 121, 3.0, 1.2, 0.2, and 0.2 million tons, respectively. The emissions of CO2 from the Baltic Sea were evaluated to be more than a half (55 %) of the emissions of the North Sea shipping; the combined contribution of these two sea regions was almost as high (88 %) as the total emissions from ships in the Mediterranean. As expected, the shipping emissions of SOx were significantly lower in the SOx Emission Control Areas, compared with the corresponding values in the Mediterranean. Shipping in the Mediterranean Sea is responsible for 40 and 49 % of the European ship emitted CO2 and SOx emissions, respectively. In particular, this study reported significantly smaller emissions of NOx, SOx, and CO for shipping in the Mediterranean than the EMEP inventory; however, the reported PM2.5 emissions were in a fairly good agreement with the corresponding values reported by EMEP. The vessels registered to all EU member states are responsible for 55 % of the total CO2 emitted by ships in the study area. The vessels under the flags of convenience were responsible for 25 % of the total CO2 emissions.
Investigating the frequency and interannual variability in global above-cloud aerosol characteristics with CALIOP and OMI

Seven and a half years (June 2006 to November 2013) of Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aerosol and cloud layer products are compared with collocated Ozone Monitoring Instrument (OMI) aerosol index (AI) data and Aqua Moderate Resolution Imaging Spectroradiometer (MODIS) cloud products in order to investigate variability in estimates of biannual and monthly above-cloud aerosol (ACA) events globally. The active- (CALIOP) and passive-based (OMI-MODIS) techniques have their advantages and caveats for ACA detection, and thus both are used to derive a thorough and robust comparison of daytime cloudy-sky ACA distribution and climatology. For the first time, baseline above-cloud aerosol optical depth (ACAOD) and AI thresholds are derived and examined (AI  =  1.0, ACAOD  =  0.015) for each sensor. Both OMI-MODIS and CALIOP-based daytime spatial distributions of ACA events show similar patterns during both study periods (December–May) and (June–November). Divergence exists in some regions, however, such as Southeast Asia during June through November, where daytime cloudy-sky ACA frequencies of up to 10 % are found from CALIOP yet are non-existent from the OMI-based method. Conversely, annual cloudy-sky ACA frequencies of 20–30 % are reported over northern Africa from the OMI-based method yet are largely undetected by the CALIOP-based method. Using a collocated OMI-MODIS-CALIOP data set, our study suggests that the cloudy-sky ACA frequency differences between the OMI-MODIS- and CALIOP-based methods are mostly due to differences in cloud detection capability between MODIS and CALIOP as well as QA flags used. An increasing interannual variability of ∼  0.3–0.4 % per year (since 2009) in global monthly cloudy-sky ACA daytime frequency of occurrence is found using the OMI-MODIS-based method. Yet, CALIOP-based global daytime ACA frequencies exhibit a near-zero interannual variability. Further analysis suggests that the OMI-derived interannual variability in cloudy-sky ACA frequency may be affected by OMI row anomalies in later years. A few regions are found to have increasing slopes in interannual variability in cloudy-sky ACA frequency, including the Middle East and India. Regions with slightly negative slopes of the interannual variability in cloudy-sky ACA frequencies are found over South America and China, while remaining regions in the study show nearly zero change in ACA frequencies over time. The interannual variability in ACA frequency is not, however, statistically significant on both global and regional scales, given the relatively limited sample sizes. A longer data record of ACA events is needed in order to establish significant trends of ACA frequency regionally and globally.
Effect of gravity wave temperature fluctuations on homogeneous ice nucleation in the tropical tropopause layer

The impact of high-frequency fluctuations of temperature on homogeneous nucleation of ice crystals in the vicinity of the tropical tropopause is investigated using a bin microphysics scheme for air parcels. The imposed temperature fluctuations come from measurements during isopycnic balloon flights near the tropical tropopause. The balloons collected data at high frequency, guaranteeing that gravity wave signals are well resolved. With the observed temperature time series, the numerical simulations with homogeneous freezing show a full range of ice number concentration (INC) as previously observed in the tropical upper troposphere. In particular, a low INC may be obtained if the gravity wave perturbations produce a non-persistent cooling rate (even with large magnitude) such that the absolute change in temperature remains small during nucleation. This result is explained analytically by a dependence of the INC on the absolute drop in temperature (and not on the cooling rate). This work suggests that homogeneous ice nucleation is not necessarily inconsistent with observations of low INCs.
Observational estimates of detrainment and entrainment in non-precipitating shallow cumulus

