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Corrigendum to "Evaluation of black carbon estimations in global aerosol models" published in Atmos. Chem. Phys., 9, 9001-9026, 2009
Laboratory experiments on the effect of organic acids and metals on the charge transfer during ice crystal – graupel collision under the conditions similar to stratiform clouds

Laboratory investigations have been carried out to find the sign and magnitude of charge transfer during the collision between ice crystals and graupel in the presence of supercooled water droplets inside the cylindrical steel chamber kept inside a walk-in cold room, which can reach a temperature of −30 °C. The experiments were performed with pure water (Milli-Q, 18.2 Megohms-cm) and with trace amounts of organic acids and metals at low Rime Accretion Rate (<0.40 g m−2 s-1) applicable to stratiform clouds in the temperature range −5 to −27 °C. The ice crystals and supercooled droplets collided with the graupel target at a constant impact velocity of 2.2 m/s. The presence of trace chemicals (organics or metals) saw significant increase in the magnitude of charge transferred per crystal collision to the graupel. These experiments therefore suggest that the presence of trace amounts of organics or metals in cloud water can significantly alter the electrical structure of stratiform clouds.
Constraint of anthropogenic NOx emissions in China from different sectors: a new methodology using multiple satellite retrievals

A new methodology is developed to constrain Chinese anthropogenic emissions of nitrogen oxides (NOx) from four major sectors (industry, power plants, mobile and residential) in July 2008. It combines tropospheric NO2 column retrievals from GOME-2 and OMI, taking advantage of their different passing time over China (~10:00 a.m. LT (local time) versus ~02:00 p.m.) and consistent retrieval algorithms. The approach is based on the difference of NOx columns at the overpass times of the two instruments; it thus is less susceptible to the likely systematic errors embedded in individual retrievals that are consistent with each other. Also, it explicitly accounts for diurnal variations and uncertainties of NOx emissions for individual sources. Our best top-down estimate suggests a national budget of 6.8 TgN/yr (5.5 TgN/yr for East China), close to the a priori bottom-up emission estimate from the INTEX-B mission for the year of 2006. The top-down emissions are lower than the a priori near Beijing, in the northeastern provinces and along the east coast; yet they exceed the a priori over many inland regions. Systematic errors in satellite retrievals are estimated to lead to underestimation of top-down emissions by at most 17% (most likely 10%). Effects of other factors on the top-down estimate are typically less than 15% each, including lightning, soil emissions, mixing in planetary boundary layer, anthropogenic emissions of carbon monoxide and volatile organic compounds, magnitude of a priori emissions, assumptions on emission diurnal variations, and uncertainties in the four sectors. The a posteriori emission budget is 5.7 TgN/yr for East China.
Ice nucleation properties of mineral dust particles: determination of onset RHi, IN active fraction, nucleation time-lag, and the effect of active sites on contact angles

A newly developed ice nucleation experimental set up was used to investigate the heterogeneous ice nucleation properties of three Saharan and one Spanish dust particle samples. It was observed that the spread in the onset relative humidities with respect to ice (RHi) for Saharan dust particles varied from 104% to 110%, whereas for the Spanish dust from 106% to 110%. The elemental composition analysis shows a prominent Ca feature in the Spanish dust sample which could potentially explain the differences in nucleation threshold. Although the spread in the onset RHi for the three Saharan dust samples were in agreement, the active fractions and nucleation time-lags calculated at various temperature and RHi conditions were found to differ. This could be due to the subtle variation in the elemental composition of the dust samples, and surface irregularities like steps, cracks, cavities etc. A combination of classical nucleation theory and active site theory is used to understand the importance of these surface irregularities on the nucleability parameter, contact angle that is widely used in ice cloud modeling. These calculations show that the surface irregularities can reduce the contact angle by approximately 10 degrees.
The effect of misleading surface temperature estimations on the sensible heat fluxes at a high Arctic site – the Arctic Turbulence Experiment 2006 on Svalbard (ARCTEX-2006)

