| 1. |
- Paramonov, M., et al.
(författare)
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A synthesis of cloud condensation nuclei counter (CCNC) measurements within the EUCAARI network
- 2015
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 15:21, s. 12211-12229
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Tidskriftsartikel (refereegranskat)abstract
- Cloud condensation nuclei counter (CCNC) measurements performed at 14 locations around the world within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) framework have been analysed and discussed with respect to the cloud condensation nuclei (CCN) activation and hygroscopic properties of the atmospheric aerosol. The annual mean ratio of activated cloud condensation nuclei (N-CCN) to the total number concentration of particles (N-CN), known as the activated fraction A, shows a similar functional dependence on supersaturation S at many locations - exceptions to this being certain marine locations, a free troposphere site and background sites in south-west Germany and northern Finland. The use of total number concentration of particles above 50 and 100 nm diameter when calculating the activated fractions (A(50) and A(100), respectively) renders a much more stable dependence of A on S; A(50) and A(100) also reveal the effect of the size distribution on CCN activation. With respect to chemical composition, it was found that the hygroscopicity of aerosol particles as a function of size differs among locations. The hygroscopicity parameter kappa decreased with an increasing size at a continental site in south-west Germany and fluctuated without any particular size dependence across the observed size range in the remote tropical North Atlantic and rural central Hungary. At all other locations kappa increased with size. In fact, in Hyytiala, Vavihill, Jungfraujoch and Pallas the difference in hygroscopicity between Aitken and accumulation mode aerosol was statistically significant at the 5% significance level. In a boreal environment the assumption of a size-independent kappa can lead to a potentially substantial overestimation of N-CCN at S levels above 0.6 %. The same is true for other locations where kappa was found to increase with size. While detailed information about aerosol hygroscopicity can significantly improve the prediction of N-CCN, total aerosol number concentration and aerosol size distribution remain more important parameters. The seasonal and diurnal patterns of CCN activation and hygroscopic properties vary among three long-term locations, highlighting the spatial and temporal variability of potential aerosol-cloud interactions in various environments.
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| 2. |
- Wang, Z. B., et al.
(författare)
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Contributions of volatile and nonvolatile compounds (at 300 degrees C) to condensational growth of atmospheric nanoparticles: An assessment based on 8.5 years of observations at the Central Europe background site Melpitz
- 2017
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Ingår i: Journal of Geophysical Research-Atmospheres. - : American Geophysical Union (AGU). - 2169-897X. ; 122:1, s. 485-497
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Tidskriftsartikel (refereegranskat)abstract
- Long-term measurements of particle number size distributions in combination with thermodenuder analysis have been performed since July 2003 at the Central European station of Melpitz, Germany. Up to the end of 2011, 20% of all investigated days during the 8.5 years of measurements showed new particle formation and subsequent growth. To investigate the role of various chemical compound candidates for condensational nanoparticle growth, we focused on nucleation events in which the measured size distributions with and without thermodesorption both showed growth patterns (accounting for up to similar to 85% of all nucleation events). In this study, particulate compounds that volatilize at 300 degrees C were specifically defined as "volatile," in contrast to "nonvolatile" compounds, which remain in the particulate phase after being heated to 300 degrees C. A strong correlation between ambient temperature and growth rate associated with volatile substances (except gaseous sulfuric acid) was found, which implies the importance of organics (possibly oxidized biogenic organic compounds) in particle growth at Melpitz. The contributions of the volatile compounds to the growth rate due to condensation of gaseous sulfuric acid and organics were found to be about 19% and 47%, respectively. The remaining similar to 25% was attributed to nonvolatile residuals, which appear to form gradually during the particle growth process and are characterized as extremely low-volatility compounds. The growth rate associated with volatile components exhibited significant seasonal variation, with the highest value during summertime, whereas the growth rate associated with the nonvolatile fraction showed less fluctuation.
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| 3. |
- Zanatta, M., et al.
