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This paper investigates the scientific value of retrieving H218O and HDO columns in addition to H216O columns from high-resolution ground-based near-infrared spectra. We present a set of refined H216O, H218O, and HDO spectral windows. The retrieved H216O, H218O, and HDO columns are used for an a posteriori calculation of columnar δD and δ18O. We estimate the uncertainties for the so-calculated columnar δD and δ18O values. These estimations include uncertainties due to the measurement noise, errors in the a priori data, and uncertainties in spectroscopic parameters. Time series of δ18O obtained from ground-based FTIR (Fourier transform infrared) spectra are presented for the first time. For our study we use a full physics isotopic general circulation model (ECHAM5-wiso). We show that the full physics simulation of HDO and H218O can already be reasonably predicted from the H216O columns by a simple linear regression model (scatter values between full physics and linear regression simulations are 35 and 4‰ for HDO and H218O, respectively). We document that the columnar δD and δ18O values as calculated a posteriori from the retrievals of H216O, H218O, and HDO show a better agreement with the ECHAM5-wiso simulation than the δD and δ18O values as calculated from the H216O retrievals and the simple linear regression model. This suggests that the H218O and HDO column retrievals add complementary information to the H216O retrievals. However, these data have to be used carefully, because of the different vertical sensitivity of the H216O, H218O, and HDO columnar retrievals. Furthermore, we have to note that the retrievals use reanalysis humidity profiles as a priori input and the results are thus not independent of the reanalysis data.

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.

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.

The SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nucleating particle (INP) counter manufactured by Droplet Measurement Technologies in Boulder, CO. The SPIN is a continuous flow diffusion chamber with parallel plate geometry based on the Zurich Ice Nucleation Chamber and the Portable Ice Nucleation Chamber. This study presents a standard description for using the SPIN instrument and also highlights methods to analyze measurements in more advanced ways. It characterizes and describes the behavior of the SPIN chamber, reports data from laboratory measurements, and quantifies uncertainties associated with the measurements. Experiments with ammonium sulfate are used to investigate homogeneous freezing of deliquesced haze droplets and droplet breakthrough. Experiments with kaolinite, NX illite, and silver iodide are used to investigate heterogeneous ice nucleation. SPIN nucleation results are compared to those from the literature. A machine learning approach for analyzing depolarization data from the SPIN optical particle counter is also presented (as an advanced use). Overall, we report that the SPIN is able to reproduce previous INP counter measurements. Atmospheric Measurement Techniques, 9 (7) ISSN:1867-8548 ISSN:1867-1381

A method for directly measuring carbon dioxide (CO2) emissions using a mobile sensor network in cities at fine spatial resolution was developed and tested. First, a compact, mobile system was built using an infrared gas analyzer combined with open-source hardware to control, georeference, and log measurements of CO2 mixing ratios on vehicles (car, bicycles). Second, two measurement campaigns, one in summer and one in winter (heating season) were carried out. Five mobile sensors were deployed within a 1 × 12. 7 km transect across the city of Vancouver, BC, Canada. The sensors were operated for 3.5 h on pre-defined routes to map CO2 mixing ratios at street level, which were then averaged to 100 × 100 m grid cells. The averaged CO2 mixing ratios of all grids in the study area were 417.9 ppm in summer and 442.5 ppm in winter. In both campaigns, mixing ratios were highest in the grid cells of the downtown core and along arterial roads and lowest in parks and well vegetated residential areas. Third, an aerodynamic resistance approach to calculating emissions was used to derive CO2 emissions from the gridded CO2 mixing ratio measurements in conjunction with mixing ratios and fluxes collected from a 28 m tall eddy-covariance tower located within the study area. These measured emissions showed a range of −12 to 226 CO2 ha−1 h−1 in summer and of −14 to 163 kg CO2 ha−1 h−1 in winter, with an average of 35.1 kg CO2 ha−1 h−1 (summer) and 25.9 kg CO2 ha−1 h−1 (winter). Fourth, an independent emissions inventory was developed for the study area using buildings energy simulations from a previous study and routinely available traffic counts. The emissions inventory for the same area averaged to 22.06 kg CO2 ha−1 h−1 (summer) and 28.76 kg CO2 ha−1 h−1 (winter) and was used to compare against the measured emissions from the mobile sensor network. The comparison on a grid-by-grid basis showed linearity between CO2 mixing ratios and the emissions inventory (R2 = 0. 53 in summer and R2 = 0. 47 in winter). Also, 87 % (summer) and 94 % (winter) of measured grid cells show a difference within ±1 order of magnitude, and 49 % (summer) and 69 % (winter) show an error of less than a factor 2. Although associated with considerable errors at the individual grid cell level, the study demonstrates a promising method of using a network of mobile sensors and an aerodynamic resistance approach to rapidly map greenhouse gases at high spatial resolution across cities. The method could be improved by longer measurements and a refined calculation of the aerodynamic resistance.

