scholarly journals Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model

2010 ◽  
Vol 3 (2) ◽  
pp. 519-551 ◽  
Author(s):  
G. W. Mann ◽  
K. S. Carslaw ◽  
D. V. Spracklen ◽  
D. A. Ridley ◽  
P. T. Manktelow ◽  
...  

Abstract. A new version of the Global Model of Aerosol Processes (GLOMAP) is described, which uses a two-moment pseudo-modal aerosol dynamics approach rather than the original two-moment bin scheme. GLOMAP-mode simulates the multi-component global aerosol, resolving sulfate, sea-salt, dust, black carbon (BC) and particulate organic matter (POM), the latter including primary and biogenic secondary POM. Aerosol processes are simulated in a size-resolved manner including primary emissions, secondary particle formation by binary homogeneous nucleation of sulfuric acid and water, particle growth by coagulation, condensation and cloud-processing and removal by dry deposition, in-cloud and below-cloud scavenging. A series of benchmark observational datasets are assembled against which the skill of the model is assessed in terms of normalised mean bias (b) and correlation coefficient (R). Overall, the model performs well against the datasets in simulating concentrations of aerosol precursor gases, chemically speciated particle mass, condensation nuclei (CN) and cloud condensation nuclei (CCN). Surface sulfate, sea-salt and dust mass concentrations are all captured well, while BC and POM are biased low (but correlate well). Surface CN concentrations compare reasonably well in free troposphere and marine sites, but are underestimated at continental and coastal sites related to underestimation of either primary particle emissions or new particle formation. The model compares well against a compilation of CCN observations covering a range of environments and against vertical profiles of size-resolved particle concentrations over Europe. The simulated global burden, lifetime and wet removal of each of the simulated aerosol components is also examined and each lies close to multi-model medians from the AEROCOM model intercomparison exercise.

2010 ◽  
Vol 3 (2) ◽  
pp. 651-734 ◽  
Author(s):  
G. W. Mann ◽  
K. S. Carslaw ◽  
D. V. Spracklen ◽  
D. A. Ridley ◽  
P. T. Manktelow ◽  
...  

Abstract. A new version of the Global Model of Aerosol Processes (GLOMAP) is described, which uses a two-moment modal aerosol scheme rather than the original two-moment bin scheme. GLOMAP-mode simulates the multi-component global aerosol, resolving sulphate, sea-salt, dust, black carbon (BC) and particulate organic matter (POM), the latter including primary and biogenic secondary POM. Aerosol processes are simulated in a size-resolved manner including primary emissions, secondary particle formation by binary homogeneous nucleation of sulphuric acid and water, particle growth by coagulation, condensation and cloud-processing and removal by dry deposition, in-cloud and below-cloud scavenging. A series of benchmark observational datasets are assembled against which the skill of the model is assessed in terms of normalised mean bias (b) and correlation coefficient (R). Overall, the model performs well against the datasets in simulating concentrations of aerosol precursor gases, chemically speciated particle mass, condensation nuclei (CN) and cloud condensation nuclei (CCN). Surface sulphate, sea-salt and dust mass concentrations are all captured well, while BC and POM are biased low (but correlate well). Surface CN concentrations compare reasonably well in free troposphere and marine sites, but are underestimated at continental and coastal sites related to underestimation of either primary particle emissions or new particle formation. The model compares well against a compilation of CCN observations covering a range of environments and against vertical profiles of size-resolved particle concentrations over Europe. The simulated global burden, lifetime and wet removal of each of the simulated aerosol components is also examined and each lies close to multi-model medians from the AEROCOM model intercomparison exercise.


2012 ◽  
Vol 12 (1) ◽  
pp. 623-689 ◽  
Author(s):  
G. W. Mann ◽  
K. S. Carslaw ◽  
D. A. Ridley ◽  
D. V. Spracklen ◽  
K. J. Pringle ◽  
...  

