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- ItemDual-FOV Raman and Doppler lidar studies of aerosol-cloud interactions: Simultaneous profiling of aerosols, warm-cloud properties, and vertical wind(Hoboken, NJ : Wiley, 2014) Schmidt, Jörg; Ansmann, Albert; Bühl, Johannes; Baars, Holger; Wandinger, Ulla; Müller, Detlef; Malinka, Aleksey V.For the first time, colocated dual-field of view (dual-FOV) Raman lidar and Doppler lidar observations (case studies) of aerosol and cloud optical and microphysical properties below and within thin layered liquid water clouds are presented together with an updraft and downdraft characterization at cloud base. The goal of this work is to investigate the relationship between aerosol load close to cloud base and cloud characteristics of warm (purely liquid) clouds and the study of the influence of vertical motions and turbulent mixing on this relationship. We further use this opportunity to illustrate the applicability of the novel dual-FOV Raman lidar in this field of research. The dual-FOV lidar combines the well-established multiwavelength Raman lidar technique for aerosol retrievals and the multiple-scattering Raman lidar technique for profiling of the single-scattering extinction coefficient, effective radius, number concentration of the cloud droplets, and liquid water content. Key findings of our 3 year observations are presented in several case studies of optically thin altocumulus layers occurring in the lower free troposphere between 2.5 and 4 km height over Leipzig, Germany, during clean and polluted situations. For the clouds that we observed, the most direct link between aerosol proxy (particle extinction coefficient) and cloud proxy (cloud droplet number concentration) was found at cloud base during updraft periods. Above cloud base, additional processes resulting from turbulent mixing and entrainment of dry air make it difficult to determine the direct impact of aerosols on cloud processes.
- ItemCauses and importance of new particle formation in the present-day and preindustrial atmospheres(Hoboken, NJ : Wiley, 2017) Gordon, Hamish; Kirkby, Jasper; Baltensperger, Urs; Bianchi, Federico; Breitenlechner, Martin; Curtius, Joachim; Dias, Antonio; Dommen, Josef; Donahue, Neil M.; Dunne, Eimear M.; Duplissy, Jonathan; Ehrhart, Sebastian; Flagan, Richard C.; Frege, Carla; Fuchs, Claudia; Hansel, Armin; Hoyle, Christopher R.; Kulmala, Markku; Kürten, Andreas; Lehtipalo, Katrianne; Makhmutov, Vladimir; Molteni, Ugo; Rissanen, Matti P.; Stozkhov, Yuri; Tröstl, Jasmin; Tsagkogeorgas, Georgios; Wagner, Robert; Williamson, Christina; Wimmer, Daniela; Winkler, Paul M.; Yan, Chao; Carslaw, Ken S.New particle formation has been estimated to produce around half of cloud-forming particles in the present-day atmosphere, via gas-to-particle conversion. Here we assess the importance of new particle formation (NPF) for both the present-day and the preindustrial atmospheres. We use a global aerosol model with parametrizations of NPF from previously published CLOUD chamber experiments involving sulfuric acid, ammonia, organic molecules, and ions. We find that NPF produces around 67% of cloud condensation nuclei at 0.2% supersaturation (CCN0.2%) at the level of low clouds in the preindustrial atmosphere (estimated uncertainty range 45–84%) and 54% in the present day (estimated uncertainty range 38–66%). Concerning causes, we find that the importance of biogenic volatile organic compounds (BVOCs) in NPF and CCN formation is greater than previously thought. Removing BVOCs and hence all secondary organic aerosol from our model reduces low-cloud-level CCN concentrations at 0.2% supersaturation by 26% in the present-day atmosphere and 41% in the preindustrial. Around three quarters of this reduction is due to the tiny fraction of the oxidation products of BVOCs that have sufficiently low volatility to be involved in NPF and early growth. Furthermore, we estimate that 40% of preindustrial CCN0.2% are formed via ion-induced NPF, compared with 27% in the present day, although we caution that the ion-induced fraction of NPF involving BVOCs is poorly measured at present. Our model suggests that the effect of changes in cosmic ray intensity on CCN is small and unlikely to be comparable to the effect of large variations in natural primary aerosol emissions.
