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

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

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

Ground-based measurements of tropospheric and stratospheric bromine monoxide above Nairobi (1° S, 36° E)

International audienceGround based observations of stratospheric and tropospheric bromine monoxide, BrO, from a multi axial differential optical absorption spectrometer, MAXDOAS, located at the UNEP/UNON site in Nairobi (1° S, 36° E) are presented for the year 2003. Differences in BrO slant column densities at 90° and 80° solar zenith angle retrieved from the zenith-sky measurements are used to study stratospheric BrO. They show only small variations with season, as expected for the small seasonality in stratospheric Bry and NO2 in this region. A pronounced diurnal variation can be observed, the average value for the morning being 1.3×1014 molecules/cm2 and for the evening 1.5×1014 molecules/cm2. The measurements are compared with simulations from a one-dimensional photochemical stacked box model which is coupled with a radiative transfer model to allow direct comparisons between the observations and the model calculations. In general the model reproduces the measurements very well. The differences in the absolute values are 15% for the evening and 20% for the morning which is within the limits of the combined uncertainties. Both seasonality and diurnal variation are well reproduced by the model. A sensitivity study shows that inclusion of the reaction BrONO2 + O(3P) significantly improves the agreement between model calculations and measurements, indicating an important role of this reaction in the stratosphere near to the equator. Tropospheric BrO columns and profile information is derived from the combined results obtained in the different viewing directions for the average over several clear days. The resulting tropospheric BrO columns are in the range of 4?7.5×1012 molecules/cm2 which is significant but lower than in previous studies at mid and high latitudes. The vertical distribution of the tropospheric BrO peaks at about 3 km indicating the absence of local sources at this high altitude site