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Journal Publications

This section contains all refereed journal publications that have some connection either with the Mace Head Research Station or with members, both present and past, of the Atmospheric Physics Research Cluster at NUI, Galway.

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Documents

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Connecting marine productivity to sea-spray via nanoscale biological processes: Phytoplankton Dance or Death Disco? Connecting marine productivity to sea-spray via nanoscale biological processes: Phytoplankton Dance or Death Disco?

Date added: 02/02/2016
Date modified: 02/03/2016
Filesize: 1.03 MB

Connecting marine productivity to sea-spray via nanoscale biological processes: Phytoplankton Dance or Death Disco? O'Dowd, C,Ceburnis, D,Ovadnevaite, J,Bialek, J,Stengel, DB,Zacharias, M,Nitschke, U,Connan, S,Rinaldi, M,Fuzzi, S,Decesari, S,Facchini, MC,Marullo, S,Santoleri, R,Dell'Anno, A,Corinaldesi, C,Tangherlini, M,Danovaro, R., Scientific Reports 5, Article number: 14883, doi:10.1038/srep14883 (2015)


Bursting bubbles at the ocean-surface produce airborne salt-water spray-droplets, in turn, forming climate-cooling marine haze and cloud layers. The reflectance and ultimate cooling effect of these layers is determined by the spray’s water-uptake properties that are modified through entrainment of ocean-surface organic matter (OM) into the airborne droplets. We present new results illustrating a clear dependence of OM mass-fraction enrichment in sea spray (OMss) on both phytoplankton-biomass, determined from Chlorophyll-a (Chl-a) and Net Primary Productivity (NPP). The correlation coefficient for OMss as a function of Chl-a increased form 0.67 on a daily timescale to 0.85 on a monthly timescale. An even stronger correlation was found as a function of NPP, increasing to 0.93 on a monthly timescale. We suggest the observed dependence is through the demise of the bloom, driven by nanoscale biological processes (such as viral infections), releasing large quantities of transferable OM comprising cell debris, exudates and other colloidal materials. This OM, through aggregation processes, leads to enrichment in sea-spray, thus demonstrating an important coupling between biologically-driven plankton bloom termination, marine productivity and sea-spray modification with potentially significant climate impacts.



 

On the contribution of organics to the North East Atlantic aerosol number concentration On the contribution of organics to the North East Atlantic aerosol number concentration

Date added: 03/22/2013
Date modified: 03/22/2013
Filesize: 1.01 MB

Bialek, J. M. Dall’Osto C. Monahan, D. Beddows and C. O’Dowd, On the contribution of organics to the North East Atlantic aerosol number concentration, Environ. Res. Lett. 7, 044013 (7pp) doi:10.1088/1748-9326/7/4/044013, 2012.


 

Abstract. k-means statistical-cluster analysis of submicron aerosol size distributions is combined with coincident humidity tandem differential mobility analyser data, leading to five unique aerosol categories for hygroscopic growth factors (HGFs): low sea-salt background marine, high sea-salt background marine, coastal nucleation, open ocean nucleation and anthropogenically influenced scenarios. When considering only marine conditions, and generic aerosol species associated with this environment (e.g. non-sea-salt sulfate, sea-salt, partly soluble organic matter and water insoluble organic matter), the two-year annual average contribution to aerosol number concentration from the different generic species was made up as follows: 46% (30–54%) of partially modified ammonium sulfate particles; 23% (11–40%) of partially modified sea-salt; and the remaining 31% (25–35%) contribution attributed to two distinct organic species as evidenced by different, but low, HGFs. The analysis reveals that on annual timescales, _30% of the submicron marine aerosol number concentration is sourced from predominantly organic aerosol while 60% of the anthropogenic aerosol number is predominantly organic. Coastal nucleation events show the highest contribution of the lowest HGF mode (1.19), although this contribution is more likely to be influenced by inorganic iodine oxides. While organic mass internally mixed with inorganic salts will lower the activation potential of these mixed aerosol types, thereby potentially reducing the concentration of cloud condensation nuclei (CCN), pure organic water soluble particles are still likely to be activated into cloud droplets, thereby increasing the concentration of CCN. A combination of dynamics and aerosol concentrations will determine which effect will prevail under given conditions.

 

The regional aerosol-climate model REMO-HAM The regional aerosol-climate model REMO-HAM

Date added: 03/22/2013
Date modified: 03/22/2013
Filesize: 1.96 MB

Pietikäinen, JP, D O'Donnell, C Teichmann, U Karstens, S Pfeifer, J Kazil, R Podzun, S Fiedler, H Kokkola, W Birmili, C O'Dowd, U Baltensperger, E Weingartner, R Gehrig, G Spindler, M Kulmala, J Feichter, D Jacob, A Laaksonen, The regional aerosol-climate model REMO-HAM, Geosci. Model Dev., 5, 1323-1339, doi: 10.5194, 2012.


Abstract. REMO-HAM is a new regional aerosol-climate model. It is based on the REMO regional climate model and includes most of the major aerosol processes. The structure for aerosol is similar to the global aerosol-climate model ECHAM5-HAM, for example the aerosol module HAM is coupled with a two-moment stratiform cloud scheme. On the other hand, REMO-HAM does not include an online coupled aerosol-radiation nor a secondary organic aerosol module. In this work, we evaluate the model and compare the results against ECHAM5-HAM and measurements. Four different measurement sites were chosen for the comparison of total number concentrations, size distributions and gas phase sulphur dioxide concentrations: Hyyti¨al¨a in Finland, Melpitz in Germany, Mace Head in Ireland and Jungfraujoch in Switzerland. REMO-HAM is run with two different resolutions: 50×50 km2and 10×10 km2. Based on our simulations, REMO-HAM is in reasonable agreement with the measured values. The differences in the total number concentrations between REMO-HAM and ECHAM5-HAM can be mainly explained by the difference in the nucleation mode. Since we did not use activation nor kinetic nucleation for the boundary layer, the total number concentrations are somewhat underestimated. From the meteorological point of view, REMO-HAM represents the precipitation fields and 2m temperature profile very well compared to measurement. Overall, we show that REMO-HAM is a functional aerosol-climate model, which will be used in further studies.

Model evaluation of marine primary organic aerosol emission schemes Model evaluation of marine primary organic aerosol emission schemes

Date added: 03/21/2013
Date modified: 03/21/2013
Filesize: 2.12 MB

Gantt, B., M. S. Johnson, N. Meskhidze, J. Sciare, J. Ovadnevaite, D. Ceburnis, C. D. O’Dowd, Model evaluation of marine primary organic aerosol emission schemes, Atmos. Chem. & Phys., 12, 8553–8566, 2012

www.atmos-chem-phys.net/12/8553/2012/ doi:10.5194/acp-12-8553-2012.


Abstract. In this study, several marine primary organic aerosol (POA) emission schemes have been evaluated using the GEOS-Chem chemical transport model in order to provide guidance for their implementation in air quality and climate models. These emission schemes, based on varying dependencies of chlorophyll a concentration ([chl a]) and 10m wind speed (U10), have large differences in their magnitude, spatial distribution, and seasonality. Model comparison with weekly and monthly mean values of the organic aerosol mass concentration at two coastal sites shows that the source function exclusively related to [chl a] does a better job replicating surface observations. Sensitivity simulations in which the negative U10 and positive [chl a] dependence of the organic mass fraction of sea spray aerosol are enhanced show improved prediction of the seasonality of the marine POA concentrations. A top-down estimate of submicron marine POA emissions based on the parameterization that compares best to the observed weekly and monthly mean values of marine organic aerosol surface concentrations has a global average emission rate of 6.3 Tg yr−1. Evaluation of existing marine POA source functions against a case study during which marine POA contributed the major fraction of submicron aerosol mass shows that none of the existing parameterizations are able to reproduce the hourly-averaged observations. Our calculations suggest that in order to capture episodic events and short-term variability in submicron marine POA concentration over the ocean, new source functions need to be developed that are grounded in the physical processes unique to the organic fraction of sea spray aerosol.

 

On the spatial distribution and evolution of ultrafine aerosols in Barcelona On the spatial distribution and evolution of ultrafine aerosols in Barcelona

Date added: 03/21/2013
Date modified: 03/21/2013
Filesize: 2.29 MB

Dall'Osto, M., X. Querol, A. Alastuey, C. O'Dowd, R. M. Harrison, J. Wenger, and F. J. Gómez-Moreno, On the spatial distribution and evolution of ultrafine aerosols in Barcelona, Atmos. Chem. Phys. 13, 741–759, 2013, doi:10.5194/acp-13-741-2013.


Abstract. Sources and evolution of ultrafine particles were investigated both horizontally and vertically in the large urban agglomerate of Barcelona, Spain. Within the SAPUSS project (Solving Aerosol Problems by Using Synergistic Strategies), a large number of instruments was deployed simultaneously at different monitoring sites (road, two urban background, regional background, urban tower 150m a.s.l., urban background tower site 80m a.s.l.) during a 4 week period in September–October 2010. Particle number concentrations (N>5nm) are highly correlated with black carbon (BC) at all sites only under strong vehicular traffic influences. By contrast, under cleaner atmospheric conditions (low condensation sink, CS) such correlation diverges towards much higher N/BC ratios at all sites, indicating additional sources of particles including secondary production of freshly nucleated particles. Size-resolved aerosol distributions (N10−500) as well as particle number concentrations (N>5 nm) allow us to identify three types of nucleation and growth events: (1) a regional type event originating in the whole study region and impacting almost simultaneously the urban city of Barcelona and the surrounding urban background area; (2) a regional type event impacting only the regional background area but not the urban agglomerate; (3) an urban type event which originates only within the city centre but whose growth continues while transported away from the city to the regional background. Furthermore, during these clean air days, higher N are found at tower level than at ground level only in the city centre whereas such a difference is not so pronounced at the remote urban background tower. In other words, this study suggests that the column of air above the city ground level possesses the optimal combination between low CS and high vapour source, hence enhancing the concentrations of freshly nucleated particles. By contrast, within stagnant polluted atmospheric conditions, higher N and BC concentrations are always measured at ground level relative to tower level at all sites. Our study suggests that the city centre of Barcelona is a source of non-volatile traffic primary particles (29–39% of N>5nm), but other sources, including secondary freshly nucleated particles contribute up to 61–71% of particle number (N>5nm) at all sites. We suggest that organic compounds evaporating from freshly emitted traffic particles are a possible candidate for new particle formation within the city and urban plume.

 

 On the effect of wind speed on submicron sea salt mass concentrations and source fluxes On the effect of wind speed on submicron sea salt mass concentrations and source fluxes

Date added: 03/21/2013
Date modified: 03/21/2013
Filesize: 2.25 MB

Ovadnevaite, J., D. Ceburnis, M. Canagaratna, H. Berresheim, J. Bialek, G. Martucci, D. R. Worsnop, and C. O’Dowd, On the effect of wind speed on submicron sea salt mass concentrations and source fluxes, J. Geophys. Res., 117, D16201, doi:10.1029/2011JD017379, 2012.


Abstract. A High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was evaluated for its ability to quantify submicron sea salt mass concentrations. The evaluation included both laboratory and field studies. Quantification of the sea salt signal in the HR-ToF-AMS was achieved by taking the 23Na35Cl+ ion as a surrogate for sea salt and then identifying a calibration scaling factor through a comparison with mono-disperse laboratory generated sea salt aerosol. Ambient sea salt concentrations calculated using this method agreed well with those obtained by ion chromatography of filter samples, following a 1:1 regression slope and a correlation coefficient R = 0.93. A key advantage of this AMS-based method is that it allows for high time resolution measurements of sea salt (5 min) along with the speciation of other chemical compounds, including primary organics contributing to sea spray. The high-time resolution sea salt measurement capability enabled the quantification of sea salt mass in both increasing and decreasing wind speed regimes up to 26 m s-1. A mass flux source function was also derived and found to have a power law wind speed dependency with an exponent of 3.1 for increasing winds and 2.3 for decreasing winds. Comparison of the mass flux relationship in this study suggests that previous schemes based on the Monahan whitecap–wind speed approach significantly over-estimate the submicron mass flux. Both the whitecap–wind speed component and the differential whitecap–aerosol productivity component of the source flux function contribute toward the over-estimation.

 

Functionalization and fragmentation during ambient organic aerosol aging: application of the 2-D volatility basis set to field studies Functionalization and fragmentation during ambient organic aerosol aging: application of the 2-D volatility basis set to field studies

Date added: 03/21/2013
Date modified: 03/21/2013
Filesize: 1.84 MB

Murphy, B. N., N. M. Donahue, C. Fountoukis, M. Dall’Osto, C. O’Dowd, A. Kiendler-Scharr, and S. N. Pandis, Functionalization and fragmentation during ambient organic aerosol aging: application of the 2-D volatility basis set to field studies, Atmos. Chem. Phys., 12, 10797–10816, 2012, doi:10.5194/acp-12-10797-2012.


