High Number Concentrations Research Articles

Observations of supermicron-sized aerosols originating from biomass burning in southern Central Africa

During the 3 years of the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) campaign, the NASA Orion P-3 was equipped with a 2D stereo (2D-S) probe that imaged particles with maximum dimension (D) ranging from 10 < D < 1280 μm. The 2D-S recorded supermicron-sized aerosol particles (SAPs) outside of clouds within biomass burning plumes during flights over the southeastern Atlantic off Africa’s coast. Numerous SAPs with 10 < D < 1520 μm were observed in 2017 and 2018 at altitudes between 1230 and 4000 m, 1000 km from the coastline, mostly between 7–11° S. No SAPs were observed in 2016 as flights were conducted further south and further from the coastline. Number concentrations of refractory black carbon (rBC) measured by a single particle soot photometer ranged from 200 to 1200 cm−3 when SAPs were observed. Transmission electron microscopy images of submicron particulates, collected on Holey carbon grid filters, revealed particles with potassium salts, black carbon (BC), and organics. Energy-dispersive X-ray spectroscopy spectra also detected potassium, a tracer for biomass burning. These measurements provided evidence that the submicron particles originated from biomass burning. NOAA Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) 3 d back trajectories show a source in northern Angola for times when large SAPs were observed. Fire Information for Resource Management System (FIRMS) Moderate Resolution Imaging Spectroradiometer (MODIS) 6 active fire maps showed extensive biomass burning at these locations. Given the back trajectories, the high number concentrations of rBC, and the presence of elemental tracers indicative of biomass burning, it is hypothesized that the SAPs imaged by the 2D-S are examples of BC aerosol, ash, or unburned plant material.

Oceanic Supply of Ice‐Nucleating Particles and Its Effect on Ice Cloud Formation: A Case Study in the Arctic Ocean During a Cold‐Air Outbreak in Early Winter

AbstractThe relationship between cloud phase, ice‐nucleating particles (INPs), and ocean state is vital in climate system modeling. High wave conditions induced by the Arctic sea‐ice decline and intensified atmospheric forcing over the ice‐free ocean increase dynamical geochemical oceanic mixing and sea spray supply containing organic substances, which could act as INPs promoting formation of lower tropospheric ice‐containing clouds. Here, we show that the surface ocean state regulates INP concentration and ice cloud presence in the boundary layer. Arctic research cruise data from the marginal ice zone in the Chukchi Sea in November 2018 revealed high number concentrations of INPs active greater than °C and ice‐containing clouds under high wave conditions. Chemical analysis revealed high contents of organic carbon and sea salt that coincided with the increased oceanic turbidity. The findings suggest that elevated levels of marine organics will contribute to modification of cloud phase from liquid droplets to ice crystals.

Heat transfer potentials of ZnO/water nanofluid in free impingement jet

Heat transfer represented by jet impingement was considered due to the grown demand for such applications in the industry such as heat exchangers, metal cutting, and electronic's component cooling. Hence, ZnO/water nanofluid is embraced to enhance the heat exchanged by impinge nanofluid through a square jet. Five nanofluid were prepared thoroughly with different ZnO concentrations range of (0.1–0.5%) besides a plain de-ionized water for comparison. Validation was performed by comparing the outcome with comparable analogous studies and exhibited a content deviation. The parameter (H/Dh) which denotes the (exit of nozzle-to-hot plat spacing over the hydraulic jet diameter) was varied to be 2–8. The acquired results showed that the adoption of nanofluid in such an arrangement gives further magnification in heat transfer (Nu = 113.9%) at high Reynold's number and nanoparticle concentration (φ = 0.5%, Re = 17500, and H/Dh = 2). Whereas the minimum gained heat (Nu = 43.8%) was detected at nanoparticle concentration of (ɸ = 0.1%), Reynold's number of (Re = 5000), and H/Dh spacing of 8 respectively. It was found that applying excessive heat flux on the target plate causes rapid evaporation once the flow hits the surface plate, which leads to poor thermal performance. Eventually, the gained data were correlated and the empirical correlation is proposed.

