Search Results
Terrestrial or marine – indications towards the origin of ice-nucleating particles during melt season in the European Arctic up to 83.7° N
2021, Hartmann, Markus, Gong, Xianda, Kecorius, Simonas, van Pinxteren, Manuela, Vogl, Teresa, Welti, André, Wex, Heike, Zeppenfeld, Sebastian, Herrmann, Hartmut, Wiedensohler, Alfred, Stratmann, Frank
Ice-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.
Aerosol dynamics and dispersion of radioactive particles
2021, Schoenberg, Pontus von, Tunved, Peter, Grahn, Håkan, Wiedensohler, Alfred, Krejci, Radovan, Brännström, Niklas
In the event of a failure of a nuclear power plant with release of radioactive material into the atmosphere, dispersion modelling is used to understand how the released radioactivity is spread. For the dispersion of particles, Lagrangian particle dispersion models (LPDMs) are commonly used, in which model particles, representing the released material, are transported through the atmosphere. These model particles are usually inert and undergo only first-order processes such as dry deposition and simplified wet deposition along the path through the atmosphere. Aerosol dynamic processes including coagulation, condensational growth, chemical interactions, formation of new particles and interaction with new aerosol sources are usually neglected in such models. The objective of this study is to analyse the impact of these advanced aerosol dynamic processes if they were to be included in LPDM simulations for use in radioactive preparedness. In this investigation, a fictitious failure of a nuclear power plant is studied for three geographically and atmospherically different sites. The incident was simulated with a Lagrangian single-trajectory box model with a new simulation for each hour throughout a year to capture seasonal variability of meteorology and variation in the ambient aerosol. (a) We conclude that modelling of wet deposition by incorporating an advanced cloud parameterization is advisable, since it significantly influence simulated levels of airborne and deposited activity including radioactive hotspots, and (b) we show that inclusion of detailed ambient-aerosol dynamics can play a large role in the model result in simulations that adopt a more detailed representation of aerosol–cloud interactions. The results highlight a potential necessity for implementation of more detailed representation of general aerosol dynamic processes into LPDMs in order to cover the full range of possible environmental characteristics that can apply during a release of radionuclides into the atmosphere.
Variability in the mass absorption cross section of black carbon (BC) aerosols is driven by BC internal mixing state at a central European background site (Melpitz, Germany) in winter
2021, Yuan, Jinfeng, Modini, Robin Lewis, Zanatta, Marco, Herber, Andreas B., Müller, Thomas, Wehner, Birgit, Poulain, Laurent, Tuch, Thomas, Baltensperger, Urs, Gysel-Beer, Martin
Properties of atmospheric black carbon (BC) particles were characterized during a field experiment at a rural background site (Melpitz, Germany) in February 2017. BC absorption at a wavelength of 870 nm was measured by a photoacoustic extinctiometer, and BC physical properties (BC mass concentration, core size distribution and coating thickness) were measured by a single-particle soot photometer (SP2). Additionally, a catalytic stripper was used to intermittently remove BC coatings by alternating between ambient and thermo-denuded conditions. From these data the mass absorption cross section of BC (MACBC) and its enhancement factor (EMAC) were inferred for essentially waterfree aerosol as present after drying to low relative humidity (RH). Two methods were applied independently to investigate the coating effect on EMAC: A correlation method (MACBC; ambient vs. BC coating thickness) and a denuding method (MACBC; ambient vs. MACBC; denuded). Observed EMAC values varied from 1.0 to 1.6 (lower limit from denuding method) or 1:2 to 1.9 (higher limit from correlation method), with the mean coating volume fraction ranging from 54% to 78% in the dominating mass equivalent BC core diameter range of 200?220 nm.MACBC and EMAC were strongly correlated with coating thickness of BC. By contrast, other potential drivers of EMAC variability, such as different BC sources (air mass origin and absorption Angström exponent), coating composition (ratio of inorganics to organics) and BC core size distribution, had only minor effects. These results for ambient BC measured at Melpitz during winter show that the lensing effect caused by coatings on BC is the main driver of the variations in MACBC and EMAC, while changes in other BC particle properties such as source, BC core size or coating composition play only minor roles at this rural background site with a large fraction of aged particles. Indirect evidence suggests that potential dampening of the lensing effect due to unfavorable morphology was most likely small or even negligible.
