Dimethyl sulfide in the atmospheric surface layer of the Equatorial Pacific Ocean

This paper reports a case study of atmospheric stability effect on dimethyl sulfide(DMS) concentration in the air. Investigation includes model simulation and field measurements over the Pacific Ocean. DMS concentration in surface sea water and in the air were measured during a research cruise from Hawaii to Tahiti. The diurnal variation of air temperature over the sea surface differed from the diurnal cycle of sea surface temperature because of the high heat capacity of sea water. The diurnal cycle of average DMS concentration in the air was studied in relation to the atmospheric stability parameter and surface heat flux. All these parameters had minima at noon and maxima in the early morning. The correlation coefficient of the air DMS concentration with wind speed (at 15 m high) was 0. 64. The observed concentrations of DMS in the equatorial marine surface layer and their diurnal variability agree well with model simulations. The simulated results indicate that the amplitude of the cycle and the mean     

Iron-induced alterations of bacterial DMSP metabolism in the western subarctic Pacific during SEEDS-II

The effect of added iron on bacterial cycling of the climate-active gas dimethylsulfide (DMS) and its precursor dimethylsulfoniopropionate (DMSP) was tested during the second Subarctic Pacific Iron Experiment for Ecosystem Dynamics Study (SEEDS II) from 19 July to 21 August 2004 aboard the R/V Hakuho-Maru. The study area in the northwest Pacific Ocean (48°N 165°E) was enriched with Fe and the conservative tracer, SF₆, allowing the fertilized patch to be tracked. Microbial DMSP cycling rates were determined in the surface mixed layer (5 m) during incubations using the ³⁵S-DMSP technique. The addition of iron resulted in a 4-fold increase in concentrations of chlorophyll a (chl a) within the surface mixed layer (5 m depth), and the length of the sampling period allowed the observation of both bloom and post-bloom conditions. Inside the fertilized patch, the alleviation of resource limitation gave rise to the concurrent increase in bacterial abundance and production. Changes in the phytoplankton community within the Fe-enriched patch translated into a sustained decrease in chl a-normalized particulate DMSP (DMSP_p) concentrations, suggesting a preferential stimulation of the growth of DMSP_p-poor phytoplankton species. Despite short-lived peaks of DMSP_p within the Fe-enriched area, concentrations of DMSP_p generally remained stable during the entire sampling period inside and outside the fertilized patch. During the Fe-induced bloom, microbial DMSP-sulfur (DMSP-S) assimilation efficiency increased 2.6-fold inside the Fe-enriched area, which indicated that as bacterial production increased, a greater proportion of DMSP-S was assimilated and possibly diverted away from the bacterial cleavage pathway (i.e. production of DMS). Our results suggest that iron-induced stimulation of weak DMSP_p-producers and DMSP-assimilating bacteria may diminish the potential production of DMS and thus limit its flux towards the atmosphere over the subarctic Pacific Ocean.     

西沙大气二氧化碳浓度变化特征研究

CO2是引起全球气候变暖的最重要温室气体。大气中过量CO2被海水吸收后将改变海水中碳酸盐体系的组成,造成海水酸化,危害海洋生态环境。本文采用局部近似回归法对2013年12月—2014年11月期间西沙海洋大气CO2浓度连续监测数据进行筛分,得到西沙大气CO2区域本底浓度。结果表明,西沙大气CO2区域浓度具有明显的日变化和季节变化特征。4个季节西沙大气CO2区域本底浓度日变化均表现为白天低、夜晚高,最高值405.39×10-6(体积比),最低值399.12×10-6(体积比)。西沙大气CO2区域本底浓度季节变化特征表现为春季和冬季高,夏季和秋季低。CO2月平均浓度最高值出现在2013年12月,为406.22×10-6(体积比),最低值出现在2014年9月,为398.68×10-6(体积比)。西沙大气CO2区域本底浓度日变化主要受本区域日照和温度控制。季节变化主要控制因素是南海季风和大气环流,南海尤其是北部海域初级生产力变化和海洋对大气CO2的源/汇调节作用。     

