scholarly journals Cloud droplet activity changes of soot aerosol upon smog chamber ageing

2014 ◽  
Vol 14 (18) ◽  
pp. 9831-9854 ◽  
Author(s):  
C. Wittbom ◽  
A. C. Eriksson ◽  
J. Rissler ◽  
J. E. Carlsson ◽  
P. Roldin ◽  
...  
Keyword(s):  
Uv Radiation ◽  
Organic Material ◽  
Mass Fraction ◽  
Cloud Condensation Nuclei ◽  
Cloud Droplet ◽  
Particle Morphology ◽  
Organic Aerosol ◽  
Condensation Nuclei ◽  
Soot Particles ◽  
Kohler Theory

Abstract. Particles containing soot, or black carbon, are generally considered to contribute to global warming. However, large uncertainties remain in the net climate forcing resulting from anthropogenic emissions of black carbon (BC), to a large extent due to the fact that BC is co-emitted with gases and primary particles, both organic and inorganic, and subject to atmospheric ageing processes. In this study, diesel exhaust particles and particles from a flame soot generator spiked with light aromatic secondary organic aerosol (SOA) precursors were processed by UV radiation in a 6 m3 Teflon chamber in the presence of NOx. The time-dependent changes of the soot nanoparticle properties were characterised using a Cloud Condensation Nuclei Counter, an Aerosol Particle Mass Analyzer and a Soot Particle Aerosol Mass Spectrometer. The results show that freshly emitted soot particles do not activate into cloud droplets at supersaturations ≤2%, i.e. the BC core coated with primary organic aerosol (POA) from the exhaust is limited in hygroscopicity. Before the onset of UV radiation it is unlikely that any substantial SOA formation is taking place. An immediate change in cloud-activation properties occurs at the onset of UV exposure. This change in hygroscopicity is likely attributed to SOA formed from intermediate volatility organic compounds (IVOCs) in the diesel engine exhaust. The change of cloud condensation nuclei (CCN) properties at the onset of UV radiation implies that the lifetime of soot particles in the atmosphere is affected by the access to sunlight, which differs between latitudes. The ageing of soot particles progressively enhances their ability to act as cloud condensation nuclei, due to changes in: (I) organic fraction of the particle, (II) chemical properties of this fraction (e.g. primary or secondary organic aerosol), (III) particle size, and (IV) particle morphology. Applying κ-Köhler theory, using a κSOA value of 0.13 (derived from independent input parameters describing the organic material), showed good agreement with cloud droplet activation measurements for particles with a SOA mass fraction ≥0.12 (slightly aged particles). The activation properties are enhanced with only a slight increase in organic material coating the soot particles (SOA mass fraction < 0.12), however not as much as predicted by Köhler theory. The discrepancy between theory and experiments during the early stages of ageing might be due to solubility limitations, unevenly distributed organic material or hindering particle morphology. The change in properties of soot nanoparticles upon photochemical processing clearly increases their hygroscopicity, which affects their behaviour both in the atmosphere and in the human respiratory system.

scholarly journals Cloud droplet activity changes of soot aerosol upon smog chamber ageing

2014 ◽  
Vol 14 (7) ◽  
pp. 8851-8914 ◽  
Author(s):  
C. Wittbom ◽  
J. H. Pagels ◽  
J. Rissler ◽  
A. C. Eriksson ◽  
J. E. Carlsson ◽  
...  
Keyword(s):  
Black Carbon ◽  
Uv Radiation ◽  
Organic Material ◽  
Cloud Condensation Nuclei ◽  
Cloud Droplet ◽  
Particle Morphology ◽  
Organic Aerosol ◽  
Condensation Nuclei ◽  
Soot Particles ◽  
Kohler Theory

