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Measurements of aerosol and CCN properties in the Mackenzie River delta (Canadian Arctic) during spring-summer transition in May 2014

2018, Herenz, Paul, Wex, Heike, Henning, Silvia, Kristensen, Thomas Bjerring, Rubach, Florian, Roth, Anja, Borrmann, Stephan, Bozem, Heiko, Schulz, Hannes, Stratmann, Frank

Within the framework of the RACEPAC (Radiation-Aerosol-Cloud Experiment in the Arctic Circle) project, the Arctic aerosol, arriving at a ground-based station in Tuktoyaktuk (Mackenzie River delta area, Canada), was characterized during a period of 3 weeks in May 2014. Basic meteorological parameters and particle number size distributions (PNSDs) were observed and two distinct types of air masses were found. One type were typical Arctic haze air masses, termed accumulation-type air masses, characterized by a monomodal PNSD with a pronounced accumulation mode at sizes above 100 nm. These air masses were observed during a period when back trajectories indicate an air mass origin in the north-east of Canada. The other air mass type is characterized by a bimodal PNSD with a clear minimum around 90ĝ€†nm and with an Aitken mode consisting of freshly formed aerosol particles. Back trajectories indicate that these air masses, termed Aitken-type air masses, originated from the North Pacific. In addition, the application of the PSCF receptor model shows that air masses with their origin in active fire areas in central Canada and Siberia, in areas of industrial anthropogenic pollution (Norilsk and Prudhoe Bay Oil Field) and the north-west Pacific have enhanced total particle number concentrations (N CN). Generally, N CN ranged from 20 to 500 cmg'3, while cloud condensation nuclei (CCN) number concentrations were found to cover a range from less than 10 up to 250 cmg'3 for a supersaturation (SS) between 0.1 and 0.7 %. The hygroscopicity parameter of the CCN was determined to be 0.23 on average and variations in were largely attributed to measurement uncertainties.

Furthermore, simultaneous PNSD measurements at the ground station and on the Polar 6 research aircraft were performed. We found a good agreement of ground-based PNSDs with those measured between 200 and 1200 m. During two of the four overflights, particle number concentrations at 3000 m were found to be up to 20 times higher than those measured below 2000 m; for one of these two flights, PNSDs measured above 2000 m showed a different shape than those measured at lower altitudes. This is indicative of long-range transport from lower latitudes into the Arctic that can advect aerosol from different regions in different heights.

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The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): Laboratory intercomparison of ice nucleation measurements

2018, DeMott, Paul J., Möhler, Ottmar, Cziczo, Daniel J., Hiranuma, Naruki, Petters, Markus D., Petters, Sarah S., Belosi, Franco, Bingemer, Heinz G., Brooks, Sarah D., Budke, Carsten, Burkert-Kohn, Monika, Collier, Kristen N., Danielczok, Anja, Eppers, Oliver, Felgitsch, Laura, Garimella, Sarvesh, Grothe, Hinrich, Herenz, Paul, Hill, Thomas C. J., Höhler, Kristina, Kanji, Zamin A., Kiselev, Alexei, Koop, Thomas, Kristensen, Thomas B., Krüger, Konstantin, Kulkarni, Gourihar, Levin, Ezra J. T., Murray, Benjamin J., Nicosia, Alessia, O'Sullivan, Daniel, Peckhaus, Andreas, Polen, Michael J., Price, Hannah C., Reicher, Naama, Rothenberg, Daniel A., Rudich, Yinon, Santachiara, Gianni, Schiebel, Thea, Schrod, Jann, Seifried, Teresa M., Stratmann, Frank, Sullivan, Ryan C., Suski, Kaitlyn J., Szakáll, Miklós, Taylor, Hans P., Ullrich, Romy, Vergara-Temprado, Jesus, Wagner, Robert, Whale, Thomas F., Weber, Daniel, Welti, André, Wilson, Theodore W., Wolf, Martin J., Zenker, Jake

