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- ItemVertical distribution of aerosol optical properties in the Po Valley during the 2012 summer campaigns(Katlenburg-Lindau : EGU, 2018) Bucci, Silvia; Cristofanelli, Paolo; Decesari, Stefano; Marinoni, Angela; Sandrini, Silvia; Größ, Johannes; Wiedensohler, Alfred; Di Marco, Chiara F.; Nemitz, Eiko; Cairo, Francesco; Di Liberto, Luca; Fierli, FedericoStudying the vertical distribution of aerosol particle physical and chemical properties in the troposphere is essential to understand the relative importance of local emission processes vs. long-range transport for column-integrated aerosol properties (e.g. the aerosol optical depth, AOD, affecting regional climate) as well as for the aerosol burden and its impacts on air quality at the ground. The main objective of this paper is to investigate the transport of desert dust in the middle troposphere and its intrusion into the planetary boundary layer (PBL) over the Po Valley (Italy), a region considered one of the greatest European pollution hotspots for the frequency that particulate matter (PM) limit values are exceeded. Events of mineral aerosol uplift from local (soil) sources and phenomena of hygroscopic growth at the ground are also investigated, possibly affecting the PM concentration in the region as well. During the PEGASOS 2012 field campaign, an integrated observing-modelling system was set up based on near-surface measurements (particle concentration and chemistry), vertical profiling (backscatter coefficient profiles from lidar and radiosoundings) and Lagrangian air mass transport simulations by FLEXPART model. Measurements were taken at the San Pietro Capofiume supersite (44°39′ĝ€N, 11°37′ĝ€E; 11ĝ€mĝ€a.s.l.), located in a rural area relatively close to some major urban and industrial emissive areas in the Po Valley. Mt. Cimone (44°12′ĝ€N, 10°42′ĝ€E; 2165ĝ€mĝ€a.s.l.) WMO/GAW station observations are also included in the study to characterize regional-scale variability. Results show that, in the Po Valley, aerosol is detected mainly below 2000ĝ€mĝ€a.s.l. with a prevalent occurrence of non-depolarizing particles ( > 50ĝ€% throughout the campaign) and a vertical distribution modulated by the PBL daily evolution. Two intense events of mineral dust transport from northern Africa (19-21 and 29 June to 2 July) are observed, with layers advected mainly above 2000ĝ€m, but subsequently sinking and mixing in the PBL. As a consequence, a non-negligible occurrence of mineral dust is observed close to the ground ( ĝ1/4 7ĝ€% of occurrence during a 1-month campaign). The observations unambiguously show Saharan dust layers intruding the Po Valley mixing layer and directly affecting the aerosol concentrations near the surface. Finally, lidar observations also indicate strong variability in aerosol on shorter timescales (hourly). Firstly, these highlight events of hygroscopic growth of anthropogenic aerosol, visible as shallow layers of low depolarization near the ground. Such events are identified during early morning hours at high relative humidity (RH) conditions (RHĝ€ > 80ĝ€%). The process is observed concurrently with high PM1 nitrate concentration (up to 15ĝ€μgĝ€cmĝ'3) and hence mainly explicable by deliquescence of fine anthropogenic particles, and during mineral dust intrusion episodes, when water condensation on dust particles could instead represent the dominant contribution. Secondly, lidar images show frequent events (mean daily occurrence of ĝ1/4 ĝ€22ĝ€% during the whole campaign) of rapid uplift of mineral depolarizing particles in afternoon-evening hours up to 2000ĝ€mĝ€a.s.l. height. The origin of such particles cannot be directly related to long-range transport events, being instead likely linked to processes of soil particle resuspension from agricultural lands.
- ItemThe efficiency of secondary organic aerosol particles acting as ice-nucleating particles under mixed-phase cloud conditions(Katlenburg-Lindau : EGU, 2018) Frey, Wiebke; Hu, Dawei; Dorsey, James; Alfarra, M. Rami; Pajunoja, Aki; Virtanen, Annele; Connolly, Paul; McFiggans, GordonSecondary organic aerosol (SOA) particles have been found to be efficient ice-nucleating particles under the cold conditions of (tropical) upper-tropospheric cirrus clouds. Whether they also are efficient at initiating freezing under slightly warmer conditions as found in mixed-phase clouds remains undetermined. Here, we study the ice-nucleating ability of photochemically produced SOA particles with the combination of the Manchester Aerosol Chamber and Manchester Ice Cloud Chamber. Three SOA systems were tested resembling biogenic and anthropogenic particles as well as particles of different phase state. These are namely α-pinene, heptadecane, and 1,3,5-trimethylbenzene. After the aerosol particles were formed, they were transferred into the cloud chamber, where subsequent quasi-adiabatic cloud activation experiments were performed. Additionally, the ice-forming abilities of ammonium sulfate and kaolinite were investigated as a reference to test the experimental setup.