- ItemIce residual properties in mixed-phase clouds at the high-alpine Jungfraujoch site(Hoboken, NJ : Wiley, 2016) Kupiszewski, Piotr; Zanatta, Marco; Mertes, Stephan; Vochezer, Paul; Lloyd, Gary; Schneider, Johannes; Schenk, Ludwig; Schnaiter, Martin; Baltensperger, Urs; Weingartner, Ernest; Gysel, MartinIce residual (IR) and total aerosol properties were measured in mixed-phase clouds (MPCs) at the high-alpine Jungfraujoch research station. Black carbon (BC) content and coating thickness of BC-containing particles were determined using single-particle soot photometers. The ice activated fraction (IAF), derived from a comparison of IR and total aerosol particle size distributions, showed an enrichment of large particles in the IR, with an increase in the IAF from values on the order of 10−4 to 10−3 for 100 nm (diameter) particles to 0.2 to 0.3 for 1 μm (diameter) particles. Nonetheless, due to the high number fraction of submicrometer particles with respect to total particle number, IR size distributions were still dominated by the submicrometer aerosol. A comparison of simultaneously measured number size distributions of BC-free and BC-containing IR and total aerosol particles showed depletion of BC by number in the IR, suggesting that BC does not play a significant role in ice nucleation in MPCs at the Jungfraujoch. The potential anthropogenic climate impact of BC via the glaciation effect in MPCs is therefore likely to be negligible at this site and in environments with similar meteorological conditions and a similar aerosol population. The IAF of the BC-containing particles also increased with total particle size, in a similar manner as for the BC-free particles, but on a level 1 order of magnitude lower. Furthermore, BC-containing IR were found to have a thicker coating than the BC-containing total aerosol, suggesting the importance of atmospheric aging for ice nucleation.
- ItemRadiative effect of aerosols above the northern and southern Atlantic Ocean as determined from shipborne lidar observations(Hoboken, NJ : Wiley, 2013) Kanitz, T.; Ansmann, Albert; Seifert, P.; Engelmann, R.; Althausen, D.The direct solar radiative effect of aerosols over the Atlantic Ocean was investigated on the basis of aerosol Raman/polarization lidar observations aboard the research vessel Polarsternbetween Germany (50°N) and either South America (50°S) or South Africa (40°S) in 2009 and 2010. First, a case study of complex aerosol conditions with marine aerosol, dust, and smoke particles in the boundary layer and free troposphere is presented to demonstrate that detailed knowledge of aerosol layering (boundary layer, free troposphere) and aerosol mixing state is required for an accurate determination of the resulting radiative effects. A statistical analysis based on all lidar observations revealed the highest daily mean radiative effect (−43±59 W m−2at the surface, −14±18 W m−2at top of atmosphere) in the latitudinal belt from 0°N–15°N in the Saharan dust outflow region. Mean aerosol radiative effects of the polluted northern and clean southern midlatitudes were contrasted. In the northern midlatitudes, the averaged aerosol radiative effect of all simulations was −24±33 W m−2at the surface which is a factor of 1.6 higher than at similar southern hemispheric latitudes. The simulations based on the lidar observations are in good agreement with colocated pyranometer measurements.
- ItemIncreasing Resolution and Resolving Convection Improve the Simulation of Cloud-Radiative Effects Over the North Atlantic(Hoboken, NJ : Wiley, 2020) Senf, Fabian; Voigt, Aiko; Clerbaux, Nicolas; Hünerbein, Anja; Deneke, HartwigClouds interact with atmospheric radiation and substantially modify the Earth's energy budget. Cloud formation processes occur over a vast range of spatial and temporal scales, which make their thorough numerical representation challenging. Therefore, the impact of parameter choices for simulations of cloud-radiative effects is assessed in the current study. Numerical experiments are carried out using the ICOsahedral Nonhydrostatic (ICON) model with varying grid spacings between 2.5 and 80 km and with different subgrid-scale parameterization approaches. Simulations are performed over the North Atlantic with either one-moment or two-moment microphysics and with convection being parameterized or explicitly resolved by grid-scale dynamics. Simulated cloud-radiative effects are compared to products derived from Meteosat measurements. Furthermore, a sophisticated cloud classification algorithm is applied to understand the differences and dependencies of simulated and observed cloud-radiative effects. The cloud classification algorithm developed for the satellite observations is also applied to the simulation output based on synthetic infrared brightness temperatures, a novel approach that is not impacted by changing insolation and guarantees a consistent and fair comparison. It is found that flux biases originate equally from clear-sky and cloudy parts of the radiation field. Simulated cloud amounts and cloud-radiative effects are dominated by marine, shallow clouds, and their behavior is highly resolution dependent. Bias compensation between shortwave and longwave flux biases, seen in the coarser simulations, is significantly diminished for higher resolutions. Based on the analysis results, it is argued that cloud-microphysical and cloud-radiative properties have to be adjusted to further improve agreement with observed cloud-radiative effects. © 2020. The Authors.