The second phase of the Fifth International Ice Nucleation Workshop (FIN-02) involved the gathering of a large number of researchers at the Karlsruhe Institute of Technology's Aerosol Interactions and Dynamics of the Atmosphere (AIDA) facility to promote characterization and understanding of ice nucleation measurements made by a variety of methods used worldwide. Compared to the previous workshop in 2007, participation was doubled, reflecting a vibrant research area. Experimental methods involved sampling of aerosol particles by direct processing ice nucleation measuring systems from the same volume of air in separate experiments using different ice nucleating particle (INP) types, and collections of aerosol particle samples onto filters or into liquid for sharing amongst measurement techniques that post-process these samples. In this manner, any errors introduced by differences in generation methods when samples are shared across laboratories were mitigated. Furthermore, as much as possible, aerosol particle size distribution was controlled so that the size limitations of different methods were minimized. The results presented here use data from the workshop to assess the comparability of immersion freezing measurement methods activating INPs in bulk suspensions, methods that activate INPs in condensation and/or immersion freezing modes as single particles on a substrate, continuous flow diffusion chambers (CFDCs) directly sampling and processing particles well above water saturation to maximize immersion and subsequent freezing of aerosol particles, and expansion cloud chamber simulations in which liquid cloud droplets were first activated on aerosol particles prior to freezing. The AIDA expansion chamber measurements are expected to be the closest representation to INP activation in atmospheric cloud parcels in these comparisons, due to exposing particles freely to adiabatic cooling. The different particle types used as INPs included the minerals illite NX and potassium feldspar (K-feldspar), two natural soil dusts representative of arable sandy loam (Argentina) and highly erodible sandy dryland (Tunisia) soils, respectively, and a bacterial INP (Snomax®). Considered together, the agreement among post-processed immersion freezing measurements of the numbers and fractions of particles active at different temperatures following bulk collection of particles into liquid was excellent, with possible temperature uncertainties inferred to be a key factor in determining INP uncertainties. Collection onto filters for rinsing versus directly into liquid in impingers made little difference. For methods that activated collected single particles on a substrate at a controlled humidity at or above water saturation, agreement with immersion freezing methods was good in most cases, but was biased low in a few others for reasons that have not been resolved, but could relate to water vapor competition effects. Amongst CFDC-style instruments, various factors requiring (variable) higher supersaturations to achieve equivalent immersion freezing activation dominate the uncertainty between these measurements, and for comparison with bulk immersion freezing methods. When operated above water saturation to include assessment of immersion freezing, CFDC measurements often measured at or above the upper bound of immersion freezing device measurements, but often underestimated INP concentration in comparison to an immersion freezing method that first activates all particles into liquid droplets prior to cooling (the PIMCA-PINC device, or Portable Immersion Mode Cooling chAmber-Portable Ice Nucleation Chamber), and typically slightly underestimated INP number concentrations in comparison to cloud parcel expansions in the AIDA chamber; this can be largely mitigated when it is possible to raise the relative humidity to sufficiently high values in the CFDCs, although this is not always possible operationally. Correspondence of measurements of INPs among direct sampling and post-processing systems varied depending on the INP type. Agreement was best for Snomax® particles in the temperature regime colder than -10°C, where their ice nucleation activity is nearly maximized and changes very little with temperature. At temperatures warmer than -10°C, Snomax® INP measurements (all via freezing of suspensions) demonstrated discrepancies consistent with previous reports of the instability of its protein aggregates that appear to make it less suitable as a calibration INP at these temperatures. For Argentinian soil dust particles, there was excellent agreement across all measurement methods; measures ranged within 1 order of magnitude for INP number concentrations, active fractions and calculated active site densities over a 25 to 30°C range and 5 to 8 orders of corresponding magnitude change in number concentrations. This was also the case for all temperatures warmer than -25°C in Tunisian dust experiments. In contrast, discrepancies in measurements of INP concentrations or active site densities that exceeded 2 orders of magnitude across a broad range of temperature measurements found at temperatures warmer than -25°C in a previous study were replicated for illite NX. Discrepancies also exceeded 2 orders of magnitude at temperatures of -20 to -25°C for potassium feldspar (K-feldspar), but these coincided with the range of temperatures at which INP concentrations increase rapidly at approximately an order of magnitude per 2°C cooling for K-feldspar. These few discrepancies did not outweigh the overall positive outcomes of the workshop activity, nor the future utility of this data set or future similar efforts for resolving remaining measurement issues. Measurements of the same materials were repeatable over the time of the workshop and demonstrated strong consistency with prior studies, as reflected by agreement of data broadly with parameterizations of different specific or general (e.g., soil dust) aerosol types. The divergent measurements of the INP activity of illite NX by direct versus post-processing methods were not repeated for other particle types, and the Snomax° data demonstrated that, at least for a biological INP type, there is no expected measurement bias between bulk collection and direct immediately processed freezing methods to as warm as -10°C. Since particle size ranges were limited for this workshop, it can be expected that for atmospheric populations of INPs, measurement discrepancies will appear due to the different capabilities of methods for sampling the full aerosol size distribution, or due to limitations on achieving sufficient water supersaturations to fully capture immersion freezing in direct processing instruments. Overall, this workshop presents an improved picture of present capabilities for measuring INPs than in past workshops, and provides direction toward addressing remaining measurement issues.

