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Atmospheric Chemistry and Physics - Current Research Articles



Current research articles: Atmospheric Chemistry

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Atmospheric Chemistry and Physics - published by Copernicus Publications

ACP is an international scientific open access journal dedicated to the publication and public discussion of high quality studies investigating the Earth's atmosphere and the underlying chemical and physical processes. It covers the altitude range from the land and ocean surface up to the turbopause, including the troposphere, stratosphere and mesosphere.




Current articles of the journal:



Impacts of different plant functional types on ambient ozone predictions in the Seoul Metropolitan Areas (SMAs), Korea

Impacts of different plant functional types on ambient ozone predictions in the Seoul Metropolitan Areas (SMAs), Korea

Atmospheric Chemistry and Physics, 14, 7461-7484, 2014

Author(s): H.-K. Kim, J.-H. Woo, R. S. Park, C. H. Song, J.-H. Kim, S.-J. Ban, and J.-H. Park

Plant functional type (PFT) distributions affect the results of biogenic emission modeling as well as O3 and particulate matter (PM) simulations using chemistry-transport models (CTMs). This paper analyzes the variations of both surface biogenic volatile organic compound (BVOC) emissions and O3 concentrations due to changes in the PFT distributions in the Seoul Metropolitan Areas, Korea. The Fifth-Generation NCAR/Pennsylvania State Meso-scale Model (MM5)/the Model of Emissions of Gases and Aerosols from Nature (MEGAN)/the Sparse Matrix Operator Kernel Emissions (SMOKE)/the Community Multiscale Air Quality (CMAQ) model simulations were implemented over the Seoul Metropolitan Areas in Korea to predict surface O3 concentrations for the period of 1 May to 31 June 2008. Starting from a performance check of CTM predictions, we consecutively assessed the effects of PFT area deviations on the MEGAN BVOC and CTM O3 predictions, and we further considered the basis of geospatial and statistical analyses. The three PFT data sets considered were (1) the Korean PFT, developed with Korea-specific vegetation database; (2) the CDP PFT, adopted from the community data portal (CDP) of US National Center for Atmospheric Research in the United States (NCAR); (3) MODIS PFT, reclassified from the NASA Terra and Aqua combined land cover products. Although the CMAQ performance check reveals that all of the three different PFT data sets are applicable choices for regulatory modeling practice, noticeable primary data (i.e., PFT and Leaf Area Index (LAI)) was observed to be missing in many geographic locations. Based on the assessed effect of such missing data on CMAQ O3 predictions, we found that this missing data can cause spatially increased bias in CMAQ O3. Thus, it must be resolved in the near future to obtain more accurate biogenic emission and chemistry transport modeling results.

Comparisons of MEGAN biogenic emission results with the three different PFT data showed that broadleaf trees (BTs) are the most significant contributor, followed by needleleaf trees (NTs), shrub (SB), and herbaceous plants (HBs) to the total BVOCs. In addition, isoprene from BTs and terpene from NTs were recognized as significant primary and secondary BVOC species in terms of BVOC emissions distributions and O3-forming potentials in the study domain. A geographically weighted regression analysis with locally compensated ridge (LCR-GWR) with the different PFT data (?O3 vs. ?PFTs) suggests that addition of BT, SB, and NT areas can contribute to O3 increase, whereas addition of an HB area contributes to O3 decrease in the domain.

Assessment results of the simulated spatial and temporal changes of O3 distributions with the different PFT scenarios reveal that hourly and local impacts from the different PFT distributions on occasional inter-deviations of O3 are quite noticeable, reaching up to 13 ppb. The simulated maximum 1 h O3 inter-deviations between different PFT scenarios have an asymmetric diurnal distribution pattern (low in the early morning, rising during the day, peaking at 05:00 p.m., and decreasing during the night) in the study domain. Exponentially diverging hourly BVOC emissions and O3 concentrations with increasing ambient temperature suggest that the use of different PFT distribution data requires much caution when modeling (or forecasting) O3 air quality in complicated urban atmospheric conditions in terms of whether uncertainties in O3 prediction results are expected to be mild or severe.

Posted on 22 July 2014 | 12:00 am


Seasonal variation of aerosol water uptake and its impact on the direct radiative effect at Ny-Ålesund, Svalbard

Seasonal variation of aerosol water uptake and its impact on the direct radiative effect at Ny-Ålesund, Svalbard

Atmospheric Chemistry and Physics, 14, 7445-7460, 2014

Author(s): N. Rastak, S. Silvergren, P. Zieger, U. Wideqvist, J. Ström, B. Svenningsson, M. Maturilli, M. Tesche, A. M. L. Ekman, P. Tunved, and I. Riipinen

In this study we investigated the impact of water uptake by aerosol particles in ambient atmosphere on their optical properties and their direct radiative effect (ADRE, W m−2) in the Arctic at Ny-Ålesund, Svalbard, during 2008. To achieve this, we combined three models, a hygroscopic growth model, a Mie model and a radiative transfer model, with an extensive set of observational data. We found that the seasonal variation of dry aerosol scattering coefficients showed minimum values during the summer season and the beginning of fall (July-August-September), when small particles (< 100 nm in diameter) dominate the aerosol number size distribution. The maximum scattering by dry particles was observed during the Arctic haze period (March-April-May) when the average size of the particles was larger. Considering the hygroscopic growth of aerosol particles in the ambient atmosphere had a significant impact on the aerosol scattering coefficients: the aerosol scattering coefficients were enhanced by on average a factor of 4.30 ± 2.26 (mean ± standard deviation), with lower values during the haze period (March-April-May) as compared to summer and fall. Hygroscopic growth of aerosol particles was found to cause 1.6 to 3.7 times more negative ADRE at the surface, with the smallest effect during the haze period (March-April-May) and the highest during late summer and beginning of fall (July-August-September).

