Mitsuo Uematsu

Impacts of Atmospheric Anthropogenic Nitrogen on the Open Ocean

Increasing quantities of atmospheric anthropogenic fixed nitrogen entering the open ocean could account for up to about a third of the oceans external (nonrecycled) nitrogen supply and up to ∼3% of the annual new marine biological production, ∼0.3 petagram of carbon per year. This input could account for the production of up to ∼1.6 teragrams of nitrous oxide (N2O) per year. Although ∼10% of the oceans drawdown of atmospheric anthropogenic carbon dioxide may result from this atmospheric nitrogen fertilization, leading to a decrease in radiative forcing, up to about two-thirds of this amount may be offset by the increase in N2O emissions. The effects of increasing atmospheric nitrogen deposition are expected to continue to grow in the future.

Impacts of atmospheric nutrient deposition on marine productivity: Roles of nitrogen, phosphorus, and iron

Nutrients are supplied to the mixed layer of the open ocean by either atmospheric deposition or mixing from deeper waters, and these nutrients drive nitrogen and carbon fixation. To evaluate the importance of atmospheric deposition, we estimate marine nitrogen and carbon fixation from present-day simulations of atmospheric deposition of nitrogen, phosphorus, and iron. These are compared with observed rates of marine nitrogen and carbon fixation. We find that Fe deposition is more important than P deposition in supporting N fixation. Estimated rates of atmospherically supported carbon fixation are considerably lower than rates of marine carbon fixation derived from remote sensing, indicating the subsidiary role atmospheric deposition plays in total C uptake by the oceans. Nonetheless, in high-nutrient, low-chlorophyll areas, the contribution of atmospheric deposition of Fe to the surface ocean could account for about 50% of C fixation. In marine areas typically thought to be N limited, potential C fixation supported by atmospheric deposition of N is only ~1%-2% of observed rates. Although these systems are N-limited, the amount of N supplied from below appears to be much larger than that deposited from above. Atmospheric deposition of Fe has the potential to augment atmospherically supported rates of C fixation in N-limited areas. In these areas, atmospheric Fe relieves the Fe limitation of diazotrophic organisms, thus contributing to the rate of N fixation. The most important uncertainties in understanding the relative importance of different atmospheric nutrients are poorly understood speciation and solubility of Fe as well as the N:Fe ratio of diazotrophic organisms.

Atmospheric fluxes of organic N and P to the global ocean

The global tropospheric budget of gaseous and particulate non-methane organic matter (OM) is re-examined to provide a holistic view of the role that OM plays in transporting the essential nutrients nitrogen and phosphorus to the ocean. A global 3-dimensional chemistry-transport model was used to construct the first global picture of atmospheric transport and deposition of the organic nitrogen (ON) and organic phosphorus (OP) that are associated with OM, focusing on the soluble fractions of these nutrients. Model simulations agree with observations within an order of magnitude. Depending on location, the observed water soluble ON fraction ranges from similar to 3% to 90% (median of similar to 35%) of total soluble N in rainwater; soluble OP ranges from similar to 20-83% (median of similar to 35%) of total soluble phosphorus. The simulations suggest that the global ON cycle has a strong anthropogenic component with similar to 45% of the overall atmospheric source (primary and secondary) associated with anthropogenic activities. In contrast, only 10% of atmospheric OP is emitted from human activities. The model-derived present-day soluble ON and OP deposition to the global ocean is estimated to be similar to 16 Tg-N/yr and similar to 0.35 Tg-P/yr respectively with an order of magnitude uncertainty. Of these amounts similar to 40% and similar to 6%, respectively, are associated with anthropogenic activities, and 33% and 90% are recycled oceanic materials. Therefore, anthropogenic emissions are having a greater impact on the ON cycle than the OP cycle; consequently increasing emissions may increase P-limitation in the oligotrophic regions of the worlds ocean that rely on atmospheric deposition as an important nutrient source.