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Simulation of atmospheric organic aerosol using its volatility-oxygen-content distribution during the PEGASOS 2012 campaign

2018, Karnezi, Eleni, Murphy, Benjamin N., Poulain, Laurent, Herrmann, Hartmut, Wiedensohler, Alfred, Rubach, Florian, Kiendler-Scharr, Astrid, Mentel, Thomas F., Pandis, Spyros N.

A lot of effort has been made to understand and constrain the atmospheric aging of the organic aerosol (OA). Different parameterizations of the organic aerosol formation and evolution in the two-dimensional volatility basis set (2D-VBS) framework are evaluated using ground and airborne measurements collected in the 2012 Pan-European Gas AeroSOls-climate interaction Study (PEGASOS) field campaign in the Po Valley (Italy). A number of chemical aging schemes are examined, taking into account various functionalization and fragmentation pathways for biogenic and anthropogenic OA components. Model predictions and measurements, both at the ground and aloft, indicate a relatively oxidized OA with little average diurnal variation. Total OA concentration and O: C ratios are reproduced within experimental error by a number of chemical aging schemes. Anthropogenic secondary OA (SOA) is predicted to contribute 15-25% of the total OA, while SOA from intermediate volatility compound oxidation contributes another 20-35%. Biogenic SOA (bSOA) contributions varied from 15 to 45% depending on the modeling scheme. Primary OA contributed around 5% for all schemes and was comparable to the hydrocarbon-like OA (HOA) concentrations derived from the positive matrix factorization of the aerosol mass spectrometer (PMF-AMS) ground measurements. The average OA and O: C diurnal variation and their vertical profiles showed a surprisingly modest sensitivity to the assumed vaporization enthalpy for all aging schemes. This can be explained by the interplay between the partitioning of the semi-volatile compounds and their gas-phase chemical aging reactions.

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Helicopter-borne observations of the continental background aerosol in combination with remote sensing and ground-based measurements

2018, Düsing, Sebastian, Wehner, Birgit, Seifert, Patric, Ansmann, Albert, Baars, Holger, Ditas, Florian, Henning, Silvia, Ma, Nan, Poulain, Laurent, Siebert, Holger, Wiedensohler, Alfred, Macke, Andreas

