The contribution of anthropogenic bromine emissions to past stratospheric ozone trends: a modelling study

International audienceBromine compounds play an important role in the depletion of stratospheric ozone. We have calculated the changes in stratospheric ozone in response to changes in the halogen loading over the past decades, using a two-dimensional (latitude/height) model constrained by source gas mixing ratios at the surface. Model calculations of the decrease of total column ozone since 1980 agree reasonably well with observed ozone trends, in particular when the contribution from very short-lived bromine compounds is included. Model calculations with bromine source gas mixing ratios fixed at 1959 levels, corresponding approximately to a situation with no anthropogenic bromine emissions, show an ozone column reduction between 1980 and 2005 at northern hemisphere mid-latitudes of only ?55% compared to a model run including all halogen source gases. In this sense anthropogenic bromine emissions are responsible for ?45% of the model estimated column ozone loss at northern hemisphere mid-latitudes. The chemical efficiency of bromine relative to chlorine for global total ozone depletion from our model calculations, expressed by the so called ?-factor, is about 73 on an annual average. This value is much higher than previously published results. Updates in reaction rate constants can explain only part of the differences in ?. The inclusion of bromine from very short-lived source gases has only a minor effect on the global mean ?-factor

The contribution of anthropogenic bromine emissions to past stratospheric ozone trends: a modelling study

Bromine compounds play an important role in the depletion of stratospheric ozone. We have calculated the changes in stratospheric ozone in response to changes in the halogen loading over the past decades, using a two-dimensional (latitude/height) model constrained by source gas mixing ratios at the surface. Model calculations of the decrease of total column ozone since 1980 agree reasonably well with observed ozone trends, in particular when the contribution from very short-lived bromine compounds is included. Model calculations with bromine source gas mixing ratios fixed at 1959 levels, corresponding approximately to a situation with no anthropogenic bromine emissions, show an ozone column reduction between 1980 and 2005 at Northern Hemisphere mid-latitudes of only ≈55% compared to a model run including all halogen source gases. In this sense anthropogenic bromine emissions are responsible for ≈45% of the model estimated column ozone loss at Northern Hemisphere mid-latitudes. However, since a large fraction of the bromine induced ozone loss is due to the combined BrO/ClO catalytic cycle, the effect of bromine would have been smaller in the absence of anthropogenic chlorine emissions. The chemical efficiency of bromine relative to chlorine for global total ozone depletion from our model calculations, expressed by the so called α-factor, is 64 on an annual average. This value is much higher than previously published results. Updates in reaction rate constants can explain only part of the differences in α. The inclusion of bromine from very short-lived source gases has only a minor effect on the global mean α-factor

Estimating the contribution of bromoform to stratospheric bromine and its relation to dehydration in the tropical tropopause layer

International audienceThe contribution of bromoform to the stratospheric bromine loading is estimated using the one-dimensional tropical mean model of Folkins and Martin (2005), which is constrained by observed mean profiles of temperature and humidity. In order to reach the stratosphere, bromoform needs to be lifted by deep convection into the tropical tropopause layer (TTL), above the level of zero radiative heating. The contribution of bromoform to stratospheric bromine then depends critically on the rate of removal of the degradation products of bromoform (collectively called Bry here) from the TTL, which is believed to be due to scavenging by falling ice. This relates the transport of short-lived bromine species into the stratosphere to processes of dehydration in the TTL. In the extreme case of dehydration occurring only through overshooting deep convection, the loss of Bry from the TTL may be negligible and consequently bromoform will fully contribute with its boundary layer mixing ratio to the stratospheric bromine loading, i.e. with 3 pptv for an assumed 1 pptv of bromoform in the boundary layer. For the other extreme that Bry is removed from the TTL almost instantaneously, the model calculations predict a contribution of about 0.5 pptv for the assumed 1 pptv of boundary layer bromoform. While this gives some constraints on the contribution of bromoform to stratospheric bromine, a key uncertainty in estimating the contribution of short-lived bromine source gases to the stratospheric bromine loading is the mechanism and rate of removal of Bry within the TTL

