Seasonal and areal variation of continental aerosol in the surface air over the western North Pacific region

Weekly aerosol samples were collected for two years from 1981 at six stations in the western North Pacific region. The samples were analyzed for aluminum to determine the mineral dust concentration in the air. By combining our data with observations in the central and eastern North Pacific by a US research group, the following results and conclusions have been obtained. Spring peaks in atmospheric mineral dust were observed at all the stations accompanied byKosa episodes (hazes due to mineral dust of Chinese origin). The spring peaks, however, varied from year to year. The mean concentration of mineral dust depends not only on the distance from the Asian coast but also on the latitude of the sampling station. The half-decrease distance of the atmospheric mineral dust turned out to be 500–600 km for all latitudes in the western North Pacific. This indicates that the rate of deposition of mineral dust in the western North Pacific is much larger than that in the central and eastern North Pacific.     

Study of continental material transported through the atmosphere to the oeean

I am deeply honored to have been selected as a recipient of the 1987 Okada Prize by the Oceanographical Society of Japan. The present paper reviews my work and recent studies of other investigators concerning mineral aerosol (dust) particles in the marine atmosphere over the Pacific Ocean. I would like to emphasize the importance of atmospheric deposition of continental substances to the ocean environment. From consecutive measurements of atmospheric dust concentrations and total deposition fluxes at 13 island stations in the Pacific Ocean, a strong seasonal transfort pattern of dust particles was found at most of the stations. High atmospheric dust concentrations occurred during the spring in both hemispheres. There was a latitudinal gradient in both the atmospheric dust concentration and flux, with the highest values observed at midlatitudes. When combined with observations of dust storms in Asia and isentropic trajectory analysis, it was clear that the dust over the central North Pacific was transported by the upper westerly winds from the arid desert regions in central and eastern Asia. Transport times were 1–2 weeks, and in some cases, atmospheric transport paths of over 10,000 km were observed. Infrequent short-term dust events contributed most of annual atmospheric dust flux to the open ocean. These sporadic inputs are major sources for both suspended mineral matter in the water column and the non-biogenic component of deep-sea sediments in the Pacific Ocean. The impact of atmospheric dust fluxes on chemical and biological processes in the water column remains to be determined.     

Distributions of low molecular weight dicarboxylic acids in the North Pacific aerosol samples

Marine aerosol samples collected from the North Pacific atmosphere were studied for molecular distributions of dicarboxylic acids by using a capillary gas chromatography and mass spectrometery. A homologous series of dicarboxylic acids (C₂–C₁₀) was detected in the marine aerosol samples as dibutyl esters. All the samples showed that the smallest diacid (oxalic acid: C₂) was the most abundant and comprised 41–67% of the total diacids. The second most abundant species was malonic acid (C₃) or succinic acid (C₄). The diacids with more carbon numbers were generally less abundant. Total diacid concentration range was 17–1040 ng m^–3, which accounted for up to 1.6% of total aerosol mass. This indicates that low molecular weight dicarboxylic acids are important class of organic compounds in the marine atmosphere. The concentrations were generally higher in the western North Pacific and lower in the central North Pacific. The major portion of diacids is probably derived from the Asian Continent and East Asian countries by long-range atmospheric transport and partly fromin situ photochemical production in the marine atmosphere.     

Open-ocean deployment of a buoy-mounted aerosol sampler on the Bermuda Testbed Mooring: Aerosol iron and sea salt over the Sargasso Sea