This paper examines the representativeness of ground-based in situ measurements for the planetary boundary layer (PBL) and conducts a closure study between airborne in situ and ground-based lidar measurements up to an altitude of 2300 m. The related measurements were carried out in a field campaign within the framework of the High-Definition Clouds and Precipitation for Advancing Climate Prediction (HD(CP)2) Observational Prototype Experiment (HOPE) in September 2013 in a rural background area of central Europe. The helicopter-borne probe ACTOS (Airborne Cloud and Turbulence Observation System) provided measurements of the aerosol particle number size distribution (PNSD), the aerosol particle number concentration (PNC), the number concentration of cloud condensation nuclei (CCN-NC), and meteorological atmospheric parameters (e.g., temperature and relative humidity). These measurements were supported by the ground-based 3+2 wavelength polarization lidar system PollyXT, which provided profiles of the particle backscatter coefficient (σbsc) for three wavelengths (355, 532, and 1064 nm). Particle extinction coefficient (σext) profiles were obtained by using a fixed backscatter-to-extinction ratio (also lidar ratio, LR). A new approach was used to determine profiles of CCN-NC for continental aerosol. The results of this new approach were consistent with the airborne in situ measurements within the uncertainties. In terms of representativeness, the PNSD measurements on the ground showed a good agreement with the measurements provided with ACTOS for lower altitudes. The ground-based measurements of PNC and CCN-NC are representative of the PBL when the PBL is well mixed. Locally isolated new particle formation events on the ground or at the top of the PBL led to vertical variability in the cases presented here and ground-based measurements are not entirely representative of the PBL. Based on Mie theory (Mie, 1908), optical aerosol properties under ambient conditions for different altitudes were determined using the airborne in situ measurements and were compared with the lidar measurements. The investigation of the optical properties shows that on average the airborne-based particle light backscatter coefficient is 50.1 % smaller for 1064 nm, 27.4 % smaller for 532 nm, and 29.5 % smaller for 355 nm than the measurements of the lidar system. These results are quite promising, since in situ measurement-based Mie calculations of the particle light backscattering are scarce and the modeling is quite challenging. In contrast, for the particle light extinction coefficient we found a good agreement. The airborne-based particle light extinction coefficient was just 8.2 % larger for 532 nm and 3 % smaller for 355 nm, for an assumed LR of 55 sr. The particle light extinction coefficient for 1064 nm was derived with a LR of 30 sr. For this wavelength, the airborne-based particle light extinction coefficient is 5.2 % smaller than the lidar measurements. For the first time, the lidar ratio of 30 sr for 1064 nm was determined on the basis of in situ measurements and the LR of 55 sr for 355 and 532 nm wavelength was reproduced for European continental aerosol on the basis of this comparison. Lidar observations and the in situ based aerosol optical properties agree within the uncertainties. However, our observations indicate that a determination of the PNSD for a large size range is important for a reliable modeling of aerosol particle backscattering.

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Vertical profiles of aerosol mass concentration derived by unmanned airborne in situ and remote sensing instruments during dust events

2018, Mamali, Dimitra, Marinou, Eleni, Sciare, Jean, Pikridas, Michael, Kokkalis, Panagiotis, Kottas, Michael, Binietoglou, Ioannis, Tsekeri, Alexandra, Keleshis, Christos, Engelmann, Ronny, Baars, Holger, Ansmann, Albert, Amiridis, Vassilis, Russchenberg, Herman, Biskos, George

In situ measurements using unmanned aerial vehicles (UAVs) and remote sensing observations can independently provide dense vertically resolved measurements of atmospheric aerosols, information which is strongly required in climate models. In both cases, inverting the recorded signals to useful information requires assumptions and constraints, and this can make the comparison of the results difficult. Here we compare, for the first time, vertical profiles of the aerosol mass concentration derived from light detection and ranging (lidar) observations and in situ measurements using an optical particle counter on board a UAV during moderate and weak Saharan dust episodes. Agreement between the two measurement methods was within experimental uncertainty for the coarse mode (i.e. particles having radii > 0.5 μm), where the properties of dust particles can be assumed with good accuracy. This result proves that the two techniques can be used interchangeably for determining the vertical profiles of aerosol concentrations, bringing them a step closer towards their systematic exploitation in climate models.

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Aircraft-based observations of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX-SOA) in the tropical upper troposphere over the Amazon region

2018, Schulz, Christiane, Schneider, Johannes, Amorim Holanda, Bruna, Appel, Oliver, Costa, Anja, de Sá, Suzane S., Dreiling, Volker, Fütterer, Daniel, Jurkat-Witschas, Tina, Klimach, Thomas, Knote, Christoph, Krämer, Martina, Martin, Scot T., Mertes, Stephan, Pöhlker, Mira L., Sauer, Daniel, Voigt, Christiane, Walser, Adrian, Weinzierl, Bernadett, Ziereis, Helmut, Zöger, Martin, Andreae, Meinrat O., Artaxo, Paulo, Machado, Luiz A. T., Pöschl, Ulrich, Wendisch, Manfred, Borrmann, Stephan

