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Spectral measurements of BrO using zenith-sky and off-axis viewinggeometries are combined in a linear multiple regression retrieval algorithmto provide stratospheric and tropospheric BrO vertical columns. One year ofmeasurement data are investigated over Reunion-Island (20.9° S, 55.5° E),from August 2004 to June 2005. A comparison between the stratosphericcolumns retrieved at 45°, 80°, 85°, 87.5° and92.5°solar zenith angles and photochemical simulations initialized by chemicalfields from the 3-D-CTM SLIMCAT and further constrained by observed NO2profiles shows a good agreement only by considering a contribution from thevery short-lived organic bromine substances to the stratospheric inorganicbromine budget, of 6 to 8 pptv. Furthermore, stratospheric BrO profilesretrieved from late twilight zenith-sky observations are consistent with atotal inorganic bromine (Bry) loading of approximately 23 pptv. Thisrepresents 6 to 7 pptv more than can be supplied by long-lived organicbromine sources, and therefore supports an added contribution from veryshort-lived organic bromine substances as recently suggested in severalother studies. Moreover strong evidences are presented for the existence ofa substantial amount of BrO in the tropical free-troposphere, around 6 kmaltitude, possibly supplied by the decomposition of short-lived biogenicbromine organic compounds. Tropospheric BrO vertical columns of 1.1±0.45×1013 molec/cm² are derived for the entire observationperiod. Comparisons between ground-based BrO vertical columns and total BrOcolumns derived from SCIAMACHY (onboard the ENVISAT satellite) nadirobservations in a latitudinal band centered around 21° S present a goodlevel of consistency, which further strengthens the conclusions of ourstudy

Retrieval of stratospheric and tropospheric BrO columns from multi-axis DOAS measurements at Reunion Island (21° S, 56° E)