Abstract. Particles containing soot, or black carbon, are generally considered to contribute to global warming. However, large uncertainties remain in the net climate forcing resulting from anthropogenic emissions of black carbon (BC), to a large extent due to the fact that BC is co-emitted with gases and primary particles, both organic and inorganic, and subject to atmospheric ageing processes. In this study, diesel exhaust particles and particles from a flame soot generator spiked with light aromatic secondary organic aerosol (SOA) precursors were processed by UV-radiation in a 6 m3 Teflon chamber in the presence of NOx. The time-dependent changes of the soot nanoparticle properties were characterised using a Cloud Condensation Nuclei Counter, an Aerosol Particle Mass Analyzer and a Soot Particle Aerosol Mass Spectrometer. The results show that freshly emitted soot particles do not activate into cloud droplets at supersaturations ≤ 2%, i.e. the black carbon core coated with primary organic aerosol (POA) from the exhaust is limited in hygroscopicity. Before the onset of UV radiation it is unlikely that any substantial SOA formation is taking place. An immediate change in cloud-activation properties occurs at the onset of UV exposure. This change in hygroscopicity is likely attributed to SOA formed from intermediate volatile organic compounds (IVOC) in the diesel engine exhaust. The change of cloud condensation nuclei (CCN) properties at the onset of UV radiation implies that the lifetime of soot particles in the atmosphere is affected by the access to sunlight, which differs between latitudes. The ageing of soot particles progressively enhances their ability to act as cloud condensation nuclei, due to changes in: (I) organic fraction of the particle, (II) chemical properties of this fraction (POA or SOA), (III) particle size, and (IV) particle morphology. Applying κ-Köhler theory, using a κSOA value of 0.13 (derived from independent input parameters describing the organic material), showed good agreement with cloud droplet activation measurements for particles with a SOA mass fraction (mfSOA(APM)) ≥ 0.12 (slightly aged particles). The activation properties are enhanced with only a slight increase in organic material coating the soot particles (mfSOA(APM) < 0.12), however not as much as predicted with Köhler theory. The discrepancy between theory and experiments might be due to solubility limitations, unevenly distributed organic material or hindering particle morphology. The change in properties of soot nanoparticles upon photochemical processing clearly increases their hygroscopicity, which affects their behaviour both in the atmosphere and in the human respiratory system.

scholarly journals Impact of isolated atmospheric aging processes on the cloud condensation nuclei activation of soot particles

2019 ◽  
Vol 19 (24) ◽  
pp. 15545-15567 ◽  
Author(s):  
Franz Friebel ◽  
Prem Lobo ◽  
David Neubauer ◽  
Ulrike Lohmann ◽  
Saskia Drossaart van Dusseldorp ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Climate Model ◽  
Cloud Condensation Nuclei ◽  
Particle Diameter ◽  
Cloud Droplet ◽  
High Sensitivity ◽  
Condensation Nuclei ◽  
Soot Particles ◽  
Atmospheric Aging ◽  
Ccn Activity

Abstract. The largest contributors to the uncertainty in assessing the anthropogenic contribution in radiative forcing are the direct and indirect effects of aerosol particles on the Earth's radiative budget. Soot particles are of special interest since their properties can change significantly due to aging processes once they are emitted into the atmosphere. Probably the largest obstacle for the investigation of these processes in the laboratory is the long atmospheric lifetime of 1 week, requiring tailored experiments that cover this time span. This work presents results on the ability of two types of soot, obtained using a miniCAST soot generator, to act as cloud condensation nuclei (CCN) after exposure to atmospherically relevant levels of ozone (O3) and humidity. Aging times of up to 12 h were achieved by successful application of the continuous-flow stirred tank reactor (CSTR) concept while allowing for size selection of particles prior to the aging step. Particles of 100 nm diameter and rich in organic carbon (OC) that were initially CCN inactive showed significant CCN activity at supersaturations (SS) down to 0.3 % after 10 h of exposure to 200 ppb of O3. While this process was not affected by different levels of relative humidity in the range of 5 %–75 %, a high sensitivity towards the ambient/reaction temperature was observed. Soot particles with a lower OC content required an approximately 4-fold longer aging duration to show CCN activity at the same SS. Prior to the slow change in the CCN activity, a rapid increase in the particle diameter was detected which occurred within several minutes. This study highlights the applicability of the CSTR approach for the simulation of atmospheric aging processes, as aging durations beyond 12 h can be achieved in comparably small aerosol chamber volumes (<3 m3). Implementation of our measurement results in a global aerosol-climate model, ECHAM6.3-HAM2.3, showed a statistically significant increase in the regional and global CCN burden and cloud droplet number concentration.

scholarly journals Measured and modelled cloud condensation nuclei number concentration at the high alpine site Jungfraujoch

2010 ◽  
Vol 10 (16) ◽  
pp. 7891-7906 ◽  
Author(s):  
Z. Jurányi ◽  
M. Gysel ◽  
E. Weingartner ◽  
P. F. DeCarlo ◽  
L. Kammermann ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Hydrological Cycle ◽  
Cloud Condensation Nuclei ◽  
Sensitivity Study ◽  
Research Station ◽  
Condensation Nuclei ◽  
Composition Data ◽  
Particle Mobility ◽  
Kohler Theory ◽  
Highly Correlated