The observed rapid climate warming in the Arctic requires improvements in permafrost and carbon cycle monitoring, accomplished by setting up long-term observation sites with high-quality in-situ measurements of turbulent heat, water and carbon fluxes as well as soil physical parameters in Arctic landscapes. But accurate quantification and well adapted parameterizations of turbulent fluxes in polar environments presents fundamental problems in soil-snow-ice-vegetation-atmosphere interaction studies. One of these problems is the accurate estimation of the surface or aerodynamic temperature T(0) required to force most of the bulk aerodynamic formulae currently used. Results from the Arctic-Turbulence-Experiment (ARCTEX-2006) performed on Svalbard during the winter/spring transition 2006 helped to better understand the physical exchange and transport processes of energy. The existence of an atypical temperature profile close to the surface in the Arctic spring at Svalbard could be proven to be one of the major issues hindering estimation of the appropriate surface temperature. Thus, it is essential to adjust the set-up of measurement systems carefully when applying flux-gradient methods that are commonly used to force atmosphere-ocean/land-ice models. The results of a comparison of different sensible heat-flux parameterizations with direct measurements indicate that the use of a hydrodynamic three-layer temperature-profile model achieves the best fit and reproduces the temporal variability of the surface temperature better than other approaches.
Modeling of Saharan dust outbreaks over the Mediterranean by RegCM3: case studies

The regional climate model RegCM3 coupled with a radiatively active aerosol model with online feedback is used to investigate direct and semi-direct radiative aerosol effects over the Sahara and Europe in a test case of July 2003. The aerosol model includes dust particles in addition to sulfates, hydrophobic and hydrophilic black carbon and organic carbon. The role of the aerosol online feedback on the radiation budget and the direct radiative forcing (short-wave and long-wave) by dust particles are investigated by intercomparing results from three experiments: REF, including all interactive aerosol components, Exp1, not accounting for the aerosol radiative feedback, and Exp2 not accounting for desert dust particles. The comparison of results in the REF experiment with satellite observations, sun/sky radiometer measurements, and lidar profiles at selected Central Mediterranean sites reveals that the spatio-temporal evolution of the aerosol optical depth is reasonably well reproduced by the model during the entire month of July. Results for the dust outbreaks of 17 and 24 July, averaged over the simulation domain, show that the daily-mean SW direct radiative forcing by all particles is −24 Wm−2 and −3.4 Wm−2 on 17 July and −25 Wm−2 and −3.5 Wm−2 on 24 July at the surface and top of the atmosphere, respectively. This is partially offset by the LW direct radiative forcing, which is 7.6 Wm−2 and 1.9 Wm−2 on 17 July and 8.4 Wm−2 and 1.9 Wm−2 on 24 July at the surface and top of the atmosphere, respectively. Hence, the daily-mean SW forcing is offset by the LW forcing of ~30% at the surface and of ~50% at the ToA. It is also shown that atmospheric dynamics and hence dust production and advection processes are dependent on the simulation assumptions and may significantly change within few tens of kilometers. The comparison of REF and Exp1 shows that the aerosol online feedback on the radiation budget decreases the domain-average daily-mean value of the 2 m-temperature, aerosol column burden (CB), and short-wave (SW) atmospheric forcing by −0.52 °C, 14%, and 0.9%, respectively on 17 July and by −0.39 °C, 12% and 12%, respectively on 24 July. The comparison of REF and Exp2 reveals that on 17 July, radiatively-active dust particles decrease the daily-mean 2 m-temperature averaged over the whole simulation domain by 0.4% even if are responsible for 99.8% and 97% of the daily-mean aerosol column burden and SW atmospheric forcing, respectively.
Annual cycle of ozone at and above the tropical tropopause: observations versus simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS)

