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The Indian summer monsoon rainfall: interplay of coupled dynamics, radiation and cloud microphysics

The Indian summer monsoon rainfall (ISMR), which has a strong connection to agricultural food production, has been less predictable by conventional models in recent times. Two distinct years 2002 and 2003 with lower and higher July rainfall, respectively, are selected to help understand the natural and anthropogenic influences on ISMR. We show that heating gradients along the meridional monsoon circulation are reduced due to aerosol radiative forcing and the Indian Ocean Dipole in 2002. An increase in the dust and biomass-burning component of the aerosols through the zonal monsoon circulation resulted in reduction of cloud droplet growth in July 2002. These conditions were opposite to those in July 2003 which led to an above average ISMR. In this study, we have utilized NCEP/NCAR reanalyses for meteorological data (e.g. sea-surface temperature, horizontal winds, and precipitable water), NOAA interpolated outgoing long-wave radiation, IITM constructed all-India rainfall amounts, aerosol parameters as observed from the TOMS and MODIS satellites, and ATSR fire count maps. Based on this analysis, we suggest that monsoon rainfall prediction models should include synoptic as well as interannual variability in both atmospheric dynamics and chemical composition.
Characterisation of the photolytic HONO-source in the atmosphere simulation chamber SAPHIR

HONO formation has been proposed as an important OH radical source in simulation chambers for more than two decades. Besides the heterogeneous HONO formation by the dark reaction of NO2 and adsorbed water, a photolytic source has been proposed to explain the elevated reactivity in simulation chamber experiments. However, the mechanism of the photolytic process is not well understood so far. As expected, production of HONO and NOx was also observed inside the new atmospheric simulation chamber SAPHIR under solar irradiation. This photolytic HONO and NOx formation was studied with a sensitive HONO instrument under reproducible controlled conditions at atmospheric concentrations of other trace gases. It is shown that the photolytic HONO source in the SAPHIR chamber is not caused by NO2 reactions and that it is the only direct NOy source under illuminated conditions. In addition, the photolysis of nitrate which was recently postulated for the observed photolytic HONO formation on snow, ground, and glass surfaces, can be excluded in the chamber. A photolytic HONO source at the surface of the chamber is proposed which is strongly dependent on humidity, on light intensity, and on temperature. An empirical function describes these dependencies and reproduces the observed HONO formation rates to within 10%. It is shown that the photolysis of HONO represents the dominant radical source in the SAPHIR chamber for typical tropospheric O3/H2O concentrations. For these conditions, the HONO concentrations inside SAPHIR are similar to recent observations in ambient air.
Large-scale validation of SCIAMACHY reflectance in the ultraviolet

In this paper we present an extensive validation of calibrated SCIAMACHY nadir reflectance in the UV (240-400 nm) by comparison with spectra calculated with a fast radiative transfer model. We use operationally delivered near-real-time level 1 data, processed with standard calibration tools. A total of 9 months of data has been analysed. This is the first reflectance validation study incorporating such a large amount of data. It is shown that this method is a valuable tool for spotting spatial and temporal anomalies. We conclude that SCIAMACHY reflectance data in this wavelength range are stable over the investigated period. In addition, we show an example of an anomaly in the data due to an error in the processing chain that could be detected by our comparison. This validation method could be extremely useful too for validation of other satellite spectrometers, such as OMI and GOME-2.
Technical note: application of α-QSS to the numerical integration of kinetic equations in tropospheric chemistry

