| 21. |
- Burton, S. P., et al.
(författare)
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Observations of the spectral dependence of linear particle depolarization ratio of aerosols using NASA Langley airborne High Spectral Resolution Lidar
- 2015
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:23, s. 13453-13473
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Tidskriftsartikel (refereegranskat)abstract
- Linear particle depolarization ratio is presented for three case studies from the NASA Langley airborne High Spectral Resolution Lidar-2 (HSRL-2). Particle depolarization ratio from lidar is an indicator of non-spherical particles and is sensitive to the fraction of non-spherical particles and their size. The HSRL-2 instrument measures depolarization at three wavelengths: 355, 532, and 1064 nm. The three measurement cases presented here include two cases of dust-dominated aerosol and one case of smoke aerosol. These cases have partial analogs in earlier HSRL-1 depolarization measurements at 532 and 1064 nm and in literature, but the availability of three wavelengths gives additional insight into different scenarios for non-spherical particles in the atmosphere. A case of transported Saharan dust has a spectral dependence with a peak of 0.30 at 532 nm with smaller particle depolarization ratios of 0.27 and 0.25 at 1064 and 355 nm, respectively. A case of aerosol containing locally generated wind-blown North American dust has a maximum of 0.38 at 1064 nm, decreasing to 0.37 and 0.24 at 532 and 355 nm, respectively. The cause of the maximum at 1064 nm is inferred to be very large particles that have not settled out of the dust layer. The smoke layer has the opposite spectral dependence, with the peak of 0.24 at 355 nm, decreasing to 0.09 and 0.02 at 532 and 1064 nm, respectively. The depolarization in the smoke case may be explained by the presence of coated soot aggregates. We note that in these specific case studies, the linear particle depolarization ratio for smoke and dust-dominated aerosol are more similar at 355 nm than at 532 nm, having possible implications for using the particle depolarization ratio at a single wavelength for aerosol typing.
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| 22. |
- Castarède, Dimitri, et al.
(författare)
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A thermodynamic description for the hygroscopic growth of atmospheric aerosol particles
- 2018
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:20, s. 14939-14948
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Tidskriftsartikel (refereegranskat)abstract
- The phase state of atmospheric particulate is important to atmospheric processes, and aerosol radiative forcing remains a large uncertainty in climate predictions. That said, precise atmospheric phase behavior is difficult to quantify and observations have shown that "precondensation" of water below predicted saturation values can occur. We propose a revised approach to understanding the transition from solid soluble particles to liquid droplets, typically described as cloud condensation nucleation - a process that is traditionally captured by Kohler theory, which describes a modified equilibrium saturation vapor pressure due to (i) mixing entropy (Raoult's law) and (ii) droplet geometry (Kelvin effect). Given that observations of precondensation are not predicted by Kohler theory, we devise a more complete model that includes interfacial forces giving rise to predeliquescence, i.e., the formation of a brine layer wetting a salt particle at relative humidities well below the deliquescence point.
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| 23. |
- Chauvigné, Aurélien, et al.
(författare)
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Biomass burning and urban emission impacts in the Andes Cordillera region based on in situ measurements from the Chacaltaya observatory, Bolivia (5240 m a.s.l.)
- 2019
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:23, s. 14805-14824
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Tidskriftsartikel (refereegranskat)abstract
- This study documents and analyses a 4-year continuous record of aerosol optical properties measured at the Global Atmosphere Watch (GAW) station of Chacaltaya (CHC; 5240 m a.s.l.), in Bolivia. Records of particle light scattering and particle light absorption coefficients are used to investigate how the high Andean Cordillera is affected by both long-range transport and by the fast-growing agglomeration of La Paz-El Alto, located approximately 20 km away and 1.5 km below the sampling site. The extended multiyear record allows us to study the properties of aerosol particles for different air mass types, during wet and dry seasons, also covering periods when the site was affected by biomass burning in the Bolivian lowlands and the Amazon Basin. The absorption, scattering, and extinction coefficients (median annual values of 0.74, 12.14, and 12.96 Mm(-1) respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94, and 8.68 Mm(-1) respectively) and higher values during the dry season (0.80, 11.23, and 14.51 Mm(-1) respectively). The record is driven by variability at both seasonal and diurnal scales. At a diurnal scale, all records of intensive and extensive aerosol properties show a pronounced variation (daytime maximum, night-time minimum), as a result of the dynamic and convective effects. The particle light absorption, scattering, and extinction coefficients are on average 1.94, 1.49, and 1.55 times higher respectively in the turbulent thermally driven conditions than the more stable conditions, due to more efficient transport from the boundary layer. Retrieved intensive optical properties are significantly different from one season to the other, reflecting the changing aerosol emission sources of aerosol at a larger scale. Using the wavelength dependence of aerosol particle optical properties, we discriminated between contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass burning and urban transport or industries) emissions according to seasons and local circulation. The main sources influencing measurements at CHC are from the urban area of La Paz-El Alto in the Altiplano and from regional biomass burning in the Amazon Basin. Results show a 28 % to 80 % increase in the extinction coefficients during the biomass burning season with respect to the dry season, which is observed in both tropospheric dynamic conditions. From this analysis, long-term observations at CHC provide the first direct evidence of the impact of biomass burning emissions of the Amazon Basin and urban emissions from the La Paz area on atmospheric optical properties at a remote site all the way to the free troposphere.
