bluuebunny/crossref_metadata_2025 huggingface dataset:
Retrieval of aerosol single scattering albedo at ultraviolet wavelengths at the T1 site during MILAGRO
Authors: Corr C. A. , Krotkov N. , Madronich S. , Slusser J. R. , Holben B. , Gao W. , Flynn J. , Lefer B. , Kreidenweis S. M.
Published: April 2010

Abstract. Surface measurements of direct and diffuse voltages at UV wavelengths were made at the T1 site during the MILAGRO (Megacity Initiative: Local and Global Research Observations) field campaign in March 2006, using a multifilter rotating shadowband radiometer (UV-MFRSR). We used the MFRSR data, together with measurements from a co-located CIMEL Sun photometer at the site operating as part of the AERONET network, to deduce aerosol single scattering albedo (ω) at 368 and 332 nm for four cloud-free days during the study. Our retrievals suggest that T1 aerosols with aerosol extinction optical depth τ368>0.1 that are influenced by Mexico City emissions, blowing dust, and biomass burning, are characterized by low ω368=0.73–0.85 and ω332=0.70–0.86, with small or no spectral variation of ω between 368 and 332 nm. Our findings are consistent with other published estimates of ω for Mexico City aerosols, including those that suggest that the absorption attributable to these aerosols is enhanced at UV wavelengths relative to visible wavelengths. We also demonstrate, via sensitivity tests, the importance of accurate τ and surface albedo measurements in ω retrievals at UV wavelengths.
Ozone Monitoring Instrument spectral UV irradiance products: comparison with ground based measurements at an urban environment
Authors: Kazadzis S. , Bais A. , Arola A. , Krotkov N. , Kouremeti N. , Meleti C.
Published: April 2010

Abstract. We have compared spectral ultraviolet overpass irradiances from the Ozone Monitoring Instruments (OMI) against ground-based Brewer measurements at Thessaloniki, Greece from September 2004 to December 2007. It is demonstrated that OMI overestimates UV irradiances by 30%, 17% and 13% for 305 nm, 324 nm, and 380 nm respectively and 20% for erythemally weighted irradiance. The bias between OMI and Brewer increases with increasing aerosol absorption optical thickness. We present methodologies that can be applied for correcting this bias based on experimental results derived from the comparison period and also theoretical approaches using radiative transfer model calculations. All correction approaches minimize the bias and the standard deviation of the ratio OMI versus Brewer ratio. According to the results, the best correction approach suggests that the OMI UV product has to be multiplied by a correction factor CA(λ) of the order of 0.8, 0.88 and 0.9 for 305 nm, 324 nm and 380 nm respectively. Limitations and possibilities for applying such methodologies in a global scale are also discussed.
Quantifying transport into the lowermost stratosphere using simultaneous in-situ measurements of SF6 and CO2
Authors: Bönisch H. , Engel A. , Curtius J. , Birner Th. , Hoor P.
Published: April 2010

Abstract. The seasonality of transport and mixing of air into the lowermost stratosphere (LMS) is studied using distributions of mean age of air and a mass balance approach, based on in-situ observations of SF6 and CO2 during the SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) aircraft campaigns. Combining the information of the mean age of air and the water vapour distributions we demonstrate that the tropospheric air transported into the LMS above the extratropical tropopause layer (ExTL) originates predominantly from the tropical tropopause layer (TTL). The concept of our mass balance is based on simultaneous measurements of the two passive tracers and the assumption that transport into the LMS can be described by age spectra which are superposition of two different modes. Based on this concept we conclude that the stratospheric influence on LMS composition is strongest in April with extreme values of the tropospheric fractions (α1) below 20% and that the strongest tropospheric signatures are found in October with α1 greater than 80%. Beyond the fractions, our mass balance concept allows us to calculate the associated transit times for transport of tropospheric air from the tropics into the LMS. The shortest transit times (<0.3 years) are derived for the summer, continuously increasing up to 0.8 years by the end of spring. These findings suggest that strong quasi-horizontal mixing across the weak subtropical jet from summer to mid of autumn and the considerably shorter residual transport time-scales within the lower branch of the Brewer-Dobson circulation in summer than in winter dominates the tropospheric influence in the LMS until the beginning of next year's summer.
The effect of the solar rotational irradiance variation on the middle and upper atmosphere calculated by a three-dimensional chemistry-climate model
Authors: Gruzdev A. N. , Schmidt H. , Brasseur G. P.
Published: April 2010

