ABSTRACT
The oceans represent a significant global source of atmospheric aerosols. Sea spray aerosol (SSA) particles comprise sea salts and organic species in varying proportions. In addition to size, the overall composition of SSA particles determines how effectively they can form cloud droplets and ice crystals. Thus, understanding the factors controlling SSA composition is critical to predicting aerosol impacts on clouds and climate. It is often assumed that submicrometer SSAs are mainly formed by film drops produced from bursting bubble-cap films, which become enriched with hydrophobic organic species contained within the sea surface microlayer. In contrast, jet drops formed from the base of bursting bubbles are postulated to mainly produce larger supermicrometer particles from bulk seawater, which comprises largely salts and water-soluble organic species. However, here we demonstrate that jet drops produce up to 43% of total submicrometer SSA number concentrations, and that the fraction of SSA produced by jet drops can be modulated by marine biological activity. We show that the chemical composition, organic volume fraction, and ice nucleating ability of submicrometer particles from jet drops differ from those formed from film drops. Thus, the chemical composition of a substantial fraction of submicrometer particles will not be controlled by the composition of the sea surface microlayer, a major assumption in previous studies. This finding has significant ramifications for understanding the factors controlling the mixing state of submicrometer SSA particles and must be taken into consideration when predicting SSA impacts on clouds and climate.
ABSTRACT
Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using "dry" geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean.
ABSTRACT
High-spatial-resolution, near-surface vertical profiling of atmospheric chemical composition is currently limited by the availability of experimental platforms that can sample in constrained environments. As a result, measurements of near-surface gradients in trace gas and aerosol particle concentrations have been limited to studies conducted from fixed location towers or tethered balloons. Here, we explore the utility of a quadrotor unmanned aircraft system (UAS) as a sampling platform to measure vertical and horizontal concentration gradients of trace gases and aerosol particles at high spatial resolution (1 m) within the mixed layer (0-100 m). A 3D Robotics Iris+ autonomous quadrotor UAS was outfitted with a sensor package consisting of a two-channel aerosol optical particle counter and a CO2 sensor. The UAS demonstrated high precision in both vertical (±0.5 m) and horizontal positions (±1 m), highlighting the potential utility of quadrotor UAS drones for aerosol- and trace-gas measurements within complex terrain, such as the urban environment, forest canopies, and above difficult-to-access areas such as breaking surf. Vertical profiles of aerosol particle number concentrations, acquired from flights conducted along the California coastline, were used to constrain sea-spray aerosol-emission rates from coastal wave breaking.
Subject(s)
Aerosols/analysis , Air Pollutants/chemistry , Aircraft , Particle Size , CaliforniaABSTRACT
The production, size, and chemical composition of sea spray aerosol (SSA) particles strongly depend on seawater chemistry, which is controlled by physical, chemical, and biological processes. Despite decades of studies in marine environments, a direct relationship has yet to be established between ocean biology and the physicochemical properties of SSA. The ability to establish such relationships is hindered by the fact that SSA measurements are typically dominated by overwhelming background aerosol concentrations even in remote marine environments. Herein, we describe a newly developed approach for reproducing the chemical complexity of SSA in a laboratory setting, comprising a unique ocean-atmosphere facility equipped with actual breaking waves. A mesocosm experiment was performed in natural seawater, using controlled phytoplankton and heterotrophic bacteria concentrations, which showed SSA size and chemical mixing state are acutely sensitive to the aerosol production mechanism, as well as to the type of biological species present. The largest reduction in the hygroscopicity of SSA occurred as heterotrophic bacteria concentrations increased, whereas phytoplankton and chlorophyll-a concentrations decreased, directly corresponding to a change in mixing state in the smallest (60-180 nm) size range. Using this newly developed approach to generate realistic SSA, systematic studies can now be performed to advance our fundamental understanding of the impact of ocean biology on SSA chemical mixing state, heterogeneous reactivity, and the resulting climate-relevant properties.
