Wind speed dependent size-resolved parameterization for the organic mass fraction of sea spray aerosol

For oceans to be a significant source of primary organic aerosol (POA), sea spray aerosol (SSA) must be highly enriched with organics relative to the bulk seawater. We propose that organic enrichment at the air-sea interface, chemical composition of seawater, and the aerosol size are three main parameters controlling the organic mass fraction of sea spray aerosol (OM<sub>SSA</sub>). To test this hypothesis, we developed a new marine POA emission function based on a conceptual relationship between the organic enrichment at the air-sea interface and surface wind speed. The resulting parameterization is explored using aerosol chemical composition and surface wind speed from Atlantic and Pacific coastal stations, and satellite-derived ocean concentrations of chlorophyll-<i>a</i>, dissolved organic carbon, and particulate organic carbon. Of all the parameters examined, a multi-variable logistic regression revealed that the combination of 10 m wind speed and surface chlorophyll-<i>a</i> concentration ([Chl-<i>a</i>]) are the most consistent predictors of OM<sub>SSA</sub>. This relationship, combined with the published aerosol size dependence of OM<sub>SSA</sub>, resulted in a new parameterization for the organic mass fraction of SSA. Global emissions of marine POA are investigated here by applying this newly-developed relationship to existing sea spray emission functions, satellite-derived [Chl-<i>a</i>], and modeled 10 m winds. Analysis of model simulations shows that global annual submicron marine organic emission associated with sea spray is estimated to be from 2.8 to 5.6 Tg C yr<sup>−1</sup>. This study provides additional evidence that marine primary organic aerosols are a globally significant source of organics in the atmosphere

Ground-based retrieval of continental and marine warm cloud microphysics

A technique for retrieving warm cloud microphysics using synergistic ground based remote sensing instruments is presented. The SYRSOC (SYnergistic Remote Sensing Of Cloud) technique utilises a K<sub><i>a</i></sub>-band Doppler cloud RADAR, a LIDAR (or ceilometer) and a multichannel microwave radiometer. SYRSOC retrieves the main microphysical parameters such as cloud droplet number concentration (CDNC), droplets effective radius (<i>r</i><sub>eff</sub>), cloud liquid water content (LWC), and the departure from adiabatic conditions within the cloud. Two retrievals are presented for continental and marine stratocumulus advected over the Mace Head Atmospheric Research Station. Whilst the continental case exhibited high CDCN (<span style="border-top: 1px solid #000; color: #000;"><i>N</i></span> = 382 cm<sup>−3</sup>; 10th-to-90th percentile [9.4–842.4] cm<sup>−3</sup>) and small mean effective radius (<span style="border-top: 1px solid #000; color: #000;"><i>r</i><sub>eff</sub></span> = 4.3; 10th-to-90th percentile [2.9–6.5] μm), the marine case showed low CDNC and large mean effective radius (<span style="border-top: 1px solid #000; color: #000;"><i>N</i></span> = 25 cm<sup>−3</sup>, 10th-to-90th percentile [1.5–69] cm<sup>−3</sup>; <span style="border-top: 1px solid #000; color: #000;"><i>r</i><sub>eff</sub></span> = 28.4 μm, 10th-to-90th percentile [11.2–42.7] μm) as expected since continental air at this location is typically more polluted than marine air. The mean LWC was comparable for the two cases (continental: 0.19 g m<sup>−3</sup>; marine: 0.16 g m<sup>−3</sup>) but the 10th–90th percentile range was wider in marine air (continental: 0.11–0.22 g m<sup>−3</sup>; marine: 0.01–0.38 g m<sup>−3</sup>). The calculated algorithm uncertainty for the continental and marine case for each variable was, respectively, σ<sub><i>N</i></sub> = 161.58 cm<sup>−3</sup> and 12.2 cm<sup>−3</sup>, σ<sub><i>r</i><sub>eff</sub></sub> = 0.86 μm and 5.6 μm, σ<sub>LWC</sub> = 0.03 g m<sup>−3</sup> and 0.04 g m<sup>−3</sup>. The retrieved CDNC are compared to the cloud condensation nuclei concentrations and the best agreement is achieved for a supersaturation of 0.1% in the continental case and between 0.1%–0.75% for the marine stratocumulus. The retrieved <i>r</i><sub>eff</sub> at the top of the clouds are compared to the MODIS satellite <i>r</i><sub>eff</sub>: 7 μm (MODIS) vs. 6.2 μm (SYRSOC) and 16.3 μm (MODIS) vs. 17 μm (SYRSOC) for continental and marine cases, respectively. The combined analysis of the CDNC and the <i>r</i><sub>eff</sub>, for the marine case shows that the drizzle modifies the droplet size distribution and <span style="border-top: 1px solid #000; color: #000;"><i>r</i><sub>eff</sub></span> especially if compared to <i>r</i><sub>eff</sub><sup>MOD</sup>. The study of the cloud subadiabaticity and the LWC shows the general sub-adiabatic character of both clouds with more pronounced departure from adiabatic conditions in the continental case than in the marine