Rapid meridional transport of tropical airmasses to the Arctic during the major stratospheric warming in January 2003

International audienceWe present observations of unusually high values of ozone and N2O in the middle stratosphere that were observed by the airborne submillimeter radiometer ASUR in the Arctic. The observations took place in the meteorological situation of a major stratospheric warming that occurred in mid-January 2003 and was dominated by a wave 2 event. On 23 January 2003 the observed N2O and O3 mixing ratios around 69° N in the middle stratosphere reached maximum values of ~190 ppb and ~10 ppm, respectively. The similarities of these N2O profiles in a potential temperature range between 800 and 1200 K with N2O observations around 20° N on 1 March 2003 by the same instrument suggest that the observed Arctic airmasses were transported from the tropics quasi-isentropically. This is confirmed by 5-day back trajectory calculations which indicate that the airmasses between about 800 and 1000 K had been located around 20° N 3?5 days prior to the measurement in the Arctic. Calculations with a linearized ozone chemistry model along calculated as well as idealized trajectories, initialized with the low-latitude ASUR ozone measurements, give reasonable agreement with the Arctic ozone measurement by ASUR. PV distributions suggest that these airmasses did not stay confined in the Arctic region which makes it unlikely that this dynamical situation lead to the formation of dynamically caused pockets of low ozone

Impact of deep convection and dehydration on bromine loading in the upper troposphere and lower stratosphere

Stratospheric bromine loading due to very short-lived substances is investigated with a three-dimensional chemical transport model over a period of 21 years using meteorological input data from the European Centre for Medium-Range Weather Forecasts ERA-Interim reanalysis from 1989 to the end of 2009. Within this framework we analyze the impact of dehydration and deep convection on the amount of stratospheric bromine using an idealized and a detailed full chemistry approach. We model the two most important brominated short-lived substances, bromoform (CHBr<sub>3</sub>) and dibromomethane (CH<sub>2</sub>Br<sub>2</sub>), assuming a uniform convective detrainment mixing ratio of 1 part per trillion by volume (pptv) for both species. The contribution of very short-lived substances to stratospheric bromine varies drastically with the applied dehydration mechanism and the associated scavenging of soluble species ranging from 3.4 pptv in the idealized setup up to 5 pptv using the full chemistry scheme. In the latter case virtually the entire amount of bromine originating from very short-lived source gases is able to reach the stratosphere thus rendering the impact of dehydration and scavenging on inorganic bromine in the tropopause insignificant. Furthermore, our long-term calculations show that the mixing ratios of very short-lived substances are strongly correlated to convective activity, i.e. intensified convection leads to higher amounts of very short-lived substances in the upper troposphere/lower stratosphere especially under extreme conditions like El Niño seasons. However, this does not apply to the inorganic brominated product gases whose concentrations are anti-correlated to convective activity mainly due to convective dilution and possible scavenging, depending on the applied approach

Space-borne measurements of mesospheric magnesium species ? a retrieval algorithm and preliminary profiles

International audienceWe present a joint retrieval as well as first results for mesospheric air density and mesospheric Magnesium species (Mg and Mg+) using limb data from the SCIAMACHY instrument on board the European ENVISAT satellite.considered. These species feature Metallic species like neutral Mg, ionized Mg+ and others (Fe, Si, Li, etc.) ablate from meteoric dust, enter the gas phase and occur at high altitudes (?70 km). Emissions from these species are clearly observed in the SCIAMACHY limb measurements. These emissions are used to retrieve total and thermospheric column densities as well as preliminary profiles of metallic species in the altitude range of 70?92 km. In this paper, neutral Magnesium as well as its ionized counterpart Mg+ is considered. These species feature resonance fluorescence in the wavelength range 279 and 285 nm and thus have a rather simple excitation process. A radiative transfer model (RTM) for the mesosphere has been developed and validated. Based on a ray tracing kernel, radiances in a large wavelength range from 240?300 nm covering limb as well as nadir geometry can be calculated. The forward model has been validated and shows good agreement with established models in the given wavelength range and a large altitude range. The RTM has been coupled to a retrieval based on Optimal Estimation. Air density is retrieved from Rayleigh backscattered light. Mesospheric Mg and Mg+ number densities are retrieved from their emission signals observed in the limb scans of SCIAMACHY. Other species like iron, silicon, OH and NO can be investigated in principle with the same algorithm. Based on the retrieval presented here, SCIAMACHY offers the opportunity to investigate mesospheric species on a global scale and with good vertical resolution for the first time