The important roles of surface tension and growth rate in the contribution of new particle formation (NPF) to cloud condensation nuclei (CCN) number concentration: evidence from field measurements in southern China

Abstract. The contribution of new particle formation (NPF) to cloud condensation nuclei (CCN) number concentration (NCCN) varies largely under different environments and depends on several key factors such as formation rate (J), growth rate (GR), distribution of preexisting particles, and properties of new particles during NPF events. This study investigates the contribution of NPF to the NCCN and its controlling factors based on measurements conducted at the Heshan supersite, in the Pearl River Delta (PRD) region of China during fall 2019. The size-resolved cloud condensation nuclei activity and size-resolved particle hygroscopicity were measured by a cloud condensation nuclei counter (CCNc) and a hygroscopic tandem differential mobility analyzer (HTDMA), respectively, along with a scanning mobility particle sizer (SMPS) and a diethylene glycol scanning mobility particle sizer (DEG-SMPS) for particle number size distribution (PNSD). A typical NPF event on 29 October was chosen to investigate the contribution of the NPF to NCCN under several supersaturation (SS) ratios. Two particle properties (hygroscopicity and surface tension) affect CCN activation with the latter being more important in terms of the CCN concentration (NCCN). A lower value of surface tension (i.e., 0.06 N m−1) than the pure-water assumption (0.073 N m−1) could increase the NCCN at SS = 1.0 % by about 20 % during the nonevent period and by about 40 % during the event. In addition, an earlier peak time corresponding to a lower critical diameter (D50) was also observed. The results show that high formation rate, growth rate, and low background particle concentration lead to high number concentrations of newly formed particles. The high growth rate was found to have the most significant impact on the NCCN, which can be attributed to the fact that a higher growth rate can grow particles to the CCN size in a shorter time before they are scavenged by preexisting particles. Two other NPF events (an event on 18 October in this campaign and an event on 12 December 2014 in Panyu) were chosen to perform sensitivity tests under different scenarios (growth rate, formation rate, and background particle concentration). The calculated NCCN at SS = 1.0 % on 12 December 2014 was significantly lower than that from the other two events. The event on 12 December was re-simulated using the growth rate taken from the event on 18 October which resulted in similar CCN concentrations between the two events (12 December and 18 October), implying that the growth rate is the major impact factor for CCN activation. Our results highlight the importance of growth rate and surface tension when evaluating the contribution of NPF to the NCCN.

Effects of multiple injections on the transport of CMC-nZVI in saturated sand columns

The multiple injections of nanoscale zero valent iron (nZVI) slurry, an efficient method to remediate contaminated groundwater, requires an accurate assessment of the transport and risks of these particles in saturated porous medium. However, the influencing mechanism of nZVI transport under multiple injection conditions is not fully understood. In this experimental study, one-dimensional sand columns were used to evaluate the effects of injection concentrations, particle sizes and surface chemical corrosion on the transport of carboxymethyl cellulose modified nZVI (CMC-nZVI) under triple injection conditions, where the different volumes of NaCl solution were flushed through the columns between the injections. Based on the breakthrough curves and retention profiles under flushing 4 pore volumes of NaCl solution between the injections, the transport of CMC-nZVI particles was gradually enhanced attributable to the exclusion among these particles at injection concentration of 200 mg/L, but the opposite was observed due to large aggregation caused by strong magnetic force among particles at 500 mg/L. However, the magnitudes of enhancement or reduction on maximum C/C0 under the above injection concentrations were related to the smallest particle size of Dh = 3.926 μm because of high particle number concentrations leading to intense competition on depositional sites at 200 mg/L and significant aggregation at 500 mg/L. Conversely, the transport of CMC-nZVI was reduced under flushing 76 pore volumes of NaCl solution between the injections because of pronounced corrosion of CMC-nZVI in water as evidenced by the XPS and XRD analyses of particles. This corrosion could cause the decrease in repulsion among particles due to the increase in surface negative zeta potential and the CMC desorption from nZVI. Accordingly, this study revealed that relative high injection concentrations and chemical corrosion in groundwater could restrain the mobility of nZVI under multiple injection conditions and the potential risks posed by CMC-nZVI are controllable.

