ALBERT

Description: This study attempts a new identification of mechanisms of secondary ice production (SIP) based on the observation of small faceted ice crystals (hexagonal plates or columns) with typical sizes smaller than 100 µm. Due to their young age, such small ice crystals can be used as tracers for identifying the conditions for SIP. Observations reported here were conducted in oceanic tropical mesoscale convective systems (MCSs) and midlatitude frontal clouds in the temperature range from 0 to −15 ∘C and heavily seeded by aged ice particles. It was found that in both MCSs and frontal clouds, SIP was observed right above the melting layer and extended to higher altitudes with colder temperatures. The roles of six possible mechanisms to generate the SIP particles are assessed using additional observations. In most observed SIP cases, small secondary ice particles spatially correlated with liquid-phase, vertical updrafts and aged rimed ice particles. However, in many cases, neither graupel nor liquid drops were observed in the SIP regions, and therefore, the conditions for an active Hallett–Mossop process were not met. In many cases, large concentrations of small pristine ice particles were observed right above the melting layer, starting at temperatures as warm as −0.5 ∘C. It is proposed that the initiation of SIP above the melting layer is stimulated by the recirculation of large liquid drops through the melting layer with convective turbulent updrafts. After re-entering a supercooled environment above the melting layer, they impact with aged ice, freeze, and shatter. The size of the splinters generated during SIP was estimated as 10 µm or less. A principal conclusion of this work is that only the freezing-drop-shattering mechanism could be clearly supported by the airborne in situ observations.

Description: The combined effects of elevated pCO2 and temperature were investigated during an autumn phytoplankton bloom in the Western English Channel (WEC). A full factorial 36-day microcosm experiment was conducted under year 2100 predicted temperature (+4.5 °C) and pCO2 levels (800 μatm). The starting phytoplankton community biomass was 110.2 (±5.7 sd) mg carbon (C) m−3 and was dominated by dinoflagellates (~ 50 %) with smaller contributions from nanophytoplankton (~ 13 %), cryptophytes (~ 11 %)and diatoms (~ 9 %). Over the experimental period total biomass was significantly increased by elevated pCO2 (20-fold increase) and elevated temperature (15-fold increase). In contrast, the combined influence of these two factors had little effect on biomass relative to the ambient control. The phytoplankton community structure shifted from dinoflagellates to nanophytoplankton at the end of the experiment in all treatments. Under elevated pCO2 nanophytoplankton contributed 90% of community biomass and was dominated by Phaeocystis spp., while under elevated temperature nanophytoplankton contributed 85 % of the community biomass and was dominated by smaller nano-flagellates. Under ambient conditions larger nano-flagellates dominated while the smallest nanophytoplankton contribution was observed under combined elevated pCO2 and temperature (~ 40 %). Dinoflagellate biomass declined significantly under the individual influences of elevated pCO2, temperature and ambient conditions. Under the combined effects of elevated pCO2 and temperature, dinoflagellate biomass almost doubled from the starting biomass and there was a 30-fold increase in the harmful algal bloom (HAB) species, Prorocentrum cordatum. Chlorophyll a normalised maximum photosynthetic rates (PBm) increased 〉 6-fold under elevated pCO2 and 〉 3-fold under elevated temperature while no effect on PBm was observed when pCO2 and temperature were elevated simultaneously. The results suggest that future increases in temperature and pCO2 do not appear to influence coastal phytoplankton productivity during autumn in the WEC which would have a negative feedback on atmospheric CO2.

Description: There is a lack of knowledge of how biomass burning aerosols in the tropics age, including those in the fire-prone Northern Territory in Australia. This paper reports chemical characterization of fresh and aged aerosols monitored during the 1-month-long SAFIRED (Savannah Fires in the Early Dry Season) field study, with an emphasis on the chemical signature and aging of organic aerosols. The campaign took place in June 2014 during the early dry season when the surface measurement site, the Australian Tropical Atmospheric Research Station (ATARS), located in the Northern Territory, was heavily influenced by thousands of wild and prescribed bushfires. ATARS was equipped with a wide suite of instrumentation for gaseous and aerosol characterization. A compact time-of-flight aerosol mass spectrometer was deployed to monitor aerosol chemical composition. Approximately 90 % of submicron non-refractory mass was composed of organic material. Ozone enhancement in biomass burning plumes indicated increased air mass photochemistry. The diversity in biomass burning emissions was illustrated through variability in chemical signature (e.g. wide range in f44, from 0.06 to 0.18) for five intense fire events. The background particulate loading was characterized using positive matrix factorization (PMF). A PMF-resolved BBOA (biomass burning organic aerosol) factor comprised 24 % of the submicron non-refractory organic aerosol mass, confirming the significance of fire sources. A dominant PMF factor, OOA (oxygenated organic aerosol), made up 47 % of the sampled aerosol, illustrating the importance of aerosol aging in the Northern Territory. Biogenic isoprene-derived organic aerosol factor was the third significant fraction of the background aerosol (28 %).