We report results from the first deployment of a buoy-mounted aerosol sampler on the Bermuda Testbed Mooring (BTM) in the Sargasso Sea, in which a time-series of 21 aerosol samples were collected over the period May 5–September 29, 2004. These aerosol samples were analyzed for iron and soluble sodium (as a proxy for sea salt). Also analyzed was a time-series of 22 aerosol samples collected over the same period at the Tudor Hill atmospheric sampling tower on Bermuda. The buoy sampler worked as intended and successfully collected a time-series of aerosol samples, thus demonstrating that moored buoys can be used as oceanic observatories to provide information on the temporal (weekly, monthly and seasonal) variability in the concentration of aerosol iron (and other trace elements) over the surface ocean. The magnitude and time variation of aerosol Fe concentrations calculated from the BTM buoy samples are in close agreement with the corresponding aerosol Fe record from the Tudor Hill tower, which is located approximately 80 km northwest of the mooring site. Both the BTM and Tudor Hill samples record periods of high aerosol iron loadings in late June and late July 2004, reflecting the transport of soil dust from North Africa, with the highest concentration of aerosol iron at the BTM site (0.83 μg m⁻³) measured in late June. Concentrations of sea-salt aerosol calculated from the BTM samples are comparable to values measured over the Sargasso Sea and for samples collected at the Tudor Hill tower. Sea-salt aerosols do not appear to impede the collection of mineral aerosols by the buoy-mounted sampler.     

晚新生代风尘沉积的稀土元素地球化学特征及其古气候意义

通过西峰巴家咀剖面晚新生代风尘沉积中的红粘土、黄土、古土壤的稀土元素、分布模式、特征参数的研究，并与晚第三纪红色沙漠风成砂、晚第三纪河流相细砂岩、第四纪沙漠风成砂、现代尘暴粉尘、中国黄土以及青藏高原远源西风粉尘进行对比分析，结果表明，晚新生代风尘沉积物均具有轻稀土适度富集、缓右倾斜型、Eu负异常的REE分布模式；晚第三纪红色沙漠是红粘土的主要物源之一；红粘土和典型的风尘物质－现代尘暴粉尘及中国黄土有相似的沙漠物质来源和形成过程，与基岩明显不同，这为红粘土的“风成说”而非“残积说”提供了新的证据。巴家咀红粘土的堆积过程与第四纪黄土相似，东亚季风环流而非西风环流控制着沙漠区粉尘物质的输送。     

Spatial variations of rare earth elements in north pacific surface water

The concentration of dissolved rare earth elements (REE) were determined at 47 stations in the North Pacific surface waters. Combining with other previous data, we present the surface REE distribution in the North Pacific and discuss the controlling factors. The surface concentrations increase toward the high latitude and continental margin (e.g. [Nd] > 10 pmol kg⁻¹) from the central North Pacific (e.g. [Nd] < 5 pmol kg⁻¹). The North Pacific Deep Water-normalized REE patterns are varied, indicating that two or more factors contribute to the REE distribution. We examined four factors making the regional variation of surface REE concentrations mainly; a) particle scavenging, b) atmospheric dust input, c) vertical mixing and d) lateral transport from the coastal region. Flux calculations for Nd showed that the influence of atmospheric dust was less significant than the vertical input even in the western upwelling zone. Moreover, the longitudinal and latitudinal transitions of surface REE seem to reflect the lateral supply from the coastal areas. We constructed the diagram of surface Er/Lu and Er/Yb molar ratios in order to assess the origin and the input processes of the surface REE. Both molar ratios showed increasing trend toward PEW (Er/Lu (>10.5) and Er/Yb (>1.4)) from PSUW (Er/Lu (>7) and Er/Yb (>1.2)). The high Er/Lu and Er/Yb ratios in PEW indicate that the lateral supply of terrestrial materials from the coastal area is possibly the important factor in PEW, because only weathering and dissolution of rocks can explain such high Er/Lu and Er/Yb ratios to our knowledge.     

