Aerosol Fluxes Research Articles

The sensitivity of Southern Ocean aerosols and cloud microphysics to sea spray and sulfate aerosol production in the HadGEM3-GA7.1 chemistry–climate model

Abstract. With low concentrations of tropospheric aerosol, the Southern Ocean offers a “natural laboratory” for studies of aerosol–cloud interactions. Aerosols over the Southern Ocean are produced from biogenic activity in the ocean, which generates sulfate aerosol via dimethylsulfide (DMS) oxidation, and from strong winds and waves that lead to bubble bursting and sea spray emission. Here, we evaluate the representation of Southern Ocean aerosols in the Hadley Centre Global Environmental Model version 3, Global Atmosphere 7.1 (HadGEM3-GA7.1) chemistry–climate model. Compared with aerosol optical depth (AOD) observations from two satellite instruments (the Moderate Resolution Imaging Spectroradiometer, MODIS-Aqua c6.1, and the Multi-angle Imaging Spectroradiometer, MISR), the model simulates too-high AOD during winter and too-low AOD during summer. By switching off DMS emission in the model, we show that sea spray aerosol is the dominant contributor to AOD during winter. In turn, the simulated sea spray aerosol flux depends on near-surface wind speed. By examining MODIS AOD as a function of wind speed from the ERA-Interim reanalysis and comparing it with the model, we show that the sea spray aerosol source function in HadGEM3-GA7.1 overestimates the wind speed dependency. We test a recently developed sea spray aerosol source function derived from measurements made on a Southern Ocean research voyage in 2018. In this source function, the wind speed dependency of the sea spray aerosol flux is less than in the formulation currently implemented in HadGEM3-GA7.1. The new source function leads to good agreement between simulated and observed wintertime AODs over the Southern Ocean; however, it reveals partially compensating errors in DMS-derived AOD. While previous work has tested assumptions regarding the seawater climatology or sea–air flux of DMS, we test the sensitivity of simulated AOD, cloud condensation nuclei and cloud droplet number concentration to three atmospheric sulfate chemistry schemes. The first scheme adds DMS oxidation by halogens and the other two test a recently developed sulfate chemistry scheme for the marine troposphere; one tests gas-phase chemistry only, while the second adds extra aqueous-phase sulfate reactions. We show how simulated sulfur dioxide and sulfuric acid profiles over the Southern Ocean change as a result and how the number concentration and particle size of the soluble Aitken, accumulation and coarse aerosol modes are affected. The new DMS chemistry scheme leads to a 20 % increase in the number concentration of cloud condensation nuclei and cloud droplets, which improves agreement with observations. Our results highlight the importance of atmospheric chemistry for simulating aerosols and clouds accurately over the Southern Ocean.

Sea spray fluxes from the southwest coast of the United Kingdom – dependence on wind speed and wave height

Abstract. Fluxes of sea spray aerosols were measured with the eddy covariance technique from the Penlee Point Atmospheric Observatory (PPAO) on the southwest coast of the United Kingdom over several months from 2015 to 2017. Two different fast-responding aerosol instruments were employed: an ultra-fine condensation particle counter (CPC) that detects aerosols with a radius above ca. 1.5 nm and a compact lightweight aerosol spectrometer probe (CLASP) that provides a size distribution between ca. 0.1 and 6 µm. The measured sea spray emission fluxes essentially all originated from the shallow waters upwind, rather than from the surf zone/shore break. Fluxes from the CPC and from the CLASP (integrated over all sizes) were generally comparable, implying a reasonable closure in the aerosol number flux. Compared to most previous observations over the open ocean, at the same wind speed the mean sea spray number fluxes at PPAO are much greater. Significant wave height and wave Reynolds numbers explain more variability in sea spray fluxes than wind speed does, implying that enhanced wave breaking resulting from shoaling in shallow coastal waters is a dominant control on sea spray emission. Comparisons between two different wind sectors (open water vs. fetch-limited Plymouth Sound) and between two sets of sea states (growing vs. falling seas) further confirm the importance of wave characteristics on sea spray fluxes. These results suggest that spatial variability in wave characteristics need to be taken into account in predictions of coastal sea spray productions and also aerosol loading.

