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Measurements of total and tropospheric ozone from IASI: comparison with correlative satellite, ground-based and ozonesonde observations

In this paper, we present measurements of total and tropospheric ozone, retrieved from infrared radiance spectra recorded by the Infrared Atmospheric Sounding Interferometer (IASI), which was launched on board the MetOp-A European satellite in October 2006. We compare IASI total ozone columns to Global Ozone Monitoring Experiment-2 (GOME-2) observations and ground-based measurements from the Dobson and Brewer network for one full year of observations (2008). The IASI total ozone columns are shown to be in good agreement with both GOME-2 and ground-based data, with correlation coefficients of about 0.9 and 0.85, respectively. On average, IASI ozone retrievals exhibit a positive bias of about 9 DU (3.3%) compared to both GOME-2 and ground-based measurements. In addition to total ozone columns, the good spectral resolution of IASI enables the retrieval of tropospheric ozone concentrations. Comparisons of IASI tropospheric columns to 490 collocated ozone soundings available from several stations around the globe have been performed for the period of June 2007–August 2008. IASI tropospheric ozone columns compare well with sonde observations, with correlation coefficients of 0.95 and 0.77 for the [surface–6 km] and [surface–12 km] partial columns, respectively. IASI retrievals tend to overestimate the tropospheric ozone columns in comparison with ozonesonde measurements. Positive average biases of 0.15 DU (1.2%) and 3 DU (11%) are found for the [surface–6 km] and for the [surface–12 km] partial columns respectively.
Comparative study of the effect of water on the heterogeneous reactions of carbonyl sulfide on the surface of α-Al2O3 and MgO

Here we compared the heterogeneous reactions of carbonyl sulfide (OCS) on the surface of α-Al2O3 and MgO and the effect of water on the reactions at 300 K using Knudsen cell–mass spectrometry, diffuse reflectance infrared Fourier transform spectroscopy, and temperature programmed reactions. H2S and CO2 were found to be hydrolysis products of OCS on both α–Al2O3 and MgO at ambient temperature. At low water vapor pressure (<6.8×10−6 Torr), when water vapor pressure in the Knudsen cell reactor increased from 2.3×10−6 to 6.8×10−6 Torr, the initial true uptake coefficient of OCS on α-Al2O3 decreased from 4.70±0.45×10−7 to 3.59±0.34×10−7; while it increased from 5.19±0.49×10−7 to 6.48±0.62×10−7 on MgO under the same conditions. At high relative humidity (0.07–0.67), the observed uptake coefficients of OCS on α-Al2O3 and MgO, which were measured using an in situ DRIFTS, decreased from 4.63±0.22×10−6 to 1.00±0.47×10−6 and from 9.72±0.46×10−5 to 7.68±0.36×10−5, respectively, when RH increased from 0.07 to 0.67 corresponding to 1.7–15.9 Torr of water vapor pressure. In the RH region of 0.17–0.67, the average observed uptake coefficient of OCS on α-Al2O3 and MgO was equal to 8.34±2.19×10−7 and 8.19±0.48×10−5, respectively. The restrictive effect of water on the heterogeneous reaction of OCS on the surface of α-Al2O3 and MgO was found to be related to competitive adsorption between water and OCS molecules; while the promotive effect of water on the heterogeneous reaction of OCS on the surface of MgO at low coverage was ascribed to the formation of surface hydroxyl groups. When the environmental RH was greater than the RH of the monolayer, which occurred readily at the atmospherically relevant humidity in the troposphere, thick water layer formed on the mineral dusts, especially, the basic thick water layer formed on the basic component of mineral dusts may be the primary contributor to the heterogeneous hydrolysis of OCS in the troposphere.
Factors controlling contrail cirrus optical depth

Aircraft contrails develop into contrail cirrus by depositional growth and sedimentation of ice particles and horizontal spreading due to wind shear. Factors controlling this development include temperature, ice supersaturation, thickness of ice-supersaturated layers, and vertical gradients in the horizontal wind field. An analytical microphysical cloud model is presented and validated that captures these processes. Many individual contrail cirrus are simulated that develop differently owing to the variability in the controlling factors, resulting in large samples of cloud properties that are statistically analyzed. Contrail cirrus development is studied over the first four hours past formation, similar to the ages of line-shaped contrails that were tracked in satellite imagery on regional scales. On these time scales, contrail cirrus optical depth and microphysical variables exhibit a marked variability, expressed in terms of broad and skewed probability distribution functions. Simulated mean optical depths at a wavelength of 0.55 μm range from 0.05-0.5 and a substantial fraction 20-50% of contrail cirrus stay subvisible (optical depth <0.02), depending on meteorological conditions. A detailed analysis based on an observational case study over the continental USA suggests that previous satellite measurements of line-shaped persistent contrails have missed about 89%, 50%, and 11% of contrails with optical depths 0-0.05, 0.05-0.1, and 0.1-0.2, respectively, amounting to 65% of contrail coverage of all optical depths. When comparing observations with simulations and when estimating the contrail cirrus climate impact, not only mean values but also the variability in optical depth and microphysical properties need to be considered.
Study of columnar aerosol size distribution in Hong Kong

