Atmospheric dust aerosols over the Eastern Pamirs: major element concentrations and composition

This study measured the major element concentrations and compositions of atmospheric dust aerosol samples collected weekly for nearly 2 years at Mt. Muztagata, a remote and high-elevation site (38°17′N, 75°01′E, 4,430 m) in the Eastern Pamirs. Inductively coupled plasma mass spectroscopy (ICP–MS) results show that on the weekly timescale, air at Muztagata contained average element Al concentrations of 842 ng m⁻³ between June 2004 and December 2005, and 509 ng m⁻³ between June 2005 and April 2006. The dust load over the Eastern Pamirs appears to be far lower (by more than an order of magnitude) than those in northern China. The Muztagata dust aerosols show Ca/Al ratios (~0.7) and Fe/Al ratios (~0.7) that differ from that in northern China. The general homogeneity exists in the major element compositions, expect Ca/Al ratios which show minor but clear seasonal variations. Element ratios vary with aerosol concentration. Results indicate that concentrations and compositions of Asian dust change significantly between different emission regions, and confirm that major element ratios can be used to efficiently characterize the dust aerosols composition at different sites in northern China.     

Concentrations and composition of aerosols and particulate matter in surface waters along the transatlantic section

Along the transatlantic section from Ushuaia to Gdańsk (March 26–May 7, 2015; cruise 47 of R/V Akademik Ioffe), data were obtained on the concentrations of aerosols in the near-water layer of the atmosphere and of particulate matter in surface waters, as well as of organic compounds within the considered matter (C_org, chlorophyll a, lipids, and hydrocarbons). The concentrations of aerosols amounted to 1237–111 739 particles/L for the fraction of 0.3–1 μm and to 0.02–34.4 μg/m²/day for the matter collected by means of the network procedure. The distribution of aerosols is affected by circumcontinental zoning and by the fluxes from arid areas of African deserts. The maximum concentration of the treated compounds were found in the river–sea frontal area (the runoff of the Colorado River, Argentina), as well as when nearing the coasts, especially in the English Channel.     

Natural factors controlling the temporal variability of the major-element chemical composition of mineral aerosols over the Northern Caspian

This paper considers characteristic features of the composition and distribution of chemical elements in aerosols over the Northern Caspian, which can be used for a more reliable prediction of possible negative consequences of atmospheric pollution related to the beginning of the large-scale exploitation of oil and gas deposits in the shelf zone of the Caspian Sea. It was shown that the contents of aerosols, their grain-size composition, and major-element composition change under the influence of (1) transboundary transport of terrigenous dust by air masses, (2) variations in the intensity of turbulent and convective mixing in the near-surface atmosphere, and (3) variations in air humidity.     

太原市灰霾期间黑碳气溶胶形貌与成分分析

为掌握太原市冬季灰霾发生期间黑碳气溶胶形貌特征和化学成分变化特点,分别于2011-12-30T08:00至2012-01-01 T 04:00和2018-11-25 T 08:00至2018-11-27 T 04:00灰霾发生期间在山西大学环境与资源学院楼顶使用MAY七级冲击式颗粒采样器每隔4h采集空气动力学直径分别为0.25～0.5μm、0.5～1.0μm以及1～2μm的大气单颗粒分析样品,运用带超薄窗口能谱仪的扫描电镜(JEOL JSM-6390)测定了样品中4330个颗粒的二次电子像及X射线能谱,通过基于蒙特卡罗模拟程序的定量电子探针微区分析技术对每个颗粒的元素原子浓度进行了计算,并对颗粒进行了分类与计数。共检测到6类颗粒,分别是矿物尘、碳质颗粒、钠盐颗粒、二次颗粒、富铁颗粒和其他,其中黑碳气溶胶数量相对丰度在2011和2018年样品中平均为26.8%和34.2%。按照伸长率(E)、纵横比(R)、是否与其他物质结合等将其分为伸展型、支链型、嵌入或粘附型和团聚型4种,反映了黑碳颗粒不同的老化过程。2011年样品中团聚型和支链型数量较多,而2018年样品中伸展型和嵌入型多于团聚型和支...     