Aerosol vertical mass flux measurements during heavy aerosol pollution episodes at a rural site and an urban site in the Beijing area of the North China Plain

Abstract. Due to excessive anthropogenic emissions, heavy aerosol pollution episodes (HPEs) often occur during winter in the Beijing–Tianjin–Hebei (BTH) area of the North China Plain. Extensive observational studies have been carried out to understand the causes of HPEs; however, few measurements of vertical aerosol fluxes exist, despite them being the key to understanding vertical aerosol mixing, specifically during weak turbulence stages in HPEs. In the winter of 2016 and the spring of 2017 aerosol vertical mass fluxes were measured by combining large aperture scintillometer (LAS) observations, surface PM2.5 and PM10 mass concentrations, and meteorological observations, including temperature, relative humidity (RH), and visibility, at a rural site in Gucheng (GC), Hebei Province, and an urban site at the Chinese Academy of Meteorological Sciences (CAMS) in Beijing located 100 km to the northeast. These are based on the light propagation theory and surface-layer similarity theory. The near-ground aerosol mass flux was generally lower in winter than in spring and weaker in rural GC than in urban Beijing. This finding provides direct observational evidence for a weakened turbulence intensity and low vertical aerosol fluxes in winter and polluted areas such as GC. The HPEs included a transport stage (TS), an accumulative stage (AS), and a removal stage (RS). During the HPEs from 25 to 31 January 2017, in Beijing, the mean mass flux decreased by 51 % from 0.0049 mg m−2 s−1 in RSs to 0.0024 mg m−2 s−1 in the TSs. During the ASs, the mean mass flux decreased further to 0.00087 mg m−2 s−1, accounting for approximately one-third of the flux in the TSs. A similar reduction from the TSs to ASs was observed in the HPE from 16 to 22 December 2016 in GC. It can be seen that from the TS to the AS, the aerosol vertical turbulent flux decreased, but the aerosol particle concentration within the surface layer increased, and it is inferred that in addition to the contribution of regional transport from upwind areas during the TS, suppression of vertical turbulence mixing confining aerosols to a shallow boundary layer increased accumulation.

Size-resolved aerosol fluxes above a broadleaved deciduous forest

In order to understand the aerosol exchange dynamics between the atmosphere and a peri-urban forest ecosystem located in the Po Valley, a region characterized by high PM concentrations, eddy covariance (EC) aerosol fluxes were measured between September and December 2017. The aerosol sampling, performed with an Electrical Low Pressure Impactor (ELPI +, DEKATI), involved a wide range of particle sizes including both ultrafine and fine aerosol. The monitoring campaign comprised a period with leaves (PL) and a period without leaves (PNL) to assess their influence on the emission and deposition fluxes.The diurnal profiles of particle number (PN) fluxes associated to the geometric mean diameters (GMD) of 0.02 µm and 0.48 µm were chosen as representative of the behaviour of ultrafine and fine particles, respectively. Fluxes of ultrafine particles showed a net emission pattern both in PL and PNL assuming values up to 5.6 106 m−2 s−1 and 4.5·106 m−2 s−1, respectively. Instead, fine particles fluxes showed a net deposition pattern in PL, assuming values up to −1.1 · 106 m−2 s−1, while in PNL a slight emission up to 4.1 ·105 m−2 s−1 occurred. The behaviour of the fluxes of the cumulative classes PM0.1 and PM1 was similar to the one of the PN fluxes of ultrafine and fine aerosol, respectively.Deposition velocities were calculated for PL and PNL depending on the atmospheric stability class. The values emerged from this study (from −0.25 cm s−1 up to 0.12 cm s−1) evidenced that under stable and very stable atmospheric conditions all size classes presented negative or slightly positive deposition velocities both in PL and PNL. Instead under unstable conditions fine particles showed deposition velocities whose direction changed in the two periods (PL and PNL).

