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    Reactive 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.
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    Evaluating stratospheric ozone and water vapour changes in CMIP6 models from 1850 to 2100
    (Katlenburg-Lindau : European Geosciences Union, 2021) Keeble, James; Hassler, Birgit; Banerjee, Antara; Checa-Garcia, Ramiro; Chiodo, Gabriel; Davis, Sean; Eyring, Veronika; Griffiths, Paul T.; Morgenstern, Olaf; Nowack, Peer; Zeng, Guang; Zhang, Jiankai; Bodeker, Greg; Burrows, Susannah; Cameron-Smith, Philip; Cugnet, David; Danek, Christopher; Deushi, Makoto; Horowitz, Larry W.; Kubin, Anne; Li, Lijuan; Lohmann, Gerrit; Michou, Martine; Mills, Michael J.; Nabat, Pierre; Olivié, Dirk; Park, Sungsu; Seland, Øyvind; Stoll, Jens; Wieners, Karl-Hermann; Wu, Tongwen
    Stratospheric ozone and water vapour are key components of the Earth system, and past and future changes to both have important impacts on global and regional climate. Here, we evaluate long-term changes in these species from the pre-industrial period (1850) to the end of the 21st century in Coupled Model Intercomparison Project phase 6 (CMIP6) models under a range of future emissions scenarios. There is good agreement between the CMIP multi-model mean and observations for total column ozone (TCO), although there is substantial variation between the individual CMIP6 models. For the CMIP6 multi-model mean, global mean TCO has increased from ∼300 DU in 1850 to ∼ 305 DU in 1960, before rapidly declining in the 1970s and 1980s following the use and emission of halogenated ozone-depleting substances (ODSs). TCO is projected to return to 1960s values by the middle of the 21st century under the SSP2-4.5, SSP3-7.0, SSP4-3.4, SSP4-6.0, and SSP5-8.5 scenarios, and under the SSP3-7.0 and SSP5-8.5 scenarios TCO values are projected to be ∼ 10 DU higher than the 1960s values by 2100. However, under the SSP1-1.9 and SSP1-1.6 scenarios, TCO is not projected to return to the 1960s values despite reductions in halogenated ODSs due to decreases in tropospheric ozone mixing ratios. This global pattern is similar to regional patterns, except in the tropics where TCO under most scenarios is not projected to return to 1960s values, either through reductions in tropospheric ozone under SSP1-1.9 and SSP1-2.6, or through reductions in lower stratospheric ozone resulting from an acceleration of the Brewer-Dobson circulation under other Shared Socioeconomic Pathways (SSPs). In contrast to TCO, there is poorer agreement between the CMIP6 multi-model mean and observed lower stratospheric water vapour mixing ratios, with the CMIP6 multi-model mean underestimating observed water vapour mixing ratios by ∼ 0.5 ppmv at 70 hPa. CMIP6 multi-model mean stratospheric water vapour mixing ratios in the tropical lower stratosphere have increased by ∼ 0.5 ppmv from the pre-industrial to the present-day period and are projected to increase further by the end of the 21st century. The largest increases (∼ 2 ppmv) are simulated under the future scenarios with the highest assumed forcing pathway (e.g. SSP5-8.5). Tropical lower stratospheric water vapour, and to a lesser extent TCO, shows large variations following explosive volcanic eruptions. © Author(s) 2021.
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    Long-term behavior of the concentration of the minor constituents in the mesosphere-a model study
    (Göttingen : Copernicus, 2009) Grygalashvyly, M.; Sonnemann, G.R.; Hartogh, P.
