scholarly journals The impact of the 1783–1784 AD Laki eruption on global aerosol formation processes and 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 ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Northern Hemisphere ◽  
General Circulation ◽  
Cloud Condensation Nuclei ◽  
General Circulation Models ◽  
Aerosol Formation ◽  
Condensation Nuclei ◽  
Upper Troposphere ◽  
Microphysical Processes ◽  
The Impact

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.

scholarly journals The impact of the 1783–1784 AD Laki eruption on global aerosol formation processes and cloud condensation nuclei

2010 ◽  
Vol 10 (13) ◽  
pp. 6025-6041 ◽  
Author(s):  
A. Schmidt ◽  
K. S. Carslaw ◽  
G. W. Mann ◽  
M. Wilson ◽  
T. J. Breider ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Northern Hemisphere ◽  
General Circulation ◽  
Cloud Condensation Nuclei ◽  
General Circulation Models ◽  
Aerosol Formation ◽  
Condensation Nuclei ◽  
Upper Troposphere ◽  
Microphysical Processes ◽  
The Impact

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.

scholarly journals Weak Land–Atmosphere Coupling Strength in HadAM3: The Role of Soil Moisture Variability

2005 ◽  
Vol 6 (5) ◽  
pp. 670-680 ◽  
Author(s):  
David M. Lawrence ◽  
Julia M. Slingo
Keyword(s):  
Boundary Layer ◽  
Soil Moisture ◽  
Coupling Strength ◽  
General Circulation ◽  
General Circulation Models ◽  
Soil Conditions ◽  
Wide Range ◽  
The Impact ◽  
Soil Moisture Variability ◽  
Moisture Variability

Abstract A recent model intercomparison, the Global Land–Atmosphere Coupling Experiment (GLACE), showed that there is a wide range of land–atmosphere coupling strengths, or the degree that soil moisture affects the generation of precipitation, amongst current atmospheric general circulation models (AGCMs). Coupling strength in the Hadley Centre atmosphere model (HadAM3) is among the weakest of all AGCMs considered in GLACE. Reasons for the weak HadAM3 coupling strength are sought here. In particular, the impact of pervasive saturated soil conditions and low soil moisture variability on coupling strength is assessed. It is found that when the soil model is modified to reduce the occurrence of soil moisture saturation and to encourage soil moisture variability, the soil moisture–precipitation feedback remains weak, even though the relationship between soil moisture and evaporation is strengthened. Composites of the diurnal cycle, constructed relative to soil moisture, indicate that the model can simulate key differences in boundary layer development over wet versus dry soils. In particular, the influence of wet or dry soil on the diurnal cycles of Bowen ratio, boundary layer height, and total heat flux are largely consistent with the observed influence of soil moisture on these properties. However, despite what appears to be successful simulation of these key aspects of the indirect soil moisture–precipitation feedback, the model does not capture observed differences for wet and dry soils in the daily accumulation of boundary layer moist static energy, a crucial feature of the feedback mechanism.

scholarly journals Sensitivity of global cloud condensation nuclei concentrations to primary sulfate emission parameterizations

2011 ◽  
Vol 11 (5) ◽  
pp. 1949-1959 ◽  
Author(s):  
G. Luo ◽  
F. Yu
Keyword(s):  
Boundary Layer ◽  
Compensation Effect ◽  
Particle Number ◽  
Cloud Condensation Nuclei ◽  
Nucleation And Growth ◽  
Ambient Atmosphere ◽  
Condensation Nuclei ◽  
Growth Processes ◽  
Particle Properties ◽  
The Impact

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).

scholarly journals Preconditioning of overcast-to-broken cloud transitions by riming in marine cold air outbreaks

2021 ◽  
Vol 21 (15) ◽  
pp. 12049-12067
Author(s):  
Florian Tornow ◽  
Andrew S. Ackerman ◽  
Ann M. Fridlind
Keyword(s):  
Boundary Layer ◽  
Liquid Water ◽  
Cloud Condensation Nuclei ◽  
Mixed Phase ◽  
Climate Feedback ◽  
Condensation Nuclei ◽  
Cold Air ◽  
Ice Particles ◽  
The Impact ◽  
Cold Air Outbreaks