Subject(s)
Aerosols/chemistry , Atmosphere/chemistry , Bacteria/metabolism , Phytoplankton/metabolism , Seawater/chemistry , Chlorophyll/chemistry , Chlorophyll A , Ecology , Oceanography , Oceans and SeasABSTRACT
Dinoflagellate bioluminescence, a common source of bioluminescence in coastal waters, is stimulated by flow agitation. Although bubbles are anecdotally known to be stimulatory, the process has never been experimentally investigated. This study quantified the flash response of the bioluminescent dinoflagellate Lingulodinium polyedrum to stimulation by bubbles rising through still seawater. Cells were stimulated by isolated bubbles of 0.3-3 mm radii rising at their terminal velocity, and also by bubble clouds containing bubbles of 0.06-10 mm radii for different air flow rates. Stimulation efficiency, the proportion of cells producing a flash within the volume of water swept out by a rising bubble, decreased with decreasing bubble radius for radii less than approximately 1 mm. Bubbles smaller than a critical radius in the range 0.275-0.325 mm did not stimulate a flash response. The fraction of cells stimulated by bubble clouds was proportional to the volume of air in the bubble cloud, with lower stimulation levels observed for clouds with smaller bubbles. An empirical model for bubble cloud stimulation based on the isolated bubble observations successfully reproduced the observed stimulation by bubble clouds for low air flow rates. High air flow rates stimulated more light emission than expected, presumably because of additional fluid shear stress associated with collective buoyancy effects generated by the high air fraction bubble cloud. These results are relevant to bioluminescence stimulation by bubbles in two-phase flows, such as in ship wakes, breaking waves, and sparged bioreactors.
Subject(s)
Dinoflagellida/chemistry , Luminescence , Luminescent Measurements , Particle Size , Surface PropertiesABSTRACT
Sea spray aerosol (SSA) particles represent one of the most abundant surfaces available for heterogeneous reactions to occur upon and thus profoundly alter the composition of the troposphere. In an effort to better understand tropospheric heterogeneous reaction processes, fundamental laboratory studies must be able to accurately reproduce the chemical complexity of SSA. Here we describe a new approach that uses microbial processes to control the composition of seawater and SSA particle composition. By inducing a phytoplankton bloom, we are able to create dynamic ecosystem interactions between marine microorganisms, which serve to alter the organic mixtures present in seawater. Using this controlled approach, changes in seawater composition become reflected in the chemical composition of SSA particles 4 to 10 d after the peak in chlorophyll-a. This approach for producing and varying the chemical complexity of a dominant tropospheric aerosol provides the foundation for further investigations of the physical and chemical properties of realistic SSA particles under controlled conditions.
Subject(s)
Aerosols/chemistry , Chlorophyll/chemistry , Models, Chemical , Seawater/chemistry , Chlorophyll A , LaboratoriesABSTRACT
Variable wind speeds over the ocean can have a significant impact on the formation mechanism and physical-chemical properties of sea spray aerosols (SSA), which in turn influence their climate-relevant impacts. Herein, for the first time, we investigate the effects of wind speed on size-dependent morphology and composition of individual nascent SSA generated from wind-wave interactions of natural seawater within a wind-wave channel as a function of size and their particle-to-particle variability. Filter-based thermal optical analysis, atomic force microscopy (AFM), AFM infrared spectroscopy (AFM-IR), and scanning electron microscopy (SEM) were employed in this regard. This study focuses on SSA with sizes within 0.04-1.8 µm generated at two wind speeds: 10 m/s, representing a wind lull scenario over the ocean, and 19 m/s, indicative of the wind speeds encountered in stormy conditions. Filter-based measurements revealed a reduction of the organic mass fraction as the wind speed increases. AFM imaging at 20% relative humidity of individual SSA identified six main morphologies: prism-like, rounded, core-shell, rod, rod inclusion core-shell, and aggregates. At 10 m/s, most SSA were rounded, while at 19 m/s, core-shells became predominant. Based on AFM-IR, rounded SSA at both wind speeds had similar composition, mainly composed of aliphatic and oxygenated species, whereas the shells of core-shells displayed more oxygenated organics at 19 m/s and more aliphatic organics at 10 m/s. Collectively, our observations can be attributed to the disruption of the sea surface microlayer film structure at higher wind speeds. The findings reveal a significant impact of wind speed on morphology and composition of SSA, which should be accounted for accurate assessment of their climate effects.
