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A new bubble-generating glass chamber with an extensive set of aerosol production experiments is presented. Compared to the experiments described in the literature since the ground-setting works of Edward C.​​​​​​​ Monahan et al. in 1980s, the current setup is among the medium-sized installations allowing for accurate control of the air discharge, water temperature, and salinity. The size and material of the chamber offer a variety of applications due to its portability, measurement setup adjustability, and sterilization option. The experiments have been conducted in a cylindrical bubbling tank of 10 L volume that was filled by ∼ 30 %–40 % with water of controlled salt content and temperature and covered with a hermetic lid. The chamber was used to study the characteristics of aerosols produced by bursting bubbles under different conditions. In line with previous findings, the sea spray aerosol production was shown to depend linearly on the surface area covered by the bubbles, which in turn is a near-linear function of the air discharge through the water. Observed dependencies of the aerosol size spectra and particle fluxes on water salinity and temperature, being qualitatively comparable with the previous experiments, substantially refined the existing parameterizations. In particular, the bubble size was practically independent from the air discharge through the water body, except in the case of very small flows. Also, the dependence of aerosol spectrum and amount on salinity was much weaker than suggested in some previous experiments. The temperature dependence, to the contrary, was significant and consistent, with a transition in the spectrum shape at ∼ 10 ∘C. Theoretical analysis based on the basic conservation laws supported the main results of the experiments but also highlighted the need for a better understanding of the aerosol production from a cold water surface.

Emissions of methane (CH4) from offshore oil and gas installations are poorly ground-truthed, and quantification relies heavily on the use of emission factors and activity data. As part of the United Nations Climate & Clean Air Coalition (UN CCAC) objective to study and reduce short-lived climate pollutants (SLCPs), a Twin Otter aircraft was used to survey CH4 emissions from UK and Dutch offshore oil and gas installations. The aims of the surveys were to (i) identify installations that are significant CH4 emitters, (ii) separate installation emissions from other emissions using carbon-isotopic fingerprinting and other chemical proxies, (iii) estimate CH4 emission rates, and (iv) improve flux estimation (and sampling) methodologies for rapid quantification of major gas leaks. In this paper, we detail the instrument and aircraft set-up for two campaigns flown in the springs of 2018 and 2019 over the southern North Sea and describe the developments made in both the planning and sampling methodology to maximise the quality and value of the data collected. We present example data collected from both campaigns to demonstrate the challenges encountered during offshore surveys, focussing on the complex meteorology of the marine boundary layer and sampling discrete plumes from an airborne platform. The uncertainties of CH4 flux calculations from measurements under varying boundary layer conditions are considered, as well as recommendations for attribution of sources through either spot sampling for volatile organic compounds (VOCs) ∕ δ13CCH4 or using in situ instrumental data to determine C2H6–CH4 ratios. A series of recommendations for both planning and measurement techniques for future offshore work within marine boundary layers is provided. Atmospheric Measurement Techniques, 14 (1) ISSN:1867-8548 ISSN:1867-1381

Atmospheric ethane can be used as a tracer to distinguish methane sources, both at the local and global scale. Currently, ethane can be measured in the field using flasks or in situ analyzers. In our study, we characterized the CRDS Picarro G2201-i instrument, originally designed to measure isotopic CH4 and CO2, for measurements of ethane-to-methane ratio in mobile-measurement scenarios, near sources and under field conditions. We evaluated the limitations and potential of using the CRDS G2201-i to measure the ethane-to-methane ratio, thus extending the instrument application to simultaneously measure two methane source proxies in the field: carbon isotopic ratio and the ethane-to-methane ratio. First, laboratory tests were run to characterize the instrument in stationary conditions. Subsequently, the instrument performance was tested in field conditions as part of a controlled release experiment. Finally, the instrument was tested during mobile measurements focused on gas compressor stations. The results from the field were afterwards compared with the results obtained from instruments specifically designed for ethane measurements. Our study shows the potential of using the CRDS G2201-i instrument in a mobile configuration to determine the ethane-to-methane ratio in methane plumes under measurement conditions with an ethane uncertainty of 50 ppb. Assuming typical ethane-to-methane ratios ranging between 0 and 0.1 ppb ppb−1, we conclude that the instrument can accurately estimate the “true” ethane-to-methane ratio within 1σ uncertainty when CH4 enhancements are at least 1 ppm, as can be found in the vicinity of strongly emitting sites such as natural gas compressor stations and roadside gas pipeline leaks.

Emissions of methane (CH4) from offshore oil and gas installations are poorly ground-truthed and quantification relies heavily on the use of emission factors and activity data. As part of the United Nations Climate and Clean Air Coalition (UN CCAC) objective to study and reduce short-lived climate pollutants (SLCP) a Twin Otter aircraft was used to survey CH4 emissions from UK and Dutch offshore oil and gas installations. The aims of the surveys were to i) identify installations that are significant CH4 emitters, ii) separate installation emissions from other emissions using carbon-isotopic fingerprinting and other chemical proxies, iii) estimate CH4 emission rates, and iv) improve flux estimation (and sampling) methodologies for rapid quantification of major gas leaks. In this paper, we detail the instrument and aircraft set up for two campaigns flown in the springs of 2018 and 2019 over the southern North Sea and describe the developments made in both planning and sampling methodology in order to maximise the quality and value of the data collected. We present example data collected from both campaigns to demonstrate the challenges encountered during offshore surveys, focussing on the complex meteorology of the marine boundary layer, and sampling discrete plumes from an airborne platform. The uncertainties of CH4 flux calculations from measurements under varying boundary layer conditions are considered, as well as recommendations for attribution of sources through either spot sampling for VOCs / δ13CCH4 or using in-situ instrumental data to determine C2H6-CH4 ratios. A series of recommendations for both planning and measurement techniques for future offshore work within the marine boundary layers are provided.