Model evaluation of marine primary organic aerosol emission schemes

In this study, several marine primary organic aerosol (POA) emission schemes have been evaluated using the GEOS-Chem chemical transport model in order to provide guidance for their implementation in air quality and climate models. These emission schemes, based on varying dependencies of chlorophyll <i>a</i> concentration ([chl <i>a</i>]) and 10 m wind speed (<i>U</i><sub>10</sub>), have large differences in their magnitude, spatial distribution, and seasonality. Model comparison with weekly and monthly mean values of the organic aerosol mass concentration at two coastal sites shows that the source function exclusively related to [chl <i>a</i>] does a better job replicating surface observations. Sensitivity simulations in which the negative <i>U</i><sub>10</sub> and positive [chl <i>a</i>] dependence of the organic mass fraction of sea spray aerosol are enhanced show improved prediction of the seasonality of the marine POA concentrations. A top-down estimate of submicron marine POA emissions based on the parameterization that compares best to the observed weekly and monthly mean values of marine organic aerosol surface concentrations has a global average emission rate of 6.3 Tg yr<sup>−1</sup>. Evaluation of existing marine POA source functions against a case study during which marine POA contributed the major fraction of submicron aerosol mass shows that none of the existing parameterizations are able to reproduce the hourly-averaged observations. Our calculations suggest that in order to capture episodic events and short-term variability in submicron marine POA concentration over the ocean, new source functions need to be developed that are grounded in the physical processes unique to the organic fraction of sea spray aerosol

Investigating organic aerosol loading in the remote marine environment

Aerosol loading in the marine environment is investigated using aerosol composition measurements from several research ship campaigns (ICEALOT, MAP, RHaMBLe, VOCALS and OOMPH), observations of total AOD column from satellite (MODIS) and ship-based instruments (Maritime Aerosol Network, MAN), and a global chemical transport model (GEOS-Chem). This work represents the most comprehensive evaluation of oceanic OM emission inventories to date, by employing aerosol composition measurements obtained from campaigns with wide spatial and temporal coverage. The model underestimates AOD over the remote ocean on average by 0.02 (21 %), compared to satellite observations, but provides an unbiased simulation of ground-based Maritime Aerosol Network (MAN) observations. Comparison with cruise data demonstrates that the GEOS-Chem simulation of marine sulfate, with the mean observed values ranging between 0.22 μg m−3 and 1.34 μg m−3, is generally unbiased, however surface organic matter (OM) concentrations, with the mean observed concentrations between 0.07 μg m−3 and 0.77 μg m−3, are underestimated by a factor of 2–5 for the standard model run. Addition of a sub-micron marine OM source of approximately 9 TgC yr−1 brings the model into agreement with the ship-based measurements, however this additional OM source does not explain the model underestimate of marine AOD. The model underestimate of marine AOD is therefore likely the result of a combination of satellite retrieval bias and a missing marine aerosol source (which exhibits a different spatial pattern than existing aerosol in the model)

The spatial distribution of the reactive iodine species IO from simultaneous active and passive DOAS observations

