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- ItemReal-time detection of highly oxidized organosulfates and BSOA marker compounds during the F-BEACh 2014 field study(München : European Geopyhsical Union, 2017) Brüggemann, Martin; Poulain, Laurent; Held, Andreas; Stelzer, Torsten; Zuth, Christoph; Richters, Stefanie; Mutzel, Anke; van Pinxteren, Dominik; Iinuma, Yoshiteru; Katkevica, Sarmite; Rabe, René; Herrmann, Hartmut; Hoffmann, ThorstenThe chemical composition of ambient organic aerosols was analyzed using complementary mass spectrometric techniques during a field study in central Europe in July 2014 (Fichtelgebirge – Biogenic Emission and Aerosol Chemistry, F-BEACh 2014). Among several common biogenic secondary organic aerosol (BSOA) marker compounds, 93 acidic oxygenated hydrocarbons were detected with elevated abundances and were thus attributed to be characteristic for the organic aerosol mass at the site. Monoterpene measurements exhibited median mixing ratios of 1.6 and 0.8 ppbV for in and above canopy levels respectively. Nonetheless, concentrations for early-generation oxidation products were rather low, e.g., pinic acid (c = 4.7 (±2.5) ng m−3). In contrast, high concentrations were found for later-generation photooxidation products such as 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA, c = 13.8 (±9.0) ng m−3) and 3-carboxyheptanedioic acid (c = 10.2 (±6.6) ng m−3), suggesting that aged aerosol masses were present during the campaign period. In agreement, HYSPLIT trajectory calculations indicate that most of the arriving air masses traveled long distances (> 1500 km) over land with high solar radiation. In addition, around 47 % of the detected compounds from filter sample analysis contained sulfur, confirming a rather high anthropogenic impact on biogenic emissions and their oxidation processes. Among the sulfur-containing compounds, several organosulfates, nitrooxy organosulfates, and highly oxidized organosulfates (HOOS) were tentatively identified by high-resolution mass spectrometry. Correlations among HOOS, sulfate, and highly oxidized multifunctional organic compounds (HOMs) support the hypothesis of previous studies that HOOS are formed by reactions of gas-phase HOMs with particulate sulfate. Moreover, periods with high relative humidity indicate that aqueous-phase chemistry might play a major role in HOOS production. However, for dryer periods, coinciding signals for HOOS and gas-phase peroxyradicals (RO2•) were observed, suggesting RO2• to be involved in HOOS formation.
- ItemMulti-year ACSM measurements at the central European research station Melpitz (Germany)-Part 1: Instrument robustness, quality assurance, and impact of upper size cutoff diameter(Katlenburg-Lindau : Copernicus, 2020) Poulain, Laurent; Spindler, Gerald; Grüner, Achim; Tuch, Thomas; Stieger, Bastian; van Pinxteren, Dominik; Petit, Jean-Eudes; Favez, Olivier; Herrmann, Hartmut; Wiedensohler, AlfredThe aerosol chemical speciation monitor (ACSM) is nowadays widely used to identify and quantify the main components of fine particles in ambient air. As such, its deployment at observatory platforms is fully incorporated within the European Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS). Regular intercomparisons are organized at the Aerosol Chemical Monitoring Calibration Center (ACMCC; part of the European Center for Aerosol Calibration, Paris, France) to ensure the consistency of the dataset, as well as instrumental performance and variability. However, in situ quality assurance remains a fundamental aspect of the instrument's stability. Here, we present and discuss the main outputs of long-term quality assurance efforts achieved for ACSM measurements at the research station Melpitz (Germany) since 2012 onwards. In order to validate the ACSM measurements over the years and to characterize seasonal variations, nitrate, sulfate, ammonium, organic, and particle mass concentrations were systematically compared against the collocated measurements of daily offline high-volume PM1 and PM2:5 filter samples and particle number size distribution (PNSD) measurements. Mass closure analysis was made by comparing the total particle mass (PM) concentration obtained by adding the mass concentration of equivalent black carbon (eBC) from the multi-angle absorption photometer (MAAP) to the ACSM chemical composition, to that of PM1 and PM2:5 during filter weighing, as well as to the derived mass concentration of PNSD. A combination of PM1 and PM2:5 filter samples helped identifying the critical importance of the upper size cutoff of the ACSM during such exercises. The ACSM-MAAP-derived mass concentrations systematically deviated from the PM1 mass when the mass concentration of the latter represented less than 60% of PM2:5, which was linked to the transmission efficiency of the aerodynamic lenses of the ACSM. The best correlations are obtained for sulfate (slopeD 0:96; R2 D 0:77) and total PM (slopeD 1:02; R2 D 0:90). Although, sulfate did not exhibit a seasonal dependency, total PM mass concentration revealed a small seasonal variability linked to the increase in non-water-soluble fractions. The nitrate suffers