Abstract. Marine cold air outbreaks (CAOs) commonly form overcast cloud decks that transition into broken cloud fields downwind, dramatically altering the local radiation budget. In this study, we investigate the impact of frozen hydrometeors on these transitions. We focus on a CAO case in the NW Atlantic, the location of the multi-year flight campaign ACTIVATE (Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment). We use MERRA-2 (Modern-Era Retrospective analysis for Research and Applications, version 2) reanalysis fields to drive large eddy simulations with mixed-phase two-moment microphysics in a Lagrangian framework. We find that transitions are triggered by substantial rain (rainwater paths >25 g m−2), and only simulations that allow for aerosol depletion result in sustained breakups, as observed. Using a range of diagnostic ice nucleating particle concentrations, Ninp, we find that increasing ice progressively accelerates transitions, thus abbreviating the overcast state. Ice particles affect the cloud-topped boundary layer evolution, primarily through riming-related processes prior to substantial rain, leading to (1) a reduction in cloud liquid water, (2) early consumption of cloud condensation nuclei, and (3) early and light precipitation cooling and moistening below cloud. We refer to these three effects collectively as “preconditioning by riming”. Greater boundary layer aerosol concentrations available as cloud condensation nuclei (CCN) delay the onset of substantial rain. However, cloud breakup and low CCN concentration final stages are found to be inevitable in this case, due, primarily, to liquid water path buildup. An ice-modulated cloud transition speed suggests the possibility of a negative cloud–climate feedback. To address prevailing uncertainties in the model representation of mixed-phase processes, the magnitude of ice formation and riming impacts and, thereby, the strength of an associated negative cloud–climate feedback process, requires further observational evaluation by targeting riming hot spots with in situ imaging probes that allow for both the characterization of ice particles and abundance of supercooled droplets.

scholarly journals Global and regional modeling of clouds and aerosols in the marine boundary layer during VOCALS: the VOCA intercomparison

2015 ◽  
Vol 15 (1) ◽  
pp. 153-172 ◽  
Author(s):  
M. C. Wyant ◽  
C. S. Bretherton ◽  
R. Wood ◽  
G. R. Carmichael ◽  
A. Clarke ◽  
...  
Keyword(s):  
Boundary Layer ◽  
General Circulation ◽  
Marine Boundary Layer ◽  
Quantitative Estimation ◽  
Cloud Condensation Nuclei ◽  
Cloud Droplet ◽  
General Circulation Models ◽  
Free Troposphere ◽  
Aerosol Cloud ◽  
Aerosol Cloud Interactions

Abstract. A diverse collection of models are used to simulate the marine boundary layer in the southeast Pacific region during the period of the October–November 2008 VOCALS REx (VAMOS Ocean Cloud Atmosphere Land Study Regional Experiment) field campaign. Regional models simulate the period continuously in boundary-forced free-running mode, while global forecast models and GCMs (general circulation models) are run in forecast mode. The models are compared to extensive observations along a line at 20° S extending westward from the South American coast. Most of the models simulate cloud and aerosol characteristics and gradients across the region that are recognizably similar to observations, despite the complex interaction of processes involved in the problem, many of which are parameterized or poorly resolved. Some models simulate the regional low cloud cover well, though many models underestimate MBL (marine boundary layer) depth near the coast. Most models qualitatively simulate the observed offshore gradients of SO2, sulfate aerosol, CCN (cloud condensation nuclei) concentration in the MBL as well as differences in concentration between the MBL and the free troposphere. Most models also qualitatively capture the decrease in cloud droplet number away from the coast. However, there are large quantitative intermodel differences in both means and gradients of these quantities. Many models are able to represent episodic offshore increases in cloud droplet number and aerosol concentrations associated with periods of offshore flow. Most models underestimate CCN (at 0.1% supersaturation) in the MBL and free troposphere. The GCMs also have difficulty simulating coastal gradients in CCN and cloud droplet number concentration near the coast. The overall performance of the models demonstrates their potential utility in simulating aerosol–cloud interactions in the MBL, though quantitative estimation of aerosol–cloud interactions and aerosol indirect effects of MBL clouds with these models remains uncertain.

scholarly journals Microphysical simulations of new particle formation in the upper troposphere and lower stratosphere