Vertical transport associated with cumulus clouds is important to the redistribution of gases, particles, and energy, with subsequent consequences for many aspects of the climate system. Previous studies have suggested that detrainment from clouds can be comparable to the updraft mass flux, and thus represents an important contribution to vertical transport. In this study, we describe a new method to deduce the amounts of gross detrainment and entrainment experienced by non-precipitating cumulus clouds using aircraft observations. The method utilizes equations for three conserved variables: cloud mass, total water, and moist static energy. Optimizing these three equations leads to estimates of the mass fractions of adiabatic mixed-layer air, entrained air and detrained air that the sampled cloud has experienced. The method is applied to six flights of the CIRPAS Twin Otter during the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) which took place in the Houston, Texas region during the summer of 2006 during which 176 small, non-precipitating cumuli were sampled. Using our novel method, we find that, on average, these clouds were comprised of 30 to 70 % mixed-layer air, with entrained air comprising most of the remainder. The mass fraction of detrained air was usually very small, less than 2 %, although values larger than 10 % were found in 15 % of clouds. Entrained and detrained air mass fractions both increased with altitude, consistent with some previous observational studies. The largest detrainment events were almost all associated with air that was at their level of neutral buoyancy, which has been hypothesized in previous modeling studies. This new method could be readily used with data from other previous aircraft campaigns to expand our understanding of detrainment for a variety of cloud systems.
A two-dimensional volatility basis set – Part 3: Prognostic modeling and NOx dependence

When NOx is introduced to organic emissions, aerosol production is sometimes, but not always, reduced. Under certain conditions, these interactions will instead increase aerosol concentrations. We expanded the two-dimensional volatility basis set (2D-VBS) to include the effects of NOx on aerosol formation. This includes the formation of organonitrates, where the addition of a nitrate group contributes to a decrease of 2.5 orders of magnitude in volatility. With this refinement, we model outputs from experimental results, such as the atomic N : C ratio, organonitrate mass, and nitrate fragments in Aerosol Mass Spectrometer (AMS) measurements. We also discuss the mathematical methods underlying the implementation of the 2D-VBS and provide the complete code in the Supplement. A developer version is available on Bitbucket, an online community repository.
Sensitivity of polar stratospheric cloud formation to changes in water vapour and temperature

More than a decade ago it was suggested that a cooling of stratospheric temperatures by 1 K or an increase of 1 ppmv of stratospheric water vapour could promote denitrification, the permanent removal of nitrogen species from the stratosphere by solid polar stratospheric cloud (PSC) particles. In fact, during the two Arctic winters 2009/10 and 2010/11 the strongest denitrification in the recent decade was observed. Sensitivity studies along air parcel trajectories are performed to test how a future stratospheric water vapour (H2O) increase of 1 ppmv or a temperature decrease of 1 K would affect PSC formation. We perform our study based on measurements made during the Arctic winter 2010/11. Air parcel trajectories were calculated 6 days backward in time based on PSCs detected by CALIPSO (Cloud Aerosol Lidar and Infrared Pathfinder satellite observations). The sensitivity study was performed on single trajectories as well as on a trajectory ensemble. The sensitivity study shows a clear prolongation of the potential for PSC formation and PSC existence when the temperature in the stratosphere is decreased by 1 K and water vapour is increased by 1 ppmv. Based on 15 years of satellite measurements (2000–2014) from UARS/HALOE, Envisat/MIPAS, Odin/SMR, Aura/MLS, Envisat/SCIAMACHY and SCISAT/ACE-FTS it is further investigated if there is a decrease in temperature and/or increase of water vapour (H2O) observed in the polar regions similar to that observed at midlatitudes and in the tropics. Performing linear regression analyses we derive from the Envisat/MIPAS (2002–2012) and Aura/MLS (2004–2014) observations predominantly positive changes in the potential temperature range 350 to 1000 K. The linear changes in water vapour derived from Envisat/MIPAS observations are largely insignificant, while those from Aura/MLS are mostly significant. For the temperature neither of the two instruments indicate any significant changes. Given the strong inter-annual variation observed in water vapour and particular temperature the severe denitrification observed in 2010/11 cannot be directly related to any changes in water vapour and temperature since the millennium. However, the observations indicate a clear correlation between cold winters and enhanced water vapour mixing ratios. This indicates a connection between dynamical and radiative processes that govern water vapour and temperature in the Arctic lower stratosphere.
An adsorption theory of heterogeneous nucleation of water vapour on nanoparticles

Heterogeneous nucleation of water vapour on insoluble nuclei is a phenomenon that can induce atmospheric water and ice cloud formation. However, modelling of the phenomenon is hampered by the fact that the predictive capability of the classical heterogeneous nucleation theory is rather poor. A reliable theoretical description of the influence of different types of water-insoluble nuclei in triggering the water condensation or ice deposition would help to decrease uncertainty in large-scale model simulations. In this paper we extend a recently formulated adsorption theory of heterogeneous nucleation to be applicable to highly curved surfaces, and test the theory against laboratory data for water vapour nucleation on silica, titanium dioxide and silver oxide nanoparticles. We show that unlike the classical heterogeneous nucleation theory, the new theory is able to quantitatively predict the experimental results.
Delivery of anthropogenic bioavailable iron from mineral dust and combustion aerosols to the ocean

