Climatology of aerosols over the Caribbean islands: aerosol types, synoptic patterns and transport

We present a climatological study of aerosols in four representative Caribbean islands based on daily mean values of aerosol optical properties for the period 2008- 2016, using the Aerosol Optical Depth (AOD) and Ångström Exponent (AE) to classify the dominant aerosol type. A climatological assessment of the spatio-temporal distribution of the main aerosol types, their links with synoptic patterns and the transport from different sources is provided. Maximum values of AOD occur in the rainy season, coinciding with the minimum in AE and an increased occurrence of dust, while the minimum of AOD occurs in the dry season, due to the predominance of marine aerosols. Marine and dust aerosol are more frequent in the easternmost islands and decrease westwards due to an increasing of continental and mixture dust aerosols. Therefore, the westernmost station displays the most heterogeneous composition of aerosols. Using a weather type classification, we identify a quantifiable influence of the atmospheric circulation in the distribution of Caribbean aerosols. However, they can occur under relatively weak and/or diverse synoptic patterns, typically involving transient systems and specific configurations of the Azores High that depend on the considered station. Backward trajectories indicate that dry-season marine aerosols and rainy-season dust are transported by air parcels travelling within the tropical easterly winds. The main source region for both types of aerosols is the subtropical eastern Atlantic, except for Cuba, where the largest contributor to dry-season marine aerosols is the subtropical western Atlantic. Different aerosol types follow similar pathways, suggesting a key role of emission sources in determining the spatio-temporal distribution of Caribbean aerosols.

Analysis and Sources Identification of Atmospheric PM10 and Its Cation and Anion Contents in Makkah, Saudi Arabia

In this paper, atmospheric water-soluble cation and anion contents of PM10 are analysed in Makkah, Saudi Arabia. PM10 samples were collected at five sites for a whole year. PM10 concentrations (µg/m3) ranged from 82.11 to 739.61 at Aziziyah, 65.37 to 421.71 at Sanaiyah, 25.20 to 466.60 at Misfalah, 52.56 to 507.23 at Abdeyah, and 40.91 to 471.99 at Askan. Both daily and annual averaged PM10 concentrations exceeded WHO and Saudi Arabia national air quality limits. Daily averaged PM10 concentration exceeded the national air quality limits of 340 µg/m3, 32% of the time at Aziziyah, 8% of the time at Sanaiyah, and 6% of the time at the other three sites. On average, the cations and anions made a 37.81% contribution to the PM10 concentrations. SO42−, NO3−, Ca2+, Na+, and Cl− contributed 50.25%, 16.43%, 12.11%, 11.12%, and 8.70% to the total ion concentrations, respectively. The minor ions (F−, Br−, Mg2+, NO2−, and PO43−) contributed just over 1% to the ion mass. Four principal components explained 89% variations in PM10 concentrations. Four major emission sources were identified: (a) Road traffic, including emission from the exhaust, wear-and-tear, and the resuspension of dust particles (F−, SO42−, NO3−, Ca2+, Na+, Mg+, Br−, Cl−, NO2−, PO43−); (b) Mineral dust (Cl−, F−, Na+, Ca2+, Mg2+, PO43−); (c) Industries and construction–demolition work (F−, SO42−, Ca2+, Mg2+); and (d) Seaspray and marine aerosols (Cl−, Br−, Mg2+, Na+). Future work would include an analysis of the metal contents of PM10 and their spatiotemporal variability in Makkah.

Precipitation chemistry over the Indian region

The present study is based on the precipitation chemistry data from the Background Air Pollution Monitoring Network (BAPMoN) in the Indian region, for the period 1976-87. Sampling is made on an event basis and the pH and electrical conductivity of the samples are determined from filtered samples immediately after cessation of rain. The chemical analysis is performed on monthly mixed samples. No trend is found in the pH of rainwater from background areas except at Allahabad, Pune and Visakhapatnam which suffer from sizable anthropogenic influences. The pH seems to be related more to NO3 ions compared to SO4-2 ions. A natural buffer appearing in the form of alkaline soil-derived species seems adequateat most places (except Mohanbari), in keeping a check on progressive acidification despite steady increase in concentration of nitrates. The ion balance cannot be achieved without including the presence of HCO3, which when done explains the observed electrical conductivity of rainwater. The interaction of marine aerosols with acid aerosols has also been studied for the marine regions in the Indian areas and reveals a substantial removal of chloride from sea-salt. Inland sources of NaCl have also been identified from the BAPMoN data.

