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- ItemNear-surface profiles of aerosol number concentration and temperature over the Arctic Ocean(München : European Geopyhsical Union, 2011) Held, A.; Orsini, D.A.; Vaattovaara, P.; Tjernström, M.; Leck, C.Temperature and particle number concentration profiles were measured at small height intervals above open and frozen leads and snow surfaces in the central Arctic. The device used was a gradient pole designed to investigate potential particle sources over the central Arctic Ocean. The collected data were fitted according to basic logarithmic flux-profile relationships to calculate the sensible heat flux and particle deposition velocity. Independent measurements by the eddy covariance technique were conducted at the same location. General agreement was observed between the two methods when logarithmic profiles could be fitted to the gradient pole data. In general, snow surfaces behaved as weak particle sinks with a maximum deposition velocity vd = 1.3 mm s−1 measured with the gradient pole. The lead surface behaved as a weak particle source before freeze-up with an upward flux Fc = 5.7 × 104 particles m−2 s−1, and as a relatively strong heat source after freeze-up, with an upward maximum sensible heat flux H = 13.1 W m−2. Over the frozen lead, however, we were unable to resolve any significant aerosol profiles.
- ItemHomogeneous and heterogeneous ice nucleation at LACIS: Operating principle and theoretical studies(München : European Geopyhsical Union, 2011) Hartmann, S.; Niedermeier, D.; Voigtländer, J.; Clauss, T.; Shaw, R.A.; Wex, H.; Kiselev, A.; Stratmann, F.At the Leipzig Aerosol Cloud Interaction Simulator (LACIS) experiments investigating homogeneous and heterogeneous nucleation of ice (particularly immersion freezing in the latter case) have been carried out. Here both the physical LACIS setup and the numerical model developed to design experiments at LACIS and interpret their results are presented in detail. Combining results from the numerical model with experimental data, it was found that for the experimental parameter space considered, classical homogeneous ice nucleation theory is able to predict the freezing behavior of highly diluted ammonium sulfate solution droplets, while classical heterogeneous ice nucleation theory, together with the assumption of a constant contact angle, fails to predict the immersion freezing behavior of surrogate mineral dust particles (Arizona Test Dust, ATD). The main reason for this failure is the compared to experimental data apparently overly strong temperature dependence of the nucleation rate coefficient. Assuming, in the numerical model, Classical Nucleation Theory (CNT) for homogeneous ice nucleation and a CNT-based parameterization for the nucleation rate coefficient in the immersion freezing mode, recently published by our group, it was found that even for a relatively effective ice nucleating agent such as pure ATD, there is a temperature range where homogeneous ice nucleation is dominant. The main explanation is the apparently different temperature dependencies of the two freezing mechanisms. Finally, reviewing the assumptions made during the derivation of the CNT-based parameterization for immersion freezing, it was found that the assumption of constant temperature during ice nucleation and the chosen ice nucleation time were justified, underlining the applicability of the method to determine the fitting coefficients in the parameterization equation.