海洋中生源活性气体的来源与迁移转化

海洋生源活性气体主要包括二甲基硫（DMS）、甲烷（CH₄）、氧化亚氮（N₂O）、一氧化碳（CO）、挥发性卤代烃（VHCs）和非甲烷烃（NMHCs）等。它们通过海-气交换进入大气，不仅在全球碳、氮和硫循环中发挥关键作用，而且会直接或间接地对环境和气候变化产生重要影响。海洋释放的活性气体一类属于温室效应气体（CH₄、N₂O、VHCs和CO等），另一类会在大气中发生化学反应，控制着大气氧化平衡和臭氧浓度（VHCs和NMHCs）。而DMS属于负温室效应气体，其在大气中被快速氧化形成硫酸盐气溶胶，进而对云的形成和辐射强迫产生重要影响。本文综述了国内外海洋生源活性气体的研究现状，着重介绍了DMS、CH₄和N₂O的来源、迁移转化、海-气通量及其影响机制，并指明了该领域存在的科学问题及今后的研究方向。     

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.     

Biogeochemical ocean-atmosphere transfers in the Arabian Sea

Transfers of some important biogenic atmospheric constituents, carbon dioxide (CO₂), methane (CH₄), molecular nitrogen (N₂), nitrous oxide (N₂O), nitrate , ammonia (NH₃), methylamines (MAs) and dimethylsulphide (DMS), across the air–sea interface are investigated using published data generated mostly during the Arabian Sea Process Study (1992–1997) of the Joint Global Ocean Flux Study (JGOFS). The most important contribution of the region to biogeochemical fluxes is through the production of N₂ and N₂O facilitated by an acute, mid-water deficiency of dissolved oxygen (O₂); emissions of these gases to the atmosphere from the Arabian Sea are globally significant. For the other constituents, especially CO₂, even though the surface concentrations and atmospheric fluxes exhibit extremely large variations both in space and time, arising from the unique physical forcing and associated biogeochemical environment, the overall significance in terms of their global fluxes is not much because of the relatively small area of the Arabian Sea. Distribution and air–sea exchanges of some of these constituents are likely to be greatly influenced by alterations of the subsurface O₂ field forced by human-induced eutrophication and/or modifications to the regional hydrography.     

Responses of DMS in the seawater and atmosphere to iron enrichment in the subarctic western North Pacific (SEEDS-II)

Simultaneous measurements of dimethylsulfide (DMS) in the seawater and atmosphere were conducted during SEEDS-II to investigate the responses of DMS to iron (Fe) fertilization in the subarctic North Pacific. No significant increases in the seawater DMS (DMSw) concentration were observed inside the fertilized patch compared to those outside the patch, while particulate dimethylsulfoniopropionate (DMSPp) concentration inside the patch increased 2-fold compared to those outside the patch in the phytoplankton bloom of major DMSP producers such as prasinophytes, cryptophytes, diatoms and prymnesiophytes. In the decline phase of the bloom, maximum DMSw was observed both inside the patch (ca. 6.2 nM) and outside the patch (ca. 9.3 nM). In this period, increases in mesozooplankton and decreases in the DMSP producers (prymnesiophytes and diatoms) were observed both sides of the patch, but larger inside the patch than outside the patch. Large decreases in the DMSPp inside the patch, which was probably related to the large increases in mesozooplankton inside the patch, did not result in increases in the DMSw concentration. Considering biological and nonbiological parameters, we discussed these results, although they could not be completely explained. Unfortunately, the impact of Fe fertilization on the atmospheric DMS (DMSa) concentration was not detected due to no significant changes in DMSw. However, it is noted that DMSa concentrations were dependent on the sea–air DMS flux in the air from higher latitudes and/or the Eurasian continent, though the DMS flux was a minor role to the budget of DMSw. Therefore if DMSw were significantly changed by Fe fertilization, DMSa might be affected through changes in the sea-air flux in this condition.     