Differing Growth Responses of Major Phylogenetic Groups of Marine Bacteria to Natural Phytoplankton Blooms in the Western North Pacific Ocean

ABSTRACT Growth and productivity of phytoplankton substantially change organic matter characteristics, which affect bacterial abundance, productivity, and community structure in aquatic ecosystems. We analyzed bacterial community structures and measured activities inside and outside phytoplankton blooms in the western North Pacific Ocean by using bromodeoxyuridine immunocytochemistry and fluorescence in situ hybridization (BIC-FISH). Roseobacter/Rhodobacter, SAR11, Betaproteobacteria, Alteromonas, SAR86, and Bacteroidetes responded differently to changes in organic matter supply. Roseobacter/Rhodobacter bacteria remained widespread, active, and proliferating despite large fluctuations in organic matter and chlorophyll a (Chl-a) concentrations. The relative contribution of Bacteroidetes to total bacterial production was consistently high. Furthermore, we documented the unexpectedly large contribution of Alteromonas to total bacterial production in the bloom. Bacterial abundance, productivity, and growth potential (the proportion of growing cells in a population) were significantly correlated with Chl-a and particulate organic carbon concentrations. Canonical correspondence analysis showed that organic matter supply was critical for determining bacterial community structures. The growth potential of each bacterial group as a function of Chl-a concentration showed a bell-shaped distribution, indicating an optimal organic matter concentration to promote growth. The growth of Alteromonas and Betaproteobacteria was especially strongly correlated with organic matter supply. These data elucidate the distinctive ecological role of major bacterial taxa in organic matter cycling during open ocean phytoplankton blooms.

Multielemental analysis and characterization of fine aerosols at several key ACE‐Asia sites

loadings of 29, 16, and 9.1 mg/m 3 and coarse mass loadings of 33, 14, and 11 mg/m 3 were measured at Hong Kong, Cheju, and Sado Island sites, respectively, during the study period. The corresponding maximum PM2.5 and coarse mass values for the three sites were 109, 81, and 78 mg/m 3 and 101, 162, and 253 mg/m 3 , respectively. Accelerator-based ion beam analysis (IBA) techniques were used to quantify major components as well as significant trace elements. These included total hydrogen, black carbon, F, Na, Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Br, and Pb, with detection limits close to or below 1 ng/m 3 . The average PM2.5 percentage composition by weight across the three sites was estimated to be around (8.4 ± 4)% black carbon, (7.7 ± 7)% soil, (43 ± 14)% ammonium sulfate, (11 ± 16)% organic matter, (10 ± 12)% salinity, and (0.6 ± 0.3)% trace elements. Soil fingerprints for the east Asian region were generated using oxides of measured Al, Si, K, Ca, Ti, Mn, and Fe concentrations. The coarse fraction was dominated by wind blown soil (23%) and sea salts (48%). [PM10/PM2.5] mass ratios were typically (2.1 ± 0.4) averaged across all sites for the whole year. [PM10/PM2.5] mass ratios for the 21 IBA elements analyzed were also provided. This quantitative data providing both masses and dates over an 18-month period provide useful input for aerosol transport modeling for the east Asia region. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0345 Atmospheric Composition and Structure: Pollution—urban and regional (0305); 0399 Atmospheric Composition and Structure: General or miscellaneous; 1610 Global Change: Atmosphere (0315, 0325); 1620 Global Change: Climate dynamics (3309); KEYWORDS: PM2.5, PM10, aerosols, fine particle characterization, Asian region, ACE-Asia, IBA techniques

Lead isotope ratios in the urban air of eastern and central Russia

In order to characterize airborne lead in eastern and central Russian cities in terms of lead isotope ratios, aerosol samples were collected at six selected cities and Moscow, and their lead concentrations and isotope ratios were studied by comparing them to the data of ore lead used in Russia. All eastern Russian cities (Vladivostok, Khabarovsk and Yakutsk) were found to have isotope ratios similar to those of ore leads in Kazakhstan, the major lead producer for Russia. Samples collected in Moscow also showed isotope ratios similar to those of eastern Russian cities. The contribution from coal combustion to airborne lead was considered to be small even in winter, in these cities. This observation suggested that the origin of lead in these Russian atmosphere regions is closely related to the lead products (e.g. leaded gasoline). The lead isotope ratios in three eastern Russian cities were very close to the value for Russian air mass reported previously in Japan, which were also in good agreement with the same observation in Sweden. However, considerably different lead isotope ratios were observed in central Russian cities, Kemerovo and Nizhnevartovsk, indicating that specific lead emissions, such as industrial activities using Precambrian-age ores or unique leaded gasoline, might contribute to the atmospheric lead.