喜马拉雅珠峰地区冬季大气气溶胶化学组分及光学特征

为了研究喜马拉雅山北坡冬季大气气溶胶化学组分、光学特征及来源,2017年11—12月在珠穆朗玛峰站(QOMS)共采集22个PM2.5样品.结果显示:PM2.5中包括水溶性离子(WSIs)、有机质(OM)、元素碳(EC)在内的所有检测成分,总质量浓度为(3.36±1.06)μg·m-3;有机碳(OC)、元素碳(EC)和水...     

天然源二次有机气溶胶的研究进展

二次有机气溶胶由于其对环境、气候和人体健康的影响,正日益受到人们的关注.我国地域辽阔,森林占国土面积的12%,几乎具有北半球的全部植被类型,对天然源二次有机气溶胶的研究不容忽视.综合当前的研究成果,着重阐述了两种代表性生物挥发性有机化合物,异戊二烯和α.蒎烯与大气中主要的氧化剂,如03、OH和NO,等物种的反应,以及其二次气溶胶形成的过程.最后,对目前的研究手段和未来的研究方向进行了探讨.     

Organic stable carbon isotopic composition reveals late Quaternary vegetation changes in the dune fields of northern China

Vegetation changes during the late Quaternary in the dune fields of northern China are not well understood. We investigated organic carbon stable isotopic composition of surface soils, related mainly to the ratio of C₃ and C₄ plants, across a range of arid to subhumid climates in this region. Isotopic composition is weakly related to both temperature and moisture (multiple R² = 0.53), with the highest δ¹³C (greatest C₄ abundance) in the warm, subhumid Horqin dune field. In late Quaternary, eolian stratigraphic sections of the Mu Us and Horqin dune fields, but not in the much colder Otindag dune field, δ¹³C is higher in organic carbon from paleosols than in eolian sands. This contrast, most evident for paleosols recording a major early to middle Holocene phase of dune stabilization, is interpreted as evidence for expansion of C₄ plants due to increased effective moisture, high temperature because of high insolation, and decreased disturbance related to eolian erosion and deposition.     

Organic petrological composition of Triassic source rocks and their clastic depositional environments in some Australian sedimentary basins

Kerogen from terrestrial plant debris (type III) has commonly been considered to be a good source for hydrocarbon gas, but not for oil, compared with types I and II kerogen from marine and lacustrine sediments. The Gippsland Basin, Australia, contains giant oil fields producing from organic matter of land plant origin. Clearly some terrestrial paleodepositional environments have produced organic matter of land plant origin with the potential to generate large volumes of oil. An attempt has been made here to identify some environments that contain organic matter of terrestrial origin with the potential to generate oil.The dispersed organic matter (DOM) in sediments from various paleodepositional environments in the Northern Carnarvon, Clarence-Moreton, Simpson Desert, Bowen and Gunnedah Basins of Australia has been analysed petrographically. To reduce variations in organic matter type due to differences in geological age, examples of Triassic age only have been compared. DOM with relatively high contents of liptinite, which is widely accepted as having a better potential to generate oil than vitrinite and inertinite, was found in the following environments: fluvio-deltaic (Bowen Basin), proximal lacustrine (Gunnedah Basin) and fluvio-deltaic (Northern Carnarvon).Relationships between Triassic DOM types and paleodepositional environments found in one basin did not necessarily hold true for other basins. It is not valid to infer a unique paleodepositional environment from DOM type, but within a given basin, DOM type may be predicted from environment.     

