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Speciation analysis of iodine in aerosols is a very useful approach forunderstanding geochemical cycling of iodine in the atmosphere. In this study,overall iodine species, including water-soluble iodine species (iodide,iodate and water-soluble organic iodine), NaOH-soluble iodine, and insolubleiodine have been determined for 129I and 127I in the aerosolscollected at Risø, Denmark, during March and May 2011 (shortly after theFukushima nuclear accident) and in December 2014. The measured concentrationsof total iodine are in the range of 1.04–2.48 ng m−3 for 127Iand (11.3–97.0)  ×  105 atoms m−3 for 129I,corresponding to 129I ∕ 127I atomic ratios of(17.8–86.8)  ×  10−8. The contribution of Fukushima-derived129I (peak value of 6.3  ×  104 atoms m−3) isestimated to be negligible (less than 6 %) compared to the total129I concentration in northern Europe. The concentrations andspecies of 129I and 127I in the aerosols are found to be stronglyrelated to their sources and atmospheric pathways. Aerosols that weretransported over the contaminated seas contained higher concentrations of129I than aerosols transported over the European continent. The high129I concentrations of the marine aerosols are attributed to secondaryemission of marine discharged 129I in the contaminated seawater in theNorth Sea, North Atlantic Ocean, English Channel, Kattegat, etc., rather thandirect gaseous release from the European nuclear reprocessing plants (NRPs).Water-soluble iodine was found to be a minor fraction to the total iodine forboth 127I (7.8–13.7 %) and 129I (6.5–14.1 %) inocean-derived aerosols, but accounted for 20.2–30.3 % for 127I and25.6–29.5 % for 129I in land-derived aerosols. Iodide was thepredominant form of water-soluble iodine, accounting for more than 97 %of the water-soluble iodine. NaOH-soluble iodine seems to be independent ofthe sources of aerosols. The significant proportion of 129I and127I found in NaOH-soluble fractions is likely bound with organicsubstances. In contrast to water-soluble iodine, the sources of airmasses exerted distinct influences on insoluble iodine for both 129I and127I, with higher values for marine air masses and lower values forterrestrial air masses

atmospheric chemistry and physics

Speciation of &amp;lt;sup&amp;gt;127&amp;lt;/sup&amp;gt;I and &amp;lt;sup&amp;gt;129&amp;lt;/sup&amp;gt;I in atmospheric aerosols at Risø, Denmark: insight into sources of iodine isotopes and their species transformations