Search Results
Results and recommendations from an intercomparison of six Hygroscopicity-TDMA systems
2011, Massling, A., Niedermeier, N., Hennig, T., Fors, E.O., Swietlicki, E., Ehn, M., Hämeri, K., Villani, P., Laj, P., Good, N., McFiggans, G., Wiedensohler, A.
The performance of six custom-built Hygrocopicity-Tandem Differential Mobility Analyser (H-TDMA) systems was investigated in the frame of an international calibration and intercomparison workshop held in Leipzig, February 2006. The goal of the workshop was to harmonise H-TDMA measurements and develop recommendations for atmospheric measurements and their data evaluation. The H-TDMA systems were compared in terms of the sizing of dry particles, relative humidity (RH) uncertainty, and consistency in determination of number fractions of different hygroscopic particle groups. The experiments were performed in an air-conditioned laboratory using ammonium sulphate particles or an external mixture of ammonium sulphate and soot particles. The sizing of dry particles of the six H-TDMA systems was within 0.2 to 4.2% of the selected particle diameter depending on investigated size and individual system. Measurements of ammonium sulphate aerosol found deviations equivalent to 4.5% RH from the set point of 90% RH compared to results from previous experiments in the literature. Evaluation of the number fraction of particles within the clearly separated growth factor modes of a laboratory generated externally mixed aerosol was done. The data from the H-TDMAs was analysed with a single fitting routine to investigate differences caused by the different data evaluation procedures used for each H-TDMA. The differences between the H-TDMAs were reduced from +12/−13% to +8/−6% when the same analysis routine was applied. We conclude that a common data evaluation procedure to determine number fractions of externally mixed aerosols will improve the comparability of H-TDMA measurements. It is recommended to ensure proper calibration of all flow, temperature and RH sensors in the systems. It is most important to thermally insulate the aerosol humidification unit and the second DMA and to monitor these temperatures to an accuracy of 0.2 °C. For the correct determination of external mixtures, it is necessary to take into account size-dependent losses due to diffusion in the plumbing between the DMAs and in the aerosol humidification unit.
Radiative budget and cloud radiative effect over the Atlantic from ship-based observations
2012, Kalisch, J., Macke, A.
The aim of this study is to determine cloud-type resolved cloud radiative budgets and cloud radiative effects from surface measurements of broadband radiative fluxes over the Atlantic Ocean. Furthermore, based on simultaneous observations of the state of the cloudy atmosphere, a radiative closure study has been performed by means of the ECHAM5 single column model in order to identify the model's ability to realistically reproduce the effects of clouds on the climate system. An extensive database of radiative and atmospheric measurements has been established along five meridional cruises of the German research icebreaker Polarstern. Besides pyranometer and pyrgeometer for downward broadband solar and thermal radiative fluxes, a sky imager and a microwave radiometer have been utilized to determine cloud fraction and cloud type on the one hand and temperature and humidity profiles as well as liquid water path for warm non-precipitating clouds on the other hand. Averaged over all cruise tracks, we obtain a total net (solar + thermal) radiative flux of 144 W m−2 that is dominated by the solar component. In general, the solar contribution is large for cirrus clouds and small for stratus clouds. No significant meridional dependencies were found for the surface radiation budgets and cloud effects. The strongest surface longwave cloud effects were shown in the presence of low level clouds. Clouds with a high optical density induce strong negative solar radiative effects under high solar altitudes. The mean surface net cloud radiative effect is −33 W m−2. For the purpose of quickly estimating the mean surface longwave, shortwave and net cloud effects in moderate, subtropical and tropical climate regimes, a new parameterisation was created, considering the total cloud amount and the solar zenith angle. The ECHAM5 single column model provides a surface net cloud effect that is more cooling by 17 W m−2 compared to the radiation observations. This overestimation in solar cooling is mostly caused by the shortwave impact of convective clouds. The latter show a large overestimation in solar cooling of up to 114 W m−2. Mean cloud radiative effects of cirrus and stratus clouds were simulated close to the observations.
Measurements of gaseous H2SO4 by AP-ID-CIMS during CAREBeijing 2008 Campaign
2011, Zheng, J., Hu, M., Zhang, R., Yue, D., Wang, Z., Guo, S., Li, X., Bohn, B., Shao, M., He, L., Huang, X., Wiedensohler, A., Zhu, T.