Abstract. This paper analyzes the effects of the solar rotational (27-day) irradiance variations on the chemical composition and temperature of the stratosphere, mesosphere and lower thermosphere as simulated by the three-dimensional chemistry-climate model HAMMONIA. Different methods are used to analyze the model results, including high resolution spectral and cross-spectral techniques. To force the simulations, an idealized irradiance variation with a constant period of 27 days (apparent solar rotation period) and with constant amplitude is used. While the calculated thermal and chemical responses are very distinct and permanent in the upper atmosphere, the responses in the stratosphere and mesosphere vary considerably in time despite the constant forcing. The responses produced by the model exhibit a non-linear behavior: in general, the response sensitivities (not amplitudes) decrease with increasing amplitude of the forcing. In the extratropics the responses are, in general, seasonally dependent with frequently stronger sensitivities in winter than in summer. Amplitude and phase lag of the ozone response in the tropical stratosphere and lower mesosphere are in satisfactory agreement with available observations. The agreement between the calculated and observed temperature response is generally worse than in the case of ozone.
Effect of regional precursor emission controls on long-range ozone transport – Part 1: Short-term changes in ozone air quality
Authors: West J. J. , Naik V. , Horowitz L. W. , Fiore A. M.
Published: April 2010

Abstract. Observations and models demonstrate that ozone and its precursors can be transported between continents and across oceans. We model the influences of 10% reductions in anthropogenic nitrogen oxide (NOx) emissions from each of nine world regions on surface ozone air quality in that region and all other regions. In doing so, we quantify the relative importance of long-range transport between all source-receptor pairs, for direct short-term ozone changes. We find that for population-weighted concentrations during the three-month "ozone-season", the strongest inter-regional influences are from Europe to the Former Soviet Union, East Asia to Southeast Asia, and Europe to Africa. The largest influences per unit of NOx reduced, however, are seen for source regions in the tropics and Southern Hemisphere, which we attribute mainly to greater sensitivity to changes in NOx in the lower troposphere, and secondarily to increased vertical convection to the free troposphere in tropical regions, allowing pollutants to be transported further. Results show, for example, that NOx reductions in North America are ~20% as effective per unit NOx in reducing ozone in Europe during summer, as NOx reductions from Europe itself. Reducing anthropogenic emissions of non-methane volatile organic compounds (NMVOCs) and carbon monoxide (CO) by 10% in selected regions, can have as large an impact on long-range ozone transport as NOx reductions, depending on the source region. We find that for many source-receptor pairs, the season of greatest long-range influence does not coincide with the season when ozone is highest in the receptor region. Reducing NOx emissions in most source regions causes a larger decrease in export of ozone from the source region than in ozone production outside of the source region.
Eddy covariance fluxes of acyl peroxy nitrates (PAN, PPN and MPAN) above a Ponderosa pine forest
Authors: Wolfe G. M. , Thornton J. A. , Yatavelli R. L. N. , McKay M. , Goldstein A. H. , LaFranchi B. , Min K.-E. , Cohen R. C.
Published: April 2010

Abstract. During the Biosphere Effects on AeRosols and Photochemistry EXperiment 2007 (BEARPEX-2007), we observed eddy covariance (EC) fluxes of speciated acyl peroxy nitrates (APNs), including peroxyacetyl nitrate (PAN), peroxypropionyl nitrate (PPN) and peroxymethacryloyl nitrate (MPAN), above a Ponderosa pine forest in the western Sierra Nevada. All APN fluxes are net downward during the day, with a median midday PAN exchange velocity of −0.3 cm s−1; nighttime storage-corrected APN EC fluxes are smaller than daytime fluxes but still downward. Analysis with a standard resistance model shows that loss of PAN to the canopy is not controlled by turbulent or molecular diffusion. Stomatal uptake can account for 25 to 50% of the observed downward PAN flux. Vertical gradients in the PAN thermal decomposition (TD) rate explain a similar fraction of the flux, suggesting that a significant portion of the PAN flux into the forest results from chemical processes in the canopy. The remaining "unidentified" portion of the net PAN flux (~15%) is ascribed to deposition or reactive uptake on non-stomatal surfaces (e.g. leaf cuticles or soil). Shifts in temperature, moisture and ecosystem activity during the summer – fall transition alter the relative contribution of stomatal uptake, non-stomatal uptake and thermochemical gradients to the net PAN flux. Daytime PAN and MPAN exchange velocities are a factor of 3 smaller than those of PPN during the first two weeks of the measurement period, consistent with strong intra-canopy chemical production of PAN and MPAN during this period. Depositional loss of APNs can be 3–21% of the gross gas-phase TD loss depending on temperature. As a source of nitrogen to the biosphere, PAN deposition represents approximately 4–19% of that due to dry deposition of nitric acid at this site.
Study of columnar aerosol size distribution in Hong Kong
Authors: Yang X. , Wenig M.
Published: April 2010