Variability of trace gases in the atmospheric surface layer from observations in the city of Moscow

The results of continuous minute measurements of the surface concentrations of ozone, nitric oxide, nitrogen dioxide, carbon monoxide, and sulfur dioxide during the 2002–2004 period at the environmental station of the Oboukhov Institute of Atmospheric Physics, Russian Academy of Sciences (IAP), and the Faculty of Geography, Moscow State University (MSU), are discussed. It is shown that the conditions of Moscow’s southwestern region remote from large local pollution sources reflect the general regularities of the variability of trace gases in an urban atmosphere. This is manifested in the mean annual value of the ratio NO/NO₂ (a little less than 1), decreased daylight values of O₃, increased values of the rest of the trace gases as compared to the background region, and the presence of a secondary nocturnal maximum in the diurnal cycle of O₃. The features of the annual and diurnal cycles of the concentrations of the substances under analysis are discussed. In the diurnal cycle of the primary products of combustion (NO and CO), an excess of the morning maximum (over the evening one) is observed during both warm and transition periods and higher values of the night maximum (as compared to the daylight one) are noted for summer. The temperature stratification properties determined from the MSU long-term acoustic sounding data serve as a possible cause for both of the effects revealed. The annual cycle of the concentration of surface ozone is characterized by the highest values for spring and summer. The annual cycles of NO, NO₂, CO, and SO₂ do not demonstrate any obvious seasonal regularities. A significant seasonal variation of the ratio NO/NO₂, which is associated with the oxidizing properties of the urban atmosphere, is revealed. The record high concentrations of trace gases in the atmosphere over Moscow are given, and the meteorological conditions for their accumulation are discussed.     

Atmospheric remote sensing constraints on direct sea-air methane flux from the 22/4b North Sea massive blowout bubble plume

A new airborne remote sensing approach to estimate an upper limit of the direct sea-air methane emission flux was applied over the 22/4b blowout site located at N57.92°, E1.63° in the North Sea. Passive remote sensing data using sunglint/sunglitter geometry were collected during instrumental tests with the Methane Airborne MAPper – MAMAP – instrument installed aboard the Alfred Wegener Institute (AWI) Polar-5 aircraft on 3. June 2011. MAMAP is a passive short wave infrared (SWIR) remote sensing spectrometer for airborne measurements and retrieval of the atmospheric column-averaged dry air mole fractions of methane (XCH₄) and carbon dioxide (XCO₂). In addition to MAMAP a fast CH₄ in-situ analyzer (Los-Gatos Research Inc. RMT-200), two 5-hole turbulence probes and the Polar-5 basic sensor suite comprising different temperature, pressure, humidity and camera sensors were installed aboard the aircraft. The collected MAMAP remote sensing data acquired in the vicinity of the 22/4b blowout site showed no detectable increase in the derived XCH₄ (with respect to the atmospheric background). Based on the absence of a detectable XCH₄ column increase, an approximate top-down upper-limit for the direct atmospheric 22/4b blowout CH₄ emissions from the main bubble plume of less than 10 ktCH₄/yr has been derived. The constraint has been determined by comparing XCH₄ information derived by the remote sensing measurements with results obtained from a Gaussian plume forward model simulation taking into account the actual flight track, the instrument sensitivity and measurement geometry, as well as the prevailing atmospheric conditions.     

挪威海和格陵兰海海水DMS分布特征及影响因素研究

于2012年7—9月现场测定了北极挪威海和格陵兰海区域海水二甲基硫(DMS)及其前体物质二甲巯基丙酸内盐(DMSP,分溶解态DMSPd和颗粒态DMSPp)的含量,研究了其空间分布格局及其影响因素,探讨了表层海水DMS的生物周转和去除途径。结果表明,表层海水DMS、DMSPd和DMSPp的平均浓度分别为5.36nmol/L、15.63nmol/L和96.73nmol/L,受挪威海流和北极深层水影响,表层海水二甲基硫化物浓度呈现出由低纬度向高纬度海域递减的趋势。DMSPd和DMSPp浓度与Chl a浓度均有显著的相关性,说明浮游植物生物量是影响挪威海和格陵兰海二甲基硫化物生产的重要因素。表层海水DMS生物生产和消费速率平均值分别为18.19nmol/(L·d)、15.67nmol/(L·d)。DMS微生物周转时间变化范围为0.03~1.80d,平均值为0.49d,DMS海-气周转时间是微生物消费时间的90倍,说明夏季挪威海和格陵兰海表层海水中DMS微生物消费过程是比海-气扩散更具优势的去除机制。     

