scholarly journals Evaluation of a global aerosol microphysics model against size-resolved particle statistics in the marine atmosphere

2007 ◽  
Vol 7 (8) ◽  
pp. 2073-2090 ◽  
Author(s):  
D. V. Spracklen ◽  
K. J. Pringle ◽  
K. S. Carslaw ◽  
G. W. Mann ◽  
P. Manktelow ◽  
...  

Abstract. A statistical synthesis of marine aerosol measurements from experiments in four different oceans is used to evaluate a global aerosol microphysics model (GLOMAP). We compare the model against observed size resolved particle concentrations, probability distributions, and the temporal persistence of different size particles. We attempt to explain the observed sub-micrometre size distributions in terms of sulfate and sea spray and quantify the possible contributions of anthropogenic sulfate and carbonaceous material to the number and mass distribution. The model predicts a bimodal size distribution that agrees well with observations as a grand average over all regions, but there are large regional differences. Notably, observed Aitken mode number concentrations are more than a factor 10 higher than in the model for the N Atlantic but a factor 7 lower than the model in the NW Pacific. We also find that modelled Aitken mode and accumulation mode geometric mean diameters are generally smaller in the model by 10–30%. Comparison with observed free tropospheric Aitken mode distributions suggests that the model underpredicts growth of these particles during descent to the marine boundary layer (MBL). Recent observations of a substantial organic component of free tropospheric aerosol could explain this discrepancy. We find that anthropogenic continental material makes a substantial contribution to N Atlantic MBL aerosol, with typically 60–90% of sulfate across the particle size range coming from anthropogenic sources, even if we analyse air that has spent an average of >120 h away from land. However, anthropogenic primary black carbon and organic carbon particles (at the emission size and quantity assumed here) do not explain the large discrepancies in Aitken mode number. Several explanations for the discrepancy are suggested. The lack of lower atmospheric particle formation in the model may explain low N Atlantic particle concentrations. However, the observed and modelled particle persistence at Cape Grim in the Southern Ocean, does not reveal a diurnal cycle consistent with a photochemically driven local particle source. We also show that a physically based cloud drop activation scheme better explains the observed change in accumulation mode geometric mean diameter with particle number.

2006 ◽  
Vol 6 (5) ◽  
pp. 8871-8915
Author(s):  
D. V. Spracklen ◽  
K. J. Pringle ◽  
K. S. Carslaw ◽  
G. W. Mann ◽  
P. Manktelow ◽  
...  

Abstract. A statistical synthesis of marine aerosol measurements from experiments in four different oceans is used to evaluate a global aerosol microphysics model (GLOMAP). We compare the model against observed size resolved particle concentrations, probability distributions, and the temporal persistence of different size particles. We attempt to explain the observed size distributions in terms of sulfate and sea spray and quantify the possible contributions of anthropogenic sulfate and carbonaceous material to the number and mass distribution. The model predicts a bimodal size distribution that agrees well with observations as a grand average over all regions, but there are large regional differences. Notably, observed Aitken mode number concentrations are more than a factor 10 higher than in the model for the N Atlantic but a factor 7 lower than the model in the NW Pacific. We also find that modelled Aitken mode and accumulation mode geometric mean diameters are generally smaller in the model by 10–30%. Comparison with observed free tropospheric Aitken mode distributions suggests that the model underpredicts growth of these particles during descent to the MBL. Recent observations of a substantial organic component of free tropospheric aerosol could explain this discrepancy. We find that anthropogenic continental material makes a substantial contribution to N Atlantic marine boundary layer (MBL) aerosol, with typically 60–90% of sulfate across the particle size range coming from anthropogenic sources, even if we analyse air that has spent an average of >120 h away from land. However, anthropogenic primary black carbon and organic carbon particles do not explain the large discrepancies in Aitken mode number. Several explanations for the discrepancy are suggested. The lack of lower atmospheric particle formation in the model may explain low N Atlantic particle concentrations. However, the observed and modelled particle persistence at Cape Grim in the Southern Ocean, does not reveal a diurnal cycle consistent with a photochemically driven local particle source. We also show that a physically based cloud drop activation scheme is needed to explain the observed change in accumulation mode geometric mean diameter with particle number.


2005 ◽  
Vol 5 (6) ◽  
pp. 1527-1543 ◽  
Author(s):  
R. Krejci ◽  
J. Ström ◽  
M. de Reus ◽  
J. Williams ◽  
H. Fischer ◽  
...  