Characteristics of CCN activation and cloud microphysics over the east coast of India during the Northeast Monsoon onset

Airborne observations conducted during the Northeast Monsoon onset as part of the Cloud Aerosol Interaction and Precipitation Enhancement Experiment (CAIPEEX 2011) are used to link the activation properties of aerosols with the observed cloud microphysics. This study illustrates the significant spatial variability in the aerosol spectrum, cloud condensation nuclei (CCN) activation characteristics, and the cloud droplet spectral properties over a coastal and an inland location. High concentrations of Aitken mode and black carbon aerosols were observed in the free troposphere and are attributed to the convectively transported smoke and aerosols from the coastal boundary layer. The assumption of an internally mixed organic and inorganic aerosol composition provided a better CCN closure over assumptions of either purely organic or purely inorganic aerosols. The coastal clouds were equally polluted as the inland clouds with high cloud droplet number concentrations near the cloud base. The vertical distribution of cloud droplet spectral characteristics was similar in both coastal and inland clouds. An increase in droplet number concentration up to 2 km above the cloud base indicated a prominent influence of submicron particles on the cloud microphysical parameters. Evidence for an enhanced concentration of supercooled drops above the freezing level up to temperatures below −12 °C is documented. The secondary ice production was evident through observations of graupel and snow particles. Heavy loading of aerosols near the cloud base leads to enhanced mixed-phase processes in these clouds.

Evaluation of the contribution of new particle formation to cloud droplet in urban atmosphere

Abstract. New particle formation (NPF) is a large source of cloud condensation nuclei (CCN) and cloud droplet in the troposphere. In this study, we quantified the contribution of NPF to cloud droplet number concentration (CDNC, or Nd) at typical updraft velocities (V) in clouds using a field campaign data of aerosol number size distribution and chemical composition observed on May 25–June 18, 2017 in urban Beijing. We show that the NPF drives the variations of CCN and cloud droplet and increases Nd by 30–33 % at V = 0.3–3 m s−1 in urban atmosphere. A markedly reduction in Nd is observed due to water vapor competition with consideration of actual environmental updraft velocity, decreasing by 11.8 ± 5.0 % at V = 3 m s−1 and 19.0 ± 4.5 % at V = 0.3 m s−1 compared to that from a prescribed supersaturation. The effect of water vapor competition becomes smaller at larger V that can provide more sufficient water vapor. Essentially, water vapor competition led to the reduction in Nd by decreasing the environmental maximum supersaturation (Smax) for the activation of aerosol particles. It is shown that Smax was decreased by 14.5–11.7 % for V = 0.3–3 m s−1. Particularly, the largest suppression of cloud droplet formation due to the water vapor competition is presented at extremely high aerosol particle number concentrations. As a result, although a larger increase of CCN-size particles by NPF event is derived on clean NPF day when pre-existing background aerosol particles are very low, there is no large discrepancy in the enhancement of Nd by NPF between the clean and polluted NPF day. We finally show a considerable impact of the primary sources when evaluating the NPF contribution to cloud droplet based on a case study. Our study highlights the importance of fully consideration of both the environmental meteorological conditions and multiple sources (i.e. secondary and primary) to evaluate the NPF effect on clouds and the associated climate effects in polluted regions.

Southern Ocean Cloud Properties Derived From CAPRICORN and MARCUS Data

AbstractThe properties of Southern Ocean (SO) liquid phase non precipitating clouds (hereafter clouds) are examined using shipborne data collected during the Measurements of Aerosols, Radiation and Clouds over the Southern Ocean and the Clouds Aerosols Precipitation Radiation and atmospheric Composition Over the SoutheRN ocean I and II campaigns that took place south of Australia during Autumn 2016 and Summer 2017–2018. Cloud properties are derived using data from W‐band radars, lidars, and microwave radiometers using an optimal estimation algorithm. The SO clouds tended to have larger liquid water paths (LWP, 115 ± 117 g m−2), smaller effective radii (re, 8.7 ± 3 μm), and higher number concentrations (Nd, 90 ± 107 cm−3) than typical values of eastern ocean basin stratocumulus. The clouds demonstrated a tendency for the LWP to increase with Nd presumably due to precipitation suppression up to Nd of approximately 100 cm−3 when mean LWP decreased with increasing Nd. Due to higher optical depth, cloud albedos were less susceptible to changes in Nd compared to subtropical stratocumulus. The highest latitude clouds of the datasets, observed along and near the Antarctic coast, presented a distinctly bimodal character. One mode had the properties of marine clouds further north. The other mode occurred in an aerosol environment characterized by high cloud condensation nuclei concentrations and elevated sulfate aerosol without obvious continental aerosol markers. These regions of higher cloud condensation nuclei tended to have higher Nd, smaller re and higher LWP suggesting sensitivity of cloud properties to seasonal biogenic aerosol production in the high latitude SO.