Abstract. Multigenerational oxidation chemistry of atmospheric organic compounds and its effects on aerosol loadings and chemical composition is investigated by implementing the Two-Dimensional Volatility Basis Set (2-D-VBS) in a Lagrangian host chemical transport model. Three model formulations were chosen to explore the complex interactions between functionalization and fragmentation processes during gas-phase oxidation of organic compounds by the hydroxyl radical. The base case model employs a conservative transformation by assuming a reduction of one order of magnitude in effective saturation concentration and an increase of oxygen content by one or two oxygen atoms per oxidation generation. A second scheme simulates functionalization in more detail using group contribution theory to estimate the effects of oxygen addition to the carbon backbone on the compound volatility. Finally, a fragmentation scheme is added to the detailed functionalization scheme to create a functionalization-fragmentation parameterization. Two condensed-phase chemistry pathways are also implemented as additional sensitivity tests to simulate (1) heterogeneous oxidation via OH uptake to the particle-phase and (2) aqueous-phase chemistry of glyoxal and methylglyoxal. The model is applied to summer and winter periods at three sites where observations of organic aerosol (OA) mass and O:C were obtained during the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) campaigns. The base case model reproduces observed mass concentrations and O:C well, with fractional errors (FE) lower than 55% and 25 %, respectively. The detailed functionalization scheme tends to overpredict OA concentrations, especially in the summertime, and also underpredicts O:C by approximately a factor of 2. The detailed functionalization model with fragmentation agrees well with the observations for OA concentration, but still underpredicts O:C. Both heterogeneous oxidation and aqueous-phase processing have small effects on OA levels but heterogeneous oxidation, as implemented here, does enhance O:C by about 0.1. The different schemes result in very different fractional attribution for OA between anthropogenic and biogenic sources.

 

Simulating ultrafine particle formation in Europe using a regional CTM: contribution of primary emissions versus secondary formation to aerosol number concentrations Simulating ultrafine particle formation in Europe using a regional CTM: contribution of primary emissions versus secondary formation to aerosol number concentrations

Date added: 03/21/2013
Date modified: 03/21/2013
Filesize: 2.01 MB

Fountoukis, C., I. Riipinen, H. A. C. Denier van der Gon, P. E. Charalampidis, C. Pilinis, A. Wiedensohler, C. O'Dowd, J. P. Putaud, M. Moerman, and S. N. Pandis, Simulating ultrafine particle formation in Europe using a regional CTM: contribution of primary emissions versus secondary formation to aerosol number concentrations, Atmos. Chem. Phys., 12, 8663–8677, 2012 www.atmos-chem-phys.net/12/8663/2012/ doi:10.5194/acp-12-8663-2012.


Abstract. A three-dimensional regional chemical transport model (CTM) with detailed aerosol microphysics, PMCAMx-UF, was applied to the European domain to simulate the contribution of direct emissions and secondary formation to total particle number concentrations during May 2008. PMCAMx-UF uses the Dynamic Model for Aerosol Nucleation and the Two-Moment Aerosol Sectional (TOMAS) algorithm to track both aerosol number and mass concentration using a sectional approach. The model predicts nucleation events that occur over scales of hundreds up to thousands of kilometers especially over the Balkans and Southeast Europe. The model predictions were compared against measurements from 7 sites across Europe. The model reproduces more than 70% of the hourly concentrations of particles larger than 10 nm (N10) within a factor of 2. About half of these particles are predicted to originate from nucleation in the lower troposphere. Regional nucleation is predicted to increase the total particle number concentration by approximately a factor of 3. For particles larger than 100 nm the effect varies from an increase of 20% in the eastern Mediterranean to a decrease of 20% in southern Spain and Portugal resulting in a small average increase of around 1% over the whole domain. Nucleation has a significant effect in the predicted N50 levels (up to a factor of 2 increase) mainly in areas where there are condensable vapors to grow the particles to larger sizes. A semi-empirical ternary sulfuric acid-ammonia-water parameterization performs better than the activation or the kinetic parameterizations in reproducing the observations. Reducing emissions of ammonia and sulfur dioxide affects certain parts of the number size distribution.

 

Coastal Iodine Emissions: Part 2. Particle Nucleation Processes Coastal Iodine Emissions: Part 2. Particle Nucleation Processes

Date added: 03/21/2013
Date modified: 03/21/2013
Filesize: 2.57 MB

Monahan, C.; Ashu-Ayem, E. R.; Nitschke, U.; Darby, S. B.; Smith, P. D.; Stengel, D. B.; Venables, D. S.; O’Dowd, C. D. Coastal Iodine Emissions: Part 2. Particle Nucleation Processes, dx.doi.org/10.1021/es3011805 | Environ. Sci. Technol. 2012, 46, 10422−10428.


Abstract. Laboratory studies into particle formation from Laminaria digitata macroalgae were undertaken to elucidate aerosol formation for a range of I2 (0.376 ppbv) and O3 (<396 ppbv) mixing ratios and light levels (EPAR = 15, 100, and 235 μmol photons m2 s1). No clear pattern was observed for I2 or aerosol parameters as a function of light levels. Aerosol mass fluxes and particle number concentrations, were, however, correlated with I2 mixing ratios for low O3 mixing ratios of <3 ppbv (R2 = 0.7 and 0.83, respectively for low light levels, and R2 = 0.95 and 0.98, respectively for medium light levels). Additional experiments into particle production as a function of laboratory-generated I2, over a mixing ratio range of 18 ppbv, were conducted under moderate O3 mixing ratios (≈24 ppbv) where a clear, 100-fold or greater, increase in the aerosol number concentrations and mass fluxes was observed compared to the low O3 experiments. A linear relationship between particle concentration and I2 was found, in reasonable agreement with previous studies. Scaling the laboratory relationship to aerosol concentrations typical of the coastal boundary layer suggests a I2 mixing ratio range of 693 pptv can account for the observed particle production events. Aerosol number concentration produced from I2 is more than a factor of 10 higher than that produced from CH2I2 for the same mixing ratios.

 

Coastal iodine emissions: Part 1. Release of I2 by Laminaria digitata in chamber experiments Coastal iodine emissions: Part 1. Release of I2 by Laminaria digitata in chamber experiments

Date added: 03/19/2013
Date modified: 03/19/2013
Filesize: 3.16 MB

Ashu-Ayem, E.R., U, Nitschke, C. Monahan, J. Chen, S.B. Darby, P.D. Smith, C.D. O’Dowd, D. B. Stengel, D.S. Venables. Coastal iodine emissions: Part 1. Release of I2 by Laminaria digitata in chamber experiments, dx.doi.org/10.1021/es204534v | Environ. Sci. Technol. 2012, 46, 10413−10421.


Abstract. Tidally exposed macroalgae emit large amounts of I2 and iodocarbons that produce hotspots of iodine chemistry and intense particle nucleation events in the coastal marine boundary layer. Current emission rates are poorly characterized, however, with reported emission rates varying by 3 orders of magnitude. In this study, I2 emissions from 25 Laminaria digitata samples were investigated in a simulation chamber using incoherent broadband cavity-enhanced absorption spectroscopy (IBBCEAS). The chamber design allowed gradual extraction of seawater to simulate tidal emersion of algae. Samples were exposed to air with or without O3 and to varying irradiances. Emission of I2 occurred in four distinct stages: (1) moderate emissions from partially submerged samples; (2) a strong release by fully emerged samples; (3) slowing or stopping of I2 release; and (4) later pulses of I2 evident in some samples. Emission rates were highly variable and ranged from 7 to 616 pmol min1 gFW1 in ozone-free air, with a median value of 55 pmol min1 gFW1 for 20 samples.

 

Particle mobility size spectrometers: harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions Particle mobility size spectrometers: harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions

Date added: 03/19/2013
Date modified: 03/19/2013
Filesize: 1021.65 kB

Wiedensohler, A., Birmili, W., Nowak, A., Sonntag, A., Weinhold, K., Merkel, M., Wehner, B., Tuch, T., Pfeifer, S., Fiebig, M., Fjäraa, A. M., Asmi, E., Sellegri, K., Depuy, R., Venzac, H., Villani, P., Laj, P., Aalto, P., Ogren, J. A., Swietlicki, E., Roldin, P., Williams, P., Quincey, P., Hüglin, C., Fierz-Schmidhauser, R., Gysel, M., Weingartner, E., Riccobono, F., Santos, S., Grüning, C., Faloon, K., Beddows, D., Harrison, R. M., Monahan, C., Jennings, S. G., O'Dowd, C. D., Marinoni, A., Horn, H.-G., Keck, L., Jiang, J., Scheckman, J., McMurry, P. H., Deng, Z., Zhao, C. S., Moerman, M., Henzing, B., and de Leeuw, G.: Particle mobility size spectrometers: harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions, Atmos. Meas. Techs., Vol 5 Issue 3 Pages 657-685 DOI: 10.5194/amt-5-657-2012,2012.


Abstract. Mobility particle size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide range of applications in atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards and guidelines with respect to the instrumental setup, measurement mode, data evaluation as well as quality control. Technical standards were developed for a minimum requirement of mobility size spectrometry to perform long-term atmospheric aerosol measurements. Technical recommendations include continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyzer. We compared commercial and custom-made inversion routines to calculate the particle number size distributions from the measured electrical mobility distribution. All inversion routines are comparable within few per cent uncertainty for a given set of raw data. Furthermore, this work summarizes the results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research) and ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) to determine present uncertainties especially of custom-built mobility particle size spectrometers. Under controlled laboratory conditions, the particle number size distributions from 20 to 200 nm determined by mobility particle size spectrometers of different design are within an uncertainty range of around ±10% after correcting internal particle losses, while below and above this size range the discrepancies increased. For particles larger than 200 nm, the uncertainty range increased to 30 %, which could not be explained. The network reference mobility spectrometers with identical design agreed within ±4% in the peak particle number concentration when all settings were done carefully. The consistency of these reference instruments to the total particle number concentration was demonstrated to be less than 5 %. Additionally, a new data structure for particle number size distributions was introduced to store and disseminate the data at EMEP (European Monitoring and Evaluation Program). This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data.

 

Photochemical impact on ozone fluxes in Coastal Waters Photochemical impact on ozone fluxes in Coastal Waters

Date added: 03/19/2013
Date modified: 03/19/2013
Filesize: 496.45 kB

Coleman, L., P. McVeigh, H. Berresheim, M. Martino, C.D. O’Dowd, Photochemical impact on ozone fluxes in Coastal Waters, Advances in Meteorology, Volume 2012, Article ID 943785, doi:10.1155/2012/943785, 2012


Abstract. Ozone fluxes, derived from gradient measurements in Northeast Atlantic coastal waters, were observed to depend on both tide height and solar radiation. Peak ozone fluxes of 0.26 ±0.04 μg m2 s1 occurred during low-tide conditions when exposed microalgae fields contributed to the flux footprint. Additionally, at mid-to-high tide, when water surfaces contribute predominantly to the flux footprint, fluxes of the order of 0.12 ±0.03 μg m2 s1 were observed. Considering only fluxes over water covered surfaces, and using an advanced ozone deposition model that accounts for surface-water chemistry enhancing the deposition sink, it is demonstrated that a photochemical enhancement reaction with dissolved organic carbon (DOC) is required to explain the enhanced ozone deposition during daylight hours. This sink amounts to an ozone loss rate of up to 0.6 ppb per hour under peak solar irradiance and points to a missing sink in the marine boundary layer ozone budget.

 

Evaluation of a three-dimensional chemical transport model (PMCAMx) in the European domain during the EUCAARI May 2008 campaign Evaluation of a three-dimensional chemical transport model (PMCAMx) in the European domain during the EUCAARI May 2008 campaign

Date added: 03/19/2013
Date modified: 03/19/2013
Filesize: 1.84 MB

Fountoukis, C., P. N. Racherla, H. A. C. Denier van der Gon, P. Polymeneas, P. E. Haralabidis, C. Pilinis, A. Wiedensohler, M. Dall’Osto, C. O'Dowd, and S. N. Pandis, Evaluation of a three-dimensional chemical transport model (PMCAMx) in the European domain during the EUCAARI May 2008 campaign, Atmos. Chem. Phys., 11, 10331–10347, 2011, doi:10.5194/acp-11-10331-2011, 2011.