Posted on 21 July 2014 | 12:00 am


Uptake of HO2 radicals onto Arizona test dust particles using an aerosol flow tube

Uptake of HO2 radicals onto Arizona test dust particles using an aerosol flow tube

Atmospheric Chemistry and Physics, 14, 7397-7408, 2014

Author(s): P. S. J. Matthews, M. T. Baeza-Romero, L. K. Whalley, and D. E. Heard

Uptake coefficients for HO2 radicals onto Arizona test dust (ATD) aerosols were measured at room temperature and atmospheric pressure using an aerosol flow tube and the sensitive fluorescence assay by gas expansion (FAGE) technique, enabling HO2 concentrations in the range 3–10 × 108 molecule cm?3 to be investigated. The uptake coefficients were measured as 0.031 ± 0.008 and 0.018 ± 0.006 for the lower and higher HO2 concentrations, respectively, over a range of relative humidities (5–76%). A time dependence for the HO2 uptake onto the ATD aerosols was observed, with larger uptake coefficients observed at shorter reaction times. The combination of time and HO2 concentration dependencies suggest either the partial saturation of the dust surface or that a chemical component of the dust is partially consumed whilst the aerosols are exposed to HO2. A constrained box model is used to show that HO2 uptake to dust surfaces may be an important loss pathway of HO2 in the atmosphere.

Posted on 18 July 2014 | 12:00 am


Single-particle characterization of the high-Arctic summertime aerosol

Single-particle characterization of the high-Arctic summertime aerosol

Atmospheric Chemistry and Physics, 14, 7409-7430, 2014

Author(s): B. Sierau, R. Y.-W. Chang, C. Leck, J. Paatero, and U. Lohmann

Single-particle mass-spectrometric measurements were carried out in the high Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS). The instrument deployed was an aerosol time-of-flight mass spectrometer (ATOFMS) that provides information on the chemical composition of individual particles and their mixing state in real time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 and 3000 nm in diameter showed mass-spectrometric patterns, indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the high Arctic. To assess the importance of long-range particle sources for aerosol–cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest the presence of a particle type of unknown composition and source. In general, the study suffered from low counting statistics due to the overall small number of particles found in this pristine environment, the small sizes of the prevailing aerosol below the detection limit of the ATOFMS, and its low hit rate. To our knowledge, this study reports on the first in situ single-particle mass-spectrometric measurements in the marine boundary layer of the high-Arctic pack ice region.

Posted on 18 July 2014 | 12:00 am


Balloon-borne match measurements of midlatitude cirrus clouds

Balloon-borne match measurements of midlatitude cirrus clouds

Atmospheric Chemistry and Physics, 14, 7341-7365, 2014

Author(s): A. Cirisan, B. P. Luo, I. Engel, F. G. Wienhold, M. Sprenger, U. K. Krieger, U. Weers, G. Romanens, G. Levrat, P. Jeannet, D. Ruffieux, R. Philipona, B. Calpini, P. Spichtinger, and T. Peter

Observations of high supersaturations with respect to ice inside cirrus clouds with high ice water content (> 0.01 g kg−1) and high crystal number densities (> 1 cm−3) are challenging our understanding of cloud microphysics and of climate feedback processes in the upper troposphere. However, single measurements of a cloudy air mass provide only a snapshot from which the persistence of ice supersaturation cannot be judged. We introduce here the "cirrus match technique" to obtain information about the evolution of clouds and their saturation ratio. The aim of these coordinated balloon soundings is to analyze the same air mass twice. To this end the standard radiosonde equipment is complemented by a frost point hygrometer, "SnowWhite", and a particle backscatter detector, "COBALD" (Compact Optical Backscatter AerosoL Detector). Extensive trajectory calculations based on regional weather model COSMO (Consortium for Small-Scale Modeling) forecasts are performed for flight planning, and COSMO analyses are used as a basis for comprehensive microphysical box modeling (with grid scale of 2 and 7 km, respectively). Here we present the results of matching a cirrus cloud to within 2–15 km, realized on 8 June 2010 over Payerne, Switzerland, and a location 120 km downstream close to Zurich. A thick cirrus cloud was detected over both measurement sites. We show that in order to quantitatively reproduce the measured particle backscatter ratios, the small-scale temperature fluctuations not resolved by COSMO must be superimposed on the trajectories. The stochastic nature of the fluctuations is captured by ensemble calculations. Possibilities for further improvements in the agreement with the measured backscatter data are investigated by assuming a very slow mass accommodation of water on ice, the presence of heterogeneous ice nuclei, or a wide span of (spheroidal) particle shapes. However, the resulting improvements from these microphysical refinements are moderate and comparable in magnitude with changes caused by assuming different regimes of temperature fluctuations for clear-sky or cloudy-sky conditions, highlighting the importance of proper treatment of subscale fluctuations. The model yields good agreement with the measured backscatter over both sites and reproduces the measured saturation ratios with respect to ice over Payerne. Conversely, the 30% in-cloud supersaturation measured in a massive 4 km thick cloud layer over Zurich cannot be reproduced, irrespective of the choice of meteorological or microphysical model parameters. The measured supersaturation can only be explained by either resorting to an unknown physical process, which prevents the ice particles from consuming the excess humidity, or – much more likely – by a measurement error, such as a contamination of the sensor housing of the SnowWhite hygrometer by a precipitation drop from a mixed-phase cloud just below the cirrus layer or from some very slight rain in the boundary layer. This uncertainty calls for in-flight checks or calibrations of hygrometers under the special humidity conditions in the upper troposphere.