Abstract. 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.
Atmospheric nanoparticle observations in the low free troposphere during upward orographic flows at Izaña Mountain Observatory
Authors: Rodríguez S. , González Y. , Cuevas E. , Ramos R. , Romero P. M. , Abreu-Afonso J. , Redondas A.
Published: April 2010

Abstract. 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
Authors: Crevoisier C. , Nobileau D. , Fiore A. M. , Armante R. , Chédin A. , Scott N. A.
Published: April 2010

Abstract. 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.
Land use change suppresses precipitation
Authors: Junkermann W. , Hacker J. , Lyons T. , Nair U.
Published: April 2010

Abstract. A feedback loop between regional scale deforestation and climate change was investigated in an experiment using novel, small size airborne platforms and instrument setups. Experiments were performed in a worldwide unique natural laboratory in Western Australia, characterized by two adjacent homogeneous observation areas with distinctly different land use characteristics. Conversion of several ten thousand square km of forests into agricultural land began more than a century ago. Changes in albedo, surface roughness, the soil water budget and the planetary boundary layer evolved over decades. Besides different meteorology, we found a significant up to now overlooked source of aerosol over the agriculture area. The enhanced number of cloud condensation nuclei is coupled through the hydrological groundwater cycle with deforestation. Modification of surface properties and aerosol number concentrations are key factors for the observed reduction of precipitation. The results document the importance of aerosol indirect effects on climate due to nanometer size biogenic aerosol and human impact on aerosol sources.
Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) – Part 1: Fine particle composition and organic source apportionment
Authors: Aiken A. C. , Salcedo D. , Cubison M. J. , Huffman J. A. , DeCarlo P. F. , Ulbrich I. M. , Docherty K. S. , Sueper D. , Kimmel J. R. , Worsnop D. R. , Trimborn A. , Northway M. , Stone E. A. , Schauer J. J. , Volkamer R. M. , Fortner E. , de Foy B. , Wang J. , Laskin A. , Shutthanandan V. , Zheng J. , Zhang R. , Gaffney J. , Marley N. A. , Paredes-Miranda G. , Arnott W. P. , Molina L. T. , Sosa G. , Jimenez J. L.
Published: April 2010

Abstract. Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and complementary instrumentation. Mass concentrations, diurnal cycles, and size distributions of inorganic and organic species are similar to results from the CENICA supersite in April 2003 with organic aerosol (OA) comprising about half of the fine PM mass. Positive Matrix Factorization (PMF) analysis of the high resolution OA spectra identified three major components: chemically-reduced urban primary emissions (hydrocarbon-like OA, HOA), oxygenated OA (OOA, mostly secondary OA or SOA), and biomass burning OA (BBOA) that correlates with levoglucosan and acetonitrile. BBOA includes several very large plumes from regional fires and likely also some refuse burning. A fourth OA component is a small local nitrogen-containing reduced OA component (LOA) which accounts for 9% of the OA mass but one third of the organic nitrogen, likely as amines. OOA accounts for almost half of the OA on average, consistent with previous observations. OA apportionment results from PMF-AMS are compared to the PM2.5 chemical mass balance of organic molecular markers (CMB-OMM, from GC/MS analysis of filters). Results from both methods are overall consistent. Both assign the major components of OA to primary urban, biomass burning/woodsmoke, and secondary sources at similar magnitudes. The 2006 Mexico City emissions inventory underestimates the urban primary PM2.5 emissions by a factor of ~4, and it is ~16 times lower than afternoon concentrations when secondary species are included. Additionally, the forest fire contribution is at least an order-of-magnitude larger than in the inventory.
Primary and secondary organic carbon downwind of Mexico City
Authors: Yu X.-Y. , Cary R. A. , Laulainen N. S.
Published: April 2010