Abstract. We present measurements of aerosol physico-chemical properties below 5 km altitude over the tropical rain forest and the marine boundary layer (MBL) obtained during the LBA-CLAIRE 1998 project. The MBL aerosol size distribution some 50-100km of the coast of French Guyana and Suriname showed a bi-modal shape typical of aged and cloud processed aerosol. The average particle number density in the MBL was 383cm-3. The daytime mixed layer height over the rain forest for undisturbed conditions was estimated to be between 1200-1500m. During the morning hours the height of the mixed layer increased by 144-180mh-1. The median daytime aerosol number density in the mixed layer increased from 450cm-3 in the morning to almost 800cm-3 in the late afternoon. The evolution of the aerosol size distribution in the daytime mixed layer over the rain forest showed two distinct patterns. Between dawn and midday, the Aitken mode particle concentrations increased, whereas later during the day, a sharp increase of the accumulation mode aerosol number densities was observed, resulting in a doubling of the morning accumulation mode concentrations from 150cm-3 to 300cm-3. Potential sources of the Aitken mode particles are discussed here including the rapid growth of ultrafine aerosol particles formed aloft and subsequently entrained into the mixed layer, as well as the contribution of emissions from the tropical vegetation to Aitken mode number densities. The observed increase of the accumulation mode aerosol number densities is attributed to the combined effect of: the direct emissions of primary biogenic particles from the rain forest and aerosol in-cloud processing by shallow convective clouds. Based on the similarities among the number densities, the size distributions and the composition of the aerosol in the MBL and the nocturnal residual layer we propose that the air originating in the MBL is transported above the nocturnal mixed layer up to 300-400km inland over the rain forest by night without significant processing.


2004 ◽  
Vol 4 (3) ◽  
pp. 3565-3606
Author(s):  
R. Krejci ◽  
J. Ström ◽  
M. de Reus ◽  
J. Williams ◽  
H. Fischer ◽  
...  

Abstract. We present measurements of aerosol physico-chemical properties below 5 km altitude over the tropical rain forest and the marine boundary layer (MBL) obtained during the LBA-CLAIRE 1998 project. The MBL aerosol size distribution some 50–100 km of the coast of French Guyana and Suriname showed a bi-modal shape typical of aged and cloud processed aerosol. The average particle number density in the MBL was 383 cm−3. The daytime mixed layer height over the rain forest for undisturbed conditions was estimated to be between 1200–1500 m. During the morning hours the height of the mixed layer increased by 4–5 cm s−1. The median daytime aerosol number density in the mixed layer increased from 450 cm−3 in the morning to almost 800 cm−3 in the late afternoon. The evolution of the aerosol size distribution in the daytime mixed layer over the rain forest showed two distinct patterns. Between dawn and midday, the Aitken mode particle concentrations increased, whereas later during the day, a sharp increase of the accumulation mode aerosol number densities was observed, resulting in a doubling of the morning accumulation mode concentrations from 150 cm−3 to 300 cm−3. Potential sources of the Aitken mode particles are discussed here including the rapid growth of ultrafine aerosol particles formed aloft and subsequently entrained into the mixed layer, as well as the contribution of emissions from the tropical vegetation to Aitken mode number densities. The observed increase of the accumulation mode aerosol number densities is attributed to the combined effect of: the direct emissions of primary biogenic particles from the rain forest and aerosol in-cloud processing by shallow convective clouds. Based on the similarities among the number densities, the size distributions and the composition of the aerosol in the MBL and the nocturnal residual layer we propose that the air originating in the MBL is transported above the nocturnal mixed layer up to 300–400 km inland over the rain forest by night without significant processing.


2021 ◽  
Author(s):  
Erik H. Hoffmann ◽  
Andreas Tilgner ◽  
Simonas Kecorius ◽  
Hartmut Herrmann