We present investigations of the reactive iodine species (RIS) IO, OIO and I<sub>2</sub> in a coastal region from a field campaign simultaneously employing active long path differential optical absorption spectroscopy (LP-DOAS) as well as passive multi-axis differential optical absorption spectroscopy (MAX-DOAS). The campaign took place at the Martin Ryan Institute (MRI) in Carna, County Galway at the Irish West Coast about 6 km south-east of the atmospheric research station Mace Head in summer 2007. In order to study the horizontal distribution of the trace gases of interest, we established two almost parallel active LP-DOAS light paths, the shorter of 1034 m length just crossing the intertidal area, whereas the longer one of 3946 m length also crossed open water during periods of low tide. In addition we operated two passive Mini-MAX-DOAS instruments with the same viewing direction. While neither OIO nor I<sub>2</sub> could be unambiguously identified with any of the instruments, IO could be detected with active as well as passive DOAS. The IO column densities seen at both active LP-DOAS light paths are almost the same. Thus it can be concluded that coastal IO is almost exclusively located in the intertidal area, where we detected mixing ratios of up to 35±7.7 ppt (equivalent to pmol/mol). Nucleation events with particle concentrations of 10<sup>6</sup> cm<sup>−3</sup> particles were observed each day correlating with high IO mixing ratios. Therefore we feel that our detected IO concentrations confirm the results of model studies, which state that in order to explain such particle bursts, IO mixing ratios of 50 to 100 ppt in so called "hot-spots" are required

Primary marine aerosol emissions: size resolved eddy covariance measurements with estimates of the sea salt and organic carbon fractions

International audiencePrimary marine aerosol fluxes were measured using eddy covariance (EC), a condensation particle counter (CPC) and an optical particle counter (OPC) with a heated inlet. The later was used to discriminate between sea salt and total aerosol. Measurements were made from the 25 m tower at the research station Mace Head at the Irish west coast, May to September 2002. The aerosol fluxes were dominated by upward fluxes, sea spray from bubble bursting at the ocean surface. The sea salt aerosol number emissions increased two orders of magnitude with declining diameter from 1 to 0.1 ?m where it peaked at values of 105 to 107 particles m?2s?1. The sea salt emissions increased at all sizes in the wind range 4 to 22 ms?1, in consistency with a power function of the wind speed. The sea salt emission data were compared to three recent sub micrometer sea salt source parameterisations. The best agreement was with Mårtensson et al. (2003), which appear to apply from 0.1 to 1.1 ?m diameters in temperate water (12°C) as well as tropical water (25°C). The total aerosol emissions were independent of the wind speed below 10 ms?1, but increased with the wind above 10 ms?1. The aerosol volume emissions were larger for the total aerosol than for the sea salt at all wind speeds, while the sea salt number emissions approached the total number emissions at 15 ms?1. It is speculated that this is caused by organic carbon in the surface water that is depleted at high wind speeds. The data are consistent with an internal aerosol mixture of sea salt, organic carbon and water. Using the aerosol model by Ellison et al. (1999) (a mono-layer of organic carbon surrounding a water-sea-salt brine) we show that the total and sea salt aerosol emissions are consistent. This predict that the organic carbon fraction increase with decreasing diameter from a few % at 1 ?m over 50% at about 0.5 ?m to about 90% at 0.1 ?m, in consistency with simultaneous chemical data by Cavalli et al. (2004). The combined models of Mårtensson et al. (2003) and Ellison et al. (1999) reproduce the observed total aerosol emissions and offer an approach to model the organic sea spray fraction

Ocean Acidification: An Emerging Threat to our Marine Environment

This report aims to provide a concise overview of the present state of scientific knowledge of ocean acidification and its likely impacts on organisms and ocean ecosystems. This is particularly relevant in the context of the possible implications and ramifications of ocean acidification for Irish marine areas. Discussion on how mankind’s CO2 emissions are changing ocean chemistry; consequences of ocean acidification; ocean acidification as an emerging cause for concern; international policy drivers, strategies and necessary actions; and research and information needs are presented. Ireland’s marine location and extensive marine resources in our shelf seas, Atlantic waters and habitats of the west coast mean we are uniquely positioned to contribute to international scientific efforts to monitor and understand the impacts of ocean acidification. Monitoring and research of key biological, chemical and physical factors in these regions will allow us to determine the current status of Irish Marine waters, the rate of change in the carbonate cycle and the influence of this change on natural communities and ecosystems. The Marine Institute’s SSTI funded Sea Change programme includes a Rapid Climate Change programme. Under this, a two year collaborative project between NUI Galway and Marine Institute ‘Impacts of increased atmospheric CO2 on ocean chemistry and ecosystems’ is developing capabilities for measuring pCO2 fluxes, inorganic carbon chemistry and pH and is initiating baseline measurements of these parameters in coastal and offshore waters. This report summarises the issues and state of knowledge and communicates ongoing monitoring and research needs into acidification.Funder: Marine Institut

