Accumulation Mode Aerosol Research Articles

Aitken Mode Aerosols Buffer Decoupled Mid‐Latitude Boundary Layer Clouds Against Precipitation Depletion

AbstractAerosol‐cloud‐precipitation interactions are a leading source of uncertainty in estimating climate sensitivity. Remote marine boundary layers where accumulation mode (∼100–400 nm diameter) aerosol concentrations are relatively low are very susceptible to aerosol changes. These regions also experience heightened Aitken mode aerosol (∼10–100 nm) concentrations associated with ocean biology. Aitken aerosols may significantly influence cloud properties and evolution by replenishing cloud condensation nuclei and droplet number lost through precipitation (i.e., Aitken buffering). We use a large‐eddy simulation with an Aitken‐mode enabled microphysics scheme to examine the role of Aitken buffering in a mid‐latitude decoupled boundary layer cloud regime observed on 15 July 2017 during the Aerosol and Cloud Experiments in the Eastern North Atlantic flight campaign: cumulus rising into stratocumulus under elevated Aitken concentrations (∼100–200 mg−1). In situ measurements are used to constrain and evaluate this case study. Our simulation accurately captures observed aerosol‐cloud‐precipitation interactions and reveals time‐evolving processes driving regime development and evolution. Aitken activation into the accumulation mode in the cumulus layer provides a reservoir for turbulence and convection to carry accumulation aerosols into the drizzling stratocumulus layer above. Further Aitken activation occurs aloft in the stratocumulus layer. Together, these activation events buffer this cloud regime against precipitation removal, reducing cloud break‐up and associated increases in heterogeneity. We examine cloud evolution sensitivity to initial aerosol conditions. With halved accumulation number, Aitken aerosols restore accumulation concentrations, maintain droplet number similar to original values, and prevent cloud break‐up. Without Aitken aerosols, precipitation‐driven cloud break‐up occurs rapidly. In this regime, Aitken buffering sustains brighter, more homogeneous clouds for longer.

WSOC in accumulation mode aerosols: Distribution and relationship with BrC light absorption at an urban background site

This paper presents the outcomes of a one-month long campaign (Jan 11, 2021 to Feb 11, 2021) of size segregated particulate matter (PM) in the accumulation mode (AM). Samples were collected at an urban background station (southeastern Iberian Peninsula) using a micro-orifice uniform deposit impactor (MOUDI). PM mass and water-soluble organic carbon (WSOC) were subsequently measured. The main goals of this research were: (1) to explore differences in WSOC mass size distributions under different meteorological conditions and (2) to determine the most efficient size for light absorption by WSOC. For the second objective, measurements of absorption coefficients (σap,λ) were obtained by means of an Aethalometer (AE33). Significant differences in WSOC concentrations and σap,λ values during stagnation episodes compared to non-event days were observed. Increases in WSOC concentrations during these episodes were most likely associated with the photochemical production of secondary compounds (in small-size ranges of the AM) and with water uptake (in large-size ranges of the AM). The average σap,λ value during this type of event was 2.6 higher than for non-event days. No significant increases in WSOC levels were detected under Saharan dust events. The average contribution of BrC to light absorption at 370 nm was ∼35%, revealing a significant influence of BrC on the absorption process. High contributions from BrC to light absorption were associated with AAE values above 1.5 and, in general, with high WSOC concentrations. WSOC in the smallest size mode (0.25 μm) was mainly emitted from biomass burning (BB) and showed the highest light absorption efficiency.

Ion-induced cloud modulation through new particle formation and runaway cloud condensation nuclei production

Abstract Cloud formation in the Pi Convection–Cloud Chamber is achieved via ionization in humid conditions, without the injection of aerosol particles to serve as cloud condensation nuclei (CCN). Abundant ions, turbulence, and supersaturated water vapor combine to produce new particles, which grow to become CCN sized and eventually are activated to form clouds. Coupling between the new particle formation and cloud droplets causes predator-prey type oscillations in aerosol and droplet concentrations under turbulent conditions. Leading terms are identified in the budgets for Aitken and accumulation mode aerosols and for cloud droplets. The cloud coupling is proposed to be a result of cloud-induced runaway CCN production through aerosol scavenging. The experiments suggest potential applications to marine cloud brightening, in which ions rather than sea-salt aerosols are generated.

