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. Sulfates present in urban aerosols collected worldwide usuallyexhibit significant non-zero Δ33S signatures (from −0.6  ‰ to 0.5 ‰) whose origin still remains unclear. Tobetter address this issue, we recorded the seasonal variations of themultiple sulfur isotope compositions of PM10 aerosols collectedover the year 2013 at five stations within the Montreal Island (Canada), eachcharacterized by distinct types and levels of pollution. The δ34S -values ( n=  155) vary from 2.0 ‰ to11.3 ‰ ( ±0.2  ‰, 2 σ ), the Δ33S -values from −0.080  ‰ to 0.341 ‰ ( ±0.01  ‰, 2 σ ) and the Δ36S -values from −1.082  ‰ to 1.751 ‰ ( ±0.2  ‰, 2 σ ).Our study evidences a seasonality for both the δ34S and Δ33S , which can be observed either when considering allmonitoring stations or, to a lesser degree, when considering themindividually. Among them, the monitoring station located at the most westernend of the island, upstream of local emissions, yields the lowest mean δ34S coupled to the highest mean Δ33S -values.The Δ33S -values are higher during both summer and winter, andare < 0.1 ‰ during both spring and autumn. As these higher Δ33S -values are measured in “upstream” aerosols, we concludethat the mechanism responsible for these highly positive S-MIF also occursoutside and not within the city, at odds with common assumptions. While theorigin of such variability in the Δ33S -values of urbanaerosols (i.e. −0.6  ‰ to 0.5 ‰) is still subject todebate, we suggest that oxidation by Criegee radicals and/or photooxidationof atmospheric SO2 in the presence of mineral dust may play a rolein generating such large ranges of S-MIF.

atmospheric chemistry and physics

Seasonality in the Δ&amp;lt;sup&amp;gt;33&amp;lt;/sup&amp;gt;S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;