Relative importance of gas uptake on aerosol and ground surfaces characterized by equivalent uptake coefficients

Abstract. Quantifying the relative importance of gas uptake on the ground and aerosol surfaces helps to determine which processes should be included in atmospheric chemistry models. Gas uptake by aerosols is often characterized by an effective uptake coefficient (γeff), whereas gas uptake on the ground is usually described by a deposition velocity (Vd). For efficient comparison, we introduce an equivalent uptake coefficient (γeqv) at which the uptake flux of aerosols would equal that on the ground surface. If γeff is similar to or larger than γeqv, aerosol uptake is important and should be included in atmospheric models. In this study, we compare uptake fluxes in the planetary boundary layer (PBL) for different reactive trace gases (O3, NO2, SO2, N2O5, HNO3 and H2O2), aerosol types (mineral dust, soot, organic aerosol and sea salt aerosol), environments (urban areas, agricultural land, the Amazon forest and water bodies), seasons and mixing heights. For all investigated gases, γeqv ranges from magnitudes of 10−6–10−4 in polluted urban environments to 10−4–10−1 under pristine forest conditions. In urban areas, aerosol uptake is relevant for all species (γeff≥γeqv) and should be considered in models. On the contrary, contributions of aerosol uptakes in the Amazon forest are minor compared with the dry deposition. The phase state of aerosols could be one of the crucial factors influencing the uptake rates. Current models tend to underestimate the O3 uptake on liquid organic aerosols which can be important, especially over regions with γeff≥γeqv. H2O2 uptakes on a variety of aerosols are yet to be measured under laboratory conditions and evaluated. Given the fact that most models have considered the uptakes of these species on the ground surface, we suggest also considering the following processes in atmospheric models: N2O5 uptake by all types of aerosols, HNO3 and SO2 uptake by mineral dust and sea salt aerosols, H2O2 uptake by mineral dust, NO2 uptakes by sea salt aerosols and O3 uptake by liquid organic aerosols.

Optical density of testing aerosol and fire smoke in a road tunnel with longitudinal ventilation: comparison by FDS6

Specific testing aerosol is used for road tunnel ventilation tests to represent steady-state movement of fire smoke downstream of the fire and to avoid the damage of the tunnel. This study investigates the spread of aerosol in 240 m long section of a road tunnel by computer simulation using the well-known FDS simulation system and compares it with the fire smoke spread. Conditions under which optical density for both cases is similar are determined, mainly the mass flux of aerosol needed to represent the smoke produced by fire and the distance at which steady-state flow of smoke is formed. The influence of the fire HRR and air flow velocity on the determined aerosol mass flux is studied as well. The determined value of mass flux increases with increasing flow velocity and decreases with increasing fire HRR. The results indicate that the aerosol can be used to represent the optical density of steady-state fire smoke spread downstream of the fire in tunnel ventilation tests.

Abundance and Emission Flux of the Anthropogenic Iron Oxide Aerosols From the East Asian Continental Outflow

AbstractAnthropogenic iron oxide (FeOx) aerosols can affect atmospheric radiation, marine biogeochemistry, and human health. However, due to lack of observational data, their atmospheric abundance and emission flux are not well understood. In this study, we observed size‐resolved concentrations of FeOx (170–2100 nm) and black carbon (BC, 70–850 nm) aerosols at a remote site in the East China Sea in March 2016 using a modified single‐particle soot photometer (SP2). Light signals measured by the SP2 and particle morphology and compositions analyzed by a transmission electron microscope revealed that most of the observed FeOx aerosols are of anthropogenic origin. Clear correlations were found between mass concentrations of FeOx and BC (R2 = 0.717) and between FeOx and carbon monoxide (CO) (R2 = 0.718) in air masses from China, indicating that their emission sources are spatially similar. The correlation slopes of mass concentration (ng/m3) are ~0.3 and 0.0015, respectively. Based on the correlation slopes and emission inventories of BC and CO in China, we estimated emission flux of anthropogenic FeOx aerosols from China to be 0.21–0.49 FeTg/yr. Based on the observed size distribution and previous studies on mass fraction of FeOx and non‐FeOx, we also estimated emission flux of anthropogenic Fe (FeOx + non‐FeOx) in PM10 as 0.74–1.7 FeTg/yr. These emission fluxes from China are comparable to global emission fluxes in currently reported inventories of anthropogenic Fe (0.51–1.91 FeTg/yr). Our results suggest that the current emission inventories of anthropogenic Fe are underestimated.

