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- ItemReactive Halogens in the Marine Boundary Layer (RHaMBLe): The tropical North Atlantic experiments(München : European Geopyhsical Union, 2010) Lee, J.D.; McFiggans, G.; Allan, J.D.; Baker, A.R.; Ball, S.M.; Benton, A.K.; Carpenter, L.J.; Commane, R.; Finley, B.D.; Evans, M.; Fuentes, E.; Furneaux, K.; Goddard, A.; Good, N.; Hamilton, J.F.; Heard, D.E.; Herrmann, H.; Hollingsworth, A.; Hopkins, J.R.; Ingham, T.; Irwin, M.; Jones, C.E.; Jones, R.L.; Keene, W.C.; Lawler, M.J.; Lehmann, S.; Lewis, A.C.; Long, M.S.; Mahajan, A.; Methven, J.; Moller, S.J.; Müller, K.; Müller, T.; Niedermeier, N.; O'Doherty, S.; Oetjen, H.; Plane, J.M.C.; Pszenny, A.A.P.; Read, K.A.; Saiz-Lopez, A.; Saltzman, E.S.; Sander, R.; von Glasow, R.; Whalley, L.; Wiedensohler, A.; Young, D.The NERC UK SOLAS-funded Reactive Halogens in the Marine Boundary Layer (RHaMBLe) programme comprised three field experiments. This manuscript presents an overview of the measurements made within the two simultaneous remote experiments conducted in the tropical North Atlantic in May and June 2007. Measurements were made from two mobile and one ground-based platforms. The heavily instrumented cruise D319 on the RRS Discovery from Lisbon, Portugal to São Vicente, Cape Verde and back to Falmouth, UK was used to characterise the spatial distribution of boundary layer components likely to play a role in reactive halogen chemistry. Measurements onboard the ARSF Dornier aircraft were used to allow the observations to be interpreted in the context of their vertical distribution and to confirm the interpretation of atmospheric structure in the vicinity of the Cape Verde islands. Long-term ground-based measurements at the Cape Verde Atmospheric Observatory (CVAO) on São Vicente were supplemented by long-term measurements of reactive halogen species and characterisation of additional trace gas and aerosol species during the intensive experimental period. This paper presents a summary of the measurements made within the RHaMBLe remote experiments and discusses them in their meteorological and chemical context as determined from these three platforms and from additional meteorological analyses. Air always arrived at the CVAO from the North East with a range of air mass origins (European, Atlantic and North American continental). Trace gases were present at stable and fairly low concentrations with the exception of a slight increase in some anthropogenic components in air of North American origin, though NOx mixing ratios during this period remained below 20 pptv (note the non-IUPAC adoption in this manuscript of pptv and ppbv, equivalent to pmol mol−1 and nmol mol−1 to reflect common practice). Consistency with these air mass classifications is observed in the time series of soluble gas and aerosol composition measurements, with additional identification of periods of slightly elevated dust concentrations consistent with the trajectories passing over the African continent. The CVAO is shown to be broadly representative of the wider North Atlantic marine boundary layer; measurements of NO, O3 and black carbon from the ship are consistent with a clean Northern Hemisphere marine background. Aerosol composition measurements do not indicate elevated organic material associated with clean marine air. Closer to the African coast, black carbon and NO levels start to increase, indicating greater anthropogenic influence. Lower ozone in this region is possibly associated with the increased levels of measured halocarbons, associated with the nutrient rich waters of the Mauritanian upwelling. Bromide and chloride deficits in coarse mode aerosol at both the CVAO and on D319 and the continuous abundance of inorganic gaseous halogen species at CVAO indicate significant reactive cycling of halogens. Aircraft measurements of O3 and CO show that surface measurements are representative of the entire boundary layer in the vicinity both in diurnal variability and absolute levels. Above the inversion layer similar diurnal behaviour in O3 and CO is observed at lower mixing ratios in the air that had originated from south of Cape Verde, possibly from within the ITCZ. ECMWF calculations on two days indicate very different boundary layer depths and aircraft flights over the ship replicate this, giving confidence in the calculated boundary layer depth.