International audience; Abstract. The Maritime Aerosol Network (MAN) has been collecting data over the oceans since November 2006. The MAN archive provides a valuable resource for aerosol studies in maritime environments. In the current paper we investigate correlations between ship-borne aerosol optical depth (AOD) and near-surface wind speed, either measured (onboard or from satellite) or modeled (NCEP). According to our analysis, wind speed influences columnar aerosol optical depth, although the slope of the linear regression between AOD and wind speed is not steep (~0.004–0.005), even for strong winds over 10 m s−1. The relationships show significant scatter (correlation coefficients typically in the range 0.3–0.5); the majority of this scatter can be explained by the uncertainty on the input data. The various wind speed sources considered yield similar patterns. Results are in good agreement with the majority of previously published relationships between surface wind speed and ship-based or satellite-based AOD measurements. The basic relationships are similar for all the wind speed sources considered; however, the gradient of the relationship varies by around a factor of two depending on the wind data used.

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

Abstract. The ozone profile records of a large number of limb and occultation satellite instruments are widely used to address several key questions in ozone research. Further progress in some domains depends on a more detailed understanding of these data sets, especially of their long-term stability and their mutual consistency. To this end, we made a systematic assessment of 14 limb and occultation sounders that, together, provide more than three decades of global ozone profile measurements. In particular, we considered the latest operational Level-2 records by SAGE II, SAGE III, HALOE, UARS MLS, Aura MLS, POAM II, POAM III, OSIRIS, SMR, GOMOS, MIPAS, SCIAMACHY, ACE-FTS and MAESTRO. Central to our work is a consistent and robust analysis of the comparisons against the ground-based ozonesonde and stratospheric ozone lidar networks. It allowed us to investigate, from the troposphere up to the stratopause, the following main aspects of satellite data quality: long-term stability, overall bias and short-term variability, together with their dependence on geophysical parameters and profile representation. In addition, it permitted us to quantify the overall consistency between the ozone profilers. Generally, we found that between 20 and 40 km the satellite ozone measurement biases are smaller than ±5 %, the short-term variabilities are less than 5–12 % and the drifts are at most ±5 % decade−1 (or even ±3 % decade−1 for a few records). The agreement with ground-based data degrades somewhat towards the stratopause and especially towards the tropopause where natural variability and low ozone abundances impede a more precise analysis. In part of the stratosphere a few records deviate from the preceding general conclusions; we identified biases of 10 % and more (POAM II and SCIAMACHY), markedly higher single-profile variability (SMR and SCIAMACHY) and significant long-term drifts (SCIAMACHY, OSIRIS, HALOE and possibly GOMOS and SMR as well). Furthermore, we reflected on the repercussions of our findings for the construction, analysis and interpretation of merged data records. Most notably, the discrepancies between several recent ozone profile trend assessments can be mostly explained by instrumental drift. This clearly demonstrates the need for systematic comprehensive multi-instrument comparison analyses.