As part of the 2008 Campaign of Air Quality Research in Beijing and Surrounding Regions (CAREBeijing 2008), measurements of gaseous sulfuric acid (H2SO4) have been conducted at an urban site in Beijing, China from 7 July to 25 September 2008 using atmospheric pressure ion drift – chemical ionization mass spectrometry (AP-ID-CIMS). This represents the first gaseous H2SO4 measurements in China. Diurnal profile of sulfuric acid is strongly dependent on the actinic flux, reaching a daily maximum around noontime and with an hourly average concentration of 5 × 106 molecules cm−3. Simulation of sulfuric acid on the basis of the measured sulfur dioxide concentration, photolysis rates of ozone and nitrogen dioxide, and aerosol surface areas captures the trend of the measured H2SO4 diurnal variation within the uncertainties, indicating that photochemical production and condensation onto preexisting particle surface dominate the observed diurnal H2SO4 profile. The frequency of the peak H2SO4 concentration exceeding 5 × 106 molecules cm−3 increases by 16 % during the period of the summer Olympic Games (8–24 August 2008), because of the implementation of air quality control regulations. Using a multivariate statistical method, the critical nucleus during nucleation events is inferred, containing two H2SO4 molecules (R2 = 0.85). The calculated condensation rate of H2SO4 can only account for 10–25 % of PM1 sulfate formation, indicating that either much stronger sulfate production exists at the SO2 source region or other sulfate production mechanisms are responsible for the sulfate production.
Heterogeneous ice nucleation: Exploring the transition from stochastic to singular freezing behavior
2011, Niedermeier, D., Shaw, R.A., Hartmann, S., Wex, H., Clauss, T., Voigtländer, J., Stratmann, F.
Heterogeneous ice nucleation, a primary pathway for ice formation in the atmosphere, has been described alternately as being stochastic, in direct analogy with homogeneous nucleation, or singular, with ice nuclei initiating freezing at deterministic temperatures. We present an idealized, conceptual model to explore the transition between stochastic and singular ice nucleation. This "soccer ball" model treats particles as being covered with surface sites (patches of finite area) characterized by different nucleation barriers, but with each surface site following the stochastic nature of ice embryo formation. The model provides a phenomenological explanation for seemingly contradictory experimental results obtained in our research groups. Even with ice nucleation treated fundamentally as a stochastic process this process can be masked by the heterogeneity of surface properties, as might be typical for realistic atmospheric particle populations. Full evaluation of the model findings will require experiments with well characterized ice nucleating particles and the ability to vary both temperature and waiting time for freezing.
Design and performance of a three-wavelength LED-based total scatter and backscatter integrating nephelometer
2011, Müller, T., Laborde, M., Kassell, G., Wiedensohler, A.
Integrating nephelometers are instruments that directly measure a value close to the light scattering coefficient of airborne particles. Different models of nephelometers have been used for decades for monitoring and research applications. Now, a series of nephelometers (Ecotech models M9003, Aurora 1000 and Aurora 3000) with newly designed light sources based on light emitting diodes are available. This article reports on the design of these integrating nephelometers and a comparison of the Aurora 3000 to another commercial instrument (TSI model 3563) that uses an incandescent lamp. Both instruments are three-wavelength, total and backscatter integrating nephelometers. We present a characterization of the new light source design of the Aurora 3000 and provide parameterizations for its angular sensitivity functions. These parameterizations facilitate to correct for measurement artefacts using Mie-theory. Furthermore, correction factors are provided as a function of the Ångström exponent. Comparison measurements against the TSI 3563 with laboratory generated white particles and ambient air are also shown and discussed. Both instruments agree well within the calibration uncertainties and detection limit for total scattering with differences less than 5 %. Differences for backscattering are higher by up to 11 %. Highest differences were found for the longest wavelengths, where the signal to noise ratio is lowest. Differences at the blue and green wavelengths are less than 4 % and 3 %, respectively, for both total and backscattering.
Chemical composition and mixing-state of ice residuals sampled within mixed phase clouds
2011, Ebert, M., Worringen, A., Benker, N., Mertes, S., Weingartner, E., Weinbruch, S.