The Western North Pacific Playing a Key Role in Global Biogeochemical Fluxes

The oceanic biogeochemical fluxes in the North Pacific, especially its northwestern part, are discussed to prove their importance on a global scale. First, the air-sea exchange processes of chemical substances are considered quantitatively. The topics discussed are sea salt particles transported to land, sporadic transport of soil dust to the ocean and its role in the marine ecosystem, the larger gas transfer velocity of CO₂ indicating the effect of bubbles, and DMS and greenhouse gases other than CO₂. Next, chemical tracers are utilized to reveal the water circulation systems in the region, which are the Pacific Deep Water including its vertical eddy diffusivity, the North Pacific Intermediate Water and the Japan Sea Deep Water. Thirdly, the particulate transport process of chemical substances through the water column is clarified by analyzing the distribution of insoluble radionuclides and the results obtained from sediment trap experiments. Fourthly, the northern North Pacific is characterized by stating the site decomposing organic matter and Si playing a key role in the marine ecosystem. Both are induced by the upwelled Pacific Deep Water. Fifthly, the oceanic CO₂ system related to global warming is presented by clarifying the distribution of anthropogenic CO₂ in the western North Pacific, and roles of the upwelled Pacific Deep Water and the continental shelf zone in the absorption of atmospheric CO₂. Finally, Mn and other chemical substances in sediments are discussed as recorders of the early diagenesis and indicators of low biological productivity during glacial ages in the northwestern North Pacific. It is concluded that the western North Pacific is characterized mainly by the Pacific Deep Water bringing nutrients to the northern North Pacific, located at the exit of the global deep water circulation and, therefore, the region plays a key role in the global biogeochemical fluxes. This revised version was published online in August 2006 with corrections to the Cover Date.     

Eolian dust from the lower atmosphere of the eastern Atlantic and Indian Oceans,China Sea and Sea of Japan

Dust-loadings in the lower atmosphere of the Atlantic and Indian Oceans and the China Sea and Sea of Japan are given. Average dust-loadings decrease in the following order: North Atlantic (northeast trades, ～ 7.7 μg/m³ of air) > northern Indian Ocean (～ 1.2 μg/m³ of air) > South Atlantic (southeast trades, ～ 0.78 μg/m³ of air) = southern Indian Ocean (～ 0.68 μg/m³ of air) > China Sea (～ 0.21 μg/m³ of air).There are differences in the clay mineralogies of dusts transported in similar latitudes in the North Atlantic and northern Indian Oceans. Dusts in the Atlantic northeast trades are dominated by kaolinite from the soils of equatorial Africa; dusts in the northeast monsoons of the northern Indian Ocean have a source in the arid regions of the Rajasthan desert where illite is the principal clay mineral.In the regions investigated quartz occurs in larger amounts in the dusts of the Northern Hemisphere (～ 7% quartz) than those of the Southern Hemisphere (～ 3% quartz) over both the Atlantic and Indian Oceans.From the results given in the present paper and those reported in the literature a map is presented illustrating the order of magnitude of lower atmospheric dust-loadings in part of the world ocean.     

Mercury concentration in the ocean

Seventy percent of 342 seawater samples collected in the Bering Sea, North and South Pacific, Japan Sea, East and South China Seas, and Indian Ocean had concentrations of “total” mercury ranging from 3 to 6 ng Hg l^?1 with an arithmetic mean of 5.3 ng l^?1 and a geometric mean of 5.0 ng l^?1. In some cases, a higher concentration was observed at the surface, at the halocline or thermocline, or in the bottom water. But in general, there was no consistent correlation between mercury concentration and depth, except for a statistical tendency for mercury concentration to be slightly higher in the surface water. This tendency suggests that mercury in the ocean is supplied from the atmosphere by rain washout. The latitudinal variation of surface mercury concentrations showed that the maximum concentration at each latitude decreased from 40°N to 30°S. This variation provides evidence that atmospheric mercury is emitted mainly from continental areas naturally or anthropogenically.     