Remote sensing of spectral signatures of tropospheric aerosols

With the launch of the German Aerospace Agency's (DLR) Modular Opto-electronic Scanner (MOS) sensor on board the Indian Remote Sensing satellite (IRS-P3) launched by the Indian Space Research Organization (ISRO) in March 1996, 13 channel multi-spectral data in the range of 408 to 1010 nm at high radiometric resolution, precision, and with narrow spectral bands have been available for a variety of land, atmospheric and oceanic studies. We found that these data are best for validation of radiative transfer model and the corresponding code developed by one of the authors at Space Applications Centre, and called ATMRAD (abbreviated for ATMospheric RADiation). Once this model/code is validated, it can be used for retrieving information on tropospheric aerosols over ocean or land. This paper deals with two clear objectives, viz.,

Physical properties of aerosols at Maitri,Antarctica

Measurements of the submicron aerosol size distribution made at the Indian Antarctic station, Maitri (70‡45′S, 11‡44′E) from January 10th to February 24th, 1997, are reported. Total aerosol concentrations normally range from 800 to 1200 particles cm⁻³ which are typical values for the coastal stations at Antarctica in summer. Aerosol size distributions are generally trimodal and open-ended with a peak between 75 and 133 nm and two minima at 42 and 420 nm. Size distributions remain almost similar for several hours or even days in absence of any meteorological disturbance. Total aerosol concentration increases by approximately an order of magnitude whenever a low pressure system passes over the station. Based on the evolution of aerosol size-distributions during such aerosol enhancement periods, three types of cases have been identified. The nucleation mode in all three cases has been suggested to result from the photochemical conversion of the DMS emissions transported either by the marine air or by the air from the ice-melt regions around Maitri. Subsidence of midtropospheric air during the weakening of radiative inversion is suggested as a possible source of the nucleation mode particles in the third case. Growth of the nucleation mode particles by condensation, coagulation and/or by cloud processes has been suggested to be responsible for other modes in size distributions.     

Heavy metal concentrations and Pb isotopic composition in urban and suburban aerosols of Hong Kong and Guangzhou, South China-Evidence of the long-range transport of air contaminants

Rapid urbanization and industrialization in South China has placed a great strain on the environment and human health. In the present study, the total suspended particulate matter （TSP） in the urban and suburban areas of Hong Kong and Guangzhou, the two largest urban centres in South China, was sampled from December 2003 to January 2005. The samples were analyzed for their concentrations of major elements （Al, Fe, Mg and Mn） and trace metals （Cd, Cr, Cu, Pb, V and Zn）, and for Pb isotopic composition. Elevated concentrations of metals, especially Cd, Pb, V and Zn, were observed in the urban and suburban areas of Guangzhou, showing significant atmospheric trace element pollution. Distinct seasonal patterns were observed in the heavy metal concentrations of aerosols in Hong Kong, with higher metal concentrations during the winter monsoon period, and lower concentrations during summer time. The seasonal variations in metal concentrations of the aerosols of Guangzhou were less distinct, suggesting the dominance of local sources of pollution around the city. The Pb isotopic composition in the aerosols of Hong Kong had higher ^206Pb/^207Pb and ^208Pb/^207Pb ratios in winter, showing the influence of Pb from the northern inland areas of China and the Pearl River Delta （PRD） region, and lower ^206Pb/^207Pb and ^208Pb/^207Pb ratios in summer, indicating the influence of Pb from the South Asian region and from marine sources.     

Magma mixing in the subvolcanic environment: petrology of the Gerena interaction zone near Seville,Spain

The mechanisms by which felsic and mafic magmas interact and approach a uniform hybrid composition through the processes of mingling and mixing have been studied in a high-level subvolcanic setting in the Spanish Hercynian at Gerena, near Seville. The compositions involved are calc-alkaline and the situation is one of tonalite-quartz diorite synplutonic dykes injected into a granitic magma chamber. The resulting hybrids include dykes, pillows and globules of tonalite with chilled margins which are variously disrupted and homogenised with the host granite. The present investigation is based on field and petrographic observations of hybridization textures, the identification of different stages in the crystallisation history of the tonalite through mineral textures, and the characterization of mineral compositions at these various stages. Proportions of the end-member magmas involved were obtained by major-oxide mixing models and tested satisfactorily with trace elements. A mechanistic model is presented to account for these observations which involves the early quenching of the tonalite when it was emplaced into the granite magma chamber. After high temperature crystallization had occurred the two magmas attained thermal equilibrium and disruption of the tonalite in the high energy regime of this subvolcanic complex resulted in dispersion of fragments and crystals through the granite giving rise to hybrid granodiorite compositions. It is argued that such high-energy flow conditions are a necessary requirement for effective hybridization in this environment in contrast to most large-scale magma chamber settings where mixing is driven by thermal and buoyancy contrasts.     