Posted on 18 July 2014 | 12:00 am


Systematic analysis of tropospheric NO2 long-range transport events detected in GOME-2 satellite data

Systematic analysis of tropospheric NO2 long-range transport events detected in GOME-2 satellite data

Atmospheric Chemistry and Physics, 14, 7367-7396, 2014

Author(s): A. W. Zien, A. Richter, A. Hilboll, A.-M. Blechschmidt, and J. P. Burrows

Intercontinental long-range transport (LRT) events of NO2 relocate the effects of air pollution from emission regions to remote, pristine regions. We detect transported plumes in tropospheric NO2 columns measured by the GOME-2/MetOp-A instrument with a specialized algorithm and trace the plumes to their sources using the HYSPLIT Lagrangian transport model. With this algorithm we find 3808 LRT events over the ocean for the period 2007 to 2011. LRT events occur frequently in the mid-latitudes, emerging usually from coastal high-emission regions. In the free troposphere, plumes of NO2 can travel for several days to the polar oceanic atmosphere or to other continents. They travel along characteristic routes and originate from both continuous anthropogenic emission and emission events such as bush fires. Most NO2 LRT events occur during autumn and winter months, when meteorological conditions and emissions are most favorable. The evaluation of meteorological data shows that the observed NO2 LRT is often linked to cyclones passing over an emission region.

Posted on 18 July 2014 | 12:00 am


Black carbon concentrations and sources in the marine boundary layer of the tropical Atlantic Ocean using four methodologies

Black carbon concentrations and sources in the marine boundary layer of the tropical Atlantic Ocean using four methodologies

Atmospheric Chemistry and Physics, 14, 7431-7443, 2014

Author(s): K. Pohl, M. Cantwell, P. Herckes, and R. Lohmann

Combustion-derived aerosols in the marine boundary layer have been poorly studied, especially in remote environments such as the open Atlantic Ocean. The tropical Atlantic has the potential to contain a high concentration of aerosols, such as black carbon, due to the African emission plume of biomass and agricultural burning products. Atmospheric particulate matter samples across the tropical Atlantic boundary layer were collected in the summer of 2010 during the southern hemispheric dry season when open fire events were frequent in Africa and South America. The highest black carbon concentrations were detected in the Caribbean Sea and within the African plume, with a regional average of 0.6 μg m−3 for both. The lowest average concentrations were measured off the coast of South America at 0.2 to 0.3 μg m−3. Samples were quantified for black carbon using multiple methods to provide insights into the form and stability of the carbonaceous aerosols (i.e., thermally unstable organic carbon, soot like, and charcoal like). Soot-like aerosols composed up to 45% of the carbonaceous aerosols in the Caribbean Sea to as little as 4% within the African plume. Charcoal-like aerosols composed up to 29% of the carbonaceous aerosols over the oligotrophic Sargasso Sea, suggesting that non-soot-like particles could be present in significant concentrations in remote environments. To better apportion concentrations and forms of black carbon, multiple detection methods should be used, particularly in regions impacted by biomass burning emissions.

Posted on 18 July 2014 | 12:00 am


Air quality in the mid-21st century for the city of Paris under two climate scenarios; from the regional to local scale

Air quality in the mid-21st century for the city of Paris under two climate scenarios; from the regional to local scale

Atmospheric Chemistry and Physics, 14, 7323-7340, 2014

Author(s): K. Markakis, M. Valari, A. Colette, O. Sanchez, O. Perrussel, C. Honore, R. Vautard, Z. Klimont, and S. Rao

Ozone and PM2.5 concentrations over the city of Paris are modeled with the CHIMERE air-quality model at 4 km × 4 km horizontal resolution for two future emission scenarios. A high-resolution (1 km × 1 km) emission projection until 2020 for the greater Paris region is developed by local experts (AIRPARIF) and is further extended to year 2050 based on regional-scale emission projections developed by the Global Energy Assessment. Model evaluation is performed based on a 10-year control simulation. Ozone is in very good agreement with measurements while PM2.5 is underestimated by 20% over the urban area mainly due to a large wet bias in wintertime precipitation. A significant increase of maximum ozone relative to present-day levels over Paris is modeled under the "business-as-usual" scenario (+7 ppb) while a more optimistic "mitigation" scenario leads to a moderate ozone decrease (?3.5 ppb) in year 2050. These results are substantially different to previous regional-scale projections where 2050 ozone is found to decrease under both future scenarios. A sensitivity analysis showed that this difference is due to the fact that ozone formation over Paris at the current urban-scale study is driven by volatile organic compound (VOC)-limited chemistry, whereas at the regional-scale ozone formation occurs under NOx-sensitive conditions. This explains why the sharp NOx reductions implemented in the future scenarios have a different effect on ozone projections at different scales. In rural areas, projections at both scales yield similar results showing that the longer timescale processes of emission transport and ozone formation are less sensitive to model resolution. PM2.5 concentrations decrease by 78% and 89% under business-as-usual and mitigation scenarios, respectively, compared to the present-day period. The reduction is much more prominent over the urban part of the domain due to the effective reductions of road transport and residential emissions resulting in the smoothing of the large urban increment modeled in the control simulation.

