ORCID Profile
0000-0002-0979-0227
Current Organisations
NIWA - The National Institute of Water and Atmospheric Research Ltd.
,
National Institute of Water and Atmospheric Research Wellington
Does something not look right? The information on this page has been harvested from data sources that may not be up to date. We continue to work with information providers to improve coverage and quality. To report an issue, use the Feedback Form.
Publisher: Copernicus GmbH
Date: 16-11-2017
DOI: 10.5194/ACP-17-13645-2017
Abstract: Abstract. Establishing the relationship between marine boundary layer (MBL) aerosols and surface water biogeochemistry is required to understand aerosol and cloud production processes over the remote ocean and represent them more accurately in earth system models and global climate projections. This was addressed by the SOAP (Surface Ocean Aerosol Production) c aign, which examined air–sea interaction over biologically productive frontal waters east of New Zealand. This overview details the objectives, regional context, s ling strategy and provisional findings of a pilot study, PreSOAP, in austral summer 2011 and the following SOAP voyage in late austral summer 2012. Both voyages characterized surface water and MBL composition in three phytoplankton blooms of differing species composition and biogeochemistry, with significant regional correlation observed between chlorophyll a and DMSsw. Surface seawater dimethylsulfide (DMSsw) and associated air–sea DMS flux showed spatial variation during the SOAP voyage, with maxima of 25 nmol L−1 and 100 µmol m−2 d−1, respectively, recorded in a dinoflagellate bloom. Inclusion of SOAP data in a regional DMSsw compilation indicates that the current climatological mean is an underestimate for this region of the southwest Pacific. Estimation of the DMS gas transfer velocity (kDMS) by independent techniques of eddy covariance and gradient flux showed good agreement, although both exhibited periodic deviations from model estimates. Flux anomalies were related to surface warming and sea surface microlayer enrichment and also reflected the heterogeneous distribution of DMSsw and the associated flux footprint. Other aerosol precursors measured included the halides and various volatile organic carbon compounds, with first measurements of the short-lived gases glyoxal and methylglyoxal in pristine Southern Ocean marine air indicating an unidentified local source. The application of a real-time clean sector, contaminant markers and a common aerosol inlet facilitated multi-sensor measurement of uncontaminated air. Aerosol characterization identified variable Aitken mode and consistent submicron-sized accumulation and coarse modes. Submicron aerosol mass was dominated by secondary particles containing ammonium sulfate/bisulfate under light winds, with an increase in sea salt under higher wind speeds. MBL measurements and chamber experiments identified a significant organic component in primary and secondary aerosols. Comparison of SOAP aerosol number and size distributions reveals an underprediction in GLOMAP (GLObal Model of Aerosol Processes)-mode aerosol number in clean marine air masses, suggesting a missing marine aerosol source in the model. The SOAP data will be further examined for evidence of nucleation events and also to identify relationships between MBL composition and surface ocean biogeochemistry that may provide potential proxies for aerosol precursors and production.
Publisher: Copernicus GmbH
Date: 25-08-2014
DOI: 10.5194/ACPD-14-21659-2014
Abstract: Abstract. Dicarbonyls glyoxal and methylglyoxal have been measured with 2,4-dinitrophenylhydrazine (2,4-DNPH) cartridges and high performance liquid chromatography (HPLC), optimised for dicarbonyl detection, in clean marine air over the temperate Southern Hemisphere (SH) oceans. Measurements of a range of dicarbonyl precursors (volatile organic compounds, VOCs) were made in parallel. These are the first in situ measurements of glyoxal and methylglyoxal over the remote temperate oceans. Six 24 h s les were collected in late summer (February–March) over the Chatham Rise in the South West Pacific Ocean during the Surface Ocean Aerosol Production (SOAP) voyage in 2012, while 34 24 h s les were collected at Cape Grim Baseline Air Pollution Station in late winter (August–September) 2011. Average glyoxal mixing ratios in clean marine air were 7 ppt at Cape Grim, and 24 ppt over Chatham Rise. Average methylglyoxal mixing ratios in clean marine air were 28 ppt at Cape Grim and 12 ppt over Chatham Rise. The mixing ratios of glyoxal at Cape Grim are the lowest observed over the remote oceans, while mixing ratios over Chatham Rise are in good agreement with other temperate and tropical observations, including concurrent MAX-DOAS observations. Methylglyoxal mixing ratios at both sites are comparable to the only other marine methylglyoxal observations available over the tropical Northern Hemisphere (NH) ocean. Ratios of glyoxal : methylglyoxal 1 over Chatham Rise but 1 at Cape Grim, suggesting different formation and/or loss processes or rates dominate at each site. Dicarbonyl precursor VOCs, including isoprene and monoterpenes, are used to calculate an upper estimate yield of glyoxal and methylglyoxal in the remote marine boundary layer and explain at most 1–3 ppt of dicarbonyls observed, corresponding to 11 and 17% of the observed glyoxal and 28 and 10% of the methylglyoxal at Chatham Rise and Cape Grim, respectively, highlighting a significant but as yet unknown production mechanism. Glyoxal surface observations from both sites were converted to vertical columns and compared to average vertical column densities (VCDs) from GOME-2 satellite retrievals. Both satellite columns and in situ observations are higher in summer than winter, however satellite vertical column densities exceeded the surface observations by more than 1.5 × 1014 molecules cm−2 at both sites. This discrepancy may be due to the incorrect assumption that all glyoxal observed by satellite is within the boundary layer, or may be due to challenges retrieving low VCDs of glyoxal over the oceans due to interferences by liquid water absorption, or use of an inappropriate normalisation reference value in the retrieval algorithm. This study provides much needed data to verify the presence of these short lived gases over the remote ocean and provide further evidence of an as yet unidentified source of both glyoxal and also methylglyoxal over the remote oceans.