    We investigate the influence the rising concentrations of methane, nitrous oxide and carbon dioxide which have occurred since the pre-industrial era, have had on the chemistry of the mesosphere. For this investigation we use our global 3-D-model COMMA-IAP which was designed for the exploration of the MLT-region and in particular the extended mesopause region. Assumptions and approximations for the trends in the Lyman-flux (needed for the water vapor dissociation rate), methane and the water vapor mixing ratio at the hygropause are necessary to accomplish this study. To approximate the solar Lyman-α flux back to the pre-industrial time, we derived a quadratic fit using the sunspot number record which extends back to 1749 and is the only solar proxy available for the Lyman-α flux prior to 1947. We assume that methane increases with a constant growth rate from the pre-industrial era to the present. An unsolved problem for the model calculations consists of how the water vapor mixing ratio at the hygropause should be specified during this period. We assume that the hygropause was dryer during pre-industrial times than the present. As a consequence of methane oxidation, the model simulation indicates that the middle atmosphere has become more humid as a result of the rising methane concentration, but with some dependence on height and with a small time delay of few years. The solar influence on the water vapor mixing ratio is insignificant below about 80 km in summer high latitudes, but becomes increasingly more important above this altitude. The enhanced water vapor concentration increasesthe hydrogen radical concentration and reduces the mesospheric ozone. A second region of stronger ozone decrease is located in the vicinity of the stratopause. Increases in CO2 concentration enhance slightly the concentration of CO in the mesosphere. However, its influence upon the chemistry is small and its main effect is connected with a cooling of the upper atmosphere. The long-term behavior of water vapor is discussed in particular with respect to its impact on the NLC region.
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    Long-term measurements of aerosol and carbon monoxide at the ZOTTO tall tower to characterize polluted and pristine air in the Siberian taiga
    (München : European Geopyhsical Union, 2013) Chi, X.; Winderlich, J.; Mayer, J.-C.; Panov, A.V.; Heimann, M.; Birmili, W.; Heintzenberg, J.; Cheng, Y.; Andreae, M.O.
    Siberia is one of few continental regions in the Northern Hemisphere where the atmosphere may sometimes approach pristine background conditions. We present the time series of aerosol and carbon monoxide (CO) measurements between September 2006 and December 2011 at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E). We investigate the seasonal, weekly and diurnal variations of aerosol properties (including absorption and scattering coefficients and derived parameters, such as equivalent black carbon (BCe), Ångström exponent, single scattering albedo, and backscattering ratio) and the CO mixing ratios. Criteria were established to distinguish polluted from near-pristine air masses, providing quantitative characteristics for each type. Depending on the season, 23–36% of the sampling time at ZOTTO was found to be representative of a clean atmosphere. The summer pristine data indicate that primary biogenic and secondary organic aerosol formation are quite strong particle sources in the Siberian taiga. The summer seasons 2007–2008 were dominated by an Aitken mode around 80 nm size, whereas the summer 2009 with prevailing easterly winds produced particles in the accumulation mode around 200 nm size. We found these differences to be mainly related to air temperature, through its effect on the production rates of biogenic volatile organic compounds (VOC) precursor gases. In winter, the particle size distribution peaked at 160 nm, and the footprint of clean background air was characteristic for aged particles from anthropogenic sources at great distances from ZOTTO and diluted biofuel burning emissions from domestic heating. The wintertime polluted air originates mainly from large cities south and southwest of the site; these particles have a dominant mode around 100 nm, and the ΔBCe / ΔCO ratio of 7–11 ng m−3 ppb−1 suggests dominant contributions from coal and biofuel burning for heating. During summer, anthropogenic emissions are the dominant contributor to the pollution particles at ZOTTO, while only 12% of the polluted events are classified as biomass-burning-dominated, but then often associated with extremely high CO concentrations and aerosol absorption coefficients. Two biomass-burning case studies revealed different ΔBCe / ΔCO ratios from different fire types, with the agricultural fires in April~2008 yielding a very high ratio of 21 ng m−3 ppb−1. Overall, we find that anthropogenic sources dominate the aerosol population at ZOTTO most of the time, even during nominally clean episodes in winter, and that near-pristine conditions are encountered only in the growing season and then only episodically.
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    Exploring the atmospheric chemistry of nitrous acid (HONO) at a rural site in Southern China
    (München : European Geopyhsical Union, 2012) Li, X.; Brauers, T.; Häseler, R.; Bohn, B.; Fuchs, H.; Hofzumahaus, A.; Holland, F.; Lou, S.; Lu, K.D.; Rohrer, F.; Hu, M.; Zeng, L.M.; Zhang, Y.H.; Garland, R.M.; Su, H.; Nowak, A.; Wiedensohler, A.; Takegawa, N.; Shao, M.; Wahner, A.