Posted on 17 July 2014 | 12:00 am


The effect of solar zenith angle on MODIS cloud optical and microphysical retrievals within marine liquid water clouds

The effect of solar zenith angle on MODIS cloud optical and microphysical retrievals within marine liquid water clouds

Atmospheric Chemistry and Physics, 14, 7291-7321, 2014

Author(s): D. P. Grosvenor and R. Wood

In this paper we use a novel observational approach to investigate MODIS satellite retrieval biases of ? and re (using three different MODIS bands: 1.6, 2.1 and 3.7 μm, denoted as re1.6, re2.1 and re3.7, respectively) that occur at high solar zenith angles (θ0) and how they affect retrievals of cloud droplet concentration (Nd). Utilizing the large number of overpasses for polar regions and the diurnal variation of θ0 we estimate biases in the above quantities for an open ocean region that is dominated by low level stratiform clouds.

We find that the mean ? is fairly constant between θ0 = 50° and ~65–70°, but then increases rapidly with an increase of over 70 % between the lowest and highest θ0. The re2.1 and re3.7 decrease with θ0, with effects also starting at around θ0 = 65–70°. At low θ0, the re values from the three different MODIS bands agree to within around 0.2 μm, whereas at high θ0 the spread is closer to 1 μm. The percentage changes of re with θ0 are considerably lower than those for ?, being around 5 % and 7% for re2.1 and re3.7. For re1.6 there was very little change with θ0. Evidence is provided that these changes are unlikely to be due to any physical diurnal cycle.

The increase in ? and decrease in re both contribute to an overall increase in Nd of 40–70% between low and high θ0. Whilst the overall re changes are quite small, they are not insignificant for the calculation of Nd; we find that the contributions to Nd biases from the ? and re biases were roughly comparable for re3.7, although for the other re bands the ? changes were considerably more important. Also, when considering only the clouds with the more heterogeneous tops, the importance of the re biases was considerably enhanced for both re2.1 and re3.7.

When using the variability of 1 km resolution ? data (γτ) as a heterogeneity parameter we obtained the expected result of increasing differences in ? between high and low θ0 as heterogeneity increased, which was not the case when using the variability of 5 km resolution cloud top temperature (σCTT), suggesting that γτ is a better predictor of ? biases at high θ0 than σCTT. For a given θ0, large decreases in re were observed as the cloud top heterogeneity changed from low to high values, although it is possible that physical changes to the clouds associated with cloud heterogeneity variation may account for some of this. However, for a given cloud top heterogeneity we find that the value of θ0 affects the sign and magnitude of the relative differences between re1.6, re2.1 and re3.7, which has implications for attempts to retrieve vertical cloud information using the different MODIS bands. The relatively larger decrease in re3.7 and the lack of change of re1.6 with both θ0 and cloud top heterogeneity suggest that re3.7 is more prone to retrieval biases due to high θ0 than the other bands. We discuss some possible reasons for this.

Our results have important implications for individual MODIS swaths at high θ0, which may be used for case studies for example. θ0 values > 65° can occur at latitudes as low as 28° in mid-winter and for higher latitudes the problem will be more acute. Also, Level-3 daily averaged MODIS cloud property data consist of the averages of several overpasses for the high latitudes, which will occur at a range of θ0 values. Thus, some biased data are likely to be included. It is also likely that some of the θ0 effects described here would apply to ? and re retrievals from satellite instruments that use visible light at similar wavelengths along with forward retrieval models that assume plane parallel clouds, such as the GOES imagers, SEVIRI, etc.

Posted on 17 July 2014 | 12:00 am


Simulating the integrated summertime ?14CO2 signature from anthropogenic emissions over Western Europe

Simulating the integrated summertime ?14CO2 signature from anthropogenic emissions over Western Europe

Atmospheric Chemistry and Physics, 14, 7273-7290, 2014

Author(s): D. Bozhinova, M. K. van der Molen, I. R. van der Velde, M. C. Krol, S. van der Laan, H. A. J. Meijer, and W. Peters

Radiocarbon dioxide (14CO2, reported in Δ14CO2) can be used to determine the fossil fuel CO2 addition to the atmosphere, since fossil fuel CO2 no longer contains any 14C. After the release of CO2 at the source, atmospheric transport causes dilution of strong local signals into the background and detectable gradients of Δ14CO2 only remain in areas with high fossil fuel emissions. This fossil fuel signal can moreover be partially masked by the enriching effect that anthropogenic emissions of 14CO2 from the nuclear industry have on the atmospheric Δ14CO2 signature. In this paper, we investigate the regional gradients in 14CO2 over the European continent and quantify the effect of the emissions from nuclear industry. We simulate the emissions and transport of fossil fuel CO2 and nuclear 14CO2 for Western Europe using the Weather Research and Forecast model (WRF-Chem) for a period covering 6 summer months in 2008. We evaluate the expected CO2 gradients and the resulting Δ14CO2 in simulated integrated air samples over this period, as well as in simulated plant samples.

We find that the average gradients of fossil fuel CO2 in the lower 1200 m of the atmosphere are close to 15 ppm at a 12 km × 12 km horizontal resolution. The nuclear influence on Δ14CO2 signatures varies considerably over the domain and for large areas in France and the UK it can range from 20 to more than 500% of the influence of fossil fuel emissions. Our simulations suggest that the resulting gradients in Δ14CO2 are well captured in plant samples, but due to their time-varying uptake of CO2, their signature can be different with over 3‰ from the atmospheric samples in some regions. We conclude that the framework presented will be well-suited for the interpretation of actual air and plant 14CO2 samples.