During the ACRIDICON-CHUVA field project (September-October 2014; based in Manaus, Brazil) aircraft-based in situ measurements of aerosol chemical composition were conducted in the tropical troposphere over the Amazon using the High Altitude and Long Range Research Aircraft (HALO), covering altitudes from the boundary layer (BL) height up to 14.4km. The submicron non-refractory aerosol was characterized by flash-vaporization/electron impact-ionization aerosol particle mass spectrometry. The results show that significant secondary organic aerosol (SOA) formation by isoprene oxidation products occurs in the upper troposphere (UT), leading to increased organic aerosol mass concentrations above 10km altitude. The median organic mass concentrations in the UT above 10km range between 1.0 and 2.5μgm-3 (referring to standard temperature and pressure; STP) with interquartile ranges of 0.6 to 3.2μgm-3 (STP), representing 78% of the total submicron non-refractory aerosol particle mass. The presence of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX-SOA) was confirmed by marker peaks in the mass spectra. We estimate the contribution of IEPOX-SOA to the total organic aerosol in the UT to be about 20%. After isoprene emission from vegetation, oxidation processes occur at low altitudes and/or during transport to higher altitudes, which may lead to the formation of IEPOX (one oxidation product of isoprene). Reactive uptake or condensation of IEPOX on preexisting particles leads to IEPOX-SOA formation and subsequently increasing organic mass in the UT. This organic mass increase was accompanied by an increase in the nitrate mass concentrations, most likely due to NOx production by lightning. Analysis of the ion ratio of NO+ to NO2+ indicated that nitrate in the UT exists mainly in the form of organic nitrate. IEPOX-SOA and organic nitrates are coincident with each other, indicating that IEPOX-SOA forms in the UT either on acidic nitrate particles forming organic nitrates derived from IEPOX or on already neutralized organic nitrate aerosol particles.

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Airborne observations of newly formed boundary layer aerosol particles under cloudy conditions

2018, Altstädter, Barbara, Platis, Andreas, Jähn, Michael, Baars, Holger, Lückerath, Janine, Held, Andreas, Lampert, Astrid, Bange, Jens, Hermann, Markus, Wehner, Birgit

This study describes the appearance of ultrafine boundary layer aerosol particles under classical “non-favourable” conditions at the research site of TROPOS (Leibniz Institute for Tropospheric Research). Airborne measurements of meteorological and aerosol properties of the atmospheric boundary layer (ABL) were repeatedly performed with the unmanned aerial system ALADINA (Application of Light-weight Aircraft for Detecting IN-situ Aerosol) during three seasons between October 2013 and July 2015. More than 100 measurement flights were conducted on 23 different days with a total flight duration of 53 h. In 26 % of the cases, maxima of ultrafine particles were observed close to the inversion layer at altitudes between 400 and 600 m and the particles were rapidly mixed vertically and mainly transported downwards during short time intervals of cloud gaps. This study focuses on two measurement days affected by low-level stratocumulus clouds, but different wind directions (NE, SW) and minimal concentrations (< 4.6 µg m−3) of SO2, as a common indicator for precursor gases at ground. Taken from vertical profiles, the onset of clouds led to a non-linearity of humidity that resulted in an increased turbulence at the local-scale and caused fast nucleation (e.g. Bigg, 1997; Wehner et al., 2010), but in relation to rapid dilution of surrounding air, seen in sporadic clusters of ground data, so that ultrafine particles disappeared in the verticality. The typical “banana shape” (Heintzenberg et al., 2007) of new particle formation (NPF) and growth was not seen at ground and thus these days might not have been classified as NPF event days by pure surface studies.

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Separation of the optical and mass features of particle components in different aerosol mixtures by using POLIPHON retrievals in synergy with continuous polarized Micro-Pulse Lidar (P-MPL) measurements

2018, Córdoba-Jabonero, Carmen, Sicard, Michaël, Ansmann, Albert, del Águila, Ana, Baars, Holger