This paper presents studies on columnar aerosol optical properties in Hong Kong with focus on aerosol volume size distribution, which helps understand local aerosol properties, variation, hygroscopic growth and coagulation. Long-term ground measurements in the wet season in the years of 2002, 2003, 2004 and 2008 have been performed using a sun-sky radiometer. Data validation made using MODIS and local AERONET shows agreement. A bimodal size distribution is found with the fine mode centering at ~0.2 μm and coarse mode centering at ~3 μm respectively. The fine and coarse mode have close volume concentrations of nearly 50% fraction in composing local aerosols. Intercomparison of different years shows similar aerosol properties while a small increase of fine mode aerosol could be observed. A systematic shift of size distribution parameters is observed with different atmospheric conditions, where higher aerosol loadings and Angstrom exponent correspond to more fine mode aerosols. The fine mode is found to be more closely correlated with this shift than the coarse mode. A higher fine mode volume fraction and smaller median fine radius correspond to a larger Angstrom exponent. The fine mode aerosol hygroscopic growth is one of the main mechanisms for such systematic shifting. A third mode centering at ~1–2 μm could be discovered under high aerosol loading and high fine mode aerosol conditions. It becomes more pronounced with high aerosol optical depth and larger Angstrom exponent. Investigation of its variation with corresponding optical parameters and correlation with atmospheric conditions appears to support the hypothesis that it is mainly due to the fine mode aerosol hygroscopic growth and coagulation rather than the contribution from the coarse mode. While the very humid environment facilitates the aerosol hygroscopic growth, aerosol coagulation might further produce larger aerosols under high fine aerosol conditions. The continental outflow with transported aging aerosols and biomass burning might have also contributed to this additional mode.
Evaluating simulated primary anthropogenic and biomass burning organic aerosols during MILAGRO: implications for assessing treatments of secondary organic aerosols

Simulated primary organic aerosols (POA), as well as other particulates and trace gases, in the vicinity of Mexico City are evaluated using measurements collected during the 2006 Megacity Initiative: Local and Global Research Observations (MILAGRO) field campaigns. Since the emission inventories, transport, and turbulent mixing will directly affect predictions of total organic matter and consequently total particulate matter, our objective is to assess the uncertainties in predicted POA before testing and evaluating the performance of secondary organic aerosol (SOA) treatments. Carbon monoxide (CO) is well simulated on most days both over the city and downwind, indicating that transport and mixing processes were usually consistent with the meteorological conditions observed during MILAGRO. Predicted and observed elemental carbon (EC) in the city was similar, but larger errors occurred at remote locations since the overall CO/EC emission ratios in the national emission inventory were lower than in the metropolitan emission inventory. Components of organic aerosols derived from Positive Matrix Factorization of data from several Aerodyne Aerosol Mass Spectrometer instruments deployed both at ground sites and on research aircraft are used to evaluate the model. Modeled POA was consistently lower than the measured organic matter at the ground sites, which is consistent with the expectation that SOA should be a large fraction of the total organic matter mass. A much better agreement was found when modeled POA was compared with the sum of "primary anthropogenic" and "biomass burning" components derived from Positive Matrix Factorization (PMF) on most days, especially at the surface sites, suggesting that the overall magnitude of primary organic particulates released was reasonable. However, simulated POA from anthropogenic sources was often lower than "primary anthropogenic" components derived from PMF, consistent with two recent reports that these emissions are underestimated. The modeled POA was greater than the total observed organic matter when the aircraft flew directly downwind of large fires, suggesting that biomass burning emission estimates from some large fires may be too high.
Influence of aerosols on the formation and development of radiation fog