Posted on 17 July 2014 | 12:00 am


Top-down estimates of biomass burning emissions of black carbon in the Western United States

Top-down estimates of biomass burning emissions of black carbon in the Western United States

Atmospheric Chemistry and Physics, 14, 7195-7211, 2014

Author(s): Y. H. Mao, Q. B. Li, D. Chen, L. Zhang, W.-M. Hao, and K.-N. Liou

We estimate biomass burning and anthropogenic emissions of black carbon (BC) in the western US for May–October 2006 by inverting surface BC concentrations from the Interagency Monitoring of PROtected Visual Environment (IMPROVE) network using a global chemical transport model. We first use active fire counts from the Moderate Resolution Imaging Spectroradiometer (MODIS) to improve the spatiotemporal distributions of the biomass burning BC emissions from the Global Fire Emissions Database (GFEDv2). The adjustment primarily shifts emissions from late to middle and early summer (a 33% decrease in September–October and a 56% increase in June–August) and leads to appreciable increases in modeled surface BC concentrations in early and middle summer, especially at the 1–2 and 2–3 km altitude ranges. We then conduct analytical inversions at both 2° × 2.5° and 0.5° × 0.667° (nested over North America) horizontal resolutions. The a posteriori biomass burning BC emissions for July–September are 31.7 Gg at 2° × 2.5° (an increase by a factor of 4.7) and 19.2 Gg at 0.5° × 0.667° (an increase by a factor of 2.8). The inversion results are rather sensitive to model resolution. The a posteriori biomass burning emissions at the two model resolutions differ by a factor of ~6 in California and the Southwest and by a factor of 2 in the Pacific Northwest. The corresponding a posteriori anthropogenic BC emissions are 9.1 Gg at 2° × 2.5° (a decrease of 48%) and 11.2 Gg at 0.5° × 0.667° (a decrease of 36%). Simulated surface BC concentrations with the a posteriori emissions capture the observed major fire episodes at most sites and the substantial enhancements at the 1–2 and 2–3 km altitude ranges. The a posteriori emissions also lead to large bias reductions (by ~30% on average at both model resolutions) in modeled surface BC concentrations and significantly better agreement with observations (increases in Taylor skill scores of 95% at 2° × 2.5° and 42 % at 0.5° × 0.667°).

Posted on 16 July 2014 | 12:00 am


Trajectory model simulations of ozone (O3) and carbon monoxide (CO) in the lower stratosphere

Trajectory model simulations of ozone (O3) and carbon monoxide (CO) in the lower stratosphere

Atmospheric Chemistry and Physics, 14, 7135-7147, 2014

Author(s): T. Wang, W. J. Randel, A. E. Dessler, M. R. Schoeberl, and D. E. Kinnison

A domain-filling, forward trajectory model originally developed for simulating stratospheric water vapor is used to simulate ozone (O3) and carbon monoxide (CO) in the lower stratosphere. Trajectories are initialized in the upper troposphere, and the circulation is based on reanalysis wind fields. In addition, chemical production and loss rates along trajectories are included using calculations from the Whole Atmosphere Community Climate Model (WACCM). The trajectory model results show good overall agreement with satellite observations from the Aura Microwave Limb Sounder (MLS) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) in terms of spatial structure and seasonal variability. The trajectory model results also agree well with the Eulerian WACCM simulations. Analysis of the simulated tracers shows that seasonal variations in tropical upwelling exerts strong influence on O3 and CO in the tropical lower stratosphere, and the coupled seasonal cycles provide a useful test of the transport simulations. Interannual variations in the tracers are also closely coupled to changes in upwelling, and the trajectory model can accurately capture and explain observed changes during 2005–2011. This demonstrates the importance of variability in tropical upwelling in forcing chemical changes in the tropical lower stratosphere.

Posted on 16 July 2014 | 12:00 am


Diurnal variations of stratospheric ozone measured by ground-based microwave remote sensing at the Mauna Loa NDACC site: measurement validation and GEOSCCM model comparison

Diurnal variations of stratospheric ozone measured by ground-based microwave remote sensing at the Mauna Loa NDACC site: measurement validation and GEOSCCM model comparison

Atmospheric Chemistry and Physics, 14, 7255-7272, 2014

Author(s): A. Parrish, I. S. Boyd, G. E. Nedoluha, P. K. Bhartia, S. M. Frith, N. A. Kramarova, B. J. Connor, G. E. Bodeker, L. Froidevaux, M. Shiotani, and T. Sakazaki