2011 ◽  
Vol 11 (17) ◽  
pp. 9303-9322 ◽  
Author(s):  
J. M. English ◽  
O. B. Toon ◽  
M. J. Mills ◽  
F. Yu
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
General Circulation ◽  
Lower Stratosphere ◽  
Three Dimensional ◽  
Circulation Model ◽  
Number Concentration ◽  
Aerosol Formation ◽  
Upper Troposphere ◽  
Microphysical Processes

Abstract. Using a three-dimensional general circulation model with sulfur chemistry and sectional aerosol microphysics (WACCM/CARMA), we studied aerosol formation and microphysics in the upper troposphere and lower stratosphere (UTLS) as well as the middle and upper stratosphere based on three nucleation schemes (two binary homogeneous schemes and an ion-mediated scheme related to one of the binary schemes). Simulations suggest that ion-mediated nucleation rates in the UTLS are 25 % higher than its related binary scheme, but that the rates predicted by the two binary schemes vary by two orders of magnitude. None of the nucleation schemes is superior at matching the limited observations available at the smallest sizes. However, it is found that coagulation, not nucleation, controls number concentration at sizes greater than approximately 10 nm. Therefore, based on this study, processes relevant to atmospheric chemistry and radiative forcing in the UTLS are not sensitive to the choice of nucleation schemes. The dominance of coagulation over other microphysical processes in the UTLS is consistent with other recent work using microphysical models. Simulations using all three nucleation schemes compare reasonably well to observations of size distributions, number concentration across latitude, and vertical profiles of particle mixing ratio in the UTLS. Interestingly, we find that we need to include Van der Waals forces in our coagulation scheme to match the UTLS aerosol concentrations. We conclude that this model can reasonably represent sulfate microphysical processes in the UTLS, and that the properties of particles at atmospherically relevant sizes appear to be insensitive to the details of the nucleation scheme. We also suggest that micrometeorites, which are not included in this model, dominate the aerosol properties in the upper stratosphere above about 30 km.

scholarly journals Impact of aerosol-radiation interaction on new particle formation

2021 ◽  
Author(s):  
Gang Zhao ◽  
Yishu Zhu ◽  
Zhijun Wu ◽  
Taomou Zong ◽  
Jingchuan Chen ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Cloud Condensation Nuclei ◽  
Particle Formation ◽  
Aerosol Size Distribution ◽  
Transfer Model ◽  
New Particle Formation ◽  
Condensation Nuclei ◽  
The Impact ◽  
Different Altitudes ◽  
Upper Boundary

Abstract. New particle formation (NPF) is thought to contribute to half of the global cloud condensation nuclei. A better understanding of the NPF at different altitudes can help assess the impact of NPF on cloud formation and corresponding physical properties. However, NPF is not sufficiently understood in the upper boundary layer because previous studies mainly focus on ground-level measurements. In this study, the developments of aerosol size distribution at different altitudes are characterized based on the field measurement conducted in January 2019, in Beijing, China. We find that the partition of nucleation mode particles at the upper boundary layer is larger than that at the ground, which implies that the nucleation processing is more likely to happen in the upper boundary layer than that at the ground. Results of the radiative transfer model show that the photolysis rates of the nitrogen dioxide and ozone increase with altitude within the boundary layer, which lead to a higher concentration of sulfuric acid at the upper boundary layer than that at the ground. Therefore, the nucleation processing in the upper boundary layer should be stronger than that at the ground, which is consistent with our measurement results. Our study emphasizes the influence of aerosol-radiation interaction on the NPF. These results have the potential to improve our understanding of source of cloud condensation nuclei in global scale due to the impacts of aerosol-radiation interaction.

scholarly journals A global off-line model of size-resolved aerosol microphysics: I. Model development and prediction of aerosol properties

2005 ◽  
Vol 5 (1) ◽  
pp. 179-215 ◽  
Author(s):  
D. V. Spracklen ◽  
K. J. Pringle ◽  
K. S. Carslaw ◽  
M. P. Chipperfield ◽  
G. W. Mann
Keyword(s):  
Boundary Layer ◽  
Sulfuric Acid ◽  
Size Distribution ◽  
Marine Boundary Layer ◽  
Transport Model ◽  
Cloud Condensation Nuclei ◽  
Aerosol Size Distribution ◽  
Sea Spray ◽  
Condensation Nuclei ◽  
Upper Troposphere