Aerosol Properties and Their Influences on Marine Boundary Layer Cloud Condensation Nuclei over the Southern Ocean

Five overcast marine stratocumulus cases during the Southern Ocean Clouds Radiation Aerosol Transport Experimental Study (SOCRATES) aircraft field campaign were selected to examine aerosol and cloud condensation nuclei (CCN) properties with cloud influence. The Aitken- and accumulation-mode aerosols contributed approximately 70% and 30% of the total aerosols, respectively. The aerosol properties before and after periods of drizzle were investigated using in situ measurements during one case. Sub-cloud drizzle processes impacted accumulation-mode aerosols and CCN distribution. There was a nearly linear increase in CCN number concentration (NCCN) with supersaturation (S) during the ‘before drizzle’ period, but this was not true for the ‘after drizzle’ period, particularly when S > 0.4%. Using the hygroscopicity parameter (κ) to quantitatively investigate the chemical cloud-processing mechanisms, we found that higher κ values (>0.4) represent cloud-processing aerosols, while lower κ values (<0.1) represent newly formed aerosols. When the supersaturation is less than the Hoppel minimum (0.22%), cloud processing is dominant, whereas sea-spray aerosols are dominant contributors to CCN activation when S exceeds 0.22% but is less than 0.32%, the effective supersaturation threshold. Sea salt is considered a non-cloud-processing aerosol and is large and hygroscopic enough to form cloud droplets.

Measurement report: High Arctic aerosol hygroscopicity at sub- and supersaturated conditions during spring and summer

Abstract. Aerosol hygroscopic growth and cloud droplet formation influence the radiation transfer budget of the atmosphere and thereby the climate. In the Arctic, these aerosol properties may have a more pronounced effect on the climate compared to the midlatitudes. Hygroscopic growth and cloud condensation nuclei (CCN) concentrations of high Arctic aerosols were measured during two field studies in the spring and summer of 2016. The study site was the Villum Research Station (Villum) at Station Nord in the northeastern region of Greenland. Aerosol hygroscopic growth was measured with a hygroscopic tandem differential mobility analyzer (HTDMA) over a total of 23 d, and CCN concentrations were measured over a period of 95 d. Continuous particle number size distributions were recorded, facilitating calculations of aerosol CCN activation diameters and aerosol κ values. In spring, average CCN concentrations, at supersaturations (SSs) of 0.1 % to 0.3 %, ranged from 53.7 to 85.3 cm−3, with critical activation diameters ranging from 130.2 to 80.2 nm and κCCN ranging from 0.28–0.35. In summer, average CCN concentrations were 20.8 to 47.6 cm−3, while critical activation diameters and κCCN were from 137.1 to 76.7 nm and 0.23–0.35, respectively. Mean particle hygroscopic growth factors ranged from 1.60 to 1.75 at 90 % relative humidity in spring, while values between 1.47 and 1.67 were observed in summer depending on the initial dry size. Although the summer aerosol number size distributions were characterized by frequent new particle formation events, the CCN population at cloud-relevant supersaturations was determined by accumulation-mode aerosols.

Contribution of regional aerosol nucleation to low-level CCN in an Amazonian deep convective environment: results from a regionally nested global model

