Abstract. Halogenated very short-lived substances (VSLSs) are naturally produced in the ocean and emitted to the atmosphere. When transported to the stratosphere, these compounds can have a significant influence on the ozone layer and climate. During a research cruise on RV Sonne in the subtropical and tropical west Indian Ocean in July and August 2014, we measured the VSLSs, methyl iodide (CH 3 I) and for the first time bromoform (CHBr 3 ) and dibromomethane (CH 2 Br 2 ), in surface seawater and the marine atmosphere to derive their emission strengths. Using the Lagrangian particle dispersion model FLEXPART with ERAInterim meteorological fields, we calculated the direct contribution of observed VSLS emissions to the stratospheric halogen burden during the Asian summer monsoon. Furthermore, we compare the in situ calculations with the interannual variability of transport from a larger area of the west Indian Ocean surface to the stratosphere for July 2000-2015. We found that the west Indian Ocean is a strong source for CHBr 3 (910 pmol m −2 h −1 ), very strong source for CH 2 Br 2 (930 pmol m −2 h −1 ), and an average source for CH 3 I (460 pmol m −2 h −1 ). The atmospheric transport from the tropical west Indian Ocean surface to the stratosphere experiences two main pathways. On very short timescales, especially relevant for the shortest-lived compound CH 3 I (3.5 days lifetime), convection above the Indian Ocean lifts oceanic air masses and VSLSs towards the tropopause. On a longer timescale, the Asian summer monsoon circulation transports oceanic VSLSs towards India and the Bay of Bengal, where they are lifted with the monsoon convection and reach stratospheric levels in the southeastern part of the Asian monsoon anticyclone. This transport pathway is more important for the longer-lived brominated compounds (17 and 150 days lifetime for CHBr 3 and CH 2 Br 2 ). The entrainment of CHBr 3 and CH 3 I from the west Indian Ocean to the stratosphere during the Asian summer monsoon is lower than from previous cruises in the tropical west Pacific Ocean during boreal autumn and early winter but higher than from the tropical Atlantic during boreal summer. In contrast, the projected CH 2 Br 2 entrainment was very high because of the high emissions during the west Indian Ocean cruise. The 16-year July time series shows highest interannual variability for the shortest-lived CH 3 I and lowest for the longest-lived CH 2 Br 2 . During this time period, a small increase in VSLS entrainment from the west Indian Ocean through the Asian monsoon to the stratosphere is found. Overall, this study confirms that the subtropical and tropical west Indian Ocean is an important source region of halogenated VSLSs, especially CH 2 Br 2 , to the troposphere and stratosphere during the Asian summer monsoon.

Abstract. A severe reduction of greenhouse gas emissions is necessary to reach the objectives of the Paris Agreement. The implementation and continuous evaluation of mitigation measures requires regular independent information on emissions of the two main anthropogenic greenhouse gases, carbon dioxide (CO2) and methane (CH4). Our aim is to employ an observation-based method to determine regional-scale greenhouse gas emission estimates with high accuracy. We use aircraft- and ground-based in situ observations of CH4, CO2, carbon monoxide (CO), and wind speed from two research flights over the Upper Silesian Coal Basin (USCB), Poland, in summer 2018. The flights were performed as a part of the Carbon Dioxide and Methane (CoMet) mission above this European CH4 emission hot-spot region. A kriging algorithm interpolates the observed concentrations between the downwind transects of the trace gas plume, and then the mass flux through this plane is calculated. Finally, statistic and systematic uncertainties are calculated from measurement uncertainties and through several sensitivity tests, respectively. For the two selected flights, the in-situ-derived annual CH4 emission estimates are 13.8±4.3 and 15.1±4.0 kg s−1, which are well within the range of emission inventories. The regional emission estimates of CO2, which were determined to be 1.21±0.75 and 1.12±0.38 t s−1, are in the lower range of emission inventories. CO mass balance emissions of 10.1±3.6 and 10.7±4.4 kg s−1 for the USCB are slightly higher than the emission inventory values. The CH4 emission estimate has a relative error of 26 %–31 %, the CO2 estimate of 37 %–62 %, and the CO estimate of 36 %–41 %. These errors mainly result from the uncertainty of atmospheric background mole fractions and the changing planetary boundary layer height during the morning flight. In the case of CO2, biospheric fluxes also add to the uncertainty and hamper the assessment of emission inventories. These emission estimates characterize the USCB and help to verify emission inventories and develop climate mitigation strategies.