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| 24. |
- Chen, J., et al.
(författare)
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Ice-nucleating particle concentrations unaffected by urban air pollution in Beijing, China
- 2018
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:5, s. 3523-3539
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Tidskriftsartikel (refereegranskat)abstract
- Exceedingly 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 (N-INP) in the range from 6 to 25 degrees C in Beijing. No correlations between N-INP 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 N-INP 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.
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| 25. |
- Christensen, Ole Martin, 1984, et al.
(författare)
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The relationship between polar mesospheric clouds and their background atmosphere as observed by Odin-SMR and Odin-OSIRIS
- 2016
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:19, s. 12587-12600
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Tidskriftsartikel (refereegranskat)abstract
- In this study the properties of polar mesospheric clouds (PMCs) and the background atmosphere in which they exist are studied using measurements from two instruments, OSIRIS and SMR, on board the Odin satellite. The data comes from a set of tomographic measurements conducted by the satellite during 2010 and 2011. The expected ice mass density and cloud frequency for conditions of thermodynamic equilibrium, calculated using the temperature and water vapour as measured by SMR, are compared to the ice mass density and cloud frequency as measured by OSIRIS. We find that assuming thermodynamic equilibrium reproduces the seasonal, latitudinal and vertical variations in ice mass density and cloud frequency, but with a high bias of a factor of 2 in ice mass density. To investigate this bias, we use a simple ice particle growth model to estimate the time it would take for the observed clouds to sublimate completely and the time it takes for these clouds to reform. We find a difference in the median sublimation time (1.8 h) and the reformation time (3.2 h) at peak cloud altitudes (82-84 km). This difference implies that temperature variations on these timescales have a tendency to reduce the ice content of the clouds, possibly explaining the high bias of the equilibrium model. Finally, we detect and are, for the first time, able to positively identify cloud features with horizontal scales of 100 to 300 km extending far below the region of supersaturation (>2 km). Using the growth model, we conclude these features cannot be explained by sedimentation alone and suggest that these events may be an indication of strong vertical transport.
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| 26. |
- Christodoulakis, John, et al.
(författare)
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Impacts of air pollution and climate on materials in Athens, Greece
- 2017
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:1, s. 439-448
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Tidskriftsartikel (refereegranskat)abstract
- For more than 10 years now the National and Kapodistrian University of Athens, Greece, has contributed to the UNECE (United Nations Economic Commission for Europe) ICP Materials (International Co-operative Programme on Effects on Materials including Historic and Cultural Monuments) programme for monitoring the corrosion/soiling levels of different kinds of materials due to environmental air-quality parameters. In this paper we present the results obtained from the analysis of observational data that were collected in Athens during the period 2003-2012. According to these results, the corrosion/soiling of the particular exposed materials tends to decrease over the years, except for the case of copper. Based on this long experimental database that is applicable to the multi-pollutant situation in the Athens basin, we present dose-response functions (DRFs) considering that "dose" stands for the air pollutant concentration, "response" for the material mass loss (normally per annum) and "function", the relationship derived by the best statistical fit to the data.
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| 27. |
- Chung, Chul Eddy, et al.
(författare)
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Relationship between low-cloud presence and the amount of overlying aerosols
- 2016
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:9, s. 5781-5792
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Tidskriftsartikel (refereegranskat)abstract
- Aerosols are often advected above cloud decks, and the amount of aerosols over cloud has been assumed to be similar to that at the same heights in nearby clear sky. In this assumption, cloud and aerosol above cloud-top height are considered randomly located with respect to each other. The Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) data are analyzed here to investigate this assumption on global scales. The CALIPSO data reveal that the aerosol optical depth (AOD) above low cloud tends to be smaller than in nearby clear sky during the daytime, and the opposite is true during the nighttime. In particular, over oceanic regions with wide-spread low cloud, such as the tropical southeastern Atlantic Ocean and northeastern Pacific Ocean, the daytime AOD above low cloud is often 40aEuro-% smaller than in surrounding clear skies.
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| 28. |
- Croft, Betty, et al.