Generation of ZnO nanoparticles by chemical vapor synthesis using quenching air

With the increasing interest in manufacturing nano-sized metal particles in large quantities for their numerous applications in industry, medicine and daily life as well as nanotoxicity testing, there is a critical demand to improve methods to generate nanoparticles with controllable nano-size and high number concentrations. Here, a stable method for the generation of zinc oxide nanoparticles (ZnO-NPs), especially for the size below 10 nm, by chemical vapor synthesis (CVS) using quenching air was proposed. The present study found that the oxidation step of Zn vapor in the ZnO-NP formation process is the rate-controlling step. Six conditions were tested with various furnace temperatures, carrier gas and quenching air flow rates in a tubular furnace. The experimental results showed that the quenching air flow rates (1-5 L/min) have a great impact on ZnO-NPs generation and characteristics. The geometric mean diameter of synthesized ZnO-NPs or aggregates was decreased from 15.26 to 3.27 nm, the total number concentration was increased from 2.56 × 107 to 4.28 × 107 #/cm3 and the morphology changed from tetrapod-shaped to isometric-shaped when the quenching air flow rate was increased from 1 to 5 L/min at 1 L/min carrier gas flow rate and 500 °C furnace temperature. The diameter and concentration remained stable with only small fluctuations for 5 h at all test conditions, which is very useful for nanotoxicity testing. The size of ZnO-NPs was decreased below 10 nm when the quenching rate was 11,000 K/s or higher at 1 L/min carrier gas flow rate and 500 °C furnace temperature. The experimental yield of ZnO-NPs was found to be 11.93% at 600 °C furnace temperature and less than 1.5% at 500 °C. The low yield of small ZnO-NPs is mainly attributed to the low conversion ratio of Zn vapor by the oxidation reaction, and convection-diffusion deposition loss of Zn vapor, ZnO vapor and small ZnO-NPs, which needs further improvement for future mass production using CVS method.

Examination of the evolution of iron oxide nanoparticles in flame spray pyrolysis by tailored in situ particle sampling techniques

In this report, a flame spray pyrolysis setup has been examined with various in situ extraction methods of particle samples along the flame axis. First, two precursor formulations leading to the formation of iron oxide nanoparticles were used in a standardized SpraySyn burner system, and the final particle outcome was characterized by a broad range of established powder characterization techniques (TEM/HRTEM, SAXS, XRD, BET). The characterization of the powder products evidenced that mostly homogeneous gas-to-particle conversion takes place when applying an acidic precursor solution, whereas the absence of the acid leads to a dominant droplet-to-particle pathway. Our study indicates that a droplet-to-particle-pathway could be present even when processing the acidic formulation. However, even if a secondary pathway might take place in this case as well, it is not dominant and nearly negligible. Subsequently, the in situ particle structure evolution was investigated for the dominant gas-to-particle pathway, and particles were extracted along the flame axis for online SMPS and offline TEM/HRTEM analysis. Due to the highly reactive conditions within the flame (high temperatures, turbulent flow field, high particle number concentrations), the extraction of representative samples from spray flames is challenging. In order to handle the reactive conditions, two extraction techniques were tailored in this report. To extract an aerosol sample within the flame for SMPS measurement, a Hole in a Tube probe was adjusted. Thus, the mobility particle diameter as well as the corresponding distribution widths were obtained at different heights above the burner along the flame axis. For TEM/HRTEM image analysis, particle samples were collected thermophoretically by means of a tailored shutter system. Since all sampling grids were protected until reaching the flame axis and due to the low sampling time, momentary captures of local particle structures could be extracted precisely. The particle morphologies have clearly shown an evolution from spherical and paired particles in the flame center to fractal and compact agglomerates at later synthesis stages.

