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- ItemPhotocurrent modelling and experimental confirmation for meteoric smoke particle detectors on board atmospheric sounding rockets(Katlenburg-Lindau : Copernicus, 2018-9-20) Giono, Gabriel; Strelnikov, Boris; Asmus, Heiner; Staszak, Tristan; Ivchenko, Nickolay; LĂ¼bken, Franz-JosefCharacterising the photoelectron current induced by the Sun's UV radiation is crucial to ensure accurate daylight measurements from particle detectors. This article lays out the methodology used to address this problem in the case of the meteoric smoke particle detectors (MSPDs), developed by the Leibniz Institute of Atmospheric Physics in KĂ¼hlungsborn (IAP) and flown on board the PMWEs (Polar Mesosphere Winter Echoes) sounding rockets in April 2018. The methodology focuses on two complementary aspects: modelling and experimental measurements. A detailed model of the MSPD photocurrent was created based on the expected solar UV flux, the atmospheric UV absorption as a function of height by molecular oxygen and ozone, the photoelectric yield of the material coating the MSPD as a function of wavelength, the index of refraction of these materials as a function of wavelength and the angle of incidence of the illumination onto the MSPD. Due to its complex structure, composed of a central electrode shielded by two concentric grids, extensive ray-tracing calculations were conducted to obtain the incidence angles of the illumination on the central electrode, and this was done for various orientations of the MSPD in respect to the Sun. Results of the modelled photocurrent at different heights and for different materials, as well as for different orientations of the detector, are presented. As a pre-flight confirmation, the model was used to reproduce the experimental measurements conducted by Robertson et al. (2014) and agrees within an order of magnitude. An experimental setup for the calibration of the MSPD photocurrent is also presented. The photocurrent induced by the Lyman-alpha line from a deuterium lamp was recorded inside a vacuum chamber using a narrowband filter, while a UV-sensitive photodiode was used to monitor the UV flux. These measurements were compared with the model prediction, and also matched within an order of magnitude. Although precisely modelling the photocurrent is a challenging task, this article quantitatively improved the understanding of the photocurrent on the MSPD and discusses possible strategies to untangle the meteoric smoke particles (MSPs) current from the photocurrent recorded in-flight.
- ItemIce-nucleating particle concentrations unaffected by urban air pollution in Beijing, China(Katlenburg-Lindau : EGU, 2018) Chen, Jie; Wu, Zhijun; Augustin-Bauditz, Stefanie; Grawe, Sarah; Hartmann, Markus; Pei, Xiangyu; Liu, Zirui; Ji, Dongsheng; Wex, HeikeExceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated whether anthropogenic PM2.5 may significantly contribute to ice-nucleating particles (INP). However, few studies have focused on the ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the atmospheric number concentration of INP (NINP) in the range from -6 to -25 °C in Beijing. No correlations between NINP and either PM2.5 or black carbon mass concentrations were found, although both varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between NINP and either total particle number concentration or number concentrations for particles with diameters > 500 nm. Furthermore, there was no clear difference between day and night samples. All these results indicate that Beijing air pollution did not increase or decrease INP concentrations in the examined temperature range above values observed in nonurban areas; hence, the background INP concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined temperature range.
- ItemAssessment of lidar depolarization uncertainty by means of a polarimetric lidar simulator(MĂ¼nchen : European Geopyhsical Union, 2016) Bravo-Aranda, Juan Antonio; Belegante, Livio; Freudenthaler, Volker; Alados-Arboledas, Lucas; Nicolae, Doina; Granados-Muñoz, MarĂa JosĂ©; Guerrero-Rascado, Juan Luis; Amodeo, Aldo; D'Amico, Giusseppe; Engelmann, Ronny; Pappalardo, Gelsomina; Kokkalis, Panos; Mamouri, Rodanthy; Papayannis, Alex; Navas-GuzmĂ¡n, Francisco; Olmo, Francisco JosĂ©; Wandinger, Ulla; Amato, Francesco; Haeffelin, MartialLidar depolarization measurements distinguish between spherical and non-spherical aerosol particles based on the change of the polarization state between the emitted and received signal. The particle shape information in combination with other aerosol optical properties allows the characterization of different aerosol types and the retrieval of aerosol particle microphysical properties. Regarding the microphysical inversions, the lidar depolarization technique is becoming a key method since particle shape information can be used by algorithms based on spheres and spheroids, optimizing the retrieval procedure. Thus, the identification of the depolarization error sources and the quantification of their effects are crucial. This work presents a new tool to assess the systematic error of the volume linear depolarization ratio (δ), combining the Stokes–MĂ¼ller formalism and the complete sampling of the error space using the lidar model presented in Freudenthaler (2016a). This tool is applied to a synthetic lidar system and to several EARLINET lidars with depolarization capabilities at 355 or 532 nm. The lidar systems show relative errors of δ larger than 100 % for δ values around molecular linear depolarization ratios (∼ 0.004 and up to ∼  10 % for δ = 0.45). However, one system shows only relative errors of 25 and 0.22 % for δ = 0.004 and δ = 0.45, respectively, and gives an example of how a proper identification and reduction of the main error sources can drastically reduce the systematic errors of δ. In this regard, we provide some indications of how to reduce the systematic errors.
