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Technical Note: The horizontal scale dependence of the cloud overlap parameter α

The cloud overlap parameter α relates the combined cloud fraction between two altitude levels in a grid box to the cloud fraction as derived under the maximum and random overlap assumptions. In a number of published studies in this and other journals, it is found that α tends to increase with an increasing scale. In this Technical Note, we investigate this analytically by considering what happens to α when two grid boxes are merged to give a grid box with twice the area. Assuming that α depends only on scale, then between any two fixed altitudes, there will be a linear relationship between the values of α on the two scales. We illustrate this by finding the relationship when cloud cover fractions are assumed to be uniformly distributed, but with varying degrees of horizontal and vertical correlation. Based on this, we conclude that α increases with scale if its value is less than the vertical correlation coefficient in cloud fraction between the two altitude levels. This occurs when the clouds are deeper than would be expected at random (i.e. for exponentially distributed cloud depths).
Corrigendum to "Advances in understanding and parameterization of small-scale physical processes in the marine Arctic climate system: a review" published in Atmos. Chem. Phys., 14, 9403–9450, 2014
Experimental determination of the temperature dependence of water activities for a selection of aqueous organic solutions

This work presents experimental data of the temperature dependence of water activity in aqueous organic solutions relevant for tropospheric conditions (200–273 K). Water activity (aw) at low temperatures (T) is a crucial parameter for predicting homogeneous ice nucleation. We investigated temperature-dependent water activities, ice freezing and melting temperatures of solutions, and vapour pressures of a selection of atmospherically relevant aqueous organic systems. To measure aw over a wide composition range and with a focus on low temperatures, we use various aw measurement techniques and instruments: a dew point water activity meter, an electrodynamic balance (EDB), differential scanning calorimetry (DSC), and a setup to measure the total gas phase pressure at equilibrium over aqueous solutions. Water activity measurements were performed for aqueous multicomponent and multifunctional organic mixtures containing the functional groups typically found in atmospheric organic aerosols, such as hydroxyl, carboxyl, ketone, ether, ester, and aromatic groups. The aqueous organic systems studied at several fixed compositions over a considerable temperature range differ significantly in their temperature dependence. Aqueous organic systems of 1,4-butanediol and methoxyacetic acid show a moderate decrease in aw with decreasing temperature. The aqueous M5 system (a multicomponent system containing five different dicarboxylic acids) and aqueous 2-(2-ethoxyethoxy)ethanol solutions both show a strong increase of water activity with decreasing temperature at high solute concentrations for T < 270 K and T < 260 K, respectively. These measurements show that the temperature trend of aw can be reversed at low temperatures and that linear extrapolations of high-temperature data may lead to erroneous predictions. To avoid this, experimentally determined aw at low temperature are needed to improve thermodynamic models towards lower temperatures and for improved predictions of the ice nucleation ability of organic–water systems.
Source apportionment and seasonal variation of PM2.5 in a Sub-Saharan African city: Nairobi, Kenya

Sources of airborne particulate matter and their seasonal variation in urban areas in Sub-Saharan Africa are poorly understood due to lack of long-term measurement data. In view of this, filter samples of airborne particulate matter (particle diameter ≤2.5 μm, PM2.5) were collected between May 2008 and April 2010 at two sites (urban background site and suburban site) within the Nairobi metropolitan area. A total of 780 samples were collected and analyzed for particulate mass, black carbon (BC) and 13 trace elements. The average PM2.5 concentration at the urban background site was 21±9.5 μg m−3, whereas the concentration at the suburban site was 13±7.3 μg m−3. The daily PM2.5 concentrations exceeded 25 μg m−3 (the World Health Organization 24 h guideline value) on 29% of the days at the urban background site and 7% of the days at the suburban site. At both sites, BC, Fe, S and Cl accounted for approximately 80% of all detected elements. Positive matrix factorization analysis identified five source factors that contribute to PM2.5 in Nairobi, namely traffic, mineral dust, industry, combustion and a mixed factor (composed of biomass burning, secondary aerosol and aged sea salt). Mineral dust and traffic factors were related to approximately 74% of PM2.5. The identified source factors exhibited seasonal variation, apart from the traffic factor, which was prominently consistent throughout the sampling period. Weekly variations were observed in all factors, with weekdays having higher concentrations than weekends. The results provide information that can be exploited for policy formulation and mitigation strategies to control air pollution in Sub-Saharan African cities.
How stratospheric are deep stratospheric intrusions?

