The concentrations of dimethyl sulfide in air were obtained during a cruise between the United Kingdom and the Antarctic in the period October 1992 to January 1993 using a method of sampling and analysis optimized to avoid interferences from oxidants. In equatorial regions (30°N to 30°S) the atmospheric DMS concentration ranged from 3 to 46 ng (S) m−3, with an average of 18 ng (S) m−3. In the polar waters and regions south of the Falkland Islands, concentrations from 3 to 714 ng (S) m−3 were observed, with a mean concentration of 73 ng (S) m−3. The concentrations of a range of DMS oxidation products were also obtained. No clear relationships between reactant and product concentrations were seen. Information on particle number concentration, Fuchs surface area and the thermal volatility characteristics of the ambient aerosol was obtained, but again no clear relationships with sulfur concentrations were observed. Accumulation mode particle concentrations averaged 25 cm−3 in the clean marine and polar air masses south of 58°S while background condensation nuclei (CN) concentrations were of the order of 400–600 cm−3. Simplistic calculations suggest that a particle source strength of about 20–60 particles cm−3 d−1 is required to sustain this background CN concentration. It is not clear whether boundary layer nucleation of new CN or entrainment from the free troposphere provided the source of CN. Periods of elevated CN concentrations (>4000 cm−3) were regularly observed in the boundary layer over the Weddell Sea and were attributed to “bursts” of new particle formation. However, shortly after these nucleation events the CN concentration rapidly decayed to the background level through coagulation losses, suggesting little impact on the background CN or cloud condensation nuclei (CCN) concentration.