Abstract. PMCAMx-2008, a detailed three-dimensional chemical transport model (CTM), was applied to Europe to simulate the mass concentration and chemical composition of particulate matter (PM) during May 2008. The model includes a state-of-the-art organic aerosol module which is based on the volatility basis set framework treating both primary and secondary organic components as semivolatile and photochemically reactive. The model performance is evaluated against high time resolution aerosol mass spectrometer (AMS) ground and airborne measurements. Overall, organic aerosol is predicted to account for 32% of total PM1 at ground level during May 2008, followed by sulfate (30 %), crustal material and sea-salt (14 %), ammonium (13 %), nitrate (7 %), and elemental carbon (4 %). The model predicts that fresh primary OA (POA) is a small contributor to organic PM concentrations in Europe during late spring, and that oxygenated species (oxidized primary and biogenic secondary) dominate the ambient OA. The Mediterranean region is the only area in Europe where sulfate concentrations are predicted to be much higher than the OA, while organic matter is predicted to be the dominant PM1 species in central and northern Europe. The comparison of the model predictions with the ground measurements in four measurement stations is encouraging. The model reproduces more than 94% of the daily averaged data and more than 87% of the hourly data within a factor of 2 for PM1 OA. The model tends to predict relatively flat diurnal profiles for PM1 OA in many areas, both rural and urban in agreement with the available measurements. The model performance against the high time resolution airborne measurements at multiple altitudes and locations is as good as its performance against the ground level hourly measurements. There is no evidence of missing sources of OA aloft over Europe during this period.

 

A Statistical Analysis of North East Atlantic (submicron) Aerosol Size Distributions A Statistical Analysis of North East Atlantic (submicron) Aerosol Size Distributions

Date added: 03/19/2013
Date modified: 03/19/2013
Filesize: 516.78 kB

Dall’Osto, M., C. Monahan, R. Greaney, D.C.S. Beddows, R. M. Harrison, D. Ceburnis and C. D. O’Dowd. A Statistical Analysis of North East Atlantic (submicron) Aerosol Size Distributions., Atmos. Chem. Phys., 11, 12567–12578, 2011, doi:10.5194/acp-11-12567-2011.


Abstract. The Global Atmosphere Watch research station at Mace Head (Ireland) offers the possibility to sample some of the cleanest air masses being imported into Europe as well as some of the most polluted being exported out of Europe. We present a statistical cluster analysis of the physical characteristics of aerosol size distributions in air ranging from the cleanest to the most polluted for the year 2008. Data coverage achieved was 75% throughout the year. By applying the Hartigan-Wong k-Means method, 12 clusters were identified as systematically occurring. These 12 clusters could be further combined into 4 categories with similar characteristics, namely: coastal nucleation category (occurring 21.3% of the time), open ocean nucleation category (occurring 32.6% of the time), background clean marine category (occurring 26.1% of the time) and anthropogenic category (occurring 20% of the time) aerosol size distributions. The coastal nucleation category is characterised by a clear and dominant nucleation mode at sizes less than 10 nm while the open ocean nucleation category is characterised by a dominant Aitken mode between 15 nm and 50 nm. The background clean marine aerosol exhibited a clear bimodality in the sub-micron size distribution, with although it should be noted that either the Aitken mode or the accumulation mode may dominate the number concentration. However, peculiar background clean marine size distributions with coarser accumulation modes are also observed during winter months. By contrast, the continentally-influenced size distributions are generally more monomodal (accumulation), albeit with traces of bimodality. The open ocean category occurs more often during May, June and July, corresponding with the North East (NE) Atlantic high biological period. Combined with the relatively high percentage frequency of occurrence (32.6 %), this suggests that the marine biota is an important source of new nano aerosol particles in NE Atlantic Air.

 

Impact of volcanic ash plume aerosol on cloud microphysics Impact of volcanic ash plume aerosol on cloud microphysics

Date added: 03/19/2013
Date modified: 03/19/2013
Filesize: 3.41 MB

Martucci, M., J. Ovadnevaite, D. Ceburnis, H. Berresheim, S .Varghese, D. Martin, R. Flanagan, C. D. O'Dowd, Impact of volcanic ash plume aerosol on cloud microphysics., Atmos Environ, doi:10.1016/j.atmosenv.2011.12.033 , 2011


Abstract. This study focuses on the dispersion of the Eyjafjallajökull volcanic ash plume over the west of Ireland, at the Mace Head Supersite, and its influence on cloud formation and microphysics during one significant event spanning May 16th and May 17th, 2010. Ground-based remote sensing of cloud microphysics was performed using a Ka-band Doppler cloud RADAR, a LIDAR-ceilometer and a multi-channel microwave radiometer combined with the synergistic analysis scheme SYRSOC (Synergistic Remote Sensing Of Cloud). For this case study of volcanic aerosol interaction with clouds, cloud droplet number concentration (CDNC), liquid water content (LWC), and droplet effective radius (reff) and the relative dispersion were retrieved. A unique cloud type formed over Mace Head characterized by layer-averaged maximum, mean and standard deviation values of the CDNC, reff and LWC: Nmax = 948 cm-3, N = 297 cm-3, σN = 250 cm-3, reff max = 35.5 μm, reff = 4:8 μm, σreff = 4:4 μm, LWCmax =0:23 g m-3, LWC = 0:055 g m-3, σLWC =0:054 g m-3, respectively. The high CDNC, for marine clean air, were associated with large accumulation mode diameter (395 nm) and a hygroscopic growth factor consistent with sulphuric acid aerosol, despite being almost exclusively internally mixed in submicron sizes. Additionally, the Condensation Nuclei (CN, d > 10 nm) to Cloud Condensation Nuclei (CCN) ratio, CCN:CN ~1 at the moderately low supersaturation of 0.25%. This case study illustrates the influence of volcanic aerosols on cloud formation and microphysics and shows that volcanic aerosol can be an efficient CCN.

 

Primary and secondary marine organic aerosols over the North Atlantic Ocean during the MAP experiment Primary and secondary marine organic aerosols over the North Atlantic Ocean during the MAP experiment

Date added: 03/19/2013
Date modified: 03/19/2013
Filesize: 1.9 MB

Decesari, S., E. Finessi, M. Rinaldi, M. Paglione, S. Fuzzi, E. G. Stephanou, T. Tziaras, A.Spyros, D. Ceburnis, C. O'Dowd, M. Dall’Osto, R. Harrison, J. Allan, H. Coe, M. C. Facchini, Primary and secondary marine organic aerosols over the North Atlantic Ocean during the MAP experiment, J. Geophys. Res., 116, D22210, doi:10.1029/2011JD016204, 2011


Abstract.

The organic chemical composition of atmospheric submicron particles in the marine boundary layer was characterized over the northeast Atlantic Ocean in summer 2006, during the season of phytoplankton blooms, in the frame of the Marine Aerosol Production (MAP) experiment. First measurements of water insoluble organic carbon (WIOC) in marine aerosol particles by nuclear magnetic resonance (NMR) spectroscopy showed that it is structurally similar to lipids, resembling the organic fraction of sea spray formed during bubble bursting experiments. The composition of the watersoluble organic carbon (WSOC) fraction was investigated by liquid chromatography mass spectrometry and by 1D and 2DNMR spectroscopy, and showed a less hydrophilic fraction containing traces of fatty acids and rich of alkanoic acids formed by lipid degradation, and a more hydrophilic fraction, containing more functionalized species encompassing short chain aliphatic acids and sulfate esters of hydroxyl carboxylic acids. The more oxidized fraction of WSOC accounts for the oxidized organic aerosol components, which can form by either gastoparticle conversion or extensive chemical aging of lipidcontaining primary particles, as also suggested by the parallel measurements using online mass spectrometric techniques (presented in a companion paper), showing oxidized organic substances internally mixed with sea salt particles. These measurements are also compared with online measurements using an Aerosol TimeOfFlight Mass Spectrometer (ATOFMS) and Aerodyne Aerosol Mass Spectrometer (AMS). Given the large variability in the chemical composition of marine organic aerosol particles, a multitechnique approach is recommended to reduce method dependent categorizations and oversimplifications and to improve the comparability with the results obtained in different oceanic areas.

 

Evidence of a natural marine source of oxalic acid and a possible link to glyoxal Evidence of a natural marine source of oxalic acid and a possible link to glyoxal

Date added: 03/14/2013
Date modified: 03/14/2013
Filesize: 410.96 kB
Rinaldi, Matteo, Stefano Decesari, Claudio Carbone, Emanuela Finessi, Sandro Fuzzi, Darius Ceburnis, Colin D. O’Dowd, Jean Sciare, John P. Burrows, Mihalis Vrekoussis, Barbara Ervens, Kostas Tsigaridis, and Maria Cristina Facchini, Evidence of a natural marine source of oxalic acid and a possible link to glyoxal, J. Geophys. Res., 116, D162,04, 12 PP., 2011, doi:10.1029/2011JD015659, 2011 __________________________________________________ Abstract. This paper presents results supporting the existence of a natural source of oxalic acid over the oceans. Oxalate was detected in “clean‐sector” marine aerosol samples at Mace Head (Ireland) (53°20’N, 9°54′W) during 2006, and at Amsterdam Island (37°48′S, 77°34′E) from 2003 to 2007, in concentrations ranging from 2.7 to 39 ng m−3 and from 0.31 to 17 ng m−3, respectively. The oxalate concentration showed a clear seasonal trend at both sites, with maxima in spring‐summer and minima in fall‐winter, being consistent with other marine biogenic aerosol components (e.g., methanesulfonic acid, non‐sea‐salt sulfate, and aliphatic amines). The observed oxalate was distributed along the whole aerosol size spectrum, with both a submicrometer and a supermicrometer mode, unlike the dominant submicrometer mode encountered in many polluted environments. Given its mass size distribution, the results suggest that over remote oceanic regions oxalate is produced through a combination of different formation processes. It is proposed that the cloud‐mediated oxidation of gaseous glyoxal, recently detected over remote oceanic regions, may be an important source of submicrometer oxalate in the marine boundary layer. Supporting this hypothesis, satellite‐retrieved glyoxal column concentrations over the two sampling sites exhibited the same seasonal concentration trend of oxalate. Furthermore, chemical box model simulations showed that the observed submicrometer oxalate concentrations were consistent with the in‐cloud oxidation of typical marine air glyoxal mixing ratios, as retrieved by satellite measurements, at both sites.

Aerosol analysis and forecast in the ECMWF Integrated Forecast System: 3. Evaluation by means of case studies Aerosol analysis and forecast in the ECMWF Integrated Forecast System: 3. Evaluation by means of case studies

Date added: 03/14/2013
Date modified: 03/14/2013
Filesize: 4.4 MB

Mangold, A., H. De Backer, B. De Paepe, S. Dewitte, I. Chiapello, Y. Derimian, M. Kacenelenbogen, J.‐F. Léon, N. Huneeus, M. Schulz, D. Ceburnis, C. O’Dowd, H. Flentje, S. Kinne, A. Benedetti, J.‐J. Morcrette and O. Boucher, Aerosol analysis and forecast in the ECMWF Integrated Forecast System: 3. Evaluation by means of case studies, J. Geophys. Res., 116, D03302, doi:10.1029/2010JD014864., 2011.


Abstract. A near real‐time system for assimilation and forecasts of aerosols, greenhouse and trace gases, extending the ECMWF Integrated Forecasting System (IFS), has been developed in the framework of the Global and regional Earth‐system Monitoring using Satellite and in‐situ data (GEMS) project. The GEMS aerosol modeling system is novel as it is the first aerosol model fully coupled to a numerical weather prediction model with data assimilation. A reanalysis of the period 2003–2009 has been carried out with the same system. During its development phase, the aerosol system was first run for the time period January 2003 to December 2004 and included sea salt, desert dust, organic matter, black carbon, and sulfate aerosols. In the analysis, Moderate Resolution Imaging Spectroradiometer (MODIS) total aerosol optical depth (AOD) at 550 nm over ocean and land (except over bright surfaces) was assimilated. This work evaluates the performance of the aerosol system by means of case studies. The case studies include (1) the summer heat wave in Europe in August 2003, characterized by forest fire aerosol and conditions of high temperatures and stagnation, favoring photochemistry and secondary aerosol formation, (2) a large Saharan dust event in March 2004, and (3) periods of high and low sea salt aerosol production. During the heat wave period in 2003, the linear correlation coefficients between modeled and observed AOD (550 nm) and between modeled and observed PM2.5 mass concentrations are 0.82 and 0.71, respectively, for all investigated sites together. The AOD is slightly and the PM2.5 mass concentration is clearly overestimated by the aerosol model during this period. The simulated sulfate mass concentration is significantly correlated with observations but is distinctly overestimated. The horizontal and vertical locations of the main features of the aerosol distribution during the Saharan dust outbreak are generally well captured, as well as the timing of the AOD peaks. The aerosol model simulates winter sea salt AOD reasonably well, however, showing a general overestimation. Summer sea salt events show a better agreement. Overall, the assimilation of MODIS AOD data improves the subsequent aerosol predictions when compared with observations, in particular concerning the correlation and AOD peak values. The assimilation is less effective in correcting a positive (PM2.5, sulfate mass concentration, Angström exponent) or negative (desert dust plume AOD) model bias.