Aerosol activation characteristics and prediction at the central European ACTRIS research station of Melpitz, Germany
2022, Wang, Yuan, Henning, Silvia, Poulain, Laurent, Lu, Chunsong, Stratmann, Frank, Wang, Yuying, Niu, Shengjie, Pöhlker, Mira L., Herrmann, Hartmut, Wiedensohler, Alfred
Understanding aerosol particle activation is essential for evaluating aerosol indirect effects (AIEs) on climate. Long-term measurements of aerosol particle activation help to understand the AIEs and narrow down the uncertainties of AIEs simulation. However, they are still scarce. In this study, more than 4 years of comprehensive aerosol measurements were utilized at the central European research station of Melpitz, Germany, to gain insight into the aerosol particle activation and provide recommendations on improving the prediction of number concentration of cloud condensation nuclei (CCN, NCCN). (1) The overall CCN activation characteristics at Melpitz are provided. As supersaturation (SS) increases from 0.1% to 0.7%, the median NCCN increases from 399 to 2144cm-3, which represents 10% to 48% of the total particle number concentration with a diameter range of 10-800nm, while the median hygroscopicity factor (κ) and critical diameter (Dc) decrease from 0.27 to 0.19 and from 176 to 54nm, respectively. (2) Aerosol particle activation is highly variable across seasons, especially at low-SS conditions. At SSCombining double low line0.1%, the median NCCN and activation ratio (AR) in winter are 1.6 and 2.3 times higher than the summer values, respectively. (3) Both κ and the mixing state are size-dependent. As the particle diameter (Dp) increases, κ increases at Dp of 1/440 to 100nm and almost stays constant at Dp of 100 to 200nm, whereas the degree of the external mixture keeps decreasing at Dp of 1/440 to 200nm. The relationships of κ vs. Dp and degree of mixing vs. Dp were both fitted well by a power-law function. (4) Size-resolved κ improves the NCCN prediction. We recommend applying the κ-Dp power-law fit for NCCN prediction at Melpitz, which performs better than using the constant κ of 0.3 and the κ derived from particle chemical compositions and much better than using the NCCN (AR) vs. SS relationships. The κ-Dp power-law fit measured at Melpitz could be applied to predict NCCN for other rural regions. For the purpose of improving the prediction of NCCN, long-term monodisperse CCN measurements are still needed to obtain the κ-Dp relationships for different regions and their seasonal variations.
Contrasting ice formation in Arctic clouds: surface-coupled vs. surface-decoupled clouds
2021, Griesche, Hannes J., Ohneiser, Kevin, Seifert, Patric, Radenz, Martin, Engelmann, Ronny, Ansmann, Albert
In the Arctic summer of 2017 (1 June to 16 July) measurements with the OCEANET-Atmosphere facility were performed during the Polarstern cruise PS106. OCEANET comprises amongst other instruments the multiwavelength polarization lidar PollyXT_OCEANET and for PS106 was complemented with a vertically pointed 35 GHz cloud radar. In the scope of the presented study, the influence of cloud height and surface coupling on the probability of clouds to contain and form ice is investigated. Polarimetric lidar data were used for the detection of the cloud base and the identification of the thermodynamic phase. Both radar and lidar were used to detect cloud top. Radiosonde data were used to derive the thermodynamic structure of the atmosphere and the clouds. The analyzed data set shows a significant impact of the surface-coupling state on the probability of ice formation. Surface-coupled clouds were identified by a quasi-constant potential temperature profile from the surface up to liquid layer base. Within the same minimum cloud temperature range, ice-containing clouds have been observed more frequently than surface-decoupled clouds by a factor of up to 6 (temperature intervals between -7.5 and -5 C, 164 vs. 27 analyzed intervals of 30 min). The frequency of occurrence of surface-coupled ice-containing clouds was found to be 2-3 times higher (e.g., 82% vs. 35% between -7.5 and -5 C). These findings provide evidence that above -10 C heterogeneous ice formation in Arctic mixed-phase clouds occurs by a factor of 2-6 more often when the cloud layer is coupled to the surface. In turn, for minimum cloud temperatures below -15 C, the frequency of ice-containing clouds for coupled and decoupled conditions approached the respective curve for the central European site of Leipzig, Germany (51 N, 12 E). This corroborates the hypothesis that the free-tropospheric ice nucleating particle (INP) reservoir over the Arctic is controlled by continental aerosol. Two sensitivity studies, also using the cloud radar for detection of ice particles and applying a modified coupling state detection, both confirmed the findings, albeit with a lower magnitude. Possible explanations for the observations are discussed by considering recent in situ measurements of INP in the Arctic, of which much higher concentrations were found in the surface-coupled atmosphere in close vicinity to the ice shore.