Publisher: American Meteorological Society
Date: 04-2021
Abstract: Weather and climate models are challenged by uncertainties and biases in simulating Southern Ocean (SO) radiative fluxes that trace to a poor understanding of cloud, aerosol, precipitation, and radiative processes, and their interactions. Projects between 2016 and 2018 used in situ probes, radar, lidar, and other instruments to make comprehensive measurements of thermodynamics, surface radiation, cloud, precipitation, aerosol, cloud condensation nuclei (CCN), and ice nucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase clouds common to this pristine environment. Data including soundings were collected from the NSF–NCAR G-V aircraft flying north–south gradients south of Tasmania, at Macquarie Island, and on the R/V Investigator and RSV Aurora Australis . Synergistically these data characterize boundary layer and free troposphere environmental properties, and represent the most comprehensive data of this type available south of the oceanic polar front, in the cold sector of SO cyclones, and across seasons. Results show largely pristine environments with numerous small and few large aerosols above cloud, suggesting new particle formation and limited long-range transport from continents, high variability in CCN and cloud droplet concentrations, and ubiquitous supercooled water in thin, multilayered clouds, often with small-scale generating cells near cloud top. These observations demonstrate how cloud properties depend on aerosols while highlighting the importance of dynamics and turbulence that likely drive heterogeneity of cloud phase. Satellite retrievals confirmed low clouds were responsible for radiation biases. The combination of models and observations is examining how aerosols and meteorology couple to control SO water and energy budgets.
Publisher: Copernicus GmbH
Date: 04-03-2021
DOI: 10.5194/EGUSPHERE-EGU21-8110
Abstract: & & Even though oceans cover over 70% of the Earth& #8217 s surface, the ways in which oceans interact with climate are not fully known. Marine micro-organisms such as phytoplankton can play an important role in regulating climate by releasing different chemical species into air. In air these chemical species can react and form new aerosol particles. If grown to large enough sizes, aerosols can influence climate by acting as cloud condensation nuclei which influence the formation and properties of clouds. Even though a connection of marine biology and climate through aerosol formation was first proposed already over 30 years ago, the processes related to this connection are still uncertain.& & & & To unravel how seawater properties affect aerosol formation and to identify which chemical species are responsible for aerosol formation, we built two Air-Sea-Interaction Tanks (ASIT) that isolate 1000 l of seawater and 1000 l of air directly above the water. The used seawater was collected from different locations during a ship c aign on board the R/V Tangaroa in the South West Pacific Ocean, close to Chatham Rise, east of New Zealand. Seawater from one location was kept in the tanks for 2-3 days and then changed. By using seawater collected from different locations, we could obtain water with different biological populations. To monitor the seawater, we took daily s les to determine its chemical and biological properties.& & & & The air in the tanks was continuously flushed with particle filtered air. This way the air had on average 40 min to interact with the seawater surface before being s led. Our air s ling was continuous and consisted of aerosol and air chemistry measurements. The instrumentation included measurements of aerosol number concentration from 1 to 500 nm and& chemical species ranging from ozone and sulphur dioxide to volatile organic compounds and chemical composition of molecular clusters.& & & & Joining the seawater and atmospheric data together can give us an idea of what chemical species are emitted from the water into the atmosphere and whether these species can form new aerosol particles. Our preliminary results show a small number of particles in the freshly nucleated size range of 1-3 nm in the ASIT headspaces, indicating that new aerosol particles can form in the ASIT headspaces. In this presentation, we will also explore which chemical species could be responsible for aerosol formation and which plankton groups could be related to the emissions of these species. Combining these results with ambient data and modelling work can shed light on how important new particle formation from marine sources is for climate.& & & & Acknowledgements: Sea2Cloud project is funded by European Research Council (ERC) under the European Union& #8217 s Horizon 2020 research and innovation programme (Grant agreement No. 771369).& &
Publisher: Copernicus GmbH
Date: 20-06-2017
DOI: 10.5194/ACP-2017-535