Clouds were formed in the temperature range of −20 to −28.6 °C. Only the reference experiment using dust particles showed evidence of ice nucleation. No ice particles were observed in any other experiment. Thus, we conclude that SOA particles produced under the conditions of the reported experiments are not efficient ice-nucleating particles starting at liquid saturation under mixed-phase cloud conditions. - ItemPhase transition observations and discrimination of small cloud particles by light polarization in expansion chamber experiments(München : European Geopyhsical Union, 2016) Nichman, Leonid; Fuchs, Claudia; Järvinen, Emma; Ignatius, Karoliina; Höppel, Niko Florian; Dias, Antonio; Heinritzi, Martin; Simon, Mario; Tröstl, Jasmin; Wagner, Andrea Christine; Wagner, Robert; Williamson, Christina; Yan, Chao; Connolly, Paul James; Dorsey, James Robert; Duplissy, Jonathan; Ehrhart, Sebastian; Frege, Carla; Gordon, Hamish; Hoyle, Christopher Robert; Kristensen, Thomas Bjerring; Steiner, Gerhard; McPherson Donahue, Neil; Flagan, Richard; Gallagher, Martin William; Kirkby, Jasper; Möhler, Ottmar; Saathoff, Harald; Schnaiter, Martin; Stratmann, Frank; Tomé, AntónioCloud microphysical processes involving the ice phase in tropospheric clouds are among the major uncertainties in cloud formation, weather, and general circulation models. The detection of aerosol particles, liquid droplets, and ice crystals, especially in the small cloud particle-size range below 50 μm, remains challenging in mixed phase, often unstable environments. The Cloud Aerosol Spectrometer with Polarization (CASPOL) is an airborne instrument that has the ability to detect such small cloud particles and measure the variability in polarization state of their backscattered light. Here we operate the versatile Cosmics Leaving OUtdoor Droplets (CLOUD) chamber facility at the European Organization for Nuclear Research (CERN) to produce controlled mixed phase and other clouds by adiabatic expansions in an ultraclean environment, and use the CASPOL to discriminate between different aerosols, water, and ice particles. In this paper, optical property measurements of mixed-phase clouds and viscous secondary organic aerosol (SOA) are presented. We report observations of significant liquid–viscous SOA particle polarization transitions under dry conditions using CASPOL. Cluster analysis techniques were subsequently used to classify different types of particles according to their polarization ratios during phase transition. A classification map is presented for water droplets, organic aerosol (e.g., SOA and oxalic acid), crystalline substances such as ammonium sulfate, and volcanic ash. Finally, we discuss the benefits and limitations of this classification approach for atmospherically relevant concentrations and mixtures with respect to the CLOUD 8–9 campaigns and its potential contribution to tropical troposphere layer analysis.
- ItemVariations in tropospheric submicron particle size distributions across the European continent 2008-2009(München : European Geopyhsical Union, 2014) Beddows, D.C.S.; Dall'Osto, M.; Harrison, R.M.; Kulmala, M.; Asmi, A.; Wiedensohler, A.; Laj, P.; Fjaeraa, A.M.; Sellegri, K.; Birmili, W.; Bukowiecki, N.; Weingartner, E.; Baltensperger, U.; Zdimal, V.; Zikova, N.; Putaud, J.-P.; Marinoni, A.; Tunved, P.; Hansson, H.-C.; Fiebig, M.; Kivekäs, N.; Swietlicki, E.; Lihavainen, H.; Asmi, E.; Ulevicius, V.; Aalto, P.P.; Mihalopoulos, N.; Kalivitis, N.; Kalapov, I.; Kiss, G.; de Leeuw, G.; Henzing, B.; O'Dowd, C.; Jennings, S.G.; Flentje, H.; Meinhardt, F.; Ries, L.; Denier van der Gon, H.A.C.; Visschedijk, A.J.H.Cluster~analysis of particle number size distributions from~background sites across Europe~is presented. This generated a total of nine clusters of particle size distributions which could be further combined into two main groups, namely: a south-to-north category (four clusters) and a west-to-east category (five clusters). The first group was identified as most frequently being detected inside and around northern Germany and neighbouring countries, showing clear evidence of local afternoon nucleation and growth events that could be linked to movement of air masses from south to north arriving ultimately at the Arctic contributing to Arctic haze.~The second group of particle size spectra proved to have narrower size distributions and collectively showed a dependence of modal diameter upon the longitude of the site (west to east) at which they were most frequently detected.~These clusters indicated regional nucleation (at the coastal sites) growing to larger modes further inland. The apparent growth rate of the modal diameter was around 0.6–0.9 nm h−1. Four specific air mass back-trajectories were successively taken as case studies to examine in real time the evolution of aerosol size distributions across Europe. ~While aerosol growth processes can be observed as aerosol traverses Europe, the processes are often obscured by the addition of aerosol by emissions en route. This study revealed that some of the 24 stations exhibit more complex behaviour than others, especially when impacted by local sources or a variety of different air masses. Overall, the aerosol size distribution clustering analysis greatly simplifies the complex data set and allows a description of aerosol aging processes, which reflects the longer-term average development of particle number size distributions as air masses advect across Europe.