Abstract. In order to study particulate matter transport and transformation in the Megacity environment, fine particulate carbon was measured simultaneously at two supersites, suburban T1 and rural T2, downwind of Mexico City during the MILAGRO field campaign in March 2006. Organic carbon (OC), element carbon (EC), and total carbon (TC=OC+EC) were determined in near real-time using a Sunset semi-continuous OCEC field analyzer. The semi-empirical EC tracer method was used to derive primary organic carbon (POC) and secondary organic carbon (SOC). Diurnal variations of primary and secondary carbon were observed at T1 and T2, which resulted from boundary layer inversion and impacted by local traffic patterns. The majority of organic carbon particles at T1 and T2 were secondary. The SOCTC% (SOC%=SOC/TC×100%) at T1 ranged from 0.5–93.8% with an average of 63.5±17.2%. The SOCTC% at T2 ranged from 9.3–98.1% with an average of 67.4±12.4%. The average EC to PM2.5 percentage (ECPM%=EC/PM2.5×100%) and OCPM% were 6.0% and 20.0% over the whole sampling time at T1. The POC to PM percentage (POCPM%) and SOCPM% were 3.7% and 16.3%, respectively at the same site. The maximum ECPM% was 21.2%, and the maximum OCPM% was 57.2% at T1. The maximum POCPM% was 12.9%, and the maximum SOCPM% was 49.7% at T1. Comparison of SOC and POC at T1 and T2 showed similar characteristics under favorable meteorological conditions, which indicated that transport from T1 towards T2 took place. Strong correlations between EC and carbon monoxide (CO) and odd nitrogen species (NO and NOx) were observed at T1. This indicated that EC had nearby sources, such as local traffic emissions. The EC/CO ratio derived by linear regression analysis, with units of μg C/m3 and μg/m3, respectively, was 0.004 at T1. Correlations were also seen between OC and SOC vs. the sum of oxidants, such as O3 and NO2, suggesting the secondary nature of carbons observed at T1.
An operational system for the assimilation of the satellite information on wild-land fires for the needs of air quality modelling and forecasting
Authors: Sofiev M. , Vankevich R. , Lotjonen M. , Prank M. , Petukhov V. , Ermakova T. , Koskinen J. , Kukkonen J.
Published: April 2010

Abstract. This paper investigates a potential of two remotely sensed wild-land fire characteristics: 4-μm Brightness Temperature Anomaly (TA) and Fire Radiative Power (FRP) for the needs of operational chemical transport modelling and short-term forecasting of atmospheric composition and air quality. The treatments of the TA and FRP data are presented and a methodology for evaluating the emission fluxes of primary aerosols (PM2.5 and total PM) is described. The method does not include the complicated analysis of vegetation state, fuel load, burning efficiency and related factors, which are uncertain but inevitably involved in approaches based on burnt-area scars or similar products. The core of the current methodology is based on the empirical emission factors that are used to convert the observed temperature anomalies and fire radiative powers into emission fluxes. These factors have been derived from the analysis of several fire episodes in Europe (28.4–5.5.2006, 15.8–25.8.2006 and in August 2008). These episodes were characterised by: (i) well-identified FRP and TA values, and (ii) available ground-based observations of aerosol concentrations, and optical thickness for the regions where the contribution of the fire smoke to the concentrations of PM2.5 was dominant, in comparison with those of other pollution sources. The emission factors were determined separately for the forested and grassland areas; in case of mixed-type land use, an intermediate scaling was assumed. Despite significant differences between the TA and FRP methodologies, an accurate non-linear fitting was found between the predictions of these approaches. The agreement was comparatively weak only for small fires, for which the accuracy of both products is expected to be low. The applications of the Fire Assimilation System (FAS) in combination with the dispersion model SILAM showed that both the TA and FRP products are suitable for the evaluation of the emission fluxes from wild-land fires. The fire-originated concentrations of aerosols (PM2.5, PM10, sulphates and nitrates) and AOD, as predicted by the SILAM model were mainly within a factor of 2–3 compared with the observations. The main challenges of the FAS improvement include refining of the emission factors globally, determination of the types of fires (smouldering vs flaming), evaluation of the injection heights of the plumes, and predicting the temporal evolution of fires.
Physical properties of High Arctic tropospheric particles during winter
Authors: Bourdages L. , Duck T. J. , Lesins G. , Drummond J. R. , Eloranta E. W.
Published: April 2010