Preliminary attempts of quantifying the stratospheric ozone contribution in the observations at the Zugspitze summit (2962 m a.s.l.) next to Garmisch-Partenkirchen in the German Alps had yielded an approximate doubling of the stratospheric fraction of the Zugspitze ozone during the time period 1978 to 2004. These investigations had been based on data filtering by using low relative humidity (RH) and elevated 7Be as the criteria for selecting half-hour intervals of ozone data representative of stratospheric intrusion air. To quantify the residual stratospheric component in stratospherically influenced air masses, however, the mixing of tropospheric air into the stratospheric intrusion layers must be taken into account. In fact, the dewpoint mirror instrument at the Zugspitze summit station rarely registers RH values lower than 10% in stratospheric air intrusions. Since 2007 a programme of routine lidar sounding of ozone, water vapour and aerosol has been conducted in the Garmisch-Partenkirchen area. The lidar results demonstrate that the intrusion layers are drier by roughly one order of magnitude than indicated in the in situ measurements. Even in thin layers RH values clearly below 1% have frequently been observed. These thin, undiluted layers present an important challenge for atmospheric modelling. Although the ozone values never reach values typical of the lower-stratosphere it becomes, thus, obvious that, without strong wind shear or convective processes, mixing of stratospheric and tropospheric air must be very slow in most of the free troposphere. As a consequence, the analysis the Zugspitze data can be assumed to be more reliable than anticipated. Finally, the concentrations of Zugspitze carbon monoxide rarely drop inside intrusion layers and normally stay clearly above full stratospheric values. This indicates that most of the CO, and thus the intrusion air mass, originates in the shallow "mixing layer" around the thermal tropopause. The CO mixing ratio in these descending layers between 1990 and 2004 exhibits a slightly positive trend indicating some Asian influence on the lowermost stratosphere in the high-latitude source region of most intrusions reaching the station.
Aviation 2006 NOx-induced effects on atmospheric ozone and HOx in Community Earth System Model (CESM)

The interaction between atmospheric chemistry and ozone (O3) in the upper troposphere–lower stratosphere (UTLS) presents a major uncertainty in understanding the effects of aviation on climate. In this study, two configurations of the atmospheric model from the Community Earth System Model (CESM), Community Atmosphere Model with Chemistry, Version 4 (CAM4) and Version 5 (CAM5), are used to evaluate the effects of aircraft nitrogen oxide (NOx = NO + NO2) emissions on ozone and the background chemistry in the UTLS. CAM4 and CAM5 simulations were both performed with extensive tropospheric and stratospheric chemistry including 133 species and 330 photochemical reactions. CAM5 includes direct and indirect aerosol effects on clouds using a modal aerosol module (MAM), whereby CAM4 uses a bulk aerosol module, which can only simulate the direct effect. To examine the accuracy of the aviation NOx-induced ozone distribution in the two models, results from the CAM5 and CAM4 simulations are compared to ozonesonde data. Aviation NOx emissions for 2006 were obtained from the AEDT (Aviation Environmental Design Tool) global commercial aircraft emissions inventory. Differences between simulated O3 concentrations and ozonesonde measurements averaged at representative levels in the troposphere and different regions are 13% in CAM5 and 18% in CAM4. Results show a localized increase in aviation-induced O3 concentrations at aviation cruise altitudes that stretches from 40° N to the North Pole. The results indicate a greater and more disperse production of aviation NOx-induced ozone in CAM5, with the annual tropospheric mean O3 perturbation of 1.2 ppb (2.4%) for CAM5 and 1.0 ppb (1.9%) for CAM4. The annual mean O3 perturbation peaks at about 8.2 ppb (6.4%) and 8.8 ppb (5.2%) in CAM5 and CAM4, respectively. Aviation emissions also result in increased hydroxyl radical (OH) concentrations and methane (CH4) loss rates, reducing the tropospheric methane lifetime in CAM5 and CAM4 by 1.69 and 1.40%, respectively. Aviation NOx emissions are associated with an instantaneous change in global mean short-term O3 radiative forcing (RF) of 40.3 and 36.5 mWm−2 in CAM5 and CAM4, respectively.
Concentrations and fluxes of isoprene and oxygenated VOCs at a French Mediterranean oak forest