The application of the POLIPHON (POlarization-LIdar PHOtometer Networking) method is presented for the first time in synergy with continuous 24/7 polarized Micro-Pulse Lidar (P-MPL) measurements to derive the vertical separation of two or three particle components in different aerosol mixtures, and the retrieval of their particular optical properties. The procedure of extinction-to-mass conversion, together with an analysis of the mass extinction efficiency (MEE) parameter, is described, and the relative mass contribution of each aerosol component is also derived in a further step. The general POLIPHON algorithm is based on the specific particle linear depolarization ratio given for different types of aerosols and can be run in either 1-step (POL-1) or 2 steps (POL-2) versions with dependence on either the 2- or 3-component separation. In order to illustrate this procedure, aerosol mixing cases observed over Barcelona (NE Spain) are selected: a dust event on 5 July 2016, smoke plumes detected on 23 May 2016 and a pollination episode observed on 23 March 2016. In particular, the 3-component separation is just applied for the dust case: a combined POL-1 with POL-2 procedure (POL-1/2) is used, and additionally the fine-dust contribution to the total fine mode (fine dust plus non-dust aerosols) is estimated. The high dust impact before 12:00 UTC yields a mean mass loading of 0.6±0.1 g m'2 due to the prevalence of Saharan coarse-dust particles. After that time, the mean mass loading is reduced by two-thirds, showing a rather weak dust incidence. In the smoke case, the arrival of fine biomass-burning particles is detected at altitudes as high as 7 km. The smoke particles, probably mixed with less depolarizing non-smoke aerosols, are observed in air masses, having their origin from either North American fires or the Arctic area, as reported by HYSPLIT back-trajectory analysis. The particle linear depolarization ratio for smoke shows values in the 0.10-0.15 range and even higher at given times, and the daily mean smoke mass loading is 0.017±0.008 g m'2, around 3 % of that found for the dust event. Pollen particles are detected up to 1.5 km in height from 10:00 UTC during an intense pollination event with a particle linear depolarization ratio ranging between 0.10 and 0.15. The maximal mass loading of Platanus pollen particles is 0.011±0.003 g m'2, representing around 2 % of the dust loading during the higher dust incidence. Regarding the MEE derived for each aerosol component, their values are in agreement with others referenced in the literature for the specific aerosol types examined in this work: 0.5±0.1 and 1.7±0.2 m2 g'1 are found for coarse and fine dust particles, 4.5±1.4 m2 g'1 is derived for smoke and 2.4±0.5 m2 g'1 for non-smoke aerosols with Arctic origin, and a MEE of 2.4±0.8 m2 g'1 is obtained for pollen particles, though it can reach higher or lower values depending on predominantly smaller or larger pollen grain sizes. Results reveal the high potential of the P-MPL system, a simple polarization-sensitive elastic backscatter lidar working in a 24/7 operation mode, to retrieve the relative optical and mass contributions of each aerosol component throughout the day, reflecting the daily variability of their properties. In fact, this procedure can be simply implemented in other P-MPLs that also operate within the worldwide Micro-Pulse Lidar Network (MPLNET), thus extending the aerosol discrimination at a global scale. Moreover, the method has the advantage of also being relatively easily applicable to space-borne lidars with an equivalent configuration such as the ongoing Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) on board NASA CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) and the forthcoming Atmospheric Lidar (ATLID) on board the ESA EarthCARE mission.

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Global relevance of marine organic aerosol as ice nucleating particles

2018, Huang, Wan Ting Katty, Ickes, Luisa, Tegen, Ina, Rinaldi, Matteo, Ceburnis, Darius, Lohmann, Ulrike

Ice nucleating particles (INPs) increase the temperature at which supercooled droplets start to freeze. They are therefore of particular interest in mixed-phase cloud temperature regimes, where supercooled liquid droplets can persist for extended periods of time in the absence of INPs. When INPs are introduced to such an environment, the cloud can quickly glaciate following ice multiplication processes and the Wegener–Bergeron–Findeisen (WBF) process. The WBF process can also cause the ice to grow to precipitation size and precipitate out. All of these processes alter the radiative properties. Despite their potential influence on climate, the ice nucleation ability and importance of different aerosol species is still not well understood and is a field of active research. In this study, we use the aerosol–climate model ECHAM6-HAM2 to examine the global relevance of marine organic aerosol (MOA), which has drawn much interest in recent years as a potentially important INPs in remote marine regions. We address the uncertainties in emissions and ice nucleation activity of MOA with a range of reasonable set-ups and find a wide range of resulting MOA burdens. The relative importance of MOA as an INP compared to dust is investigated and found to depend strongly on the type of ice nucleation parameterisation scheme chosen. On the zonal mean, freezing due to MOA leads to relative increases in the cloud ice occurrence and in-cloud number concentration close to the surface in the polar regions during summer. Slight but consistent decreases in the in-cloud ice crystal effective radius can also be observed over the same regions during all seasons. Regardless, MOA was not found to affect the radiative balance significantly on the global scale, due to its relatively weak ice activity and a low sensitivity of cloud ice properties to heterogeneous ice nucleation in our model.