Abstract. A climatology of particle scattering properties in the wintertime High Arctic troposphere, including vertical distributions and effective radii, is presented. The measurements were obtained using a lidar and cloud radar located at Eureka, Nunavut Territory (80° N, 86° W). Four different particle groupings are considered: boundary-layer ice crystals, ice clouds, mixed-phase clouds, and aerosols. Two-dimensional histograms of occurrence probabilities against depolarization, radar/lidar colour ratio and height are given. Colour ratios are related to particle minimum dimensions (i.e., widths rather than lengths) using a Mie scattering model. Ice cloud crystals have effective radii spanning 25–220 µm, with larger particles observed at lower altitudes. Topographic blowing snow residuals in the boundary layer have the smallest crystals at 15–70 µm. Mixed-phase clouds have water droplets and ice crystal precipitation in the 5–40 µm and 40–220 µm ranges, respectively. Ice cloud crystals have depolarization decreasing with height. The depolarization trend is associated with the large ice crystal sub-population. Small crystals depolarize more than large ones in ice clouds at a given altitude, and show constant modal depolarization with height. Ice clouds in the mid-troposphere are sometimes observed to precipitate to the ground. Water clouds are constrained to the lower troposphere (0.5–3.5 km altitude). Aerosols are most abundant near the ground and are frequently mixed with the other particle types. The data are used to construct a classification chart for particle scattering in wintertime Arctic conditions.
Technical Note: An assessment of the accuracy of the RTTOV fast radiative transfer model using IASI data
Authors: Matricardi M.
Published: April 2010

Abstract. IASI measurements of spectral radiances made between the 1st April 2008 and the 15th April 2008 are compared with simulations performed using the RTTOV fast radiative transfer model utilizing regression coefficients based on different line-by-line models. The comparisons are performed within the framework of the European Centre for Medium-Range Weather Forecasts Integrated Forecast System using fields of temperature, water vapour and ozone obtained from short-range forecasts. Simulations are performed to assess the accuracy of the RTTOV computations and investigate relative differences between the line-by-line models and the quality of the spectroscopic databases on which the RTTOV coefficients are based.
Dust events in Beijing, China (2004–2006): comparison of ground-based measurements with columnar integrated observations
Authors: Wu Z. J. , Cheng Y. F. , Hu M. , Wehner B. , Sugimoto N. , Wiedensohler A.
Published: April 2010

Abstract. Ambient particle number size distributions spanning three years were used to characterize the frequency and intensity of atmospheric dust events in the urban areas of Beijing, China in combination with AERONET sun/sky radiometer data. Dust events were classified into two types based on the differences in particle number and volume size distributions and local weather conditions. This categorization was confirmed by aerosol index images, columnar aerosol optical properties, and vertical potential temperature profiles. During the type-1 events, dust particles dominated the total particle volume concentration (<10 μm), with a relative share over 70%. Anthropogenic particles in the Aitken and accumulation mode played a subordinate role here because of high wind speeds (>4 m s−1). The type-2 events occurred in rather stagnant air masses and were characterized by a lower volume fraction of coarse mode particles (on average, 55%). Columnar optical properties showed that the superposition of dust and anthropogenic aerosols in type-2 events resulted in a much higher AOD (average: 1.51) than for the rather pure dust aerosols in type-1 events (average AOD: 0.36). A discrepancy was found between the ground-based and column integrated particle volume size distributions, especially for the coarse mode particles. This discrepancy likely originates from both the limited comparability of particle volume size distributions derived from Sun photometer and in situ number size distributions, and the inhomogeneous vertical distribution of particles during dust events.
Elevated nitrogen-containing particles observed in Asian dust aerosol samples collected at the marine boundary layer of the Bohai Sea and the Yellow Sea
Authors: Geng H. , Park Y. , Hwang H. , Kang S. , Ro C.-U.
Published: April 2010

Abstract. Low-Z particle electron probe X-ray microanalysis (low-Z particle EPMA) shows powerful advantages for the characterization of ambient particulate matter in environmental and geological applications. By the application of the low-Z particle EPMA single particle analysis, an overall examination of 1800 coarse and fine particles (aerodynamic diameters: 2.5–10 μm and 1.0–2.5 μm, respectively) in six samples collected on 28 April–1 May 2006 in the marine boundary layer (MBL) of the Bohai Sea and Yellow Sea was conducted. Three samples (D1, D2, and D3) were collected along the Bohai Bay, Bohai Straits, and Yellow Sea near Korea during an Asian dust storm event while the other three samples (N3, N2, and N1) were collected on non-Asian dust (NAD) days. Based on X-ray spectral and secondary electron image data, 15 different types of particles were identified, in which soil-derived particles were encountered with the largest frequency, followed by (C, N, O)-rich droplets (likely the mixture of organic matter and NH4NO3), particles of marine origin, and carbonaceous, Fe-rich, fly ash, and (C, N, O, S)-rich droplet particles. Results show that during the Asian dust storm event relative abundances of the (C, N, O)-rich droplets and the nitrate-containing secondary soil-derived particles were markedly increased (on average by a factor of 4.5 and 2, respectively in PM2.5−10 fraction and by a factor of 1.9 and 1.5, respectively in PM1.0−2.5 fraction) in the MBL of the Bohai Sea and Yellow Sea, implying that Asian dust aerosols in springtime are an important carrier of gaseous inorganic nitrogen species, especially NOx (or HNO3) and NH3.
Tempo-spatial variation of emission inventories of speciated volatile organic compounds from on-road vehicles in China
Authors: Cai H. , Xie S. D.
Published: April 2010