Chemistry of Aerosols over Chukchi Sea and Bering Sea

The contents of elements in aerosols sampled during the First Chinese Arctic Research Expedition (CHINARE-1) show great differences from one element to another. Na, K,Ca, Mg, A1, F, and Cl are the major components in the aerosols, whose contents are larger than 30 ng/m^3. The chemical elements whose contents vary between 0.1 - 30 ng/m^3 are Br,Sr, Cr, Ni, and Zn. The chemical elements whose contents are close to or slightly higher than 0.1 ng/m^3 are Rb, Ba, Zr, Th, and Pb. The contents of As, Sb, W, Mo, Au, La, Ce, Nd,Sin, Eu, Tb, Yb, Lu, Sc, Co, Hf, Ta, and Cd are less than 0.1 ng/m^3. The mass concentration data for the same element, as observed during CHINARE-1, are almost accordant, but much lower than what is observed in the China‘ s seas or the coasts of China. The enrichment factor and electron microscopic analyses and lead isotope tracing were used to distinguish their sources.Four groups of sources can be classified as follows: anthropogenic: As, Sb, W, F, Mo, Au,Cu, Pb, Cd, V; crustal: La, Ce, Nd, Sm, Eu, Tb, Yb, Lu, Fe, Sc, Cr, Co, Ba, Zr, Hf,Ta, Cs, Mn, Th, U; oceanic:Na, K, Ca, and Mg; and mixing: Rb, Sr, Ca, and Mg.     

Turbulent transport of atmospheric aerosols and formation of large-scale structures

Turbulent transport of aerosols and droplets in a random velocity field with a finite correlation time is studied. We derived a mean-field equation and an equation for the second moment for a number density of aerosols. The finite correlation time of random velocity field results in the appearance of the high-order spatial derivatives in these equations. The finite correlation time and compressibility of the velocity field can cause a depletion of turbulent diffusion and a modification of an effective mean drift velocity. The coefficient of turbulent diffusion in the vertical direction can be depleted by 25 % due to the finite correlation time of a turbulent velocity field. The latter result is in compliance with the known anisotropy of the coefficient of turbulent diffusion in the atmosphere. The effective mean drift velocity is caused by a compressibility of particles velocity field and results in formation of large-scale inhomogeneities in spatial distribution of aerosols in the vicinity of the atmospheric temperature inversion. Results obtained by Saffman (1960) for the effect of molecular diffusivity in turbulent diffusion are generalized for the case of compressible and anisotropic random velocity field. A mechanism of formation of small-scale inhomogeneities in particles spatial distribution is also discussed. This mechanism is associated with an excitation of a small-scale instability of the second moment of number density of particles. The obtained results are important in the analysis of various atmospheric phenomena, e.g., atmospheric aerosols, droplets and smog formation.     

Seasonal changes in stable carbon isotopic composition of n-alkanes in the marine aerosols from the western North Pacific: Implications for the source and atmospheric transport

To constrain seasonal changes in the long-range atmospheric transport of land-derived lipid biomarker compounds, we investigated the compound-specific stable isotopic composition of marine aerosol n-alkanes collected from 1990 to 1993 at a remote island, Chichi-Jima (27°04′N, 142°13′E), in the western North Pacific. Compound-specific isotope analysis revealed, in particular, strong seasonal changes in the δ¹³C values of the C₂₉ and C₃₁n-alkanes (biomarkers for higher plants). Lighter δ¹³C values were observed in winter (typically −32 to −34‰), with a transition to heavier values in summer (typically −28 to −31‰). Using a mixing equation and typical end members for C₃ and C₄ plants, we found that this is due to relative increases in the contributions from C₄ plants in the summer season. Using backward air-mass trajectory analyses, it was shown that the Asian continent was the major source region for C₃ plant material during winter/spring, whereas Indonesia/Australia and possibly the Americas were the major source regions for C₄ material during the summer/autumn. Also observed was an enhanced atmospheric transport of n-alkanes from C₄ plants in 1991 summer/autumn during a strong El Nino event, which was associated with forest and bushfires in Indonesia and Australia. In addition to providing information on contemporary processes, this study also provides a base for future paleoclimatological work in ocean sediments.     