ABSTRACT
The behavioural response study (BRS) is an experimental design used by field biologists to determine the function and/or behavioural effects of conspecific, heterospecific or anthropogenic stimuli. When carrying out these studies in marine mammals it is difficult to make basic observations and achieve sufficient samples sizes because of the high cost and logistical difficulties. Rarely are other factors such as social context or the physical environment considered in the analysis because of these difficulties. This paper presents results of a BRS carried out in humpback whales to test the response of groups to one recording of conspecific social sounds and an artificially generated tone stimulus. Experiments were carried out in September/October 2004 and 2008 during the humpback whale southward migration along the east coast of Australia. In total, 13 'tone' experiments, 15 'social sound' experiments (using one recording of social sounds) and three silent controls were carried out over two field seasons. The results (using a mixed model statistical analysis) suggested that humpback whales responded differently to the two stimuli, measured by changes in course travelled and dive behaviour. Although the response to 'tones' was consistent, in that groups moved offshore and surfaced more often (suggesting an aversion to the stimulus), the response to 'social sounds' was highly variable and dependent upon the composition of the social group. The change in course and dive behaviour in response to 'tones' was found to be related to proximity to the source, the received signal level and signal-to-noise ratio (SNR). This study demonstrates that the behavioural responses of marine mammals to acoustic stimuli are complex. In order to tease out such multifaceted interactions, the number of replicates and factors measured must be sufficient for multivariate analysis.
Subject(s)
Humpback Whale/physiology , Tape Recording , Vocalization, Animal , Animals , Multivariate Analysis , Queensland , Seasons , Signal-To-Noise Ratio , Social Behavior , Sound SpectrographyABSTRACT
Deterministic structures in sound reflected by gravity waves, such as focused arrivals and Doppler shifts, have implications for underwater acoustics and sonar, and the performance of underwater acoustic communications systems. A stationary phase analysis of the Helmholtz-Kirchhoff scattering integral yields the trajectory of focused arrivals and their relationship to the curvature of the surface wave field. Deterministic effects along paths up to 70 water depths long are observed in shallow water measurements of surface-scattered sound at the Martha's Vineyard Coastal Observatory. The arrival time and amplitude of surface-scattered pulses are reconciled with model calculations using measurements of surface waves made with an upward-looking sonar mounted mid-way along the propagation path. The root mean square difference between the modeled and observed pulse arrival amplitude and delay, respectively, normalized by the maximum range of amplitudes and delays, is found to be 0.2 or less for the observation periods analyzed. Cross-correlation coefficients for modeled and observed pulse arrival delays varied from 0.83 to 0.16 depending on surface conditions. Cross-correlation coefficients for normalized pulse energy for the same conditions were small and varied from 0.16 to 0.06. In contrast, the modeled and observed pulse arrival delay and amplitude statistics were in good agreement.
Subject(s)
Acoustics , Sound , Water , Acoustics/instrumentation , Gravitation , Models, Theoretical , Motion , Oceans and Seas , Scattering, Radiation , Signal Processing, Computer-Assisted , Sound Spectrography , Surface Properties , Time Factors , Transducers , Water Movements , WindABSTRACT
High-latitude polar deserts are among the most extreme environments on Earth. Here we describe a large and previously unappreciated habitat for photosynthetic life under opaque rocks in the Arctic and Antarctic polar deserts. This habitat is created by the periglacial movement of the rocks, which allows some light to reach their underside. The productivity of this ecosystem is at least as great as that of above-ground biomass and potentially doubles previous productivity estimates for the polar desert ecozone.