Chemical and isotopic evidence for the nature of the fluid in CH4-containing sediments of the Håkon Mosby Mud Volcano

The pore waters of CH₄-containing sediments of the Håkon Mosby Mud Volcano were rich in NH⁺ ₄, Br^-, and I^-; exhibited a high total alkalinity; but were poor in Cl^-and SO^2- ₄. The geological evidence and our data suggest that organic matter decomposition in preglacial or early interglacial sediments took place during early diagenesis (bacterial processes) and during metamorphism (thermogenic processes under the 3100-m-thick layer of glacial sediments), accompanied by mud volcano fluid generation. It is argued that the CH₄of the mud volcano sediments has a mixed, biogenic and thermogenic, origin.     

Spatial variability and temporal dynamics of surface water pCO2, ��O2/Ar and dimethylsulfide in the Ross Sea, Antarctica

We report results from two surveys of pCO₂, biological O₂ saturation (??O₂/Ar) and dimethylsulfide (DMS) in surface waters of the Ross Sea polynya. Measurements were made during early spring (November 2006-December 2006) and mid-summer (December 2005-January 2006) using ship-board membrane inlet mass spectrometry (MIMS) for high spatial resolution (i.e. sub-km) analysis. During the early spring survey, the polynya was in the initial stages of development and exhibited a rapid increase in open water area and phytoplankton biomass over the course of our ∼3 week occupation. We observed a rapid transition from a net heterotrophic ice-covered system (supersaturated pCO₂ and undersaturated O₂) to a high productivity regime associated with a Phaeocystis-dominated phytoplankton bloom. The timing of the early spring phytoplankton bloom was closely tied to increasing sea surface temperature across the polynya, as well as reduced wind speeds and ice cover, leading to enhanced vertical stratification. There was a strong correlation between pCO₂, ??O₂/Ar, DMS and chlorophyll a (Chl a) during the spring phytoplankton bloom, indicating a strong biological imprint on gas distributions. Box model calculations suggest that pCO₂ drawdown was largely attributable to net community production, while gas exchange and shoaling mixed layers also exerted a strong control on the re-equilibration of mixed layer ??₂ with the overlying atmosphere. DMS concentrations were closely coupled to Phaeocystis biomass across the early spring polynya, with maximum concentrations exceeding 100 nM.During the summer cruise, we sampled a large net autotrophic polynya, shortly after the seasonal peak in phytoplankton productivity. Both diatoms and Phaeocystis were abundant in the phytoplankton assemblages during this time. Minimum pCO₂ was less than 100 ppm, while ??O₂/Ar exceeded 30% in some regions. Mean DMS concentrations were ∼2-fold lower than during the spring, although the range of concentrations was similar between the two surveys. There was a significant correlation between pCO₂, ??O₂/Ar and Chl a across the summer polynya, but the strength of these correlations and the slope of O₂ vs. CO₂ relationship were significantly lower than during the early spring. Summertime DMS concentrations were not significantly correlated to phytoplankton biomass (Chl a), pCO₂ or ??O₂/Ar. In contrast to the early spring time, there were no clear temporal trends in summertime gas concentrations. Rather, small-scale spatial variability, likely resulting from mixing and localized sea-ice melt, was clearly evident in surface gas distributions across the polynya. Analysis of length-scale dependent variability demonstrated that much of the spatial variance in surface water gases occurred at scales of <20 km, suggesting that high resolution analysis is needed to fully capture biogeochemical heterogeneity in this system.     