- ItemEARLINET: Potential operationality of a research network(MĂ¼nchen : European Geopyhsical Union, 2015) Sicard, M.; D'Amico, G.; ComerĂ³n, A.; Mona, L.; Alados-Arboledas, L.; Amodeo, A.; Baars, H.; Baldasano, J.M.; Belegante, L.; Binietoglou, I.; Bravo-Aranda, J.A.; FernĂ¡ndez, A.J.; FrĂ©ville, P.; GarcĂa-VizcaĂno, D.; Giunta, A.; Granados-Muñoz, M.J.; Guerrero-Rascado, J.L.; Hadjimitsis, D.; Haefele, A.; Hervo, M.; Iarlori, M.; Kokkalis, P.; Lange, D.; Mamouri, R.E.; Mattis, I.; Molero, F.; Montoux, N.; Muñoz, A.; Muñoz Porcar, C.; Navas-GuzmĂ¡n, F.; Nicolae, D.; Nisantzi, A.; Papagiannopoulos, N.; Papayannis, A.; Pereira, S.; PreiĂŸler, J.; Pujadas, M.; Rizi, V.; Rocadenbosch, F.; Sellegri, K.; Simeonov, V.; Tsaknakis, G.; Wagner, F.; Pappalardo, G.In the framework of ACTRIS (Aerosols, Clouds, and Trace Gases Research Infrastructure Network) summer 2012 measurement campaign (8 June–17 July 2012), EARLINET organized and performed a controlled exercise of feasibility to demonstrate its potential to perform operational, coordinated measurements and deliver products in near-real time. Eleven lidar stations participated in the exercise which started on 9 July 2012 at 06:00 UT and ended 72 h later on 12 July at 06:00 UT. For the first time, the single calculus chain (SCC) – the common calculus chain developed within EARLINET for the automatic evaluation of lidar data from raw signals up to the final products – was used. All stations sent in real-time measurements of a 1 h duration to the SCC server in a predefined netcdf file format. The pre-processing of the data was performed in real time by the SCC, while the optical processing was performed in near-real time after the exercise ended. 98 and 79 % of the files sent to SCC were successfully pre-processed and processed, respectively. Those percentages are quite large taking into account that no cloud screening was performed on the lidar data. The paper draws present and future SCC users' attention to the most critical parameters of the SCC product configuration and their possible optimal value but also to the limitations inherent to the raw data. The continuous use of SCC direct and derived products in heterogeneous conditions is used to demonstrate two potential applications of EARLINET infrastructure: the monitoring of a Saharan dust intrusion event and the evaluation of two dust transport models. The efforts made to define the measurements protocol and to configure properly the SCC pave the way for applying this protocol for specific applications such as the monitoring of special events, atmospheric modeling, climate research and calibration/validation activities of spaceborne observations.
