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. To better understand the formation and the oxidation pathwaysleading to gypsum-forming “black crusts” and investigate their bearing onthe whole atmospheric SO2 cycle, we measured the oxygen (δ17O, δ18O, and Δ17O) and sulfur (δ33S, δ34S, δ36S, Δ33S, andΔ36S) isotopic compositions of black crust sulfates sampled oncarbonate building stones along a NW–SE cross section in the Parisian basin.The δ18O and δ34S values, ranging between 7.5 ‰ and 16.7±0.5 ‰ (n=27, 2σ) and between −2.66 ‰and 13.99±0.20 ‰, respectively, showanthropogenic SO2 as the main sulfur source (from ∼2 % to81 %, average ∼30 %) with host-rock sulfates making thecomplement. This is supported by Δ17O values (up to 2.6 ‰, on average ∼0.86 ‰), requiring&gt; 60 % of atmosphericsulfates in black crusts. Negative Δ33S and Δ36S values between −0.34 ‰ and 0.00±0.01 ‰and between −0.76 ‰ and -0.22±0.20 ‰, respectively,were measured in black crust sulfates, which is typical of a magnetic isotopeeffect that would occur during the SO2 oxidation on the building stone,leading to 33S depletion in black crust sulfates and subsequent33S enrichment in residual SO2. Except for a few samples, sulfateaerosols mostly have Δ33S values &gt; 0 ‰,and no processes can yet explain this enrichment, resulting in aninconsistent S budget: black crust sulfates could well represent thecomplementary negative Δ33S reservoir of the sulfate aerosols, thussolving the atmospheric SO2 budget.

atmospheric chemistry and physics

Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative Δ&amp;lt;sup&amp;gt;33&amp;lt;/sup&amp;gt;S reservoir of sulfate aerosols?