The CANOPEE project aims to better understand the biosphere–atmosphere exchanges of biogenic volatile organic compounds (BVOCs) in the case of Mediterranean ecosystems and the impact of in-canopy processes on the atmospheric chemical composition above the canopy. Based on an intensive field campaign, the objective of our work was to determine the chemical composition of the air inside a canopy as well as the net fluxes of reactive species between the canopy and the boundary layer. Measurements were carried out during spring 2012 at the field site of the Oak Observatory of the Observatoire de Haute Provence (O3HP) located in the southeast of France. The site is a forest ecosystem dominated by downy oak, Quercus pubescens Willd., a typical Mediterranean species which features large isoprene emission rates. Mixing ratios of isoprene, its degradation products methylvinylketone (MVK) and methacrolein (MACR) and several other oxygenated VOC (OxVOC) were measured above the canopy using an online proton transfer reaction mass spectrometer (PTR-MS), and fluxes were calculated by the disjunct eddy covariance approach. The O3HP site was found to be a very significant source of isoprene emissions, with daily maximum ambient concentrations ranging between 2–16 ppbv inside and 2–5 ppbv just above the top of the forest canopy. Significant isoprene fluxes were observed only during daytime, following diurnal cycles with midday net emission fluxes from the canopy ranging between 2.0 and 9.7 mg m−2 h1. Net isoprene normalized flux (at 30 °C, 1000 μmol quanta m−2 s−1) was estimated at 7.4 mg m−2 h−1. Evidence of direct emission of methanol was also found exhibiting maximum daytime fluxes ranging between 0.2 and 0.6 mg m−2 h−1, whereas flux values for monoterpenes and others OxVOC such as acetone and acetaldehyde were below the detection limit. The MVK+MACR-to-isoprene ratio provided useful information on the oxidation of isoprene, and is in agreement with recent findings proposing weak production yields of MVK and MACR, in remote forest regions where the NOx concentrations are low. In-canopy chemical oxidation of isoprene was found to be weak and did not seem to have a significant impact on isoprene concentrations and fluxes above the canopy.
Size distribution, mixing state and source apportionment of black carbon aerosol in London during wintertime

Black carbon aerosols (BC) at a London urban site were characterised in both winter- and summertime 2012 during the Clean Air for London (ClearfLo) project. Positive matrix factorisation (PMF) factors of organic aerosol mass spectra measured by a high-resolution aerosol mass spectrometer (HR-AMS) showed traffic-dominant sources in summer but in winter the influence of additional non-traffic sources became more important, mainly from solid fuel sources (SF). Measurements using a single particle soot photometer (SP2, DMT), showed the traffic-dominant BC exhibited an almost uniform BC core size (Dc) distribution with very thin coating thickness throughout the detectable range of Dc. However, the size distribution of Dc (project average mass median Dc = 149 ± 22 nm in winter, and 120 ± 6 nm in summer) and BC coating thickness varied significantly in winter. A novel methodology was developed to attribute the BC number concentrations and mass abundances from traffic (BCtr) and from SF (BCsf), by using a 2-D histogram of the particle optical properties as a function of BC core size, as measured by the SP2. The BCtr and BCsf showed distinctly different Dc distributions and coating thicknesses, with BCsf displaying larger Dc and larger coating thickness compared to BCtr. BC particles from different sources were also apportioned by applying a multiple linear regression between the total BC mass and each AMS-PMF factor (BC–AMS–PMF method), and also attributed by applying the absorption spectral dependence of carbonaceous aerosols to 7-wavelength Aethalometer measurements (Aethalometer method). Air masses that originated from westerly (W), southeasterly (SE), and easterly (E) sectors showed BCsf fractions that ranged from low to high, and whose mass median Dc values were 137 ± 10 nm, 143 ± 11 nm and 169 ± 29 nm, respectively. The corresponding bulk relative coating thickness of BC (coated particle size/BC core – Dp/Dc) for these same sectors was 1.28 ± 0.07, 1.45 ± 0.16 and 1.65 ± 0.19. For W, SE and E air masses, the number fraction of BCsf ranged from 6 ± 2% to 11 ± 5% to 18 ± 10%, respectively, but importantly the larger BC core sizes lead to an increased fraction of BCsf in terms of mass than number (for W, SE and E air masses, the BCsf mass fractions ranged from 16 ± 6%, 24 ± 10% and 39 ± 14%, respectively). An increased fraction of non-BC particles (particles that did not contain a BC core) was also observed when SF sources were more significant. The BC mass attribution by the SP2 method agreed well with the BC–AMS–PMF multiple linear regression method (BC–AMS–PMF : SP2 ratio = 1.05, r2 = 0.80) over the entire experimental period. Good agreement was found between BCsf attributed with the Aethalometer model and the SP2. However, the assumed absorption Ångström exponent (αwb) had to be changed according to the different air mass sectors to yield the best comparison with the SP2. This could be due to influences of fuel type or burn phase.
Carbon balance of China constrained by CONTRAIL aircraft CO2 measurements