Abstract: Abstract. Establishing the relationship between marine boundary layer (MBL) aerosols and surface water biogeochemistry over the remote ocean is required to understand aerosol and cloud production processes, and also represent them accurately in Earth System Models and global climate projections. This was addressed in the SOAP (Surface Ocean Aerosol Production) c aign, which examined air-sea interaction over biologically-productive frontal waters east of New Zealand. This overview details the objectives, regional context, s ling strategy, and provisional findings of a pilot study, PreSOAP, in austral summer 2011, and the following SOAP voyage in late austral summer 2012. Both voyages characterised surface water and MBL composition in three phytoplankton blooms of differing species composition and biogeochemistry, with significant regional correlation observed between chlorophyll-a and DMSsw. Surface seawater dimethylsulfide (DMSsw) and associated air-sea DMS flux showed spatial variation during the SOAP voyage, with maxima of 25 nmol L−1 and 100 µmol m−2 d−1, respectively, recorded in a dinoflagellate bloom. Inclusion of SOAP data in a regional DMSsw compilation confirmed that the current climatological mean is an underestimate for this region of the South-west Pacific. Estimation of the DMS gas transfer velocity (kDMS) by independent techniques of eddy covariance and gradient flux showed good agreement, although both exhibited periodic deviations from model estimates. Flux anomalies were related to surface warming and sea surface microlayer enrichment, and also reflected the heterogeneous distribution of DMSsw and the associated flux footprint. Other aerosol precursors measured included the halides and various volatile organic carbon compounds, with the first measurements of the short-lived gases glyoxal and methylglyoxal in pristine Southern Ocean marine air indicating an unidentified local source. The application of a real-time clean-sector, contaminant markers, and a common aerosol inlet facilitated multi-sensor measurement of uncontaminated air. Aerosol characterisation identified variable Aitken mode, and consistent sub-micron sized accumulation and coarse modes. Sub-micron aerosol mass was dominated by secondary particles containing ammonium sulfate/bisulfate under light winds, with an increase in sea-salt under higher wind-speeds. MBL measurements and chamber experiments identified a significant organic component in primary and secondary aerosols. Comparison of SOAP aerosol number and size distributions reveals an underprediction in GLOMAP-mode aerosol number in clean marine air masses, suggesting a missing marine aerosol source in the model. The SOAP data will be further examined for evidence of nucleation events, and also for relationships between MBL composition and surface ocean biogeochemistry with the aim of identifying potential proxies for aerosol precursors and production.
Publisher: University of California Press
Date: 2022
DOI: 10.1525/ELEMENTA.2021.00050
Abstract: This commentary paper from the recently formed International Global Atmospheric Chemistry (IGAC) Southern Hemisphere Working Group outlines key issues in atmospheric composition research that particularly impact the Southern Hemisphere. In this article, we present a broad overview of many of the challenges for understanding atmospheric chemistry in the Southern Hemisphere, before focusing in on the most significant factors that differentiate it from the Northern Hemisphere. We present sections on the importance of biogenic emissions and fires in the Southern Hemisphere, showing that these emissions often dominate over anthropogenic emissions in many regions. We then describe how these and other factors influence air quality in different parts of the Southern Hemisphere. Finally, we describe the key role of the Southern Ocean in influencing atmospheric chemistry and conclude with a description of the aims and scope of the newly formed IGAC Southern Hemisphere Working Group.
Publisher: Springer Science and Business Media LLC
Date: 10-2000
DOI: 10.1038/35037500
Abstract: Changes in iron supply to oceanic plankton are thought to have a significant effect on concentrations of atmospheric carbon dioxide by altering rates of carbon sequestration, a theory known as the 'iron hypothesis'. For this reason, it is important to understand the response of pelagic biota to increased iron supply. Here we report the results of a mesoscale iron fertilization experiment in the polar Southern Ocean, where the potential to sequester iron-elevated algal carbon is probably greatest. Increased iron supply led to elevated phytoplankton biomass and rates of photosynthesis in surface waters, causing a large drawdown of carbon dioxide and macronutrients, and elevated dimethyl sulphide levels after 13 days. This drawdown was mostly due to the proliferation of diatom stocks. But downward export of biogenic carbon was not increased. Moreover, satellite observations of this massive bloom 30 days later, suggest that a sufficient proportion of the added iron was retained in surface waters. Our findings demonstrate that iron supply controls phytoplankton growth and community composition during summer in these polar Southern Ocean waters, but the fate of algal carbon remains unknown and depends on the interplay between the processes controlling export, remineralisation and timescales of water mass subduction.
