ALBERT

Description: The quasi‐biennial oscillation (QBO) of the equatorial zonal wind leads to zonally symmetric temperature variations in the stratosphere that descend downward. Here we investigate the QBO‐induced temperature anomalies in the tropical tropopause layer (TTL) and detect pronounced longitudinal variations of the signal. In addition, the QBO temperature anomalies show a strong seasonal variability. The magnitude of these seasonal and longitudinal QBO variations is comparable to the magnitude of the well‐known zonal mean QBO signal in the TTL. At the cold point tropopause, the strongest QBO variations of around ±1.6 K are found over regions of active convection such as the West Pacific and Africa during boreal winter. The weakest QBO variations of ±0.25 K are detected over the East Pacific during boreal summer, while the zonal mean signal ranges around ±0.7 K. The longitudinal variations are associated with enhanced convective activity that occurs during QBO cold phases and locally enhances the cold anomalies.

Description: Transport of air masses from the subtropics, enriched in trace gases from the oceans, coasts and islands, towards lower latitudes under the trade inversion and uplift to the stratosphere in tropical deep convection. The organic bromine compounds bromoform (CHBr 3 ) and dibromomethane (CH 2 Br 2 ) influence tropospheric chemistry and stratospheric ozone depletion. Their atmospheric abundance is generally related to a common marine source, which is not well characterized. A cruise between the three Macaroenesian Archipelagos of Cape Verde, the Canaries and Madeira revealed that anthropogenic sources increased oceanic CHBr 3 emissions significantly close to some islands, especially at the Canaries, while heterotrophic processes in the ocean increased the flux of CH 2 Br 2 from the sea to the atmosphere in the Cape Verde region. As anthropogenic disinfection processes, which release CHBr 3 in coastal areas increase, and as more CH 2 Br 2 may be produced from increased heterotrophy in a warming, deoxygenated ocean, both sources could supply higher fractions of stratospheric bromine in the future, with yet unknown consequences for stratospheric ozone.

Description: The tropical tropopause layer (TTL) is the transition region between the well-mixed convective troposphere and the radiatively controlled stratosphere with air masses showing chemical and dynamical properties of both regions. The representation of the TTL in meteorological reanalysis data sets is important for studying the complex interactions of circulation, convection, trace gases, clouds, and radiation. In this paper, we present the evaluation of climatological and long-term TTL temperature and tropopause characteristics in the reanalysis data sets ERA-Interim, ERA5, JRA-25, JRA-55, MERRA, MERRA-2, NCEP-NCAR (R1), and CFSR. The evaluation has been performed as part of the SPARC (Stratosphere–troposphere Processes and their Role in Climate) Reanalysis Intercomparison Project (S-RIP). The most recent atmospheric reanalysis data sets (ERA-Interim, ERA5, JRA-55, MERRA-2, and CFSR) all provide realistic representations of the major characteristics of the temperature structure within the TTL. There is good agreement between reanalysis estimates of tropical mean temperatures and radio occultation data, with relatively small cold biases for most data sets. Temperatures at the cold point and lapse rate tropopause levels, on the other hand, show warm biases in reanalyses when compared to observations. This tropopause-level warm bias is related to the vertical resolution of the reanalysis data, with the smallest bias found for data sets with the highest vertical resolution around the tropopause. Differences in the cold point temperature maximize over equatorial Africa, related to Kelvin wave activity and associated disturbances in TTL temperatures. Interannual variability in reanalysis temperatures is best constrained in the upper TTL, with larger differences at levels below the cold point. The reanalyses reproduce the temperature responses to major dynamical and radiative signals such as volcanic eruptions and the quasi-biennial oscillation (QBO). Long-term reanalysis trends in temperature in the upper TTL show good agreement with trends derived from adjusted radiosonde data sets indicating significant stratospheric cooling of around −0.5 to −1 K per decade. At 100 hPa and the cold point, most of the reanalyses suggest small but significant cooling trends of −0.3 to −0.6 K per decade that are statistically consistent with trends based on the adjusted radiosonde data sets. Advances of the reanalysis and observational systems over the last decades have led to a clear improvement in the TTL reanalysis products over time. Biases of the temperature profiles and differences in interannual variability clearly decreased in 2006, when densely sampled radio occultation data started being assimilated by the reanalyses. While there is an overall good agreement, different reanalyses offer different advantages in the TTL such as realistic profile and cold point temperature, continuous time series, or a realistic representation of signals of interannual variability. Their use in model simulations and in comparisons with climate model output should be tailored to their specific strengths and weaknesses.