Abstract. Global model studies and observations have shown that downward transport of aerosol nucleated in the free troposphere is a major source of cloud condensation nuclei (CCN) to the global boundary layer. In Amazonia, observations show that this downward transport can occur during strong convective activity. However, it is not clear from these studies over what spatial scale this cycle of aerosol formation and downward supply of CCN is occurring. Here, we aim to quantify the extent to which the supply of aerosol to the Amazonian boundary layer is generated from nucleation within a 1000 km regional domain or from aerosol produced further afield and the effectiveness of the transport by deep convection. We run the atmosphere-only configuration of the HadGEM3 climate model incorporating a 440 km × 1080 km regional domain over Amazonia with 4 km resolution. Simulations were performed over several diurnal cycles of convection. Below 2 km altitude in the regional domain, our results show that new particle formation within the regional domain accounts for only between 0.2 % and 3.4 % of all Aitken and accumulation mode aerosol particles, whereas nucleation that occurred outside the domain (in the global model) accounts for between 58 % and 81 %. The remaining aerosol is primary in origin. Above 10 km, the regional-domain nucleation accounts for up to 66 % of Aitken and accumulation mode aerosol, but over several days very few of these particles nucleated above 10 km in the regional domain are transported into the boundary layer within the 1000 km region, and in fact very little air is mixed that far down. Rather, particles transported downwards into the boundary layer originated from outside the regional domain and entered the domain at lower altitudes. Our model results show that CCN entering the Amazonian boundary layer are transported downwards gradually over multiple convective cycles on scales much larger than 1000 km. Therefore, on a 1000 km scale in the model (approximately one-third the size of Amazonia), trace gas emission, new particle formation, transport and CCN production do not form a “closed loop” regulated by the biosphere. Rather, on this scale, long-range transport of aerosol is a much more important factor controlling CCN in the boundary layer.

African smoke particles act as cloud condensation nuclei in the wintertime tropical North Atlantic boundary layer over Barbados

Abstract. The number concentration and properties of aerosol particles serving as cloud condensation nuclei (CCN) are important for understanding cloud properties, including in the tropical Atlantic marine boundary layer (MBL), where marine cumulus clouds reflect incoming solar radiation and obscure the low-albedo ocean surface. Studies linking aerosol source, composition, and water uptake properties in this region have been conducted primarily during the summertime dust transport season, despite the region receiving a variety of aerosol particle types throughout the year. In this study, we compare size-resolved aerosol chemical composition data to the hygroscopicity parameter κ derived from size-resolved CCN measurements made during the Elucidating the Role of Clouds–Circulation Coupling in Climate (EUREC4A) and Atlantic Tradewind Ocean-Atmosphere Mesoscale Interaction Campaign (ATOMIC) campaigns from January to February 2020. We observed unexpected periods of wintertime long-range transport of African smoke and dust to Barbados. During these periods, the accumulation-mode aerosol particle and CCN number concentrations as well as the proportions of dust and smoke particles increased, whereas the average κ slightly decreased (κ=0.46±0.10) from marine background conditions (κ=0.52±0.09) when the submicron particles were mostly composed of marine organics and sulfate. Size-resolved chemical analysis shows that smoke particles were the major contributor to the accumulation mode during long-range transport events, indicating that smoke is mainly responsible for the observed increase in CCN number concentrations. Earlier studies conducted at Barbados have mostly focused on the role of dust on CCN, but our results show that aerosol hygroscopicity and CCN number concentrations during wintertime long-range transport events over the tropical North Atlantic are also affected by African smoke. Our findings highlight the importance of African smoke for atmospheric processes and cloud formation over the Caribbean.

A New Aerosol Dry Deposition Model for Air Quality and Climate Modeling

AbstractDry deposition of aerosols from the atmosphere is an important but poorly understood and inadequately modeled process in atmospheric systems for climate and air quality. Comparisons of currently used aerosol dry deposition models to a compendia of published field measurement studies in various landscapes show very poor agreement over a wide range of particle sizes. In this study, we develop and test a new aerosol dry deposition model that is a modification of the current model in the Community Multiscale Air Quality (CMAQ) model. The new model agrees much better with measured dry deposition velocities across particle sizes. The key innovation is the addition of a second inertial impaction term for microscale obstacles such as leaf hairs, microscale ridges, and needleleaf edge effects. The most significant effect of the new model is to increase the mass dry deposition of the accumulation mode aerosols in CMAQ. Accumulation mode mass dry deposition velocities increase by almost an order of magnitude in forested areas with lesser increases for shorter vegetation. Peak PM2.5 concentrations are reduced in some forested areas by up to 40% in CMAQ simulations. Over the continuous United States, the new model reduced PM2.5 by an average of 16% for July 2018 at the Air Quality System monitoring sites. For summer 2018 simulations, bias and error of PM2.5 concentrations are significantly reduced, especially in forested areas.