There is presently renewed interest in diurnal variations of stratospheric and mesospheric ozone for the purpose of supporting homogenization of records of various ozone measurements that are limited by the technique employed to being made at certain times of day. We have made such measurements for 19 years using a passive microwave remote sensing technique at the Mauna Loa Observatory (MLO) in Hawaii, which is a primary station in the Network for Detection of Atmospheric Composition Change (NDACC). We have recently reprocessed these data with hourly time resolution to study diurnal variations. We inspected differences between pairs of the ozone spectra (e.g., day and night) from which the ozone profiles are derived to determine the extent to which they may be contaminated by diurnally varying systematic instrumental or measurement effects. These are small, and we have reduced them further by selecting data that meet certain criteria that we established. We have calculated differences between profiles measured at different times: morning–night, afternoon–night, and morning–afternoon and have intercompared these with like profiles derived from the Aura Microwave Limb Sounder (Aura-MLS), the Upper Atmosphere Research Satellite Microwave Limb Sounder (UARS-MLS), the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES), and Solar Backscatter Ultraviolet version 2 (SBUV/2) measurements. Differences between averages of coincident profiles are typically < 1.5% of typical nighttime values over most of the covered altitude range with some exceptions. We calculated averages of ozone values for each hour from the Mauna Loa microwave data, and normalized these to the average for the first hour after midnight for comparison with corresponding values calculated with the Goddard Earth Observing System Chemistry Climate Model (GEOSCCM). We found that the measurements and model output mostly agree to better than 1.5% of the midnight value, with one noteworthy exception: The measured morning–night values are significantly (2–3 %) higher than the modeled ones from 3.2 to 1.8 hPa (~39–43 km), and there is evidence that the measured values are increasing compared to the modeled values before sunrise in this region.

Posted on 16 July 2014 | 12:00 am


Elucidating multipollutant exposure across a complex metropolitan area by systematic deployment of a mobile laboratory

Elucidating multipollutant exposure across a complex metropolitan area by systematic deployment of a mobile laboratory

Atmospheric Chemistry and Physics, 14, 7173-7193, 2014

Author(s): I. Levy, C. Mihele, G. Lu, J. Narayan, N. Hilker, and J. R. Brook

This study evaluates a deployment strategy of a heavily instrumented mobile lab for characterizing multipollutant spatial patterns based upon a limited number of measurement days spread over different seasons. The measurements obtained through this deployment strategy are used to gain insight into average pollutant levels between routine monitoring sites and in relation to emission sources in the region, as well as to assess correlations between pollutant patterns to better understand the nature of urban air pollutant mixtures. A wide range of locations were part of the deployment in order to characterize the distribution of chronic exposures potentially allowing development of exposure models. Comparison of the mobile lab averages to the available adjacent air quality monitoring network stations to evaluate their representativeness showed that they were in reasonable agreement with the annual averages at the monitoring sites, thus providing some evidence that, through the deployment approach, the mobile lab is able to capture the main features of the average spatial patterns. The differences between mobile lab and network averages varied by pollutant with the best agreement for NO2 with a percentage difference of 20%. Sharp differences in the average spatial distribution were found to exist between different pollutants on multiple scales, particularly on the sub-urban scale, i.e., the neighborhood to street scales. For example, NO2 was observed to be 210–265% higher by the main highway in the study region compared to the nearby urban background monitoring site, while black carbon was higher by 180–200% and particle number concentration was 300% higher. The repeated measurements of near-roadway gradients showed that the rate of change differed by pollutant with elevated concentrations detected up to 600–700 m away for some pollutants. These results demonstrate that through systematic deployment mobile laboratory measurements can be used to characterize average or typical concentration patterns, thus providing data to assess monitoring site representativeness, spatial relationships between pollutants, and chronic multipollutant exposure patterns useful for evaluating and developing exposure models for outdoor concentrations in an urban environment.

Posted on 16 July 2014 | 12:00 am


TEM analysis of the internal structures and mineralogy of Asian dust particles and the implications for optical modeling

TEM analysis of the internal structures and mineralogy of Asian dust particles and the implications for optical modeling

Atmospheric Chemistry and Physics, 14, 7233-7254, 2014

Author(s): G. Y. Jeong and T. Nousiainen

Mineral dust interacts with incoming/outgoing electromagnetic radiation in the atmosphere. This interaction depends on the microphysical properties of the dust particles, including size, mineral composition, external morphology, and internal structure. Ideally all of these properties should be accounted for in the remote sensing of dust, the modeling of single-scattering properties, and radiative effect assessment. There have been many reports on the microphysical characterizations of mineral dust, but no investigations of the internal structures of individual dust particles. We explored the interiors of Asian dust particles using the combined application of focused ion beam thin-slice preparation and high-resolution transmission electron microscopy. The results showed that individual dust particles consisted of numerous mineral grains, which were organized into several types of internal structure: single and polycrystalline cores of quartz, feldspars, calcite, and amphibole often with oriented clay coatings; individual clay agglomerates of nano-thin clay platelets showing preferred to random orientations common with coarser mineral inclusions; and platy coarse phyllosilicates (muscovite, biotite, and chlorite). Micron to submicron pores were scattered throughout the interior of particles. Clays in the coatings and agglomerates were dominated by nano-thin platelets of the clay minerals of illite–smectite series including illite, smectite, and their mixed layers with subordinate kaolinite and clay-sized chlorite. Submicron iron oxide grains, dominantly goethite, were distributed throughout the clay agglomerates and coatings. Unlike the common assumptions and simplifications, we found that the analyzed dust particles were irregularly shaped with birefringent, polycrystalline, and polymineralic heterogeneous compositions. Accounting for this structural and mineralogical makeup may improve the remote sensing retrieval of dust and the evaluation of radiation effects, but will also require sophisticated single-scattering modeling. In particular, the observed internal structures of dust particles such as clay coatings, preferred orientation, embedded grains in clays, and pores, have the potential to considerably impact on the light scattering by dust particles. The distribution and size of structural components with contrasting dielectric properties, such as iron oxides, should also be explicitly accounted for.