Megacities and Large Urban Agglomerations in the Coastal Zone: Interactions Between Atmosphere, Land, and Marine Ecosystems

Megacities are not only important drivers for socio-economic development but also sources of environmental challenges. Many megacities and large urban agglomerations are located in the coastal zone where land, atmosphere, and ocean meet, posing multiple environmental challenges which we consider here. The atmospheric flow around megacities is complicated by urban heat island effects and topographic flows and sea breezes and influences air pollution and human health. The outflow of polluted air over the ocean perturbs biogeochemical processes. Contaminant inputs can damage downstream coastal zone ecosystem function and resources including fisheries, induce harmful algal blooms and feedback to the atmosphere via marine emissions. The scale of influence of megacities in the coastal zone is hundreds to thousands of kilometers in the atmosphere and tens to hundreds of kilometers in the ocean. We list research needs to further our understanding of coastal megacities with the ultimate aim to improve their environmental management.

Numerical study of the atmospheric input of anthropogenic total nitrate to the marginal seas in the western North Pacific region

[1] Atmospheric input of anthropogenic total nitrate to marginal seas in the western North Pacific region was simulated using a regional chemical transport model over East Asia based on year-to-year emission estimates during 1980-2003. Seasonal cycles and concentration levels of gas and aerosol were examined using observation data from various studies. The model simulated total nitrate deposition over the East China Sea (ECS) as 140 GgN/yr, which is the same order of the annual river discharge from the Yangtze River. The ratio of dry and wet deposition over ECS was obtained as approximately 6: 4. Total nitrate deposition over ECS corresponds to 3.2% (N base) of total NO x emission in China. The total deposition at present is three times larger than that of 1980, corresponding with increased NO x emissions.

Hygroscopicity and cloud condensation nucleus activity of marine aerosol particles over the western North Pacific

Received 14 July 2010; revised 12 October 2010; accepted 27 October 2010; published 19 March 2011. [1] Hygroscopic growth of aerosol particles at 85% relative humidity and the number fraction of cloud condensation nuclei (CCN; 0.42%, 0.23%, and 0.10% supersaturation) as a function of dry diameter (24.1–359 nm) were measured simultaneously on board R/V Hakuho‐Maru over the western North Pacific during August–September 2008. Highly hygroscopic and unimodal growth distributions were observed, except for aerosols, which showed lower hygroscopic growth over the northern Pacific. The measured particle hygroscopicity, CCN activation diameters, and chemical composition data suggest the dominance of internally mixed sulfate aerosols. Backward air mass trajectory analysis exhibits an intrusion of free tropospheric aerosol, which was likely influenced by Kasatochi’s volcanic plume and which was linked to the low‐hygroscopicity event. Frequent observation of the Hoppel minimum suggests that in‐cloud processing over the Pacific enhanced and/or maintained the high hygroscopicity of accumulation mode particles. The CCN activation diameters predicted from median hygroscopic growth factors (gmedian) agreed well with those determined from the CCN efficiency spectra, without assuming surface tension reduction caused by organics or enhancement of bulk hygroscopicity at high RH caused by sparingly soluble or polymeric compounds. The CCN spectra predicted from gmedian and measured CCN activation diameters suggest that the high CCN activities of particles over the North Pacific are sustained by high hygroscopicity, while sporadic changes of aerosol origins produce the diversity of the aerosol properties.

Equilibrator Inlet-Proton Transfer Reaction-Mass Spectrometry (EI-PTR-MS) for Sensitive, High-Resolution Measurement of Dimethyl Sulfide Dissolved in Seawater

We developed an equilibrator inlet-proton transfer reaction-mass spectrometry (EI-PTR-MS) method for fast detection of dimethyl sulfide (DMS) dissolved in seawater. Dissolved DMS extracted by bubbling pure nitrogen through the sample was continuously directed to the PTR-MS instrument. The equilibration of DMS between seawater and the carrier gas, and the response time of the system, were evaluated in the laboratory. DMS reached equilibrium with an overall response time of 1 min. The detection limit (50 pmol L(-1) at 5 s integration) was sufficient for detection of DMS concentrations in the open ocean. The EI-PTR-MS instrument was deployed during a research cruise in the western North Pacific Ocean. Comparison of the EI-PTR-MS results with results obtained by means of membrane tube equilibrator-gas chromatography/mass spectrometry agreed reasonably well on average (R(2) = 0.99). EI-PTR-MS captured temporal variations of dissolved DMS concentrations, including elevated peaks associated with patches of high biogenic activity. These results demonstrate that the EI-PTR-MS technique was effective for highly time-resolved measurements of DMS in the open ocean. Further measurements will improve our understanding of the biogeochemical mechanisms of the production, consumption, and distribution of DMS on the ocean surface and, hence, the air-sea flux of DMS, which is a climatically important species.