    We performed measurements of nitrous acid (HONO) during the PRIDE-PRD2006 campaign in the Pearl River Delta region 60 km north of Guangzhou, China, for 4 weeks in June 2006. HONO was measured by a LOPAP in-situ instrument which was setup in one of the campaign supersites along with a variety of instruments measuring hydroxyl radicals, trace gases, aerosols, and meteorological parameters. Maximum diurnal HONO mixing ratios of 1–5 ppb were observed during the nights. We found that the nighttime build-up of HONO can be attributed to the heterogeneous NO2 to HONO conversion on ground surfaces and the OH + NO reaction. In addition to elevated nighttime mixing ratios, measured noontime values of ≈200 ppt indicate the existence of a daytime source higher than the OH + NO→HONO reaction. Using the simultaneously recorded OH, NO, and HONO photolysis frequency, a daytime additional source strength of HONO (PM) was calculated to be 0.77 ppb h−1 on average. This value compares well to previous measurements in other environments. Our analysis of PM provides evidence that the photolysis of HNO3 adsorbed on ground surfaces contributes to the HONO formation.
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    Calibration of Raman lidar water vapor profiles by means of AERONET photometer observations and GDAS meteorological data
    (München : European Geopyhsical Union, 2018) Dai, Guangyao; Althausen, Dietrich; Hofer, Julian; Engelmann, Ronny; Seifert, Patric; Bühl, Johannes; Mamouri, Rodanthi-Elisavet; Wu, Songhua; Ansmann, Albert
    We present a practical method to continuously calibrate Raman lidar observations of water vapor mixing ratio profiles. The water vapor profile measured with the multiwavelength polarization Raman lidar PollyXT is calibrated by means of co-located AErosol RObotic NETwork (AERONET) sun photometer observations and Global Data Assimilation System (GDAS) temperature and pressure profiles. This method is applied to lidar observations conducted during the Cyprus Cloud Aerosol and Rain Experiment (CyCARE) in Limassol, Cyprus. We use the GDAS temperature and pressure profiles to retrieve the water vapor density. In the next step, the precipitable water vapor from the lidar observations is used for the calibration of the lidar measurements with the sun photometer measurements. The retrieved calibrated water vapor mixing ratio from the lidar measurements has a relative uncertainty of 11 % in which the error is mainly caused by the error of the sun photometer measurements. During CyCARE, nine measurement cases with cloud-free and stable meteorological conditions are selected to calculate the precipitable water vapor from the lidar and the sun photometer observations. The ratio of these two precipitable water vapor values yields the water vapor calibration constant. The calibration constant for the PollyXT Raman lidar is 6.56 g kg−1 ± 0.72 g kg−1 (with a statistical uncertainty of 0.08 g kg−1 and an instrumental uncertainty of 0.72 g kg−1). To check the quality of the water vapor calibration, the water vapor mixing ratio profiles from the simultaneous nighttime observations with Raman lidar and Vaisala radiosonde sounding are compared. The correlation of the water vapor mixing ratios from these two instruments is determined by using all of the 19 simultaneous nighttime measurements during CyCARE. Excellent agreement with the slope of 1.01 and the R2 of 0.99 is found. One example is presented to demonstrate the full potential of a well-calibrated Raman lidar. The relative humidity profiles from lidar, GDAS (simulation) and radiosonde are compared, too. It is found that the combination of water vapor mixing ratio and GDAS temperature profiles allow us to derive relative humidity profiles with the relative uncertainty of 10–20 %.
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    Multi-wavelength Raman lidar, sun photometric and aircraft measurements in combination with inversion models for the estimation of the aerosol optical and physico-chemical properties over Athens, Greece
    (München : European Geopyhsical Union, 2012) Mamouri, R.E.; Papayannis, A.; Amiridis, V.; Müller, D.; Kokkalis, P.; Rapsomanikis, S.; Karageorgos, E.T.; Tsaknakis, G.; Nenes, A.; Kazadzis, S.; Remoundaki, E.