During an intensive campaign at the high alpine research station Jungfraujoch, Switzerland, in February/March 2006 ice particle residuals within mixed-phase clouds were sampled using the Ice-counterflow virtual impactor (Ice-CVI). Size, morphology, chemical composition, mineralogy and mixing state of the ice residual and the interstitial (i.e., non-activated) aerosol particles were analyzed by scanning and transmission electron microscopy. Ice nuclei (IN) were identified from the significant enrichment of particle groups in the ice residual (IR) samples relative to the interstitial aerosol. In terms of number lead-bearing particles are enriched by a factor of approximately 25, complex internal mixtures with silicates or metal oxides as major components by a factor of 11, and mixtures of secondary aerosol and carbonaceous material (C-O-S particles) by a factor of 2. Other particle groups (sulfates, sea salt, Ca-rich particles, external silicates) observed in the ice-residual samples cannot be assigned unambiguously as IN. Between 9 and 24% of all IR are Pb-bearing particles. Pb was found as major component in around 10% of these particles (PbO, PbCl2). In the other particles, Pb was found as some 100 nm sized agglomerates consisting of 3–8 nm sized primary particles (PbS, elemental Pb). C-O-S particles are present in the IR at an abundance of 17–27%. The soot component within these particles is strongly aged. Complex internal mixtures occur in the IR at an abundance of 9–15%. Most IN identified at the Jungfraujoch station are internal mixtures containing anthropogenic components (either as main or minor constituent), and it is concluded that admixture of the anthropogenic component is responsible for the increased IN efficiency within mixed phase clouds. The mixing state appears to be a key parameter for the ice nucleation behaviour that cannot be predicted from the sole knowledge of the main component of an individual particle.
Number size distributions and seasonality of submicron particles in Europe 2008–2009
2011, Asmi, A., Wiedensohler, A., Laj, P., Fjaeraa, A.-M., Sellegri, K., Birmili, W., Weingartner, E., Baltensperger, U., Zdimal, V., Zikova, N., Putaud, J.-P., Marinoni, A., Tunved, P., Hansson, H.-C., Fiebig, M., Kivekäs, N., Lihavainen, H., Asmi, E., Ulevicius, V., Aalto, P.P., Swietlicki, E., Kristensson, A., Mihalopoulos, N., Kalivitis, N., Kalapov, I., Kiss, G., de Leeuw, G., Henzing, B., Harrison, R.M., Beddows, D., O'Dowd, C., Jennings, S.G., Flentje, H., Weinhold, K., Meinhardt, F., Ries, L., Kulmala, M.
Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000 m a.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, and very low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional coverage of these results. Aerosol number concentrations over the Britain and Ireland had very high variance and there are indications of mixed air masses from several source regions; the Mediterranean aerosol exhibit high seasonality, and a strong accumulation mode in the summer. The greatest concentrations were observed at the Ispra station in Northern Italy with high accumulation mode number concentrations in the winter. The aerosol number concentrations at the Arctic station Zeppelin in Ny-\AA lesund in Svalbard have also a strong seasonal cycle, with greater concentrations of accumulation mode particles in winter, and dominating summer Aitken mode indicating more recently formed particles. Observed particles did not show any statistically significant regional work-week or weekday related variation in number concentrations studied. Analysis products are made for open-access to the research community, available in a freely accessible internet site. The results give to the modelling community a reliable, easy-to-use and freely available comparison dataset of aerosol size distributions.
Near-surface profiles of aerosol number concentration and temperature over the Arctic Ocean
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.
Homogeneous and heterogeneous ice nucleation at LACIS: Operating principle and theoretical studies
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.
Surface modification of mineral dust particles by sulphuric acid processing: Implications for ice nucleation abilities
2011, Reitz, P., Spindler, C., Mentel, T.F., Poulain, L., Wex, H., Mildenberger, K., Niedermeier, D., Hartmann, S., Clauss, T., Stratmann, F., Sullivan, R.C., DeMott, P.J., Petters, M.D., Sierau, B., Schneider, J.
The ability of coated mineral dust particles to act as ice nuclei (IN) was investigated at LACIS (Leipzig Aerosol Cloud Interaction Simulator) during the FROST1- and FROST2-campaigns (Freezing of dust). Sulphuric acid was condensed on the particles which afterwards were optionally humidified, treated with ammonia vapour and/or heat. By means of aerosol mass spectrometry we found evidence that processing of mineral dust particles with sulphuric acid leads to surface modifications of the particles. These surface modifications are most likely responsible for the observed reduction of the IN activation of the particles. The observed particle mass spectra suggest that different treatments lead to different chemical reactions on the particle surface. Possible chemical reaction pathways and products are suggested and the implications on the IN efficiency of the treated dust particles are discussed.