<p>New particle formation (NPF) and early growth are efficient processes producing high concentrations of cloud condensation nuclei (CCNs) precursors in the Arctic marine boundary layer (AMBL). However, due to short lifetime and lack of condensable vapors, newly formed particles do often not grow beyond 50 nm and cause low CCN particle concentrations in the AMBL. Thus, even the smallest amount of Aitken mode particle growth is capable to significantly increase the CCN budget. However, the growth mechanism of Aitken-mode particles from NPF into CCN range in the Arctic is still rather unclear and was therefore investigated during the cruise campaign PASCAL in 2017.</p> <p>During PASCAL, aerosol particles measurements were performed and an unexpected rapid growth of Aitken mode particles was observed right after fog episodes. Combined field data analyses and detailed multiphase chemistry box model simulations with the CAPRAM mechanism were performed to study the underlying processes. Resulting, a new mechanism is proposed explaining how particles with d < 50 nm are able to grow into CCN size range in the Arctic without requiring high water vapor supersaturation (SS). The investigations demonstrated that the rapid post-fog particle growth of Aitken mode is related to chemical processes within the Arctic fog. The redistribution of semi-volatile acidic (e.g., methanesulfonic acid) and basic (e.g., ammonia) compounds from processed CCN-active particles to smaller CCN-inactive particles can cause a rapid particle growth of Aitken mode particles after fog evaporation enabling them to grow towards CCN size. Comparisons of the model results with Berner impactor measurements supports the proposed growth mechanism.</p> <p>Overall, this study provided new insights on how the increasing frequency of NPF and fog-related particle processing can increase in the number of CCNs and cloud droplets leading to an increased albedo of Arctic clouds and thus affect the radiative balance in the Arctic. Since fogs will occur more frequently in the Arctic as a result of climate change, this growth mechanism and a deeper knowledge on its feedbacks can be essential to understand Arctic warming.</p>


2005 ◽  
Vol 5 (1) ◽  
pp. 57-66 ◽  
Author(s):  
P. Mönkkönen ◽  
I. K. Koponen ◽  
K. E. J. Lehtinen ◽  
K. Hämeri ◽  
R. Uma ◽  
...  

Abstract. Diurnal variation of number size distribution (particle size 3-800nm) and modal parameters (geometric standard deviation, geometric mean diameter and modal aerosol particle concentration) in a highly polluted urban environment was investigated during October and November 2002 in New Delhi, India. Continuous monitoring for more than two weeks with the time resolution of 10min was conducted using a Differential Mobility Particle Sizer (twin DMPS). The results indicated clear increase in Aitken mode (25-100nm) particles during traffic peak hours, but towards the evenings there were more Aitken mode particles compared to the mornings. Also high concentrations of accumulation mode particles (>100nm) were detected in the evenings only. In the evenings, biomass/refuse burning and cooking are possible sources beside the traffic. We have also shown that nucleation events are possible in this kind of atmosphere even though as clear nucleation events as observed in rural sites could not be detected. The formation rate of 3nm particles (J3) of the observed events varied from 3.3 to 13.9cm-3s-1 and the growth rate varied from 11.6 to 18.1nmh-1 showing rapid growth and high formation rate, which seems to be typical in urban areas.


2018 ◽  
Author(s):  
Luciana Varanda Rizzo ◽  
Pontus Roldin ◽  
Joel Brito ◽  
John Backman ◽  
Erik Swietlicki ◽  
...  

Abstract. The Amazon Basin is a unique region to study atmospheric aerosols, given their relevance for the regional hydrological cycle and large uncertainty of their sources. Multi-year datasets are crucial when contrasting periods of natural conditions and periods influenced by anthropogenic emissions. In the wet season, biogenic sources and processes prevail, and the Amazonian atmospheric composition resembles pre-industrial conditions. In the dry season, the Basin is influenced by widespread biomass burning emissions. This work reports multi-year observations of high time resolution submicrometer (10–600 nm) particle number size distributions at a rain forest site in Amazonia (TT34 tower, 60 km NW from Manaus city), between years 2008–2010 and 2012–2014. Median particle number concentration was 403 cm−3 in the wet season and 1254 cm−3 in the dry season. The Aitken mode (~ 30–100 nm in diameter) was prominent during the wet season, while accumulation mode (~ 100–600 nm in diameter) dominated the particle size spectra during the dry season. Cluster analysis identified groups of aerosol number size distribution influenced by convective downdrafts, nucleation events and fresh biomass burning emissions. New particle formation and subsequent growth was rarely observed during the 749 days of observations, similar to previous observations in the Amazon Basin. A stationary 1D column model (ADCHEM – Aerosol Dynamics, gas and particle phase CHEMistry and radiative transfer model) was used to assess importance of processes behind the observed diurnal particle size distribution trends. Three major particle source types are required in the model to reproduce the observations: (i) a surface source of particles in the evening, possibly related to primary biological emissions (ii) entrainment of accumulation mode aerosols in the morning, and (iii) convective downdrafts transporting Aitken mode particles into the boundary layer mostly during the afternoon. The latter process has the largest influence on the modelled particle number size distributions. However, convective downdrafts are often associated with rain and thus act both as a source of Aitken mode particles, and as a sink of accumulation mode particles, causing a net reduction in the median total particle number concentrations in the surface layer. Our study shows that the combination of the three mentioned particle sources are essential to sustain particle number concentrations in Amazonia.