Comparison of Microphysical Characteristics between the Southern Korean Peninsula and Oklahoma Using Two-Dimensional Video Disdrometer Data

AbstractDifferences in atmospheric environments can have a significant impact on microphysical processes of precipitation. Dominant warm (cold) rain processes in East Asia (southern Great Plains of the United States) are implied by a large (small or constant) gradient of reflectivity at low levels in vertical reflectivity profiles. Long-term ground observations using two-dimensional video disdrometers were conducted in the southern Korean Peninsula (KOR) and Norman, Oklahoma, United States (OKL). Raindrop size distributions (RSD) and their moments in the two regions were analyzed in the framework of scaling normalized RSDs. Results show that the concentrations of small (big) raindrops were higher (smaller) in KOR than in OKL. KOR RSDs were also found to be characterized by relatively high characteristic number concentrations and small characteristic diameters when compared to OKL RSDs. The increases with increasing in both KOR and OKL at lower Z with the opposite trend at higher Z. In addition, OKL RSDs with indicate the existence of an equilibrium between coalescence and breakup processes. Rainfall estimation relationships between the rain rate R and radar variables were retrieved from scattering simulations at S-, C-, and X-band wavelengths. KOR RSDs showed relatively small horizontal reflectivity and specific differential phase shift at the same R and same wavelength when compared to OKL RSDs. The regional dependency was significant due to the different microphysical process in KOR and OKL. The specific attenuation of KOR was, however, similar to that of OKL only at S band, indicating an advantage of using specific attenuation in S band in rainfall estimation.

Effect of disc material on particulate matter emissions during high-temperature braking

Brake emissions during high-temperature brake applications were investigated using four different brake discs—FC170 and FC250 Gy iron discs, oxynitride-coated gray iron discs, and ceramic discs. The brake emission tests were performed with a low-steel brake pad using a 1/5 scale brake dynamometer with a high resolution electrical low-pressure impactor. The highest number concentration was observed using ceramic discs, whereas the gray iron discs produced higher mass concentrations than others. The effect of the disc material on brake emissions at elevated temperatures was primarily determined by the thermal conductivity of the disc and the time- and temperature-dependent variations of contact plateaus on the pad surface.

Fast and Purification-Free Characterization of Bio-Nanoparticles in Biological Media by Electrical Asymmetrical Flow Field-Flow Fractionation Hyphenated with Multi-Angle Light Scattering and Nanoparticle Tracking Analysis Detection.

Accurate physico-chemical characterization of exosomes and liposomes in biological media is challenging due to the inherent complexity of the sample matrix. An appropriate purification step can significantly reduce matrix interferences, and thus facilitate analysis of such demanding samples. Electrical Asymmetrical Flow Field-Flow Fractionation (EAF4) provides online sample purification while simultaneously enabling access to size and Zeta potential of sample constituents in the size range of approx. 1–1000 nm. Hyphenation of EAF4 with Multi-Angle Light Scattering (MALS) and Nanoparticle Tracking Analysis (NTA) detection adds high resolution size and number concentration information turning this setup into a powerful analytical platform for the comprehensive physico-chemical characterization of such challenging samples. We here present EAF4-MALS hyphenated with NTA for the analysis of liposomes and exosomes in complex, biological media. Coupling of the two systems was realized using a flow splitter to deliver the sample at an appropriate flow speed for the NTA measurement. After a proof-of-concept study using polystyrene nanoparticles, the combined setup was successfully applied to analyze liposomes and exosomes spiked into cell culture medium and rabbit serum, respectively. Obtained results highlight the benefits of the EAF4-MALS-NTA platform to study the behavior of these promising drug delivery vesicles under in vivo like conditions.

Characterization of raindrop size distributions and its response to cloud microphysical properties