Abstract. Atmospheric aerosol particles are able to act as cloud condensation nuclei (CCN) and are therefore important for the climate and the hydrological cycle, but their properties are not fully understood. Total CCN number concentrations at 10 different supersaturations in the range of SS=0.12–1.18% were measured in May 2008 at the remote high alpine research station, Jungfraujoch, Switzerland (3580 m a.s.l.). In this paper, we present a closure study between measured and predicted CCN number concentrations. CCN predictions were done using dry number size distribution (scanning particle mobility sizer, SMPS) and bulk chemical composition data (aerosol mass spectrometer, AMS, and multi-angle absorption photometer, MAAP) in a simplified Köhler theory. The predicted and the measured CCN number concentrations agree very well and are highly correlated. A sensitivity study showed that the temporal variability of the chemical composition at the Jungfraujoch can be neglected for a reliable CCN prediction, whereas it is important to know the mean chemical composition. The exact bias introduced by using a too low or too high hygroscopicity parameter for CCN prediction was further quantified and shown to be substantial for the lowest supersaturation. Despite the high average organic mass fraction (~45%) in the fine mode, there was no indication that the surface tension was substantially reduced at the point of CCN activation. A comparison between hygroscopicity tandem differential mobility analyzer (HTDMA), AMS/MAAP, and CCN derived κ values showed that HTDMA measurements can be used to determine particle hygroscopicity required for CCN predictions if no suitable chemical composition data are available.

scholarly journals Organic acids as cloud condensation nuclei: Laboratory studies of highly soluble and insoluble species

2003 ◽  
Vol 3 (1) ◽  
pp. 949-982 ◽  
Author(s):  
P. Pradeep Kumar ◽  
K. Broekhuizen ◽  
J. P. D. Abbatt
Keyword(s):  
Organic Acids ◽  
Room Temperature ◽  
Cloud Condensation Nuclei ◽  
Particle Diameter ◽  
Diffusion Chamber ◽  
Laboratory Studies ◽  
Condensation Nuclei ◽  
Gradient Diffusion ◽  
Kohler Theory ◽  
Good Agreement

Abstract. The ability of sub-micron-sized organic acid particles to act as cloud condensation nuclei (CCN) has been examined at room temperature using a newly constructed continuous-flow, thermal-gradient diffusion chamber (TGDC). The organic acids studied were: oxalic, malonic, glutaric, oleic and stearic. The CCN properties of the highly soluble acids – oxalic, malonic and glutaric – match very closely Kohler theory predictions which assume full dissolution of the dry particle and a surface tension of the growing droplet equal to that of water. In particular, for supersaturations between 0.3 and 0.6, agreement between the dry particle diameter which gives 50% activation and that calculated from Kohler theory is to within 3 nm on average. In the course of the experiments, considerable instability of glutaric acid particles was observed as a function of time and there is evidence that they fragment to some degree to smaller particles. Stearic acid and oleic acid, which are both highly insoluble in water, did not activate at supersaturations of 0.6% with dry diameters up to 140 nm. Finally, to validate the performance of the TGDC, we present results for the activation of ammonium sulfate particles that demonstrate good agreement with Kohler theory if solution non-ideality is considered. Our findings support earlier studies in the literature that showed highly soluble organics to be CCN active but insoluble species to be largely inactive.

scholarly journals Remote sensing the vertical profile of cloud droplet effective radius, thermodynamic phase, and temperature

2011 ◽  
Vol 11 (18) ◽  
pp. 9485-9501 ◽  
Author(s):  
J. V. Martins ◽  
A. Marshak ◽  
L. A. Remer ◽  
D. Rosenfeld ◽  
Y. J. Kaufman ◽  
...  
Keyword(s):  
Remote Sensing ◽  
Energy Balance ◽  
Brightness Temperature ◽  
Vertical Profile ◽  
Water Cycle ◽  
Cloud Condensation Nuclei ◽  
Cloud Droplet ◽  
Cloud Microphysics ◽  
Condensation Nuclei ◽  
Thermodynamic Phase