格陵兰海气溶胶光学深度、海冰、浮游植物与二甲基硫的关系及其对未来气候的影响

dimethylsulphide (DMS)的海空通量是海洋生物气溶胶的主要来源之一,对气候（特别是北冰洋的气候）具有重要的辐射影响。利用卫星数据得到的气溶胶光学深度(AOD)作为气溶胶负荷的代表,在夏季和秋季表现的尤其明显。春季海冰的融化是北极气溶胶前体的重要来源。然而,早春的高浓度气溶胶可能与南方大陆污染的平流有关(北极霾)。更高的AOD通常在研究区域的南部出现。海冰浓度(SIC)和AOD呈正相关,而云盖(CLD)和AOD则呈负相关。SIC和CLD的季节性峰值均在AOD峰值的前一个月。AOD与SIC之间存在强烈的正相关关系。融冰与叶绿素（CHL)几乎在3月至9月呈正相关,但与春季和初夏的AOD呈负相关。春季和初夏较高的AOD有可能是由融冰和春季强风在该地区的结合影响。由于春季风的升高和冰的融化,在春季出现了DMS通量的峰值。从3月到五月,DMS浓度和AOD及融冰都呈正相关。早秋季升高的AOD可能与浮游植物合成的生物气溶胶的排放有关。到2100年，格陵兰海的DMS通量将增加3倍以上。生物气溶胶的显著增加可以部分抵消格陵兰海的增温现象。     

Dry and wet deposition of nutrients from the tropical Atlantic atmosphere: Links to primary productivity and nitrogen fixation

Atmospheric deposition fluxes of soluble nutrients (N, P, Si, Fe, Co, Zn) to the tropical North Atlantic were determined during cruise M55 of the German SOLAS programme. Nutrient fluxes were highest in the east of the section along 10°N, owing to the proximity of source regions in West Africa and Europe, and lowest in the west, for both dry and wet deposition modes. In common with other recent studies, atmospheric P and Si inputs during M55 were strongly depleted relative to the stoichiometry of phytoplankton Fe, N, P and Si requirements. Atmospheric N inputs were equivalent to 0.1–4.7% of observed primary productivity during the cruise. Atmospheric nutrient supply was also compared to observed nitrogen fixation rates during M55. While atmospheric Fe supply may have been sufficient to support N fixation (depending on the relationship between our simple Fe leaching experiment and aerosol Fe dissolution in seawater), atmospheric P supply was well below the required rate. The stable nitrogen isotope composition of nitrate–N in aerosol and rain was also determined. Results of a simple model indicate that atmospheric deposition and nitrogen fixation introduce similar amounts of isotopically light nitrogen into surface waters of the study region. This implies that nitrogen isotope-based methods would overestimate nitrogen fixation here by a factor of 2, if atmospheric inputs were not taken into account.     

Diurnal and seasonal variation in physico-chemical conditions within intertidal rock pools

A study of the diurnal and seasonal variation in the physico-chemical conditions within intertidal rock pools on the West coast of Scotland was undertaken to provide data on the environmental conditions experienced by animals inhabiting these pools. The temperature, pH, partial pressure of oxygen (P_O2) and salinity were measured every hour for 24 h and the total alkalinity, partial pressure of carbon dioxide (P_CO2) and carbon dioxide content (C_CO2) calculated. This sampling regime was carried out once a month for 12 months to determine the extent of seasonal variation in conditions within temperate pools.Large diurnal variations were recorded in nearly all the physico-chemical parameters measured. The greatest variation was recorded in the temperature and P_O2 of the water but significant changes in pH and P_CO2 were also recorded. Total alkalinity varied little during any 24 h period but carbonate alkalinity, which was always lower than total alkalinity, showed slightly greater variation. There was also considerable variation in the magnitude of these diurnal changes between pools at different heights on the shore.Diurnal variation in the physico-chemical conditions within the pools were observed throughout the year although the magnitude of these changes varied seasonally. Detailed studies on individual pools demonstrated that appreciable local variation existed in the physico-chemical conditions within each pool.     