- ItemNew particle formation and its effect on cloud condensation nuclei abundance in the summer Arctic: A case study in the Fram Strait and Barents Sea(Katlenburg-Lindau : EGU, 2019) Kecorius, Simonas; Vogl, Teresa; Paasonen, Pauli; Lampilahti, Janne; Rothenberg, Daniel; Wex, Heike; Zeppenfeld, Sebastian; van Pinxteren, Manuela; Hartmann, Markus; Henning, Silvia; Gong, Xianda; Welti, Andre; Kulmala, Markku; Stratmann, Frank; Herrmann, Hartmut; Wiedensohler, AlfredIn a warming Arctic the increased occurrence of new particle formation (NPF) is believed to originate from the declining ice coverage during summertime. Understanding the physico-chemical properties of newly formed particles, as well as mechanisms that control both particle formation and growth in this pristine environment, is important for interpreting aerosol-cloud interactions, to which the Arctic climate can be highly sensitive. In this investigation, we present the analysis of NPF and growth in the high summer Arctic. The measurements were made on-board research vessel Polarstern during the PS106 Arctic expedition. Four distinctive NPF and subsequent particle growth events were observed, during which particle (diameter in a range 10-50 nm) number concentrations increased from background values of approx. 40 up to 4000 cm-3. Based on particle formation and growth rates, as well as hygroscopicity of nucleation and the Aitken mode particles, we distinguished two different types of NPF events. First, some NPF events were favored by negative ions, resulting in more-hygroscopic nucleation mode particles and suggesting sulfuric acid as a precursor gas. Second, other NPF events resulted in less-hygroscopic particles, indicating the influence of organic vapors on particle formation and growth. To test the climatic relevance of NPF and its influence on the cloud condensation nuclei (CCN) budget in the Arctic, we applied a zero-dimensional, adiabatic cloud parcel model. At an updraft velocity of 0.1 m s-1, the particle number size distribution (PNSD) generated during nucleation processes resulted in an increase in the CCN number concentration by a factor of 2 to 5 compared to the background CCN concentrations. This result was confirmed by the directly measured CCN number concentrations. Although particles did not grow beyond 50 nm in diameter and the activated fraction of 15-50 nm particles was on average below 10 %, it could be shown that the sheer number of particles produced by the nucleation process is enough to significantly influence the background CCN number concentration. This implies that NPF can be an important source of CCN in the Arctic. However, more studies should be conducted in the future to understand mechanisms of NPF, sources of precursor gases and condensable vapors, as well as the role of the aged nucleation mode particles in Arctic cloud formation. © Author(s) 2019. This work is distributed under the Creative Commons Attribution 4.0 License.
- ItemAnnual variability of ice-nucleating particle concentrations at different Arctic locations(Göttingen : Copernicus GmbH, 2019) Wex, H.; Huang, L.; Zhang, W.; Hung, H.; Traversi, R.; Becagli, S.; Sheesley, R.J.; Moffett, C.E.; Barrett, T.E.; Bossi, R.; Skov, H.; HĂ¼nerbein, A.; Lubitz, J.; Löffler, M.; Linke, O.; Hartmann, M.; Herenz, P.; Stratmann, F.Number concentrations of ice-nucleating particles (NINP) in the Arctic were derived from ground-based filter samples. Examined samples had been collected in Alert (Nunavut, northern Canadian archipelago on Ellesmere Island), Utqiagvik, formerly known as Barrow (Alaska), Nyalesund (Svalbard), and at the Villum Research Station (VRS; northern Greenland). For the former two stations, examined filters span a full yearly cycle. For VRS, 10 weekly samples, mostly from different months of one year, were included. Samples from Ny-Alesund were collected during the months from March until September of one year. At all four stations, highest concentrations were found in the summer months from roughly June to September. For those stations with sufficient data coverage, an annual cycle can be seen. The spectra of NINP observed at the highest temperatures, i.e., those obtained for summer months, showed the presence of INPs that nucleate ice up to-5 °C. Although the nature of these highly ice-active INPs could not be determined in this study, it often has been described in the literature that ice activity observed at such high temperatures originates from the presence of ice-active material of biogenic origin. Spectra observed at the lowest temperatures, i.e., those derived for winter months, were on the lower end of the respective values from the literature on Arctic INPs or INPs from midlatitude continental sites, to which a comparison is presented herein. An analysis concerning the origin of INPs that were ice active at high temperatures was carried out using back trajectories and satellite information. Both terrestrial locations in the Arctic and the adjacent sea were found to be possible source areas for highly active INPs.