from a loss of ammonium nitrate during filter collection, and the contribution of organo-nitrate compounds to the ACSM nitrate signal make it difficult to directly compare the two methods. The contribution of m=z 44 (f44) to the total organic mass concentration was used to convert the ACSM organic mass (OM) to organic carbon (OC) by using a similar approach as for the aerosol mass spectrometer (AMS). The resulting estimated OCACSM was compared with the measured OCPM1 (slopeD 0:74; R2 D 0:77), indicating that the f44 signal was relatively free of interferences during this period. The PM2:5 filter samples use for the ACSM data quality might suffer from a systematic bias due to a size truncation effect as well as to the presence of chemical species that cannot be detected by the ACSM in coarse mode (e.g., sodium nitrate and sodium sulfate). This may lead to a systematic underestimation of the ACSM particle mass concentration and/or a positive artifact that artificially decreases the discrepancies between the two methods. Consequently, ACSM data validation using PM2:5 filters has to be interpreted with extreme care. The particle mass closure with the PNSD was satisfying (slopeD 0:77; R2 D 0:90 over the entire period), with a slight overestimation of the mobility particle size spectrometer (MPSS)-derived mass concentration in winter. This seasonal variability was related to a change on the PNSD and a larger contribution of the supermicrometer particles in winter. This long-term analysis between the ACSM and other collocated instruments confirms the robustness of the ACSM and its suitability for long-term measurements. Particle mass closure with the PNSD is strongly recommended to ensure the stability of the ACSM. A near-real-time mass closure procedure within the entire ACTRIS-ACSM network certainly represents an optimal quality control and assurance of both warranting the quality assurance of the ACSM measurements as well as identifying cross-instrumental biases. © Author(s) 2020.
- ItemVariability 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(Katlenburg-Lindau : European Geosciences Union, 2021) Yuan, Jinfeng; Modini, Robin Lewis; Zanatta, Marco; Herber, Andreas B.; Müller, Thomas; Wehner, Birgit; Poulain, Laurent; Tuch, Thomas; Baltensperger, Urs; Gysel-Beer, MartinProperties 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.
- ItemSource apportionment and impact of long-range transport on carbonaceous aerosol particles in central Germany during HCCT-2010(Katlenburg-Lindau : EGU, 2021) Poulain, Laurent; Fahlbusch, Benjamin; Spindler, Gerald; Mueller, Konrad; van Pinxteren, Dominik; Wu, Zhijun; Iinuma, Yoshiteru; Birmili, Wolfram; Wiedensohler, Alfred; Herrmann, HartmutThe identification of different sources of the carbonaceous aerosol (organics and black carbon) was investigated at a mountain forest site located in central Germany from September to October 2010 to characterize incoming air masses during the Hill Cap Cloud Thuringia 2010 (HCCT-2010) experiment. The near-PM1 chemical composition, as measured by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), was dominated by organic aerosol (OA; 41 %) followed by sulfate (19 %) and nitrate (18 %). Source apportionment of the OA fraction was performed using the multilinear engine (ME-2) approach, resulting in the identification of the following five factors: hydrocarbon-like OA (HOA; 3 % of OA mass), biomass burning OA (BBOA; 13 %), semi-volatile-like OA (SV-OOA; 19 %), and two oxygenated OA (OOA) factors. The more oxidized OOA (MO-OOA, 28 %) was interpreted as being influenced by aged, polluted continental air masses, whereas the less oxidized OOA (LO-OOA, 37 %) was found to be more linked to aged biogenic sources. Equivalent black carbon (eBC), measured by a multi-angle absorption photometer (MAAP) represented 10 % of the total particulate matter (PM). The eBC was clearly associated with HOA, BBOA, and MO-OOA factors (all together R2=0.83). Therefore, eBC's contribution to each factor was achieved using a multi-linear regression model. More than half of the eBC (52 %) was associated with long-range transport (i.e., MO-OOA), whereas liquid fuel eBC (35 %) and biomass burning eBC (13 %) were associated with local emissions, leading to a complete apportionment of the carbonaceous aerosol. The separation between local and transported eBC was well supported by the mass size distribution of elemental carbon (EC) from Berner impactor samples. Air masses with the strongest marine influence, based on back trajectory analysis, corresponded with a low particle mass concentration (6.4–7.5 µg m−3) and organic fraction (≈30 %). However, they also had the largest contribution of primary OA (HOA ≈ 4 % and BBOA 15 %–20 %), which was associated with local emissions. Continental air masses had the highest mass concentration (11.4–12.6 µg m−3), and a larger fraction of oxygenated OA (≈45 %) indicated highly processed OA. The present results emphasize the key role played by long-range transport processes not only in the OA fraction but also in the eBC mass concentration and the importance of improving our knowledge on the identification of eBC sources.