Distribution of biogenic sulphur compounds during and just after the southwest monsoon in the Arabian Sea

The Arabian Sea is characterised by strong seasonal oscillations of biological productivity generated by its monsoonal climate. The southwest monsoon causes reversal in the surface circulation of the Arabian Sea, which generates a seasonal upwelling of nutrient-rich waters along the coast of Oman. Concentrations of biogenic sulphur compounds were measured on a transect from the eutrophic waters off the coast of Oman to the oligotrophic waters of the open Arabian Sea, during the UK NERC Arabesque cruise 27 August–4 October 1994. The concentrations of dimethylsulphide (DMS), dimethylsulphoxide (DMSO) and dimethylsulphoniopropionate (DMSP) were found to be elevated in the eutrophic area due to enhanced biological production. However, this increase in DMS, DMSO and DMSP concentration was not observed until after the southwest monsoon had relaxed, and appeared to correspond to increased concentrations of hexanoyloxyfucoxanthin, an indicator of prymnesiophytes. DMSO concentrations were correlated with those of DMS and DMSP in the near surface waters of the Arabian Sea. Additionally, DMSO appeared to be ubiquitous throughout the water column, being easily detectable in deep waters, which suggests that DMSO may act as a sink for DMS in the world’s oceans.     

Seasonal Study of Methane and Nitrous Oxide in the Coastal Waters of the Southern Baltic Sea

Atmospheric and dissolved methane (CH₄) and nitrous oxide (N₂O) were measured in the unique coastal ecosystem of theBoddenwaters, including the western Oder estuary, (southern Baltic Sea) during five campaigns between 1994 and 1997. The CH₄saturations, ranging from 105–15 500%, showed great spatial and temporal variability with maximum values in September and minimum values in December. The N₂O saturations were in the range of 91–312% with a maximum in March. Enhanced concentrations of both gases were observed only in the western Oder estuary near the mouth of the Peene River. Thus, we conclude that the distributions of CH₄and N₂O in the investigatedBoddenwaters are, directly or indirectly, linked to the Peene River runoff and not to the Oder River. Our estimate of the annual CH₄emissions from theBoddenwaters to the atmosphere indicates a significant contribution (c. 17%) to the overall CH₄emissions from the Baltic Sea. In contrast, theBoddenwaters represent only a small source for atmospheric N₂O.CH₄production rates estimated from sediment slurry experiments revealed a significant spatial variability and indicated that methanogenic activity was related to acetate consumption in the surface sediment layer. Sedimentary CH₄production might depend on different amounts of accumulation of organic material.     

西太平洋雅浦海沟区海水中CH4和DMSP的垂直变化特征

本研究首次探究了西太平洋雅浦海沟北段从表层到超深渊海水中甲烷（CH₄）及二甲基硫（DMS）的前体物质二甲基巯基丙酸内盐（DMSP）的浓度变化情况。结果表明:雅浦海沟海水甲烷浓度变化范围为1.49~3.87 nmol/L。其上层海水甲烷平均浓度最高，有明显的次表层极大现象。雅浦海沟氧最小层海水的甲烷平均浓度最低；在500~1 000 m中层水中甲烷浓度有一定程度的增大，1 000 m以下至底层甲烷浓度继续升高。研究海区溶解态DMSP（DMSPd）和总DMSP（DMSPt）平均浓度的垂直变化随深度呈先增大后减小趋势，颗粒态DMSP（DMSPp）的平均浓度随深度呈波动式变化，在中层达到最大。雅浦海沟CH₄和DMSP浓度垂直变化受浮游生物、微生物、光照、温度、压力、大洋环流等的复杂影响。在真光层海水中，CH₄浓度与DMSPd、DMSPp和DMSPt浓度表现为负相关关系，在200 m至底层海水中，CH₄浓度与DMSPd、DMSPp和DMSPt浓度表现为正相关关系，显示光照条件是造成雅浦海沟不同深度海水CH₄和DMSP浓度相关性差异的关键因素。     