Publisher: Copernicus GmbH
Date: 04-03-2021
DOI: 10.5194/EGUSPHERE-EGU21-14323
Abstract: & & Atmospheric observations of CO& sub& & /sub& and other greenhouse gases have been widely used to constrain estimates of terrestrial and oceanic CO& sub& & /sub& fluxes through atmospheric inverse modelling. Yet, applying these methods at national scale to verify and improve the National Inventory Report (NIR) and support the Paris agreement remains at the frontier of CO& sub& & /sub& science.& & & & We use inverse modelling to estimate New Zealand& #8217 s carbon uptake and emissions using atmospheric measurements and model. This effort is part of a five year CarbonWatch-NZ research programme, which aims to develop a complete top-down picture of New Zealand's carbon balance using national inverse modelling and targeted studies of New Zealand& #8217 s forest, grassland and urban environments. In addition to quantifying New Zealand& #8217 s carbon emissions on a national scale, we also focus on identifying the prevailing processes driving CO& sub& & /sub& changes in New Zealand to support climate mitigation.& & & & In an initial study based on the inversion system used in CarbonWatch-NZ, a significantly stronger (30-60 %) sink was found relative to the NIR (Steink et al., 2017), suggesting a strong CO& sub& & /sub& uptake in Fiordland, a region covered by indigenous temperate rainforest in New Zealand's South Island. Here, we present new results of CarbonWatch-NZ by expanding the studied time period from 2011-2013 to 2020, expanding our atmospheric observing network from two (Baring Head, 41.41& #176 S, 174.87& #176 E and Lauder, 38.33& #176 S, 176.38& #176 E) to a total of eleven in situ greenhouse gas measurement sites and improving our atmospheric model resolution by roughly a factor of ten (NAME model, 1.5 km).& & & & Our new results suggest that the strong sink observed in 2011-2013 did not diminish, but for recent years we have found an even stronger sink than for before. Additional measurements collected in the Fiordland region (i.e., mixing ratios, CO& sub& & /sub& isotopes, carbonyl sulphide) also suggest a stronger CO& sub& & /sub& uptake, supporting our inversion results. Both the measurements and inversion results show that the CO& sub& & /sub& uptake does not seem to shut down completely during winter time, suggesting that there might be something about this ecosystem that we do not yet understand. This winter uptake signal is also present in independent data collected in and around New Zealand as part of the ATom c aigns (Atmospheric Tomography Mission). Implementing observations from an additional site in the North Island (Maunga Kakaramea, 45.034& #176 S, 169.68& #176 E) has increased the strength of the sink, pointing to additional strong sink region at the top of the North Island.& & & & & & & & & References& & & & Kay Steink , Sara E. Mikaloff Fletcher, Gordon Brailsford, Dan Smale, Stuart Moore, Elizabeth D. Keller, W. Troy Baisden, Hitoshi Mukai and Britton B. Stephens, Atmospheric CO2 observations and models suggest strong carbon uptake by forests in New Zealand, Atmospheric Chemistry and Physics, 2017.& &
Publisher: Copernicus GmbH
Date: 05-04-2019
DOI: 10.5194/ACP-2019-201
Abstract: Abstract. Southern Ocean (SO) shortwave (SW) radiation biases are a common problem in contemporary general circulation models (GCMs), with most models exhibiting a tendency to absorb too much incoming SW radiation. These biases have been attributed to deficiencies in the representation of clouds during the austral summer months, either due to cloud cover or cloud optical thickness being too low. The problem has been the focus of many studies, most of which utilised satellite datasets for model evaluation. We use multi-year ship based observations and the CERES spaceborne radiation budget measurements to contrast cloud representation and SW radiation in the atmospheric component Global Atmosphere (GA) version 7.0 and 7.1 of the HadGEM3 GCM and the MERRA-2 reanalysis. We find that MERRA-2 is biased in the opposite direction to GA (reflects too much SW radiation). In addition, MERRA-2 performs better in terms of absolute SW bias than nudged runs of GA7.0 and GA7.1 in the 60–70° S latitude band. GA7.1 reduces the SO SW radiation biases relative to GA7.0, but significant errors remain at up to 20 W m−2 between 60 and 70° S in the austral summer months. Using ship-based ceilometer observations, we find low cloud below 2 km to be predominant in the Ross Sea and the Indian Ocean sector of the SO. Utilising a novel surface lidar simulator developed for this study, derived from an existing COSP-ACTSIM spaceborne lidar simulator, we find that GA7.0 and MERRA-2 both underestimate low cloud occurrence relative to the ship observations by 18–25 % on average, though the cloud cover in MERRA-2 is closer to observations by about 7 %. Based on radiosonde observations, we also find the low cloud to be strongly linked to boundary-layer atmospheric stability and the sea surface temperature. GA7.0 and MERRA-2 agree well with observations in terms of boundary-layer stability, suggesting that subgrid-scale parametrisations do not generate enough cloud in response to the thermodynamic profile of the atmosphere and the surface temperature. Our analysis shows that MERRA-2 has a much greater proportion of cloud liquid water in the SO in January than GA7.0, a likely key contributor to the difference in SW radiation. We show that boundary-layer stability and relative humidity fields are very similar in GA7.0 and MERRA-2, and unlikely to be the cause of the different cloud representation, suggesting that subgrid-scale parametrisations are responsible for the difference between the models.
Publisher: Copernicus GmbH
Date: 22-06-2022
DOI: 10.5194/EGUSPHERE-2022-499
Abstract: Abstract. Elevated dimethyl sulfide (DMS) concentrations in the sea surface microlayer (SML) have been previously related to DMS air-sea flux anomalies in the South West Pacific. To further address this, DMS, its precursor dimethylsulfoniopropionate (DMSP), and ancillary variables were s led in the SML and also subsurface water at 0.5 m depth (SSW) in different water masses east of New Zealand. Despite high phytoplankton biomass at certain stations significant chlorophyll a and DMSP enrichments were only apparent at one of six stations, with the DMSP enrichment factor (EF) ranging from 0.81 to 1.25. DMS in the SML was determined using a novel gas-permeable tube technique which measured consistently higher concentrations than with the traditional glass plate technique however, DMS enrichment was also present at only one station, with the EF ranging from 0.40 to 1.22. SML DMSP and DMS were influenced by phytoplankton community composition, with correlations with dinoflagellate and Gymnodinium biomass, respectively. DMSP and DMS concentrations were also correlated between the SML and SSW, with the difference in ratio attributable to greater DMS loss to the atmosphere from the SML. DMS in the SML did not significantly influence regional DMS emissions, with the calculated air-sea DMS flux of 1.0 to 11.0 µmol m-2 d-1 consistent with climatological estimates for the region. These results extend previous regional observations that DMS is associated with dinoflagellate abundance but indicate that additional factors are required for significant enrichment in the SML.