Assessing the benefits of Imaging Infrared Radiometer observations to the CALIOP version 4 cloud and aerosol discrimination algorithm

The features detected in monolayer atmospheric columns sounded by the Cloud and Aerosol Lidar with Orthogonal Polarization (CALIOP) and classified as cloud or aerosol layers by the CALIOP version 4 (V4) cloud and aerosol discrimination (CAD) algorithm are reassessed using perfectly collocated brightness temperatures measured by the Imaging Infrared Radiometer (IIR) onboard the same satellite. Using the IIR’s three wavelength measurements of layers that are confidently classified by the CALIOP CAD algorithm, we calculate two-dimensional (2-D) probability distribution functions (PDFs) of IIR brightness temperature differences (BTDs) for different cloud and aerosol types. We then compare these PDFs with 1-D radiative transfer simulations for ice and water clouds and dust and marine aerosols. Using these IIR 2-D BTD signature PDFs, we develop and deploy a new IIR-based CAD algorithm and compare the classifications obtained to the results reported by the CALIOP-only V4 CAD algorithm. IIR observations are shown to be able to identify clouds with a good accuracy. The IIR cloud identifications agree very well with layers classified as confident clouds by the V4 CAD algorithm (88 %). More importantly, simultaneous use of IIR information reduces the ambiguity in a notable fraction of "not confident" V4 cloud classifications. 28 % and 14 % of the ambiguous V4 cloud classifications are confirmed thanks to the IIR observations in the tropics and in the midlatitudes respectively. IIR observations are of relatively little help in deriving high confidence classifications for most aerosols, as the low altitudes and small optical depths of aerosol layers yield IIR signatures that are similar to those from clear skies. However, misclassifications of aerosol layers, such as dense dust or elevated smoke layers, by the V4 CAD algorithm can be corrected to cloud layer classification by including IIR information. 10 %, 16 %, and 6 % of the ambiguous V4 dust, polluted dust, and tropospheric elevated smoke respectively are found to be misclassified cloud layers by the IIR measurements.

Soluble Iodine Speciation in Marine Aerosols Across the Indian and Pacific Ocean Basins

Iodine affects the radiative budget and the oxidative capacity of the atmosphere and is consequently involved in important climate feedbacks. A fraction of the iodine emitted by oceans ends up in aerosols, where complex halogen chemistry regulates the recycling of iodine to the gas-phase where it effectively destroys ozone. The iodine speciation and major ion composition of aerosol samples collected during four cruises in the East and West Pacific and Indian Oceans was studied to understand the influences on iodine’s gas-aerosol phase recycling. A significant inverse relationship exists between iodide (I–) and iodate (IO3–) proportions in both fine and coarse mode aerosols, with a relatively constant soluble organic iodine (SOI) fraction of 19.8% (median) for fine and coarse mode samples of all cruises combined. Consistent with previous work on the Atlantic Ocean, this work further provides observational support that IO3– reduction is attributed to aerosol acidity, which is associated to smaller aerosol particles and air masses that have been influenced by anthropogenic emissions. Significant correlations are found between SOI and I–, which supports hypotheses that SOI may be a source for I–. This data contributes to a growing observational dataset on aerosol iodine speciation and provides evidence for relatively constant proportions of iodine species in unpolluted marine aerosols. Future development in our understanding of iodine speciation depends on aerosol pH measurements and unravelling the complex composition of SOI in aerosols.