Description: Halogenated very short-lived substances (VSLSs), such as bromoform (CHBr3), can be transported to the stratosphere and contribute to the halogen loading and ozone depletion. Given their highly variable emission rates and their short atmospheric lifetimes, the exact amount as well as the spatio-temporal variability of their contribution to the stratospheric halogen loading are still uncertain. We combine observational data sets with Lagrangian atmospheric modelling in order to analyse the spatial and temporal variability of the CHBr3 injection into the stratosphere for the time period 1979–2013. Regional maxima with mixing ratios of up to 0.4–0.5 ppt at 17 km altitude are diagnosed to be over Central America (1) and over the Maritime Continent–west Pacific (2), both of which are confirmed by high-altitude aircraft campaigns. The CHBr3 maximum over Central America is caused by the co-occurrence of convectively driven short transport timescales and strong regional sources, which in conjunction drive the seasonality of CHBr3 injection. Model results at a daily resolution reveal isolated, exceptionally high CHBr3 values in this region which are confirmed by aircraft measurements during the ACCENT campaign and do not occur in spatially or temporally averaged model fields. CHBr3 injection over the west Pacific is centred south of the Equator due to strong oceanic sources underneath prescribed by the here-applied bottom-up emission inventory. The globally largest CHBr3 mixing ratios at the cold point level of up to 0.6 ppt are diagnosed to occur over the region of India, Bay of Bengal, and Arabian Sea (3); however, no data from aircraft campaigns are available to confirm this finding. Inter-annual variability of stratospheric CHBr3 injection of 10 %–20 % is to a large part driven by the variability of coupled ocean–atmosphere circulation systems. Long-term changes, on the other hand, correlate with the regional sea surface temperature trends resulting in positive trends of stratospheric CHBr3 injection over the west Pacific and Asian monsoon region and negative trends over the east Pacific. For the tropical mean, these opposite regional trends balance each other out, resulting in a relatively weak positive trend of 0.017±0.012 ppt Br per decade for 1979–2013, corresponding to 3 % Br per decade. The overall contribution of CHBr3 together with CH2Br2 to the stratospheric halogen loading accounts for 4.7 ppt Br, in good agreement with existing studies, with 50 % and 50 % being injected in the form of source and product gases, respectively.

Description: Abstract

Description: These data files contain the results of Evolved Gas Analysis (EGA) on a Mettler-Toledo TGA-DSC 3+ attached to a Pfeiffer Vacuum GSD 320 gas mass spectrometer on ash samples from the 15 January 2022 eruption of Hunga volcano, Tonga. Samples were heated in Nitrogen at a rate of 5 °C/min from 30 to 150 °C for dehydration purposes and then at a rate of 30 °C/min from 150 °C to 1300 °C. During heating, the relative amount of different volatile species (H2O, CO2, SO2, HCl, and H2S, which are extracted from mass-to-charge ratios of 18, 44, 64, 36, and 34, respectively) were recorded by the gas mass spectrometer. Natural samples collected for the analysis were bulk ash material or correspond to a given ash fraction. Particles were unwashed and dried at 40°C before analysis. We compared the signals for natural samples with (i) a mixture of salt-free dense glassy particles, white and dark pumice (HT10), (ii) pure halite, anhydrite, gypsum, calcite and pyrit, (iii) mix between pure magmatic particles (HT10) from (i) and manually added components from (iii).