- ItemHemispheric and Seasonal Contrast in Cloud Thermodynamic Phase From A‐Train Spaceborne Instruments(Hoboken, NJ : Wiley, 2021) Villanueva, Diego; Senf, Fabian; Tegen, InaAerosol-cloud interactions are an important source of uncertainty in current climate models. To understand and quantify the influence of ice-nucleating particles in cloud glaciation, it is crucial to have a reliable estimation of the hemispheric and seasonal contrast in cloud top phase, which is believed to result from the higher dust aerosol loading in boreal spring. For this reason, we locate and quantify these contrasts by combining three different A-Train cloud-phase products for the period 2007–2010. These products rely on a spaceborne lidar, a lidar-radar synergy, and a radiometer-polarimeter synergy. We show that the cloud-phase from the product combination is more reliable and that the estimation of the hemispheric and seasonal contrast has a lower error compared to the individual products. To quantify the contrast in cloud-phase, we use the hemispheric difference in ice cloud frequency normalized by the liquid cloud frequency in the southern hemisphere between −42 °C and 0 °C. In the midlatitudes, from −15 to −30 °C, the hemispheric contrasts increase with decreasing temperature. At −30 °C, the hemispheric contrast varies from 29% to 39% for the individual cloud-phase products and from 52% to 73% for the product combination. Similarly, in the northern hemisphere, we assess the seasonal contrast between spring and fall normalized by the liquid cloud frequency during fall. At −30 °C, the seasonal contrast ranges from 21% to 39% for the individual cloud-phase products and from 54% to 75% for the product combination.
- ItemSources, Occurrence and Characteristics of Fluorescent Biological Aerosol Particles Measured Over the Pristine Southern Ocean(Hoboken, NJ : Wiley, 2021) Moallemi, Alireza; Landwehr, Sebastian; Robinson, Charlotte; Simó, Rafel; Zamanillo, Marina; Chen, Gang; Baccarini, Andrea; Schnaiter, Martin; Henning, Silvia; Modini, Robin L.; Gysel-Beer, Martin; Schmale, JuliaIn this study, we investigate the occurrence of primary biological aerosol particles (PBAP) over all sectors of the Southern Ocean (SO) based on a 90-day data set collected during the Antarctic Circumnavigation Expedition (ACE) in austral summer 2016-2017. Super-micrometer PBAP (1-16 µm diameter) were measured by a wide band integrated bioaerosol sensor (WIBS-4). Low (3σ) and high (9σ) fluorescence thresholds are used to obtain statistics on fluorescent and hyper-fluorescent PBAP, respectively. Our focus is on data obtained over the pristine ocean, that is, more than 200 km away from land. The results indicate that (hyper-)fluorescent PBAP are correlated to atmospheric variables associated with sea spray aerosol (SSA) particles (wind speed, total super-micrometer aerosol number concentration, chloride and sodium concentrations). This suggests that a main source of PBAP over the SO is SSA. The median percentage contribution of fluorescent and hyper-fluorescent PBAP to super-micrometer SSA was 1.6% and 0.13%, respectively. We demonstrate that the fraction of (hyper-)fluorescent PBAP to total super-micrometer particles positively correlates with concentrations of bacteria and several taxa of pythoplankton measured in seawater, indicating that marine biota concentrations modulate the PBAP source flux. We investigate the fluorescent properties of (hyper-)fluorescent PBAP for several events that occurred near land masses. We find that the fluorescence signal characteristics of particles near land is much more variable than over the pristine ocean. We conclude that the source and concentration of fluorescent PBAP over the open ocean is similar across all sampled sectors of the SO.