Assessment of tropospheric CALIPSO Version 4.2 aerosol types over the ocean using independent CALIPSO-SODA lidar ratios

We assess the CALIPSO Version 4.2 (V4) aerosol typing and assigned lidar ratios over ocean using aerosol optical depth (AOD) retrievals from the Synergized Optical Depth of Aerosols (SODA) algorithm and retrieved columnar lidar ratio estimated by combining SODA AOD and CALIPSO attenuated backscatter (CALIPSO-SODA). Six aerosol types – clean marine, dusty marine, dust, polluted continental/smoke, polluted dust, and elevated smoke – are characterized using CALIPSO-SODA over ocean and the results are compared against the prescribed V4 lidar ratios, when only one aerosol type is present in the atmospheric column. For samples detected at 5-km or 20-km spatial resolutions and having AOD > 0.05, the CALIPSO-SODA lidar ratios are significantly different between different aerosol types, and are consistent with the type-specific values assigned in V4 to within 10 sr (except for polluted continental/smoke). This implies that the CALIPSO classification scheme generally categorizes aerosols correctly. We find remarkable daytime/nighttime regional agreement for clean marine aerosol over the open ocean (CALIPSO-SODA = 20–25 sr, V4 = 23 sr), elevated smoke over the southeast Atlantic (CALIPSO-SODA = 65–75 sr, V4 = 70 sr), and dust over the subtropical Atlantic adjacent to the African continent (CALIPSO-SODA = 40–50 sr, V4 = 44 sr). In contrast, daytime polluted continental/smoke lidar ratio is more than 20 sr smaller than the constant V4 vaue for that type, attributed in part to the challenge of classifying tenuous aerosol with low signal-to-noise ratio. Dust over most of the Atlantic Ocean features CALIPSO-SODA lidar ratios less than 40 sr, possibly suggesting the presence of dust mixed with marine aerosols or lidar ratio values that depend on source and evolution of the aerosol plume. The new dusty marine type introduced in V4 features similar magnitudes and spatial distribution as its clean marine counterpart with lidar ratio differences of less than 3 sr, and nearly identical values over the open ocean, implying that some modification of the classification scheme for the marine subtypes is warranted.

Contribution of combustion Fe in marine aerosols over the northwestern Pacific estimated by Fe stable isotope ratios

The source apportionment of aerosol iron (Fe), including natural and combustion Fe, is an important issue because aerosol Fe can enhance oceanic primary production in the surface ocean. Based on our previous finding that combustion Fe emitted by evaporation processes has Fe isotope ratios (δ56Fe) that are approximately 4 ‰ lower than those of natural Fe, this study aimed to distinguish aerosol Fe sources over the northwestern Pacific using two size-fractionated marine aerosols. The δ56Fe values of fine and coarse particles from the eastern or northern Pacific were found to be similar to each other, ranging from 0.0 ‰ to 0.4 ‰. Most of them were close to the crustal average, suggesting the dominance of natural Fe. On the other hand, particles from the direction of East Asia demonstrated lower δ56Fe values in fine particles (−0.5 ‰ to −2.2 ‰) than in coarse particles (on average −0.02 ± 0.12 ‰). The correlations between the δ56Fe values and the enrichment factors of lead and vanadium suggested that the low δ56Fe values obtained were due to the presence of combustion Fe. The δ56Fe values of the soluble component of fine particles in this region were lower than the total, indicating the preferential dissolution of combustion Fe. In addition, we found a negative correlation between the δ56Fe value and the fractional Fe solubility in air masses from the direction of East Asia. These results suggest that the presence of combustion Fe is an important factor in controlling the fractional Fe solubility in air masses from the direction of East Asia, whereas other factors are more important in the other areas. By assuming typical δ56Fe values for combustion and natural Fe, the contribution of combustion Fe to the total (acid-digested) Fe in aerosols was estimated to reach up to 50 % of fine and 21 % of bulk (coarse + fine) particles in air masses from the direction of East Asia, whereas its contribution was small in the other areas. The contribution of combustion Fe to the soluble Fe component estimated for one sample was approximately twice as large as the total, indicating the importance of combustion Fe as a soluble Fe source despite lower emissions than the natural. These isotope-based estimates were compared with those estimated using an atmospheric chemical transport model (IMPACT), in which the fractions of combustion Fe in fine particles, especially in air masses from the direction of East Asia, were consistent with each other. In contrast, the model estimated a relatively large contribution from combustion Fe in coarse particles, probably because of the different characteristics of combustion Fe that are included in the model calculation and the isotope-based estimation. This highlights the importance of observational data on δ56Fe for size-fractionated aerosols to scale the combustion Fe emission by the model. The average deposition fluxes of soluble Fe to the surface ocean were 1.4 and 2.9 nmol m−2 d−1 from combustion and natural aerosols, respectively, in air masses from the direction of East Asia, which suggests that combustion Fe could be an important Fe source to the surface seawater among other Fe sources. Distinguishing Fe sources using the δ56Fe values of marine aerosols and seawater is anticipated to lead to a more quantitative understanding of the Fe cycle in the atmosphere and surface ocean.