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Long-term study on coarse mode aerosols in the Amazon rain forest with the frequent intrusion of Saharan dust plumes

2018, Moran-Zuloaga, Daniel, Ditas, Florian, Walter, David, Saturno, Jorge, Brito, Joel, Carbone, Samara, Chi, Xuguang, Hrabě de Angelis, Isabella, Baars, Holger, Godoi, Ricardo H. M., Heese, Birgit, Holanda, Bruna A., Lavrič, Jošt V., Martin, Scot T., Ming, Jing, Pöhlker, Mira L., Ruckteschler, Nina, Su, Hang, Wang, Yaqiang, Wang, Qiaoqiao, Wang, Zhibin, Weber, Bettina, Wolff, Stefan, Artaxo, Paulo, Pöschl, Ulrich, Andreae, Meinrat O., Pöhlker, Christopher

In the Amazonian atmosphere, the aerosol coarse mode comprises a complex, diverse, and variable mixture of bioaerosols emitted from the rain forest ecosystem, long-range transported Saharan dust (we use Sahara as shorthand for the dust source regions in Africa north of the Equator), marine aerosols from the Atlantic Ocean, and coarse smoke particles from deforestation fires. For the rain forest, the coarse mode particles are of significance with respect to biogeochemical and hydrological cycling, as well as ecology and biogeography. However, knowledge on the physicochemical and biological properties as well as the ecological role of the Amazonian coarse mode is still sparse. This study presents results from multi-year coarse mode measurements at the remote Amazon Tall Tower Observatory (ATTO) site. It combines online aerosol observations, selected remote sensing and modeling results, as well as dedicated coarse mode sampling and analysis. The focal points of this study are a systematic characterization of aerosol coarse mode abundance and properties in the Amazonian atmosphere as well as a detailed analysis of the frequent, pulse-wise intrusion of African long-range transport (LRT) aerosols (comprising Saharan dust and African biomass burning smoke) into the Amazon Basin.We find that, on a multi-year time scale, the Amazonian coarse mode maintains remarkably constant concentration levels (with 0.4 cmĝ'3 and 4.0 μg mĝ'3 in the wet vs. 1.2 cmĝ'3 and 6.5 μg mĝ'3 in the dry season) with rather weak seasonality (in terms of abundance and size spectrum), which is in stark contrast to the pronounced biomass burning-driven seasonality of the submicron aerosol population and related parameters. For most of the time, bioaerosol particles from the forest biome account for a major fraction of the coarse mode background population. However, from December to April there are episodic intrusions of African LRT aerosols, comprising Saharan dust, sea salt particles from the transatlantic passage, and African biomass burning smoke. Remarkably, during the core period of this LRT season (i.e., February-March), the presence of LRT influence, occurring as a sequence of pulse-like plumes, appears to be the norm rather than an exception. The LRT pulses increase the coarse mode concentrations drastically (up to 100 μg mĝ'3) and alter the coarse mode composition as well as its size spectrum. Efficient transport of the LRT plumes into the Amazon Basin takes place in response to specific mesoscale circulation patterns in combination with the episodic absence of rain-related aerosol scavenging en route. Based on a modeling study, we estimated a dust deposition flux of 5-10 kg haĝ'1 aĝ'1 in the region of the ATTO site. Furthermore, a chemical analysis quantified the substantial increase of crustal and sea salt elements under LRT conditions in comparison to the background coarse mode composition. With these results, we estimated the deposition fluxes of various elements that are considered as nutrients for the rain forest ecosystem. These estimates range from few g haĝ'1 aĝ'1 up to several hundreds of g haĝ'1 aĝ'1 in the ATTO region.The long-term data presented here provide a statistically solid basis for future studies of the manifold aspects of the dynamic coarse mode aerosol cycling in the Amazon. Thus, it may help to understand its biogeochemical relevance in this ecosystem as well as to evaluate to what extent anthropogenic influences have altered the coarse mode cycling already.