Cloud feedbacks continue to alter with climate change, which remains the largest source of uncertainty in global climate. Raindrop size distribution (DSD) is a fundamental characteristic of cloud microphysical and dynamical processes. This study characterizes the DSD and its response to cloud microphysical properties during the Indian Summer Monsoon season (June-October 2013–2015). The derived rain rate varied from 0.50 to 395.4 mm/h, which was segregated into stratiform rain (mean and standard deviation of 2.12 ± 1.24 mm/h) and convective rain (13.10 ± 14.45 mm/h). We found that as the convective DSD mode diameter gradually shifts to a larger drop size with increasing rain rate, the number concentration of small-sized rain drops decreased by about three orders of magnitude. While the mass-weighted mean diameter and normalized DSD scaling parameter were significantly higher for convective rain than stratiform rain, the normalized DSD scaling parameter was lowest for both convective and stratiform rain compared to previous studies over this region. The stratiform DSD was more skewed towards large raindrop size at a high cloud effective radius compared to a low cloud effective radius. However, the opposite response of the DSD for convective rain suggests the predominance of small-sized cloud/ice hydrometeors. This finding was further corroborated by the presence of narrower DSD at high cloud droplet number concentration compared to a low cloud droplet number concentration for the convective rain. The low wind shear and high convective available potential energy for convective rain further substantiated the persistent convective cores during monsoon accompanied by the formation of large size raindrops in the convective systems. Such a distinct response of DSD to different rain regimes could help in the short-term prediction of extreme rainfall events.

Direct numerical simulations of nanoparticle formation in premixed and non-premixed flame–vortex interactions

Direct numerical simulations (DNSs) of nanoparticle formation in reactive flows are challenging, and only greatly simplified DNS test-cases are possible, which help clarify the turbulence–particle–dynamics interaction and guide the necessary modeling efforts. As a basis for such studies, a new DNS database is introduced, which resolves the smallest relevant scales of the nanoparticle concentration field to obtain insights into the statistics of nanoparticle formation in reactive flows. Formation and evolution of iron oxide nanoparticles in premixed and non-premixed flames wrapped-up by a vortex have been investigated using the sectional model and direct chemistry. The DNSs capture the “engulfing” and local dilution of the particle fields. Different zones of high particle number concentration have been found in every flame, and it was shown that the thickness of these zones decreases with increasing Schmidt number, which confirms that in simulations of nanoparticle-forming turbulent reacting flows, the grid resolution has to be very fine to resolve the characteristic scale for high sections. The contributions to the change in particle concentration due to diffusion, coagulation, and nucleation have been analyzed in detail, and dominant contributions across the particle number concentration layers and across the flames have been identified. This analysis has also been carried out in terms of flat, concave, and convex iso-surface geometries, induced by the flame–vortex interaction and characterized by the curvature of the particle number concentration fields and also by the flame curvature. The results demonstrate that the flame curvature effects cannot be ignored in modeling strategies. The probability density functions for the particle number concentrations have been analyzed and quantified in terms of Shannon information entropy, which illustrates the effect of fast diffusion (and entropy production) of the smaller particles and slow diffusion (and entropy production) of the largest particles with high Schmidt numbers. In addition, the unclosed filtered or averaged agglomeration term was evaluated as a basis for future modeling efforts, showing that agglomeration rates will be underestimated by orders of magnitude unless suitable models are developed.

Assessing emission and power tradeoffs of biodiesel and n-Butanol in diesel blends for fuel sustainability

The use of renewable biodiesel and additives diversifies transportation fuel supply. Combustion tests on neat ultra-low sulfur No.2 diesel (D100) and its blends with biodiesel and the n-butanol additive were conducted to investigate environmental impacts and tradeoffs in engine emission and power output. The testing results show measurable changes in power output and engine emission, particularly in diesel particulate matter (DPM) size distribution and black carbon compositions. The binary diesel-biodiesel blend D80B20 (80% D100 and 20%B100 by volume) offers reduced PM and black carbon emission, but higher NOx in engine exhaust. Comparatively the tertiary diesel-biodiesel-butanol blend B15Bu5 (80% D100, 15% B100, and 5% Bu100 by volume) shows superior environmental tradeoff in the black carbon and NOx emission than D80B20. Both fuel blends suffer a 3.0–5.6% increase in brake-specific fuel consumption. At higher combustion temperature, the butanol-oxygenated diesel fuel produces DPMs of smaller size, higher number concentrations, greater OC fractions, and more amorphous black carbon particles. The peak DPM aerodynamic size dpmax for D80B20 and B15Bu5 blends is 0.20–0.32 μm, smaller than >0.40 μm dpmax for D100 and the 0.30 μm cut-off size of regular DPM filters. For an internal combustion engine capable of accommodating biodiesel and water fraction in the fuel mixture, the B15Bu5 blend offers a viable fuel alternative according to the comparative testing results. The use of biodiesel and butanol additive in petroleum diesel can decrease the DPM emission, while the undesired NOx formation in tradeoff can be managed through optimizing the tertiary composition of petroleum diesel, biodiesel, and fuel additives.