Terrestrial carbon dioxide (CO2) flux estimates in China using atmospheric inversion method are beset with considerable uncertainties because very few atmospheric CO2 concentration measurements are available. In order to improve these estimates, nested atmospheric CO2 inversion during 2002–2008 is performed in this study using passenger aircraft-based CO2 measurements over Eurasia from the Comprehensive Observation Network for Trace gases by Airliner (CONTRAIL) project. The inversion system includes 43 regions with a focus on China, and is based on the Bayesian synthesis approach and the TM5 transport model. The terrestrial ecosystem carbon flux modeled by the Boreal Ecosystems Productivity Simulator (BEPS) model and the ocean exchange simulated by the OPA-PISCES-T model are considered as the prior fluxes. The impacts of CONTRAIL CO2 data on inverted China terrestrial carbon fluxes are quantified, the improvement of the inverted fluxes after adding CONTRAIL CO2 data are rationed against climate factors and evaluated by comparing the simulated atmospheric CO2 concentrations with three independent surface CO2 measurements in China. Results show that with the addition of CONTRAIL CO2 data, the inverted carbon sink in China increases while those in South and Southeast Asia decrease. Meanwhile, the posterior uncertainties over these regions are all reduced (2–12%). CONTRAIL CO2 data also have a large effect on the inter-annual variation of carbon sinks in China, leading to a better correlation between the carbon sink and the annual mean climate factors. Evaluations against the CO2 measurements at three sites in China also show that the CONTRAIL CO2 measurements may have improved the inversion results.
Summertime tropospheric ozone assessment over the Mediterranean region using the thermal infrared IASI/MetOp sounder and the WRF-Chem model

Over the Mediterranean region, elevated tropospheric ozone (O3) values are recorded, especially in summer. We use the thermal Infrared Atmospheric Sounding Interferometer (IASI) and the Weather Research and Forecasting Model with Chemistry (WRF-Chem) to understand and interpret the factors and emission sources responsible for the high O3 concentrations observed in the Mediterranean troposphere. Six years (2008–2013) of IASI data have been analyzed and results show consistent maxima during summer, with an increase of up to 22% in the [0–8] km O3 column in the eastern part of the basin compared to the middle of the basin. We focus on summer 2010 to investigate the processes that contribute to these summer maxima. Using two modeled O3 tracers (inflow to the model domain and local anthropogenic emissions), we show that, between the surface and 2 km, O3 is mostly formed from anthropogenic emissions, while above 4 km it is mostly transported from outside the domain or from stratospheric origins. Evidence of stratosphere-to-troposphere exchange (STE) events in the eastern part of the basin is shown, and corresponds to a low water vapor mixing ratio and high potential vorticity.