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Influence of Giant CCN on warm rain processes in the ECHAM5 GCM

Increased Cloud Condensation Nuclei (CCN) load due to anthropogenic activity might lead to non-precipitating clouds because the cloud drops become smaller (for a constant liquid water content) and, therefore, less efficient in rain formation (aerosol indirect effect). Adding giant CCN (GCCN) into such a cloud can initiate precipitation (namely, drizzle) and, therefore, might counteract the aerosol indirect effect. The effect of GCCN on global climate on warm clouds and precipitation within the ECHAM5 General Circulation Model (GCM) is investigated. Therefore, the newly introduced prognostic rain scheme (Posselt and Lohmann, 2007) is applied so that GCCN are directly activated into rain drops. The ECHAM5 simulations with incorporated GCCN show that precipitation is affected only locally. On the global scale, the precipitation amount does not change. Cloud properties like total water (liquid + rain water) and cloud drop number show a larger sensitivity to GCCN. Depending on the amount of added GCCN, the reduction of total water and cloud drops account for up to 20% compared to the control run without GCCN. Thus, the incorporation of the GCCN accelerate the hydrological cycle so that clouds precipitate faster (but not more) and less condensed water is accumulated in the atmosphere. An estimate of the anthropogenic aerosol indirect effect on the climate is obtained by comparing simulations for present-day and pre-industrial climate. The introduction of the prognostic rain scheme lowered the anthropogenic aerosol indirect effect significantly compared to the standard ECHAM5 with the diagnostic rain scheme. The incorporation of the GCCN changes the model state, especially the cloud properties like TWP and Nl. The precipitation changes only locally but globally the precipitation is unaffected because it has to equal the global mean evaporation rate. Changing the cloud properties leads to a local reduction of the aerosol indirect effect and, hence, partly compensating for the increased anthropogenic CCN concentrations in that regions. Globally, the aerosol indirect effect is nearly the same for all simulations.
How small is a small cloud?

The interplay between clouds and aerosols and their contribution to the radiation budget is one of the largest uncertainties of climate change. Most work to date has separated cloudy and cloud-free areas in order to evaluate the individual radiative forcing of aerosols, clouds, and aerosol effects on clouds. Here we examine the size distribution and the optical properties of small, sparse cumulus clouds and the associated optical properties of what is considered a cloud-free atmosphere within the cloud field. We show that any separation between clouds and cloud free atmosphere will incur errors in the calculated radiative forcing. The nature of small cumulus cloud size distributions suggests that at any resolution, a significant fraction of the clouds are missed, and their optical properties are relegated to the apparent cloud-free optical properties. At the same time, the cloudy portion incorporates significant contribution from non-cloudy pixels. We show that the largest contribution to the total cloud reflectance comes from the smallest clouds and that the spatial resolution changes the apparent energy flux of a broken cloudy scene. When changing the resolution from 30 m to 1 km (Landsat to MODIS) the average "cloud-free" reflectance at 1.65 μm increases from 0.0095 to 0.0115 (>20%), the cloud reflectance decreases from 0.13 to 0.066 (~50%), and the cloud coverage doubles, resulting in an important impact on climate forcing estimations. The apparent aerosol forcing is on the order of 0.5 to 1 Wm−2 per cloud field.
Corrigendum to "Vertical profiles of urban aerosol complex refractive index in the frame of ESQUIF airborne measurements" published in Atmos. Chem. Phys., 8, 901–919, 2008
Estimation of the vertical profile of sulfur dioxide injection into the atmosphere by a volcanic eruption using satellite column measurements and inverse transport modeling

An analytical inversion method has been developed to estimate the vertical profile of SO2 emissions from volcanic eruptions. The method uses satellite-observed total SO2 columns and an atmospheric transport model (FLEXPART) to exploit the fact that winds change with altitude – thus, the position and shape of the volcanic plume bear information on its emission altitude. The method finds the vertical emission distribution which minimizes the total difference between simulated and observed SO2 columns while also considering a priori information. We have tested the method with the eruption of Jebel at Tair, Yemen, on 30 September 2007 for which a comprehensive observational data set from various satellite instruments (AIRS, OMI, SEVIRI, CALIPSO) is available. Using satellite data from the first 24 h after the eruption for the inversion, we found an emission maximum near 16 km above sea level (a.s.l.), and secondary maxima near 5, 9, 12 and 14 km a.s.l. 60% of the emission occurred above the tropopause. The emission profile obtained in the inversion was then used to simulate the transport of the plume over the following week. The modeled plume agrees very well with SO2 total columns observed by OMI, and its altitude agrees with CALIPSO aerosol observations to within 1–2 km. The inversion result is robust against various changes in both the a priori and the observations. Even when using only SEVIRI data from the first 15 h after the eruption, the emission profile was reasonably well estimated. The method is computationally very fast. It is therefore suitable for implementation within an operational environment, such as the Volcanic Ash Advisory Centers, to predict the threat posed by volcanic ash for air traffic. It could also be helpful for assessing the sulfur input into the stratosphere, be it in the context of volcanic processes or also for proposed geo-engineering techniques to counteract global warming.
Diagnosing recent CO emissions and ozone evolution in East Asia using coordinated surface observations, adjoint inverse modeling, and MOPITT satellite data