 

 

 

 

 

 

Nitrogenated and aliphatic organic vapors as possible drivers for marine secondary organic aerosol growth Nitrogenated and aliphatic organic vapors as possible drivers for marine secondary organic aerosol growth

Date added: 03/13/2013
Date modified: 03/13/2013
Filesize: 1.02 MB

DallOsto, Manuel,Darius Ceburnis, Ciaran Monahan, Douglas R. Worsnop,

Jakub Bialek, Markku Kulmala, Theo Kurtén, Mikael Ehn, John Wenger,

John Sodeau, Robert Healy, and Colin ODowd. (2012), Nitrogenated and aliphatic organic vapors as possible drivers for marine secondary organic aerosol growth, J. Geophys. Res., 117, D12311, doi:10.1029/2012JD017522.


Abstract. Measurements of marine aerosol chemistry, using state-of-the-art mass spectrometry, as well as aerosol microphysics, hygroscopicity and cloud condensation nuclei (CCN) activity were undertaken during new particle growth events. The events were detected in air advecting over North East (NE) Atlantic waters during the EUCAARI Intensive Observation Period in June 2008 at Mace Head, Ireland. During these growth events, the aerosol mass spectrometers illustrated increases in accumulation mode aerosol phase nitrogenated and aliphatic compounds thought to condense from the gas phase. Since the composition changes observed in the accumulation mode occurred simultaneously to the growth of the accumulation, Aitken and nucleation modes, the growth of both the nucleation mode and the Aitken mode is attributed to the condensation of these species. Nitrogenated compounds like amines are also plausible candidates in the nucleation process, as suggested by quantum mechanic calculations. It is also plausible that amides and organic nitrites, also identified by the mass spectrometers, are possible candidate chemical compounds, suggesting that multiple types of chemical species may be contributing. Given that these open ocean aerosol formation and growth events occur in very clean polar marine air masses, we suggest that the organic compounds responsible for particle formation and growth are mainly of biogenic origin. Despite increasing the particle number concentration, the initial effect is to suppress hygroscopicity and CCN activity.

Uncertainties in the determination of global sub-micron marine organic matter emissions Uncertainties in the determination of global sub-micron marine organic matter emissions

Date added: 03/13/2013
Date modified: 03/13/2013
Filesize: 2.97 MB

Albert , M. F. M. A., M. Schaap, A.M.M. Manders, C. Scannell, C.D. ODowd and G. de Leeuw, Uncertainties in the determination of global sub-micron marine organic

matter emissions, Atmos. Environ., 57, 289-300, 2012 http://dx.doi.org/10.1016/j.atmosenv.2012.04.009


Abstract. Organic matter (OM) constitutes an important contribution to the composition of sub-micron sea-spray aerosol produced from biologically active waters. However, OM emission estimates vary by more than an order of magnitude. To estimate the uncertainties in the OM production estimates a sensitivity analysis has been performed in which various parameters have been varied. These include different sea-spray source functions, satellite-retrieved chlorophyll distributions, and a relationship correlating in situ organic mass measurements with satellite-retrieved chlorophyll data. The starting point was a baseline model from which the annual global emission of the water insoluble organic matter (WIOM) fraction in sea spray has been estimated to be 20.4 Tg. In this baseline the global WIOM emission is dominated by the contribution (80%) of the chlorophyll-poor regions (< 0.3 mg m-3). Significant deviations from this estimate are introduced by the choice of the sea-spray source function and the assumed background organic mass fraction, each of which leads to an uncertainty of at least a factor of 2. In particular the chlorophyll-poor regions which dominate the WIOM contribution are strongly affected by the choice of the organic mass fraction parameterisation. The way the chlorophyll data are handled, such as different gap filling approaches, causes deviations in the OM emission that are in the order of 10% and is therefore of less importance. The present research indicates that special attention should be given to the low chlorophyll areas in e.g. the tropics, since there the parameterisations are most uncertain and at the same time these regions dominate total WIOM emissions.

 

Aerosol decadal trends – Part 2: In-situ aerosol particle number concentrations at GAW and ACTRIS stations Aerosol decadal trends – Part 2: In-situ aerosol particle number concentrations at GAW and ACTRIS stations

Date added: 03/12/2013
Date modified: 03/12/2013
Filesize: 6.1 MB

Asmi, A., M. Collaud Coen, J.A. Ogren, E. Andrews, P. Sheridan, A. Jefferson, E. Weingartner, U. Baltensperger, N. Bukowiecki, H. Lihavainen, N. Kivekäs, E. Asmi, P. P. Aalto, M. Kulmala, A. Wiedensohler, W. Birmili, A. Hamed, C. O'Dowd, S. G Jennings, R. Weller, H. Flentje, A. M. Fjaeraa, M. Fiebig, C. L. Myhre, A. G. Hallar, E. Swietlicki, A. Kristensson, and P. Laj,Aerosol decadal trends – Part 2: In-situ aerosol particle number concentrations at GAW and ACTRIS stations, Atmos. Chem. Phys., 13, 895-916, 2013, www.atmos-chem-phys.net/13/895/2013/ doi:10.5194/acp-13-895-2013


Abstract. We have analysed the trends of total aerosol particle number concentrations (N) measured at long-term measurement stations involved either in the Global Atmosphere Watch (GAW) and/or EU infrastructure project ACTRIS. The sites are located in Europe, North America, Antarctica, and on Pacific Ocean islands. The majority of the sites showed clear decreasing trends both in the full-length time series, and in the intra-site comparison period of 2001–2010, especially during the winter months. Several potential driving processes for the observed trends were studied, and even though there are some similarities between N trends and air temperature changes, the most likely cause of many northern hemisphere trends was found to be decreases in the anthropogenic emissions of primary particles, SO2 or some co-emitted species. We could not find a consistent agreement between the trends of N and particle optical properties in the few stations with long time series of all of these properties. The trends of N and the proxies for cloud condensation nuclei (CCN) were generally consistent in the few European stations where the measurements were available. This work provides a useful comparison analysis for modelling studies of trends in aerosol number concentrations.

 

Aerosol decadal trends – Part 1: In-situ optical measurements at GAW and IMPROVE stations Aerosol decadal trends – Part 1: In-situ optical measurements at GAW and IMPROVE stations

Date added: 03/12/2013
Date modified: 03/12/2013
Filesize: 2.64 MB

Collaud Coen, M., E. Andrews, A. Asmi, U. Baltensperger, N. Bukowiecki, D. Day, M. Fiebig, A. M. Fjaeraa, H. Flentje, A. Hyvärinen, A. Jefferson, S. G. Jennings, G. Kouvarakis, H. Lihavainen, C. Lund Myhre, W. C. Malm, N. Mihapopoulos, J. V. Molenar, C. O'Dowd, J. A. Ogren, B. A. Schichtel, P. Sheridan, A. Virkkula, E. Weingartner, R. Weller, and P. Laj,Aerosol decadal trends – Part 1: In-situ optical measurements at GAW and IMPROVE stations, Atmos. Chem. Phys., 13, 869-894, 2013, www.atmos-chem-phys.net/13/869/2013/doi:10.5194/acp-13-869-2013.


Abstract. Currently many ground-based atmospheric stations include in-situ measurements of aerosol physical and optical properties, resulting in more than 20 long-term (> 10 yr) aerosol measurement sites in the Northern Hemisphere and Antarctica. Most of these sites are located at remote locations and monitor the aerosol particle number concentration, wavelength-dependent light scattering, backscattering, and absorption coefficients. The existence of these multi-year datasets enables the analysis of long-term trends of these aerosol parameters, and of the derived light scattering Ångström exponent and backscatter fraction. Since the aerosol variables are not normally distributed, three different methods (the seasonal Mann-Kendall test associated with the Sen's slope, the generalized least squares fit associated with an autoregressive bootstrap algorithm for confidence intervals, and the least-mean square fit applied to logarithms of the data) were applied to detect the long-term trends and their magnitudes. To allow a comparison among measurement sites, trends on the most recent 10 and 15 yr periods were calculated. No significant trends were found for the three continental European sites. Statistically significant trends were found for the two European marine sites but the signs of the trends varied with aerosol property and location. Statistically significant decreasing trends for both scattering and absorption coefficients (mean slope of −2.0% yr−1) were found for most North American stations, although positive trends were found for a few desert and high-altitude sites. The difference in the timing of emission reduction policy for the Europe and US continents is a likely explanation for the decreasing trends in aerosol optical parameters found for most American sites compared to the lack of trends observed in Europe. No significant trends in scattering coefficient were found for the Arctic or Antarctic stations, whereas the Arctic station had a negative trend in absorption coefficient. The high altitude Pacific island station of Mauna Loa presents positive trends for both scattering and absorption coefficients.

 

An assessment of the surface ozone trend in Ireland relevant to air pollution and environmental protection An assessment of the surface ozone trend in Ireland relevant to air pollution and environmental protection

Date added: 03/12/2013
Date modified: 03/12/2013
Filesize: 442.05 kB

Tripathi, Om, P., Stephen G. Jennings, Colin O’Dowd, Barbara O’Leary, Keith Lambkin, Eoin Moran, Simon J. O’Doherty and T. Gerard Spain, An assessment of the surface ozone trend in Ireland relevant to air pollution and environmental protection, Atmos. Pollution Res., 3, 341-351, 2012.


Abstract. Hourly data (1994–2009) of surface ozone concentrations at eight monitoring sites have been investigated to assess target level and long–term objective exceedances and their trends. The European Union (EU) ozone target value for human health (60 ppb–maximum daily 8–hour running mean) has been exceeded for a number of years for almost all sites but never exceeded the set limit of 25 exceedances in one year. Second highest annual hourly and 4th highest annual 8–hourly mean ozone concentrations have shown a statistically significant negative trend for in–land sites of Cork–Glashaboy, Monaghan and Lough Navar and no significant trend for the Mace Head site. Peak afternoon ozone concentrations averaged over a three year period from 2007 to 2009 have been found to be lower than corresponding values over a three–year period from 1996 to 1998 for two sites: Cork–Glashaboy and Lough Navar sites. The EU long–term objective value of AOT40 (Accumulated Ozone Exposure over a threshold of 40 ppb) for protection of vegetation (3 ppm–hour, calculated from May to July) has been exceeded, on an individual year basis, for two sites: Mace Head and Valentia. The critical level for the protection of forest (10 ppm–hour from April to September) has not been exceeded for any site except at Valentia in the year 2003. AOT40–Vegetation shows a significant negative trend for a 3–year running average at Cork–Glashaboy (–0.13±0.02 ppm–hour per year), at Lough Navar (–0.05±0.02 ppm–hour per year) and at Monaghan (–0.03±0.03 ppm–hour per year–not statistically significant) sites. No statistically significant trend was observed for the coastal site of Mace head. Overall, with the exception of the Mace Head and Monaghan sites, ozone measurementrecords at Irish sites show a downward negative trend in peak values that affect human health and vegetation.

 

Wind-driven influences on aerosol light scattering in north-east Atlantic air Wind-driven influences on aerosol light scattering in north-east Atlantic air

Date added: 03/12/2013
Date modified: 03/12/2013
Filesize: 202.6 kB

Vaishya, A., S. G. Jennings, and C. O Dowd (2012), Wind-driven influences on aerosol light scattering in north-east Atlantic air, Geophys. Res. Lett., 39 , L05805, doi:10.1029/ 2011GL050556.


 

Abstract. Ten years (20012010) of aerosol light-scattering measurements in N.E. Atlantic marine air are analysed to determine wind-speed related influences on scattering properties. The scattering coefficient and the backscattering coefficient dependency on wind speed (U) was determined for the winter (Low Biological Activity-LBA) and the summer seasons (High Biological Activity-HBA), and was found to be dependent on ~ U2. In spite of having a U2 dependency, scattering properties for the LBA-period are approximately twice those of the HBA-period. 96% of the LBA-HBA scattering difference can be explained by the combined effects of size distribution and refractive index differences while 70% of the scattering difference can be attributed to a difference in refractive index alone resulting from organic-matter enrichment during the HBA period. The 550 nm scattering coefficient was ~ 70 Mm-1 for ~ 25 ms-1 wind speeds, which is considerably higher than that encountered under polluted air masses in the same region. Indeed, Mulcahy et al. [2008] reported a high correlation between aerosol optical depth (AOD) and wind-speed with AOD values of 0.30.4 at moderately high wind speed. They found a power-law dependency between wind speed and AOD and suggested that sea spray contributed significantly to the direct radiative effect. O’Dowd et al. [1999] highlighted the preferential activation of sea salt nuclei over sulphate nuclei in marine clouds, while Ovadnevaite et al. [2011] found that even the water insoluble organic sea spray plumes have almost a 100% activation efficiency even at a low supersaturation of 0.2%, pointing to a significant role for sea spray in the direct radiative effect. While there have been many studies of aerosol lightscattering in remote locations and in marine air [Bodhaine, 1996; Parameswaran et al., 1998; Pereira et al., 2011], there have been few studies [e.g., Kleefeld et al., 2002] that have reported wind-dependent scattering dependency. The aim of present study is to establish a wind-speed scattering relationship for clean marine air masses for conditions representative of periods with high organic matter enrichment and periods with low organic matter enrichment.

