scholarly journals Quantifying Long‐Term Seasonal and Regional Impacts of North American Fire Activity on Continental Boundary Layer Aerosols and Cloud Condensation Nuclei

2020 ◽  
Vol 7 (12) ◽  
Author(s):  
Timothy Logan ◽  
Xiquan Dong ◽  
Baike Xi ◽  
Xiaojian Zheng ◽  
Yuan Wang ◽  
...  
2020 ◽  
Author(s):  
Guangjie Zheng ◽  
Chongai Kuang ◽  
Janek Uin ◽  
Thomas Watson ◽  
Jian Wang

Abstract. Marine low clouds strongly influence global climate, and their radiative effects are particularly susceptible to the concentration of cloud condensation nuclei (CCN). One major source of CCN is condensational growth of pre-CCN particles, and sulfate has long been considered the major condensing species in remote marine boundary layer. While some studies suggested that secondary organic species can contribute to the particle growth, its importance remains unclear. Here we present the first long-term observational evidence that organics play an important role in particle growth over remote oceans. To the contrary of traditional thinking, sulfate dominated condensational growth for only a small (∼18 %) fraction of the 62 observed growth events, even fewer than the organic-dominated events (24 %). During most (58 %) growth events, the major condensing species included both organics and sulfate. Potential precursors of the secondary organics are volatile organic compounds from ocean biological activities and those produced by the air-sea interfacial oxidation. Our results indicate that the condensation of secondary organics contributes strongly to the growth of pre-CCN particles, and thereby the CCN population over remote oceans.


2020 ◽  
Vol 20 (21) ◽  
pp. 12515-12525
Author(s):  
Guangjie Zheng ◽  
Chongai Kuang ◽  
Janek Uin ◽  
Thomas Watson ◽  
Jian Wang

Abstract. Marine low clouds strongly influence global climate, and their radiative effects are particularly susceptible to the concentration of cloud condensation nuclei (CCN). One major source of CCN is the condensational growth of pre-CCN particles, and sulfate has long been considered the major condensing species in the remote marine boundary layer. While some studies have suggested that secondary organic species can contribute to particle growth, its importance remains unclear. Here we present the first long-term observational evidence that organics play an important role in particle growth over remote oceans. To the contrary of traditional thinking, sulfate dominated condensational growth for only a small (∼18 %) fraction of the 62 observed growth events, even fewer than the organic-dominated events (24 %). During most (58 %) growth events, the major condensing species included both organics and sulfate. Potential precursors of the secondary organics are volatile organic compounds from ocean biological activities and those produced by the air–sea interfacial oxidation. Our results indicate that the condensation of secondary organics contributes strongly to the growth of pre-CCN particles and thereby the CCN population over remote oceans.


2016 ◽  
Author(s):  
Julia Burkart ◽  
Megan D. Willis ◽  
Heiko Bozem ◽  
Jennie L. Thomas ◽  
Kathy Law ◽  
...  

Abstract. The Arctic is extremely sensitive to climate change. Shrinking sea ice extent increases the area covered by open ocean during Arctic summer, which impacts the surface albedo and aerosol and cloud properties among many things. In this context extensive aerosol measurements (aerosol composition, particle number and size, cloud condensation nuclei, and trace gases) were made during 11 flights of the NETCARE July, 2014 airborne campaign conducted from Resolute Bay, Nunavut (74N, 94W). Flights routinely included vertical profiles from about 60 to 3000 m a.g.l. as well as several low-level horizontal transects over open ocean, fast ice, melt ponds, and polynyas. Here we discuss the vertical distribution of ultrafine particles (UFP, particle diameter, dp: 5–20 nm), size distributions of larger particles (dp: 20 nm to 1 μm), and cloud condensation nuclei (CCN, supersaturation = 0.6 %) in relation to meteorological conditions and underlying surfaces. UFPs were observed predominantly within the boundary layer, where concentrations were often several hundreds to a few thousand particles per cubic centimeter. Occasionally, particle concentrations below 10 cm−3 were found. The highest UFP concentrations were observed above open ocean and at the top of low-level clouds, whereas numbers over ice-covered regions were substantially lower. Overall, UFP formation events were frequent in a clean boundary layer with a low condensation sink. In a few cases this ultrafine mode extended to sizes larger than 40 nm, suggesting that these UFP can grow into a size range where they can impact clouds and therefore climate.


2016 ◽  
Vol 97 (12) ◽  
pp. 2329-2342 ◽  
Author(s):  
Jose D. Fuentes ◽  
Marcelo Chamecki ◽  
Rosa Maria Nascimento dos Santos ◽  
Celso Von Randow ◽  
Paul C. Stoy ◽  
...  

Abstract We describe the salient features of a field study whose goals are to quantify the vertical distribution of plant-emitted hydrocarbons and their contribution to aerosol and cloud condensation nuclei production above a central Amazonian rain forest. Using observing systems deployed on a 50-m meteorological tower, complemented with tethered balloon deployments, the vertical distribution of hydrocarbons and aerosols was determined under different boundary layer thermodynamic states. The rain forest emits sufficient reactive hydrocarbons, such as isoprene and monoterpenes, to provide precursors of secondary organic aerosols and cloud condensation nuclei. Mesoscale convective systems transport ozone from the middle troposphere, enriching the atmospheric boundary layer as well as the forest canopy and surface layer. Through multiple chemical transformations, the ozone-enriched atmospheric surface layer can oxidize rain forest–emitted hydrocarbons. One conclusion derived from the field studies is that the rain forest produces the necessary chemical species and in sufficient amounts to undergo oxidation and generate aerosols that subsequently activate into cloud condensation nuclei.


