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- ItemTerrestrial or marine – indications towards the origin of ice-nucleating particles during melt season in the European Arctic up to 83.7° N(Katlenburg-Lindau : European Geosciences Union, 2021) Hartmann, Markus; Gong, Xianda; Kecorius, Simonas; van Pinxteren, Manuela; Vogl, Teresa; Welti, André; Wex, Heike; Zeppenfeld, Sebastian; Herrmann, Hartmut; Wiedensohler, Alfred; Stratmann, FrankIce-nucleating particles (INPs) initiate the primary ice formation in clouds at temperatures above ca. -38gC and have an impact on precipitation formation, cloud optical properties, and cloud persistence. Despite their roles in both weather and climate, INPs are not well characterized, especially in remote regions such as the Arctic. We present results from a ship-based campaign to the European Arctic during May to July 2017. We deployed a filter sampler and a continuous-flow diffusion chamber for offline and online INP analyses, respectively. We also investigated the ice nucleation properties of samples from different environmental compartments, i.e., the sea surface microlayer (SML), the bulk seawater (BSW), and fog water. Concentrations of INPs (NINP) in the air vary between 2 to 3 orders of magnitudes at any particular temperature and are, except for the temperatures above -10gC and below -32gC, lower than in midlatitudes. In these temperature ranges, INP concentrations are the same or even higher than in the midlatitudes. By heating of the filter samples to 95gC for 1ĝ€¯h, we found a significant reduction in ice nucleation activity, i.e., indications that the INPs active at warmer temperatures are biogenic. At colder temperatures the INP population was likely dominated by mineral dust. The SML was found to be enriched in INPs compared to the BSW in almost all samples. The enrichment factor (EF) varied mostly between 1 and 10, but EFs as high as 94.97 were also observed. Filtration of the seawater samples with 0.2ĝ€¯μm syringe filters led to a significant reduction in ice activity, indicating the INPs are larger and/or are associated with particles larger than 0.2ĝ€¯μm. A closure study showed that aerosolization of SML and/or seawater alone cannot explain the observed airborne NINP unless significant enrichment of INP by a factor of 105 takes place during the transfer from the ocean surface to the atmosphere. In the fog water samples with -3.47gC, we observed the highest freezing onset of any sample. A closure study connecting NINP in fog water and the ambient NINP derived from the filter samples shows good agreement of the concentrations in both compartments, which indicates that INPs in the air are likely all activated into fog droplets during fog events. In a case study, we considered a situation during which the ship was located in the marginal sea ice zone and NINP levels in air and the SML were highest in the temperature range above -10gC. Chlorophyll a measurements by satellite remote sensing point towards the waters in the investigated region being biologically active. Similar slopes in the temperature spectra suggested a connection between the INP populations in the SML and the air. Air mass history had no influence on the observed airborne INP population. Therefore, we conclude that during the case study collected airborne INPs originated from a local biogenic probably marine source. © Author(s) 2021.
- ItemMeasuring the morphology and density of internally mixed black carbon with SP2 and VTDMA: New insight into the absorption enhancement of black carbon in the atmosphere(München : European Geopyhsical Union, 2016) Zhang, Yuxuan; Zhang, Qiang; Cheng, Yafang; Su, Hang; Kecorius, Simonas; Wang, Zhibin; Wu, Zhijun; Hu, Min; Zhu, Tong; Wiedensohler, Alfred; He, KebinThe morphology and density of black carbon (BC) cores in internally mixed BC (In-BC) particles affect their mixing state and absorption enhancement. In this work, we developed a new method to measure the morphology and effective density of the BC cores of ambient In-BC particles using a single-particle soot photometer (SP2) and a volatility tandem differential mobility analyzer (VTDMA) during the CAREBeijing-2013 campaign from 8 to 27 July 2013 at Xianghe Observatory. This new measurement system can select size-resolved ambient In-BC particles and measure the mobility diameter and mass of the In-BC cores. The morphology and effective density of the ambient In-BC cores are then calculated. For the In-BC cores in the atmosphere, changes in their dynamic shape factor (χ) and effective density (ρeff) can be characterized as a function of the aging process (Dp∕Dc) measured by SP2 and VTDMA. During an intensive field study, the ambient In-BC cores had an average shape factor χ of ∼ 1.2 and an average density of ∼ 1.2 g cm−3, indicating that ambient In-BC cores have a near-spherical shape with an internal void of ∼ 30 %. From the measured morphology and density, the average shell ∕ core ratio and absorption enhancement (Eab) of ambient BC were estimated to be 2.1–2.7 and 1.6–1.9, respectively, for In-BC particles with sizes of 200–350 nm. When the In-BC cores were assumed to have a void-free BC sphere with a density of 1.8 g cm−3, the shell ∕ core ratio and Eab were overestimated by ∼ 13 and ∼ 17 %, respectively. The new approach developed in this work improves the calculations of the mixing state and optical properties of ambient In-BC particles by quantifying the changes in the morphology and density of ambient In-BC cores during aging.