 

Primary versus secondary contributions to particle number concentrations in the European boundary layer Primary versus secondary contributions to particle number concentrations in the European boundary layer

Date added: 03/12/2013
Date modified: 03/12/2013
Filesize: 2.77 MB

C.L. Reddington, K.S. Carslaw, D.V. Spracklen, M.G. Frontoso, L.Collins, J. Merikanto, A. Minikin, T. Hamburger, H.Coe, M. Kulmala, P. Aalto, H. Flentje, C. Plass-Dülmer, W. Birmili, A. Wiedensohler, B. Wehner, T. Tuch, A.Sonntag, C. D. O'Dowd, S.G. Jennings, R.Dupuy, U. Baltensperger, E. Weingartner, H.-C. Hansson, P. Tunved, P. Laj, K. Sellegri, J. Boulon, J.-P. Putaud, C. Gruening, E. Swietlicki, P. Roldin, J. S. Henzing, M. Moerman, N. Mihalopoulos, G. Kouvarakis, V. Ždímal, N. Zíková, A. Marinoni, P. Bonasoni, and R. Duchi,Primary versus secondary contributions to particle number concentrations in the European boundary layer, Atmos. Chem. Phys., 11, 12007-12036, 2011, www.atmos-chem-phys.net/11/12007/2011/ doi:10.5194/acp-11-12007-2011


 

 

 

Abstract. It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2 >0.8) and the normalised mean bias (NMB) was also small (18% for N50 and 1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias R2 >0.8, NMB =52% and 29 %), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the “effective emission size” and composition of primary particles appropriate for different resolution models.

 

Seasonal Variation of the Aerosol Light Scattering Coefficient in Marine Air of the Northeast Atlantic Seasonal Variation of the Aerosol Light Scattering Coefficient in Marine Air of the Northeast Atlantic

Date added: 03/12/2013
Date modified: 03/12/2013
Filesize: 677.22 kB

Aditya Vaishya, S. G. Jennings, and Colin O’Dowd. Seasonal Variation of the Aerosol Light Scattering Coefficient in Marine Air of the Northeast Atlantic, Advances in Meteorology, Volume 2011, Article ID 170490, doi:10.1155/2011/170490.


Abstract. Aerosol light scattering measurements were carried out using a TSI 3563 Nephelometer at the Mace Head Atmospheric Research Station, on the west coast of Ireland from year 2001–2010. A strong seasonal trend in the aerosol light scattering coefficient at 550nm (σscat), for clean marine air masses, is observed with a high σscat value, [average (geometric mean)] of 35.3Mm1(29.5Mm1), in January and a low σscat value of 13.7Mm1 (10.2Mm1), in July. This near threefold increase in the σscat value during the winter season is because of the large contribution of wind-speed generated sea-salt particles in the marine boundary layer. A high positive correlation coefficient of 0.82 was found between the percentage occurrence of relatively large A°ngstrom exponent (A° ) values (>1.2) and the percentage occurrence of lower σscat values (5–15Mm1) in the summer season. σscat and wind-speed have a high positive correlation coefficient of 0.88 whereas A° and wind-speed have a negative correlation coefficient of 0.89.values during the summer months indicate the dominance of sub-μm particles thus indicating the contribution of non-sea-salt sulphate and organics towards the σscat as these species show an enhanced concentration during the summer months.

 

Assessment of changing meteorology and emissions on air quality using a regional climate model: Impact on ozone Assessment of changing meteorology and emissions on air quality using a regional climate model: Impact on ozone

Date added: 03/12/2013
Date modified: 03/12/2013
Filesize: 3.64 MB

Coleman, L. , D. Martin, S. Varghese, S.G. Jennings, C.D. O’Dowd, Assessment of changing meteorology and emissions on air quality using a regional climate model: Impact on ozone, Atmos. Environ., http://dx.doi.org/10.1016/j.atmosenv.2012.11.048, 2012


 

Abstract. A regional climate model is used to assess changes in atmospheric ozone for the years 2030, 2050 and 2100 relative to 2006 brought about by changes in meteorology and emissions. The simulations are evaluated against ozone measurements for 2006, exhibiting good agreement between the model-predicted measurements and the measured annual cycles. Under the RCP6 emission scenario used in these simulations, average ozone mixing ratios are set to reduce by 2.0 ppb over domains encompassing Europe and the North East Atlantic between 2006 and 2100 with the most significant decrease occurring after 2050 due to the pattern in changing emissions. Peak reductions of more than 8 ppb are observed during summer time over mainland Europe by 2100. Model output was studied for three relevant subdomains, namely the North East Atlantic, Ireland and Europe. The relative contribution of changes in both emissions and meteorology is assessed. Over the whole domain, changing emissions are predominantly responsible for changes in surface ozone; although over the North East Atlantic domain, the changing emissions do not perturb surface ozone trends and the decrease in 2100 levels is entirely attributable to changing meteorology.

Primary Marine Organic Aerosol: A Dichotomy of Low Hygroscopicity and High CCN Activity Primary Marine Organic Aerosol: A Dichotomy of Low Hygroscopicity and High CCN Activity

Date added: 11/17/2011
Date modified: 11/17/2011
Filesize: 532.27 kB

Ovadnevaite, J., D. Ceburnis, J. Bialek, C. Monahan, G. Martucci, M. Rinaldi, M.C. Facchini, H. Berresheim, D. R. Worsnop and C. O’Dowd. Primary Marine Organic Aerosol: A Dichotomy of Low Hygroscopicity and High CCN Activity, Geophys. Res. Letts, 38, L21806, doi:10.1029/2011GL048869., 2011


Abstract. High-time resolution measurements of primary marine organic sea-spray physico-chemical properties reveal an apparent dichotomous behavior in terms of water uptake: specifically sea-spray aerosol enriched in organic matter possesses a low hydroscopic Growth Factor (GF~1.25) while simultaneously having a cloud condensation nucleus/condensation nuclei (CCN/CN) activation efficiency of between 83% at 0.25% supersaturation and 100% at 0.75%. In contrast, the activation efficiency of particles dominated by non-sea-salt (nss)-sulfate ranged between 48-100% over supersaturation range of 0.25%-1%. Simultaneous retrieval of Cloud Droplet Number Concentration (CDNC) during primary organic aerosol plumes reveals CDNC concentrations of 350 cm-3 for organic mass concentrations 3-4 mg m-3. It is demonstrated that the retrieved high CDNCs under clean marine conditions can only be explained by organic sea-spray and corroborates the high CCN activation efficiency associated with primary organics. It is postulated that marine hydrogels are responsible for this dichotomous behavior.

Seasonal variation of the aerosol light scattering coefficient in marine air of the North-East Atlan Seasonal variation of the aerosol light scattering coefficient in marine air of the North-East Atlan

Date added: 11/17/2011
Date modified: 11/17/2011
Filesize: 677.22 kB

Vaishya, A., S.G. Jennings and C.D. O'Dowd, Seasonal variation of the aerosol light scattering coefficient in marine air of the North-East Atlantic, Adv. Met., Volume 2011, Article ID 170490, doi:10.1155/2011/170490, 2011.

 

  


Aerosol light scattering measurements were carried out using a TSI 3563 Nephelometer at the Mace Head Atmospheric Research Station, on the west coast of Ireland from year 2001–2010. A strong seasonal trend in the aerosol light scattering coefficient at 550nm (σscat), for clean marine air masses, is observed with a high σscat value, [average (geometric mean)] of 35.3Mm1 (29.5Mm1), in January and a low σscat value of 13.7Mm1 (10.2Mm1), in July. This near threefold increase in the σscat value during the winter season is because of the large contribution of wind-speed generated sea-salt particles in the marine boundary layer. A high positive correlation coefficient of 0.82 was found between the percentage occurrence of relatively large A° ngstro¨m exponent (A° ) values (>1.2) and the percentage occurrence of lower σscat values (5–15Mm1) in the summer season. σscat and wind-speed have a high positive correlation coefficient of 0.88 whereas °Aand wind-speed have a negative correlation coefficient of 0.89. °A values during the summer months indicate the dominance of sub-μm particles thus indicating the contribution of non-sea-salt sulphate and organics towards the σscat as these species show an enhanced concentration during the summer months

 

The Eyjafjallajökull Ash Plume – Part II,  Forecasting the plume dispersion., The Eyjafjallajökull Ash Plume – Part II, Forecasting the plume dispersion.,

Date added: 11/17/2011
Date modified: 11/17/2011
Filesize: 2.21 MB

O’Dowd, C., S. Varghese, R. Flanagan, D. Martin, D. Ceburnis, J. Ovadnevaite, G. Martucci, J. Bialek, C. Monahan, H. Berresheim, A. Vaishya, T. Grigas, S. G. Jennings,  P. McVeigh, E. Moran, K. Lambkin, T. Semmler, and R. McGrath, The Eyjafjallajökull Ash Plume – Part II,  Forecasting the plume dispersion., 10.1016/j.atmosenv.2011.10.037, Atmos. Env. 2011.

 


The recent eruption of Iceland’s Eyjafjallajokull volcano caused extensive disruption across Europe. In this paper, we describe the volcanic ash parameterisation incorporated in the regional climate model (REMOTE) for forecasting volcanic ash dispersion. We investigate model sensitivity to emission parameters including eruption column height and vertical release distribution. Model results over a number of key ash incursion events are assessed in terms of agreement with both ground based measurements and retrieved LIDAR data at a number of European sites.

The Eyjafjallajökull Ash Plume – Part I:  Physical, Chemical and Optical Characteristics, The Eyjafjallajökull Ash Plume – Part I: Physical, Chemical and Optical Characteristics,

Date added: 11/17/2011
Date modified: 11/17/2011
Filesize: 4.93 MB

O’Dowd, C.D., Darius Ceburnis, J. Ovadnevaite, G. Martucci, J. Bialek, C. Monahan, H. Berresheim, A. Vaishya, T. Grigas, S. G. Jennings,  P. McVeigh, S. Varghese, R. Flanagan, D. Martin, E. Moran, K. Lambkin, T. Semmler, C. Perrino, and R. McGrath, The Eyjafjallajökull Ash Plume – Part I:  Physical, Chemical and Optical Characteristics, Atmos. Environ, doi:10.1016/j.atmosenv.2011.07.004, , 2011.

 

 


Abstract. The Eyjafjallajökull ash plume was detected at the Mace Head Atmospheric Research Station numerous times from April 19th till 18th May, 2010 following subsidence into, and dilution in, the boundary layer.  The three strongest of these events, lasting 12-18 hours, are analysed in detail in terms of physical, chemical and optical properties.  The ash size distribution was bimodal with a supermicron mode of 2.5 mm diameter for the one case where it was measured.  The submicron mode varied from 185 nm during the high-explosive phase to 395 nm during the low-explosive phase.  Non-sea-salt (nss)-sulphate mass was 2.5 times higher during the low-explosive phase. Total particle concentrations ranged from 760 cm-3 to 1247 cm-3 and were typical of clean air in the region.    Between 30% and 39% of submicron chemical mass (i.e. exclusive of water content) was ash primarily composed of silicon dioxide while accounting for the water content, the submicron aerosol was composed of primary ash (15%) , nss-sulphate  (25%) and water (55%).  Hygroscopic growth factors were characteristic of sulphate aerosol but revealed an internally-mixed aerosol pointing to a mix of predominantly primary ash, nss-sulphate and water.  For the majority of the ash plumes, all condensation nuclei (CN, diameter >10 nm) were activated into cloud condensation nuclei (CCN) at a supersaturation of 0.25%.  Aerosol absorption increased by about a factor of two in the plume, compared to background levels, while aerosol scattering coefficients increased by an order of magnitude.

Investigating organic aerosol loading in the remote marine environment Investigating organic aerosol loading in the remote marine environment

Date added: 09/01/2011
Date modified: 11/17/2011
Filesize: 2.42 MB

Lapina, K., C.L. Heald, D.V. Spracklen, S.R. Arnold, J.D. Allan, H Coe, G. McFiggans, S.R. Zorn, F. Drewnick, T.S. Bates, L.N. Hawkins, L.M. Russell, A. Smirnov, C. O'Dowd and A.J. Hind. Investigating organic aerosol loading in the remote marine environment, Atmos. Chem. Phys., 11, 8847–8860, 2011, doi:10.5194/acp-11-8847-2011.