The Increase of Biogenic Sulfate Aerosol and Particle Number in Marine Atmosphere over the Northwestern North Pacific

During a cruise aboard the R/V Hakuho-maru in the northwestern North Pacific in the summer of 1998 the particle number concentrations and the major ionic components of size fractionated aerosols were measured to investigate the aerosol produced by marine biological activity. Continuous low concentrations of nitrate (<1.8 nmol m⁻³), similar to the marine air background level, were found over the northwestern North Pacific (40–45°N) and the Sea of Okhotsk (44–45°N). Over the Sea of Okhotsk, a high concentration of chlorophyll-a (5.4 mg m⁻³) in seawater was observed, and atmospheric concentrations of non sea-salt (nss-) sulfate (44 nmol m⁻³), methane sulfonic acid (MSA) (1.8 nmol m⁻³) and particle number in the size range of 0.1 < D < 0.5 μm (199 cm⁻³) were found to be 9, 7, and 2 times, respectively, higher than those in the background marine air. The increase in particle number concentrations mainly in the size range of 0.2 < D < 0.3 μm was likely caused by the increase of biogenic sulfate over the high productive region of the Sea of Okhotsk. In humid air conditions (R.H. > 96%), the increased biogenic sulfate that condensed the large amount of water vapor would not have sufficient solute mass to activate as cloud condensation nuclei (CNN) and would remain as aerosol particles in the marine air with frequent sea-fogs over the high productive region. Biogenic sulfate originating from dimethyl sulfide (DMS) would gradually grow into the CCN size and continuously supply a great number of CCN to the marine air in the northwestern North Pacific. This revised version was published online in July 2006 with corrections to the Cover Date.     

Aluminum in the East China Sea and Okinawa Trough, marginal sea areas of the Western North Pacific

The distribution of aluminum (Al) in seawater has been investigated in the continental slope and the Okinawa Trough areas of the East China Sea, which is one of the marginal seas in the western North Pacific Ocean. Aluminum concentration in waters over the slope and the Trough ranged from 5.6 to 25 nmol/kg in the surface layer (0–100 m), and had a minima of 1.1 nmol/kg between 400 and 500 m depth and ranged from 1.3 to 9.7 nmol/kg in the deep or bottom waters. Aluminum values were higher than in the surface waters of the central North Pacific, while minimum values were similar to levels in the intermediate or deep waters of the central North Pacific, except for the bottom water over the slope. This suggests that the high Al concentration in the surface reflects the large atmospheric input of Asian dust around the western side of the North Pacific region. On the continental slope, Al concentrations in the upper 500 m depth decreased slopeward. This horizontal gradient of Al can be explained from the combination of dilution by upwelling of Al-poor water originated from the North Pacific Intermediate Water (NPIW) which intrudes into the mid-depth of the Okinawa Trough and the scavenging of Al by biogenic particles in the continental slope zone.     

北太平洋大气沉降的时空特征及其对副极区海洋生态系统的影响

北太平洋副极地海区作为全球海洋三个高营养盐低叶绿素(high nutrient and low chlorophyll, HNLC)海区之一, 其浮游植物生长受到微量元素铁的限制。对于开阔大洋, 大气沉降是海洋表层铁的一个重要来源, 铁元素沉降进入海洋后能够促进浮游植物生长, 进而引起海洋初级生产力和生物泵的响应。本文利用SPRINTARS(Spectral Radiation-Transport Model for Aerosol Species)模式的时长为20a的日均大气沉降数据, 对北太平洋海区大气沉降的时空特征进行了分析。结果表明, 进入北太平洋海区的大气沉降量为26.81Tg·a^-1, 并且存在显著的季节变化: 春季最高, 冬季最低, 5月份进入海洋的沉降量达到峰值。大气沉降主要来源于陆地区域, 在风场的驱动下向海洋传输, 因此大气沉降量的空间分布呈现出西高东低的特征。本文以2010年8月中旬卫星观测到的一次强沙尘(即高大气沉降量)事件为例, 研究了大气沙尘的传播路径。进一步结合2001年4月9—12日及2008年4月20—22日的沙尘事件, 分析了西北太平洋K2站位(47°N, 160°E)附近海域海洋初级生产力对大气沉降——沙尘事件的响应。结果表明, 三次沙尘事件后, K2站位的颗粒有机碳通量、叶绿素浓度均有明显增加, 即沙尘事件对北太平洋副极区海洋初级生产力存在促进作用。     