- ItemSimulation of atmospheric organic aerosol using its volatility-oxygen-content distribution during the PEGASOS 2012 campaign(Katlenburg-Lindau : EGU, 2018) Karnezi, Eleni; Murphy, Benjamin N.; Poulain, Laurent; Herrmann, Hartmut; Wiedensohler, Alfred; Rubach, Florian; Kiendler-Scharr, Astrid; Mentel, Thomas F.; Pandis, Spyros N.A lot of effort has been made to understand and constrain the atmospheric aging of the organic aerosol (OA). Different parameterizations of the organic aerosol formation and evolution in the two-dimensional volatility basis set (2D-VBS) framework are evaluated using ground and airborne measurements collected in the 2012 Pan-European Gas AeroSOls-climate interaction Study (PEGASOS) field campaign in the Po Valley (Italy). A number of chemical aging schemes are examined, taking into account various functionalization and fragmentation pathways for biogenic and anthropogenic OA components. Model predictions and measurements, both at the ground and aloft, indicate a relatively oxidized OA with little average diurnal variation. Total OA concentration and O: C ratios are reproduced within experimental error by a number of chemical aging schemes. Anthropogenic secondary OA (SOA) is predicted to contribute 15-25% of the total OA, while SOA from intermediate volatility compound oxidation contributes another 20-35%. Biogenic SOA (bSOA) contributions varied from 15 to 45% depending on the modeling scheme. Primary OA contributed around 5% for all schemes and was comparable to the hydrocarbon-like OA (HOA) concentrations derived from the positive matrix factorization of the aerosol mass spectrometer (PMF-AMS) ground measurements. The average OA and O: C diurnal variation and their vertical profiles showed a surprisingly modest sensitivity to the assumed vaporization enthalpy for all aging schemes. This can be explained by the interplay between the partitioning of the semi-volatile compounds and their gas-phase chemical aging reactions.
- 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.
- ItemLong-term cloud condensation nuclei number concentration, particle number size distribution and chemical composition measurements at regionally representative observatories(Katlenburg-Lindau : EGU, 2018) Schmale, Julia; Henning, Silvia; Decesari, Stefano; Henzing, Bas; Keskinen, Helmi; Sellegri, Karine; Ovadnevaite, Jurgita; Pöhlker, Mira L.; Brito, Joel; Bougiatioti, Aikaterini; Kristensson, Adam; Kalivitis, Nikos; Stavroulas, Iasonas; Carbone, Samara; Jefferson, Anne; Park, Minsu; Schlag, Patrick; Iwamoto, Yoko; Aalto, Pasi; Äijälä, Mikko; Bukowiecki, Nicolas; Ehn, Mikael; Frank, Göran; Fröhlich, Roman; Frumau, Arnoud; Herrmann, Erik; Herrmann, Hartmut; Holzinger, Rupert; Kos, Gerard; Kulmala, Markku; Mihalopoulos, Nikolaos; Nenes, Athanasios; O'Dowd, Colin; Petäjä, Tuukka; Picard, David; Pöhlker, Christopher; Pöschl, Ulrich; Poulain, Laurent; Prévôt, André Stephan Henry; Swietlicki, Erik; Andreae, Meinrat O.; Artaxo, Paulo; Wiedensohler, Alfred; Ogren, John; Matsuki, Atsushi; Yum, Seong Soo; Stratmann, Frank; Baltensperger, Urs; Gysel, MartinAerosol-cloud interactions (ACI) constitute the single largest uncertainty in anthropogenic radiative forcing. To reduce the uncertainties and gain more confidence in the simulation of ACI, models need to be evaluated against observations, in particular against measurements of cloud condensation nuclei (CCN). Here we present a data set - ready to be used for model validation - of long-term observations of CCN number concentrations, particle number size distributions and chemical composition from 12 sites on 3 continents. Studied environments include coastal background, rural background, alpine sites, remote forests and an urban surrounding. Expectedly, CCN characteristics are highly variable across site categories. However, they also vary within them, most strongly in the coastal background group, where CCN number concentrations can vary by up to a factor of 30 within one season. In terms of particle activation behaviour, most continental stations exhibit very similar activation ratios (relative to particles 20nm) across the range of 0.1 to 1.0% supersaturation. At the coastal sites the transition from particles being CCN inactive to becoming CCN active occurs over a wider range of the supersaturation spectrum. Several stations show strong seasonal cycles of CCN number concentrations and particle