Subject(s)
Desert Climate , Ecosystem , Geologic Sediments/microbiology , Antarctic Regions , Arctic Regions , Canada , Cyanobacteria/metabolism , Cyanobacteria/radiation effects , Eukaryota/metabolism , Eukaryota/radiation effects , Light , Photosynthesis/radiation effectsABSTRACT
A model for the underwater noise of whitecaps is presented and compared with the noise measured beneath plunging seawater laboratory waves. The noise from a few hundred hertz up to at least 80 kHz is assumed to be due to the pulses of sound radiated by bubbles formed within a breaking wave crest. The total noise level and its dependence on frequency are a function of bubble creation rate, bubble damping factor and an 'acoustical skin depth' associated with scattering and absorption by the bubble plume formed within the crest. Calculation of breaking wave noise is made using estimates of these factors, which are made independently of the noise itself. The results are in good agreement with wave noise measured in a laboratory flume when compensated for reverberation. A closed-form, analytical expression for the wave noise is presented, which shows a -11/6 power-law dependence of noise level on frequency, in good agreement with the -10/6 scaling law commonly observed in the open ocean.
ABSTRACT
On Conch Reef, Florida Keys, USA we examined the effects of reef hydrography and topography on the patterns of stable isotope values (δ18O and δ13C) in the benthic green alga, Halimeda tuna. During the summer, benthic temperatures show high-frequency fluctuations (2 to 8 °C) associated with internal waves that advected cool, nutrient-rich water across the reef. The interaction between local water flow and reef morphology resulted in a highly heterogenous physical environment even within isobaths that likely influenced the growth regime of H. tuna. Variability in H. tuna isotopic values even among closely located individuals suggest biological responses to the observed environmental heterogeneity. Although isotopic composition of reef carbonate material can be used to reconstruct past temperatures (T(°C) = 14.2-3.6 (δ18OHalimeda - δ18Oseawater); r2 = 0.92), comparing the temperatures measured across the reef with that predicted by an isotopic thermometer suggests complex interactions between the environment and Halimeda carbonate formation at temporal and spatial scales not normally considered in mixed sediment samples. The divergence in estimated range between measured and predicted temperatures demonstrates the existence of species- and location-specific isotopic relationships with physical and environmental factors that should be considered in contemporary as well as ancient reef settings.
Subject(s)
Chlorophyta/metabolism , Coral Reefs , Florida , Hydrology , Marine Biology , Oxygen Isotopes/metabolism , Oxygen Radioisotopes/metabolism , Paleontology , Seawater , TemperatureABSTRACT
An analysis of the acoustic emissions of air bubbles fragmenting in sheared fluid flow is presented. The fragmentation of bubbles into two products only is considered. While the measured pressure amplitude is highly variable, the partition of energy between fragmentation products is highly correlated. The partition of energy between products is, on average, approximately equal irrespective of the relative sizes of the bubble products. This observation suggests that the acoustic excitation mechanism is common to both bubbles immediately prior to fragmentation. A model for the excitation mechanism based on symmetric collapse of the neck of air joining fragmentation products is proposed and found to be sufficient to explain the range of observed bubble pulse amplitudes and the equal partition of energy.
Subject(s)
Acoustics , Air , Sound , Water , Models, Theoretical , Pressure , Rheology , Sound Spectrography , Surface Properties , Time FactorsABSTRACT
Songs produced by migrating whales were recorded off the coast of Queensland, Australia, over six consecutive weeks in 2003. Forty-eight independent song sessions were analyzed using information theory techniques. The average length of the songs estimated by correlation analysis was approximately 100 units, with song sessions lasting from 300 to over 3100 units. Song entropy, a measure of structural constraints, was estimated using three different methodologies: (1) the independently identically distributed model, (2) a first-order Markov model, and (3) the nonparametric sliding window match length (SWML) method, as described by Suzuki et al. [(2006). "Information entropy of humpback whale song," J. Acoust. Soc. Am. 119, 1849-1866]. The analysis finds that the song sequences of migrating Australian whales are consistent with the hierarchical structure proposed by Payne and McVay [(1971). "Songs of humpback whales," Science 173, 587-597], and recently supported mathematically by Suzuki et al. (2006) for singers on the Hawaiian breeding grounds. Both the SWML entropy estimates and the song lengths for the Australian singers in 2003 were lower than that reported by Suzuki et al. (2006) for Hawaiian whales in 1976-1978; however, song redundancy did not differ between these two populations separated spatially and temporally. The average total information in the sequence of units in Australian song was approximately 35 bits/song. Aberrant songs (8%) yielded entropies similar to the typical songs.