Atmospheric deposition of anthropogenic soluble iron (Fe) to the ocean has been suggested to modulate primary ocean productivity and thus indirectly affect the climate. A key process contributing to anthropogenic sources of soluble Fe is associated with air pollution, which acidifies Fe-containing mineral aerosols during their transport and leads to Fe transformation from insoluble to soluble forms. However, there is large uncertainty in our estimate of this anthropogenic soluble Fe. In this study, for the first time, we interactively combined laboratory kinetic experiments with global aerosol modeling to more accurately quantify anthropogenic soluble Fe due to air pollution. Firstly, we determined Fe dissolution kinetics of African dust samples at acidic pH values with and without ionic species commonly found in aerosol water (i.e., sulfate and oxalate). Then, by using acidity as a master variable, we constructed a new empirical scheme for Fe release from mineral dust due to inorganic and organic anions in aerosol water. We implemented this new scheme and applied an updated mineralogical emission database in a global atmospheric chemistry transport model to estimate the atmospheric concentration and deposition flux of soluble Fe under preindustrial and modern conditions. Our improved model successfully captured the inverse relationship of Fe solubility and total Fe loading measured over the North Atlantic Ocean (i.e., 1–2 orders of magnitude lower Fe solubility in northern-African- than combustion-influenced aerosols). The model results show a positive relationship between Fe solubility and water-soluble organic carbon (WSOC)/Fe molar ratio, which is consistent with previous field measurements. We estimated that deposition of soluble Fe to the ocean increased from 0.05–0.07 Tg Fe yr−1 in the preindustrial era to 0.11–0.12 Tg Fe yr−1 in the present day, due to air pollution. Over the high-nitrate, low-chlorophyll (HNLC) regions of the ocean, the modeled Fe solubility remains low for mineral dust (< 1 %) in a base simulation but is substantially enhanced in a sensitivity simulation, which permits the Fe dissolution for mineral aerosols in the presence of excess oxalate under low acidity during daytime. Our model results suggest that human activities contribute to about half of the soluble Fe supply to a significant portion of the oceans in the Northern Hemisphere, while their contribution to oceans in high latitudes remains uncertain due to limited understanding of Fe source and its dissolution under pristine conditions.
Stratosphere-troposphere exchange in the vicinity of a tropopause fold

Transport of air masses from the stratosphere to the troposphere along tropopause folds can lead to peaked ozone concentrations at ground level and hereby influence the long-term trend of tropospheric ozone. To improve the understanding of responsible processes and preferred regions of exchange, transient and reversible exchange processes in the vicinity of a tropopause fold are analysed on the basis of a case study. The global and regional atmospheric chemistry model system MECO(n), which couples the limited-area atmospheric chemistry and climate model COSMO-CLM/MESSy to the global model ECHAM5/MESSy for Atmospheric Chemistry (EMAC) is applied. Using similar process parametrisations in both model instances, the system allows for very consistent, simultaneous simulations at different spatial resolutions. Simulated ozone enhancements at ground level, caused by descending stratospheric air masses, are evaluated with observational data. Because of the coarse resolution of the global model, the observed ozone enhancements are not captured by the global model instance. However, the results of the finer resolved, regional model instance coincide well with the measurements. Based on the combination of Eulerian and Lagrangian analysis methods it is shown that stratosphere-troposphere-exchange (STE) in the vicintity of the tropopause fold occurs in regions of turbulence and diabatic processes. Within the framework of a Lagrangian study the efficiency of mixing along a tropopause fold is quantified, showing that almost all (97 %) of the air masses originating in the tropopause fold are transported into the troposphere during the following two days.
Light absorption properties of laboratory-generated tar ball particles

Tar balls (TBs) are a specific particle type that is abundant in the global troposphere, in particular in biomass smoke plumes. These particles belong to the family of atmospheric brown carbon (BrC), which can absorb light in the visible range of the solar spectrum. Albeit TBs are typically present as individual particles in biomass smoke plumes, their absorption properties have been only indirectly inferred from field observations or calculations based on their electron energy-loss spectra. This is because in biomass smoke TBs coexist with various other particle types (e.g., organic particles with inorganic inclusions and soot, the latter emitted mainly during flaming conditions) from which they cannot be physically separated; thus, a direct experimental determination of their absorption properties is not feasible. Very recently we have demonstrated that TBs can be generated in the laboratory from droplets of wood tar that resemble atmospheric TBs in all of their observed properties. As a follow-up study, we have installed on-line instruments to our laboratory set-up, which generate pure TB particles to measure the absorption and scattering, as well as the size distribution of the particles. In addition, samples were collected for transmission electron microscopy (TEM) and total carbon (TC) analysis. The effects of experimental parameters were also studied. The mass absorption coefficients of the laboratory-generated TBs were found to be in the range of 0.8–3.0 m2 g−1 at 550 nm, with absorption Ångström exponents (AAE) between 2.7 and 3.4 (average 2.9) in the wavelength range 467–652 nm. The refractive index of TBs as derived from Mie calculations was about 1.84 − 0.21i at 550 nm. In the brown carbon continuum, these values fall closer to those of soot than to other light-absorbing species such as humic-like substances (HULIS). Considering the abundance of TBs in biomass smoke and the global magnitude of biomass burning emissions, these findings may have substantial influence on the understanding of global radiative energy fluxes.