Effects of continental emissions on cloud condensation nuclei (CCN) activity in the northern South China Sea during summertime 2018

Abstract. Aerosol particles in marine atmosphere have been shown to significantly affect cloud formation, atmospheric optical properties, and climate change. However, high temporally and spatially resolved atmospheric measurements over the sea are currently sparse, limiting our understanding of aerosol properties in marine atmosphere. In this study, a ship-based cruise campaign was conducted over the northern South China Sea (SCS) region during summertime 2018. The chemical composition of non-refractory PM1 (NR-PM1), the particle number size distribution (PNSD), and size-resolved cloud condensation nuclei (CCN) activity were measured by a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) and the combination of a cloud condensation nuclei counter (CCNc) and a scanning mobility particle sizer (SMPS). Overall, aerosol particles exhibited a unimodal distribution centering at 60–80 nm and the chemical composition of the NR-PM1 was dominated by sulfate (∼ 46 %), which likely originated from anthropogenic emissions rather than dimethyl sulfide (DMS) oxidation. Two polluted episodes (P1 and P2) were observed, and both were characterized by high particle number concentrations (NCN) which originated from local emissions and from emissions in inland China via long-range transport. The concentrations of trace gases (i.e., O3, CO, NOx) and particles (NCN and NCCN at ss = 0.34 %) were elevated during P2 at the end of the campaign and decreased with offshore distance, further suggesting important impacts of anthropogenic emissions from the inland Pearl River Delta (PRD) region. Two relatively clean periods (C1 and C2) prior to and after tropical storm Bebinca were classified and the air was affected by air masses from the southwest and from the Indo-Chinese Peninsula, respectively. Chemical composition measurements showed an increase in organic mass fraction during P2 compared to C2; however, no obviously different κ values were obtained from the CCNc measurements, implying that the air masses carried pollutants from local sources during long-range transport. We report an average value of about 0.4 for the aerosol hygroscopicity parameter κ, which falls within the literature values (i.e., 0.2–1.0) for urban and remote marine atmosphere. In addition, our results showed that the CCN fraction (NCCN∕NCN, tot) and the κ values had no clear correlation either with the offshore distance or with concentrations of the particles. Our study highlights dynamical variations in particle properties and the impact of long-range transport from continental China and the Indo-Chinese Peninsula on the northern SCS region during summertime.

Disdrometer, Polarimetric Radar, and Condensation Nuclei Observations of Supercell and Multicell Storms on 11 June 2018 in Eastern Nebraska

Disdrometer and condensation nuclei (CN) data are compared with operational polarimetric radar data for one multicell and one supercell storm in eastern Nebraska on 11 June 2018. The radar was located ~14.3 km from the instrumentation location and provided excellent observation time series with new low-level samples every 1–2 min. Reflectivity derived by the disdrometer and radar compared well, especially in regions with high number concentration of drops and reflectivity &lt;45 dBZ. Differential reflectivity also compared well between the datasets, though it was most similar in the supercell storm. Rain rate calculated by the disdrometer closely matched values estimated by the radar when reflectivity and differential reflectivity were used to produce the estimate. Concentration of CN generally followed precipitation intensity for the leading convective cell, with evidence for higher particle concentration on the edges of the convective cell associated with outflow. The distribution of CN in the supercell was more complex and generally did not follow precipitation intensity.

In Situ Quantitative Observation of Hygroscopic Growth of Single Nanoparticle Aerosol by Surface Plasmon Resonance Microscopy.