Simultaneous ground-based measurements of ozone (O3) and carbon monoxide (CO) were conducted in March 2005 as part of the East Asian Regional Experiment (EAREX) 2005 under the umbrella of the Atmospheric Brown Clouds (ABC) project. Multiple air quality monitoring networks were integrated by performing intercomparison of individual calibration standards and measurement techniques to ensure comparability of ambient measurements, along with providing consistently high time-resolution measurements of O3 and CO at the surface sites in East Asia. Ambient data collected from eight surface stations were compared with simulation results obtained by a regional chemistry transport model to infer recent changes in CO emissions from East Asia. Our inverse estimates of the CO emissions from China up to 2005 suggested an increase of 16% since 2001, in good agreement with the recent MOPITT satellite observations and the bottom-up estimates up to 2006. The O3 enhancement relative to CO in continental pollution plumes traversed in the boundary layer were examined as a function of transport time from the Asian continent to the western Pacific Ocean. The observed ΔO3/ΔCO ratios show increasing tendency during eastward transport events due likely to en-route photochemical O3 formation, suggesting that East Asia is an important O3 source region during spring.
Observations of HNO3, ΣAN, ΣPN and NO2 fluxes: evidence for rapid HOx chemistry within a pine forest canopy

Measurements of exchange of reactive nitrogen oxides between the atmosphere and a ponderosa pine forest in the Sierra Nevada Mountains are reported. During winter, we observe upward fluxes of NO2, and downward fluxes of total peroxy and peroxy acyl nitrates (ΣPNs), total gas and particle phase alkyl and multifunctional alkyl nitrates (ΣANs(g+p)), and the sum of gaseous HNO3 and semi-volatile NO3− particles (HNO3(g+p)). We use calculations of the vertical profile and flux of NO, partially constrained by observations, to show that net midday ΣNOyi fluxes in winter are –4.9 ppt m s−1. The signs and magnitudes of these wintertime individual and ΣNOyi fluxes are in the range of prior measurements. In contrast, during summer, we observe downward fluxes only of ΣANs(g+p), and upward fluxes of HNO3(g+p), ΣPNs and NO2 with signs and magnitudes that are unlike most, if not all, previous observations and analyses of fluxes of individual nitrogen oxides. The results imply that the mechanisms contributing to NOy fluxes, at least at this site, are much more complex than previously recognized. We show that the observations of upward fluxes of HNO3(g+p) and σPNs during summer are consistent with oxidation of NO2 and acetaldehyde by an OH x residence time of 1.1×1010 molec OH cm−3 s, corresponding to 3 to 16×107 molecules cm−3 OH within the forest canopy for a 420 to 70 s canopy residence time. We show that ΣAN(g+p) fluxes are consistent with this range in OH if the reaction of OH with ΣANs produces either HNO3 or NO2 with a 6–30% yield. Calculations of NO fluxes constrained by the NO2 observations and the inferred OH indicate that NOx fluxes are downward into the canopy because of the substantial conversion of NOx to HNO3 and σPNs in the canopy. Even so, we derive that NOx emission fluxes of ~15 ng(N) m−2 s−1 at midday during summer are required to balance the NOx and NOy flux budgets. These fluxes are partly explained by estimates of soil emissions (estimated to be between 3 and 6 ng(N) m−2 s-1). One possibility for the remainder of the NOx source is large HONO emissions. Alternatively, the 15 ng(N) m−2 s−1 emission estimate may be too large, and the budget balanced if the deposition of HNO3 and σPNs is slower than we estimate, if there are large errors in either our understanding of peroxy radical chemistry, or our assumptions that the budget is required to balance because the fluxes do not obey similarity theory.
Chemistry of sprite discharges through ion-neutral reactions

We estimate the concentration changes, caused by streamer discharge in sprites, of ozone and related minor species as odd nitrogen (NOx) and hydrogen (HOx) families in the upper stratosphere and mesosphere. The streamer has an intense electric field and high electron density at its head, where a large number of chemically-radical ions and atoms are produced through electron impact on neutral molecules. After its propagation, densities of minor species can be perturbed through ion-neutral chemical reactions initiated by the relaxation of these radical products. We evaluate the production rates of ions and atoms using an electron kinetics model and by assuming that the electric field and electron density are in the head region. We calculate the density variations mainly for NOx, Ox, and HOx species using a one-dimensional model of the neutral and ion composition of the middle atmosphere, including the effect of the sprite streamer. Results at the nighttime condition show that the densities of NO, O3, H, and OH increase suddenly through reactions triggered by the first atomic nitrogen and oxygen product, and electrons just after streamer initiation. It is shown that NO and NO2 still remain for 1 h by a certain order of increase with their source-sink balance, predominantly around 60 km; for other species, increases in O3, OH, HO2, and H2O2 still remain in the range of 40–70 km. From this affirmative result of long-time behavior previously not presented, we emphasize that sprites would have the power to impact local chemistry at night. We also discuss the consistency with previous theoretical and observational studies, along with future suggestions.
A computationally-efficient secondary organic aerosol module for three-dimensional air quality models