Frequently, passive dry deposition collectors are used to sample atmospheric dust deposition. However, there exists a multitude of different instruments with different, usually not well-characterized sampling efficiencies. As a result, the acquired data might be considerably biased with respect to their size representativity and, as a consequence, also composition. In this study, individual particle analysis by automated scanning electron microscopy coupled with energydispersive X-ray analysis was used to characterize different, commonly used passive samplers with respect to their sizeresolved deposition rate and concentration. This study focuses on the microphysical properties, i.e., the aerosol concentration and deposition rates as well as the particle size distributions. In addition, computational fluid dynamics modeling was used in parallel to achieve deposition velocities from a theoretical point of view. Scanning electron microscopy (SEM)-calculated deposition rate measurements made using different passive samplers show a disagreement among the samplers. Modified Wilson and Cooke (MWAC) and Big Spring Number Eight (BSNE)-both horizontal flux samplers-collect considerably more material than the flat plate and Sigma-2 samplers, which are vertical flux samplers. The collection efficiency of MWAC increases for large particles in comparison to Sigma-2 with increasing wind speed, while such an increase is less observed in the case of BSNE. A positive correlation is found between deposition rate and PM concentration measurements by an optical particle spectrometer. The results indicate that a BSNE and Sigma-2 can be good options for PM measurement, whereas MWAC and flat-plate samplers are not a suitable choice. A negative correlation was observed in between dust deposition rate and wind speed. Deposition velocities calculated from different classical deposition models do not agree with deposition velocities estimated using computational fluid dynamics (CFD) simulations. The deposition velocity estimated from CFD was often higher than the values derived from classical deposition velocity models. Moreover, the modeled deposition velocity ratios between different samplers do not agree with the observations. This research has been supported by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) (grant nos. 264907654, 264912134 and 416816480 (KA 2280))

Low concentrations of ice-nucleating particles (INPs) are thought to be important for the properties of mixed-phase clouds, but their detection is challenging. Hence, there is a need for instruments where INP concentrations of less than 0.01 L−1 can be routinely and efficiently determined. The use of larger volumes of suspension in drop assays increases the sensitivity of an experiment to rarer INPs or rarer active sites due to the increase in aerosol or surface area of particulates per droplet. Here we describe and characterise the InfraRed-Nucleation by Immersed Particles Instrument (IR-NIPI), a new immersion freezing assay that makes use of IR emissions to determine the freezing temperature of individual 50 µL droplets each contained in a well of a 96-well plate. Using an IR camera allows the temperature of individual aliquots to be monitored. Freezing temperatures are determined by detecting the sharp rise in well temperature associated with the release of heat caused by freezing. In this paper we first present the calibration of the IR temperature measurement, which makes use of the fact that following ice nucleation aliquots of water warm to the ice–liquid equilibrium temperature (i.e. 0 ∘C when water activity is ∼1), which provides a point of calibration for each individual well in each experiment. We then tested the temperature calibration using ∼100 µm chips of K-feldspar, by immersing these chips in 1 µL droplets on an established cold stage (µL-NIPI) as well as in 50 µL droplets on IR-NIPI; the results were consistent with one another, indicating no bias in the reported freezing temperature. In addition we present measurements of the efficiency of the mineral dust NX-illite and a sample of atmospheric aerosol collected on a filter in the city of Leeds. NX-illite results are consistent with literature data, and the atmospheric INP concentrations were in good agreement with the results from the µL-NIPI instrument. This demonstrates the utility of this approach, which offers a relatively high throughput of sample analysis and access to low INP concentrations.

In June 2009, 22 spectrometers from 14 institutes measured tropospheric and stratospheric NO2 from the ground for more than 11 days during the Cabauw Intercomparison Campaign of Nitrogen Dioxide measuring Instruments (CINDI), at Cabauw, NL (51.97° N, 4.93° E). All visible instruments used a common wavelength range and set of cross sections for the spectral analysis. Most of the instruments were of the multi-axis design with analysis by differential spectroscopy software (MAX-DOAS), whose non-zenith slant columns were compared by examining slopes of their least-squares straight line fits to mean values of a selection of instruments, after taking 30-min averages. Zenith slant columns near twilight were compared by fits to interpolated values of a reference instrument, then normalised by the mean of the slopes of the best instruments. For visible MAX-DOAS instruments, the means of the fitted slopes for NO2 and O4 of all except one instrument were within 10% of unity at almost all non-zenith elevations, and most were within 5%. Values for UV MAX-DOAS instruments were almost as good, being 12% and 7%, respectively. For visible instruments at zenith near twilight, the means of the fitted slopes of all instruments were within 5% of unity. This level of agreement is as good as that of previous intercomparisons, despite the site not being ideal for zenith twilight measurements. It bodes well for the future of measurements of tropospheric NO2, as previous intercomparisons were only for zenith instruments focussing on stratospheric NO2, with their longer heritage.