This paper assesses the impact of aerosol properties on the formation and the development of radiation fog. Simulations were performed using the Meso-NH meteorological model including the ORILAM aerosol scheme coupled with a two-moment microphysical cloud scheme (number concentration of cloud droplets and cloud water content). The activation scheme used was taken from the work of Abdul-Razzak and Ghan (2004). "Off-line" sensitivity analysis of CCN (Cloud Condensation Nuclei) activation was performed on number, median diameter and chemical compounds of aerosols. During this "off-line" study, the interactions with the other physical processes (e.g. radiative) were not taken into account since the cooling rate was imposed. Different regimes of CCN activation and a critical value of aerosol number concentration were found. This critical aerosol number corresponds to the maximum of activated cloud droplets for a given cooling rate and given aerosol chemical properties. As long as the aerosol number concentration is below this critical value, the cloud droplet number increases when the aerosol number increases. But when the aerosol number concentration exceeds this critical value, the cloud droplet number decreases when aerosol number increases. A sensitivity study on aerosol chemical composition showed that the CCN activation was limited in the case of hydrophilic aerosol composed of material with a solubility in the 10% range. An event observed during the ParisFOG field experiment was simulated. This case took place in the polluted sub-urban area of Paris (France) characterized by particle concentrations of 17 000 aerosols per cm3. 1D simulations successfully reproduced the observed temporal evolution of the fog layer. Beyond the initial fog formation at the surface, cloud droplet formation occurred at the top of the fog layer where the cooling rate was maximum, reaching more than −10 K h−1. These simulations confirm that the aerosol particle number concentration is a key parameter for the accurate prediction of the microphysical properties of a fog layer and also influences the vertical development of fog. The important of the interaction between microphysical and radiative processes is illustrated, showing how the life cycle of a fog layer is determined by the CCN number concentration and chemical properties.
Influence of meteorological variability on interannual variations of springtime boundary layer ozone over Japan during 1981–2005

We investigated the influence of meteorological variability on the interannual variation of springtime boundary layer ozone over Japan during 1981–2005 by multiyear simulations with the Models-3 Community Multiscale Air Quality (CMAQ) modeling system and the Regional Emission Inventory in Asia (REAS). CMAQ/REAS generally reproduced the observed interannual variability of springtime ozone over Japan, showing year-to-year variations larger than the annual rate of increase of the long-term trend. We then analyzed the influence of the interannual variation of meteorology in simulated results by using the fixed emissions for 2000 and meteorological fields for each year. As a reference parameter, we calculated the area-weighted surface pressure anomaly over the Pacific Ocean east of Japan. When the anomaly has a large negative value, polluted air masses from continental Asia tend to be transported directly to Japan by westerly winds. In contrast, when the anomaly has a large positive value, influence of the outflow from continental Asia tends to be small because the westerly components of wind fields around Japan are comparatively weak. Instead, southerly winds are relatively strong and transport clean air masses from the Pacific Ocean to Japan. Consequently, springtime ozone over Japan is higher (lower) than in ordinary years when the anomaly has a large negative (positive) value. In general, the interannual variation of springtime ozone over Japan is sensitive to the outflow from continental Asia. We also found some correlation between springtime ozone over Japan and the El Niño-Southern Oscillation, indicating that higher and lower springtime ozone over Japan are related to La Niña and El Niño, respectively. Differences in the meridional displacement and diversity of cyclone tracks near Japan between El Niño and La Niña years may be responsible for interannual variations in the springtime boundary layer ozone over Japan.
Atmospheric nanoparticle observations in the low free troposphere during upward orographic flows at Izaña Mountain Observatory