Posted on 16 July 2014 | 12:00 am


Impact of optimized mixing heights on simulated regional atmospheric transport of CO2

Impact of optimized mixing heights on simulated regional atmospheric transport of CO2

Atmospheric Chemistry and Physics, 14, 7149-7172, 2014

Author(s): R. Kretschmer, C. Gerbig, U. Karstens, G. Biavati, A. Vermeulen, F. Vogel, S. Hammer, and K. U. Totsche

The mixing height (MH) is a crucial parameter in commonly used transport models that proportionally affects air concentrations of trace gases with sources/sinks near the ground and on diurnal scales. Past synthetic data experiments indicated the possibility to improve tracer transport by minimizing errors of simulated MHs. In this paper we evaluate a method to constrain the Lagrangian particle dispersion model STILT (Stochastic Time-Inverted Lagrangian Transport) with MH diagnosed from radiosonde profiles using a bulk Richardson method. The same method was used to obtain hourly MHs for the period September/October 2009 from the Weather Research and Forecasting (WRF) model, which covers the European continent at 10 km horizontal resolution. Kriging with external drift (KED) was applied to estimate optimized MHs from observed and modelled MHs, which were used as input for STILT to assess the impact on CO2 transport. Special care has been taken to account for uncertainty in MH retrieval in this estimation process. MHs and CO2 concentrations were compared to vertical profiles from aircraft in situ data. We put an emphasis on testing the consistency of estimated MHs to observed vertical mixing of CO2. Modelled CO2 was also compared with continuous measurements made at Cabauw and Heidelberg stations. WRF MHs were significantly biased by ~10–20% during day and ~40–60% during night. Optimized MHs reduced this bias to ~5% with additional slight improvements in random errors. The KED MHs were generally more consistent with observed CO2 mixing. The use of optimized MHs had in general a favourable impact on CO2 transport, with bias reductions of 5–45% (day) and 60–90% (night). This indicates that a large part of the found CO2 model–data mismatch was indeed due to MH errors. Other causes for CO2 mismatch are discussed. Applicability of our method is discussed in the context of CO2 inversions at regional scales.

Posted on 16 July 2014 | 12:00 am


Long-term aerosol-mediated changes in cloud radiative forcing of deep clouds at the top and bottom of the atmosphere over the Southern Great Plains

Long-term aerosol-mediated changes in cloud radiative forcing of deep clouds at the top and bottom of the atmosphere over the Southern Great Plains

Atmospheric Chemistry and Physics, 14, 7113-7124, 2014

Author(s): Hongru Yan, Zhanqing Li, Jianping Huang, Maureen Cribb, and Jianjun Liu

Aerosols can alter the macro- and micro-physical properties of deep convective clouds (DCCs) and their radiative forcing (CRF). This study presents what is arguably the first long-term estimate of the aerosol-mediated changes in CRF (AMCRF) for deep cloud systems derived from decade-long continuous ground-based and satellite observations, model simulations, and reanalysis data. Measurements were made at the US Department of Energy's Atmospheric Radiation Measurement Program's Southern Great Plains (SGP) site. Satellite retrievals are from the Geostationary Operational Environmental Satellite. Increases in aerosol loading were accompanied by the thickening of DCC cores and the expansion and thinning of anvils, due presumably to the aerosol invigoration effect (AIV) and the aerosol microphysical effect. Meteorological variables dictating these cloud processes were investigated. Consistent with previous findings, the AIV is most significant when the atmosphere is moist and unstable with weak wind shear. Such aerosol-mediated systematic changes in DCC core thickness and anvil size alter CRF at the top of atmosphere (TOA) and at the surface. Using extensive observations, ~300 DCC systems were identified over a 10 years period at the SGP site (2000–2011) and analyzed. Daily mean AMCRF at the TOA and at the surface are 29.3 W m?2 and 22.2 W m?2, respectively. This net warming effect due to changes in DCC microphysics offsets the cooling resulting from the first aerosol indirect effect.

Posted on 16 July 2014 | 12:00 am


Study of global cloud droplet number concentration with A-Train satellites

Study of global cloud droplet number concentration with A-Train satellites

Atmospheric Chemistry and Physics, 14, 7125-7134, 2014

Author(s): S. Zeng, J. Riedi, C. R. Trepte, D. M. Winker, and Y.-X. Hu

Cloud droplet number concentration (CDNC) is an important microphysical property of liquid clouds that impacts radiative forcing, precipitation and is pivotal for understanding cloud–aerosol interactions. Current studies of this parameter at global scales with satellite observations are still challenging, especially because retrieval algorithms developed for passive sensors (i.e., MODerate Resolution Imaging Spectroradiometer (MODIS)/Aqua) have to rely on the assumption of cloud adiabatic growth. The active sensor component of the A-Train constellation (i.e., Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP)/CALIPSO) allows retrievals of CDNC from depolarization measurements at 532 nm. For such a case, the retrieval does not rely on the adiabatic assumption but instead must use a priori information on effective radius (re), which can be obtained from other passive sensors.

In this paper, re values obtained from MODIS/Aqua and Polarization and Directionality of the Earth Reflectance (POLDER)/PARASOL (two passive sensors, components of the A-Train) are used to constrain CDNC retrievals from CALIOP. Intercomparison of CDNC products retrieved from MODIS and CALIOP sensors is performed, and the impacts of cloud entrainment, drizzling, horizontal heterogeneity and effective radius are discussed. By analyzing the strengths and weaknesses of different retrieval techniques, this study aims to better understand global CDNC distribution and eventually determine cloud structure and atmospheric conditions in which they develop. The improved understanding of CDNC can contribute to future studies of global cloud–aerosol–precipitation interaction and parameterization of clouds in global climate models (GCMs).