Abstract. A global modal aerosol microphysics module (GLOMAP-mode) is evaluated and improved by comparing against a sectional version (GLOMAP-bin) and observations in the same 3-D global offline chemistry transport model. With both schemes, the model captures the main features of the global particle size distribution, with sub-micron aerosol approximately unimodal in continental regions and bi-modal in marine regions. Initial bin-mode comparisons showed that various size distribution parameter settings (mode widths and inter-modal separation sizes) resulted in clear biases compared to the sectional scheme. By adjusting these parameters in the modal scheme, much better agreement is achieved against the bin scheme and observations. Surface mass of sulphate, sea-salt, black carbon (BC) and organic carbon (OC) are, on the annual mean, within 25 % in the two schemes in nearly all regions. On the annual mean, surface level concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), surface area density and condensation sink also compare within 25 % in most regions. However, marine CCN concentrations between 30° N and 30° S are systematically higher in the modal scheme, by 25–60 %, which we attribute to differences in size-resolved particle growth or cloud-processing. Larger differences also exist in regions or seasons dominated by biomass burning and in free-troposphere and high-latitude regions. Indeed, in the free-troposphere, GLOMAP-mode BC is a factor 2–4 higher than GLOMAP-bin, likely due to differences in size-resolved scavenging. Nevertheless, in most parts of the atmosphere, we conclude that bin-mode differences are much less than model-observation differences, although some processes are missing in these runs which may pose a bigger challenge to modal schemes (e.g. boundary layer nucleation, ultra-fine sea-spray). The findings here underline the need for a spectrum of complexity in global models, with size-resolved aerosol properties predicted by modal schemes needing to be continually benchmarked and improved against freely evolving sectional schemes and observations.


2016 ◽  
Vol 16 (22) ◽  
pp. 14635-14656 ◽  
Author(s):  
Carlos Eduardo Souto-Oliveira ◽  
Maria de Fátima Andrade ◽  
Prashant Kumar ◽  
Fábio Juliano da Silva Lopes ◽  
Marly Babinski ◽  
...  

Abstract. Atmospheric aerosol is the primary source of cloud condensation nuclei (CCN). The microphysics and chemical composition of aerosols can affect cloud development and the precipitation process. Among studies conducted in Latin America, only a handful have reported the impact of urban aerosol on CCN activation parameters such as activation ratio (AR) and activation diameter (Dact). With over 20 million inhabitants, the Metropolitan Area of São Paulo (MASP) is the largest megacity in South America. To our knowledge, this is the first study to assess the impact that remote sources and new particle formation (NPF) events have on CCN activation properties in a South American megacity. The measurements were conducted in the MASP between August and September 2014. We measured the CCN within the 0.2–1.0 % range of supersaturation, together with particle number concentration (PNC) and particle number distribution (PND), as well as trace-element concentrations and black carbon (BC). NPF events were identified on 35 % of the sampling days. Combining multivariate analysis in the form of positive matrix factorization (PMF) with an aerosol profile from lidar and HYSPLIT model analyses allowed us to identify the main contribution of vehicular traffic on all days and sea salt and biomass burning from remote regions on 28 and 21 % of the sampling days, respectively. The AR and Dact parameters showed distinct patterns for daytime with intense vehicular traffic and nighttime periods. For example, CCN activation was lower during the daytime than during the nighttime periods, a pattern that was found to be associated mainly with local road-traffic emissions. A decrease in CCN activation was observed on the NPF event days, mainly due to high concentrations of particles with smaller diameters. We also found that aerosols from sea salt, industrial emissions, and biomass burning had minor effects on Dact. For example, nights with biomass burning and vehicular emissions showed slightly lower CCN activation properties than sea-salt, industrial and non-event nights. Our results show that particulate matter from local vehicular emissions during the daytime has a greater effect on CCN activation parameters than that from remote sources.


2020 ◽  
Author(s):  
Kevin J. Sanchez ◽  
Gregory C. Roberts ◽  
Georges Saliba ◽  
Lynn M. Russell ◽  
Cynthia Twohy ◽  
...  