Seasonal variation of size-resolved aerosol fluxes in a Peri-urban deciduous broadleaved forest

Eddy covariance measurements of aerosol fluxes were performed above an oak-hornbeam forest in the Po Plain (Northern Italy), from February to May and from September to December 2019. Measurements aimed at assessing the influence of forest phenology and leaf presence/absence on the seasonal evolution of size-segregated aerosol fluxes. The size-resolved aerosol concentration in the range 0.006-10 μm was sampled with a 14-stage impactor (ELPI+, Dekati, FI), and the filters exposed in May were subjected to chemical analysis. Over the whole sampling period, the forest removed from the atmosphere an average of 3.12 mg of aerosol m−2 d−1. The direction and the intensity of the aerosol fluxes were not constant through the year, as a strong seasonal and size-dependent variability emerged. In particular, leaf-presence drove a net deposition of the accumulation mode aerosol (100 nm< particle diameter Dp<1000 nm) and an emission of the Aitken (10 nm< Dp<100 nm) and coarse mode (Dp>1000 nm) aerosols. On the contrary, in absence of leaves all the sub-micrometer aerosol size-classes showed net daily upward fluxes, while coarse mode aerosol fluxes were prevalently downward. Monthly averages of deposition velocities of Aitken and accumulation mode aerosols correlated with the Leaf Area Index (LAI) seasonal trend, thus indicating an important role of the amount of the leaf surface area on the deposition and emission of these size-classes. Furthermore, an influence of the stomatic activity was suggested for the Aitken mode aerosol, since its deposition velocity followed the same diel course of the stomatal conductance to water. The analysis of the influence of meteorological parameters on aerosol deposition velocities highlighted that dynamic and convective turbulence (described by friction velocity, u* and Deardorff velocity, w*) enhanced the vertical aerosol exchanges, both upward and downward, while the approaching of condensing conditions reduced the flux intensities.

Regional characteristics of fine aerosol mass increase elucidated from long-term observations and KORUS-AQ campaign at a Northeast Asian background site

Northeast Asia has suffered from severe PM2.5 pollution and the exact mechanisms have yet to be fully understood. Here, we investigated the transformation processes of submicron aerosols using a 4-year data set obtained at Jeju, a Northeast Asian background site. The diurnal-cycle constrained empirical orthogonal function analysis of nanoparticle size–number distribution distinguished 2 modes: burst of nucleation–Aitken particles and increase in accumulation mode particles, representing “new particle formation and growth” and “PM2.5 mass increase,” respectively. In these events, aerosol and meteorological characteristics changed progressively over several days, revealing that the PM2.5 mass increase is an episodic event occurring on a regional scale. The increase in PM2.5 mass was accompanied by an increase in aerosol liquid water content, which correlated well with SO4−2 and NO3, and a decrease in incoming solar radiation (−14.1 Wm−2 day−1) constituting a positive feedback. The “transport/haze” episode of KOREA–U.S. Air Quality campaign corresponds to “PM2.5 mass increase,” during which the vertical evolution of particles demonstrates that nanoparticles ≥3.5 nm were entrained into the shallow boundary layer upon vertical mixing and converted to accumulation-mode particles ≥0.3 μm at relative humidity (RH) exceeding the deliquescence RH of secondary inorganic aerosol (SIA). Coincidently, at ground, the coating thickness of refractory black carbon (rBC) (48 ± 39 nm) and SIA concentration increased. Furthermore, the diameter of rBC (180–220 nm)-containing particle in core–shell configuration linearly increased with PM2.5 mass, reaching 300–400 nm at PM2.5 ≥ 40 μg m−3. This observational evidence suggests that the thick coating of rBCs resulted from the active conversion of condensable gases into the particulate phase on the rBC surface, thereby increasing the mass of the accumulation-mode aerosol. Consequently, this result complies with the strategy to reduce primary emissions of gaseous precursors for SIA and particulates such as rBC as a way to effectively mitigate haze pollution as well as climate change in Northeast Asia.