Abstract. Cloud-aerosol interaction is a key issue in the climate system, affecting the water cycle, the weather, and the total energy balance including the spatial and temporal distribution of latent heat release. Information on the vertical distribution of cloud droplet microphysics and thermodynamic phase as a function of temperature or height, can be correlated with details of the aerosol field to provide insight on how these particles are affecting cloud properties and their consequences to cloud lifetime, precipitation, water cycle, and general energy balance. Unfortunately, today's experimental methods still lack the observational tools that can characterize the true evolution of the cloud microphysical, spatial and temporal structure in the cloud droplet scale, and then link these characteristics to environmental factors and properties of the cloud condensation nuclei. Here we propose and demonstrate a new experimental approach (the cloud scanner instrument) that provides the microphysical information missed in current experiments and remote sensing options. Cloud scanner measurements can be performed from aircraft, ground, or satellite by scanning the side of the clouds from the base to the top, providing us with the unique opportunity of obtaining snapshots of the cloud droplet microphysical and thermodynamic states as a function of height and brightness temperature in clouds at several development stages. The brightness temperature profile of the cloud side can be directly associated with the thermodynamic phase of the droplets to provide information on the glaciation temperature as a function of different ambient conditions, aerosol concentration, and type. An aircraft prototype of the cloud scanner was built and flew in a field campaign in Brazil. The CLAIM-3D (3-Dimensional Cloud Aerosol Interaction Mission) satellite concept proposed here combines several techniques to simultaneously measure the vertical profile of cloud microphysics, thermodynamic phase, brightness temperature, and aerosol amount and type in the neighborhood of the clouds. The wide wavelength range, and the use of multi-angle polarization measurements proposed for this mission allow us to estimate the availability and characteristics of aerosol particles acting as cloud condensation nuclei, and their effects on the cloud microphysical structure. These results can provide unprecedented details on the response of cloud droplet microphysics to natural and anthropogenic aerosols in the size scale where the interaction really happens.

scholarly journals Combustion Organic Aerosol as Cloud Condensation Nuclei in Ship Tracks

2000 ◽  
Vol 57 (16) ◽  
pp. 2591-2606 ◽  
Author(s):  
Lynn M. Russell ◽  
Kevin J. Noone ◽  
Ronald J. Ferek ◽  
Robert A. Pockalny ◽  
Richard C. Flagan ◽  
...  
Keyword(s):  
Cloud Condensation Nuclei ◽  
Organic Aerosol ◽  
Condensation Nuclei ◽  
Ship Tracks

scholarly journals Cloud condensation nuclei from the activation with ozone of soot particles sampled from a kerosene diffusion flame

2018 ◽  
Vol 52 (8) ◽  
pp. 814-827 ◽  
Author(s):  
Symphorien Grimonprez ◽  
Alessandro Faccinetto ◽  
Sébastien Batut ◽  
Junteng Wu ◽  
Pascale Desgroux ◽  
...  
Keyword(s):  
Diffusion Flame ◽  
Cloud Condensation Nuclei ◽  
Condensation Nuclei ◽  
Soot Particles

scholarly journals Technical Note: Frenkel Halsey and Hill analysis of water on clay minerals: Toward closure between cloud condensation nuclei activity and water adsorption

2019 ◽  
Author(s):  
Courtney D. Hatch ◽  
Paul R. Tumminello ◽  
Megan A. Cassingham ◽  
Ann L. Greenaway ◽  
Rebecca Meredith ◽  
...  
Keyword(s):  
Water Adsorption ◽  
Cloud Condensation Nuclei ◽  
Cloud Droplet ◽  
Technical Note ◽  
Condensation Nuclei ◽  
Adsorption Parameters ◽  
Climate Effect ◽  
Montmorillonite Clays ◽  
Activation Theory ◽  
Cloud Droplet Number Concentration

Abstract. Insoluble atmospheric aerosol, such as mineral dust, has been identified as an important contributor to the cloud droplet number concentration and indirect climate effect. However, empirically-derived Frenkel-Halsey-Hill (FHH) water adsorption parameters remain the largest source of uncertainty in assessing the effect of insoluble aerosol on climate using the FHH activation theory (FHH-AT). Furthermore, previously reported FHH water adsorption parameters for illite and montmorillonite determined from water adsorption measurements below 100 % RH do not satisfactorily agree with values determined from FHH-AT analysis of experimental cloud condensation nuclei (CCN) measurements under supersaturated conditions. The work reported here uses previously reported experimental water adsorption measurements for illite and montmorillonite clays (Hatch et al., 2012; Hatch et al., 2014) to show that improved analysis methods that account for the surface microstructure are necessary to obtain better agreement of FHH parameters between water adsorption and experimental CCN-derived FHH parameters.

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