Abstract. Emission inventories of sixty-seven speciated non-methane volatile organic compounds (NMVOC) from on-road vehicles in China were estimated for the period of 1980–2005, using seven NMVOC emission profiles, which were summarized based on local and international measurements from published literatures dealing with specific vehicle categories running under particular modes. Results show an exponential growth trend of China's historical emissions of alkanes, alkenes, alkines, aromatics and carbonyls during the period of 1980–2005, increasing from 63.9, 39.3, 6.9, 36.8 and 24.1 thousand tons, respectively, in 1980 to 2778.2, 1244.5, 178.7, 1351.7 and 406.0 thousand tons, respectively, in 2005, which coincided well with China's economic growth. Emission inventories of alkenes, aromatics and carbonyls were gridded at a high resolution of 40 km×40 km for air quality simulation and health risk evaluation, using the geographic information system (GIS) methodology. Spatial distribution of speciated NMVOC emissions shows a clear difference in emission densities between developed eastern and relatively underdeveloped western and inland China. Besides, the appearance and expansion of high-emission areas was another notable characteristic of spatial distribution of speciated NMVOC emissions during the period. Emission contributions of vehicle categories to speciated NMVOC groups showed annual variation, due to the variance in the provincial emissions and in the relative fractions of the seven emission profiles adopted at the provincial level. Highly reactive and toxic compounds accounted for high proportions of emissions of speciated NMVOC groups. The most abundant compounds were isopentane, pentane and butane from alkanes; ethene, propene, 2-methyl-2-butene and ethyne from alkenes and alkines; benzene, toluene, ethylbenzene, o-xylene, and m,p-xylene (BTEX) and 1,2,4-trimethylbenzene from aromatics and formaldehyde, acetaldehyde, benzaldehyde and acetone from carbonyls.
Nitric acid in the stratosphere based on Odin observations from 2001 to 2009 – Part 2: High-altitude polar enhancements
Authors: Orsolini Y. J. , Urban J. , Murtagh D. P.
Published: April 2010

Abstract. The wintertime abundance of nitric acid (HNO3) in the polar upper stratosphere displays a strong inter-annual variability, and is known to be strongly influenced by energetic particle precipitation (EPP), primarily by protons during solar proton events (SPEs), but also by precipitating auroral or relativistic electrons. We analyse a multi-year record (August 2001 to April 2009) of middle atmospheric HNO3 measurements by the Sub-Millimeter Radiometer instrument aboard the Odin satellite, with a focus on the polar upper stratosphere. SMR observations show clear evidence of two different types of polar high-altitude HNO3 enhancements linked to EPP. In the first type, referred to as direct enhancements by analogy with the EPP/NOx direct effect, enhanced HNO3 mixing ratios are observed for a short period (1 week) after a SPE, upwards of a level typically in the mid-stratosphere. In a second type, referred to as indirect enhancements by analogy with the EPP/NOx indirect effect, the descent of mesospheric air triggers a stronger and longer-lasting enhancement. Each of the three major SPEs that occurred during the Northern Hemisphere autumn or winter, in November 2001, October–November 2003 and January 2005, are observed to lead to both direct and indirect HNO3 enhancements. On the other hand, indirect enhancements occur recurrently in winter, are stronger in the Southern Hemisphere, and are influenced by EPP at higher altitudes.
Modelling of cirrus clouds – Part 1b: Structuring cirrus clouds by dynamics
Authors: Spichtinger P. , Gierens K. M.
Published: April 2010