Posted on 16 July 2014 | 12:00 am


Radiative signature of absorbing aerosol over the eastern Mediterranean basin

Radiative signature of absorbing aerosol over the eastern Mediterranean basin

Atmospheric Chemistry and Physics, 14, 7213-7231, 2014

Author(s): A. K. Mishra, K. Klingmueller, E. Fredj, J. Lelieveld, Y. Rudich, and I. Koren

The effects of absorbing aerosols on the atmospheric radiation budget and dynamics over the eastern Mediterranean region are studied using satellites and ground-based observations, and radiative transfer model calculations, under summer conditions. Climatology of aerosol optical depth (AOD), single scattering albedo (SSA) and size parameters were analyzed using multi-year (1999–2012) observations from Moderate Resolution Imaging Spectroradiometer (MODIS), Multi-angle Imaging SpectroRadiometer (MISR) and AErosol RObotic NETwork (AERONET). Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP)-derived aerosol vertical distributions and their classifications are used to calculate the AOD of four dominant aerosol types: dust, polluted dust, polluted continental, and marine aerosol over the region. The seasonal mean (June–August 2010) AODs are 0.22 ± 0.02, 0.11 ± 0.04, 0.10 ± 0.04 and 0.06 ± 0.01 for polluted dust, polluted continental, dust and marine aerosol, respectively. Changes in the atmospheric temperature profile as a function of absorbing aerosol loading were derived for the same period using observations from the AIRS satellite. We inferred heating rates in the aerosol layer of ~1.7 ± 0.8 K day?1 between 925 and 850 hPa, which is attributed to aerosol absorption of incoming solar radiation. Radiative transfer model (RTM) calculations show significant atmospheric warming for dominant absorbing aerosol over the region. A maximum atmospheric forcing of +16.7 ± 7.9 Wm?2 is calculated in the case of polluted dust, followed by dust (+9.4 ± 4.9 Wm−2) and polluted continental (+6.4 ± 4.5 Wm−2). RTM-derived heating rate profiles for dominant absorbing aerosol show warming of 0.1–0.9 K day?1 in the aerosol layer (< 3.0 km altitudes), which primarily depend on AODs of the different aerosol types. Diabatic heating due to absorbing aerosol stabilizes the lower atmosphere, which could significantly reduce the atmospheric ventilation. These conditions can enhance the "pollution pool" over the eastern Mediterranean.

Posted on 16 July 2014 | 12:00 am


A global 3-D CTM evaluation of black carbon in the Tibetan Plateau

A global 3-D CTM evaluation of black carbon in the Tibetan Plateau

Atmospheric Chemistry and Physics, 14, 7091-7112, 2014

Author(s): C. He, Q. B. Li, K. N. Liou, J. Zhang, L. Qi, Y. Mao, M. Gao, Z. Lu, D. G. Streets, Q. Zhang, M. M. Sarin, and K. Ram

We systematically evaluate the black carbon (BC) simulations for 2006 over the Tibetan Plateau by a global 3-D chemical transport model (CTM) (GEOS-Chem) driven by GEOS-5 assimilated meteorological fields, using in situ measurements of BC in surface air, BC in snow, and BC absorption aerosol optical depth (AAOD). Using improved anthropogenic BC emission inventories for Asia that account for rapid technology renewal and energy consumption growth (Zhang et al., 2009; Lu et al., 2011) and improved global biomass burning emission inventories that account for small fires (van der Werf et al., 2010; Randerson et al., 2012), we find that model results of both BC in surface air and in snow are statistically in good agreement with observations (biases < 15%) away from urban centers. Model results capture the seasonal variations of the surface BC concentrations at rural sites in the Indo-Gangetic Plain, but the observed elevated values in winter are absent. Modeled surface-BC concentrations are within a factor of 2 of the observations at remote sites. Part of the discrepancy is explained by the deficiencies of the meteorological fields over the complex Tibetan terrain. We find that BC concentrations in snow computed from modeled BC deposition and GEOS-5 precipitation are spatiotemporally consistent with observations (r = 0.85). The computed BC concentrations in snow are a factor of 2–4 higher than the observations at several Himalayan sites because of excessive BC deposition. The BC concentrations in snow are biased low by a factor of 2 in the central plateau, which we attribute to the absence of snow aging in the CTM and strong local emissions unaccounted for in the emission inventories. Modeled BC AAOD is more than a factor of 2 lower than observations at most sites, particularly to the northwest of the plateau and along the southern slopes of the Himalayas in winter and spring, which is attributable in large part to underestimated emissions and the assumption of external mixing of BC aerosols in the model. We find that assuming a 50% increase of BC absorption associated with internal mixing reduces the bias in modeled BC AAOD by 57% in the Indo-Gangetic Plain and the northeastern plateau and to the northeast of the plateau, and by 16% along the southern slopes of the Himalayas and to the northwest of the plateau. Both surface BC concentration and AAOD are strongly sensitive to anthropogenic emissions (from China and India), while BC concentration in snow is especially responsive to the treatment of BC aerosol aging. We find that a finer model resolution (0.5° × 0.667° nested over Asia) reduces the bias in modeled surface-BC concentration from 15 to 2%. The large range and non-homogeneity of discrepancies between model results and observations of BC across the Tibetan Plateau undoubtedly undermine current assessments of the climatic and hydrological impact of BC in the region and thus warrant imperative needs for more extensive measurements of BC, including its concentration in surface air and snow, AAOD, vertical profile and deposition.

Posted on 11 July 2014 | 12:00 am





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