<p><strong>Abstract.</strong> Halogenated very short-lived substances (VSLS) are naturally produced in the ocean and emitted to the atmosphere. When transported to the stratosphere, these compounds can have a significant influence on the ozone layer and climate. During a research cruise on RV <i>Sonne</i> in the subtropical and tropical West Indian Ocean in July and August 2014, we measured the VSLS, methyl iodide (CH<sub>3</sub>I) and for the first time bromoform (CHBr<sub>3</sub>) and dibromomethane (CH<sub>2</sub>Br<sub>2</sub>), in surface seawater and the marine atmosphere to derive their emission strengths. Using the Lagrangian transport model Flexpart with ERA-Interim meteorological fields, we calculated the direct contribution of observed VSLS emissions to the stratospheric halogen burden during Asian summer monsoon. Furthermore, we compare the in situ calculations with the interannual variability of transport from a larger area of the West Indian Ocean surface to the stratosphere for July 2000–2015. We found that the West Indian Ocean is a strong source region for CHBr<sub>3</sub> (910 pmol m<sup>−2</sup> h<sup>−1</sup>), very strong for CH<sub>2</sub>Br<sub>2</sub> (930 pmol m<sup>−2</sup> h<sup>−1</sup>), and average for CH<sub>3</sub>I (460 pmol m<sup>−2</sup> h<sup>−1</sup>). The atmospheric transport from the tropical West Indian Ocean surface to the stratosphere experiences two main pathways. On very short timescales, especially relevant for the shortest-lived compound CH<sub>3</sub>I (3.5 days lifetime), convection above the Indian Ocean lifts oceanic air masses and VSLS towards the tropopause. On a longer timescale, the Asian summer monsoon circulation transports oceanic VSLS towards India and Bay of Bengal, where they are lifted with the monsoon convection and reach stratospheric levels in the southeastern part of the Asian monsoon anticyclone. This transport pathway is more important for the longer-lived brominated compounds (17 and 150 days lifetime for CHBr<sub>3</sub> and CH<sub>2</sub>Br<sub>2</sub>). The entrainment of CHBr<sub>3</sub> and CH<sub>3</sub>I from the West Indian Ocean to the stratosphere during Asian summer monsoon is less than from previous cruises in the tropical West Pacific Ocean during boreal autumn/early winter, but higher than from the tropical Atlantic during boreal summer. In contrast, the projected CH<sub>2</sub>Br<sub>2</sub> entrainment was very high because of the high emissions during the West Indian Ocean cruise. The 16-year July time series shows highest interannual variability for the short-lived CH<sub>3</sub>I and lowest for the long-lived CH<sub>2</sub>Br<sub>2</sub>. During this time period, a small increase of VSLS entrainment from the West Indian Ocean through the Asian monsoon to the stratosphere is found. Overall, this study confirms that the subtropical and tropical West Indian Ocean is an important source region of halogenated VSLS, especially CH<sub>2</sub>Br<sub>2</sub>, to the troposphere and stratosphere during the Asian summer monsoon.</p>