- ItemExperimental study of the role of physicochemical surface processing on the IN ability of mineral dust particles(München : European Geopyhsical Union, 2011) Niedermeier, D.; Hartmann, S.; Clauss, T.; Wex, H.; Kiselev, A.; Sullivan, R.C.; DeMott, P.J.; Petters, M.D.; Reitz, P.; Schneider, J.; Mikhailov, E.; Sierau, B.; Stetzer, O.; Reimann, B.; Bundke, U.; Shaw, R.A.; Buchholz, A.; Mentel, T.F.; Stratmann, F.During the measurement campaign FROST 2 (FReezing Of duST 2), the Leipzig Aerosol Cloud Interaction Simulator (LACIS) was used to investigate the influence of various surface modifications on the ice nucleating ability of Arizona Test Dust (ATD) particles in the immersion freezing mode. The dust particles were exposed to sulfuric acid vapor, to water vapor with and without the addition of ammonia gas, and heat using a thermodenuder operating at 250 °C. Size selected, quasi monodisperse particles with a mobility diameter of 300 nm were fed into LACIS and droplets grew on these particles such that each droplet contained a single particle. Temperature dependent frozen fractions of these droplets were determined in a temperature range between −40 °C ≤T≤−28 °C. The pure ATD particles nucleated ice over a broad temperature range with their freezing behavior being separated into two freezing branches characterized through different slopes in the frozen fraction vs. temperature curves. Coating the ATD particles with sulfuric acid resulted in the particles' IN potential significantly decreasing in the first freezing branch (T>−35 °C) and a slight increase in the second branch (T≤−35 °C). The addition of water vapor after the sulfuric acid coating caused the disappearance of the first freezing branch and a strong reduction of the IN ability in the second freezing branch. The presence of ammonia gas during water vapor exposure had a negligible effect on the particles' IN ability compared to the effect of water vapor. Heating in the thermodenuder led to a decreased IN ability of the sulfuric acid coated particles for both branches but the additional heat did not or only slightly change the IN ability of the pure ATD and the water vapor exposed sulfuric acid coated particles. In other words, the combination of both sulfuric acid and water vapor being present is a main cause for the ice active surface features of the ATD particles being destroyed. A possible explanation could be the chemical transformation of ice active metal silicates to metal sulfates. The strongly enhanced reaction between sulfuric acid and dust in the presence of water vapor and the resulting significant reductions in IN potential are of importance for atmospheric ice cloud formation. Our findings suggest that the IN concentration can decrease by up to one order of magnitude for the conditions investigated.
- ItemOn the formation of sulphuric acid – Amine clusters in varying atmospheric conditions and its influence on atmospheric new particle formation(München : European Geopyhsical Union, 2012) Paasonen, P.; Olenius, T.; Kupiainen, O.; Kurtén, T.; Petäjä, T.; Birmili, W.; Hamed, A.; Hu, M.; Huey, L.G.; Plass-Duelmer, C.; Smith, J.N.; Wiedensohler, A.; Loukonen, V.; McGrath, M.J.; Ortega, I.K.; Laaksonen, A.; Vehkamäki, H.; Kerminen, V.-M.; Kulmala, M.Sulphuric acid is a key component in atmospheric new particle formation. However, sulphuric acid alone does not form stable enough clusters to initiate particle formation in atmospheric conditions. Strong bases, such as amines, have been suggested to stabilize sulphuric acid clusters and thus participate in particle formation. We modelled the formation rate of clusters with two sulphuric acid and two amine molecules (JA2B2) at varying atmospherically relevant conditions with respect to concentrations of sulphuric acid ([H2SO4]), dimethylamine ([DMA]) and trimethylamine ([TMA]), temperature and relative humidity (RH). We also tested how the model results change if we assume that the clusters with two sulphuric acid and two amine molecules would act as seeds for heterogeneous nucleation of organic vapours (other than amines) with higher atmospheric concentrations than sulphuric acid. The modelled formation rates JA2B2 were functions of sulphuric acid concentration with close to quadratic dependence, which is in good agreement with atmospheric observations of the connection between the particle formation rate and sulphuric acid concentration. The coefficients KA2B2 connecting the cluster formation rate and sulphuric acid concentrations as JA2B2=KA2B2[H2SO4]2 turned out to depend also on amine concentrations, temperature and relative humidity. We compared the modelled coefficients KA2B2 with the corresponding coefficients calculated from the atmospheric observations (Kobs) from environments with varying temperatures and levels of anthropogenic influence. By taking into account the modelled behaviour of JA2B2 as a function of [H2SO4], temperature and RH, the atmospheric particle formation rate was reproduced more closely than with the traditional semi-empirical formulae based on sulphuric acid concentration only. The formation rates of clusters with two sulphuric acid and two amine molecules with different amine compositions (DMA or TMA or one of both) had different responses to varying meteorological conditions and concentrations of vapours participating in particle formation. The observed inverse proportionality of the coefficient Kobs with RH and temperature agreed best with the modelled coefficient KA2B2 related to formation of a cluster with two H2SO4 and one or two TMA molecules, assuming that these clusters can grow in collisions with abundant organic vapour molecules. In case this assumption is valid, our results suggest that the formation rate of clusters with at least two of both sulphuric acid and amine molecules might be the rate-limiting step for atmospheric particle formation. More generally, our analysis elucidates the sensitivity of the atmospheric particle formation rate to meteorological variables and concentrations of vapours participating in particle formation (also other than H2SO4).