Abstract. Long-range transport of biogenic emissions from the coast of Antarctica, precipitation scavenging, and cloud processing are the main processes that influence the observed variability in Southern Ocean (SO) marine boundary layer (MBL) condensation nuclei (CN) and cloud condensation nuclei (CCN) concentrations during the austral summer. Airborne particle measurements on the HIAPER GV from north-south transects between Hobart, Tasmania and 62° S during the Southern Ocean Clouds, Radiation Aerosol Transport Experimental Study (SOCRATES) were separated into four regimes comprising combinations of high and low concentrations of CCN and CN. In 5-day HYSPLIT back trajectories, air parcels with elevated CCN concentrations were almost always shown to have crossed the Antarctic coast, a location with elevated phytoplankton emissions relative to the rest of the SO. The presence of high CCN concentrations was also consistent with high cloud fractions over their trajectory, suggesting there was substantial growth of biogenically formed particles through cloud processing. Cases with low cloud fraction, due to the presence of cumulus clouds, had high CN concentrations, consistent with previously reported new particle formation in cumulus outflow regions. Measurements associated with elevated precipitation during the previous 1.5-days of their trajectory had low CCN concentrations indicating CCN were effectively scavenged by precipitation. A course-mode fitting algorithm was used to determine the primary marine aerosol (PMA) contribution which accounted for  0.07 µm) indicated that particle formation occurs more frequently above the MBL; however, the growth of recently formed particles typically occurs in the MBL, consistent with cloud processing and the condensation of volatile compound oxidation products. CCN measurements on the R/V Investigator as part of the second Clouds, Aerosols, Precipitation, Radiation and atmospheric Composition Over the southeRn Ocean (CAPRICORN-2) campaign were also conducted during the same period as the SOCRATES study. The R/V Investigator observed elevated CCN concentrations near Australia, likely due to continental and coastal biogenic emissions. The Antarctic coastal source of CCN from the south as well as CCN sources from the mid-latitudes create a latitudinal gradient in CCN concentration with an observed minimum in the SO between 55° S and 60° S. The SOCRATES airborne measurements are not influenced by Australian continental emissions, but still show evidence of elevated CCN concentrations to the south of 60° S, consistent with biogenic coastal emissions. In addition, a latitudinal gradient in the particle composition is observed; more hygroscopic particles to the north, consistent with a greater fraction of sea salt from PMA, and more sulfate and organic particles to the south, which are likely from biogenic sources in coastal Antarctica.


2021 ◽  
Vol 21 (5) ◽  
pp. 3427-3446
Author(s):  
Kevin J. Sanchez ◽  
Gregory C. Roberts ◽  
Georges Saliba ◽  
Lynn M. Russell ◽  
Cynthia Twohy ◽  
...  

Abstract. Long-range transport of biogenic emissions from the coast of Antarctica, precipitation scavenging, and cloud processing are the main processes that influence the observed variability in Southern Ocean (SO) marine boundary layer (MBL) condensation nuclei (CN) and cloud condensation nuclei (CCN) concentrations during the austral summer. Airborne particle measurements on the HIAPER GV from north–south transects between Hobart, Tasmania, and 62∘ S during the Southern Ocean Clouds, Radiation Aerosol Transport Experimental Study (SOCRATES) were separated into four regimes comprising combinations of high and low concentrations of CCN and CN. In 5 d HYSPLIT back trajectories, air parcels with elevated CCN concentrations were almost always shown to have crossed the Antarctic coast, a location with elevated phytoplankton emissions relative to the rest of the SO in the region south of Australia. The presence of high CCN concentrations was also consistent with high cloud fractions over their trajectory, suggesting there was substantial growth of biogenically formed particles through cloud processing. Cases with low cloud fraction, due to the presence of cumulus clouds, had high CN concentrations, consistent with previously reported new particle formation in cumulus outflow regions. Measurements associated with elevated precipitation during the previous 1.5 d of their trajectory had low CCN concentrations indicating CCN were effectively scavenged by precipitation. A coarse-mode fitting algorithm was used to determine the primary marine aerosol (PMA) contribution, which accounted for <20 % of CCN (at 0.3 % supersaturation) and cloud droplet number concentrations. Vertical profiles of CN and large particle concentrations (Dp>0.07 µm) indicated that particle formation occurs more frequently above the MBL; however, the growth of recently formed particles typically occurs in the MBL, consistent with cloud processing and the condensation of volatile compound oxidation products. CCN measurements on the R/V Investigator as part of the second Clouds, Aerosols, Precipitation, Radiation and atmospheric Composition Over the southeRn Ocean (CAPRICORN-2) campaign were also conducted during the same period as the SOCRATES study. The R/V Investigator observed elevated CCN concentrations near Australia, likely due to continental and coastal biogenic emissions. The Antarctic coastal source of CCN from the south, CCN sources from the midlatitudes, and enhanced precipitation sink in the cyclonic circulation between the Ferrel and polar cells (around 60∘ S) create opposing latitudinal gradients in the CCN concentration with an observed minimum in the SO between 55 and 60∘ S. The SOCRATES airborne measurements are not influenced by Australian continental emissions but still show evidence of elevated CCN concentrations to the south of 60∘ S, consistent with biogenic coastal emissions. In addition, a latitudinal gradient in the particle composition, south of the Australian and Tasmanian coasts, is apparent in aerosol hygroscopicity derived from CCN spectra and aerosol particle size distribution. The particles are more hygroscopic to the north, consistent with a greater fraction of sea salt from PMA, and less hygroscopic to the south as there is more sulfate and organic particles originating from biogenic sources in coastal Antarctica.


