F. Arnold et al., OBSERVATION OF UPPER-TROPOSPHERIC SULFUR-DIOXIDE-POLLUTION AND ACETONE-POLLUTION - POTENTIAL IMPLICATIONS FOR HYDROXYL RADICAL AND AEROSOL FORMATION, Geophysical research letters, 24(1), 1997, pp. 57-60
Aircraft-based measurements of sulfur dioxide, acetone, carbon dioxide
, and condensation nuclei (CN) were made over the north-eastern Atlant
ic at upper tropospheric altitudes, around 9000 m. On October 14, 1993
, strong SO2- and acetone-pollution (both up to 3 ppbv) were observed,
which were accompanied by a CO2-enhancement of up to 6 ppmv, and larg
e CN-concentrations of up to about 1500 cm(-3) (for radii greater than
or equal to 6 nm). CN, excess CO2, and to a lesser degree also aceton
e, were positively correlated with SO2. Air mass trajectory analyses i
ndicate, that most of the air masses encountered by our aircraft origi
nated from the polluted planetary boundary layer of the North-Eastern
U. S. approximately 4-5 days prior to our measurements, and that pollu
ted boundary layer air experienced fast vertical transport to the uppe
r troposphere as well as horizontal transport across the Atlantic. Fro
m our data we conclude, that in the polluted air mass around 9000 m al
titude HOx-formation, photochemical SO2-conversion to gaseous H2SO4, a
nd eventually also CN-formation by homogeneous bimolecular (H2SO4-H2O)
nucleation may have taken place with enhanced efficiency.