The SOLAS air-sea gas exchange experiment (SAGE) 2004

The SOLAS air-sea gas exchange experiment (SAGE) was a multiple-objective study investigating gas-transfer processes and the influence of iron fertilisation on biologically driven gas exchange in high-nitrate low-silicic acid low-chlorophyll (HNLSiLC) Sub-Antarctic waters characteristic of the expansive subpolar zone of the southern oceans. This paper provides a general introduction and summary of the main experimental findings. The release site was selected from a pre-voyage desktop study of environmental parameters to be in the south-west Bounty Trough (46.5°S 172.5°E) to the south-east of New Zealand and the experiment was conducted between mid-March and mid-April 2004. In common with other mesoscale iron addition experiments (FeAX’s), SAGE was designed as a Lagrangian study, quantifying key biological and physical drivers influencing the air-sea gas exchange processes of CO₂, DMS and other biogenic gases associated with an iron-induced phytoplankton bloom. A dual tracer SF₆/³He release enabled quantification of both the lateral evolution of a labelled volume (patch) of ocean and the air-sea tracer exchange at tenths of kilometer scale, in conjunction with the iron fertilisation. Estimates from the dual-tracer experiment found a quadratic dependency of the gas exchange coefficient on windspeed that is widely applicable and describe air-sea gas exchange in strong wind regimes. Within the patch, local and micrometeorological gas exchange process studies (100 m scale) and physical variables such as near-surface turbulence, temperature microstructure at the interface, wave properties and windspeed were quantified to further assist the development of gas exchange models for high-wind environments.There was a significant increase in the photosynthetic competence (F_v/F_m) of resident phytoplankton within the first day following iron addition, but in contrast to other FeAX’s, rates of net primary production and column-integrated chlorophyll a concentrations had only doubled relative to the unfertilised surrounding waters by the end of the experiment. After 15 days and four iron additions totalling 1.1 ton Fe²⁺, this was a very modest response compared to other mesoscale iron enrichment experiments. An investigation of the factors limiting bloom development considered co-limitation by light and other nutrients, the phytoplankton seed-stock and grazing regulation. Whilst incident light levels and the initial Si:N ratio were the lowest recorded in all FeAXs to date, there was only a small seed-stock of diatoms (less than 1% of biomass) and the main response to iron addition was by the picophytoplankton. A high rate of dilution of the fertilised patch relative to phytoplankton growth rate, the greater than expected depth of the surface mixed layer and microzooplankton grazing were all considered as factors that prevented significant biomass accumulation. In line with the limited response, the enhanced biological draw-down of pCO₂ was small and masked by a general increase in pCO₂ due to mixing with higher pCO₂ waters. The DMS precursor DMSP was kept in check through grazing activity and in contrast to most FeAX’s dissolved dimethylsulfide (DMS) concentration declined through the experiment. SAGE is an important low-end member in the range of responses to iron addition in FeAX’s. In the context of iron fertilisation as a geoengineering tool for atmospheric CO₂ removal, SAGE has clearly demonstrated that a significant proportion of the low iron ocean may not produce a phytoplankton bloom in response to iron addition.     

The Air-Sea Exchange of CO2 in the East Sea (Japan Sea)

During CREAMS expeditions, fCO₂ for surface waters was measured continuously along the cruise tracks. The fCO₂ in surface waters in summer varied in the range 320–440 μatm, showing moderate supersaturation with respect to atmospheric CO₂. In winter, however, fCO₂ showed under-saturation of CO₂ in most of the area, while varying in a much wider range from 180 to 520 μatm. Some very high fCO₂ values observed in the northern East Sea (Japan Sea) appeared to be associated with the intensive convection system developed in the area. A gas-exchange model was developed for describing the annual variation of fCO₂ and for estimating the annual flux of CO₂ at the air-sea interface. The model incorporated annual variations in SST, the thickness of the mixed layer, gas exchange associated with wind velocity, biological activity and atmospheric concentration of CO₂. The model shows that the East Sea releases CO₂ into the atmosphere from June to September, and absorbs CO₂ during the rest of the year, from October through May. The net annual CO₂ flux at the air-sea interface was estimated to be 0.032 (±0.012) Gt-C per year from the atmosphere into the East Sea. Water column chemistry shows penetration of CO₂ into the whole water column, supporting a short turnover time for deep waters in the East Sea. This revised version was published online in August 2006 with corrections to the Cover Date.