基于遥感数据对比南海和阿拉伯海夏季叶绿素a浓度

The South China Sea(SCS) and the Arabian Sea(AS) are both located roughly in the north tropical zone with a range of similar latitude(0°–24°N). Monsoon winds play similar roles in the upper oceanic circulations of the both seas. But the distinct patterns of chlorophyll a(Chl a) concentration are observed between the SCS and the AS.The Chl a concentration in the SCS is generally lower than that in the AS in summer(June–August); the summer Chl a concentration in the AS shows stronger interannual variation, compared with that in the SCS; Moderate resolution imaging spectroradiometer(MODIS)-derived data present higher atmospheric aerosol deposition and stronger wind speed in the AS. And it has also been found that good correlations exist between the index of the dust precipitation indicated by aerosol optical thickness(AOT) and the Chl a concentration, or between wind and Chl a concentration. These imply that the wind and the dust precipitation bring more nutrients into the AS from the sky, the sub-layer or coast regions, inducing higher Chl a concentration. The results indicate that the wind velocity and the dust precipitation can play important roles in the Chl a concentration for the AS and the SCS in summer. However aerosol impact is weak on the biological productivity in the west SCS and wind-induced upwelling is the main source.     

Total amount of oceanic excess CO2 taken from the North Pacific subpolar region

Concentrations of total carbonate, alkalinity and dissolved oxygen were obtained near the 1973 GEOSECS stations in the North Pacific subpolar region north of 40°N along 175°E between 1993 and 1994. A difference of excess CO₂ content between the GEOSECS and our expeditions was estimated. The maximum difference in water column inventory of excess CO₂ has increased by about 280 gC m^–2 above 2000 m depth which apparently means an uptake of excess CO₂ taken from air to sea during the last two decades. An averaged value of the annual flux of excess CO₂ at 75–1000 m depth was 8.63±2.01 gC m^–2yr^–1 in the North Pacific subpolar region. By introducing the annual flux of excess CO₂ into a two-box model for the North Pacific subpolar region, a penetration factor of excess CO₂ from air to sea was obtained to be 1.08×10^–2 gC m^–3ppm^–1 in the North Pacific subpolar region. Based on this factor, the surface concentration of excess CO₂ in the North Pacific subpolar region was estimated to be 68 mole I^–1, suggesting that the North Pacific subpolar region absorbed atmospheric excess CO₂ more than the saturated concentration of excess CO₂. Total amount of excess CO₂ taken from the North Pacific subpolar region by 1993 was estimated to be 36.2×10¹⁵ gC, which was equal to about one tenth of that released by human activities after the preindustrial era.     

福岛核事故泄漏入海的137Cs长期输运的数值研究

The Fukushima nuclear accident in 2011 released large amounts of radionuclides, including ~(137)Cs, into the Pacific Ocean. A quasi-global ocean radioactive transport model with horizontal grid spacing of 0.5°×0.5° and 21 vertical layers was thereafter established to study the long-term transport of the Fukushima-derived ~(137)Cs in the ocean.The simulation shows that the plume of ~(137)Cs would be rapidly transported eastward alongside the Kuroshio Current and its extensions. Contaminated waters with concentrations lower than 2 Bq/m3 would reach the west coast of North America 4 or 5 years after the accident. The ~(137)Cs tends to be carried, despite its very low concentration, into the Indian and South Pacific Oceans by 2016 via various branches of ocean currents.Meanwhile, the ~(137)Cs concentrations in the western part of the North Pacific Ocean decrease rapidly with time. Up to now the highly contaminated waters have remained in the upper 400 m, showing no evidence of significant penetration to deeper layers.     