- ItemAtmospheric boundary layer top height in South Africa: Measurements with lidar and radiosonde compared to three atmospheric models(München : European Geopyhsical Union, 2014) Korhonen, K.; Giannakaki, E.; Mielonen, T.; Pfüller, A.; Laakso, L.; Vakkari, V.; Baars, H.; Engelmann, R.; Beukes, J.P.; Van Zyl, P.G.; Ramandh, A.; Ntsangwane, L.; Josipovic, M.; Tiitta, P.; Fourie, G.; Ngwana, I.; Chiloane, K.; Komppula, M.Atmospheric lidar measurements were carried out at Elandsfontein measurement station, on the eastern Highveld approximately 150 km east of Johannesburg in South Africa throughout 2010. The height of the planetary boundary layer (PBL) top was continuously measured using a Raman lidar, PollyXT (POrtabLe Lidar sYstem eXTended). High atmospheric variability together with a large surface temperature range and significant seasonal changes in precipitation were observed, which had an impact on the vertical mixing of particulate matter, and hence, on the PBL evolution. The results were compared to radiosondes, CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) space-borne lidar measurements and three atmospheric models that followed different approaches to determine the PBL top height. These models included two weather forecast models operated by ECMWF (European Centre for Medium-range Weather Forecasts) and SAWS (South African Weather Service), and one mesoscale prognostic meteorological and air pollution regulatory model TAPM (The Air Pollution Model). The ground-based lidar used in this study was operational for 4935 h during 2010 (49% of the time). The PBL top height was detected 86% of the total measurement time (42% of the total time). Large seasonal and diurnal variations were observed between the different methods utilised. High variation was found when lidar measurements were compared to radiosonde measurements. This could be partially due to the distance between the lidar measurements and the radiosondes, which were 120 km apart. Comparison of lidar measurements to the models indicated that the ECMWF model agreed the best with mean relative difference of 15.4%, while the second best correlation was with the SAWS model with corresponding difference of 20.1%. TAPM was found to have a tendency to underestimate the PBL top height. The wind speeds in the SAWS and TAPM models were strongly underestimated which probably led to underestimation of the vertical wind and turbulence and thus underestimation of the PBL top height. Comparison between ground-based and satellite lidar shows good agreement with a correlation coefficient of 0.88. On average, the daily maximum PBL top height in October (spring) and June (winter) was 2260 m and 1480 m, respectively. To our knowledge, this study is the first long-term study of PBL top heights and PBL growth rates in South Africa.