- ItemNear-global aerosol mapping in the upper troposphere and lowermost stratosphere with data from the CARIBIC project(Milton Park : Taylor & Francis, 2017) Heintzenberg, Jost; Hermann, Markus; Weigelt, Andreas; Kapustin, Vladimir; Anderson, Bruce; Thornhill, Kenneth; Van Velthoven, Peter; Zahn, Andreas; Brenninkmeijer, CarlThis study extrapolates aerosol data of the CARIBIC project from 1997 until June 2008 in along trajectories to compose large-scale maps and vertical profiles of submicrometre particle concentrations in the upper troposphere and lowermost stratosphere (UT/LMS). The extrapolation was validated by comparing extrapolated values with CARIBIC data measured near the respective trajectory position and by comparing extrapolated CARIBIC data to measurements by other experiments near the respective trajectory positions. Best agreement between extrapolated and measured data is achieved with particle lifetimes longer than the maximum length of used trajectories. The derived maps reveal regions of strong and frequent new particle formation, namely the Tropical Central and Western Africa with the adjacent Atlantic, South America, the Caribbean and Southeast Asia. These regions of particle formation coincide with those of frequent deep convective clouds. Vertical particle concentration profiles for the troposphere and the stratosphere confirm statistically previous results indicating frequent new particle formation in the tropopause region. There was no statistically significant increase in Aitken mode particle concentration between the first period of CARIBIC operation, 1997–2002, and the second period, 2004–2009. However, a significant increase in concentration occurred within the latter period when considering it in isolation.
- ItemAerosol particle number size distributions and particulate light absorption at the ZOTTO tall tower (Siberia), 2006–2009(München : European Geopyhsical Union, 2011) Heintzenberg, J.; Birmili, W.; Otto, R.; Andreae, M.O.; Mayer, J.-C.; Chi, X.; Panov, A.This paper analyses aerosol particle number size distributions, particulate absorption at 570 nm wavelength and carbon monoxide (CO) measured between September 2006 and January 2010 at heights of 50 and 300 m at the Zotino Tall Tower Facility (ZOTTO) in Siberia (60.8° N; 89.35° E). Average number, surface and volume concentrations are broadly comparable to former studies covering shorter observation periods. Fits of multiple lognormal distributions yielded three maxima in probability distribution of geometric mean diameters in the Aitken and accumulation size range and a possible secondary maximum in the nucleation size range below 25 nm. The seasonal cycle of particulate absorption shows maximum concentrations in high winter (December) and minimum concentrations in mid-summer (July). The 90th percentile, however, indicates a secondary maximum in July/August that is likely related to forest fires. The strongly combustion derived CO shows a single winter maximum and a late summer minimum, albeit with a considerably smaller seasonal swing than the particle data due to its longer atmospheric lifetime. Total volume and even more so total number show a more complex seasonal variation with maxima in winter, spring, and summer. A cluster analysis of back trajectories and vertical profiles of the pseudo-potential temperature yielded ten clusters with three levels of particle number concentration: Low concentrations in Arctic air masses (400–500 cm−3), mid-level concentrations for zonally advected air masses from westerly directions between 55° and 65° N (600–800 cm−3), and high concentrations for air masses advected from the belt of industrial and population centers in Siberia and Kazakhstan (1200 cm−3). The observational data is representative for large parts of the troposphere over Siberia and might be particularly useful for the validation of global aerosol transport models.
- ItemProfiling 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, MikaWe 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.