Multi-annual simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS) were conducted to study the seasonality of O3 within the stratospheric part of the tropical tropopause layer (TTL), i.e. above θ=360 K potential temperature level. In agreement with satellite (HALOE) and in-situ observations (SHADOZ), CLaMS simulations show a pronounced annual cycle in O3, at and above θ=380 K, with the highest mixing ratios in the late boreal summer. Within the model, this cycle is driven by the seasonality of both upwelling and in-mixing. The latter process occurs through enhanced horizontal transport from the extratropics into the TTL that is mainly driven by the meridional, isentropic winds. The strongest in-mixing occurs during the late boreal summer from the Northern Hemisphere in the potential temperature range between 370 and 420 K. Complementary, the strongest upwelling occurs in winter reducing O3 to the lowest values in early spring. Both CLaMS simulations and Aura MLS O3 observations consistently show that enhanced in-mixing in summer is mainly driven by the Asian monsoon anticyclone.
Overview: oxidant and particle photochemical processes above a south-east Asian tropical rainforest (the OP3 project): introduction, rationale, location characteristics and tools

In April–July 2008, intensive measurements were made of atmospheric composition and chemistry in Sabah, Malaysia, as part of the "Oxidant and particle photochemical processes above a South-East Asian tropical rainforest" (OP3) project. Fluxes and concentrations of trace gases and particles were made from and above the rainforest canopy at the Bukit Atur Global Atmosphere Watch station and at the nearby Sabahmas oil palm plantation, using both ground-based and airborne measurements. Here, the measurement and modelling strategies used, the characteristics of the sites and an overview of data obtained are described. Composition measurements show that the rainforest site was not significantly impacted by anthropogenic pollution, and this is confirmed by satellite retrievals of NO2 and HCHO. The dominant modulators of atmospheric chemistry at the rainforest site were therefore emissions of BVOCs and soil emissions of reactive nitrogen oxides. At the observed BVOC:NOx volume mixing ratio (~100 pptv/pptv), current chemical models suggest that daytime maximum OH concentrations should be ca. 105 radicals cm−3, but observed OH concentrations were an order of magnitude greater than this. We confirm, therefore, previous measurements that suggest that an unexplained source of OH must exist above tropical rainforest and we continue to interrogate the data to find explanations for this.
Aerosols that form subvisible cirrus at the tropical tropopause

The composition of residual particles from evaporated cirrus ice crystals near the tropical tropopause as well as unfrozen aerosols were measured with a single particle mass spectrometer. Subvisible cirrus residuals were predominantly composed of internal mixtures of neutralized sulfate with organic material and were chemically indistinguishable from unfrozen sulfate-organic aerosols. Ice residuals were also similar in size to unfrozen aerosol. Heterogeneous ice nuclei such as mineral dust were not enhanced in these subvisible cirrus residuals. Biomass burning particles were depleted in the residuals. Cloud probe measurements showing low cirrus ice crystal number concentrations were inconsistent with conventional homogeneous freezing. Recent laboratory studies provide heterogeneous nucleation scenarios that may explain tropopause level subvisible cirrus formation.
Trend in ice moistening the stratosphere – constraints from isotope data of water and methane

Water plays a major role in the chemistry and radiative budget of the stratosphere. Air enters the stratosphere predominantly in the tropics, where the very low temperatures around the tropopause constrain water vapour mixing ratios to a few parts per million. Observations of stratospheric water vapour show a large positive long-term trend, which can not be explained by change in tropopause temperatures. Trends in the partitioning between vapour and ice of water entering the stratosphere have been suggested to resolve this conundrum. We present measurements of stratospheric H2O, HDO, CH4 and CH3D in the period 1991–2007 to evaluate this hypothesis. Because of fractionation processes during phase changes, the hydrogen isotopic composition of H2O is a sensitive indicator of changes in the partitioning of vapour and ice. We find that the seasonal variations of H2O are mirrored in the variation of the ratio of HDO to H2O with a slope of the correlation consistent with water entering the stratosphere mainly as vapour. The variability in the fractionation over the entire observation period is well explained by variations in H2O. The isotopic data allow concluding that the trend in ice arising from particulate water is no more than (0.01±0.13) ppmv/decade in the observation period. Our observations suggest that between 1991 and 2007 the contribution from changes in particulate water transported through the tropopause plays only a minor role in altering in the amount of water entering the stratosphere.