Publisher: Copernicus GmbH
Date: 12-01-2015
Abstract: Abstract. The dicarbonyls glyoxal and methylglyoxal have been measured with 2,4-dinitrophenylhydrazine (2,4-DNPH) cartridges and high-performance liquid chromatography (HPLC), optimised for dicarbonyl detection, in clean marine air over the temperate Southern Hemisphere (SH) oceans. Measurements of a range of dicarbonyl precursors (volatile organic compounds, VOCs) were made in parallel. These are the first in situ measurements of glyoxal and methylglyoxal over the remote temperate oceans. Six 24 h s les were collected in summer (February–March) over the Chatham Rise in the south-west Pacific Ocean during the Surface Ocean Aerosol Production (SOAP) voyage in 2012, while 34 24 h s les were collected at Cape Grim Baseline Air Pollution Station in the late winter (August–September) of 2011. Average glyoxal mixing ratios in clean marine air were 7 ppt at Cape Grim and 23 ppt over Chatham Rise. Average methylglyoxal mixing ratios in clean marine air were 28 ppt at Cape Grim and 10 ppt over Chatham Rise. The mixing ratios of glyoxal at Cape Grim are the lowest observed over the remote oceans, while mixing ratios over Chatham Rise are in good agreement with other temperate and tropical observations, including concurrent Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations. Methylglyoxal mixing ratios at both sites are comparable to the only other marine methylglyoxal observations available over the tropical Northern Hemisphere (NH) ocean. Ratios of glyoxal : methylglyoxal 1 over Chatham Rise but 1 at Cape Grim suggest that a different formation and/or loss processes or rates dominate at each site. Dicarbonyl precursor VOCs, including isoprene and monoterpenes, are used to calculate an upper-estimate yield of glyoxal and methylglyoxal in the remote marine boundary layer and explain at most 1–3 ppt of dicarbonyls observed, corresponding to 10% and 17% of the observed glyoxal and 29 and 10% of the methylglyoxal at Chatham Rise and Cape Grim, respectively, highlighting a significant but as yet unknown production mechanism. Surface-level glyoxal observations from both sites were converted to vertical columns and compared to average vertical column densities (VCDs) from GOME-2 satellite retrievals. Both satellite columns and in situ observations are higher in summer than winter however, satellite vertical column densities exceeded the surface observations by more than 1.5 × 1014 molecules cm−2 at both sites. This discrepancy may be due to the incorrect assumption that all glyoxal observed by satellite is within the boundary layer, or it may be due to challenges retrieving low VCDs of glyoxal over the oceans due to interferences by liquid water absorption or the use of an inappropriate normalisation reference value in the retrieval algorithm. This study provides much-needed data to verify the presence of these short-lived gases over the remote ocean and provide further evidence of an as yet unidentified source of both glyoxal and also methylglyoxal over the remote oceans.
Publisher: Springer International Publishing
Date: 2021
Publisher: CSIRO Publishing
Date: 2007
DOI: 10.1071/EN07011
Abstract: Environmental context. The marine environment covers 71% of the Earth’s surface, and accounts for most of the planet’s cloud cover. Water droplets in these clouds all form on pre-existing marine aerosol particles. The number, size and composition of these particles determine the cloud droplet size and consequently, the cloud’s light scattering and precipitation behaviour. Marine aerosols, therefore, have a major influence on the planet’s radiation balance and climate. The origin of marine aerosols is still not completely resolved. The newly developed VH-TDMA technique has been applied to marine aerosols that come from the Southern Ocean. The technique enabled new insights into the composition and structure of these aerosols. It has been found that organic matter constitutes 20–40% of these particles, which suppresses their hygroscopic growth. Abstract. Simultaneous measurement of particle hygroscopic and volatile properties was performed using a VH-TDMA on both Aitken and accumulation mode particles. In addition, deliquescence measurements at different thermodenuder temperatures were also performed. The measurements were part of the P2P c aign which took place in February 2006 at the Cape Grim monitoring station in Tasmania, Australia. During baseline conditions, there was often a volatilisation step that occurred below 125°C in the volatility scans, where up to 25% of the volume is lost. Analysis of the changes in growth as this took place indicates that different substances are responsible for this volatilisation on different days – ammonium nitrate, sulfuric acid, or a volatile non-hygroscopic organic. The major volatilisation in all cases occurred in the temperature range ~140–200°C, which is taken to indicate the presence of ammonium sulfate or ammonium bisulfate. A degree of growth suppression is generally evident before this volatilisation, which indicates that a non-hygroscopic material with a similar volatility to ammonium sulfate/bisulfate may be present, which cannot be distinguished in the volatility scans. Organic matter was typically present at around ~20–40% for these particles. When Aitken and accumulation mode particles were measured on the same day, it was found that the organic content of the smaller particles tended to be higher than the larger particles by roughly 20 percentage points.