- ItemImportance of size representation and morphology in modelling optical properties of black carbon: comparison between laboratory measurements and model simulations(Katlenburg-Lindau : Copernicus, 2022) Romshoo, Baseerat; Pöhlker, Mira; Wiedensohler, Alfred; Pfeifer, Sascha; Saturno, Jorge; Nowak, Andreas; Ciupek, Krzysztof; Quincey, Paul; Vasilatou, Konstantina; Ess, Michaela N.; Gini, Maria; Eleftheriadis, Konstantinos; Robins, Chris; Gaie-Levrel, François; Müller, ThomasBlack carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles, which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parameterization schemes for the optical properties of BC, using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. The modelling techniques were examined for bare BC particles in the first step and for BC particles with organic material in the second step. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. In general, the aggregate representation performed well for modelling the particle light absorption coefficient σabs, single-scattering albedo SSA, and mass absorption cross-section MACBC for laboratory-generated BC particles with volume mean mobility diameters dp,V larger than 100nm. However, for modelling Ångström absorption exponent AAE, it was difficult to suggest a method due to size dependence, although the spherical assumption was in better agreement in some cases. The BC fractal aggregates are usually modelled using monodispersed particles, since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25% uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the uncertainty in measured σabs to 10% for particles with dp,V between 60-160nm. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. When the BC particle is small and rather fresh, the change in the Df had relatively little effect on the optical properties. There was, however, a significant relationship between app and the particle light scattering, which increased by a factor of up to 6 with increasing total particle size. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 and 2, mim between 0.50 and 1, Df from 1.7 to 1.9, and app between 10 and 14nm. Overall, this study provides experimental support for emphasizing the importance of an appropriate size representation (polydisperse size method) and an appropriate morphological representation for optical modelling and parameterization scheme development of BC.
- ItemHelicopter-borne observations of the continental background aerosol in combination with remote sensing and ground-based measurements(Katlenburg-Lindau : EGU, 2018) Düsing, Sebastian; Wehner, Birgit; Seifert, Patric; Ansmann, Albert; Baars, Holger; Ditas, Florian; Henning, Silvia; Ma, Nan; Poulain, Laurent; Siebert, Holger; Wiedensohler, Alfred; Macke, AndreasThis 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.
- 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.
- ItemAn optical particle size spectrometer for aircraft-borne measurements in IAGOS-CARIBIC(München : European Geopyhsical Union, 2016) Hermann, Markus; Weigelt, Andreas; Assmann, Denise; Pfeifer, Sascha; Müller, Thomas; Conrath, Thomas; Voigtländer, Jens; Heintzenberg, Jost; Wiedensohler, Alfred; Martinsson, Bengt G.; Deshler, Terry; Brenninkmeijer, Carl A.M.; Zahn, AndreasThe particle number size distribution is an important parameter to characterize the atmospheric aerosol and its influence on the Earth's climate. Here we describe a new optical particle size spectrometer (OPSS) for measurements of the accumulation mode particle number size distribution in the tropopause region on board a passenger aircraft (IAGOS-CARIBIC observatory: In-service Aircraft for a Global Observing System – Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container). A modified KS93 particle sensor from RION Co., Ltd., together with a new airflow system and a dedicated data acquisition system, is the key component of the CARIBIC OPSS. The instrument records individual particle pulse signal curves in the particle size range 130–1110 nm diameter (for a particle refractive index of 1.47-i0.006) together with a time stamp and thus allows the post-flight choice of the time resolution and the size distribution bin width. The CARIBIC OPSS has a 50 % particle detection diameter of 152 nm and a maximum asymptotic counting efficiency of 98 %. The instrument's measurement performance shows no pressure dependency and no particle coincidence for free tropospheric conditions. The size response function of the CARIBIC OPSS was obtained by a polystyrene latex calibration in combination with model calculations. Particle number size distributions measured with the new OPSS in the lowermost stratosphere agreed within a factor of 2 in concentration with balloon-borne measurements over western North America. Since June 2010 the CARIBIC OPSS is deployed once per month in the IAGOS-CARIBIC observatory.