A major task in many applications of atmospheric chemistry transport problems is the numerical integration of stiff systems of Ordinary Differential Equations (ODEs) describing the chemical transformations. A faster solver that is easier to couple to the other physics in the problem is still needed. The integration method, α-QSS, corresponding to the solver CHEMEQ2 aims at meeting the demands of a process-split, reacting-flow simulation (Mott 2000; Mott and Oran, 2001). However, this integrator has yet to be applied to the numerical integration of kinetic equations in tropospheric chemistry. A zero-dimensional (box) model is developed to test how well CHEMEQ2 works on the tropospheric chemistry equations. This paper presents the testing results. The reference chemical mechanisms herein used are Regional Atmospheric Chemistry Mechanism (RACM) (Stockwell et al., 1997) and its secondary lumped successor Regional Lumped Atmospheric Chemical Scheme (ReLACS) (Crassier et al., 2000). The box model is forced and initialized by the DRY scenarios of Protocol Ver. 2 developed by EUROTRAC (Poppe et al., 2001). The accuracy of CHEMEQ2 is evaluated by comparing the results to solutions obtained with VODE. This comparison is made with parameters of the error tolerance, relative difference with respect to VODE scheme, trade off between accuracy and efficiency, global time step for integration etc. The study based on the comparison concludes that the single-point α-QSS approach is fast and moderately accurate as well as easy to couple to reacting flow simulation models, which makes CHEMEQ2 one of the best candidates for three-dimensional atmospheric Chemistry Transport Modelling (CTM) studies. In addition the RACM mechanism may be replaced by ReLACS mechanism for tropospheric chemistry transport modelling. The testing results also imply that the accuracy for chemistry numerical simulations is highly different from species to species. Therefore ozone is not the good choice for testing numerical ODE solvers or for evaluation of mechanisms because current tropospheric chemistry mechanisms are mainly designed for troposphere ozone prediction.
Physical aerosol properties and their relation to air mass origin at Monte Cimone (Italy) during the first MINATROC campaign

Aerosol physical properties were measured at the Monte Cimone Observatory (Italy) from 1 June till 6 July 2000. The measurement site is located in the transition zone between the continental boundary layer and the free troposphere (FT), at the border between the Mediterranean area and Central Europe, and is exposed to a variety of air masses. Sub-μm number size distributions, aerosol hygroscopicity near 90% RH, refractory size distribution at 270°C and equivalent black carbon mass were continuously measured. Number size distributions and hygroscopic properties indicate that the site is exposed to aged continental air masses, however during daytime it is also affected by upslope winds. The mixing of this transported polluted boundary layer air masses with relatively clean FT air leads to frequent nucleation events around local noon. Night-time size distributions, including fine and coarse fractions for each air mass episode, have been parameterized by a 3-modal lognormal distribution. Number and volume concentrations in the sub-μm modes are strongly affected by the air mass origin, with highest levels in NW-European air masses, versus very clean, free tropospheric air coming from the N-European sector. During a brief but distinct dust episode, the coarse mode is clearly enhanced. The observed hygroscopic behavior of the aerosol is consistent with the chemical composition described by Putaud et al. (2004), but no closure between known chemical composition and measured hygroscopicity could be made because the hygroscopic properties of the water-soluble organic matter (WSOM) are not known. The data suggest that WSOM is slightly-to-moderately hygroscopic (hygroscopic growth factor GF at 90% relative humidity between 1.05 and 1.51), and that this property may well depend on the air mass origin and history. External mixing of aerosol particles is observed in all air masses through the occurrence of two hygroscopicity modes (average GF of 1.22 and 1.37, respectively). However, the presence of "less" hygroscopic particles has mostly such a low occurrence rate that the average growth factor distribution for each air mass sector actually appears as a single mode. This is not the case for the dust episode, where the external mixing between less hygroscopic and more hygroscopic particles is very prominent, and indicating clearly the occurrence of a dust accumulation mode, extending down to 50 nm particles, along with an anthropogenic pollution mode. The presented physical measurements finally allow us to provide a partitioning of the sub-μm aerosol in four non-overlapping fractions (soluble/volatile, non-soluble/volatile, refractory/non-black carbon, black carbon) which can be associated with separate groups of chemical compounds determined with chemical-analytical techniques (ions, non-water soluble organic matter, dust, elemental carbon). All air masses except the free-tropospheric N-European and Dust episodes show a similar composition within the uncertainty of the data (53%, 37%, 5% and 5% respectively for the four defined fractions). Compared to these sectors, the dust episode shows a clearly enhanced refractory-non-BC fraction (17%), attributed to dust in the accumulation mode, whereas for the very clean N-EUR sector, the total refractory fraction is 25%, of which 13% non-BC and 12% BC.
A global off-line model of size-resolved aerosol microphysics: I. Model development and prediction of aerosol properties

