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Hydrocarbons are key precursors to two priority air pollutants, ozoneand particulate matter. Those with two to seven carbons havehistorically been straightforward to observe and have beensuccessfully reduced in many developed cities through air qualitypolicy interventions. Longer chain hydrocarbons released from dieselvehicles are not considered explicitly as part of air qualitystrategies and there are few direct measurements of their gaseousabundance in the atmosphere. This study describes the chemicallycomprehensive and continuous measurements of organic compounds ina developed megacity (London), which demonstrate that on a seasonalmedian basis, diesel-related hydrocarbons represent only20–30 % of the total hydrocarbon mixing ratio but comprisemore than 50 %  of the atmospheric hydrocarbon mass and area dominant local source of secondary organic aerosols. This studyshows for the first time that 60 %  of the winter primaryhydrocarbon hydroxyl radical reactivity is from diesel-relatedhydrocarbons and using the maximum incremental reactivity scale, wepredict that they contribute up to 50 %  of the ozoneproduction potential in London. Comparing real-world urban compositionwith regulatory emissions inventories in the UK and US highlightsa previously unaccounted for, but very significant, under-reporting ofdiesel-related hydrocarbons; an underestimation of a factor ~4for C<sub>9</sub> species rising to a factor of over 70 for C<sub>12</sub>during winter. These observations show that hydrocarbons from dieselvehicles can dominate gas phase reactive carbon in cities with highdiesel fleet fractions. Future control of urban particulate matter andozone in such locations requires a shift in policy focus onto gasphase hydrocarbons released from diesels as this vehicle typecontinues to displace gasoline world-wide

Diesel-related hydrocarbons can dominate gas phase reactive carbon in megacities