2021 ◽  
Vol 21 (1) ◽  
pp. 183-200
Author(s):  
Liya Ma ◽  
Yujiao Zhu ◽  
Mei Zheng ◽  
Yele Sun ◽  
Lei Huang ◽  
...  

Abstract. The growth of newly formed particles with diameters from ∼ 10 nm to larger sizes was investigated in Beijing's urban atmosphere during 10–23 December 2011, 12–27 April 2012, and June–August 2014. In 11 out of 27 new particle formation (NPF) events during June–August, the maximum geometric median diameter (Dpgmax) of newly formed particles exceeded 75 nm, and the grown new particles may contribute to the population of cloud condensation nuclei. In contrast, no apparent growth in new particles with Dpgmax < 20 nm was observed in all of the events in December, in approximately half of the NPF events in April, and in only two events during June–August. New particles observed in the latter NPF events were too small to be activated as cloud condensation nuclei. Apparent new particle growth with Dpgmax ≤ 50 nm was observed in the remaining 18 NPF events. The 11 NPF events during June–August with Dpgmax exceeding 75 nm were analyzed in detail. The particle growth patterns can be clearly classified into three types: one-stage growth and two-stage growth-A and growth-B patterns. The one-stage growth pattern is characterized by a continuous increase in Dpg with Dpgmax ≥ 80 nm (4 out of 11 NPF events), and the two-stage growth-A and growth-B patterns are characterized by no apparent growth and shrinkage of particles, respectively, in the middle 2–4 h of the growth period (7 out of 11 NPF events). Combining the observations of gaseous pollutants and measured (or modeled) concentrations of particulate chemical species, the three growth patterns were discussed in terms of the spatial heterogeneity of NPF, formation of secondary aerosols, and evaporation of semivolatile particulates. Secondary organic species and NH4NO3 were argued to be two major contributors to the growth of new particles, but NH4NO3 likely contributed to growth only in the late afternoon and/or at nighttime.


Nature ◽  
2019 ◽  
Vol 574 (7778) ◽  
pp. 399-403 ◽  
Author(s):  
Christina J. Williamson ◽  
Agnieszka Kupc ◽  
Duncan Axisa ◽  
Kelsey R. Bilsback ◽  
ThaoPaul Bui ◽  
...  

2020 ◽  
Vol 20 (10) ◽  
pp. 5911-5922 ◽  
Author(s):  
Hing Cho Cheung ◽  
Charles Chung-Kuang Chou ◽  
Celine Siu Lan Lee ◽  
Wei-Chen Kuo ◽  
Shuenn-Chin Chang

Abstract. The chemical composition of fine particulate matter (PM2.5), the size distribution and number concentration of aerosol particles (NCN), and the number concentration of cloud condensation nuclei (NCCN) were measured at the northern tip of Taiwan during an intensive observation experiment from April 2017 to March 2018. The parameters of aerosol hygroscopicity (i.e., activation ratio, activation diameter and kappa of CCN) were retrieved from the measurements. Significant variations were found in the hygroscopicity of aerosols (kappa – κ – of 0.18–0.56, for water vapor supersaturation – SS – of 0.12 %–0.80 %), which were subject to various pollution sources, including aged air pollutants originating in eastern and northern China and transported by the Asian continental outflows and fresh particles emitted from local sources and distributed by land–sea breeze circulations as well as produced by processes of new particle formation (NPF). Cluster analysis was applied to the back trajectories of air masses to investigate their respective source regions. The results showed that aerosols associated with Asian continental outflows were characterized by lower NCN and NCCN values and by higher kappa values of CCN, whereas higher NCN and NCCN values with lower kappa values of CCN were observed in the aerosols associated with local air masses. Besides, it was revealed that the kappa value of CCN exhibited a decrease during the early stage of an event of new particle formation, which turned to an increasing trend over the later period. The distinct features in the hygroscopicity of aerosols were found to be consistent with the characteristics in the chemical composition of PM2.5. This study has depicted a clear seasonal characteristic of hygroscopicity and CCN activity under the influence of a complex mixture of pollutants from different regional and/or local pollution sources. Nevertheless, the mixing state and chemical composition of the aerosols critically influence the aerosol hygroscopicity, and further investigations are necessary to elucidate the atmospheric processing involved in the CCN activation in coastal areas.


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