Abstract. A GLObal Model of Aerosol Processes (GLOMAP) has been developed as an extension to the TOMCAT 3-D Eulerian off-line chemical transport model. GLOMAP simulates the evolution of the global aerosol size distribution using a sectional two-moment scheme and includes the processes of aerosol nucleation, condensation, growth, coagulation, wet and dry deposition and cloud processing. We describe the results of a global simulation of sulfuric acid and sea spray aerosol. The model captures features of the aerosol size distribution that are well established from observations in the marine boundary layer and free troposphere. Modelled condensation nuclei (CN>3 nm) vary between about 250–500 cm-3 in remote marine boundary layer regions and between 2000 and 10 000 cm-3 (at standard temperature and pressure) in the upper troposphere. Cloud condensation nuclei (CCN) at 0.2% supersaturation vary between about 1000 cm-3 in polluted regions and between 10 and 500 cm-3 in the remote marine boundary layer. New particle formation through sulfuric acid-water binary nucleation occurs predominantly in the upper troposphere, but the model results show that these particles contribute greatly to aerosol concentrations in the marine boundary layer. It is estimated that sea spray emissions account for only ~10% of CCN in the tropical marine boundary layer, but between 20 and 75% in the mid-latitude Southern Ocean.

scholarly journals Sensitivity of global cloud condensation nuclei concentrations to primary sulfate emissions parameterizations

2010 ◽  
Vol 10 (11) ◽  
pp. 27695-27723
Author(s):  
G. Luo ◽  
F. Yu
Keyword(s):  
Boundary Layer ◽  
Growth Process ◽  
Compensation Effect ◽  
Particle Number ◽  
Cloud Condensation Nuclei ◽  
Nucleation And Growth ◽  
Ambient Atmosphere ◽  
Condensation Nuclei ◽  
Particle Properties ◽  
The Impact

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 process 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 calculate tropospheric particle formation and explicitly simulate the condensation of low volatile secondary organic gas (in addition to H2SO4 gas) on nucleated particles. 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%. 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). Our derived impact of primary sulfate emission on global CCN abundance is about a factor of ∼3–7 smaller than those found in previous studies.

scholarly journals Microphysical simulations of new particle formation in the upper troposphere and lower stratosphere

2011 ◽  
Vol 11 (4) ◽  
pp. 12441-12486 ◽  
Author(s):  
J. M. English ◽  
O. B. Toon ◽  
M. J. Mills ◽  
F. Yu
Keyword(s):  
General Circulation ◽  
Lower Stratosphere ◽  
Three Dimensional ◽  
Circulation Model ◽  
Number Concentration ◽  
Aerosol Formation ◽  
Upper Troposphere ◽  
Particle Mixing ◽  
Microphysical Processes ◽  
Atmospherically Relevant

Abstract. Using a three-dimensional general circulation model with sulfur chemistry and sectional aerosol microphysics (WACCM/CARMA), we studied aerosol formation and microphysics in the tropical upper troposphere and lower stratosphere (UTLS) based on three nucleation schemes (two binary homogeneous schemes and an ion-mediated scheme). Simulations suggest that ion-mediated nucleation rates in the UTLS are 25% higher than binary rates, but that the rates predicted by the two binary schemes vary by two orders of magnitude. However, it is found that coagulation, not nucleation, controls number concentration at sizes greater than approximately 10 nm. Therefore, based on this study, atmospherically relevant processes in the UTLS are not sensitive to the choice of nucleation schemes. The dominance of coagulation over other microphysical processes is consistent with other recent work using microphysical models. Simulations using all three nucleation schemes compare reasonably well to observations of size distributions, number concentration across latitude, and vertical profiles of particle mixing ratio in the UTLS. Interestingly, we find we need to include Van der Waals forces in our coagulation scheme to match the UTLS aerosol concentrations. We conclude that this model can accurately represent sulfate microphysical processes in the UTLS, and that the properties of particles at atmospherically relevant sizes are not sensitive to the details of the nucleation scheme. We also suggest that micrometeorites, which are not included in this model, dominate the aerosol properties in the upper stratosphere above about 30 km.

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