2018 ◽  
Vol 18 (23) ◽  
pp. 17615-17635 ◽  
Author(s):  
Guangjie Zheng ◽  
Yang Wang ◽  
Allison C. Aiken ◽  
Francesca Gallo ◽  
Michael P. Jensen ◽  
...  

Abstract. The response of marine low cloud systems to changes in aerosol concentration represents one of the largest uncertainties in climate simulations. Major contributions to this uncertainty are derived from poor understanding of aerosol under natural conditions and the perturbation by anthropogenic emissions. The eastern North Atlantic (ENA) is a region of persistent but diverse marine boundary layer (MBL) clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In this study, we examine MBL aerosol properties, trace gas mixing ratios, and meteorological parameters measured at the Atmospheric Radiation Measurement Climate Research Facility's ENA site on Graciosa Island, Azores, Portugal, during a 3-year period from 2015 to 2017. Measurements impacted by local pollution on Graciosa Island and during occasional intense biomass burning and dust events are excluded from this study. Submicron aerosol size distribution typically consists of three modes: Aitken (At, diameter Dp<∼100 nm), accumulation (Ac, Dp within ∼100 to ∼300 nm), and larger accumulation (LA, Dp>∼300 nm) modes, with average number concentrations (denoted as NAt, NAc, and NLA below) of 330, 114, and 14 cm−3, respectively. NAt, NAc, and NLA show contrasting seasonal variations, suggesting different sources and removal processes. NLA is dominated by sea spray aerosol (SSA) and is higher in winter and lower in summer. This is due to the seasonal variations of SSA production, in-cloud coalescence scavenging, and dilution by entrained free troposphere (FT) air. In comparison, SSA typically contributes a relatively minor fraction to NAt (10 %) and NAc (21 %) on an annual basis. In addition to SSA, sources of Ac-mode particles include entrainment of FT aerosols and condensation growth of Aitken-mode particles inside the MBL, while in-cloud coalescence scavenging is the major sink of NAc. The observed seasonal variation of NAc, being higher in summer and lower in winter, generally agrees with the steady-state concentration estimated from major sources and sinks. NAt is mainly controlled by entrainment of FT aerosol, coagulation loss, and growth of Aitken-mode particles into the Ac-mode size range. Our calculation suggests that besides the direct contribution from entrained FT Ac-mode particles, growth of entrained FT Aitken-mode particles in the MBL also represent a substantial source of cloud condensation nuclei (CCN), with the highest contribution potentially reaching 60 % during summer. The growth of Aitken-mode particles to CCN size is an expected result of the condensation of sulfuric acid, a product from dimethyl sulfide oxidation, suggesting that ocean ecosystems may have a substantial influence on MBL CCN populations in the ENA.


2020 ◽  
Author(s):  
Chang Hoon Jung ◽  
JiYi Lee ◽  
Junshik Um ◽  
Yong Pyo Kim

&lt;p&gt;In this study, simplified analytic type of expression for size dependent MEs (Mass efficiencies) are developed. The entire size was considered assuming lognormal size distribution for sulfate, nitrate and NaCl aerosol species and the MEE of each aerosol chemical composition was estimated by fitting Mie&amp;#8217;s calculation. The obtained results are compared with the results from the Mie-theory-based calculations and showed comparable results.&lt;/p&gt;&lt;p&gt;The mass efficiencies of all aerosol components for each size range are compared with Mie&amp;#8217;s results and approximated as a function of geometric mean diameter in the form of a power law formula. Finally, harmonic mean type approximation was used to cover entire particle size range.&lt;/p&gt;&lt;p&gt;Also, analytic expression of approximated scattering enhancement factor which stands for the effect of hygroscopic growth factor for polydispersed aerosol on aerosol optical properties are obtained.&lt;/p&gt;&lt;p&gt;Based on aerosol thermodynamic models, mass growth factor can be obtained and their optical properties can be obtained by using Mie theory with different aerosol properties and size distribution. Finally, scattering enhancement factor was approximated fRH for polydispersed aerosol as a function of RH.&lt;/p&gt;&lt;p&gt;Finally, we also compared the simple forcing efficiency (SFE, W/g) of polydisperse aerosols between the developed simple approach and by the method using the Mie theory. The results show that current obtained approximated methods are comparable with existing numercal calculation based results for polydipersed particle size.&lt;/p&gt;