Estimating cloud condensation nuclei concentrations from CALIPSO lidar measurements

We present a novel methodology to estimate cloud condensation nuclei (CCN) concentrations from spaceborne CALIPSO lidar measurements. The algorithm utilizes (i) the CALIPSO-derived backscatter and extinction coefficient, depolarization ratio, and aerosol subtype information, (ii) the normalized volume size distributions and refractive indices from the CALIPSO aerosol model, and (iii) the MOPSMAP optical modelling package. For each CALIPSO height bin, we first select the aerosol-type specific size distribution and then adjust it to reproduce the extinction coefficient derived from the CALIPSO retrieval. The scaled size distribution is integrated to estimate the aerosol number concentration which is then used in the CCN parameterizations to calculate CCN concentrations at different supersaturations. To account for the hygroscopicity of continental and marine aerosols, we use the kappa parameterization and correct the size distributions before the scaling step. We have studied the sensitivity of the thus derived CCN concentration to the effect of variations of the initial size distributions. It is found that the uncertainty associated with the algorithm can range between a factor of 2 and 3. We have also compared our results with the POLIPHON and found comparable results for extinction coefficients larger than 0.05 km−1. An initial application to a case with coincident airborne in-situ measurements for independent validation shows promising results and illustrates the potential of CALIPSO for constructing a global height-resolved CCN climatology.

Long-range transport of anthropogenic air pollutants into the marine air: Insight into fine particle transport and chloride depletion on sea salts

Long-range transport of anthropogenic air pollutants from East Asia can affect the downwind marine air quality during spring and winter. Long-range transport of continental air pollutants and their interaction with sea salt aerosols (SSA) significantly modify the radiative forcing of marine aerosols and influence ocean biogeochemical cycling. Previous studies poorly characterize variations of aerosol particles along with air mass transport from the continental edge to the remote ocean. Here, the research ship R/V Dongfanghong 2 traveled from the eastern China seas (ECS) to the northwestern Pacific Ocean (NWPO) to understand what and how air pollutants were transported from the highly polluted continental air to clean marine air in spring. A transmission electron microscope (TEM) was used to find the long-range transported anthropogenic particles and the possible Cl-depletion phenomenon of SSA in marine air. Primary and secondary anthropogenic aerosols were identified and dramatically declined from 87 % to 8 % by number from the ECS to remote NWPO. For the SSA aging, 86 % of SSA particles in the ECS were identified as fully aged, while the proportion of fully aged SSA particles in the NWPO decreased to 31 %. The result highlights that anthropogenic acidic gases in the troposphere (e.g., SO2, NOx, and volatile organic compounds) were transported longer distances compared to the anthropogenic aerosol and could exert a significant impact on marine aerosols in the NWPO. These results show that anthropogenic particles and gases from East Asia significantly perturb aerosol chemistry in marine air. The optical properties and cloud condensation nucleation of the modified SSA particles should be incorporated into the more accurately modeling of clouds in the ECS and NWPO in spring and winter.