Description: The SAFIRED (Savannah Fires in the Early Dry Season) campaign took place from 29 May until 30 June 2014 at the Australian Tropical Atmospheric Research Station (ATARS) in the Northern Territory, Australia. The purpose of this campaign was to investigate emissions from fires in the early dry season in northern Australia. Measurements were made of biomass burning aerosols, volatile organic compounds, polycyclic aromatic carbons, greenhouse gases, radon, speciated atmospheric mercury and trace metals. Aspects of the biomass burning aerosol emissions investigated included; emission factors of various species, physical and chemical aerosol properties, aerosol aging, micronutrient supply to the ocean, nucleation, and aerosol water uptake. Over the course of the month-long campaign, biomass burning signals were prevalent and emissions from several large single burning events were observed at ATARS.Biomass burning emissions dominated the gas and aerosol concentrations in this region. Dry season fires are extremely frequent and widespread across the northern region of Australia, which suggests that the measured aerosol and gaseous emissions at ATARS are likely representative of signals across the entire region of north Australia. Air mass forward trajectories show that these biomass burning emissions are carried north-west over the Timor Sea and could influence the atmosphere over Indonesia and the tropical atmosphere over the Indian Ocean. Here we present characteristics of the biomass burning observed at the sampling site and provide an overview of the more specific outcomes of the SAFIRED campaign.

Description: We have tested the ability of a high-resolution chemical transport model (CTM) to reproduce biomass burning (BB) plume strikes and ozone (O3) enhancements observed at Cape Grim in Tasmania, Australia, from the Robbins Island fire. The CTM has also been used to explore the contribution of near-field BB emissions and background sources to O3 observations under conditions of complex meteorology. Using atmospheric observations, we have tested model sensitivity to meteorology, BB emission factors (EFs) corresponding to low, medium, and high modified combustion efficiency (MCE), and spatial variability. The use of two different meteorological models (TAPM–CTM and CCAM–CTM) varied the first (BB1) plume strike time by up to 15 h and the duration of impact between 12 and 36 h, and it varied the second (BB2) plume duration between 50 and 57 h. Meteorology also had a large impact on simulated O3, with one model (TAPM–CTM) simulating four periods of O3 enhancement, while the other model (CCAM) simulating only one period. Varying the BB EFs, which in turn varied the non-methane organic compound (NMOC) ∕ oxides of nitrogen (NOx) ratio, had a strongly non-linear impact on simulated O3 concentration, with either destruction or production of O3 predicted in different simulations. As shown in previous work (Lawson et al., 2015), minor rainfall events have the potential to significantly alter EF due to changes in combustion processes. Models that assume fixed EF for O3 precursor species in an environment with temporally or spatially variable EF may be unable to simulate the behaviour of important species such as O3. TAPM–CTM is used to further explore the contribution of the Robbins Island fire to the observed O3 enhancements during BB1 and BB2. Overall, TAPM–CTM suggests that the dominant source of O3 observed at Cape Grim was aged urban air (age  = 2 days), with a contribution of O3 formed from local BB emissions. This work shows the importance of assessing model sensitivity to meteorology and EF and the large impact these variables can have in particular on simulated destruction or production of O3 in regional atmospheric chemistry simulations. This work also shows the importance of using models to elucidate the contribution from different sources to atmospheric composition, where this is difficult using observations alone.

Description: The ice water content (IWC) of cirrus clouds is an essential parameter determining their radiative properties and thus is important for climate simulations. Therefore, for a reliable measurement of IWC on board research aircraft, it is important to carefully design the ice crystal sampling and measuring devices. During the ML-CIRRUS field campaign in 2014 with the German Gulfstream GV HALO (High Altitude and Long Range Research Aircraft), IWC was recorded by three closed-path total water together with one gas-phase water instrument. The hygrometers were supplied by inlets mounted on the roof of the aircraft fuselage. Simultaneously, the IWC is determined by a cloud particle spectrometer attached under an aircraft wing. Two more examples of simultaneous IWC measurements by hygrometers and cloud spectrometers are presented, but the inlets of the hygrometers were mounted at the fuselage side (M-55 Geophysica, StratoClim campaign 2017) and bottom (NASA WB57, MacPex campaign 2011). This combination of instruments and inlet positions provides the opportunity to experimentally study the influence of the ice particle sampling position on the IWC with the approach of comparative measurements. As expected from theory and shown by computational fluid dynamics (CFD) calculations, we found that the IWCs provided by the roof inlets deviate from those measured under the aircraft wing. As a result of the inlet position in the shadow zone behind the aircraft cockpit, ice particle populations with mean mass sizes larger than about 25 µm radius are subject to losses, which lead to strongly underestimated IWCs. On the other hand, cloud populations with mean mass sizes smaller than about 12 µm are dominated by particle enrichment and thus overestimated IWCs. In the range of mean mass sizes between 12 and 25 µm, both enrichment and losses of ice crystals can occur, depending on whether the ice crystal mass peak of the size distribution – in these cases bimodal – is on the smaller or larger mass mode. The resulting deviations of the IWC reach factors of up to 10 or even more for losses as well as for enrichment. Since the mean mass size of ice crystals increases with temperature, losses are more pronounced at higher temperatures, while at lower temperatures IWC is more affected by enrichment. In contrast, in the cases where the hygrometer inlets were mounted at the fuselage side or bottom, the agreement of IWCs is most frequently within a factor of 2.5 or better – due to less disturbed ice particle sampling, as expected from theory – independently of the mean ice crystal sizes. The rather large scatter between IWC measurements reflects, for example, cirrus cloud inhomogeneities and instrument uncertainties as well as slight sampling biases which might also occur on the side or bottom of the fuselage and under the wing. However, this scatter is in the range of other studies and represent the current best possible IWC recording on fast-flying aircraft.