Publisher: Copernicus GmbH
Date: 20-06-2017
Publisher: Copernicus GmbH
Date: 16-03-2020
Abstract: Abstract. Atmospheric methanethiol (MeSHa), dimethyl sulfide (DMSa) and acetone (acetonea) were measured over biologically productive frontal waters in the remote southwest Pacific Ocean in summertime 2012 during the Surface Ocean Aerosol Production (SOAP) voyage. MeSHa mixing ratios varied from below the detection limit ( 10 ppt) up to 65 ppt and were 3 %–36 % of parallel DMSa mixing ratios. MeSHa and DMSa were correlated over the voyage (R2=0.3, slope = 0.07) with a stronger correlation over a coccolithophore-dominated phytoplankton bloom (R2=0.5, slope 0.13). The diurnal cycle for MeSHa shows similar behaviour to DMSa with mixing ratios varying by a factor of ∼ 2 according to time of day with the minimum levels of both MeSHa and DMSa occurring at around 16:00 LT (local time, all times in this paper are in local time). A positive flux of MeSH out of the ocean was calculated for three different nights and ranged from 3.5 to 5.8 µmol m−2 d−1, corresponding to 14 %–24 % of the DMS flux (MeSH ∕ (MeSH + DMS)). Spearman rank correlations with ocean biogeochemical parameters showed a moderate-to-strong positive, highly significant relationship between both MeSHa and DMSa with seawater DMS (DMSsw) and a moderate correlation with total dimethylsulfoniopropionate (total DMSP). A positive correlation of acetonea with water temperature and negative correlation with nutrient concentrations are consistent with reports of acetone production in warmer subtropical waters. Positive correlations of acetonea with cryptophyte and eukaryotic phytoplankton numbers, and high-molecular-weight sugars and chromophoric dissolved organic matter (CDOM), suggest an organic source. This work points to a significant ocean source of MeSH, highlighting the need for further studies into the distribution and fate of MeSH, and it suggests links between atmospheric acetone levels and biogeochemistry over the mid-latitude ocean. In addition, an intercalibration of DMSa at ambient levels using three independently calibrated instruments showed ∼ 15 %–25 % higher mixing ratios from an atmospheric pressure ionisation chemical ionisation mass spectrometer (mesoCIMS) compared to a gas chromatograph with a sulfur chemiluminescence detector (GC-SCD) and proton transfer reaction mass spectrometer (PTR-MS). Some differences were attributed to the DMSa gradient above the sea surface and differing approaches of integrated versus discrete measurements. Remaining discrepancies were likely due to different calibration scales, suggesting that further investigation of the stability and/or absolute calibration of DMS standards used at sea is warranted.
Publisher: Copernicus GmbH
Date: 16-10-2019
DOI: 10.5194/ACP-2019-856
Abstract: Abstract. Atmospheric methanethiol (MeSHa), dimethyl sulfide (DMSa) and acetone (acetonea) were measured over biologically productive frontal waters in the remote South West Pacific Ocean in summertime 2012 during the Surface Ocean Aerosol Production (SOAP) voyage. MeSHa mixing ratios varied from below detection limit (
Publisher: Copernicus GmbH
Date: 21-03-2011
Abstract: Abstract. The Maritime Aerosol Network (MAN) has been collecting data over the oceans since November 2006. Over 80 cruises were completed through early 2010 with deployments continuing. Measurement areas included various parts of the Atlantic Ocean, the Northern and Southern Pacific Ocean, the South Indian Ocean, the Southern Ocean, the Arctic Ocean and inland seas. MAN deploys Microtops hand-held sunphotometers and utilizes a calibration procedure and data processing traceable to AERONET. Data collection included areas that previously had no aerosol optical depth (AOD) coverage at all, particularly vast areas of the Southern Ocean. The MAN data archive provides a valuable resource for aerosol studies in maritime environments. In the current paper we present results of AOD measurements over the oceans, and make a comparison with satellite AOD retrievals and model simulations.
Publisher: Copernicus GmbH
Date: 22-06-2022
Publisher: Copernicus GmbH
Date: 05-06-2020
Abstract: Abstract. Southern Ocean (SO) shortwave (SW) radiation biases are a common problem in contemporary general circulation models (GCMs), with most models exhibiting a tendency to absorb too much incoming SW radiation. These biases have been attributed to deficiencies in the representation of clouds during the austral summer months, either due to cloud cover or cloud albedo being too low. The problem has been the focus of many studies, most of which utilised satellite datasets for model evaluation. We use multi-year ship-based observations and the CERES spaceborne radiation budget measurements to contrast cloud representation and SW radiation in the atmospheric component Global Atmosphere (GA) version 7.1 of the HadGEM3 GCM and the MERRA-2 reanalysis. We find that the prevailing bias is negative in GA7.1 and positive in MERRA-2. GA7.1 performs better than MERRA-2 in terms of absolute SW bias. Significant errors of up to 21 W m−2 (GA7.1) and 39 W m−2 (MERRA-2) are present in both models in the austral summer. Using ship-based ceilometer observations, we find low cloud below 2 km to be predominant in the Ross Sea and the Indian Ocean sectors of the SO. Utilising a novel surface lidar simulator developed for this study, derived from an existing Cloud Feedback Model Intercomparison Project (CFMIP) Observation Simulator Package (COSP) – active remote sensing simulator (ACTSIM) spaceborne lidar simulator, we find that GA7.1 and MERRA-2 both underestimate low cloud and fog occurrence relative to the ship observations on average by 4 %–9 % (GA7.1) and 18 % (MERRA-2). Based on radiosonde observations, we also find the low cloud to be strongly linked to boundary layer atmospheric stability and the sea surface temperature. GA7.1 and MERRA-2 do not represent the observed relationship between boundary layer stability and clouds well. We find that MERRA-2 has a much greater proportion of cloud liquid water in the SO in austral summer than GA7.1, a likely key contributor to the difference in the SW radiation bias. Our results suggest that subgrid-scale processes (cloud and boundary layer parameterisations) are responsible for the bias and that in GA7.1 a major part of the SW radiation bias can be explained by cloud cover underestimation, relative to underestimation of cloud albedo.