- ItemMultidecadal trend analysis of in situ aerosol radiative properties around the world(Katlenburg-Lindau : EGU, 2020) Collaud Coen, Martine; Andrews, Elisabeth; Alastuey, Andrés; Petkov Arsov, Todor; Backman, John; Brem, Benjamin T.; Bukowiecki, Nicolas; Couret, Cédric; Eleftheriadis, Konstantinos; Flentje, Harald; Fiebig, Markus; Gysel-Beer, Martin; Hand, Jenny L.; Hoffer, András; Hooda, Rakesh; Hueglin, Christoph; Joubert, Warren; Keywood, Melita; Eun Kim, Jeong; Kim, Sang-Woo; Labuschagne, Casper; Lin, Neng-Huei; Lin, Yong; Lund Myhre, Cathrine; Luoma, Krista; Lyamani, Hassan; Marinoni, Angela; Mayol-Bracero, Olga L.; Mihalopoulos, Nikos; Pandolfi, Marco; Prats, Natalia; Prenni, Anthony J.; Putaud, Jean-Philippe; Ries, Ludwig; Reisen, Fabienne; Sellegri, Karine; Sharma, Sangeeta; Sheridan, Patrick; Sherman, James Patrick; Sun, Junying; Titos, Gloria; Torres, Elvis; Tuch, Thomas; Weller, Rolf; Wiedensohler, Alfred; Zieger, Paul; Laj, PaoloIn order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann-Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010-2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient - there is a shift to statistically significant negative trends in 2009-2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes. © 2020 Royal Society of Chemistry. All rights reserved.
- ItemProperties of cloud condensation nuclei (CCN) in the trade wind marine boundary layer of the western North Atlantic(München : European Geopyhsical Union, 2016) Kristensen, Thomas B.; Müller, Thomas; Kandler, Konrad; Benker, Nathalie; Hartmann, Markus; Prospero, Joseph M.; Wiedensohler, Alfred; Stratmann, FrankCloud optical properties in the trade winds over the eastern Caribbean Sea have been shown to be sensitive to cloud condensation nuclei (CCN) concentrations. The objective of the current study was to investigate the CCN properties in the marine boundary layer (MBL) in the tropical western North Atlantic, in order to assess the respective roles of inorganic sulfate, organic species, long-range transported mineral dust and sea-salt particles. Measurements were carried out in June–July 2013, on the east coast of Barbados, and included CCN number concentrations, particle number size distributions and offline analysis of sampled particulate matter (PM) and sampled accumulation mode particles for an investigation of composition and mixing state with transmission electron microscopy (TEM) in combination with energy-dispersive X-ray spectroscopy (EDX). During most of the campaign, significant mass concentrations of long-range transported mineral dust was present in the PM, and influence from local island sources can be ruled out. The CCN and particle number concentrations were similar to what can be expected in pristine marine environments. The hygroscopicity parameter κ was inferred, and values in the range 0.2–0.5 were found during most of the campaign, with similar values for the Aitken and the accumulation mode. The accumulation mode particles studied with TEM were dominated by non-refractory material, and concentrations of mineral dust, sea salt and soot were too small to influence the CCN properties. It is highly likely that the CCN were dominated by a mixture of sulfate species and organic compounds.