    A novel procedure has been developed to retrieve, simultaneously, the optical, microphysical and chemical properties of tropospheric aerosols with a multi-wavelength Raman lidar system in the troposphere over an urban site (Athens, Greece: 37.9° N, 23.6° E, 200 m a.s.l.) using data obtained during the European Space Agency (ESA) THERMOPOLIS project, which took place between 15–31 July 2009 over the Greater Athens Area (GAA). We selected to apply our procedure for a case study of intense aerosol layers that occurred on 20–21 July 2009. The National Technical University of Athens (NTUA) EOLE 6-wavelength Raman lidar system has been used to provide the vertical profiles of the optical properties of aerosols (extinction and backscatter coefficients, lidar ratio) and the water vapor mixing ratio. An inversion algorithm was used to derive the mean aerosol microphysical properties (mean effective radius (reff), single-scattering albedo ω) and mean complex refractive index (m)) at selected heights in the 2–3 km height region. We found that reff was 0.14–0.4 (±0.14) μm, ω was 0.63–0.88 (±0.08) (at 532 nm) and m ranged from 1.44 (±0.10) + 0.01 (±0.01)i to 1.55 (±0.12) + 0.06 (±0.02)i, in good agreement (only for the reff values) with in situ aircraft measurements. The water vapor and temperature profiles were incorporated into the ISORROPIA II model to propose a possible in situ aerosol composition consistent with the retrieved m and ω values. The retrieved aerosol chemical composition in the 2–3 km height region gave a variable range of sulfate (0–60%) and organic carbon (OC) content (0–50%), although the OC content increased (up to 50%) and the sulfate content dropped (up to 30%) around 3 km height; the retrieved low ω value (0.63), indicates the presence of absorbing biomass burning smoke mixed with urban haze. Finally, the retrieved aerosol microphysical properties were compared with column-integrated sun photometer CIMEL data.
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    Profiling water vapor mixing ratios in Finland by means of a Raman lidar, a satellite and a model
    (Katlenburg-Lindau : Copernicus, 2017) Filioglou, Maria; Nikandrova, Anna; Niemelä, Sami; Baars, Holger; Mielonen, Tero; Leskinen, Ari; Brus, David; Romakkaniemi, Sami; Giannakaki, Elina; Komppula, Mika
    We present tropospheric water vapor profiles measured with a Raman lidar during three field campaigns held in Finland. Co-located radio soundings are available throughout the period for the calibration of the lidar signals. We investigate the possibility of calibrating the lidar water vapor profiles in the absence of co-existing on-site soundings using water vapor profiles from the combined Advanced InfraRed Sounder (AIRS) and the Advanced Microwave Sounding Unit (AMSU) satellite product; the Aire Limitée Adaptation dynamique Développement INternational and High Resolution Limited Area Model (ALADIN/HIRLAM) numerical weather prediction (NWP) system, and the nearest radio sounding station located 100 km away from the lidar site (only for the permanent location of the lidar). The uncertainties of the calibration factor derived from the soundings, the satellite and the model data are < 2.8, 7.4 and 3.9 %, respectively. We also include water vapor mixing ratio intercomparisons between the radio soundings and the various instruments/model for the period of the campaigns. A good agreement is observed for all comparisons with relative errors that do not exceed 50 % up to 8 km altitude in most cases. A 4-year seasonal analysis of vertical water vapor is also presented for the Kuopio site in Finland. During winter months, the air in Kuopio is dry (1.15±0.40 †kg-1); during summer it is wet (5.54±1.02 †kg-1); and at other times, the air is in an intermediate state. These are averaged values over the lowest 2 km in the atmosphere. Above that height a quick decrease in water vapor mixing ratios is observed, except during summer months where favorable atmospheric conditions enable higher mixing ratio values at higher altitudes. Lastly, the seasonal change in disagreement between the lidar and the model has been studied. The analysis showed that, on average, the model underestimates water vapor mixing ratios at high altitudes during spring and summer.
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    Towards closing the gap between hygroscopic growth and CCN activation for secondary organic aerosols-Part 3: Influence of the chemical composition on the hygroscopic properties and volatile fractions of aerosols
    (Göttingen : Copernicus, 2010) Poulain, L.; Wu, Z.; Petters, M.D.; Wex, H.; Hallbauer, E.; Wehner, B.; Massling, A.; Kreidenweis, S.M.; Stratmann, F.