A GLObal Model of Aerosol Processes (GLOMAP) has been developed as an extension to the TOMCAT 3-D Eulerian off-line chemical transport model. GLOMAP simulates the evolution of the global aerosol size distribution using a sectional two-moment scheme and includes the processes of aerosol nucleation, condensation, growth, coagulation, wet and dry deposition and cloud processing. We describe the results of a global simulation of sulfuric acid and sea spray aerosol. The model captures features of the aerosol size distribution that are well established from observations in the marine boundary layer and free troposphere. Modelled condensation nuclei (CN>3nm) vary between about 250–500 cm-3 in remote marine boundary layer regions and are generally in good agreement with observations. Modelled continental CN concentrations are lower than observed, which may be due to lack of some primary aerosol sources or the neglect of nucleation mechanisms other than binary homogeneous nucleation of sulfuric acid-water particles. Remote marine CN concentrations increase to around 2000–10 000 cm<sup-3 (at standard temperature and pressure) in the upper troposphere, which agrees with typical observed vertical profiles. Cloud condensation nuclei (CCN) at 0.2% supersaturation vary between about 1000 cm-3 in polluted regions and between 10 and 500 cm-3 in the remote marine boundary layer. New particle formation through sulfuric acid-water binary nucleation occurs predominantly in the upper troposphere, but the model results show that these particles contribute greatly to aerosol concentrations in the marine boundary layer. For this sulfur-sea salt system it is estimated that sea spray emissions account for only ~10% of CCN in the tropical marine boundary layer, but between 20 and 75% in the mid-latitude Southern Ocean. In a run with only natural sulfate and sea salt emissions the global mean surface CN concentration is more than 60% of that from a run with 1985 anthropogenic sulfur emissions, although the natural emissions comprise only 27% of total sulfur emissions. Southern hemisphere marine boundary layer CN are more than 90% natural in origin, while polluted continental CN are more than 90% anthropogenic in origin, although these numbers will change when other anthropogenic CN sources are included in the model.
Aerosol mass closure and reconstruction of the light scattering coefficient over the Eastern Mediterranean Sea during the MINOS campaign

As part of the Mediterranean Intensive Oxidant Study (MINOS) performed during August 2001 in the Eastern Mediterranean Region, intensive measurements of chemical and radiative properties of atmospheric aerosols were performed at two remote sites on Crete Island, located in the marine boundary layer (MBL), and in the lower free troposphere (FT), respectively. Gravimetric particulate mass, as well as chemically-derived masses of water soluble ions, organic and elemental carbon, and tracer elements for dust aerosols were measured for fine (<1.2 µm) and coarse (>1.2 µm) particles at the two sampling sites. Although strongly bound water, mainly associated with inorganic species, could have slightly altered our results (10% of the reconstructed mass), chemical mass closure was achieved most of the time for the fine and coarse size fractions and at both sites. Our conversion factor of 2.1 for organic carbon (OC) to particulate organic matter (POM) is at the upper end of those reported in the literature, but fits with the aged smoke particles collected during the campaign. The results indicate that this conversion factor changed during the campaign along with the BC/TC ratio. The particulate mass (PM) concentration for fine aerosols at the MBL and FT sites averaged 17.4±4.7 µg/m3 and 11.2±3.2 µg/m3, respectively, and is among the highest reported in the literature for remote sites; more than 90% of this PM was composed equally of ammonium sulfate and carbonaceous aerosols. Comparison between the MBL and FT sites showed a slight vertical gradient for PM that was not observed for dust aerosols, which averaged 10.5±4.8 and 11.7±5.0 µg/m3 for the MBL and FT sites, respectively. The results were used to reconstruct the ambient light scattering coefficient (σsp) that was measured at ambient Relative Humidity (RH) for fine particles at the MBL site. Reconstruction of σsp was achieved using ratios of wet to dry scattering, f(RH), that depend on RH for ammonium sulfate, but are kept equal to 1 for POM. This results in a low water adsorption for our organic-rich carbonaceous aerosols, although these aged biomass smoke aerosols are supposed to be highly oxidized. Mass scattering efficiencies of the main aerosol components were obtained by multivariate regression analysis, and were 2.66 and 4.19 m2/g (at the 95% confidence level) for dry ammonium sulfate and POM, respectively. The calculations indicate that one third of the reconstructed σsp was due to water uptake by ammonium sulfate aerosols, demonstrating their major role in the radiative aerosol properties in the eastern Mediterranean.
Mexico City basin wind circulation during the MCMA-2003 field campaign