- ItemAerosol decadal trends - Part 2: In-situ aerosol particle number concentrations at GAW and ACTRIS stations(München : European Geopyhsical Union, 2013) Asmi, A.; Collaud Coen, M.; Ogren, J.A.; Andrews, E.; Sheridan, P.; Jefferson, A.; Weingartner, E.; Baltensperger, U.; Bukowiecki, N.; Lihavainen, H.; Kivekäs, N.; Asmi, E.; Aalto, P.P.; Kulmala, M.; Wiedensohler, A.; Birmili, W.; Hamed, A.; O'Dowd, C.; Jennings, S.G.; Weller, R.; Flentje, H.; Fjaeraa, A.M.; Fiebig, M.; Myhre, C.L.; Hallar, A.G.; Swietlicki, E.; Kristensson, A.; Laj, P.We have analysed the trends of total aerosol particle number concentrations (N) measured at long-term measurement stations involved either in the Global Atmosphere Watch (GAW) and/or EU infrastructure project ACTRIS. The sites are located in Europe, North America, Antarctica, and on Pacific Ocean islands. The majority of the sites showed clear decreasing trends both in the full-length time series, and in the intra-site comparison period of 2001–2010, especially during the winter months. Several potential driving processes for the observed trends were studied, and even though there are some similarities between N trends and air temperature changes, the most likely cause of many northern hemisphere trends was found to be decreases in the anthropogenic emissions of primary particles, SO2 or some co-emitted species. We could not find a consistent agreement between the trends of N and particle optical properties in the few stations with long time series of all of these properties. The trends of N and the proxies for cloud condensation nuclei (CCN) were generally consistent in the few European stations where the measurements were available. This work provides a useful comparison analysis for modelling studies of trends in aerosol number concentrations.
- ItemExperimental investigation of ion-ion recombination under atmospheric conditions(München : European Geopyhsical Union, 2015) Franchin, A.; Ehrhart, S.; Leppä, J.; Nieminen, T.; Gagné, S.; Schobesberger, S.; Wimmer, D.; Duplissy, J.; Riccobono, F.; Dunne, E.M.; Rondo, L.; Downard, A.; Bianchi, F.; Kupc, A.; Tsagkogeorgas, G.; Lehtipalo, K.; Manninen, H.E.; Almeida, J.; Amorim, A.; Wagner, P.E.; Hansel, A.; Kirkby, J.; Le Rille, O.; Kürten, A.; Donahue, N.M.; Makhmutov, V.; Mathot, S.; Metzger, A.; Petäjä, T.; Schnitzhofer, R.; Sipilä, M.; Stozhkov, Y.; Tomé, A.; Kerminen, V.-M.; Carslaw, K.; Curtius, J.; Baltensperger, U.; Kulmala, M.We present the results of laboratory measurements of the ion–ion recombination coefficient at different temperatures, relative humidities and concentrations of ozone and sulfur dioxide. The experiments were carried out using the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at CERN, the walls of which are made of conductive material, making it possible to measure small ions. We produced ions in the chamber using a 3.5 GeV c−1 beam of positively charged pions (π+) generated by the CERN Proton Synchrotron (PS). When the PS was switched off, galactic cosmic rays were the only ionization source in the chamber. The range of the ion production rate varied from 2 to 100 cm−3 s−1, covering the typical range of ionization throughout the troposphere. The temperature ranged from −55 to 20 °C, the relative humidity (RH) from 0 to 70 %, the SO2 concentration from 0 to 40 ppb, and the ozone concentration from 200 to 700 ppb. The best agreement of the retrieved ion–ion recombination coefficient with the commonly used literature value of 1.6 × 10−6 cm3 s−1 was found at a temperature of 5 °C and a RH of 40 % (1.5 ± 0.6) × 10−6 cm3 s−1. At 20 °C and 40 % RH, the retrieved ion–ion recombination coefficient was instead (2.3 ± 0.7) × 10−6 cm3 s−1. We observed no dependency of the ion–ion recombination coefficient on ozone concentration and a weak variation with sulfur dioxide concentration. However, we observed a more than fourfold increase in the ion–ion recombination coefficient with decreasing temperature. We compared our results with three different models and found an overall agreement for temperatures above 0 °C, but a disagreement at lower temperatures. We observed a strong increase in the recombination coefficient for decreasing relative humidities, which has not been reported previously.