Aerosol particle hygroscopicity is an important factor in visibility reduction, cloud formation, radiation forcing, and the global climate. The high number concentration of nanoparticles (defined as particles with diameters below 100 nm) means that their hygroscopic growth abilities and potential contributions to the climate and environment are significant. Therefore, a rapid and accurate in situ analysis method for single nanoparticle hygroscopic growth in an atmospheric environment is important to characterize the effects of the particle's physical and chemical properties in this process. In this work, surface plasmon resonance microscopy with azimuthal rotation illumination (SPRM-ARI) is used to observe the hygroscopic growth and water content of single nanoparticles in situ. The hygroscopic growth results of a single-component nanoparticle are well matched with the extended aerosol inorganic model (E-AIM) results, and the proposed method remains reliable even when the relative humidity (RH) exceeds 90%. For a bicomponent nanoparticle (with NaCl as the primary content), the presence of a component without deliquescence phase transitions under increasing humidity conditions causes the measured data to differ from both the Zdanovskii-Stokes-Robinson (ZSR) model and E-AIM predictions in the low RH range. However, because of their complete liquefaction, the growth factor (GF) variation of the bicomponent nanoparticle is close to the model predictions in the high RH range. Finally, based on the positive correlation between particle volume and the gray intensity of SPRM-ARI, GF values can be obtained from the cube root of the gray intensity and the actual water content of single nanoparticles can then be derived.

Identifying a regional aerosol baseline in the eastern North Atlantic using collocated measurements and a mathematical algorithm to mask high-submicron-number-concentration aerosol events

Abstract. High-time-resolution measurements of in situ aerosol and cloud properties provide the ability to study regional atmospheric processes that occur on timescales of minutes to hours. However, one limitation to this approach is that continuous measurements often include periods when the data collected are not representative of the regional aerosol. Even at remote locations, submicron aerosols are pervasive in the ambient atmosphere with many sources. Therefore, periods dominated by local aerosol should be identified before conducting subsequent analyses to understand aerosol regional processes and aerosol–cloud interactions. Here, we present a novel method to validate the identification of regional baseline aerosol data by applying a mathematical algorithm to the data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility in the eastern North Atlantic (ENA). The ENA central facility (C1) includes an aerosol observing system (AOS) for the measurement of aerosol physical, optical, and chemical properties at time resolutions from seconds to minutes. A second temporary supplementary facility (S1), located ∼0.75 km from C1, was deployed for ∼1 year during the Aerosol and Cloud Experiments (ACE-ENA) campaign in 2017. First, we investigate the local aerosol at both locations. We associate periods of high submicron number concentration (Ntot) in the fine-mode condensation particle counter (CPC) and size distributions from the Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) as a function of wind direction using a meteorology sensor with local sources. Elevated concentrations of Aitken-mode (&lt; 100 nm diameter) particles were observed in correspondence with the wind directions associated with airport operations. At ENA, the Graciosa Airport and its associated activities were found to be the main sources of high-concentration aerosol events at ENA, causing peaks in 1 min Ntot that exceeded 8000 and 10 000 cm−3 at C1, in summer and winter, respectively, and 5000 cm−3 at S1 in summer. Periods with high Ntot not associated with these wind directions were also observed. As a result, the diverse local sources at ENA yielded a poor relationship between Ntot measurements collected at C1 and S1 (R2=0.03 with a slope =0.05±0.001). As a first approach to mask these events, the time periods when the wind direction was associated with the airport operations (west to northwest and southeast to south at C1 and east to south at S1) were applied. The meteorological masks removed 38.9 % of the data at C1 and 43.4 % at S1, and they did not significantly improve the relationship between the two sites (R2=0.18 with a slope =0.06±0.001). Due to the complexity of high-Ntot events observed at ENA, we develop and validate a mathematical ENA Aerosol Mask (ENA-AM) to identify high-Ntot events using 1 min resolution data from the AOS CPC at C1 and S1. After its parameterization and application, ENA-AM generated a high correlation between Ntot in the summer at C1 and S1 (R2=0.87 with a slope =0.84±0.001). We identified the regional baseline at ENA to be 428±228 cm−3 in the summer and 346±223 cm−3 in the winter. Lastly, we compared masked measurements from the AOS with the ARM Aerial Facility (AAF) during flights over C1 in the summer to understand submicron aerosol vertical mixing over C1. The high correlation (R2=0.71 with a slope of 1.04±0.01) observed between C1 and the AAF Ntot collected within an area of 10 km surrounding ENA and at altitudes &lt; 500 m indicated that the submicron aerosol at ENA was well mixed within the first 500 m of the marine boundary layer during the month of July during ACE-ENA. Our novel method for determining a regional aerosol baseline at ENA can be applied to other time periods and at other locations with validation by a secondary site or additional collocated measurements.