- ItemSources and mixing state of size-resolved elemental carbon particles in a European megacity: Paris(München : European Geopyhsical Union, 2012) Healy, R.M.; Sciare, J.; Poulain, L.; Kamili, K.; Merkel, M.; Müller, T.; Wiedensohler, A.; Eckhardt, S.; Stohl, A.; Sarda-Estève, R.; McGillicuddy, E.; O'Connor, I.P.; Sodeau, J.R.; Wenger, J.C.An Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed to investigate the size-resolved chemical composition of single particles at an urban background site in Paris, France, as part of the MEGAPOLI winter campaign in January/February 2010. ATOFMS particle counts were scaled to match coincident Twin Differential Mobility Particle Sizer (TDMPS) data in order to generate hourly size-resolved mass concentrations for the single particle classes observed. The total scaled ATOFMS particle mass concentration in the size range 150–1067 nm was found to agree very well with the sum of concurrent High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and Multi-Angle Absorption Photometer (MAAP) mass concentration measurements of organic carbon (OC), inorganic ions and black carbon (BC) (R2 = 0.91). Clustering analysis of the ATOFMS single particle mass spectra allowed the separation of elemental carbon (EC) particles into four classes: (i) EC attributed to biomass burning (ECbiomass), (ii) EC attributed to traffic (ECtraffic), (iii) EC internally mixed with OC and ammonium sulfate (ECOCSOx), and (iv) EC internally mixed with OC and ammonium nitrate (ECOCNOx). Average hourly mass concentrations for EC-containing particles detected by the ATOFMS were found to agree reasonably well with semi-continuous quantitative thermal/optical EC and optical BC measurements (r2 = 0.61 and 0.65–0.68 respectively, n = 552). The EC particle mass assigned to fossil fuel and biomass burning sources also agreed reasonably well with BC mass fractions assigned to the same sources using seven-wavelength aethalometer data (r2 = 0.60 and 0.48, respectively, n = 568). Agreement between the ATOFMS and other instrumentation improved noticeably when a period influenced by significantly aged, internally mixed EC particles was removed from the intercomparison. 88% and 12% of EC particle mass was apportioned to fossil fuel and biomass burning respectively using the ATOFMS data compared with 85% and 15% respectively for BC estimated from the aethalometer model. On average, the mass size distribution for EC particles is bimodal; the smaller mode is attributed to locally emitted, mostly externally mixed EC particles, while the larger mode is dominated by aged, internally mixed ECOCNOx particles associated with continental transport events. Periods of continental influence were identified using the Lagrangian Particle Dispersion Model (LPDM) "FLEXPART". A consistent minimum between the two EC mass size modes was observed at approximately 400 nm for the measurement period. EC particles below this size are attributed to local emissions using chemical mixing state information and contribute 79% of the scaled ATOFMS EC particle mass, while particles above this size are attributed to continental transport events and contribute 21% of the EC particle mass. These results clearly demonstrate the potential benefit of monitoring size-resolved mass concentrations for the separation of local and continental EC emissions. Knowledge of the relative input of these emissions is essential for assessing the effectiveness of local abatement strategies.
- ItemThe "dual-spot" Aethalometer: An improved measurement of aerosol black carbon with real-time loading compensation(München : European Geopyhsical Union, 2015) Drinovec, L.; Močnik, G.; Zotter, P.; Prévôt, A.S.H.; Ruckstuhl, C.; Coz, E.; Rupakheti, M.; Sciare, J.; Müller, T.; Wiedensohler, A.; Hansen, A.D.A.Aerosol black carbon is a unique primary tracer for combustion emissions. It affects the optical properties of the atmosphere and is recognized as the second most important anthropogenic forcing agent for climate change. It is the primary tracer for adverse health effects caused by air pollution. For the accurate determination of mass equivalent black carbon concentrations in the air and for source apportionment of the concentrations, optical measurements by filter-based absorption photometers must take into account the "filter loading effect". We present a new real-time loading effect compensation algorithm based on a two parallel spot measurement of optical absorption. This algorithm has been incorporated into the new Aethalometer model AE33. Intercomparison studies show excellent reproducibility of the AE33 measurements and very good agreement with post-processed data obtained using earlier Aethalometer models and other filter-based absorption photometers. The real-time loading effect compensation algorithm provides the high-quality data necessary for real-time source apportionment and for determination of the temporal variation of the compensation parameter k.
- ItemMethodology for high-quality mobile measurement with focus on black carbon and particle mass concentrations(Göttingen : Copernicus GmbH, 2019) Alas, H.D.C.; Weinhold, K.; Costabile, F.; Di Ianni, A.; Müller, T.; Pfeifer, S.; Di Liberto, L.; Turner, J.R.; Wiedensohler, A.Measurements of air pollutants such as black carbon (BC) and particle mass concentration in general, using mobile platforms equipped with high-time-resolution instruments, have gained popularity over the last decade due to their wide range of applicability. Assuring the quality of mobile measurement, data have become more essential, particularly when the personal exposure to pollutants is related to their spatial distribution. In the following, we suggest a methodology to achieve data from mobile measurements of equivalent black carbon (eBC) and PM2:5 mass concentrations with high data quality. Besides frequent routine quality assurance measures of the instruments, the methodology includes the following steps: (a) measures to ensure the quality of mobile instruments through repeated collocated measurements using identical instrumentation, (b) inclusion of a fixed station along the route containing quality-assured reference instruments, and (c) sufficiently long and frequent intercomparisons between the mobile and reference instruments to correct the particle number and mass size distributions obtained from mobile measurements. The application of the methodology can provide the following results. First, collocated mobile measurements with sets of identical instruments allow identification of undetected malfunctions of the instruments. Second, frequent intercomparisons against the reference instruments will ensure the quality of the mobile measurement data of the eBC mass concentration. Third, the intercomparison data between the mobile optical particle size spectrometer (OPSS) and a reference mobility particle size spectrometer (MPSS) allow for the adjustment of the OPSS particle number size distribution using physically meaningful corrections. Matching the OPSS and MPSS volume particle size distributions is crucial for the determination of PM2:5 mass concentration. Using size-resolved complex refractive indices and time-resolved fine-mode volume correction factors of the fine-particle range, the calculated PM2:5 from the OPSS was within 5 % of the reference instruments (MPSSCAPSS). However, due to the nonsphericity and an unknown imaginary part of the complex refractive index of supermicrometer particles, a conversion to a volume equivalent diameter yields high uncertainties of the particle mass concentration greater than PM2:5. The proposed methodology addresses issues regarding the quality of mobile measurements, especially for health impact studies, validation of modeled spatial distribution, and development of air pollution mitigation strategies.
- ItemCharacterization and intercomparison of aerosol absorption photometers: Result of two intercomparison workshops(München : European Geopyhsical Union, 2011) 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.; Wang, Y.Q.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.