Description: Bromoform (CHBr3), a recognized contributor to stratospheric ozone depletion, has been largely exempt from the Montreal Protocol's regulation due to its short atmospheric lifetime and large natural emissions. Using our recent CHBr3 emission inventory containing both natural and anthropogenic sources, we reevaluated the role played by the latter in the total CHBr3 flux into the Northern Hemisphere extratropical stratosphere. Derived mainly from ship ballast, power plant cooling and desalination plant brine water, these anthropogenic sources suggest a substantial underestimation in previous global CHBr3 emission estimates. Anthropogenic sources have been underestimated by 31.5% globally, and more alarmingly, this underestimation escalates to 70.5% when focusing on the Northern Hemisphere. Consequently, atmospheric CHBr3 concentrations are also significantly higher than previous estimates, especially over the NH extratropics during boreal winter. The ODP-weighted emissions in the NH based on historical ECMWF meteorology are ~28.2 Gg Br/year, increased by ~78% above previous estimates, suggesting a more significant contribution of anthropogenic CHBr3 to stratospheric ozone depletion, especially in the NH lowermost stratosphere. To study the potential impact of these revised emission inventories, we employ the Whole Atmosphere Community Climate Model (WACCM), which enables us to project the future ozone depletion from CHBr3 under climate change scenarios and evaluate the necessity for regulatory measures to manage anthropogenic sources.

Description: Key Points: - A new CHBr3 emission inventory based on natural and anthropogenic sources suggests that the latter account for 12%–28% of the global emissions - In the NH, new anthropogenic estimates increase known natural CHBr3 emissions by up to 70.5%, leading to higher atmospheric CHBr3 levels - At the NH extratropical tropopause, CHBr3 is enhanced by 0.9 ppt Br due to anthropogenic sources thus doubling natural CHBr3 abundances Bromoform (CHBr3) contributes to stratospheric ozone depletion but is not regulated under the Montreal Protocol due to its short lifetime and large natural sources. Here, we show that anthropogenic sources contribute significantly to the amount of CHBr3 transported into the Northern Hemisphere (NH) extratropical stratosphere. We present a new CHBr3 emission inventory comprised of natural and anthropogenic sources, with the latter estimated from ship ballast, power plant cooling and desalination plant brine water. Including anthropogenic sources in the new inventory increases CHBr3 emissions by up to 31.5% globally and 70.5% in the NH. In consequence, atmospheric CHBr3 is also significantly higher, especially over the NH extratropics during boreal winter. Here anthropogenic sources enhance bromine at the tropopause by 0.9 ppt Br, thus doubling natural CHBr3 abundances. For some latitudes, tropopause bromine increases by 2.4 ppt Br suggesting significant contributions of anthropogenic CHBr3 to the NH lowermost stratosphere.

Description: To mitigate the rumen enteric methane (CH4) produced by ruminant livestock, Asparagopsis taxiformis is proposed as an additive to ruminant feed. During the cultivation of Asparagopsis taxiformis in the sea or in terrestrially based systems, this macroalgae, like most seaweeds and phytoplankton, produces a large amount of bromoform (CHBr3), which contributes to ozone depletion once released into the atmosphere. In this study, we focus on the impact of CHBr3 on the stratospheric ozone layer resulting from potential emissions from proposed Asparagopsis cultivation in Australia. The impact is assessed by weighting the emissions of CHBr3 with its ozone depletion potential (ODP), which is traditionally defined for long-lived halocarbons but has also been applied to very short-lived substances (VSLSs). An annual yield of ∼3.5 × 104 Mg dry weight is required to meet the needs of 50 % of the beef feedlot and dairy cattle in Australia. Our study shows that the intensity and impact of CHBr3 emissions vary, depending on location and cultivation scenarios. Of the proposed locations, tropical farms near the Darwin region are associated with the largest CHBr3 ODP values. However, farming of Asparagopsis using either ocean or terrestrial cultivation systems at any of the proposed locations does not have the potential to significantly impact the ozone layer. Even if all Asparagopsis farming were performed in Darwin, the CHBr3 emitted into the atmosphere would amount to less than 0.02 % of the global ODP-weighted emissions. The impact of remaining farming scenarios is also relatively small even if the intended annual yield in Darwin is scaled by a factor of 30 to meet the global requirements, which will increase the global ODP-weighted emissions up to ∼0.5 %.