- ItemAtmospheric new particle formation at the research station Melpitz, Germany: Connection with gaseous precursors and meteorological parameters(Katlenburg-Lindau : EGU, 2018) GrĂ¶ĂŸ, Johannes; Hamed, Amar; Sonntag, AndrĂ©; Spindler, Gerald; Manninen, Hanna Elina; Nieminen, Tuomo; Kulmala, Markku; Hõrrak, Urmas; Plass-DĂ¼lmer, Christian; Wiedensohler, Alfred; Birmili, WolframThis paper revisits the atmospheric new particle formation (NPF) process in the polluted Central European troposphere, focusing on the connection with gas-phase precursors and meteorological parameters. Observations were made at the research station Melpitz (former East Germany) between 2008 and 2011 involving a neutral cluster and air ion spectrometer (NAIS). Particle formation events were classified by a new automated method based on the convolution integral of particle number concentration in the diameter interval 2-20 nm. To study the relevance of gaseous sulfuric acid as a precursor for nucleation, a proxy was derived on the basis of direct measurements during a 1-month campaign in May 2008. As a major result, the number concentration of freshly produced particles correlated significantly with the concentration of sulfur dioxide as the main precursor of sulfuric acid. The condensation sink, a factor potentially inhibiting NPF events, played a subordinate role only. The same held for experimentally determined ammonia concentrations. The analysis of meteorological parameters confirmed the absolute need for solar radiation to induce NPF events and demonstrated the presence of significant turbulence during those events. Due to its tight correlation with solar radiation, however, an independent effect of turbulence for NPF could not be established. Based on the diurnal evolution of aerosol, gas-phase, and meteorological parameters near the ground, we further conclude that the particle formation process is likely to start in elevated parts of the boundary layer rather than near ground level.
- ItemLong-range and local air pollution: What can we learn from chemical speciation of particulate matter at paired sites?(Katlenburg-Lindau : EGU, 2020) Pandolfi, Marco; Mooibroek, Dennis; Hopke, Philip; van Pinxteren, Dominik; Querol, Xavier; Herrmann, Hartmut; Alastuey, AndrĂ©s; Favez, Olivier; HĂ¼glin, Christoph; Perdrix, Esperanza; Riffault, VĂ©ronique; Sauvage, StĂ©phane; van der Swaluw, Eric; Tarasova, Oksana; Colette, AugustinHere we report results of a detailed analysis of the urban and non-urban contributions to particulate matter (PM) concentrations and source contributions in five European cities, namely Schiedam (the Netherlands, NL), Lens (France, FR), Leipzig (Germany, DE), Zurich (Switzerland, CH) and Barcelona (Spain, ES). PM chemically speciated data from 12 European paired monitoring sites (one traffic, five urban, five regional and one continental background) were analysed by positive matrix factorisation (PMF) and Lenschow's approach to assign measured PM and source contributions to the different spatial levels. Five common sources were obtained at the 12 sites: sulfate-rich (SSA) and nitrate-rich (NSA) aerosols, road traffic (RT), mineral matter (MM), and aged sea salt (SS). These sources explained from 55 % to 88 % of PM mass at urban low-traffic-impact sites (UB) depending on the country. Three additional common sources were identified at a subset of sites/countries, namely biomass burning (BB) (FR, CH and DE), explaining an additional 9 %-13 % of PM mass, and residual oil combustion (V-Ni) and primary industrial (IND) (NL and ES), together explaining an additional 11 %-15 % of PM mass. In all countries, the majority of PM measured at UB sites was of a regional+continental (R+C) nature (64 %-74 %). The R+C PM increments due to anthropogenic emissions in DE, NL, CH, ES and FR represented around 66 %, 62 %, 52 %, 32 % and 23 %, respectively, of UB PM mass. Overall, the R+C PM increments due to natural and anthropogenic sources showed opposite seasonal profiles with the former increasing in summer and the latter increasing in winter, even if exceptions were observed. In ES, the anthropogenic R+C PM increment was higher in summer due to high contributions from regional SSA and V-Ni sources, both being mostly related to maritime shipping emissions at the Spanish sites. Conversely, in the other countries, higher anthropogenic R+C PM increments in winter were mostly due to high contributions from NSA and BB regional sources during the cold season. On annual average, the sources showing higher R+C increments were SSA (77 %-91 % of SSA source contribution at the urban level), NSA (51 %-94 %), MM (58 %-80 %), BB (42 %-78 %) and IND (91 % in NL). Other sources showing high R+C increments were photochemistry and coal combustion (97 %-99 %; identified only in DE). The highest regional SSA increment was observed in ES, especially in summer, and was related to ship emissions, enhanced photochemistry and peculiar meteorological patterns of the Western Mediterranean. The highest R+C and urban NSA increments were observed in NL and associated with high availability of precursors such as NOx and NH3. Conversely, on average, the sources showing higher local increments were RT (62 %-90 % at all sites) and V-Ni (65 %-80 % in ES and NL). The relationship between SSA and V-Ni indicated that the contribution of ship emissions to the local sulfate concentrations in NL has strongly decreased since 2007 thanks to the shift from high-sulfur-to low-sulfur-content fuel used by ships. An improvement of air quality in the five cities included here could be achieved by further reducing local (urban) emissions of PM, NOx and NH3 (from both traffic and non-traffic sources) but also SO2 and PM (from maritime ships and ports) and giving high relevance to non-urban contributions by further reducing emissions of SO2 (maritime shipping) and NH3 (agriculture) and those from industry, regional BB sources and coal combustion. © 2020 Copernicus GmbH. All rights reserved.