Observation Analyses of Aerosol Size Distribution Properties from February to March, 2019 in Tianjin Urban Area

The aerosol size distribution is an important physical parameter reflecting the source, formation process, and pollution characteristics of aerosol particles. In order to study the properties of aerosol number concentration and size distributions in the Tianjin urban area,the aerosol number concentration and size distributions ranging from 10-600 nm were detected using a scanning mobility particle sizer (SMPS) during February and March, 2019. The results showed that in the Tianjin urban area, the aerosol number concentration,surface area concentration. and volume concentration in the size range of 10-600 nm were 22188.22 cm-3, 1581.08 μm2·cm-3, and 70.76 μm3·cm-3,respectively, in late winter and early spring. The aerosol number concentration,surface area concentration, and volume concentration spectrum were all unimodally distributed,and the peak value sizes were 109.40, 269.00, and 429.40 nm. The number concentrations of the nucleation mode (10-20 nm),Aitken mode (20-100 nm), and accumulation mode (100-600 nm) aerosols accounted for 1.40%, 52.44%, and 46.16% of the total number concentration. The diurnal variation in aerosol number concentration showed three peaks (06:00-08:00, 12:00-14:00, and 18:00-20:00) on work days and two peaks (07:00-08:00 and 19:00-21:00) on weekends. The peaks appeared 1-2 hours later on weekends,and the increment of aerosol number concentration was attributed to vehicle exhaust emissions. Meteorological factors had a significant influence on the aerosol size distribution in Tianjin; aerosol number concentration values were high in east and southwest wind. On non-precipitation days,the aerosol number size distribution moved to larger size ranges with the increment of relative humidity (RH); as the RH increased from <20% to 50%-60%,the size peak increased from 50 nm to 131 nm. The precipitation removed 100-200 nm aerosol particles discernibly,which resulted in the size peak decreasing to 98 nm.

Physical and Chemical Properties of Cloud Droplet Residuals and Aerosol Particles During the Arctic Ocean 2018 Expedition.

Detailed knowledge of the physical and chemical properties and sources of particles that form clouds is especially important in pristine areas like the Arctic, where particle concentrations are often low and observations are sparse. Here, we present in situ cloud and aerosol measurements from the central Arctic Ocean in August–September 2018 combined with air parcel source analysis. We provide direct experimental evidence that Aitken mode particles (particles with diameters ≲70 nm) significantly contribute to cloud condensation nuclei (CCN) or cloud droplet residuals, especially after the freeze‐up of the sea ice in the transition toward fall. These Aitken mode particles were associated with air that spent more time over the pack ice, while size distributions dominated by accumulation mode particles (particles with diameters ≳70 nm) showed a stronger contribution of oceanic air and slightly different source regions. This was accompanied by changes in the average chemical composition of the accumulation mode aerosol with an increased relative contribution of organic material toward fall. Addition of aerosol mass due to aqueous‐phase chemistry during in‐cloud processing was probably small over the pack ice given the fact that we observed very similar particle size distributions in both the whole‐air and cloud droplet residual data. These aerosol–cloud interaction observations provide valuable insight into the origin and physical and chemical properties of CCN over the pristine central Arctic Ocean.

Bidirectional Turbulent Fluxes of Fog at a Subtropical Montane Cloud Forest Covering a Wide Size Range of Droplets

Size-resolved turbulent fluxes of fog droplets are investigated above a subtropical montane cloud forest in Taiwan. By integrating an aerosol spectrometer into an eddy-covariance set-up, we measure droplet number fluxes and liquid water fluxes in a size range of aerosol particles and droplets with diameters ranging from 0.25 {upmu }!mathrm{m} to 17.3 {upmu }!mathrm{m}. We find two flux-direction changes within this size range: a downward flux occurs for accumulation-mode aerosols of diameters between 0.25 {upmu }!mathrm{m} and 0.83 {upmu }!mathrm{m}, an upward flux occurs for hydrated aerosols with diameters between 1.1 {upmu }!mathrm{m} and 2.4 {upmu }!mathrm{m}, and a downward flux occurs again for activated fog droplets between diameters of 3 {upmu }!mathrm{m} and 17.3 {upmu }!mathrm{m}. The droplet size distributions can be modelled by a trimodal log-normal distribution, and the modes correlate with the different flux directions. The formation of the three modes and the establishment of the respective flux directions can be explained by combining the Köhler theory on the basis of measured ion concentrations in fog with the turbulent transport of droplets. Finally, from the combined analysis of droplet fluxes and size distributions, we infer relevant processes of droplet development and dissolving during various phases of the life cycles of the fog events.