(författare)
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A European aerosol phenomenology-5 : Climatology of black carbon optical properties at 9 regional background sites across Europe
- 2016
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Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310 .- 1873-2844. ; 145, s. 346-364
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Tidskriftsartikel (refereegranskat)abstract
- A reliable assessment of the optical properties of atmospheric black carbon is of crucial importance for an accurate estimation of radiative forcing. In this study we investigated the spatio-temporal variability of the mass absorption cross-section (MAC) of atmospheric black carbon, defined as light absorption coefficient (sigma(ap)) divided by elemental carbon mass concentration (m(EC)). sigma(ap) and m(EC) have been monitored at supersites of the ACTRIS network for a minimum period of one year. The 9 rural background sites considered in this study cover southern Scandinavia, central Europe and the Mediterranean. sigma(ap) was determined using filter based absorption photometers and m(EC) using a thermal-optical technique. Homogeneity of the data-set was ensured by harmonization of all involved methods and instruments during extensive intercomparison exercises at the European Center for Aerosol Calibration (ECAC). Annual mean values of sigma(ap) at a wavelength of 637 nm vary between 0.66 and 1.3 Mm(-1) in southern Scandinavia, 3.7-11 Mm(-1) in Central Europe and the British Isles, and 2.3-2.8 Mm(-1) in the Mediterranean. Annual mean values of mEC vary between 0.084 and 0.23 mu g m(-3) in southern Scandinavia, 0.28 -1.1 in Central Europe and the British Isles, and 0.22-0.26 in the Mediterranean. Both sigma(ap) and mEC in southern Scandinavia and Central Europe have a distinct seasonality with maxima during the cold season and minima during summer, whereas at the Mediterranean sites an opposite trend was observed. Annual mean MAC values were quite similar across all sites and the seasonal variability was small at most sites. Consequently, a MAC value of 10.0 m(2) g(-1) (geometric standard deviation = 133) at a wavelength of 637 nm can be considered to be representative of the mixed boundary layer at European background sites, where BC is expected to be internally mixed to a large extent. The observed spatial variability is rather small compared to the variability of values in previous literature, indicating that the harmonization efforts resulted in substantially increased precision of the reported MAC. However, absolute uncertainties of the reported MAC values remain as high as +/- 30-70% due to the lack of appropriate reference methods and calibration materials. The mass ratio between elemental carbon and non-light-absorbing matter was used as a proxy for the thickness of coatings around the BC cores, in order to assess the influence of the mixing state on the MAC of BC. Indeed, the MAC was found to increase with increasing values of the coating thickness proxy. This provides evidence that coatings do increase the MAC of atmospheric BC to some extent, which is commonly referred to as lensing effect.
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| 4. |
- Hermann, Markus, et al.
(författare)
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An optical particle size spectrometer for aircraft-borne measurements in IAGOS-CARIBIC
- 2016
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Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 9:5, s. 2179-2194
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Tidskriftsartikel (refereegranskat)abstract
- The 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.
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| 5. |
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| 6. |
- Rose, C., et al.
(författare)
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Frequent nucleation events at the high altitude station of Chacaltaya (5240 m a.s.l.), Bolivia
- 2015
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Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310 .- 1873-2844. ; 102, s. 18-29
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Tidskriftsartikel (refereegranskat)abstract
- While nucleation may represent one of the major processes responsible for the total aerosol number burden in the atmosphere, and especially at high altitude, new particle formation (NPF) events occurring in the upper part of the troposphere are poorly documented in the literature, particularly in the southern hemisphere. NPF events were detected and analyzed at the highest measurement site in the world, Chacaltaya (5240 m a.s.l.), Bolivia between January 1 and December 31 2012, using a Neutral Aerosol and Ion Spectrometer (NAIS) that detects clusters down to 0.4 nm. NPF frequency at Chacaltaya is one of the highest reported so far (63.9%) and shows a clear seasonal dependency with maximum up to 100% during the dry season. This high seasonality of the NPF events frequency was found to be likely linked to the presence of clouds in the vicinity of the station during the wet season. Multiple NPF events are seen on almost 50% of event days and can reach up to 6 events per day, increasing the potential of nucleation to be the major contributor to the particle number concentrations in the upper troposphere. Ion-induced nucleation (IIN) was 14.8% on average, which is higher than the IIN fractions reported for boundary layer stations. The median formation rate of 2 nm particles computed for first position events is increased during the dry season (1.90 cm(-3) s(-1)) compared to the wet season (1.02 cm(-3) s(-1)), showing that events are more intense, on top of being more frequent during the dry season. On the contrary, particle growth rates (GRs) are on average enhanced during the wet season, which could be explained by higher amount of biogenic volatile organic compounds transported from the Amazon rainforest. The NPF events frequency is clearly enhanced when air masses originate from the oceanic sector, with a frequency of occurrence close to 1. However, based on the particle GRs, we calculate that particles most likely nucleate after the oceanic air masses reach the land and are presumably not originating from the marine free troposphere. The high frequency of NPF events, the occurrence of multiple events per day, and the relatively high formation rates observed at Chacaltaya imply that nucleation and growth are likely to be the major mechanism feeding the upper atmosphere with aerosol particles in this part of the continent.