Description: The Indian Ocean is coupled to atmospheric dynamics and chemical composition via several unique mechanisms, such as the seasonally varying monsoon circulation. During the winter monsoon season, high pollution levels are regularly observed over the entire northern Indian Ocean, while during the summer monsoon, clean air dominates the atmospheric composition, leading to distinct chemical regimes. The changing atmospheric composition over the Indian Ocean can interact with oceanic biogeochemical cycles and impact marine ecosystems, resulting in potential climate feedbacks. Here, we review current progress in detecting and understanding atmospheric gas-phase composition over the Indian Ocean and its local and global impacts. The review considers results from recent Indian Ocean ship campaigns, satellite measurements, station data, and information on continental and oceanic trace gas emissions. The distribution of all major pollutants and greenhouse gases shows pronounced differences between the landmass source regions and the Indian Ocean, with strong gradients over the coastal areas. Surface pollution and ozone are highest during the winter monsoon over the Bay of Bengal and the Arabian Sea coastal waters due to air mass advection from the Indo-Gangetic Plain and continental outflow from Southeast Asia. We observe, however, that unusual types of wind patterns can lead to pronounced deviations of the typical trace gas distributions. For example, the ozone distribution maxima shift to different regions under wind scenarios that differ from the regular seasonal transport patterns. The distribution of greenhouse gases over the Indian Ocean shows many similarities when compared to the pollution fields, but also some differences of the latitudinal and seasonal variations resulting from their long lifetimes and biogenic sources. Mixing ratios of greenhouse gases such as methane show positive trends over the Indian Ocean, but long-term changes in pollution and ozone due to changing emissions and transport patterns require further investigation. Although we know that changing atmospheric composition and perturbations within the Indian Ocean affect each other, the impacts of atmospheric pollution on oceanic biogeochemistry and trace gas cycling are severely understudied. We highlight potential mechanisms, future research topics, and observational requirements that need to be explored in order to fully understand such interactions and feedbacks in the Indian Ocean region.

Description: Bromoform is the major by-product from chlorination of cooling water in coastal power plants. The number of power plants in East and Southeast Asian economies has increased rapidly, exceeding mean global growth. Bottom-up estimates of bromoform emissions based on few measurements appear to under-represent the industrial sources of bromoform from East Asia. Using oceanic Lagrangian analyses, we assess the amount of bromoform produced from power plant cooling-water treatment in East and Southeast Asia. The spread of bromoform is simulated as passive particles that are advected using the three-dimensional velocity fields over the years 2005/2006 from the high-resolution NEMO-ORCA0083 ocean general circulation model. Simulations are run for three scenarios with varying initial bromoform concentrations based on the range of bromoform measurements in cooling-water discharge. Comparing the modelled anthropogenic bromoform to in situ observations in the surface ocean and atmosphere, the two lower scenarios show the best agreement, suggesting initial bromoform concentrations in cooling water to be around 20–60 µg L−1. Based on these two scenarios, the model produces elevated bromoform in coastal waters of East Asia with average concentrations of 23 and 68 pmol L−1 and maximum values in the Yellow Sea, Sea of Japan and East China Sea. The industrially produced bromoform is quickly emitted into the atmosphere with average air–sea flux of 3.1 and 9.1 nmolm−2h−1 , respectively. Atmospheric abundances of anthropogenic bromoform are derived from simulations with the Lagrangian particle dispersion model FLEXPART based on ERA-Interim wind fields in 2016. In the marine boundary layer of East Asia, the FLEXPART simulations show mean anthropogenic bromoform mixing ratios of 0.4–1.3 ppt, which are 2–6 times larger compared to the climatological bromoform estimate. During boreal winter, the simulations show that some part of the anthropogenic bromoform is transported by the northeasterly winter monsoon towards the tropical regions, whereas during boreal summer anthropogenic bromoform is confined to the Northern Hemisphere subtropics. Convective events in the tropics entrain an additional 0.04–0.05 ppt of anthropogenic bromoform into the stratosphere, averaged over tropical Southeast Asia. In our simulations, only about 10 % of anthropogenic bromoform is outgassed from power plants located in the tropics south of 20∘ N, so that only a small fraction of the anthropogenic bromoform reaches the stratosphere. We conclude that bromoform from cooling-water treatment in East Asia is a significant source of atmospheric bromine and might be responsible for annual emissions of 100–300 Mmol of Br in this region. These anthropogenic bromoform sources from industrial water treatment might be a missing factor in global flux estimates of organic bromine. While the current emissions of industrial bromoform provide a significant contribution to regional tropospheric budgets, they provide only a minor contribution to the stratospheric bromine budget of 0.24–0.30 ppt of Br.