Differentiation of coarse-mode anthropogenic, marine and dust particles in the High Arctic islands of Svalbard

Abstract. Understanding aerosol–cloud–climate interactions in the Arctic is key to predicting the climate in this rapidly changing region. Whilst many studies have focused on submicrometer aerosol (diameter less than 1 µm), relatively little is known about the supermicrometer aerosol (diameter above 1 µm). Here, we present a cluster analysis of multiyear (2015–2019) aerodynamic volume size distributions, with diameter ranging from 0.5 to 20 µm, measured continuously at the Gruvebadet Observatory in the Svalbard archipelago. Together with aerosol chemical composition data from several online and offline measurements, we apportioned the occurrence of the coarse-mode aerosols during the study period (mainly from March to October) to anthropogenic (two sources, 27 %) and natural (three sources, 73 %) origins. Specifically, two clusters are related to Arctic haze with high levels of black carbon, sulfate and accumulation mode (0.1–1 µm) aerosol. The first cluster (9 %) is attributed to ammonium sulfate-rich Arctic haze particles, whereas the second one (18 %) is attributed to larger-mode aerosol mixed with sea salt. The three natural aerosol clusters were open-ocean sea spray aerosol (34 %), mineral dust (7 %) and an unidentified source of sea spray-related aerosol (32 %). The results suggest that sea-spray-related aerosol in polar regions may be more complex than previously thought due to short- and long-distance origins and mixtures with Arctic haze, biogenic and likely blowing snow aerosols. Studying supermicrometer natural aerosol in the Arctic is imperative for understanding the impacts of changing natural processes on Arctic aerosol.

Influences of Recent Particle Formation on Southern Ocean Aerosol Variability and Low Cloud Properties

AbstractControls on pristine aerosol over the Southern Ocean (SO) are critical for constraining the strength of global aerosol indirect forcing. Observations of summertime SO clouds and aerosols in synoptically varied conditions during the 2018 SOCRATES aircraft campaign reveal novel mechanisms influencing pristine aerosol‐cloud interactions. The SO free troposphere (3–6 km) is characterized by widespread, frequent new particle formation events contributing to much larger concentrations (≥1,000 mg−1) of condensation nuclei (diameters &gt; 0.01 μm) than in typical sub‐tropical regions. Synoptic‐scale uplift in warm conveyor belts and sub‐polar vortices lifts marine biogenic sulfur‐containing gases to free‐tropospheric environments favorable for generating Aitken‐mode aerosol particles (0.01–0.1 μm). Free‐tropospheric Aitken particles subside into the boundary layer, where they grow in size to dominate the sulfur‐based cloud condensation nuclei (CCN) driving SO cloud droplet number concentrations (Nd ∼ 60–100 cm−3). Evidence is presented for a hypothesized Aitken‐buffering mechanism which maintains persistently high summertime SONdagainst precipitation removal through CCN replenishment from activation and growth of boundary layer Aitken particles. Nudged hindcasts from the Community Atmosphere Model (CAM6) are found to underpredict Aitken and accumulation mode aerosols andNd, impacting summertime cloud brightness and aerosol‐cloud interactions and indicating incomplete representations of aerosol mechanisms associated with ocean biology.

Size-segregated aerosols over a high altitude Himalayan and a tropical urban metropolis in Eastern India: Chemical characterization, light absorption, role of meteorology and long range transport