Subject(s)
Animal Migration , Humpback Whale/physiology , Information Theory , Signal Processing, Computer-Assisted , Vocalization, Animal , Animals , Australia , Entropy , Markov Chains , Models, Biological , Sound Spectrography , Time FactorsABSTRACT
The composition and surface properties of atmospheric aerosol particles largely control their impact on climate by affecting their ability to uptake water, react heterogeneously, and nucleate ice in clouds. However, in the vacuum of a conventional electron microscope, the native surface and internal structure often undergo physicochemical rearrangement resulting in surfaces that are quite different from their atmospheric configurations. Herein, we report the development of cryogenic transmission electron microscopy where laboratory generated sea spray aerosol particles are flash frozen in their native state with iterative and controlled thermal and/or pressure exposures and then probed by electron microscopy. This unique approach allows for the detection of not only mixed salts, but also soft materials including whole hydrated bacteria, diatoms, virus particles, marine vesicles, as well as gel networks within hydrated salt droplets-all of which will have distinct biological, chemical, and physical processes. We anticipate this method will open up a new avenue of analysis for aerosol particles, not only for ocean-derived aerosols, but for those produced from other sources where there is interest in the transfer of organic or biological species from the biosphere to the atmosphere.
ABSTRACT
Measurements of the sound of bubbles fragmenting in fluid shear are presented and analyzed. The frequency, amplitude, and decay rate of the acoustic emissions from 1.8-mm-radius bubbles fragmenting between opposed fluid jets have been determined. A broad band of frequencies (1.8 to 30 kHz) is observed with peak pressure amplitudes in the range of 0.03 to 2 Pa. While the peak pressure amplitudes show no significant scaling with frequency, the frequency dependence of the decay rates is consistent with the sum of thermal and acoustic radiation losses.
ABSTRACT
A model is presented for the flash response of bioluminescent dinoflagellates stimulated by fluid shear. The model is based on the idea that the response of an individual cell to stimulation is inherently probabilistic, and can be modeled as a Poisson process over short time scales. A new cell parameter, the cell anxiety, is introduced to parameterize the probability of flashing. The statistical model is incorporated into a description of fully developed fluid flow in pipes and a cylindrical Couette chamber, and found to compare favorably with previously published data from experiments.
Subject(s)
Dinoflagellida/physiology , Luminescence , Models, Statistical , Animals , Luminescent Measurements , Models, Biological , Motion , Physical Stimulation , Probability , Stress, MechanicalABSTRACT
Breaking ocean waves entrain air bubbles that enhance air-sea gas flux, produce aerosols, generate ambient noise and scavenge biological surfactants. The size distribution of the entrained bubbles is the most important factor in controlling these processes, but little is known about bubble properties and formation mechanisms inside whitecaps. We have measured bubble size distributions inside breaking waves in the laboratory and in the open ocean, and provide a quantitative description of bubble formation mechanisms in the laboratory. We find two distinct mechanisms controlling the size distribution, depending on bubble size. For bubbles larger than about 1 mm, turbulent fragmentation determines bubble size distribution, resulting in a bubble density proportional to the bubble radius to the power of -10/3. Smaller bubbles are created by jet and drop impact on the wave face, with a -3/2 power-law scaling. The length scale separating these processes is the scale where turbulent fragmentation ceases, also known as the Hinze scale. Our results will have important implications for the study of air-sea gas transfer.