This study investigates the processes and conditions favouring the formation of nanoparticles (diameter<10 nm) which are frequently observed on high mountains reaching the low free troposphere. This was done through an analysis of a data set collected at Izaña Global Atmospheric Watch Observatory (Canary Islands; 2367 m above sea level). This high mountain supersite is located well above the stratocumulus layer characteristic of the subtropical oceanic tropospheres. At night, when the catabic flow regime is well established, free troposphere aerosols were measured. The development of orographic buoyant upward flows during daylight resulted in an increase of water vapour, SO2 and NOy concentrations. These ascending airflows perturbed the free troposphere and resulted in high concentrations of 3–10 nm particles (N3–10) due to new particle formation. An analysis of the 5-min average time series allowed the identification of two main types of N3–10 event. In Type I events a linear relationship between N3–10 and SO2 was observed (r2 coefficients 0.70–0.95 and a mean slope of 11 cm−3 ppt−1 for 5-min averaged data; SO2 concentrations from tens to hundreds of ppt). These particles seem to be formed during upward transport (probably within or after the outflows of clouds typically located below Izaña). During Type II events, no correlation between SO2 and N3–10 was observed and 3–10 nm particles were formed in-situ at noon and during the afternoon due to the condensation of vapours linked to photochemistry. New particle formation was observed almost every day owing to the favourable conditions associated with the entry of boundary layer air in the low free troposphere, even if SO2 concentrations are rather low at Izaña (tens to hundreds of ppt). The low surface area of pre-existing particles, low temperature and high radiation intensity clearly favoured the formation of nanoparticles. The low surface area of pre-existing particles in the upward flows is furthered by in-cloud particles scavenging in the stratocumulus layer typically located below Izaña. The higher temperature and the presence of coarse Saharan dust particles decrease the efficiency of the new particle formation mechanisms in summer. Thus, the "N3–10 versus SO2" slope (for r2>0.7 cases) was higher in autumn and winter (~15 cm−3 ppt−1 as average) than in summer (2–8 cm−3 ppt−1). These field observations suggest that elevated mounts that reaches the free troposphere may act as source regions for new particles.
Tropospheric methane in the tropics – first year from IASI hyperspectral infrared observations

Simultaneous observations from the Infrared Atmospheric Sounding Interferometer (IASI) and from the Advanced Microwave Sounding Unit (AMSU), launched together onboard the European MetOp platform in October 2006, are used to retrieve a mid-to-upper tropospheric content of methane (CH4) in clear-sky conditions, in the tropics, over sea, for the first 16 months of operation of MetOp (July 2007–October 2008). With its high spectral resolution, IASI provides nine channels in the 7.7 μm band highly sensitive to CH4 with reduced sensitivities to other atmospheric variables. These channels, sensitive to both CH4 and temperature, are used in conjunction with AMSU channels, only sensitive to temperature, to decorrelate both signals through a non-linear inference scheme based on neural networks. A key point of this approach is that no use is made of prior information in terms of methane seasonality, trend, or geographical patterns. The precision of the retrieval is estimated to be about 16 ppbv (~0.9%). Features of the retrieved methane space-time distribution include: (1) a strong seasonal cycle of 30 ppbv in the northern tropics with a maximum in January–March and a minimum in July–September, and a flat seasonal cycle in the southern tropics, in agreement with in-situ measurements; (2) a latitudinal decrease of 30 ppbv from 20° N to 20° S, in boreal spring and summer, lower than what is observed at the surface but in excellent agreement with tropospheric aircraft measurements; (3) geographical patterns in good agreement with simulations from the atmospheric transport and chemistry model MOZART-2, but with a higher variability and a higher concentration in boreal winter; (4) signatures of CH4 emissions transported to the middle troposphere such as a large plume of elevated tropospheric methane south of the Asian continent, which might be due to Asian emissions from rice paddies uplifted by deep convection during the monsoon period and then transported towards Indonesia. In addition to bringing a greatly improved view of methane distribution, these results from IASI should provide a means to observe and understand atmospheric transport pathways of methane from the surface to the upper troposphere.
Tula industrial complex (Mexico) emissions of SO2 and NO2 during the MCMA 2006 field campaign using a mobile mini-DOAS system

The Mexico City Metropolitan Area (MCMA) has presented severe pollution problems for many years. There are several point and mobile emission sources inside and outside the MCMA which are known to affect air quality in the area. In particular, speculation has risen as to whether the Tula industrial complex, located 60 km northwest of the MCMA has any influence on high SO2 levels occurring on the northern part of the city, in the winter season mainly. As part of the MILAGRO Field Campaign, from 24 March to 17 April 2006, the differential vertical columns of sulfur dioxide (SO2) and nitrogen dioxide (NO2) were measured during plume transects in the neighborhood of the Tula industrial complex using mobile mini-DOAS instruments. Vertical profiles of wind speed and direction obtained from pilot balloons and radiosondes were used to calculate SO2 and NO2 emissions. According to our measurements, calculated average emissions of SO2 and NO2 during the field campaign were 384±103 and 24±7 tons day−1, respectively. The standard deviation of these estimations is due to actual variations in the observed emissions from the refinery and power plant, as well as to the uncertainty in the wind fields at the exact time of the measurements. Reported values in recent inventories were found to be in good agreement with calculated emissions during the field campaign. Our measurements were also found to be in good agreement with simulated plumes.