A study has been conducted focusing on the chemical and optical characterization of water soluble inorganic and organic components of aerosols at different sizes, over a high altitude Himalayan station, Darjeeling (27.1° N and 88.15° E, 2200 m amsl) and a tropical urban metropolis, Kolkata (22.5° N, 88.3° E, ~6 m amsl) for two-year long period (March 2016–February 2018). It was observed that local meteorology and long range transport of pollution plumes have played the pivotal role in governing the temporal variation of the mass distribution and concentration of aerosols and its various components over both the sites. The aerosol mass-size distributions were found to be bimodal in nature with the relative dominance of accumulation mode (0.1–1.0 μm) over coarse mode (1.8–10 μm) over both the stations, indicating dominance of the anthropogenic emissions. Among the size classes, accumulation mode aerosols alone contributed 55–75% over Darjeeling and 40–60% over Kolkata to PM10. The coarse mode aerosols were mainly consisted of primary inorganic species over Kolkata and water soluble organic carbons (WSOC) over Darjeeling whereas the fine mode aerosols (accumulation: 0.1–1.0 μm) were primarily composed of the secondary inorganic aerosols for both the stations. Irrespective of the seasons and stations, SO42− and NH4+ exhibited peaks in the mass-size distribution at 1.0–0.1 μm whereas that of NO3− varied with the seasons. The photochemical oxidation and the aqueous phase oxidation of SO2 (g) were the pathways for SO42− formation over Darjeeling whereas the later dominated over Kolkata. Concentration weighted trajectory (CWT) model has revealed that the secondary inorganic aerosols and WSOC were local/regional in origin over Kolkata megacity whereas Darjeeling was influenced by mixed sources. The accumulation mode aerosols were found to be the highest light absorbing over both the stations irrespective of the seasons. Over Darjeeling, the absorption coefficient (babs_365) and the mass absorption efficiency (MAE) of WSOC were maximum for local biomass burning aerosols than the transported plumes whereas those over Kolkata were maximum for transported biomass burning plumes from Eastern Ghats.

New Particle Formation and Growth to Climate‐Relevant Aerosols at a Background Remote Site in the Western Himalaya

AbstractNew particle formation (NPF) can influence the Earth's radiative budget when the newly formed particles grow to climate‐relevant sizes. Here, we present analysis of 21 months of continuous aerosol size distribution measurements at a background remote site in the western Himalaya and provide observational evidence that newly formed particles grow to cloud condensation nuclei (CCN)‐active sizes (i.e., &gt;20–100 nm in diameter). Out of total 55 NPF events, 38 (66%) events occurred in the pre‐monsoon season (March–May). NPF events were classified into those with and without pollution influence as polluted and cleaner, respectively, using black carbon data. The analysis of air mass age, based on the ratio of number concentration of Aitken to accumulation mode aerosols, indicated that NPF occurred in the relatively cleaner air masses reaching to the site. The median formation rate of 10 nm particles and particle growth rates for cleaner events were three‐fold and two‐fold, respectively, higher than polluted events. We present the first estimates of the survival probability of newly formed particles to 50 and 100 nm size, which was not attempted in an Indian environment previously. The survival probability to 50 nm particles ranged from 44% to 98%, with a mean and standard deviation of 82 ± 18%. On average, ∼60% of the particles surviving to 50 nm survived to 100 nm, making the overall survival probability of 100 nm to 53 ± 31%. This indicates that the probability of nucleated particles growing to CCN‐active sizes under a large source of condensing vapor (transported from nearby lower‐altitude regions) and low pre‐existing particle concentrations (background mountain site) is high compared to the previous studies. These findings highlight the importance of the efficiency of nucleation events for producing CCN, which is a critical basis of aerosol indirect effects.

Airborne extractive electrospray mass spectrometry measurements of the chemical composition of organic aerosol

Abstract. We deployed an extractive electrospray ionization time-of-flight mass spectrometer (EESI-MS) for airborne measurements of biomass burning aerosol during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study onboard the NASA DC-8 research aircraft. Through optimization of the electrospray working solution, active control of the electrospray region pressure, and precise control of electrospray capillary position, we achieved 1 Hz quantitative measurements of aerosol nitrocatechol and levoglucosan concentrations up to pressure altitudes of 7 km. The EESI-MS response to levoglucosan and nitrocatechol was calibrated for each flight, with flight-to-flight calibration variability of 60 % (1σ). Laboratory measurements showed no aerosol size dependence in EESI-MS sensitivity below particle geometric diameters of 400 nm, covering 82 % of accumulation-mode aerosol mass during FIREX-AQ. We also present a first in-field intercomparison of EESI-MS with a chemical analysis of aerosol online proton-transfer-reaction mass spectrometer (CHARON PTR-MS) and a high-resolution Aerodyne aerosol mass spectrometer (AMS). EESI-MS and CHARON PTR-MS levoglucosan concentrations were well correlated, with a regression slope of 0.94 (R2=0.77). AMS levoglucosan-equivalent concentrations and EESI-MS levoglucosan showed a greater difference, with a regression slope of 1.36 (R2=0.96), likely indicating the contribution of other compounds to the AMS levoglucosan-equivalent measurement. The total EESI-MS signal showed correlation (R2=0.9) with total organic aerosol measured by AMS, and the EESI-MS bulk organic aerosol sensitivity was 60 % of the sensitivity to levoglucosan standards.