- ItemFormation of Toxic Unsaturated Multifunctional and Organosulfur Compounds From the Photosensitized Processing of Fluorene and DMSO at the Air-Water Interface(Hoboken, NJ : Wiley, 2020) Mekic, Majda; Zeng, Jiafa; Jiang, Bin; Li, Xue; Lazarou, Yannis G.; Brigante, Marcello; Herrmann, Hartmut; Gligorovski, SashoPolycyclic aromatic hydrocarbons and dimethyl sulfoxide (DMSO) are ubiquitous at the sea surface. Photochemistry at the air-sea interface is a potentially important source of volatile organic compounds, but the relevant chemical processes are currently not well known. When aqueous solutions containing a mixture of fluorene (FL) and DMSO are irradiated with actinic radiation, a large suite of unsaturated high molecular weight compounds appear in the aqueous phase; a broad variety of saturated and unsaturated oxygenated multifunctional compounds are also observed in the gas phase, most of which are more toxic than FL. A possible sequence of steps leading to some of the observed compounds in aqueous solution as well as in the gas phase is proposed. The reaction pathways initiated by excited triplet state of FL (3FL*) are supported by theoretical calculations of the reaction Gibbs energies. The formation of organosulfur compounds has been observed to occur in the gas and the aqueous phases initiated by the reaction between 3FL* and DMSO. The aforementioned photosensitized chemistry at the water surface can have an important impact on the formation of secondary organic aerosol in marine boundary layer as polycyclic aromatic hydrocarbons and DMSO enriched at the water surface are ubiquitous. ©2020. American Geophysical Union. All Rights Reserved.
- ItemView angle dependence of MODIS liquid water path retrievals in warm oceanic clouds(Hoboken, NJ : Wiley, 2014) Horváth, Ákos; Seethala, Chellappan; Deneke, HartwigWe investigated the view angle dependence of domain mean Moderate Resolution Imaging Spectroradiometer (MODIS) liquid water path (LWP) and that of corresponding cloud optical thickness, effective radius, and liquid cloud fraction as proxy for plane-parallel retrieval biases. Independent Advanced Microwave Scanning Radiometer–EOS LWP was used to corroborate that the observed variations with sun-view geometry were not severely affected by seasonal/latitudinal changes in cloud properties. Microwave retrievals showed generally small (<10%) cross-swath variations. The view angle (cross-swath) dependence of MODIS optical thickness was weaker in backscatter than forward scatter directions and transitioned from mild ∩ shape to stronger ∪ shape as heterogeneity, sun angle, or latitude increased. The 2.2 µm effective radius variations always had a ∪ shape, which became pronounced and asymmetric toward forward scatter in the most heterogeneous clouds and/or at the lowest sun. Cloud fraction had the strongest and always ∪-shaped view angle dependence. As a result, in-cloud MODIS cloud liquid water path (CLWP) showed surprisingly good view angle (cross-swath) consistency, usually comparable to that of microwave retrievals, due to cancelation between optical thickness and effective radius biases. Larger (20–40%) nadir-relative increases were observed in the most extreme heterogeneity and sun angle bins, that is, typically in the polar regions, which, however, constituted only 3–8% of retrievals. The good consistency of MODIS in-cloud CLWP was lost for gridbox mean LWP, which was dominated by the strong cloud fraction increase with view angle. More worryingly, MODIS LWP exhibited significant and systematic absolute increases with heterogeneity and sun angle that is not present in microwave LWP.
- ItemImmersionmode ice nucleationmeasurements with the new Portable Immersion Mode Cooling chAmber (PIMCA)(Hoboken, NJ : Wiley, 2016) Kohn, Monika; Lohmann, Ulrike; Welti, André; Kanji, Zamin A.The new Portable Immersion Mode Cooling chAmber (PIMCA) has been developed for online immersion freezing of single-immersed aerosol particles. PIMCA is a vertical extension of the established Portable Ice Nucleation Chamber (PINC). PIMCA immerses aerosol particles into cloud droplets before they enter PINC. Immersion freezing experiments on cloud droplets with a radius of 5–7 μm at a prescribed supercooled temperature (T) and water saturation can be conducted, while other ice nucleation mechanisms (deposition, condensation, and contact mode) are excluded. Validation experiments on reference aerosol (kaolinite, ammonium sulfate, and ammonium nitrate) showed good agreement with theory and literature. The PIMCA-PINC setup was tested in the field during the Zurich AMBient Immersion freezing Study (ZAMBIS) in spring 2014 in Zurich, Switzerland. Significant concentrations of submicron ambient aerosol triggering immersion freezing at T > 236 K were rare. The mean frozen cloud droplet number concentration was estimated to be 7.22·105 L−1 for T < 238 K and determined from the measured frozen fraction and cloud condensation nuclei (CCN) concentrations predicted for the site at a typical supersaturation of SS = 0.3%. This value should be considered as an upper limit of cloud droplet freezing via immersion and homogeneous freezing processes. The predicted ice nucleating particle (INP) concentration based on measured total aerosol larger than 0.5 μm and the parameterization by DeMott et al. (2010) at T = 238 K is INPD10=54 ± 39 L−1. This is a lower limit as supermicron particles were not sampled with PIMCA-PINC during ZAMBIS.
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