Radiocarbon measurements of black carbon in aerosols and ocean sediments

Black carbon (BC) is the combustion-altered, solid residue remaining after biomass burning and fossil fuel combustion. Radiocarbon measurements of BC provide information on the residence time of BC in organic carbon pools like soils and sediments, and also provide information on the source of BC by distinguishing between fossil fuel and biomass combustion byproducts. We have optimized dichromate-sulfuric acid oxidation for the measurement of radiocarbon in BC. We also present comparisons of BC ¹⁴C measurements on NIST aerosol SRM 1649a with previously published bulk aromatic ¹⁴C measurements and individual polycyclic aromatic hydrocarbon (PAH) ¹⁴C measurements on the same NIST standard.Dichromate-sulfuric acid oxidation belongs to the chemical class of BC measurement methods, which rely on the resistance of some forms of BC to strong chemical oxidants. Dilute solutions of dichromate-sulfuric acid degrade BC and marine-derived carbon at characteristic rates from which a simple kinetic formula can be used to calculate concentrations of individual components (Wolbach and Anders, 1989). We show that: (1) dichromate-sulfuric acid oxidation allows precise, reproducible ¹⁴C BC measurements; (2) kinetics calculations give more precise BC yield information when performed on a % OC basis (vs. a % mass basis); (3) kinetically calculated BC concentrations are similar regardless of whether the oxidation is performed at 23°C or 50°C; and (4) this method yields ¹⁴C BC results consistent with previously published aromatic ¹⁴C data for an NIST standard.For the purposes of intercomparison, we report % mass and carbon results for two commercially available BC standards. We also report comparative data from a new thermal method applied to SRM 1649a, showing that thermal oxidation of this material also follows the simple kinetic sum of exponentials model, although with different time constants.     

Detection of marine aerosols with IRS P4-Ocean Colour Monitor

The atmospheric correction bands 7 and 8 (765nm and 865nm respectively) of the Indian Remote Sensing Satellite IRS P4-0CM (Ocean Colour Monitor) can be used for deriving aerosol optical depth (AOD) over the oceans. A retrieval algorithm has been developed which computes the AOD using band 7 data by treating the ocean surface as a dark background after removing the Rayleigh path radiance in the sensor-detected radiances. This algorithm has been used to detect marine aerosol distributions at different coastal and offshore locations around India. A comparison between OCM derived AOD and the NOAA operational AOD shows a correlation ∼0.92 while that between OCM derived AOD and the ground-based sun photometer measurements near the coast of Trivandrum shows a correlation of ∼0.90.     

Characterization of ambient aerosols in Northern Thailand and their probable sources

The present study examines variation of ambient aerosol mass and number concentrations in Chiang Mai, Thailand during winter. Aerosol particle samples were collected and measured at four different sites, representative of urban, industrial, residential and rural areas during daytime between December 2003 and January 2004. Average 10 h particulate matter (PM) mass concentrations were found to be in the range of 75–290 ì g/m³, with average value of 149 ± 45 ì g/m³. Urban and industrial areas appeared to have higher PM loading than residential and rural areas. Number concentration and size distribution of particles in the range of 0.3–10.0 ìm did not exhibit any marked variation between sites. Relatively stable number concentrations were reported. Temporal variation of number concentrations was not clearly significant. No short term peak observed during rush hours. During sampling period, the average number concentration for 0.3–0.5, 0.5–1.0, 1.0–5.0 and 5.0–10.0 ìm were 6.60 × 10⁶, 1.18 × 10⁶, 2.11 × 10⁵ and 1.12 × 10⁴/m³, respectively. Particles with diameter smaller than 1.0 ìm accounted for over 90 % of the total number concentration. Concentrations of major metals were determined by atomic absorption spectrophotometer (Pb, Fe, Al, Si, Cr, Cd, Ni, Zn) and flame photometer (K, Na and Ca). Data obtained were used to identify probable sources via a multivariate analysis. Si, Na, Fe, Ca, Al and K were the six dominant elements in the airborne PM. Principle component analysis was carried out and major sources of airborne PM in Chiang Mai were determined, namely, (1) long distance sources such as sea spray, earth soil and industrial combustion, (2) short-distance sources such as crustal re-suspension, vehicular related emissions and vegetation burning, and (3) the unknown distance sources with low influence of traffic emissions.     