Abstract. Abundant mining and industrial activities located in the Upper Silesian Coal Basin (USCB) lead to large emissions of the potent greenhouse gas (GHG) methane (CH4). The strong localization of CH4 emitters (mostly confined to known coal mine ventilation shafts) and the large emissions of 448 and 720 kt CH4 yr−1 reported in the European Pollutant Release and Transfer Register (E-PRTR 2017) and the Emissions Database for Global Atmospheric Research (EDGAR v4.3.2), respectively, make the USCB a prime research target for validating and improving CH4 flux estimation techniques. High-precision observations of this GHG were made downwind of local (e.g., single facilities) to regional-scale (e.g., agglomerations) sources in the context of the CoMet 1.0 campaign in early summer 2018. A quantum cascade–interband cascade laser (QCL–ICL)-based spectrometer adapted for airborne research was deployed aboard the German Aerospace Center (DLR) Cessna 208B to sample the planetary boundary layer (PBL) in situ. Regional CH4 emission estimates for the USCB are derived using a model approach including assimilated wind soundings from three ground-based Doppler lidars. Although retrieving estimates for individual emitters is difficult using only single flights due to sparse data availability, the combination of two flights allows for exploiting different meteorological conditions (analogous to a sparse tomography algorithm) to establish confidence on facility-level estimates. Emission rates from individual sources not only are needed for unambiguous comparisons between bottom-up and top-down inventories but also become indispensable if (independently verifiable) sanctions are to be imposed on individual companies emitting GHGs. An uncertainty analysis is presented for both the regional-scale and facility-level emission estimates. We find instantaneous coal mine emission estimates of 451/423 ± 77/79 kt CH4 yr−1 for the morning/afternoon flight of 6 June 2018. The derived fuel-exploitation emission rates coincide (±6 %) with annual-average inventorial data from E-PRTR 2017 although they are distinctly lower (−28 %/−32 %) than values reported in EDGAR v4.3.2. Discrepancies in available emission inventories could potentially be narrowed down with sufficient observations using the method described herein to bridge the gap between instantaneous emission estimates and yearly averaged inventories.

Methane (CH 4 ) is an important greenhouse gas with 28-35 times the warming potential of carbon dioxide over a 100 year period (Myhre et al., 2013). Global CH 4 concentrations in the atmosphere have nearly tripled since pre-industrial times, mainly driven by anthropogenic activity, and are responsible for a fourth of the increased radiative forcing on the planet (Myhre et al., 2013). Although CH 4 concentrations stabilized for a

 ACT-America provides a unique, weather-oriented collection of high-quality measurements of atmospheric CO2, CH4, trace gases and meteorological properties. ACT-America data are free and open to the public from the ORNL DAAC. ACT-America data are uniquely suited to improve the accuracy and precision of regional inverse GHG flux estimates.

Halogen‐ and sulfur‐containing compounds are supersaturated in the surface ocean, which results in their emission to the atmosphere. These compounds can be transported to the stratosphere, where they impact ozone, the background aerosol layer, and climate. In this study we calculate the seasonal and interannual variability of transport from the West Indian Ocean (WIO) surface to the stratosphere for 2000–2016 with the Lagrangian transport model FLEXPART using ERA‐Interim meteorological fields. We investigate the transport relevant for very short lived substances (VSLS) with tropospheric lifetimes corresponding to dimethylsulfide (1 day), methyl iodide (CH3I, 3.5 days), bromoform (CHBr3, 17 days), and dibromomethane (CH2Br2, 150 days). The stratospheric source gas injection of VSLS tracers from the WIO shows a distinct annual cycle associated with the Asian monsoon. Over the 16‐year time series, a slight increase in source gas injection from the WIO to the stratosphere is found for all VSLS tracers and during all seasons. The interannual variability shows a relationship with sea surface temperatures in the WIO as well as the El Niño–Southern Oscillation. During boreal spring of El Niño, enhanced stratospheric injection of VSLS from the tropical WIO is caused by positive sea surface temperature anomalies and enhanced vertical uplift above the WIO. During boreal fall of La Niña, strong injection is related to enhanced atmospheric upward motion over the East Indian Ocean and a prolonged Indian summer monsoon season. Related physical mechanisms and uncertainties are discussed in this study.

During the summer monsoon, the western tropical Indian Ocean is predicted to be a hot spot for dimethylsulfide emissions, the major marine sulfur source to the atmosphere, and an important aerosol precursor. Other aerosol relevant fluxes, such as isoprene and sea spray, should also be enhanced, due to the steady strong winds during the monsoon. Marine air masses dominate the area during the summer monsoon, excluding the influence of continentally derived pollutants. During the SO234‐2/235 cruise in the western tropical Indian Ocean from July to August 2014, directly measured eddy covariance DMS fluxes confirm that the area is a large source of sulfur to the atmosphere (cruise average 9.1 μmol m−2 d−1). The directly measured fluxes, as well as computed isoprene and sea spray fluxes, were combined with FLEXPART backward and forward trajectories to track the emissions in space and time. The fluxes show a significant positive correlation with aerosol data from the Terra and Suomi‐NPP satellites, indicating a local influence of marine emissions on atmospheric aerosol numbers.