    The influence of varying levels of water mixing ratio,r during the formation of secondary organic aerosol (SOA) from the ozonolysis of α-pinene on the SOA hygroscopicity and volatility was investigated. The reaction proceeded and aerosols were generated in a mixing chamber and the hygroscopic characteristics of the SOA were determined with the Leipzig Aerosol Cloud Interaction Simulator (LACIS) and a Cloud Condensation Nuclei counter (CCNc). In parallel, a High-Resolution Time-of-Flight Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS) located downstream of a thermodenuder (TD) sampling from the mixing chamber, to collect mass spectra of particles from the volatile and less-volatile fractions of the SOA. Results showed that both hygroscopic growth and the volatile fraction of the SOA increased with increases in r inside the mixing chamber during SOA generation. An effective density of 1.40 g cm-3 was observed for the generated SOA when the reaction proceeded with <1 g kg-1. Changes in the concentrations of the fragment CO2+ and the sum of CxH+y(short name CHO) and CxH+y (short name CH) fragments as measured by the HR-ToF-AMS were used to estimate changes in the oxidation level of the SOA with reaction conditions, using the ratios CO2 + to CH and CHO to CH. Under humid conditions, both ratios increased, corresponding to the presence of more oxygenated functional groups (i.e., multifunctional carboxylic acids). This result is consistent with the α-pinene ozonolysis mechanisms which suggest that water interacts with the stabilized Criegee intermediate. The volatility and the hygroscopicity results show that SOA generation via ozonolysis of α-pinene in the presence of water vapour (r <16.9 g kg-1) leads to the formation of more highly oxygenated compounds that are more hygroscopic and more volatile than compounds formed under dry conditions. © 2010 Author(s).
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    Airborne observations of the Eyjafjalla volcano ash cloud over Europe during air space closure in April and May 2010
    (München : European Geopyhsical Union, 2011) Schumann, U.; Weinzierl, B.; Reitebuch, O.; Schlager, H.; Minikin, A.; Forster, C.; Baumann, R.; Sailer, T.; Graf, K.; Mannstein, H.; Voigt, C.; Rahm, S.; Simmet, R.; Scheibe, M.; Lichtenstern, M.; Stock, P.; Rüba, H.; Schäuble, D.; Tafferner, A.; Rautenhaus, M.; Gerz, T.; Ziereis, H.; Krautstrunk, M.; Mallaun, C.; Gayet, J.-F.; Lieke, K.; Kandler, K.; Ebert, M.; Weinbruch, S.; Stohl, A.; Gasteiger, J.; Groß, S.; Freudenthaler, V.; Wiegner, M.; Ansmann, A.; Tesche, M.; Olafsson, H.; Sturm, K.
    Airborne lidar and in-situ measurements of aerosols and trace gases were performed in volcanic ash plumes over Europe between Southern Germany and Iceland with the Falcon aircraft during the eruption period of the Eyjafjalla volcano between 19 April and 18 May 2010. Flight planning and measurement analyses were supported by a refined Meteosat ash product and trajectory model analysis. The volcanic ash plume was observed with lidar directly over the volcano and up to a distance of 2700 km downwind, and up to 120 h plume ages. Aged ash layers were between a few 100 m to 3 km deep, occurred between 1 and 7 km altitude, and were typically 100 to 300 km wide. Particles collected by impactors had diameters up to 20 μm diameter, with size and age dependent composition. Ash mass concentrations were derived from optical particle spectrometers for a particle density of 2.6 g cm−3 and various values of the refractive index (RI, real part: 1.59; 3 values for the imaginary part: 0, 0.004 and 0.008). The mass concentrations, effective diameters and related optical properties were compared with ground-based lidar observations. Theoretical considerations of particle sedimentation constrain the particle diameters to those obtained for the lower RI values. The ash mass concentration results have an uncertainty of a factor of two. The maximum ash mass concentration encountered during the 17 flights with 34 ash plume penetrations was below 1 mg m−3. The Falcon flew in ash clouds up to about 0.8 mg m−3 for a few minutes and in an ash cloud with approximately 0.2 mg m−3 mean-concentration for about one hour without engine damage. The ash plumes were rather dry and correlated with considerable CO and SO2 increases and O3 decreases. To first order, ash concentration and SO2 mixing ratio in the plumes decreased by a factor of two within less than a day. In fresh plumes, the SO2 and CO concentration increases were correlated with the ash mass concentration. The ash plumes were often visible slantwise as faint dark layers, even for concentrations below 0.1 mg m−3. The large abundance of volatile Aitken mode particles suggests previous nucleation of sulfuric acid droplets. The effective diameters range between 0.2 and 3 μm with considerable surface and volume contributions from the Aitken and coarse mode aerosol, respectively. The distal ash mass flux on 2 May was of the order of 500 (240–1600) kg s−1. The volcano induced about 10 (2.5–50) Tg of distal ash mass and about 3 (0.6–23) Tg of SO2 during the whole eruption period. The results of the Falcon flights were used to support the responsible agencies in their decisions concerning air traffic in the presence of volcanic ash.