Size Distribution of Aerosol Hygroscopic Growth Factors in Winter in Tianjin

Aerosol hygroscopic growth factors[g(RH)] are key for evaluating aerosol light extinction and direct radiative forcing. The hygroscopic tandem differential mobility analyzer (HTDMA) was utilized to measure the size-resolved gm(RH) under different polluted conditions in winter in Tianjin. Furthermore, based on the size distribution of aerosol water-soluble ions, the gκ(RH) across a wide size range (60 nm to 9.8 μm) was estimated using the κ-Köhler theory, which provides a basis for the estimation of aerosol optical parameters and direct radiative forcing under ambient conditions. Under clean conditions, ultrafine particles (<100 nm) were more hygroscopic and gm(RH=80%) was higher than 1.30 due to the active photolysis reaction. However, under severely polluted conditions, the proportion of water-soluble ions in aerosols increased with the increasing size; gm(RH) increased with particle size, where gm(RH=80%) and gm(RH=85%) for 300 nm particles was 1.39 and 1.46, respectively. For a wide size range (60 nm to 9.8 μm), the aerosols in the accumulation mode were more hygroscopic and aerosols in the Aitken mode were less hygroscopic, with coarse mode aerosols being the least hygroscopic. During the polluted period, the particulate size notably increased, and the mass fraction of NO3- and SO42- in the accumulation mode aerosols was significantly higher than during the clean period. Accordingly, the hygroscopicity of accumulation mode aerosols was strongly enhanced during the polluted period[gκ(RH)=1.3-1.4] and aerosols in the 0.18-3.1 μm size range all had a strong hygroscopicity. On polluted days, the synergistic effect of the increase in particle size, water-soluble ions, and aerosol hygroscopicity results in the considerable deterioration of visibility.

Factors Influencing New Atmospheric Particle Formation in Ordos During Summer and Autumn 2019

In this study, the aerosol number size distribution in the range of 10 nm-10 μm was collected from August 16 to October 04, 2019 at Ordos using a wide-range particle spectrometer (WPS). Combined with PM (PM2.5 and PM10), pollution gases, meteorological data, and the HYSPLIT model, the characteristics and impact factors of new particle formation (NPF) were discussed. The results indicated that there were 19 NPF events during the observation period, which have different effects on diurnal variation in aerosol number concentration in different modes. The NPF events caused a sharp increase in the number concentration of nucleation and Aitken mode aerosols, but had little effect on the number concentration of accumulation and coarse mode aerosols. The temperature, wind speed, and total solar radiation during NPF days were usually higher than those in non-NPF days, and the RH during NPF days was lower. On NPF days, the mass concentrations of PM2.5, PM10, CO, and NO2 were lower than those on non-NPF days, while the mass concentrations of O3 and SO2 were higher. NPF events were observed in 40.0% of northern air masses and 29.6% of southern air masses. There were significant differences in meteorological elements in different NPF event air mass types. The southern NPF event air mass type had the lowest wind speed and the highest RH, with averages of (2.4±1.5) m·s-1 and (48.8±10.8)%, respectively. The northern NPF event air mass type had the highest wind speed and total solar radiation, with averages of (4.2±1.9) m·s-1 and (664.5±255.6) W·m-2, respectively. The western air mass type of NPF event had the lowest RH, with an average of (29.8±12.7)%. The formation rates of new particles in the different air mass types of NPF events were similar, ranging from 1.5 to 1.8 cm-3·s-1. The largest growth rate was (12.7±13.6) nm·h-1 in the southern NPF event air mass type, which was 1.2 times and 1.4 times higher than the NPF events of northern air masses and western air masses.