- ItemChemical composition and droplet size distribution of cloud at the summit of Mount Tai, China(Katlenburg-Lindau : EGU, 2017) Li, Jiarong; Wang, Xinfeng; Chen, Jianmin; Zhu, Chao; Li, Weijun; Li, Chengbao; Liu, Lu; Xu, Caihong; Wen, Liang; Xue, Likun; Wang, Wenxing; Ding, Aijun; Herrmann, HartmutThe chemical composition of 39 cloud samples and droplet size distributions in 24 cloud events were investigated at the summit of Mt. Tai from July to October 2014. Inorganic ions, organic acids, metals, HCHO, H2O2, sulfur( IV), organic carbon, and elemental carbon as well as pH and electrical conductivity were analyzed. The acidity of the cloud water significantly decreased from a reported value of pH 3.86 during 2007-2008 (Guo et al., 2012) to pH 5.87 in the present study. The concentrations of nitrate and ammonium were both increased since 2007-2008, but the overcompensation of ammonium led to an increase in the mean pH value. The microphysical properties showed that cloud droplets were smaller than 26.0 μm and most were in the range of 6.0-9.0 μm at Mt. Tai. The maximum droplet number concentration (Nd) was associated with a droplet size of 7.0 μm. High liquid water content (LWC) values could facilitate the formation of larger cloud droplets and broadened the droplet size distribution. Cloud droplets exhibited a strong interaction with atmospheric aerosols. Higher PM2.5 levels resulted in higher concentrations of water-soluble ions and smaller sizes with increased numbers of cloud droplets. The lower pH values were likely to occur at higher PM2.5 concentrations. Clouds were an important sink for soluble materials in the atmosphere. The dilution effect of cloud water should be considered when estimating concentrations of soluble components in the cloud phase.
- ItemParticulate sulfur in the upper troposphere and lowermost stratosphere - Sources and climate forcing(Katlenburg-Lindau : EGU, 2017) Martinsson, Bengt G.; Friberg, Johan; Sandvik, Oscar S.; Hermann, Markus; van Velthoven, Peter F. J.; Zahn, AndreasThis study is based on fine-mode aerosol samples collected in the upper troposphere (UT) and the lowermost stratosphere (LMS) of the Northern Hemisphere extratropics during monthly intercontinental flights at 8.8-12 km altitude of the IAGOS-CARIBIC platform in the time period 1999-2014. The samples were analyzed for a large number of chemical elements using the accelerator-based methods PIXE (particle-induced X-ray emission) and PESA (particle elastic scattering analysis). Here the particulate sulfur concentrations, obtained by PIXE analysis, are investigated. In addition, the satellite-borne lidar aboard CALIPSO is used to study the stratospheric aerosol load. A steep gradient in particulate sulfur concentration extends several kilometers into the LMS, as a result of increasing dilution towards the tropopause of stratospheric, particulate sulfur-rich air. The stratospheric air is diluted with tropospheric air, forming the extratropical transition layer (ExTL). Observed concentrations are related to the distance to the dynamical tropopause. A linear regression methodology handled seasonal variation and impact from volcanism. This was used to convert each data point into stand-alone estimates of a concentration profile and column concentration of particulate sulfur in a 3 km altitude band above the tropopause. We find distinct responses to volcanic eruptions, and that this layer in the LMS has a significant contribution to the stratospheric aerosol optical depth and thus to its radiative forcing. Further, the origin of UT particulate sulfur shows strong seasonal variation. We find that tropospheric sources dominate during the fall as a result of downward transport of the Asian tropopause aerosol layer (ATAL) formed in the Asian monsoon, whereas transport down from the Junge layer is the main source of UT particulate sulfur in the first half of the year. In this latter part of the year, the stratosphere is the clearly dominating source of particulate sulfur in the UT during times of volcanic influence and under background conditions.