MCMA-2003 was a major field campaign investigating the atmospheric chemistry of the Mexico City Metropolitan Area (MCMA) in April of 2003. This paper describes the wind circulation patterns during the campaign both within the Mexico City basin and on the regional scale. 'Time roses' are introduced to concisely analyze the diurnal wind patterns. Three episode types were identified that explain the conditions encountered: 'O3-South', 'Cold Surge' and 'O3-North'. These can be diagnosed from a combination of synoptic and basin observations based on whether the day was predominantly cloudy, or whether the O3 peak was in the north or south of the basin. O3-South days have weak synoptic forcing due to an anti-cyclone over the eastern Pacific. Strong solar heating leads to northerly flows in the basin and an evening shift due to a gap flow from the south-east. Peak ozone concentrations are in the convergence zone in the south of the city. Cold Surge days are associated with 'El Norte' events, with strong surface northerlies bringing cold moist air and rain. Stable conditions lead to high concentrations of primary pollutants and peak ozone in the city center. O3-North days occur when the sub-tropical jet is closer to Mexico City. With strong westerlies aloft, the circulation pattern is the same as O3-South days except for a wind shift in the mid-afternoon leading to ozone peaks in the north of the city. This classification is proposed as a means of understanding pollutant transport in the Mexico City basin and as a basis for future meteorological and chemical analysis. Furthermore, model evaluation and design of policy recommendations will need to take into account the three episode types.
Characterization of aerosol particle episodes in Finland caused by wildfires in Eastern Europe

We studied the sources, compositions and size distributions of aerosol particles during long-range transport (LRT) PM2.5 episodes which occurred on 12–15 August, 26–28 August and 5–6 September 2002 in Finland. Backward air mass trajectories, satellite detections of fire areas and dispersion modelling results indicate that emissions from wildfires in Russia and other Eastern European countries arrived in Finland during these episodes. Elemental analyses using scanning electron microscopy (SEM) coupled with energy dispersive X-ray microanalyses (EDX) showed that the proportions of S-rich particles and agglomerates (agglomeration was caused partly by the sampling method used) increased during the episodes, and they contained elevated fractions of K, indicating emissions from biomass burning. These aerosols were mixed with S-rich emissions from fossil fuel burning during transport since air masses came through polluted areas of Europe. Minor amounts of coarse Ca-rich particles were also brought by LRT during the episodes, and they probably originated from wildfires and/or from Estonian and Russian oil-shale-burning industrial areas. Ion chromatography analysis showed that concentrations of sulphate (SO42-), total nitrate (NO3-+HNO3(g)) and total ammonium (NH4++NH3(g)) increased during the episodes, but the ratio of the total amount of these ions to PM10 concentration decreased, indicating unusually high fractions of other chemical components. Particle number size distribution measurements with differential mobility particle sizer (DMPS) revealed that concentrations of particles 90–500 nm increased during the episodes, while concentrations of particles smaller than 90 nm decreased. The reduction of the smallest particles was caused by suppressed new particle formation due to vapour and molecular cluster uptake of LRT particles. Our results show that emissions from wildfires in Russian and other Eastern European countries deteriorated air quality of very large areas, even at distances of over 1000 km from the fire areas.
Chemical characteristics of ice residual nuclei in anvil cirrus clouds: evidence for homogeneous and heterogeneous ice formation

A counterflow virtual impactor was used to collect residual particles larger than about 0.1 μm diameter from anvil cirrus clouds generated over Florida in the southern United States. A wide variety of particle types were found. About one-third of the nuclei were salts, with varying amounts of crustal material, industrial metals, carbonaceous particles, and sulfates. Ambient aerosol particles near the anvils were found to have similar compositions, indicating that anvils act to redistribute particles over large regions of the atmosphere. Sampling occurred at a range of altitudes spanning temperatures from −21 to −56°C. More insoluble (crustal and metallic) particles typical of heterogeneous ice nuclei were found in ice crystals at warmer temperatures, while more soluble salts and sulfates were present at cold temperatures. At temperatures below about −35 to −40°C, soluble nuclei outnumbered insoluble nuclei, evidently reflecting the transition from primarily heterogeneous to primarily homogeneous freezing as a source of anvil ice.