Rare sulfur and triple oxygen isotope geochemistry of volcanogenic sulfate aerosols

We present analyses of stable isotopic ratios ¹⁷O/¹⁶O, ¹⁸O/¹⁶O, ³⁴S/³²S, and ³³S/³²S, ³⁶S/³²S in sulfate leached from volcanic ash of a series of well known, large and small volcanic eruptions. We consider eruptions of Mt. St. Helens (Washington, 1980, ∼1 km³), Mt. Spurr (Alaska, 1953, <1 km³), Gjalp (Iceland, 1996, 1998, <1 km³), Pinatubo (Phillipines, 1991, 10 km³), Bishop tuff (Long Valley, California, 0.76 Ma, 750 km³), Lower Bandelier tuff (Toledo Caldera, New Mexico, 1.61 Ma, 600 km³), and Lava Creek and Huckleberry Ridge tuffs (Yellowstone, Wyoming, 0.64 Ma, 1000 km³ and 2.04 Ma 2500 km³, respectively). This list covers much of the diversity of sizes and the character of silicic volcanic eruptions. Particular emphasis is paid to the Lava Creek tuff for which we present wide geographic sample coverage.This global dataset spans a significant range in δ³⁴S, δ¹⁸O, and Δ¹⁷O of sulfate (29‰, 30‰, and 3.3‰, respectively) with oxygen isotopes recording mass-independent (Δ¹⁷O > 0.2‰) and sulfur isotopes exhibiting mass-dependent behavior. Products of large eruptions account for most of‘ these isotopic ranges. Sulfate with Δ¹⁷O > 0.2‰ is present as 1-10 μm gypsum crystals on distal ash particles and records the isotopic signature of stratospheric photochemical reactions. Sediments that embed ash layers do not contain sulfate or contain little sulfate with Δ¹⁷O near 0‰, suggesting that the observed sulfate in ash is of volcanic origin.Mass-dependent fractionation of sulfur isotopic ratios suggests that sulfate-forming reactions did not involve photolysis of SO₂, like that inferred for pre-2.3 Ga sulfates from Archean sediments or Antarctic ice-core sulfate associated with few dated eruptions. Even though the sulfate sulfur isotopic compositions reflect mass-dependent processes, the products of caldera-forming eruptions display a large δ³⁴S range and exhibit fractionation relationships that do not follow the expected equilibrium slopes of 0.515 and 1.90 for ³³S/³²S vs. ³⁴S/³²S and ³⁶S/³²S vs. ³⁴S/³²S, respectively. The data presented here are consistent with modification of a chemical mass-dependent fractionation of sulfur isotopes in the volcanic plume by either a kinetic gas phase reaction of volcanic SO₂ with OH and/or a Rayleigh processes involving a residual Rayleigh reactant—volcanic SO₂ gas, rather than a Rayleigh product. These results may also imply at least two removal pathways for SO₂ in volcanic plumes.Above-zero Δ¹⁷O values and their positive correlation with δ¹⁸O in sulfate can be explained by oxidation by high-δ¹⁸O and high-Δ¹⁷O compounds such as ozone and radicals such as OH that result from ozone break down. Large caldera-forming eruptions have the highest Δ¹⁷O values, and the largest range of δ¹⁸O, which can be explained by stratospheric reaction with ozone-derived OH radicals. These results suggest that massive eruptions are capable of causing a temporary depletion of the ozone layer. Such depletion may be many times that of the measured 3-8% depletion following 1991 Pinatubo eruption, if the amount of sulfur dioxide released scales with the amount of ozone depletion.