Abstract. The flux of dimethylsulfide (DMS) to the atmosphere is generally inferred using water sampled at or below 2 m depth, thereby excluding any concentration anomalies at the air-sea interface. Two independent techniques were used to assess the potential for near-surface DMS enrichment to influence DMS emissions and also identify the factors influencing enrichment. DMS measurements in productive frontal waters over the Chatham Rise, east of New Zealand, did not identify any significant gradients between 0.01 and 6 m in sub-surface seawater, whereas DMS enrichment in the sea-surface microlayer was variable, with a mean enrichment factor (EF; the concentration ratio between DMS in the sea-surface microlayer and in sub-surface water) of 1.7. Physical and biological factors influenced sea-surface microlayer DMS concentration, with high enrichment (EF > 1.3) only recorded in a dinoflagellate-dominated bloom, and associated with low to medium wind speeds and near-surface temperature gradients. On occasion, high DMS enrichment preceded periods when the air-sea DMS flux, measured by eddy covariance, exceeded the flux calculated using National Oceanic and Atmospheric Administration (NOAA) CoupledOcean Atmospheric Response Experiment (COARE) parameterized gas transfer velocities and measured sub-surface seawater DMS concentrations. The results of these two independent approaches suggest that air-sea emissions may be influenced by near-surface DMS production under certain conditions, and highlight the need for further study to constrain the magnitude and mechanisms of DMS production in the sea-surface microlayer.

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) campaign, which examined air-sea interaction over biologically productive frontal waters east of New Zealand. This overview details the objectives, regional context, sampling 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 (k DMS ) 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 distributionsPublished by Copernicus Publications on behalf of the European Geosciences Union. 13646 C. S. Law et al.: Overview and preliminary results of the SOAP campaign 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 pr...

A 3-GHz Doppler radar has been used to study wave dynamics and backscatter from the sea surface at low grazing angles. Vertical polarization results are dominated by Bragg scatter even at low (•8 ø) grazing angles. Horizontal polarization results, however, show a strong upwind-downwind asymmetry with additional, highvelocity intermittent scatter in the upwind direction associated with steep or breaking waves. These characteristics have been exploited to distinguish spilling breaking events from the background Bragg scatter. While these "spikes" at a single range may appear random in time, the combined range and time information reveals a well-determined propagation pattern. It is shown that for a developing sea in deep water, group behavior modulates the occurrence of wave breaking. The frequency-wavenumber spectrum shows a clear separation between the linear dispersion curve and nonlinear effects related to breaking. The most important nonlinear feature is a line near the dominant wave group velocity which is identified with the spectrum of breaking intermittency. The slope of this line suggests that the wave components which are most likely to break lie at frequencies significantly above the dominant wave frequency. backscatter mechanism at microwave frequencies [Wright, 1968; Plant and Keller, 1990; Poulter et al., 1994]. At low grazing angles, Bragg scatter from horizontal polarization for a slightly roughened sea is predicted to be -30 dB below that of vertical polarization. Additional mechanisms at these angles such as wedge diffraction [Lyzenga et al., 1983] and backscatter from breaking plumes [Wetzel, 1990] have been invoked to explain the strong observed scatter. Despite data dating back more than 20 years a satisfactory theoretical explanation of backscatter at low grazing angles remains elusive.In this paper we investigate the properties of sea backscatter at low grazing angles (-8 ø) using an S band radar. At these angles, Bragg backscatter using horizontal polarization will theoretically be small. In section 3, properties of the backscatter mechanisms are sought in terms of the polarization ratio, azimuthal dependence, velocity of scatter, and temporal behavior. A key feature of the radar is the simultaneous acquisition of full Doppler spectra over a significant range extent. In section 4 the range coverage of the radar is exploited to show the propagating nature of the upwind HH backscatter. This is used to provide information on the group modulation of wave breaking of deep water waves where the breaking is predominantly spilling breaking. Finally in section 5, linear wave and group modulation information is derived from the frequency-wavenumber spectrum. Experimental DescriptionThe radar used in these studies operates at 3 GHz ()• = 10 cm) with an FMCW modulation [Poulter et al., 1995a]. An adaptation using interrupted modulation (FMICW) has been developed to allow a single antenna to be switched between the transmitter and the receiver [McGregor et al., 1994]. This greatly enhances the portabili...

1The SOLAS air-sea gas exchange experiment (SAGE) was a multiple-objective study investigating 2 gas-transfer processes and the influence of iron fertilisation on biologically driven gas exchange in

Abstract. Due to its remote location and extreme weather conditions, atmospheric in situ measurements are rare in the Southern Ocean. As a result, aerosol–cloud interactions in this region are poorly understood and remain a major source of uncertainty in climate models. This, in turn, contributes substantially to persistent biases in climate model simulations such as the well-known positive shortwave radiation bias at the surface, as well as biases in numerical weather prediction models and reanalyses. It has been shown in previous studies that in situ and ground-based remote sensing measurements across the Southern Ocean are critical for complementing satellite data sets due to the importance of boundary layer and low-level cloud processes. These processes are poorly sampled by satellite-based measurements and are often obscured by multiple overlying cloud layers. Satellite measurements also do not constrain the aerosol–cloud processes very well with imprecise estimation of cloud condensation nuclei. In this work, we present a comprehensive set of ship-based aerosol and meteorological observations collected on the 6-week Southern Ocean Ross Sea Marine Ecosystem and Environment voyage (TAN1802) voyage of RV Tangaroa across the Southern Ocean, from Wellington, New Zealand, to the Ross Sea, Antarctica. The voyage was carried out from 8 February to 21 March 2018. Many distinct, but contemporaneous, data sets were collected throughout the voyage. The compiled data sets include measurements from a range of instruments, such as (i) meteorological conditions at the sea surface and profile measurements; (ii) the size and concentration of particles; (iii) trace gases dissolved in the ocean surface such as dimethyl sulfide and carbonyl sulfide; (iv) and remotely sensed observations of low clouds. Here, we describe the voyage, the instruments, and data processing, and provide a brief overview of some of the data products available. We encourage the scientific community to use these measurements for further analysis and model evaluation studies, in particular, for studies of Southern Ocean clouds, aerosol, and their interaction. The data sets presented in this study are publicly available at https://doi.org/10.5281/zenodo.4060237 (Kremser et al., 2020).