2006 ◽  
Vol 63 (2) ◽  
pp. 682-696 ◽  
Author(s):  
Annica M. L. Ekman ◽  
Chien Wang ◽  
Johan Ström ◽  
Radovan Krejci

Abstract Large concentrations of small aerosols have been previously observed in the vicinity of anvils of convective clouds. A 3D cloud-resolving model (CRM) including an explicit size-resolving aerosol module has been used to examine the origin of these aerosols. Five different types of aerosols are considered: nucleation mode sulfate aerosols (here defined by 0 ≤ d ≤5.84 nm), Aitken mode sulfate aerosols (here defined by 5.84 nm ≤ d ≤ 31.0 nm), accumulation mode sulfate aerosols (here defined by d ≥ 31.0 nm), mixed aerosols, and black carbon aerosols. The model results suggest that approximately 10% of the initial boundary layer number concentration of Aitken mode aerosols and black carbon aerosols are present at the top of the convective cloud as the cloud reaches its decaying state. The simulated average number concentration of Aitken mode aerosols in the cloud anvil (∼1.6 × 104 cm−3) is in the same order of magnitude as observations. Thus, the model results strongly suggest that vertical convective transport, particularly during the active period of the convection, is responsible for a major part of the appearance of high concentrations of small aerosols (corresponding to the Aitken mode in the model) observed in the vicinity of cloud anvils. There is some formation of new aerosols within the cloud, but the formation is small. Nucleation mode aerosols are also efficiently scavenged through impaction scavenging by precipitation. Accumulation mode and mixed mode aerosols are efficiently scavenged through nucleation scavenging and their concentrations in the cloud anvil are either very low (mixed mode) or practically zero (accumulation mode). In addition to the 3D CRM, a box model, including important features of the aerosol module of the 3D model, has been used to study the formation of new aerosols after the cloud has evaporated. The possibility of these aerosols to grow to suitable cloud condensation or ice nuclei size is also examined. Concentrations of nucleation mode aerosols up to 3 × 104 cm−3 are obtained. The box model simulations thus suggest that new particle formation is a substantial source of small aerosols in the upper troposphere during and after the dissipation of the convective cloud. Nucleation mode and Aitken mode aerosols grow due to coagulation and condensation of H2SO4 on the aerosols, but the growth rate is low. Provided that there is enough OH available to oxidize SO2, parts of the aerosol population (∼400 cm−3) can reach the accumulation mode size bin of the box model after 46 h of simulation.


2003 ◽  
Vol 3 (3) ◽  
pp. 2783-2833 ◽  
Author(s):  
P. Tunved ◽  
H.-C. Hansson ◽  
M. Kulmala ◽  
P. Aalto ◽  
Y. Viisanen ◽  
...  

Abstract. Size distribution measurements performed at five different stations have been investigated during a one-year period between 01 June 2000 and 31 May 2001 with focus on diurnal, seasonal and geographical differences of size distribution properties. The stations involved cover a large geographical area ranging from the Finnish Lapland (67° N) down to southern Sweden (56° N) in the order Värriö, Pallas, Hyytiälä, Aspvreten and Vavihill. The shape of the size distribution is typically bimodal during winter with a larger fraction of accumulation mode particles compared to the other seasons. Highest Aitken mode concentration is found during summer and spring. The maximum of nucleation events occur during spring months. Nucleation events occur during other seasons as well, although not as frequently. Large differences were found between different categories of stations. Northerly located stations such as Pallas and Värriö presented well-separated Aitken and accumulation modes, while the two modes often overlap significantly at the two southernmost stations Vavihill and Aspvreten. A method to cluster trajectories was used to analyse the impact of long-range transport on the observed aerosol properties. Clusters of trajectories arriving from the continent were clearly associated with size distributions shifted towards the accumulation mode. This feature was more pronounced the further south the station was located. Marine- or Arctic-type clusters were associated with large variability in the nuclei size ranges. A quasi-lagrangian approach was used to investigate transport related changes in the aerosol properties. Typically, an increase in especially Aitken mode concentrations was observed when advection from the north occurs, i.e. allowing more continental influence on the aerosol when comparing the different measurement sites. When trajectory clusters arrive to the stations from SW, a gradual decrease in number concentration is experienced in all modes as latitude of measurement site increases.


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