- ItemParticulate sulfur in the upper troposphere and lowermost stratosphere - Sources and climate forcing(Katlenburg-Lindau : EGU, 2017) Martinsson, Bengt G.; Friberg, Johan; Sandvik, Oscar S.; Hermann, Markus; van Velthoven, Peter F. J.; Zahn, AndreasThis study is based on fine-mode aerosol samples collected in the upper troposphere (UT) and the lowermost stratosphere (LMS) of the Northern Hemisphere extratropics during monthly intercontinental flights at 8.8-12 km altitude of the IAGOS-CARIBIC platform in the time period 1999-2014. The samples were analyzed for a large number of chemical elements using the accelerator-based methods PIXE (particle-induced X-ray emission) and PESA (particle elastic scattering analysis). Here the particulate sulfur concentrations, obtained by PIXE analysis, are investigated. In addition, the satellite-borne lidar aboard CALIPSO is used to study the stratospheric aerosol load. A steep gradient in particulate sulfur concentration extends several kilometers into the LMS, as a result of increasing dilution towards the tropopause of stratospheric, particulate sulfur-rich air. The stratospheric air is diluted with tropospheric air, forming the extratropical transition layer (ExTL). Observed concentrations are related to the distance to the dynamical tropopause. A linear regression methodology handled seasonal variation and impact from volcanism. This was used to convert each data point into stand-alone estimates of a concentration profile and column concentration of particulate sulfur in a 3 km altitude band above the tropopause. We find distinct responses to volcanic eruptions, and that this layer in the LMS has a significant contribution to the stratospheric aerosol optical depth and thus to its radiative forcing. Further, the origin of UT particulate sulfur shows strong seasonal variation. We find that tropospheric sources dominate during the fall as a result of downward transport of the Asian tropopause aerosol layer (ATAL) formed in the Asian monsoon, whereas transport down from the Junge layer is the main source of UT particulate sulfur in the first half of the year. In this latter part of the year, the stratosphere is the clearly dominating source of particulate sulfur in the UT during times of volcanic influence and under background conditions.
- ItemThe impact of aerosol hygroscopic growth on the single-scattering albedo and its application on the NO2 photolysis rate coefficient(München : European Geopyhsical Union, 2014) Tao, J.C.; Zhao, C.S.; Ma, N.; Liu, P.F.Hygroscopic growth of aerosol particles can significantly affect their single-scattering albedo (ω), and consequently alters the aerosol effect on tropospheric photochemistry. In this study, the impact of aerosol hygroscopic growth on ω and its application to the NO2 photolysis rate coefficient (JNO2) are investigated for a typical aerosol particle population in the North China Plain (NCP). The variations of aerosol optical properties with relative humidity (RH) are calculated using a Mie theory aerosol optical model, on the basis of field measurements of number–size distribution and hygroscopic growth factor (at RH values above 90%) from the 2009 HaChi (Haze in China) project. Results demonstrate that ambient ω has pronouncedly different diurnal patterns from ω measured at dry state, and is highly sensitive to the ambient RHs. Ambient ω in the NCP can be described by a dry state ω value of 0.863, increasing with the RH following a characteristic RH dependence curve. A Monte Carlo simulation shows that the uncertainty of ω from the propagation of uncertainties in the input parameters decreases from 0.03 (at dry state) to 0.015 (RHs > 90%). The impact of hygroscopic growth on ω is further applied in the calculation of the radiative transfer process. Hygroscopic growth of the studied aerosol particle population generally inhibits the photolysis of NO2 at the ground level, whereas accelerates it above the moist planetary boundary layer. Compared with dry state, the calculated JNO2 at RH of 98% at the height of 1 km increases by 30.4%, because of the enhancement of ultraviolet radiation by the humidified scattering-dominant aerosol particles. The increase of JNO2 due to the aerosol hygroscopic growth above the upper boundary layer may affect the tropospheric photochemical processes and this needs to be taken into account in the atmospheric chemical models.
- ItemInertia gravity waves in the upper troposphere during the MaCWAVE winter campaign - Part I: Observations with collocated radars(München : European Geopyhsical Union, 2006) Hoffmann, P.; Serafimovich, A.; Peters, D.; Dalin, P.; Goldberg, R.; Latteck, R.During the {MaCWAVE} campaign, combined rocket, radiosonde and ground-based measurements have been performed at the Norwegian Andøya Rocket Range (ARR) near Andenes and the Swedish Rocket Range (ESRANGE) near Kiruna in January 2003 to study gravity waves in the vicinity of the Scandinavian mountain ridge. The investigations presented here are mainly based on the evaluation of continuous radar measurements with the ALWIN VHF radar in the upper troposphere/ lower stratosphere at Andenes (69.3° N, 16.0° E) and the ESRAD VHF radar near Kiruna (67.9° N, 21.9° E). Both radars are separated by about 260 km. Based on wavelet transformations of both data sets, the strongest activity of inertia gravity waves in the upper troposphere has been detected during the first period from 24–26 January 2003 with dominant vertical wavelengths of about 4–5 km as well as with dominant observed periods of about 13–14 h for the altitude range between 5 and 8 km under the additional influence of mountain waves. The results show the appearance of dominating inertia gravity waves with characteristic horizontal wavelengths of ~200 km moving in the opposite direction than the mean background wind. The results show the appearance of dominating inertia gravity waves with intrinsic periods in the order of ~5 h and with horizontal wavelengths of 200 km, moving in the opposite direction than the mean background wind. From the derived downward energy propagation it is supposed, that these waves are likely generated by a jet streak in the upper troposphere. The parameters of the jet-induced gravity waves have been estimated at both sites separately. The identified gravity waves are coherent at both locations and show higher amplitudes on the east-side of the Scandinavian mountain ridge, as expected by the influence of mountains.