- ItemPolar middle atmosphere temperature climatology from Rayleigh lidar measurements at ALOMAR (69° N)(München : European Geopyhsical Union, 2008) Schöch, A.; Baumgarten, G.; Fiedler, J.Rayleigh lidar temperature profiles have been derived in the polar middle atmosphere from 834 measurements with the ALOMAR Rayleigh/Mie/Raman lidar (69.3° N, 16.0° E) in the years 1997–2005. Since our instrument is able to operate under full daylight conditions, the unique data set presented here extends over the entire year and covers the altitude region 30 km–85 km in winter and 30 km–65 km in summer. Comparisons of our lidar data set to reference atmospheres and ECMWF analyses show agreement within a few Kelvin in summer but in winter higher temperatures below 55 km and lower temperatures above by as much as 25 K, due likely to superior resolution of stratospheric warming and associated mesospheric cooling events. We also present a temperature climatology for the entire lower and middle atmosphere at 69° N obtained from a combination of lidar measurements, falling sphere measurements and ECMWF analyses. Day to day temperature variability in the lidar data is found to be largest in winter and smallest in summer.
- ItemSmall-scale structures in neutrals and charged aerosol particles as observed during the ECOMA/MASS rocket campaign(München : European Geopyhsical Union, 2009) Strelnikov, B.; Rapp, M.; Strelnikova, I.; Engler, N.; Latteck, R.We present results of in situ measurements of neutral temperature during the ECOMA/MASS rocket campaign. We present and compare results of turbulence measurements conducted simultaneously by both in situ and doppler radar techniques. We show that the derived values of the turbulence energy dissipation rates are similar on average. We also find a region with a near adiabatic lapse rate with turbulence detected at the upper and lower edge. We note that it is consistent with expectation for a Kelvin-Helmholtz instability. We also present an estimate of the Schmidt numbers, Sc, for the charged aerosols that utilizes in situ measured small-scale density fluctuations of charged aerosols and both in situ and radar turbulence measurements. The derived Schmidt numbers fall within the range between 100 and 4500. This result agrees with previous estimates based on multi-frequency observations of PMSE (Rapp et al., 2008) and also with estimates of microphysical parameters presented in the companion paper by Rapp et al. (2009).
- ItemValidation of the Atmospheric Chemistry Experiment (ACE) version 2.2 temperature using ground-based and space-borne measurements(München : European Geopyhsical Union, 2008) Sica, R.J.; Izawa, M.R.M.; Walker, K.A.; Boone, C.; Petelina, S.V.; Argall, P.S.; Bernath, P.; Burns, G.B.; Catoire, V.; Collins, R.L.; Daffer, W.H.; De Clercq, C.; Fan, Z.Y.; Firanski, B.J.; French, W.J.R.; Gerard, P.; Gerding, M.; Granville, J.; Innis, J.L.; Keckhut, P.; Kerzenmacher, T.; Klekociuk, A.R.; Kyrö, E.; Lambert, J.C.; Llewellyn, E.J.; Manney, G.L.; McDermid, I.S.; Mizutani, K.; Murayama, Y.; Piccolo, C.; Raspollini, P.; Ridolfi, M.; Robert, C.; Steinbrecht, W.; Strawbridge, K.B.; Strong, K.; Stübi, R.; Thurairajah, B.An ensemble of space-borne and ground-based instruments has been used to evaluate the quality of the version 2.2 temperature retrievals from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). The agreement of ACE-FTS temperatures with other sensors is typically better than 2 K in the stratosphere and upper troposphere and 5 K in the lower mesosphere. There is evidence of a systematic high bias (roughly 3–6 K) in the ACE-FTS temperatures in the mesosphere, and a possible systematic low bias (roughly 2 K) in ACE-FTS temperatures near 23 km. Some ACE-FTS temperature profiles exhibit unphysical oscillations, a problem fixed in preliminary comparisons with temperatures derived using the next version of the ACE-FTS retrieval software. Though these relatively large oscillations in temperature can be on the order of 10 K in the mesosphere, retrieved volume mixing ratio profiles typically vary by less than a percent or so. Statistical comparisons suggest these oscillations occur in about 10% of the retrieved profiles. Analysis from a set of coincident lidar measurements suggests that the random error in ACE-FTS version 2.2 temperatures has a lower limit of about ±2 K.