Stage of perinatal development regulates skeletal muscle mitochondrial biogenesis and myogenic regulatory factor genes with little impact of growth restriction or cross-fostering

Foetal growth restriction impairs skeletal muscle development and adult muscle mitochondrial biogenesis. We hypothesized that key genes involved in muscle development and mitochondrial biogenesis would be altered following uteroplacental insufficiency in rat pups, and improving postnatal nutrition by cross-fostering would ameliorate these deficits. Bilateral uterine vessel ligation (Restricted) or sham (Control) surgery was performed on day 18 of gestation. Males and females were investigated at day 20 of gestation (E20), 1 (PN1), 7 (PN7) and 35 (PN35) days postnatally. A separate cohort of Control and Restricted pups were cross-fostered onto a different Control or Restricted mother and examined at PN7. In both sexes, peroxisome proliferator-activated receptor (PPAR)-&gamma; coactivator-1&alpha; (PGC-1&alpha;), cytochrome c oxidase subunits 3 and 4 (COX III and IV) and myogenic regulatory factor 4 expression increased from late gestation to postnatal life, whereas mitochondrial transcription factor A, myogenic differentiation 1 (MyoD), myogenin and insulin-like growth factor I (IGF-I) decreased. Foetal growth restriction increased MyoD mRNA in females at PN7, whereas in males IGF-I mRNA was higher at E20 and PN1. Cross-fostering Restricted pups onto a Control mother significantly increased COX III mRNA in males and COX IV mRNA in both sexes above controls with little effect on other genes. Developmental age appears to be a major factor regulating skeletal muscle mitochondrial and developmental genes, with growth restriction and cross-fostering having only subtle effects. It therefore appears that reductions in adult mitochondrial biogenesis markers likely develop after weaning.<br /

On the representativeness of coastal aerosol studies to open ocean studies: Mace Head – a case study

A unique opportunity arose during the MAP project to compare open ocean aerosol measurements with those undertaken at the Mace Head Global Atmosphere Watch Station, a station used for decades for aerosol process research and long-term monitoring. The objective of the present study is to demonstrate that the key aerosol features and processes observed at Mace Head are characteristic of the open ocean, while acknowledging and allowing for spatial and temporal gradients. Measurements were conducted for a 5-week period at Mace Head and offshore, on the Research Vessel Celtic Explorer, in generally similar marine air masses, albeit not in connected-flow scenarios. The results of the study indicate, in terms of aerosol number size distribution, higher nucleation mode particle concentrations at Mace Head than offshore, pointing to a strong coastal source of new particles that is not representative of the open ocean. The Aitken mode exhibited a large degree of similarity, with no systematic differences between Mace Head and the open ocean, while the accumulation mode showed averagely 35% higher concentrations at Mace Head. The higher accumulation mode concentration can be attributed equally to cloud processing and to a coastal enhancement in concentration. Chemical analysis showed similar or even higher offshore concentrations for dominant species, such as nss-SO&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;-2&lt;/sup&gt;, WSOC, WIOC and MSA. Sea salt concentration differences determined a 40% higher supermicron mass at Mace Head, although this difference can be attributed to a higher wind speed at Mace Head during the comparison period. Moreover, the relative chemical composition as a function of size illustrated remarkable similarity. While differences to varying degrees were observed between offshore and coastal measurements, no convincing evidence was found of local coastal effects, apart from nucleation mode aerosol, thus confirming the integrity of previously reported marine aerosol characterisation studies at Mace Head