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| 7. |
- Wang, Z. B., et al.
(författare)
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Connection of organics to atmospheric new particle formation and growth at an urban site of Beijing
- 2015
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Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310. ; 103, s. 7-17
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Tidskriftsartikel (refereegranskat)abstract
- In the present work, we aim to elucidate the roles of low-volatility organic vapors in atmospheric new particle formation in urban Beijing. Proposed organic molecules are derived from both the ambient measurement and the reasonable proxy. Several representations for the nucleation theories involving sulfuric acid and organic vapors are evaluated. The particle nucleation rates show good correlations both with sulfuric acid and organic vapors, suggesting that both play an important role in the atmospheric new particle formation. For the entire data set, the best fit (R=0.79, slope=1.1) between the observed and modeled particle nucleation rates is achieved with the homogenous nucleation theory of sulfuric acid (both homomolecularly and heteromolecularly) with separate coefficients in J=KSA1[H2SO4]2+KSA2[H2SO4][Org]. In addition, sulfuric acid concentration only contributes a small fraction (<15%) to the total observed growth rate. The growth rates of 7–30nm particles show positive correlation with the organic vapors oxidized by ozone, suggesting that particle nucleation may be controlled by the light intensity or OH concentration, while the growth of nucleation mode particles seems to be limited more by the concentrations of the organic precursors.
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| 8. |
- Wiedensohler, A., et al.
(författare)
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Black carbon emission and transport mechanisms to the free troposphere at the La Paz/El Alto (Bolivia) metropolitan area based on the Day of Census (2012)
- 2018
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Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310 .- 1873-2844. ; 194, s. 158-169
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Tidskriftsartikel (refereegranskat)abstract
- Urban development, growing industrialization, and increasing demand for mobility have led to elevated levels of air pollution in many large cities in Latin America, where air quality standards and WHO guidelines are frequently exceeded. The conurbation of the metropolitan area of La Paz/El Alto is one of the fastest growing urban settlements in South America with the particularity of being located in a very complex terrain at a high altitude. As many large cities or metropolitan areas, the metropolitan area of La Paz/El Alto and the Altiplano region are facing air quality deterioration. Long-term measurement data of the equivalent black carbon (eBC) mass concentrations and particle number size distributions (PNSD) from the Global Atmosphere Watch Observatory Chacaltaya (CHC; 5240 m a.s.l., above sea level) indicated a systematic transport of particle matter from the metropolitan area of La Paz/El Alto to this high altitude station and subsequently to the lower free troposphere. To better understand the sources and the transport mechanisms, we conducted eBC and PNSDs measurements during an intensive campaign at two locations in the urban area of La Paz/El Alto from September to November 2012. While the airport of El Alto site (4040 m a.s.l.) can be seen as representative of the urban and Altiplano background, the road site located in Central La Paz (3590 m a.s.l.) is representative for heavy traffic-dominated conditions. Peaks of eBC mass concentrations up to 5 mu g m(-3) were observed at the El Alto background site in the early morning and evening, while minimum values were detected in the early afternoon, mainly due to thermal convection and change of the planetary boundary layer height. The traffic-related eBC mass concentrations at the road site reached maximum values of 10-20 mu g m(-3). A complete traffic ban on the specific Bolivian Day of Census (November 21, 2012) led to a decrease of eBC below 1 mu g m(-3) at the road site for the entire day. Compared to the day before and after, particle number concentrations decreased by a factor between 5 and 25 over the particle size range from 10 to 800 nm, while the submicrometer particle mass concentration dropped by approximately 80%. These results indicate that traffic is the dominating source of BC and particulate air pollution in the metropolitan area of La Paz/El Alto. In general, the diurnal cycle of eBC mass concentration at the Chacaltaya observatory is anti-correlated to the observations at the El Alto background site. This pattern indicates that the traffic-related particulate matter, including BC, is transported to higher altitudes with the developing of the boundary layer during daytime. The metropolitan area of La Paz/El Alto seems to be a significant source for BC of the regional lower free troposphere. From there, BC can be transported over long distances and exert impact on climate and composition of remote southern hemisphere.
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