Size-resolved aerosol fluxes above a temperate broadleaf forest

Aerosol fluxes were measured by eddy-correlation for 8 weeks of the summer and fall of 2011 above a temperate broadleaf forest in central Ontario, Canada. These size-resolved measurements apply to particles with optical diameters between 50 and 500 nm and are the first ones reported above a temperate deciduous forest. The particle spectrometer was located on top of the flux tower in order to reduce signal dampening in the tube and thus maximize measurement efficiency. The 8-week data set extends into autumn, capturing leaf senescence and loss, offering a rare opportunity to investigate the influence of leaf area index on particle transfer. A distinct pattern of emission and deposition that depends on the particle size is highlighted: while the smallest particles (dp < 100 nm) are preferentially emitted (55% of the time), the largest particles (dp > 100 nm) are preferentially deposited (62% of the time). For the size bins with detection efficiency above 50% (68–292 nm), the median transfer velocity for each bin varies between +1.34 and −2.69 mm s−1 and is equal to −0.21 mm s−1 for the total particle count. The occurrence of the upward fluxes shows a marked diurnal pattern. Possible explanations for these upward fluxes are proposed. The measurements, and their comparison with an existing model, highlight some of the key drivers of the particle transfer onto a broadleaf forest: particle size, friction velocity, leaf area index and atmospheric stability.

Marine aerosol fluxes determined by simultaneous measurements of eddy covariance and gradient method

In this paper the results of the aerosol flux measurements in near water boundary layer are presented. Measurements were conducted using two micrometeorological methods in the southern Baltic Sea region. The preliminary results of comparisons of two methods are discussed. The eddy covariance (EC) method is shown as a method for the calibration of the gradient method (GM). The reason for proceeding with such calibration is to show that the GM, which is an indirect measuring method, is comparable with a direct method such as the EC. In the EC measurements the condensation particle counter (CPC, measuring range 0.05 - 3 m with 1 Hz counting speed) and the Research Anemometer (50 Hz measurement speed) were used. For the GM, a Classical Scattering Aerosol Spectrometer was applied (measuring range from 0.5 to 47 m diameter, within 36 measuring channels). Data from scientific cruises of the r/v Oceania in the southern Baltic Sea between 2008 and 2011 were analyzed.

Aerosols in the Near-Water Surface Layer of the Caspian Sea

The first data on the concentrations, fluxes, and mineral and chemical compositions of aerosols from the near-water surface layer of the Caspian Sea are presented. It is shown that the aerosol fluxes onto the sea surface are comparable to the fluxes of a lithogenic substance in a water column. The mineral and chemical compositions of aerosols depend on the carrying air masses that pass through different regions. The coefficients of enrichment of aerosols with chemical elements relative to the upper lithosphere and their correlation relationships are studied.

Primary marine aerosol physical flux and chemical composition during a nutrient enrichment experiment in mesocosms in the Mediterranean Sea