Description: Understanding uncertainty is essential for utilizing atmospheric volatile organic compound (VOC) measurements in robust ways to develop atmospheric science. This study describes an inter-comparison of the VOC data, and the derived uncertainty estimates, measured with three independent techniques (PTR-MS, proton-transfer-reaction mass spectrometry; GC-FID-MS, gas chromatography with flame-ionization and mass spectrometric detection; and DNPH–HPLC, 2,4-dinitrophenylhydrazine derivatization followed by analysis by high-performance liquid chromatography) during routine monitoring as part of the Sydney Particle Study (SPS) campaign in 2012. Benzene, toluene, C8 aromatics, isoprene, formaldehyde and acetaldehyde were selected for the comparison, based on objective selection criteria from the available data. Bottom-up uncertainty analyses were undertaken for each compound and each measurement system. Top-down uncertainties were quantified via the inter-comparisons. In all seven comparisons, the correlations between independent measurement techniques were high with R2 values with a median of 0.92 (range 0.75–0.98) and small root mean square of the deviations (RMSD) of the observations from the regression line with a median of 0.11 (range 0.04–0.23 ppbv). These results give a high degree of confidence that for each comparison the response of the two independent techniques is dominated by the same constituents. The slope and intercept as determined by reduced major axis (RMA) regression gives a different story. The slopes varied considerably with a median of 1.25 and a range of 1.16–2.01. The intercepts varied with a median of 0.04 and a range of −0.03 to 0.31 ppbv. An ideal comparison would give a slope of 1.00 and an intercept of 0. Some sources of uncertainty that are poorly quantified by the bottom-up uncertainty analysis method were identified, including: contributions of non-target compounds to the measurement of the target compound for benzene, toluene and isoprene by PTR-MS as well as the under-reporting of formaldehyde, acetaldehyde and acetone by the DNPH technique. As well as these, this study has identified a specific interference of liquid water with acetone measurements by the DNPH technique. These relationships reported for Sydney 2012 were incorporated into a larger analysis with 61 similar published inter-comparison studies for the same compounds. Overall, for the light aromatics, isoprene and the C1–C3 carbonyls, the uncertainty in a set of measurements varies by a factor of between 1.5 and 2. These uncertainties (∼50 %) are significantly higher than uncertainties estimated using standard propagation of error methods, which in this case were ∼22 % or less, and are the result of the presence of poorly understood or neglected processes that affect the measurement and its uncertainty. The uncertainties in VOC measurements identified here should be considered when assessing the reliability of VOC measurements from routine monitoring with individual, stand-alone instruments; when utilizing VOC data to constrain and inform air quality and climate models; when using VOC observations for human exposure studies; and for comparison with satellite retrievals.

Description: 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 (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.

Description: In this paper, we investigate the role of flow structures generated in wind farm control through yaw misalignment. A pair of counter-rotating vortices is shown to be important in deforming the shape of the wake and in explaining the asymmetry of wake steering in oppositely signed yaw angles. We also demonstrate that vortices generated by an upstream turbine that is performing wake steering can deflect wakes of downstream turbines, even if they are themselves aligned. We encourage the development of improvements to control-oriented engineering models of wind farm control, to include the effects of these large-scale flow structures. Such a new model would improve the predictability of control-oriented models. Further, we demonstrate that the vortex structures created in wake steering can lead to greater impact on power generation than currently modeled in control-oriented models. We propose that wind farm controllers can be made more effective if designed to take advantage of these effects.

Description: In this paper, we investigate the role of flow structures generated in wind farm control through yaw misalignment. A pair of counter-rotating vortices are shown to be important in deforming the shape of the wake and in explaining the asymmetry of wake steering in oppositely signed yaw angles. We motivate the development of new physics for control-oriented engineering models of wind farm control, which include the effects of these large-scale flow structures. Such a new model would improve the predictability of control-oriented models. Results presented in this paper indicate that wind farm control strategies, based on new control-oriented models with new physics, that target total flow control over wake redirection may be different, and perhaps more effective, than current approaches. We propose that wind farm control and wake steering should be thought of as the generation of large-scale flow structures, which will aid in the improved performance of wind farms.