Abstract. A recently developed and validated bulk microphysics scheme for modelling cirrus clouds (Spichtinger and Gierens, 2009), implemented into the anelastic non-hydrostatic model EULAG is used for investigation of the impact of dynamics on the evolution of an arctic cirrostratus. Sensitivity studies are performed, using variation of large-scale updraughts as well as addition of small-scale temperature fluctuations and wind shear. The results show the importance of sedimentation of ice crystals on cloud evolution. Due to non-linear processes like homogeneous nucleation situations can arise where small changes in the outer parameters have large effects on the resulting cloud structure. In-cloud ice supersaturation is a common feature of all our simulations, and we show that dynamics is as least as important for its appearance than is microphysics.
Influence of ice particle model on satellite ice cloud retrieval: lessons learned from MODIS and POLDER cloud product comparison
Authors: Zhang Z. , Yang P. , Kattawar G. , Riedi J. , -Labonnote L. C. , Baum B. A. , Platnick S. , Huang H.-L.
Published: April 2010

Abstract. The influence is investigated of the assumed ice particle microphysical and optical model on inferring ice cloud optical thickness (τ) from satellite measurements of the Earth's reflected shortwave radiance. Ice cloud τ are inferred, and subsequently compared, using products from MODIS (MODerate resolution Imaging Spectroradiometer) and POLDER (POLarization and Directionality of the Earth's Reflectances). POLDER τ values are found to be substantially smaller than those from collocated MODIS data. It is shown that this difference is caused primarily by the use of different ice particle bulk scattering models in the two retrievals, and more specifically, the scattering phase function. Furthermore, the influence of the ice particle model on the derivation of ice cloud radiative forcing (CRF) from satellite retrievals is studied. Three sets of shortwave CRF are calculated using different combinations of the retrieval and associated ice particle models. It is shown that the uncertainty associated with an ice particle model may lead to two types of errors in estimating CRF from satellite retrievals. One stems from the retrieval itself and the other is due to the optical properties, such as the asymmetry factor, used for CRF calculations. Although a comparison of the CRFs reveals that these two types of errors tend to cancel each other, significant differences are still found between the three CRFs, which indicates that the ice particle model affects not only optical thickness retrievals but also CRF calculations. In addition to CRF, the effect of the ice particle model on the derivation of seasonal variation of τ from satellite measurements is discussed. It is shown that optical thickness retrievals based on the same MODIS observations, but derived using different assumptions of the ice particle model, can be substantially different. These differences can be divided into two parts. The first-order difference is mainly caused by the differences in the asymmetry factor. The second-order difference is related to seasonal changes in the sampled scattering angles and therefore dependent on the sun-satellite viewing geometry. Because of this second-order difference, the use of different ice particle models may lead to a different understanding of the seasonal variation of τ.
Long-term tropospheric formaldehyde concentrations deduced from ground-based fourier transform solar infrared measurements
Authors: Jones N. B. , Riedel K. , Allan W. , Wood S. , Palmer P. I. , Chance K. , Notholt J.
Published: April 2010

Abstract. We report a 13-year (1992–2005) dataset of total column measurements of formaldehyde (HCHO) over Lauder, New Zealand, inferred from solar infrared spectra measured using a high-resolution Fourier Transform Spectrometer (FTS). Ambient HCHO concentrations at this rural location are often close to levels typical of remote marine environments (<250 ppt), which are close to the detection limit using standard techniques. Consequently we develop a new method that successfully produces HCHO columns with sufficient sensitivity throughout the whole season. HCHO columns over Lauder have a strong seasonal cycle (±50%), with a mean column of 4.9×1015 molecules cm−2, peaking during summer months. A simple box model of CH4 oxidation reproduces the observed broad-scale seasonal cycle, but significantly underestimates the seasonal peak HCHO ground concentrations during summer. This suggests the existence of an additional significant source of HCHO, possibly isoprene that cannot be explained by oxidation of CH4 alone. The ground-based FTS column data compare well with collocated HCHO column measurements from the Global Ozone Monitoring Experiment (GOME) satellite instrument during the operational period of GOME (1996–2001, r2=0.65, mean bias=10%, n=48).
Chemically-resolved aerosol volatility measurements from two megacity field studies
Authors: Huffman J. A. , Docherty K. S. , Aiken A. C. , Cubison M. J. , Ulbrich I. M. , DeCarlo P. F. , Sueper D. , Jayne J. T. , Worsnop D. R. , Ziemann P. J. , Jimenez J. L.
Published: April 2010