Publisher: Copernicus GmbH
Date: 19-09-2019
DOI: 10.5194/ACP-2019-797
Abstract: Abstract. The aerosol driven radiative effects on marine low-level cloud represent a large uncertainty in climate simulations, in particular over the Southern Ocean, which is also an important region for sea spray aerosol production. Observations of sea spray aerosol organic enrichment and the resulting impact on water uptake over the remote southern hemisphere are scarce, and are therefore the region is under-represented in existing parameterisations. The Surface Ocean Aerosol Production (SOAP) voyage was a 23 day voyage which s led three phytoplankton blooms in the highly productive water of the Chatham Rise, east of New Zealand. In this study we examined the enrichment of organics to nascent sea spray aerosol and the modifications to sea spray aerosol water uptake using in-situ chamber measurements of seawater s les taken during the SOAP voyage. Primary marine organics contributed up to 23 % of the sea spray mass for particles with diameter less than approximately 1 μm, and up to 87 % of the particle volume in the Aitken mode. The composition of the organic fraction was consistent throughout the voyage and was largely comprised of a polysaccharide-like component, characterised by very low alkane to hydroxyl concentration ratios of approximately 0.1–0.2. The enrichment of organics was compared to the output from the chlorophyll-a based sea spray aerosol parameterisation suggested by Gantt et al. (2011) and the OCEANFILMS models. OCEANFILMS improved on the representation of the organic fraction predicted using chlorophyll-a, in particular when the co-adsoprtion of polysaccharides was included, however the model still under predicted the proportion of polysaccharides by an average of 33 %. Nascent sea spray aerosol hygroscopic growth factors averaged 1.93 ± 0.08, and did not decrease with increasing sea spray aerosol organic fractions. The observed hygroscopicity was greater than expected from the assumption of full solubility, particularly during the most productive phytoplankton bloom (B1), during which organic fractions were greater than approximately 0.4. The water uptake behaviour observed in this study is consistent with that observed for other measurements of phytoplankton blooms, and was attributed to the surface partitioning of the organic components which leads to a decrease in particle surface tension and an increase in hygroscopicity. The compressed film model was used to estimate the influence of surface partitioning and the error in the modelled hygroscopicity was low only when the entire organic fraction was available to partition to the particle surface. The modelled sea spray aerosol hygroscopicity at high organic fractions was underestimated when only a portion of the organic component was available to be partitioned to the surface. The findings from the SOAP voyage highlight the influence of biologically-sourced organics on sea spray aerosol composition, these data improve the capacity to parameterise sea spray aerosol organic enrichment and water uptake.
Publisher: Elsevier BV
Date: 03-2011
Publisher: Copernicus GmbH
Date: 15-05-2023
DOI: 10.5194/EGUSPHERE-EGU23-8058
Abstract: Understanding ocean-cloud interactions and their effect on climate requires that atmospheric new particle formation is characterized. Yet, the process of particle formation from marine biogenic gaz-phase emissions has not been evidenced in the open ocean lower atmosphere, partly due to the naturally low concentrations of these particles in remote oceanic places. Here we show, using new ship-borne air-sea interface enclosures, that new particles are formed in relation to marine micro-biology present in the seawater. The chemical analysis of newly formed clusters with API-ToF-MS shows unexpected results, implicating nucleating coumpounds and pathways that are usually not taken into account in nucleation processes.