2010 ◽  
Vol 10 (2) ◽  
pp. 3189-3228
Author(s):  
A. Schmidt ◽  
K. S. Carslaw ◽  
G. W. Mann ◽  
B. M. Wilson ◽  
T. J. Breider ◽  
...  

Abstract. The 1783–1784 AD Laki flood lava eruption commenced on 8 June 1783 and released 122 Tg of sulphur dioxide gas over the course of 8 months into the upper troposphere and lower stratosphere above Iceland. Previous studies have examined the impact of the Laki eruption on sulphate aerosol and climate using general circulation models. Here, we study the impact on aerosol microphysical processes, including the nucleation of new particles and their growth to cloud condensation nuclei (CCN) using a comprehensive Global Model of Aerosol Processes (GLOMAP). Total particle concentrations in the free troposphere increase by a factor ~16 over large parts of the Northern Hemisphere in the 3 months following the onset of the eruption. Particle concentrations in the boundary layer increase by a factor 2 to 5 in regions as far away as North America, the Middle East and Asia due to long-range transport of nucleated particles. CCN concentrations (at 0.22% supersaturation) increase by a factor 65 in the upper troposphere with maximum changes in 3-month zonal mean concentrations of ~1400 cm−3 at high northern latitudes. 3-month zonal mean CCN concentrations in the boundary layer at the latitude of the eruption increase by up to a factor 26, and averaged over the Northern Hemisphere, the eruption caused a factor 4 increase in CCN concentrations at low-level cloud altitude. The simulations show that the Laki eruption would have completely dominated as a source of CCN in the pre-industrial atmosphere. The model also suggests an impact of the eruption in the Southern Hemisphere, where CCN concentrations are increased by up to a factor 1.4 at 20° S. Our model simulations suggest that the impact of an equivalent wintertime eruption on upper tropospheric CCN concentrations is only about one-third of that of a summertime eruption. The simulations show that the microphysical processes leading to the growth of particles to CCN sizes are fundamentally different after an eruption when compared to the unperturbed atmosphere, underlining the importance of using a fully coupled microphysics model when studying long-lasting, high-latitude eruptions.


2011 ◽  
Vol 11 (1) ◽  
pp. 885-916 ◽  
Author(s):  
H. Wang ◽  
P. J. Rasch ◽  
G. Feingold

Abstract. We use a cloud-system-resolving model to study marine-cloud brightening. We examine how injected aerosol particles that act as cloud condensation nuclei (CCN) are transported within the marine boundary layer and how the additional particles in clouds impact cloud microphysical processes, and feedback on dynamics. Results show that the effectiveness of cloud brightening depends strongly on meteorological and background aerosol conditions. Cloud albedo enhancement is very effective in a weakly precipitating boundary layer and in CCN-limited conditions preceded by heavy and/or persistent precipitation. The additional CCN help sustain cloud water by weakening the precipitation substantially in the former case and preventing the boundary layer from collapse in the latter. For a given amount of injected CCN, the injection method (i.e., number and distribution of sprayers) is critical to the spatial distribution of these CCN. Both the areal coverage and the number concentration of injected particles are key players but neither one always emerges as more important than the other. The same amount of injected material is much less effective in either strongly precipitating clouds or polluted clouds, and it is ineffective in a relatively dry boundary layer that supports clouds of low liquid water path. In the polluted case and "dry" case, the CCN injection increases drop number concentration but lowers supersaturation and liquid water path. As a result, the cloud experiences very weak albedo enhancement, regardless of the injection method.


2011 ◽  
Vol 11 (5) ◽  
pp. 1949-1959 ◽  
Author(s):  
G. Luo ◽  
F. Yu

Abstract. The impact of primary sulfate emissions on cloud condensation nuclei (CCN) concentrations, one of the major uncertainties in global CCN predictions, depends on the fraction of sulfur mass emitted as primary sulfate particles (fsulfate), the fraction of primary sulfate mass distributed into the nucleation mode particles (fnucl), and the nucleation and growth processes in the ambient atmosphere. Here, we use a global size-resolved aerosol microphysics model recently developed to study how the different parameterizations of primary sulfate emission affect particle properties and CCN abundance. Different from previous studies, we use the ion-mediated nucleation scheme to simulate tropospheric particle formation. The kinetic condensation of low volatile secondary organic gas (SOG) (in addition to H2SO4 gas) on nucleated particles is calculated based on our new scheme that considers the SOG volatility changes arising from the oxidation aging. Our simulations show a compensation effect of nucleation to primary sulfate emission. We find that the change of fnucl from 5% to 15% has a more significant impact on the simulated particle number budget than that of fsulfate within the range of 2.5–5%. Based on our model configurations, an increase of fsulfate from 0% to 2.5% (with fnucl = 5%) does not improve the agreement between simulated and observed annual mean number concentrations of particles >10 nm at 21 stations but further increase of either fsulfate from 2.5% to 5% (with fnucl = 5%) or fnucl from 5% to 15% (with fsulfate = 2.5%) substantially deteriorates the agreement. For fsulfate of 2.5%–5% and fnucl of 5%, our simulations indicate that the global CCN at supersaturation of 0.2% increases by 8–11% in the boundary layer and 3–5% in the whole troposphere (compared to the case with fsulfate=0).


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