Abstract. The volatilities of different chemical species in ambient aerosols are important but remain poorly characterized. The coupling of a recently developed rapid temperature-stepping thermodenuder (TD, operated in the range 54–230°C) with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) during field studies in two polluted megacities has enabled the first direct characterization of chemically-resolved urban particle volatility. Measurements in Riverside, CA and Mexico City are generally consistent and show ambient nitrate as having the highest volatility of any AMS standard aerosol species while sulfate showed the lowest volatility. Total organic aerosol (OA) showed volatility intermediate between nitrate and sulfate, with an evaporation rate of 0.6%·K−1 near ambient temperature, although OA dominates the residual species at the highest temperatures. Different types of OA were characterized with marker ions, diurnal cycles, and positive matrix factorization (PMF) and show significant differences in volatility. Reduced hydrocarbon-like OA (HOA, a surrogate for primary OA, POA), oxygenated OA (OOA, a surrogate for secondary OA, SOA), and biomass-burning OA (BBOA) separated with PMF were all determined to be semi-volatile. The most aged OOA-1 and its dominant ion, CO2+, consistently exhibited the lowest volatility, with HOA, BBOA, and associated ions for each among the highest. The similar or higher volatility of HOA/POA compared to OOA/SOA contradicts the current representations of OA volatility in most atmospheric models and has important implications for aerosol growth and lifetime. A new technique using the AMS background signal was demonstrated to quantify the fraction of species up to four orders-of-magnitude less volatile than those detectable in the MS mode, which for OA represent ~5% of the non-refractory (NR) OA signal. Our results strongly imply that all OA types should be considered semivolatile in models. The study in Riverside identified organosulfur species (e.g. CH3HSO3+ ion, likely from methanesulfonic acid), while both studies identified ions indicative of amines (e.g. C5H12N+) with very different volatility behaviors than inorganic-dominated ions. The oxygen-to-carbon ratio of OA in each ambient study was shown to increase both with TD temperature and from morning to afternoon, while the hydrogen-to-carbon ratio showed the opposite trend.
Analysis of the hygroscopic and volatile properties of ammonium sulphate seeded and unseeded SOA particles
Authors: Meyer N. K. , Duplissy J. , Gysel M. , Metzger A. , Dommen J. , Weingartner E. , Alfarra M. R. , Prevot A. S. H. , Fletcher C. , Good N. , McFiggans G. , Jonsson Å. M. , Hallquist M. , Baltensperger U. , Ristovski Z. D.
Published: April 2010

Abstract. The volatile and hygroscopic properties of ammonium sulphate seeded and unseeded secondary organic aerosol (SOA) derived from the photo-oxidation of atmospherically relevant concentrations of α-pinene were studied. The seed particles were electrospray generated ammonium sulphate ((NH4)2SO4) having diameters of approximately 33 nm with a quasi-mono-disperse size distribution (geometric standard deviation σg=1.3). The volatile and hygroscopic properties of both seeded and unseeded SOA were simultaneously measured with a VH-TDMA (volatility – hygroscopicity tandem differential mobility analyzer). VH-TDMA measurements of unseeded SOA show a decrease in the hygroscopic growth (HGF) factor for increased volatilisation temperatures such that the more volatile compounds appear to be more hygroscopic. This is opposite to the expected preferential evaporation of more volatile but less hygroscopic material, but could also be due to enhanced oligomerisation occurring at the higher temperature in the thermodenuder. In addition, HGF measurements of seeded SOA were measured as a function of time at two relative humidities, below (RH 75%) and above (RH 85%) the deliquescence relative humidity (DRH) of the pure ammonium sulphate seeds. As these measurements were conducted during the onset phase of photo-oxidation, during particle growth, they enabled us to find the dependence of the HGF as a function of the volume fraction of the SOA coating. HGF's measured at RH of 85% showed a continuous decrease as the SOA coating thickness increased. The measured growth factors show good agreements with ZSR predictions indicating that, at these RH values, there are only minor solute-solute interactions. At 75% RH, as the SOA fraction increased, a rapid increase in the HGF was observed indicating that an increasing fraction of the (NH4)2SO4 is subject to a phase transition, going into solution, with an increasing volume fraction of SOA. To our knowledge this is the first time that SOA derived from photo-oxidised α-pinene has been shown to affect the equilibrium water content of inorganic aerosols below their DRH. For SOA volume fractions above ~0.3 the measured growth factor followed roughly parallel to the ZSR prediction based on fully dissolved (NH4)2SO4 although with a small difference that was just larger than the error estimate. Both incomplete dissolution and negative solute-solute interactions could be responsible for the lower HGF observed compared to the ZSR predictions.