(författare)
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Processes controlling the annual cycle of Arctic aerosol number and size distributions
- 2016
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:6, s. 3665-3682
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Tidskriftsartikel (refereegranskat)abstract
- Measurements at high-Arctic sites (Alert, Nunavut, and Mt. Zeppelin, Svalbard) during the years 2011 to 2013 show a strong and similar annual cycle in aerosol number and size distributions. Each year at both sites, the number of aerosols with diameters larger than 20 nm exhibits a minimum in October and two maxima, one in spring associated with a dominant accumulation mode (particles 100 to 500 nm in diameter) and a second in summer associated with a dominant Aitken mode (particles 20 to 100 nm in diameter). Seasonal-mean aerosol effective diameter from measurements ranges from about 180 in summer to 260 nm in winter. This study interprets these annual cycles with the GEOS-Chem-TOMAS global aerosol microphysics model. Important roles are documented for several processes (new-particle formation, coagulation scavenging in clouds, scavenging by precipitation, and transport) in controlling the annual cycle in Arctic aerosol number and size. Our simulations suggest that coagulation scavenging of interstitial aerosols in clouds by aerosols that have activated to form cloud droplets strongly limits the total number of particles with diameters less than 200 nm throughout the year. We find that the minimum in total particle number in October can be explained by diminishing new-particle formation within the Arctic, limited transport of pollution from lower latitudes, and efficient wet removal. Our simulations indicate that the summertime-dominant Aitken mode is associated with efficient wet removal of accumulation-mode aerosols, which limits the condensation sink for condensable vapours. This in turn promotes new-particle formation and growth. The dominant accumulation mode during spring is associated with build up of transported pollution from outside the Arctic coupled with less-efficient wet-removal processes at colder temperatures. We recommend further attention to the key processes of new-particle formation, interstitial coagulation, and wet removal and their delicate interactions and balance in size-resolved aerosol simulations of the Arctic to reduce uncertainties in estimates of aerosol radiative effects on the Arctic climate.
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| 29. |
- Dalirian, Maryam, et al.
(författare)
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CCN activation of fumed silica aerosols mixed with soluble pollutants
- 2015
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:7, s. 3815-3829
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Tidskriftsartikel (refereegranskat)abstract
- Particle-water interactions of completely soluble or insoluble particles are fairly well understood but less is known of aerosols consisting of mixtures of soluble and insoluble components. In this study, laboratory measurements were performed to investigate cloud condensation nuclei (CCN) activity of silica particles mixed with ammonium sulfate (a salt), sucrose (a sugar) and bovine serum albumin known as BSA (a protein). The agglomerated structure of the silica particles was investigated using measurements with a differential mobility analyser (DMA) and an aerosol particle mass analyser (APM). Based on these data, the particles were assumed to be compact agglomerates when studying their CCN activation capabilities. Furthermore, the critical super-saturations of particles consisting of pure and mixed soluble and insoluble compounds were explored using existing theoretical frameworks. These results showed that the CCN activation of single-component particles was in good agreement with Kohler- and adsorption theory based models when the agglomerated structure was accounted for. For mixed particles the CCN activation was governed by the soluble components, and the soluble fraction varied considerably with particle size for our wet-generated aerosols. Our results confirm the hypothesis that knowing the soluble fraction is the key parameter needed for describing the CCN activation of mixed aerosols, and highlight the importance of controlled coating techniques for acquiring a detailed understanding of the CCN activation of atmospheric insoluble particles mixed with soluble pollutants.
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| 30. |
- Dall'Osto, Manuel, et al.
(författare)
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Simultaneous measurements of aerosol size distributions at three sites in the European high Arctic
- 2019
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:11, s. 7377-7395
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Tidskriftsartikel (refereegranskat)abstract
- Aerosols are an integral part of the Arctic climate system due to their direct interaction with radiation and indirect interaction through cloud formation. Understanding aerosol size distributions and their dynamics is crucial for the ability to predict these climate relevant effects. When of favourable size and composition, both long-rangetransported - and locally formed particles - may serve as cloud condensation nuclei (CCN). Small changes of composition or size may have a large impact on the low CCN concentrations currently characteristic of the Arctic environment. We present a cluster analysis of particle size distributions (PSDs; size range 8-500 nm) simultaneously collected from three high Arctic sites during a 3-year period (20132015). Two sites are located in the Svalbard archipelago: Zeppelin research station (ZEP; 474 m above ground) and the nearby Gruvebadet Observatory (GRU; about 2 km distance from Zeppelin, 67 m above ground). The third site (Villum Research Station at Station Nord, VRS; 30 m above ground) is 600 km west-northwest of Zeppelin, at the tip of northeastern Greenland. The GRU site is included in an inter-site comparison for the first time. K-means cluster analysis pro- vided eight specific aerosol categories, further combined into broad PSD classes with similar characteristics, namely pristine low concentrations (12 %-14 % occurrence), new particle formation (16 %-32 %), Aitken (21 %-35 %) and accumulation (20 %-50 %). Confined for longer time periods by consolidated pack sea ice regions, the Greenland site GRU shows PSDs with lower ultrafine-mode aerosol concentrations during summer but higher accumulation-mode aerosol concentrations during winter, relative to the Svalbard sites. By association with chemical composition and cloud condensation nuclei properties, further conclusions can be derived. Three distinct types of accumulation-mode aerosol are observed during winter months. These are associated with sea spray (largest detectable sizes, > 400 nm), Arctic haze (main mode at 150 nm) and aged accumulation-mode (main mode at 220 nm) aerosols. In contrast, locally produced particles, most likely of marine biogenic origin, exhibit size distributions dominated by the nucleation and Aitken mode during summer months. The obtained data and analysis point towards future studies, including apportioning the relative contribution of primary and secondary aerosol formation processes and elucidating anthropogenic aerosol dynamics and transport and removal processes across the Greenland Sea. In order to address important research questions in the Arctic on scales beyond a singular station or measurement events, it is imperative to continue strengthening international scientific cooperation.
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