 

  

Abstract: Aerosol loading in the marine environment is investigated using aerosol composition

measurements from several research ship campaigns (ICEALOT, MAP, RHaMBLe, VOCALS

and OOMPH), observations of total AOD column from satellite (MODIS) and ship-based instruments (Maritime Aerosol Network, MAN), and a global chemical transport model (GEOS-Chem). This work represents the most comprehensive evaluation of oceanic OM emission inventories to date, by employing aerosol composition measurements obtained from campaigns with wide spatial and temporal coverage. The model

underestimates AOD over the remote oceans on average by 0.02 (21 %), compared to satellite observations, but provides an unbiased simulation of ground-based Maritime Aerosol Network (MAN) observations. Comparison with cruise data demonstrates that the GEOS-Chem simulation of marine sulfate, with the mean observed values ranging between 0.22 μgm−3 and 1.34 μgm−3, is generally unbiased, however surface organic matter (OM) concentrations, with the mean observed concentrations between 0.07 μgm−3 and 0.77 μgm−3, are underestimated by a factor of 2-5 for the standard model run. Addition of a a sub-micron marine OM source of approximately 9 TgCyr−1 brings the model into agreement with the ship-based measurements, however this additional OM source does not explain the model underestimate of marine AOD. The model underestimate of marine AOD is therefore likely the result of a combination of satellite retrieval bias and a missing marine aerosol source (which exhibits a different spatial pattern than existing aerosol in the model).

  


Wind speed dependent size-resolved parameterization for the organic enrichment of sea spray Wind speed dependent size-resolved parameterization for the organic enrichment of sea spray

Date added: 08/25/2011
Date modified: 11/17/2011
Filesize: 714.57 kB

Gantt, B, N. Meskhidze, M.C. Facchini, M. Rinaldi, D. Ceburnis, C.D. O’Dowd, Wind speed dependent size-resolved parameterization for the organic enrichment of sea spray, Atmos. Chem. Phys., 11, 1–13, 2011, www.atmos-chem-phys.net/11/1/2011/doi:10.5194/acp-11-1-2011


Abstract: For oceans to become a significant source of primary organic aerosol, sea spray must be highly enriched with organics relative to the bulk seawater.  We propose that organic enrichment at the air-sea interface, chemical composition of seawater, and the aerosol size are three main parameters controlling the organic mass fraction of sea spray aerosol (OMss).  To test this hypothesis, we developed a new marine primary organic aerosol emission function based on a conceptual relationship between the organic enrichment at the air-sea interface and surface wind speed.  The resulting parameterization is explored using aerosol chemical composition and surface wind speed from Atlantic and Pacific coastal stations, and satellite-derived ocean concentrations of chlorophyll-a, dissolved organic carbon, and particulate organic carbon.  Of all the parameters examined, a multi-variable logistic regression revealed that the combination of 10 meter wind speed and surface chlorophyll-a concentration ([Chl-a]) are the most consistent predictors of OMss.  This relationship, combined the published aerosol size dependence of OMss, resulted in a new parameterization for the organic carbon fraction of sea spray.  Global marine primary organic emission is investigated here by applying this newly-developed relationship to existing sea spray emission functions, satellite-derived [Chl-a], and modeled 10 meter winds.  Analysis of model simulations show that global annual submicron marine organic emission associated with sea spray is estimated to be from 2.8 to 5.6 Tg C yr-1.  This study provides additional evidence that marine primary organic aerosols are a globally significant source of organics in the atmosphere.

 

Quantification of the carbonaceous matter origin in submicron marine aerosol particles by dual carbo Quantification of the carbonaceous matter origin in submicron marine aerosol particles by dual carbo

Date added: 08/25/2011
Date modified: 08/25/2011
Filesize: 5.12 MB

Ceburnis, A. Garbaras, S. Szidat, M. Rinaldi, S. Fahrni, N. Perron, L. Wacker, S. Leinert, V. Remeikis, M. C. Facchini, A. S. H. Prevot, S. G. Jennings, and C. D. O'Dowd. Quantification of the carbonaceous matter origin in submicron marine aerosol particles by dual carbon isotope analysis,  Atmos. Chem. Phys., 11, 8593–8606, 2011, doi:10.5194/acp-11-8593-2011



Abstract.

 

Dual carbon isotope analysis of marine aeroso samples has been performed for the first time demonstrating a potential in organic matter apportionment  etween three principal sources: marine, terrestrial (non-fossil) and fossil fuel due to unique isotopic signatures. The results presented here, utilising combinations of dual carbon isotope analysis, provides conclusive evidence of a dominant biogenic organic fraction to organic aerosol over biologically active oceans. In particular, the NE Atlantic, which is also subjected to notable anthropogenic influences via pollution transport processes, was found to contain 80% organic aerosol matter of biogenic origin directly linked to plankton emissions. The remaining carbonaceous aerosol was of terrestrial origin. By contrast, for polluted air advected out from Europe into the NE Atlantic, the source apportionment is 30% marine biogenic, 40% fossil fuel, and 30% continental non-fossil fuel. The dominant marine organic aerosol source in the atmosphere has significant implications for climate change feedback processes.

 

Evaluation of mixing height retrievals from automatic profiling lidars and ceilometers in view of fu Evaluation of mixing height retrievals from automatic profiling lidars and ceilometers in view of fu

Date added: 08/12/2011
Date modified: 08/12/2011
Filesize: 1.59 MB

Haeffelin, M.,  F. Angelini, Y. Morille, G. Martucci, S. Frey, G. P. Gobbi, S. Lolli, C. D. O'Dowd, L. Sauvage, I. Xueref-Rémy, B. Wastine,  Evaluation of mixing height retrievals from automatic profiling lidars and ceilometers in view of future integrated networks in Europe, Bound. Lay. Met., DOI 10.1007/s10546-011-9643-z, 2011

 

The determination of the depth of daytime and nighttime mixing layers mustbe known very accurately to relate boundary-layer concentrations of gases or particles to upstream fluxes. The mixing-height is parametrized in numerical weather prediction models, so improving the determination of the mixing height will improve the quality of the estimated gas and particle budgets. Datasets of mixing-height diurnal cycles with high temporal and spatial resolutions are sought by various end users. Lidars and ceilometers provide vertical profiles of backscatter from aerosol particles. As aerosols are predominantly concentrated in the mixing layer, lidar backscatter profiles can be used to trace the depth of the mixing layer. Large numbers of automatic profiling lidars and ceilometers are deployed by meteorological services and other agencies in several European countries providing systems to monitor  the mixing height on temporal and spatial scales of unprecedented density. We investigate limitations and capabilities of existing mixing height retrieval algorithms by applying five different retrieval techniques to three different lidars and ceilometers deployed during two 1-month campaigns.We studied three important steps in the mixing height retrieval process, namely the lidar/ceilometer pre-processing to reach sufficient signal-to-noise ratio, gradient detection techniques to find the significant aerosol gradients, and finally quality control and layer attribution to identify the actual mixing height from multiple possible layer detections. We found that layer attribution is by far the most uncertain step. We tested different gradient detection techniques, and found no evidence that the first derivative, wavelet transform, and two-dimensional derivative techniques have different skills to detect one or multiple significant aerosol gradients from lidar and ceilometer attenuated backscatter. However, our study shows that, when mixing height retrievals from a ultraviolet lidar and a near-infrared ceilometer agreed, they were 25–40% more likely to agree with an independent radiosonde mixing height retrieval than when each lidar or ceilometer was used alone. Furthermore, we point to directions that may assist the layer attribution step, for instance using commonly available surface measurements of radiation and temperature to derive surface sensible heat fluxes as a proxy for the intensity of convective mixing. It is a worthwhile effort to pursue such studies so that within a few years automatic profiling lidar and ceilometer networks can be utilized efficiently to monitor mixing heights at the European scale. 

On the ability of pseudo-operational ground-based Light Detection And Ranging (LIDAR) sensors to det On the ability of pseudo-operational ground-based Light Detection And Ranging (LIDAR) sensors to det

Date added: 08/05/2011
Date modified: 08/05/2011
Filesize: 3.35 MB

Milroy, C., Martucci, S. Lolli,  S. Loaec, L. S. I. Xueref-Remy, J. V. Lavrič, C.D. O’Dowd,  On the ability of pseudo-operational ground-based Light Detection And Ranging (LIDAR) sensors to determine boundary-layer structure: intercomparison and comparison with in-situ radiosounding, Atmos. Meas. Tech. Diss.. 1–35, 2011 www.atmos-meas-tech discuss.net/4/1/2011/doi:10.5194/amtd-4-1-2011, 2011

 


 

Twenty-one cases of boundary-layer (BL) structure were retrieved by three co-located remote sensors, one lidar (Leosphere ALS300) and two ceilometers (Vaisala CL31, Jenoptik CHM15K). Data were collected during the ICOS field campaign held at the

GAW Atmospheric Station of Mace Head, Ireland, from 8 to 28 June 2009. The study is a two-step investigation of the BL structure based (i) on the intercomparison of backscatter pofiles from the three laser sensors and (ii) on the comparison of the backscatter profiles with twenty-three radiosoundings performed during the period of 8 to 15 June 2009. The Temporal Height-Tracking (THT) algorithm was applied to the three sensors’ backscatter profiles to retrieve the decoupled structure of the BL over Mace Head. The results of the intercomparisons are expressed in terms of the mean correlation coefficients, mean bias (difference between two sensors’ detections), mean sigma (the standard deviation of the bias) and the consistency, i.e. the percentage of cases where the detections of the intercompared sensors were closer than 200 m.  The ALS300-CHM15K comparison provided the most consistent retrievals amongst the three comparisons with, respectively, the 86.5% and 77.2% of the lower and upper layer detections closer than 200m and with correlation coefficients equal to 0.88 and 0.83 at the lower and upper layer, respectively. The lidar and ceilometers-detected BL heights were then compared to the temperature profiles retrieved by radiosoundings. The most consistent retrievals at the lower layer are from the ALS300 with the 75% of  detections closer than 200m to the radiosoundings’ first temperature inversion. Despite the lower signal-to-noise ratio and R-value compared to the ASL300 and CHM15K, the CL31 is more consistent with  the soundings retrievals at the upper layer with 62.5% of detections closer than 200m to the radiosoundings’ econd temperature inversion. The ALS300 has larger pulse-averaged power compared to the two ceilometers and better ability in detecting fine aerosol layers within the BL. The comparison of remote and in-situ data proved both the veracity of the inherent link between temperature and aerosol backscatter profiles, and the existence of possible limitations in using aerosols as a tracer to detect the BL structure. 

Ground-based Retrieval of Continental and Marine Warm Cloud Microphysics Ground-based Retrieval of Continental and Marine Warm Cloud Microphysics

Date added: 08/05/2011
Date modified: 08/05/2011
Filesize: 3.85 MB

Martucci, G. and C.D. O’Dowd, Ground-based Retrieval of Continental and Marine Warm Cloud Microphysics. Atmos, Meas. Techs.. Diss., 4, 4825-4865, doi:10.5194/amtd-4-4825-2011,, 2011


Abstract. A technique for retrieving warm cloud microphysics using synergistic ground based remote sensing instruments is presented. The SYRSOC (SYnergistic Remote Sensing Of Cloud) technique utilises a Ka-band Doppler cloud RADAR, a LIDAR-ceilometer and a multichannel microwave radiometer. SYRSOC retrieves the main microphysical parameters such as cloud droplet number concentration (CDNC), droplets effective radius (reff), cloud liquid water content (LWC), and the departure from adiabatic conditions within the cloud. Two retrievals are presented for continental and marine stratocumulus formed over the Mace Head Atmospheric Research Station. Whilst the continental case exhibited high CDCN (N = 382 cm−3; 10th-to-90th percentile [9.4–842.4] cm−3) and small mean effective radius (reff = 4.3; 10th-to-90th percentile [2.9–6.5] μm), the marine case exhibited low CDNC and large mean effective radius (N = 25 cm−3, 10th-to-90th percentile [1.5–69] cm−3; reff = 25.6 μm, 10th-to-90th percentile [11.2–42.7] μm) as expected since the continental air at this location is typically more polluted than marine air. The large reff of the marine case was determined by the contribution of drizzle drops (large radii and few occurrences) and in fact the modal radius was reffMOD = 12 μm (smaller radius and large occurrences). The mean LWC was comparable for the two cases (continental: 0.19 g m−3; marine: 0.16 g m–3) but the 10th–90th percentile range was wider in marine air (continental: 0.11–0.22 g m−3; marine: 0.01–0.38 g m−3). The calculated algorithm uncertainty for the continental and marine case for each variable was, respectively, σN=141.34 cm−3 and 11.5 cm−3, σreff=0.8 μm and 3.2 μm, σLWC = 0.03 g m−3 and 0.03 g m−3. The retrieved CDNC are compared to the cloud condensation nuclei concentrations and the best agreement is achieved for a super-saturation of 0.1 % in the continental case and between 0.1 %–0.75 % for the marine stratocumulus. The retrieved reff at the top of the clouds are compared to the MODIS satellite reff: 7 μm (MODIS) vs 6.2 μm (SYRSOC) and 16.3 μm (MODIS) vs. 17 μm (SYRSOC) for continental and marine cases, respectively. The combined analysis of the CDNC and the reff, for the marine case shows that the drizzle modifies the droplet size distribution and reff especially if compared to reffMOD. The study of the cloud subadiabaticity and the LWC shows the general sub-adiabatic character of both clouds with more pronounced departure from adiabatic conditions in the continental case due to the shallower cloud depth and more significant mixing with dry tropospheric air.