number size distributions, e.g. at Barrow (Arctic haze in spring), at the alpine stations (stronger influence of polluted boundary layer air masses in summer), the rain forest (wet and dry season) or Finokalia (wildfire influence in autumn). The rural background and urban sites exhibit relatively little variability throughout the year, while short-term variability can be high especially at the urban site. The average hygroscopicity parameter, calculated from the chemical composition of submicron particles was highest at the coastal site of Mace Head (0.6) and lowest at the rain forest station ATTO (0.2-0.3). We performed closure studies based on -Köhler theory to predict CCN number concentrations. The ratio of predicted to measured CCN concentrations is between 0.87 and 1.4 for five different types of . The temporal variability is also well captured, with Pearson correlation coefficients exceeding 0.87. Information on CCN number concentrations at many locations is important to better characterise ACI and their radiative forcing. But long-term comprehensive aerosol particle characterisations are labour intensive and costly. Hence, we recommend operating migrating-CCNCs to conduct collocated CCN number concentration and particle number size distribution measurements at individual locations throughout one year at least to derive a seasonally resolved hygroscopicity parameter. This way, CCN number concentrations can only be calculated based on continued particle number size distribution information and greater spatial coverage of long-term measurements can be achieved.
- ItemOrganic aerosol source apportionment by offline-AMS over a full year in Marseille(Katlenburg-Lindau : EGU, 2017) Bozzetti, Carlo; El Haddad, Imad; Salameh, Dalia; Daellenbach, Kaspar Rudolf; Fermo, Paola; Gonzalez, Raquel; Minguillón, María Cruz; Iinuma, Yoshiteru; Poulain, Laurent; Elser, Miriam; Müller, Emanuel; Slowik, Jay Gates; Jaffrezo, Jean-Luc; Baltensperger, Urs; Marchand, Nicolas; Prévôt, André Stephan HenryWe investigated the seasonal trends of OA sources affecting the air quality of Marseille (France), which is the largest harbor of the Mediterranean Sea. This was achieved by measurements of nebulized filter extracts using an aerosol mass spectrometer (offline-AMS). In total 216 PM2.5 (particulate matter with an aerodynamic diameter < 2.5 μm) filter samples were collected over 1 year from August 2011 to July 2012. These filters were used to create 54 composite samples which were analyzed by offline-AMS. The same samples were also analyzed for major water-soluble ions, metals, elemental and organic carbon (EC/OC), and organic markers, including n-alkanes, hopanes, polycyclic aromatic hydrocarbons (PAHs), lignin and cellulose pyrolysis products, and nitrocatechols. The application of positive matrix factorization (PMF) to the water-soluble AMS spectra enabled the extraction of five factors, related to hydrocarbon-like OA (HOA), cooking OA (COA), biomass burning OA (BBOA), oxygenated OA (OOA), and an industry-related OA (INDOA). Seasonal trends and relative contributions of OA sources were compared with the source apportionment of OA spectra collected from the AMS field deployment at the same station but in different years and for shorter monitoring periods (February 2011 and July 2008). Online- and offline-AMS source apportionment revealed comparable seasonal contribution of the different OA sources. Results revealed that BBOA was the dominant source during winter, representing on average 48 % of the OA, while during summer the main OA component was OOA (63 % of OA mass on average). HOA related to traffic emissions contributed on a yearly average 17 % to the OA mass, while COA was a minor source contributing 4 %. The contribution of INDOA was enhanced during winter (17 % during winter and 11 % during summer), consistent with an increased contribution from light alkanes, light PAHs (fluoranthene, pyrene, phenanthrene), and selenium, which is commonly considered as a unique coal combustion and coke production marker. Online- and offline-AMS source apportionments revealed evolving levoglucosan : BBOA ratios, which were higher during late autumn and March. A similar seasonality was observed in the ratios of cellulose combustion markers to lignin combustion markers, highlighting the contribution from cellulose-rich biomass combustion, possibly related to agricultural activities.