INCREASE: An updated model suite to study the INfluence of Cosmic Rays on Exoplanetary AtmoSpherEs

Exoplanets are as diverse as they are fascinating. They vary from ultrahot Jupiter-like low-density planets to presumed gas-ice-rock mixture worlds such as GJ 1214b or worlds as LHS 1140b, which features twice the Earth\u27s bulk density. Regarding the great diversity of exoplanetary atmospheres, much remains to be explored. For a few selected objects such as GJ1214b, Proxima Centauri b, and the TRAPPIST-1 planets, the first observations of their atmospheres have already been achieved or are expected in the near future with the launch of the James Webb Space Telescope envisaged in October 2021. However, in order to interpret these observations, model studies of planetary atmospheres that account for various processes—such as atmospheric escape, outgassing, climate, photochemistry, as well as the physics of air showers and the transport of stellar energetic particles and galactic cosmic rays through the stellar astrospheres and planetary magnetic fields—are necessary. Here, we present our model suite INCREASE, a planned extension of the model suite discussed in Herbst, Grenfell, et al. (2019)

Towards a climatology of stratospheric bromine monoxide from SCIAMACHY limb observations

International audienceRetrievals of stratospheric bromine monoxide (BrO) profiles from two years of limb measurements from the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) instrument onboard ENVISAT are analysed and a global climatology of stratospheric BrO is prepared. A comparison of the SCIAMACHY BrO retrievals with a set of four balloon-borne BrO profiles shows mean relative differences in the altitude range from 18 to 30 km between ?42%. The SCIAMACHY BrO observations provide for the first time a picture of the seasonal variation of stratospheric BrO on a global scale. At mid-latitudes of both hemispheres BrO shows a strong seasonal cycle with a maximum in winter and a minimum in summer. The seasonal variation of BrO is closely correlated with changes in nitrogen dioxide (NO2), confirming our present understanding of gas phase bromine chemistry. Using the SCIAMACHY BrO observations together with the calculated bromine partitioning from a photochemical model constrained by the SCIAMACHY NO2 observations, the total stratospheric bromine loading is estimated to be 18.5±4 pptv. This indicates a contribution of about 3.5±4 pptv from short lived bromine species in addition to methyl bromide and the halons

On the climatological probability of the vertical propagation of stationary planetary waves

We introduce a diagnostic tool to assess a climatological framework of the optimal propagation conditions for stationary planetary waves. Analyzing 50 winters using NCEP/NCAR (National Center for Environmental Prediction/National Center for Atmospheric Research) reanalysis data we derive probability density functions (PDFs) of positive vertical wave number as a function of zonal and meridional wave numbers. We contrast this quantity with classical climatological means of the vertical wave number. Introducing a membership value function (MVF) based on fuzzy logic, we objectively generate a modified set of PDFs (mPDFs) and demonstrate their superior performance compared to the climatological mean of vertical wave number and the original PDFs. We argue that mPDFs allow an even better understanding of how background conditions impact wave propagation in a climatological sense. As expected, probabilities are decreasing with increasing zonal wave numbers. In addition we discuss the meridional wave number dependency of the PDFs which is usually neglected, highlighting the contribution of meridional wave numbers 2 and 3 in the stratosphere. We also describe how mPDFs change in response to strong vortex regime (SVR) and weak vortex regime (WVR) conditions, with increased probabilities of the wave propagation during WVR than SVR in the stratosphere. We conclude that the mPDFs are a convenient way to summarize climatological information about planetary wave propagation in reanalysis and climate model data