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Abstract

The budget of reactive nitrogen species, which play a central role in atmospheric chemistry (e.g. in photochemical O3 production), is poorly understood in forested regions. In this study, through observations of NO, NO2, NOy, and O3 in the Rambouillet Forest near Paris, France, we have examined nighttime processes controlling NOx in an anthropogenically impacted forest environment. The O3 mixing ratios displayed a strong diel profile at the site that was driven by a variable but generally rapid deposition to soil and foliar surfaces. The O3 diel profile was strongly influenced by relative humidity and temperature inversion. Only when the O3 mixing ratio was sufficiently low (and thus the NO lifetime sufficiently long) were sustained NO peaks observed above the instrumental detection limit, enabling the derivation of average NO emission rates of ∼1.4 ppbv h−1 from the soil. Observations of the lack of increase in NO2 at night, despite a significant production rate from the reaction of NO with O3, enabled an effective lifetime of NO2 of ∼0.5–3 h to be derived. As the loss of NO2 was not compensated for by the formation of gas- or particle-phase reactive nitrogen species, it was presumably either driven by deposition to soil and foliar surfaces or any products formed were themselves short-lived with respect to deposition. By comparison, the daytime lifetime of NO2 with respect to loss by reaction with OH is about 1 d. Our results indicate that the nighttime deposition of NO2 is a major sink of boundary layer NOx in this temperate forest environment.