Abstract. While primary marine aerosol (PMA) is an important part of global aerosol total emissions, its chemical composition and physical flux as a function of the biogeochemical properties of the seawater still remain highly uncharacterized due to the multiplicity of physical, chemical and biological parameters that are involved in the emission process. Here, two nutrient-enriched mesocosms and one control mesocosm, both filled with Mediterranean seawater, were studied over a 3-week period. PMA generated from the mesocosm waters were characterized in term of chemical composition, size distribution and size-segregated cloud condensation nuclei (CCN), as a function of the seawater chlorophyll a (Chl a) concentration, pigment composition, virus and bacteria abundances. The aerosol number size distribution flux was primarily affected by the seawater temperature and did not vary significantly from one mesocosm to the other. The aerosol number size distribution flux was primarily affected by the seawater temperature and did not vary significantly from one mesocosm to the other. Particle number and CCN aerosol fluxes increase by a factor of 2 when the temperature increases from 22 to 32 °C, for all particle submicron sizes. This effect, rarely observed in previous studies, could be specific to oligotrophic waters and/or to this temperature range. In all mesocosms (enriched and control mesocosms), we detected an enrichment of calcium (+500 %) and a deficit in chloride (−36 %) in the submicron PMA mass compared to the literature inorganic composition of the seawater. There are indications that the chloride deficit and calcium enrichment are linked to biological processes, as they are found to be stronger in the enriched mesocosms. This implies a non-linear transfer function between the seawater composition and PMA composition, with complex processes taking place at the interface during the bubble bursting. We found that the artificial phytoplankton bloom did not affect the CCN activation diameter (Dp, 50, average = 59.85±3.52 nm and Dp,50,average = 93.42±5.14 nm for supersaturations of 0.30 and 0.15 % respectively) or the organic fraction of the submicron PMA (average organic to total mass = 0.31±0.07) compared to the control mesocosm. Contrary to previous observations in natural bloom mesocosm experiments, the correlation between the particle organic fraction and the seawater Chl a was poor, indicating that Chl a is likely not a straightforward proxy for predicting, on a daily scale, PMA organic fraction in models for all types of sea and ocean waters. Instead, the organic fraction of the Aitken mode particles were more significantly linked to heterotrophic flagellates, viruses and dissolved organic carbon (DOC). We stress that different conclusions may be obtained in natural (non-enriched) or non-oligotrophic systems.

Trans-Atlantic Connections between North African Dust Flux and Tree Growth in the Florida Keys, United States

Abstract Atmospheric mineral aerosols include multiple, interrelated processes and feedbacks within the context of land–atmosphere interactions and thus are poorly understood. As the largest dust source in the world, North Africa supplies mineral dust aerosols each year to the Caribbean region and southeastern United States that alter cloud processes, ocean productivity, soil development, and the radiation budget. This study uses a suite of Earth Observation and ground-based analyses to reveal a potential novel effect of atmospheric aerosols on Pinus elliottii var. densa cambial growth during the 2010 CE growing season from the Florida Keys. Over the Florida Keys region, the Earth Observation products captured increased aerosol optical thickness with a clear geographical connection to mineral dust aerosols transported from northern Africa. The MODIS Terra and Aqua products corroborated increased Ozone Monitoring Instrument (OMI) aerosol optical thickness values. Anomalously high Aerosol Robotic Network aerosol optical depth data corresponding with low Ångstrom coefficients confirm the presence of transported mineral dust aerosols during the period circa 4–20 July 2010. The fraction of photosynthetically absorbed radiation over the region during July 2010 experienced an anomalous decrease, concurrent with reduced incoming total and direct solar radiation resulting in a reduced growth response in P. elliottii. The authors pose one of the primary mechanisms responsible for triggering growth anomalies in P. elliottii is the reduction of total photosynthetically active radiation due to a dust-derived increase in aerosol optical depth. As a rare long-lived conifer (300+ years) in a subtropical location, P. elliottii could represent a novel proxy with which to reconstruct annual or seasonal mineral dust aerosol fluxes over the Caribbean region.

Dimethylsulfide model calibration and parametric sensitivity analysis for the Greenland Sea

Sea-to-air fluxes of marine biogenic aerosols have the potential to modify cloud microphysics and regional radiative budgets, and thus moderate Earth's warming. Polar regions play a critical role in the evolution of global climate. In this work, we use a well-established biogeochemical model to simulate the DMS flux from the Greenland Sea (20°W–10°E and 70°N–80°N) for the period 2003–2004. Parameter sensitivity analysis is employed to identify the most sensitive parameters in the model. A genetic algorithm (GA) technique is used for DMS model parameter calibration. Data from phase 5 of the Coupled Model Intercomparison Project (CMIP5) are used to drive the DMS model under 4 × CO2 conditions. DMS flux under quadrupled CO2 levels increases more than 300% compared with late 20th century levels (1 × CO2). Reasons for the increase in DMS flux include changes in the ocean state—namely an increase in sea surface temperature (SST) and loss of sea ice—and an increase in DMS transfer velocity, especially in spring and summer. Such a large increase in DMS flux could slow the rate of warming in the Arctic via radiative budget changes associated with DMS-derived aerosols.