Modeled Optical Thickness of the Sea Salt Aerosol Over the World Ocean Modeled Optical Thickness of the Sea Salt Aerosol Over the World Ocean

Date added: 08/04/2011
Date modified: 08/05/2011
Filesize: 1.17 MB

Madry, L.M., O.B. Toon, C. D. O’Dowd, Modeled Optical Thickness of the Sea Salt Aerosol Over the World Ocean, J. Geophys. Res. doi:10.1029/2010JD014691, 2011.


We simulate the generation and microphysical evolution of seas

alt aerosol using a climatologically driven 3D microphysical model for the year 2006. We then apply Mie theory to calculate the extinction and scattering efficiencies of our transported, sizeresolved seasalt aerosol, accounting for hygroscopic growth due to changes in ambient relative humidity. We calculate the column optical thickness of our modeled seasalt aerosol for comparison to three previously published wind speeddependent clean  marine air optical thickness formulations. Variously derived from optical thickness measurements and retrievals taken from the Midway Island AERONET site, the satellitebased MODIS instruments, and the Global Atmospheric Watch (GAW) site at Mace Head, Ireland, the three formulations report similar background levels of clean marine AOT at zero wind speed but significantly different functional dependencies for nonzero wind speeds. We find that our modeled seasalt aerosol optical thickness very closely depends on the square of surface wind speed under steady state conditions. This relationship is consistent across all latitudes. However, due to the fact that steady state winds are seldom maintained, the 24 h mean wind is more frequently applicable to calculations of seasalt AOT, with only slightly diminished accuracy.

General Overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions General Overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions

Date added: 08/04/2011
Date modified: 08/04/2011
Filesize: 4.81 MB

M. Kulmala, A. Asmi, H.K. Lappalainen, U. Baltensperger, J.-L. Brenguier, , M. C. Facchini, H.-C. Hansson, Ø. Hov, C. O'Dowd, U. Poeschl, A. Wiedensohler,  R. Boers ,  O. Boucher,  G. De Leeuw, J. Feichter, R. Krejci ,  P. Laj, H. Lihavainen,  U. Lohmann, G. McFiggans, T. Mentel, C. Pilinis ,I.  Riipinen, M. Schultz, A. Stohl, E. Swietlicki, H. Denier Van den Gon , E. Vignati,  M. Amann,  C.Alves,  S. Arabas,  P. Artaxo, D.C.S. Beddows,  P. Beukes, R. Bergström,  M. Bilde, S. Clegg,  H. Coe,  B. d'Anna,  S. Gilardoni, J. Debernard, S.  Decesari,  M. Fischer,  A.M. Fjæraa, C. George, P. Halloran, T. Hamburger, R.M. Harrison, H. Herrman, T. Hoffmann,  C. Hoose, M Hu, U. Hõrrak, Y. Iinuma, T. Iversen,  M. Josipovic,  M. Junying, M. Kanakidou, A.Kiendler-Scharr,  A. Kirkevåg, G. Kiss,  Z. Klimont,    P. Kolmonen,  JE. Kristjansson, L. Laakso, A. Laaksonen, L. Labonnote, K.E.J. Lehtinen, R. Makkonen, G. McMeeking, J. Merikanto, A.Minikin, S.Mirme, W.T. Morgan, D. O’Donnell, TS. Panwar, H. Pawlowska, A Petzold, JJ. Pienaar, C. Pio,  C. Plass-Duelmer, A.S.H. Prévôt, S. Pryor, D. Rosenfeld, J. Schwarz, Ø. Seland, X.J. Shen, B. Sierau, D. Simpson,  J.Y.  Sun, D. Topping, P. Tunved, P. Vaattovaara, V. Vakkari, P. van Zyl, J.P. Veefkind,  B. Wehner, J. Wildt,  G. Visschedijk, S. Woodward, H. Vuollekoski, A. Zardini, K. Zhang, V.-M. Kerminen , K. Carslaw and S. N. Pandis. General Overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) - integrating aerosol research from nano to global scales, Atmos. Chem. & Phys. Disc., 11, 1–176, doi:10.5194/acpd-11-1-2011, 2011.

 


 

Abstract

In this paper we describe and summarize the main achievements of the European  Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI  started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy

including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) the first comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their ef10 fects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several  new aerosol parameterizations and computations modules for chemical transport and global climate models were  veloped and evaluated. This work enabled EUCAARI to improve our understanding of aerosol radiative forcing  15 and air quality-climate interactions. The EUCAARI results can be utilized in European  and global environmental policy to assess the erosol impacts and the corresponding  abatement strategies.

Number size distributions and seasonality of submicron particles in Europe 2008–2009 Number size distributions and seasonality of submicron particles in Europe 2008–2009

Date added: 08/04/2011
Date modified: 08/05/2011
Filesize: 11.95 MB

Asmi, A.,  A. Wiedensohler, P. Laj, A.-M. Fjaeraa, K. Sellegri, W. Birmili, E. Weingartner, U. Baltensperger, V. Zdimal, N. Zikova, J.-P. Putaud, A. Marinoni, P. Tunved, H.-C. Hansson, M. Fiebig, N. Kivekäs, H. Lihavainen, E. Asmi, V. Ulevicius, P. P. Aalto, E. Swietlicki, A. Kristensson, N. Mihalopoulos, N. Kalivitis, I. Kalapov, G. Kiss, G. de Leeuw, B. Henzing, R. M. Harrison, D. Beddows, C. O'Dowd, S. G. Jennings, H. Flentje, K. Weinhold, F. Meinhardt, L. Ries, and M. Kulmala.

Number size distributions and seasonality of submicron particles in Europe 2008–2009, Atmos. Phys. Chem. 11, 5505-5538, doi:10.5194/acp-11-5505, 2011

 


 

  

Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of  Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000ma.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, andvery low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional coverage of these results. Aerosol number concentrations over the Britain and Ireland had very high varianceand there are indications of mixed air masses from several source regions; the Mediterranean aerosol exhibit high seasonality, and a strong accumulation mode in the summer. The greatest concentrations were observed at the Ispra station in Northern Italy with high accumulation mode number concentrations n the winter. The aerosol number concentrations at the Arctic station Zeppelin in Ny-A° lesund in Svalbard have also a strong seasonal cycle, with greater concentrations of accumulation mode particles in winter, and dominating summer Aitken mode indicating more recently formed particles. Observed particles did not show any statistically significant regional work-week or weekday related variation in number concentrations studied.Analysis products are made for open-access to the research

 

 

community, available in a freely accessible internet site. The

results give to the modelling community a reliable, easy-touse

and freely available comparison dataset of aerosol size

distributions.

Decreasing trends in total gaseous mercury observations in baseline air at Mace Head, Ireland from 1 Decreasing trends in total gaseous mercury observations in baseline air at Mace Head, Ireland from 1

Date added: 05/25/2011
Date modified: 05/25/2011
Filesize: 649.24 kB

R. Ebinghaus, S.G. Jennings, H.H. Kock , R.G. Derwent , A.J. Manning , and T.G. Spain,  Decreasing trends in total gaseous mercury observations in baseline air at Mace

Head, Ireland from 1996 to 2009, Atmos. Environ., doi:10.1016/j.atmosenv.2011.01.033


In this study, the concentrations of total gaseous mercury in baseline air masses arriving at Mace Head, Ireland after having traversed the thousands of kilometres uninterrupted fetch of the North Atlantic Ocean, have been used for the assessment of possible trends in the atmospheric mercury background concentration over a 14-year period (i.e., 1996 -2009), a statistically significant negative (downwards) trend of -0.028 ±0.01 ng m-3 yr-1, representing a trend of 1.6 - 2.0% per year, has been detected in the total gaseous mercury levels in these baseline air masses. These findings are set in the context of the available literature studies of atmospheric Hg trends.

Effect of Horizontal Resolution on Meteorology and Air-Quality Prediction with a Regional Scale Mode Effect of Horizontal Resolution on Meteorology and Air-Quality Prediction with a Regional Scale Mode

Date added: 05/12/2011
Date modified: 05/12/2011
Filesize: 4.49 MB

Varghese, S., B. Langmann and C. D. O’Dowd, Effect of Horizontal Resolution on Meteorology and Air-Quality Prediction with a Regional Scale Model, Atmos. Res., doi:10.1016/j.atmosres.2011.02.007, 2011

 


 

Horizontal resolution sensitivity can significantly contribute to the uncertainty in predictions of meteorology and air-quality from a regional climate model. In the study presented here, astate-of-the-art regional scale atmospheric climate-chemistry-aerosol model REMOTE is used to understand the influence of spatial model resolutions of 1.0°, 0.5° and 0.25° on predicted meteorological and aerosol parameters for June 2003 for the European domain comprising North-east Atlantic and Western Europe. Model precipitation appears to improve with resolution while wind speed has shown best results for 0.25° resolution for most of the stations compared with ECAD data. Low root mean square error and spatial bias for surface pressure, precipitation and surface temperature show that the model is very reliable. Spatial and temporal variation in black carbon, primary organic carbon, sea-salt and sulphate concentrations and their burden are presented. In most cases, chemical species concentrations at the surface show no particular trend or improvement with increase in resolution. There has been a pronounced influence of horizontal resolution on the vertical distribution pattern of some aerosol species. Some of these effects are due to the improvement in topographical details, flow characteristics and associated vertical and horizontal dynamic processes. The different sink processes have contributed very differently to the various aerosol pecies in terms of deposition (wet and dry) and sedimentation which are strongly linked to the meteorological processes. Overall, considering the formance of meteorological parameters and chemical  pecies concentrations, a horizontal model resolution of 0.5° is suggested to achieve easonable results within the limitations of this model.

Production Flux of Sea-Spray Aerosol. Rev. of Geophys., Production Flux of Sea-Spray Aerosol. Rev. of Geophys.,

Date added: 05/12/2011
Date modified: 05/12/2011
Filesize: 2.68 MB

de Leeuw, G., E. Andreas, M. Anguelova , C. Fairall , E. Lewis , C. O'Dowd , M. Schulz , S. Schwartz , Production Flux of Sea-Spray Aerosol. Rev. of Geophys., doi:10.1029/2010RG000349, 2011


 

Knowledge of the sizeand compositiondependent production flux of primary sea spray aerosol (SSA) particles and its dependence on environmental variables is required for modeling cloud microphysical properties and aerosol radiative influences, interpreting measurements of particulate matter in coastal areas and its relation to air quality, and evaluating rates of uptake and reactions of gases in sea spray drops. This review examines recent research pertinent to SSA production flux, which deals mainly with production of particles with r80 (equilibrium radius at 80% relative humidity) less than 1 mm and as small as 0.01 mm. Production of sea spray particles and its dependence on controlling factors has been investigated in aboratory studies that have examined the dependences on water temperature, salinity, and the presence of organics and in field measurements with micrometeorological techniques that use newly developed fast optical particle sizers. Extensive measurements show that waterinsoluble organic matter contributes substantially to the omposition of SSA particles with r80 < 0.25 mm and, in locations with high biological activity, can be the ominant constituent. Orderofmagnitude variation  remains in estimates of the sizedependent production flux per white area, the quantity central to formulations of the production flux based on the whitecap method. This variation indicates that the production flux may depend on quantities such as the volume flux of air bubbles to the surfacet hat are not accounted for in current models. Variation in estimates of the whitecap fraction as a function of wind speed contributes additional, comparable uncertainty to production flux estimates.  

Characterization and intercomparison of aerosol absorption photometers: result of two intercompariso Characterization and intercomparison of aerosol absorption photometers: result of two intercompariso

Date added: 02/16/2011
Date modified: 02/16/2011
Filesize: 3.86 MB

Müller, T., Henzing, J. S., de Leeuw, G., Wiedensohler, A., Alastuey, A., Angelov, H., Bizjak, M., Collaud Coen, M., Engström, J. E., Gruening, C., Hillamo, R., Hoffer, A., Imre, K., Ivanow, P., Jennings, G., Sun, J. Y., Kalivitis, N., Karlsson, H., Komppula, M., Laj, P., Li, S.-M., Lunder, C., Marinoni, A., Martins dos Santos, S., Moerman, M., Nowak, A., Ogren, J. A., Petzold, A., Pichon, J. M., Rodriquez, S., Sharma, S., Sheridan, P. J., Teinilä, K., Tuch, T., Viana, M., Virkkula, A., Weingartner, E., Wilhelm, R., and Wang, Y. Q.: Characterization and intercomparison of aerosol absorption photometers: result of two intercomparison workshops, Atmos. Meas. Tech., 4, 245-268, doi:10.5194/amt-4-245-2011, 2011.