Accurately simulating secondary organic aerosols (SOA) in three-dimensional (3-D) air quality models is challenging due to the complexity of the physics and chemistry involved and the high computational demand required. A computationally-efficient yet accurate SOA module is necessary in 3-D applications for long-term simulations and real-time air quality forecasting. A coupled gas and aerosol box model (i.e., 0-D CMAQ-MADRID 2) is used to optimize relevant processes in order to develop such a SOA module. Solving the partitioning equations for condensable volatile organic compounds (VOCs) and calculating their activity coefficients in the multicomponent mixtures are identified to be the most computationally-expensive processes. The two processes can be speeded up by relaxing the error tolerance levels and reducing the maximum number of iterations of the numerical solver for the partitioning equations for organic species; conditionally activating organic-inorganic interactions; and parameterizing the calculation of activity coefficients for organic mixtures in the hydrophilic module. The optimal speed-up method can reduce the total CPU cost by up to a factor of 31.4 from benchmark under the rural conditions with 2 ppb isoprene and by factors of 10–71 under various test conditions with 2–10 ppb isoprene and >40% relative humidity while maintaining ±15% deviation. These speed-up methods are applicable to other SOA modules that are based on partitioning theories.
Tracing biomass burning plumes from the Southern Hemisphere during the AMMA 2006 wet season experiment

The Lagrangian particle dispersion model FLEXPART coupled with daily active fire products provided by the MODIS instrument was used to forecast the intrusions of the southern hemispheric fire plumes in the Northern Hemisphere during the AMMA (African Monsoon Multidisciplinary Analysis) fourth airborne campaign from 25 July to 31 August 2006 (Special Operation Period SOP2_a2). The imprint of the biomass burning plumes over the Gulf of Guinea showed a well marked intraseasonal variability which is controlled by the position and strength of the southern hemispheric African Easterly Jet (AEJ-S). Three different periods were identified which correspond to active and break phases of the AEJ-S: 25 July–2 August (active phase), 3 August–8 August (break phase) and 9 August–31 August (active phase). During the AEJ-S active phases, the advection of the biomass burning plumes out over the Atlantic ocean was efficient in the mid-troposphere. During the AEJ-S break phases, pollutants emitted by fires were trapped over the continent where they accumulated. The continental circulation increased the possibility for the biomass burning plumes to reach the convective regions located further north. As a consequence, biomass burning plumes were found in the upper troposphere over the Gulf of Guinea during the AEJ-S break phase. Observational evidences from the ozonesounding network at Cotonou and the carbon monoxide measured by MOPITT confirmed the alternation of the AEJ-S phases with low ozone and CO in the mid-troposphere over the Gulf of Guinea during the break phase.
CCN activity and droplet growth kinetics of fresh and aged monoterpene secondary organic aerosol

The ability of secondary organic aerosol (SOA) produced from the ozonolysis of α-pinene and monoterpene mixtures (α-pinene, β-pinene, limonene and 3-carene) to become cloud droplets was investigated. A static CCN counter and a Scanning Mobility CCN Analyser (a Scanning Mobility Particle Sizer coupled with a Continuous Flow counter) were used for the CCN measurements. Consistent with previous studies monoterpene SOA is quite active and would likely be a good source of cloud condensation nuclei (CCN) in the atmosphere. A decrease in CCN activation diameter for α-pinene SOA of approximately 3 nm hr−1 was observed as the aerosol continued to react with oxidants. Hydroxyl radicals further oxidize the SOA particles thereby enhancing the particle CCN activity with time. The initial concentrations of ozone and monoterpene precursor (for concentrations lower than 40 ppb) do not appear to affect the activity of the resulting SOA. Köhler Theory Analysis (KTA) is used to infer the molar mass of the SOA sampled online and offline from atomized filter samples. The estimated average molar mass of online SOA was determined to be 180±55 g mol−1 (consistent with existing SOA speciation studies) assuming complete solubility. KTA suggests that the aged aerosol (both from α-pinene and the mixed monoterpene oxidation) is primarily water-soluble (around 65%). CCN activity measurements of the SOA mixed with (NH4)2SO4 suggest that the organic can depress surface tension by as much as 10 N m−1 (with respect to pure water). The droplet growth kinetics of SOA samples are similar to (NH4)2SO4, except at low supersaturation, where SOA tends to grow more slowly. The CCN activation diameter of α-pinene and mixed monoterpene SOA can be modelled to within 10–15% of experiments by a simple implementation of Köhler theory, assuming complete dissolution of the particles, no dissociation into ions, a molecular weight of 180 g mol−1, a density of 1.5 g cm−3, and the surface tension of water.