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. Organosulfur compounds are found to be ubiquitous in atmospheric aerosols– a majority of which are expected to be organosulfates (OSs). Given theatmospheric abundance of OSs, and their potential to form a variety ofreaction products upon aging, it is imperative to study the transformationkinetics and chemistry of OSs to better elucidate their atmospheric fatesand impacts. In this work, we investigated the chemical transformation of anα-pinene-derived organosulfate (C10H17O5SNa, αpOS-249) through heterogeneous OH oxidation at a relative humidity of 50 % in an oxidation flow reactor (OFR). The aerosol-phase reaction productswere characterized using high-performance liquidchromatography–electrospray ionization–high-resolution mass spectrometry and ion chromatography. By monitoring the decay rates of αpOS-249,the effective heterogeneous OH reaction rate was measured to be (6.72±0.55)×10-13 cm3 molecule−1 s−1. Thisinfers an atmospheric lifetime of about 2 weeks at an average OHconcentration of 1.5×106 molecules cm−3. Productanalysis shows that OH oxidation of αpOS-249 can yield moreoxygenated OSs with a nominal mass-to-charge ratio (m/z) at 247(C10H15O5S−), 263 (C10H15O6S−), 265(C10H17O6S−), 277 (C10H13O7S−), 279(C10H15O7S−), and 281 (C10H17O7S−). The formation of fragmentation products,including both small OSs (C &lt;10) and inorganic sulfates, is foundto be insignificant. These observations suggest that functionalizationreactions are likely the dominant processes and that multigenerationaloxidation possibly leads to formation of products with one or two hydroxyland carbonyl functional groups adding to αpOS-249. Furthermore, allproduct ions except m/z=277 have been detected in laboratory-generatedα-pinene-derived secondary organic aerosols as well as inatmospheric aerosols. Our results reveal that OSs freshly formed from thephotochemical oxidation of α-pinene could react further to form OSscommonly detected in atmospheric aerosols through heterogeneous OHoxidation. Overall, this study provides more insights into the sources,transformation, and fate of atmospheric OSs.

atmospheric chemistry and physics

Chemical transformation of &amp;lt;i&amp;gt;α&amp;lt;/i&amp;gt;-pinene-derived organosulfate via heterogeneous OH oxidation: implications for sources and environmental fates of atmospheric organosulfates