The sources of trace element pollution of dry depositions nearby a drinking water source.

Miyun Reservoir is one of the most important drinking water sources for Beijing. Thirteen atmospheric PM sampling sites were established around this reservoir to analyze the mineral composition, morphological characteristics, element concentration, and sources of atmospheric PM pollution, using transmission electron microscope, X-ray diffraction, and inductively coupled plasma mass spectrometry analyses. The average monthly dry deposition flux of aerosols was 15.18g/m2, with a range of 5.78-47.56g/m2. The maximum flux season was winter, followed by summer, autumn, and spring. Zn and Pb pollution in this area was serious, and some of the sample sites had Cr, Co, Ni, and Cu pollution. Deposition fluxes of Zn/Pb in winter and summer reached 99.77/143.63 and 17.04/33.23g/(hm2 month), respectively. Principal component analysis showed two main components in the dry deposition; the first was Cr, Co, Ni, Cu, and Zn, and the other was Pb and Cd. Principal sources of the trace elements were iron mining and other anthropogenic activities in the surrounding areas and mountainous area north of the reservoir. Mineralogy analysis and microscopic conformation results showed many iron minerals and some unweathered minerals in dry deposition and atmospheric particulate matter, which came from an iron ore yard in the northern mountainous area of Miyun County. There was possible iron-rich dry deposition into Miyun Reservoir, affecting its water quality and harming the health of people living in areas around the reservoir and Beijing.

Chemical characteristics and deposition fluxes of dust-carbon mixed coarse aerosols at three sites of Delhi, NCR

The present paper reports chemistry and fluxes of dust-carbon mixed coarse particles. For the purpose of this study, different carbonaceous fractions i.e. organic carbon ((OC), elemental carbon (EC) and carbonate carbon (CC) of atmospheric dust and their respective local soils were quantified at three sites of National Capital Region (NCR) of Delhi viz. Jawaharlal Nehru University campus (JNU), Connaught Place (CP) and Vishali area of Ghaziabad (GB). It has been observed that the OC and EC levels were approximately five to nine times higher in urban atmospheric dust than their corresponding soils, whereas CC levels were about three times higher than the corresponding soils. Average dustfall fluxes were significantly different at all the sites due to their different land-use patterns. At urban background site (JNU), the dust flux was lowest (172 mg/m2/day) followed by CP, a commercial site, (192 mg/m2/day) and GB, an industrial/residential area, (302 mg/m2/day). Similar to the dustfall pattern, the mean values of OC, EC and CC deposition fluxes were also observed to be lowest at JNU (9.2, 0.8 and 1.0 mg/m2/day, respectively) as compared to CP (12.2, 1.2 and 1.3 mg/m2/day, respectively) and GB sites (11.1, 1.1 and 1.4 mg/m2/day, respectively). Interestingly, unlike fine mode, different correlation pattern of OC and EC in coarse mode dust aerosols at three sites has suggested their independent deposition processes and source contribution. Fluxes of major water soluble inorganic ions (Na+, NH4+, K+, Ca2+, Mg2+, F−, Cl−, NO3− and SO42−) were also determined. Ca2+, Cl− and SO42− were found to be the major ionic species of water soluble fraction of the urban dust at all the sites. These interactions are corroborated by the morphology of the mixed aerosols. High levels of measured chemical species and their spatial distribution revealed close correspondence with the local emissions from transport, industries, biomass burning, road dust and construction activities etc.

Land’s complex role in climate change

To mitigate climate change at local, regional, and global scales, we must begin to think beyond greenhouse gases.