Publisher: Copernicus GmbH
Date: 19-09-2019
Publisher: Copernicus GmbH
Date: 09-07-2020
Abstract: Abstract. The aerosol-driven radiative effects on marine low-level cloud represent a large uncertainty in climate simulations, in particular over the Southern Ocean, which is also an important region for sea spray aerosol production. Observations of sea spray aerosol organic enrichment and the resulting impact on water uptake over the remote Southern Hemisphere are scarce, and therefore the region is under-represented in existing parameterisations. The Surface Ocean Aerosol Production (SOAP) voyage was a 23 d voyage which s led three phytoplankton blooms in the highly productive water of the Chatham Rise, east of New Zealand. In this study we examined the enrichment of organics to nascent sea spray aerosol and the modifications to sea spray aerosol water uptake using in situ chamber measurements of seawater s les taken during the SOAP voyage. Primary marine organics contributed up to 23 % of the sea spray mass for particles with diameter less than approximately 1 µm and up to 79 % of the particle volume for 50 nm diameter sea spray. The composition of the submicron organic fraction was consistent throughout the voyage and was largely composed of a polysaccharide-like component, characterised by very low alkane-to-hydroxyl-concentration ratios of approximately 0.1–0.2. The enrichment of organics was compared to the output from the chlorophyll-a-based sea spray aerosol parameterisation suggested by Gantt et al. (2011) and the OCEANFILMS (Organic Compounds from Ecosystems to Aerosols: Natural Films and Interfaces via Langmuir Molecular Surfactants) models. OCEANFILMS improved on the representation of the organic fraction predicted using chlorophyll a, in particular when the co-adsorption of polysaccharides was included however, the model still under-predicted the proportion of polysaccharides by an average of 33 %. Nascent 50 nm diameter sea spray aerosol hygroscopic growth factors measured at 90 % relative humidity averaged 1.93±0.08 and did not decrease with increasing sea spray aerosol organic fractions. The observed hygroscopicity was greater than expected from the assumption of full solubility, particularly during the most productive phytoplankton bloom (B1), during which organic fractions were greater than approximately 0.4. The water uptake behaviour observed in this study is consistent with that observed for other measurements of phytoplankton blooms and can be partially attributed to the presence of sea salt hydrates, which lowers the sea spray aerosol hygroscopicity when the organic enrichment is low. The inclusion of surface tension effects only marginally improved the modelled hygroscopicity, and a significant discrepancy between the observed and modelled hygroscopicity at high organic volume fractions remained. The findings from the SOAP voyage highlight the influence of biologically sourced organics on sea spray aerosol composition these data improve the capacity to parameterise sea spray aerosol organic enrichment and water uptake.
Publisher: CSIRO Publishing
Date: 2007
DOI: 10.1071/EN07041
Abstract: Environmental context. Understanding the role of clouds in assessing the impact of climate change is a challenging issue. It is thought that plankton and seaweed contribute to the formation of clouds by emitting gases that lead to the particle production necessary for cloud formation. Macroalgae (kelp) at Mace Head, Ireland, produce large quantities of iodine when exposed to sunlight at low tide and this iodine results in the rapid production of particles. Cape Grim, Tasmania, also has large colonies of kelp and the role of Bull Kelp (Durvillaea potatorum) in particle production was assessed. Abstract. Iodine emissions from coastal macroalgae have been found to be important initiators for nucleation events at Mace Head, Ireland. The source of this iodine is the large beds of the brown kelp Laminaria digitata, which are significantly exposed at low tide. On the coast around Cape Grim, Tasmania, there are beds of the brown kelp Durvillaea potatrum. The Precursors to Particles 2006 (P2P 2006) c aign at the Cape Grim Baseline Air Pollution Station in late summer (February) 2006 focused on the role of this local kelp in providing precursor gases to particle formation. Durvillaea potatorum does not produce iodated precursor gases at the levels observed at Mace Head. IO was measured at 0.5 ± 0.3 ppt, while OIO was below detection limits (9 ppt). The dominant atmospheric iodated species was methyl iodide and the average concentration measured at the Cape Grim Station was 1.5 ± 0.3 pptv in baseline conditions, but showed significant variation in discrete s les collected immediately above the ocean surface. Nucleation events were not detected at the Cape Grim Station, except for one period where the plume of a local bushfire interacted with air of marine origin. The passage of four fronts did not result in nucleation bursts and measurements on the beach 94 m below the Cape Grim Station suggested that Durvillaea potatorum was only a weak source of new particles.
Publisher: Elsevier BV
Date: 03-2011
Publisher: MDPI AG
Date: 09-04-2020
DOI: 10.3390/JMSE8040268
Abstract: Surface dissolved dimethylsulfide (DMS) and depth-integrated dimethylsulfoniopropionate (DMSP) measurements were made from March to April 2004 during the SOLAS Air–Sea Gas Exchange Experiment (SAGE), a multiple iron enrichment experiment in subantarctic waters SE of New Zealand. During the first two iron enrichments, chl a and DMS production were constrained, but during the third enrichment, large pulses of DMS occurred in the fertilised IN patch, compared with the unfertilised OUT patch. During the third and fourth iron infusions, total chl a concentrations doubled from 0.52 to 1.02 µg/L. Hapto8s and prasinophytes accounted for 50%, and 20%, respectively, of total chl a. The large pulses of DMS during the third iron enrichment occurred during high dissolved DMSP concentrations and wind strength changes in dinoflagellate, haptophyte, and cyanobacteria biomass and increased microzooplankton grazing that exerted a top down control on phytoplankton production. A further fourth iron enrichment did cause surface waters to increase in DMS, but the effect was not as great as that recorded in the third enrichment. Differences in the biological response between SAGE and several other iron enrichment experiments were concluded to reflect microzooplankton grazing activities and the microbial loop dominance, resulting from mixing of the MLD during storm activity and high winds during iron enrichment.
Location: United Kingdom of Great Britain and Northern Ireland
Location: New Zealand
Location: New Zealand
No related grants have been discovered for Mike Harvey.