- ItemModelling winter organic aerosol at the European scale with CAMx: Evaluation and source apportionment with a VBS parameterization based on novel wood burning smog chamber experiments(Katlenburg-Lindau : EGU, 2017) Ciarelli, Giancarlo; Aksoyoglu, Sebnem; El Haddad, Imad; Bruns, Emily A.; Crippa, Monica; Poulain, Laurent; Äijälä, Mikko; Carbone, Samara; Freney, Evelyn; O'Dowd, Colin; Baltensperger, Urs; Prévôt, André S. H.We evaluated a modified VBS (volatility basis set) scheme to treat biomass-burning-like organic aerosol (BBOA) implemented in CAMx (Comprehensive Air Quality Model with extensions). The updated scheme was parameterized with novel wood combustion smog chamber experiments using a hybrid VBS framework which accounts for a mixture of wood burning organic aerosol precursors and their further functionalization and fragmentation in the atmosphere. The new scheme was evaluated for one of the winter EMEP intensive campaigns (February-March 2009) against aerosol mass spectrometer (AMS) measurements performed at 11 sites in Europe. We found a considerable improvement for the modelled organic aerosol (OA) mass compared to our previous model application with the mean fractional bias (MFB) reduced from -61 to -29 %. We performed model-based source apportionment studies and compared results against positive matrix factorization (PMF) analysis performed on OA AMS data. Both model and observations suggest that OA was mainly of secondary origin at almost all sites. Modelled secondary organic aerosol (SOA) contributions to total OA varied from 32 to 88% (with an average contribution of 62 %) and absolute concentrations were generally under-predicted. Modelled primary hydrocarbon-like organic aerosol (HOA) and primary biomass-burning-like aerosol (BBPOA) fractions contributed to a lesser extent (HOA from 3 to 30 %, and BBPOA from 1 to 39 %) with average contributions of 13 and 25 %, respectively. Modelled BBPOA fractions were found to represent 12 to 64% of the total residential-heating-related OA, with increasing contributions at stations located in the northern part of the domain. Source apportionment studies were performed to assess the contribution of residential and non-residential combustion precursors to the total SOA. Non-residential combustion and road transportation sector contributed about 30-40% to SOA formation (with increasing contributions at urban and near industrialized sites), whereas residential combustion (mainly related to wood burning) contributed to a larger extent, around 60-70 %. Contributions to OA from residential combustion precursors in different volatility ranges were also assessed: our results indicate that residential combustion gas-phase precursors in the semivolatile range (SVOC) contributed from 6 to 30 %, with higher contributions predicted at stations located in the southern part of the domain. On the other hand, the oxidation products of higher-volatility precursors (the sum of intermediate-volatility compounds (IVOCs) and volatile organic compounds (VOCs)) contribute from 15 to 38% with no specific gradient among the stations. Although the new parameterization leads to a better agreement between model results and observations, it still underpredicts the SOA fraction, suggesting that uncertainties in the new scheme and other sources and/or formation mechanisms remain to be elucidated. Moreover, a more detailed characterization of the semivolatile components of the emissions is needed.
- ItemAerosol activation characteristics and prediction at the central European ACTRIS research station of Melpitz, Germany(Katlenburg-Lindau : EGU, 2022) Wang, Yuan; Henning, Silvia; Poulain, Laurent; Lu, Chunsong; Stratmann, Frank; Wang, Yuying; Niu, Shengjie; Pöhlker, Mira L.; Herrmann, Hartmut; Wiedensohler, AlfredUnderstanding 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.
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