Sea spray aerosol fluxes in the Baltic Sea region: Comparison of the WAM model with measurements

Sea spray aerosol flux is an important element of sub-regional climate modeling. The majority of works related to this topic concentrate on open ocean research rather than on smaller, inland seas, e.g., the Baltic Sea. The Baltic Sea is one of the largest brackish inland seas by area, where major inflows of oceanic waters are rare. Furthermore, surface waves in the Baltic Sea have a relatively shorter lifespan in comparison with oceanic waves. Therefore, emission of sea spray aerosol may differ greatly from what is known from oceanic research and should be investigated. This article presents a comparison of sea spray aerosol measurements carried out on-board the s/y Oceania research ship with data calculated in accordance to the WAM model. The measurements were conducted in the southern region of the Baltic Sea during four scientific cruises. The gradient method was used to determinate aerosol fluxes. The fluxes were calculated for particles of diameter in range of 0.5–47 μm. The correlation between wind speed measured and simulated has a good agreement (correlation in range of 0.8). The comparison encompasses three different sea spray generation models. First, function proposed by Massel (2006) which is based only on wave parameters, such as significant wave height and peak frequency. Second, Callaghan (2013) which is based on Gong (2003) model (wind speed relation), and a thorough experimental analysis of whitecaps. Third, Petelski et al. (2014) which is based on in-situ gradient measurements with the function dependent on wind speed. The two first models which based on whitecaps analysis are insufficient. Moreover, the research shows strong relation between aerosol emission and wind speed history.

Return of naturally sourced Pb to Atlantic surface waters.

Anthropogenic emissions completely overwhelmed natural marine lead (Pb) sources during the past century, predominantly due to leaded petrol usage. Here, based on Pb isotope measurements, we reassess the importance of natural and anthropogenic Pb sources to the tropical North Atlantic following the nearly complete global cessation of leaded petrol use. Significant proportions of up to 30–50% of natural Pb, derived from mineral dust, are observed in Atlantic surface waters, reflecting the success of the global effort to reduce anthropogenic Pb emissions. The observation of mineral dust derived Pb in surface waters is governed by the elevated atmospheric mineral dust concentration of the North African dust plume and the dominance of dry deposition for the atmospheric aerosol flux to surface waters. Given these specific regional conditions, emissions from anthropogenic activities will remain the dominant global marine Pb source, even in the absence of leaded petrol combustion.

Lidar remote sensing of cloud formation caused by low‐level jets

AbstractIn May 2014, the East Hampton Roads Aerosol Flux campaign was conducted at Hampton University to examine small‐scale aerosol transport using aerosol, Raman, and Doppler lidars and rawindsonde launches. We present the results of analyses performed on these high‐resolution planetary boundary layer and lower atmospheric measurements, with a focus on the low‐level jets (LLJs) that form in this region during spring and summer. We present a detailed case study of a LLJ lasting from evening of 20 May to morning of 21 May using vertical profiles of aerosol backscatter, wind speed and direction, water vapor mixing ratio, temperature, and turbulence structure. We show with higher resolution than in previous studies that enhanced nighttime turbulence triggered by LLJs can cause the aerosol and water vapor content of the boundary layer to be transported vertically and form a well‐mixed region containing the cloud condensation nuclei that are necessary for cloud formation.

A new method for estimating aerosol mass flux in the urban surface layer using LAS technology

Abstract. Atmospheric aerosol greatly influences human health and the natural environment, as well as the weather and climate system. Therefore, atmospheric aerosol has attracted significant attention from society. Despite consistent research efforts, there are still uncertainties in understanding its effects due to poor knowledge about aerosol vertical transport caused by the limited measurement capabilities of aerosol mass vertical transport flux. In this paper, a new method for measuring atmospheric aerosol vertical transport flux is developed based on the similarity theory of surface layer, the theory of light propagation in a turbulent atmosphere, and the observations and studies of the atmospheric equivalent refractive index (AERI). The results show that aerosol mass flux can be linked to the real and imaginary parts of the atmospheric equivalent refractive index structure parameter (AERISP) and the ratio of aerosol mass concentration to the imaginary part of the AERI. The real and imaginary parts of the AERISP can be measured based on the light-propagation theory. The ratio of the aerosol mass concentration to the imaginary part of the AERI can be measured based on the measurements of aerosol mass concentration and visibility. The observational results show that aerosol vertical transport flux varies diurnally and is related to the aerosol spatial distribution. The maximum aerosol flux during the experimental period in Hefei City was 0.017 mg m−2 s−1, and the mean value was 0.004 mg m−2 s−1. The new method offers an effective way to study aerosol vertical transport in complex environments.