Non-sea-salt sulfate in the marine boundary layer and its possible impact on chloride depletion

1Introduction Sulfurisoneofthemostimportantelements whosebiogeochemicalcyclesarepivotaltotheatmo- sphericenvironmentandtotheclimaticchanges.The predominant,stablechemicalspeciesofsulfurinthe atmosphereissulfuricacidorsulfatewhichunderor- dinaryconditionsexistsmainlyinsmallaerosolparti- cles(Chinetal.,1996;Kerminenetal.,2000;Restadet al.,1998).Sulfuricacidorsulfate-dominatedaerosols areubiquitousintheloweratmosphere.Inthemarine boundarylayer(MBL),non-sea-saltsulfuricacidorsulfate(nss-SO42-)…     

239, 240Pu,137Cs and90Sr in the central North Pacific

^{239, 240}Pu,¹³⁷Cs and⁹⁰Sr concentrations were determined in sea waters from the central and western North Pacific in 1980 and 1982. The results are consistent with those reported earlier for North Pacific waters. The profiles of⁹⁰Sr and¹³⁷Cs show a monotonic decrease with depth, whilst^{239, 240}Pu shows a distinct subsurface maximum at a depth between 400 and 1,000 m. The calculated inventories of these nuclides significantly exceed the global mean fallout inputs for these latitudes. This may be due to local fallout input to the ocean at times of large-scale nuclear weapon tests in the equatorial North Pacific. The existence of measurable amounts of¹³⁷Cs and^{239, 240}Pu in deep waters suggests that these nuclides are transported by sinking particulate matter from the surface to the deep ocean.     

南海铁锰结核(壳)的稀土元素地球化学

于1987年5—6月间,中、西德在南海进行地球科学调查,获得5个铁锰结壳、6个铁锰结核样品。本文在利用X荧光法测定15个稀土元素的基础上,对南海铁锰结核(壳)的稀土丰度、配分模式与伴生元素的关系以及稀土的来源作了较为详细的探讨。研究表明,南海铁锰结核(壳)的平均丰度为1625×10~(-6),铁锰结核为2167×10~(-6),分别要比太平洋结核高1—2倍,比太平洋北部沉积物高3—4倍,比南海沉积物高10—20倍;结核和结壳的稀土经球粒陨石标准化后的配分模式基本相同,Ce正异常,Eu亏损不明显;与伴生元素、沉积物及岩石稀土对比研究表明,结核(壳)中稀土主要来自南海中酸性岩类风化、淋漓后缓慢沉积。     

海洋气团对沿海城市大气环境影响与识别研究

本研究通过识别海洋气团特征及沿海城市大气受到海洋气团的影响方式与程度,为评价沿海城市空气环境质量提供科学依据。以青岛市为例,收集大气气溶胶样品中放射性核素~(210)Pb、40K数据及采集时段当地大气颗粒物数据;分析~(210)Pb活度浓度与气溶胶颗粒物浓度变化;对当地当时大气气团进行溯源分析。研究表明:(1)研究期间青岛沿岸地区2015年4月至2016年6月与2016年6月至2017年6月大气污染特征显著不同,前者~(210)Pb活度浓度与污染颗粒物浓度显著相关,而后者~(210)Pb活度浓度与污染颗粒物无相关关系;(2)穿越海洋的陆地气团呈现出高活度浓度、低颗粒物浓度的特征;来自海洋气团的气溶胶呈现出低活度浓度、低颗粒物浓度的特征;(3)海洋气团气溶胶中~(210)Pb活度浓度较低。临近大陆的海洋(黄海、东海)上层大气受到大陆气团的影响,其海洋气团的特征有所减弱。~(210)Pb活度浓度、颗粒物浓度(PM2.5)可作为判断海洋气团的指标,识别"来自海洋的气团"与"经过海洋的气团"。     

Chemical Composition of North Atlantic Aerosols

The paper presents new information on the chemical composition of the insoluble aerosol fraction in the atmospheric surface boundary layer of different climatic zones of the North Atlantic (temperate humid, arid and semiarid, equatorial humid). The material for this study was collected during 12 expeditions. Nylon meshes were used to catch aerosols along the course of vessels. Aerosols above the North Atlantic consist of lithogenic, biogenic, and anthropogenic particles transported from different regions, which governs the differences in their concentrations and mineral and chemical compositions. Significant (by more than an order of magnitude) enrichment of aerosols in Cu, Cd, Zn, Pb, Sb, and Se is related to anthropogenic atmospheric pollution.