Absorption photometers for real time application have been available since the 1980s, but the use of filter-based instruments to derive information on aerosol properties (absorption coefficient and black carbon, BC) is still a matter of debate. Several workshops have been conducted to investigate the performance of individual instruments over the intervening years. Two workshops with large sets of aerosol absorption photometers were conducted in 2005 and 2007. The data from these instruments were corrected using existing methods before further analysis. The inter-comparison shows a large variation between the responses to absorbing aerosol particles for different types of instruments. The unit to unit variability between instruments can be up to 30% for Particle Soot Absorption Photometers (PSAPs) and Aethalometers. Multi Angle Absorption Photometers (MAAPs) showed a variability of less than 5%. Reasons for the high variability were identified to be variations in sample flow and spot size. It was observed that different flow rates influence system performance with respect to response to absorption and instrumental noise. Measurements with non absorbing particles showed that the current corrections of a cross sensitivity to particle scattering are not sufficient. Remaining cross sensitivities were found to be a function of the total particle load on the filter. The large variation between the response to absorbing aerosol particles for different types of instruments indicates that current correction functions for absorption photometers are not adequate.


Opendda: a Novel High-Performance Computational Framework for the Discrete Dipole Approximation Opendda: a Novel High-Performance Computational Framework for the Discrete Dipole Approximation

Date added: 02/15/2011
Date modified: 02/15/2011
Filesize: 1.26 MB

James Mc Donald, Aaron Golden, and S. Gerard Jennings

Opendda: a Novel High-Performance Computational Framework for the Discrete Dipole Approximation.  International Journal of High Performance Computing Applications, February 2009 23: 42-61, doi:10.1177/1094342008097914, 2009

This work presents a highly optimized computational framework for the Discrete Dipole Approximation, a numerical method for calculating the optical properties associated with a target of arbitrary geometry that is widely used in atmospheric, astrophysical and industrial simulations. Core optimizations include the bit-fielding of integer data and iterative methods that complement a new Discrete Fourier Transform (DFT) kernel, which efficiently calculates the matrix— vector products required by these iterative solution schemes. The new kernel performs the requisite 3-D DFTs as ensembles of 1-D transforms, and by doing so, is able to reduce the number of constituent 1-D transforms by 60% and the memory by over 80%. The optimizations also facilitate the use of parallel techniques to further enhance the performance. Complete OpenMP-based shared-memory and MPI-based distributed-memory implementations have been created to take full advantage of the various architectures. Several benchmarks of the new framework indicate extremely favorable performance and scalability.

 

 

 


Particle mobility size spectrometers: harmonization of technical standards and data structure to fac Particle mobility size spectrometers: harmonization of technical standards and data structure to fac

Date added: 02/15/2011
Date modified: 02/15/2011
Filesize: 2.08 MB

Wiedensohler, A., Birmili, W., Nowak, A., Sonntag, A., Weinhold, K., Merkel, M., Wehner, B., Tuch, T., Pfeifer, S., Fiebig, M., Fjäraa, A. M., Asmi, E., Sellegri, K., Depuy, R., Venzac, H., Villani, P., Laj, P., Aalto, P., Ogren, J. A., Swietlicki, E., Roldin, P., Williams, P., Quincey, P., Hüglin, C., Fierz-Schmidhauser, R., Gysel, M., Weingartner, E., Riccobono, F., Santos, S., Grüning, C., Faloon, K., Beddows, D., Harrison, R. M., Monahan, C., Jennings, S. G., O'Dowd, C. D., Marinoni, A., Horn, H.-G., Keck, L., Jiang, J., Scheckman, J., McMurry, P. H., Deng, Z., Zhao, C. S., Moerman, M., Henzing, B., and de Leeuw, G.: Particle mobility size spectrometers: harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions, Atmos. Meas. Tech. Discuss., 3, 5521-5587, doi:10.5194/amtd-3-5521-2010, 2010.


Particle mobility size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide application in atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards with respect to the instrumental set-up, measurement mode, data evaluation as well as quality control. This article results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research). Under controlled laboratory conditions, the number size distribution from 20 to 200 nm determined by mobility size spectrometers of different design are within an uncertainty range of ±10% after correcting internal particle losses, while below and above this size range the discrepancies increased. Instruments with identical design agreed within ±3% in the peak number concentration when all settings were done carefully. Technical standards were developed for a minimum requirement of mobility size spectrometry for atmospheric aerosol measurements. Technical recommendations are given for atmospheric measurements including continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyser. In cooperation with EMEP (European Monitoring and Evaluation Program), a new uniform data structure was introduced for saving and disseminating the data within EMEP. This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data.


 


 

Light scattering enhancement factors in the marine boundary layer (Mace Head, Ireland) Light scattering enhancement factors in the marine boundary layer (Mace Head, Ireland)

Date added: 02/15/2011
Date modified: 02/15/2011
Filesize: 1.01 MB

Fierz-Schmidhauser, R., P. Zieger, A. Vaishya, C. Monahan, J. Bialek, C. D. O'Dowd, S. G. Jennings, U. Baltensperger, and E. Weingartner (2010), Light scattering enhancement factors in the marine boundary layer (Mace Head, Ireland), J. Geophys. Res., 115, D20204, doi:10.1029/2009JD013755.


Direct climate aerosol radiative forcing is influenced by the light scattering of atmospheric aerosols. The chemical composition, the size distribution, and the ambient relative humidity (RH) determine the amount of visible light scattered by aerosols. We measured the aerosol light scattering coefficients at RH varying from 30% to 90% of the marine atmosphere at the Mace Head Atmospheric Research Station on the west coast of Ireland. At this site, two major air mass types can be distinguished: clean marine and polluted air. In this paper, we present measurements of light scattering enhancement factors f(RH) = σsp(RH)/σsp(dry) from a 1 month field campaign (January–February 2009). At this site in winter, the mean f(RH = 85%) (standard deviation) for marine air masses at the wavelength of 550 nm was 2.22 (±0.17) and 1.77 (±0.31) for polluted air. Measured σsp(RH) and f(RH) agreed well with calculations from Mie theory using measurements of the size distribution and hygroscopic diameter growth factors as input. In addition, we investigated the RH influence on additional intensive optical properties: the backscatter fraction and the single scattering albedo. The backscatter fraction decreased by about 20%, and the single scattering albedo increased on average by 1%–5% at 85% RH compared to dry conditions.

Minimizing light absorption measurement artifacts of the Minimizing light absorption measurement artifacts of the

Date added: 02/15/2011
Date modified: 02/15/2011
Filesize: 2.71 MB

Collaud Coen, M., E. Weingartner, A. Apituley, D. Ceburnis, R. Fierz-Schmidhauser, H, Flentje, J.S. Henzing,  S.G. Jennings, M. Moerman, A. Petzold, O. Schmid, and U. Baltensperger. Minimizing light absorption measurement artifacts of the Aethalometer: evaluation of five correction algorithms: the EUSAAR protocol. Atmos. Meas.Technol., 3, 457-474, 2010.


The aerosol light absorption coefficient is an essential parameter involved in atmospheric radiation budget

calculations. The Aethalometer (AE) has the great advantage of measuring the aerosol light absorption coefficient at several wavelengths, but the derived absorption coefficients are systematically too high when compared to reference methods. Up to now, four different correction algorithms of the AE absorption coefficients have been proposed by several authors. A new correction scheme based on these previously published methods has been developed, which accounts for the optical properties of the aerosol particles embedded in the filter. All the corrections have been tested on six datasets representing different aerosol types and loadings and include multi-wavelength AE and white-light AE. All the corrections have also been evaluated through comparison with a Multi-Angle Absorption Photometer (MAAP) for four datasets lasting between 6 months and five years. The modification of the wavelength dependence by the different corrections is analyzed in detail. The performances and the limits of all AE corrections are determined and recommendations are given.


 

 

 

 

 

, Detection of Cloud Base Height Using Jenoptik CHM15K and Vaisala CL31 Ceilometers , Detection of Cloud Base Height Using Jenoptik CHM15K and Vaisala CL31 Ceilometers

Date added: 02/08/2011
Date modified: 02/08/2011
Filesize: 8.25 MB

Martucci, G., C. Milroy, and C.D. O’Dowd, Detection of Cloud Base Height Using Jenoptik CHM15K and Vaisala CL31 Ceilometers, J. Atmos. Oceanic Techol. Vol. 27, No. 2, 305–318, 2010.


Abstract Twelve case studies of multi-layer cloud base height (CBH) retrievals from two co-located ceilometers (Vaisala CL31 and Jenoptik CHM15K) have been analysed. The studies were performed during the period from September to December 2008 at the Mace Head Research Station, Ireland. During the period of measurement, the two instruments provided vertical profiles of backscattered laser signal as well as the manufacturer’s operational cloud-base product. The cases selected covered a diverse range of cloud-cover conditions ranging from single to multiple cloud layers and from cloud base heights varying from only a few hundreds metres per day up to 3-5 km in few hours. The results show significant offsets between the two manufacturer-derived CBHs along with a considerable degree of scatter. Using a newly developed Temporal Height-Tracking (THT) algorithm applied to both ceilometers, significant improvement in the correlation between CBH derived from both instruments results in a correlation coefficient increasing to R2 = 0.997 (with a slope of 0.998) from R2 = 0.788 (with associated slope of 0.925). Also, the regression intercept (offset) is reduced from 160 m to effectively zero (-3 m). For the worst individual case study, using the THT algorithm resulted in the correlation coefficient improving from R2 = 0.52, using the manufacturer’s output, to R2 = 0.97 with a reduction in the offset reducing from 569 m to 32 m. Applying the THT algorithm to the backscatter profiles of both instruments led to retrieved cloud bases which are statistically consistent with each other and ensured reliable detection of CBH, particularly when inhomogeneous cloud fields were present and changing rapidly in time. The THT algorithm also overcomes multiple false cloud base detections, associated with the two instruments manufacturer’s output.

 

Statistical Analysis of Eight Surface Ozone Measurement Series for various sites in Ireland, Statistical Analysis of Eight Surface Ozone Measurement Series for various sites in Ireland,

Date added: 02/08/2011
Date modified: 02/08/2011
Filesize: 1.81 MB

Tripathi, O. P., Jennings S. G., O’Dowd, C. D., Coleman, L., Leinert, S., O’Leary, B., Moran, E., O’Doherty, S. J., and Spain, T. G., Statistical Analysis of Eight Surface Ozone Measurement Series for various sites in Ireland, J. Geophys. Res., 115, D19302, doi:10.1029/2010JD014040., 2010


Abstract: Data from various stations having different measurement record periods between 1988 and 2007 are analyzed to investigate the surface ozone concentration, long‐term trends, and seasonal changes in and around Ireland. Time series statistical analysis is performed on the monthly mean data using seasonal and trend decomposition procedures and the Box‐Jenkins approach (autoregressive integrated moving average). In general, ozone concentrations in the Irish region are found to have a negative trend at all sites except at the coastal sites of Mace Head and Valentia. Data from the most polluted Dublin city site have shown a very strong negative trend of −0.33 ppb/yr with a 95% confidence limit of 0.17 pp/yr (i.e., −0.33 ± 0.17) for the period 2002−2007, and for the site near the city of Cork, the trend is found to be −0.20 ± 0.11 ppb/yr over the same period. The negative trend for other sites is more pronounced when the data span is considered from around the year 2000 to 2007. Rural sites of Wexford and Monaghan have also shown a very strong negative trend of −0.99 ± 0.13 and −0.58 ± 0.12, respectively, for the period 2000−2007. Mace Head, a site that is representative of ozone changes in the air advected from the Atlantic to Europe in the marine planetary boundary layer, has shown a positive trend of about +0.16 ± 0.04 ppb per annum over the entire period 1988−2007, but this positive trend has reduced during recent years (e.g., in the period 2001−2007). Cluster analysis for back trajectories are performed for the stations having a long record of data, Mace Head and Lough Navar. For Mace Head, the northern and western clean air sectors have shown a similar positive trend (+0.17 ± 0.02 ppb/yr for the northern sector and +0.18 ± 0.02 ppb/yr for the western sector) for the whole period, but partial analysis for the clean western sector at Mace Head shows different trends during different time periods with a decrease in the positive trend since 1988 indicating a deceleration in the ozone trend for Atlantic air masses entering Europe.

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