GoTriple - Study of the unknown HONO daytime source at a European suburban site during the MEGAPOLI summer and winter field campaigns

authors

Contributors

Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)) ; Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS),

Laboratoire de météorologie physique (LaMP) ; Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS),

Institut des Sciences Analytiques (ISA) ; Institut de Chimie du CNRS (INC)-Université Claude Bernard Lyon 1 (UCBL) ; Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS),

École des Mines de Douai (Mines Douai EMD) ; Institut Mines-Télécom [Paris] (IMT),

Université Lille Nord (France),

Centre d’Analyses et de Recherche ; Centre d’Analyses et de Recherche - Lebanon,

TROPO - LATMOS ; Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS) ; Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS),

Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E) ; Observatoire des Sciences de l'Univers en région Centre (OSUC) ; Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris ; Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris ; Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES),

Paul Scherrer Institute (PSI),

Institut Pierre-Simon-Laplace (IPSL) ; École normale supérieure - Paris (ENS Paris) ; Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National d'Études Spatiales [Toulouse] (CNES)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X),

ANR-09-BLAN-0356,MEGAPOLI-PARIS,MEGAPOLI - PARIS : Pollution des AéRosols: Impact sur la qualité de l'air et quantification des Sources(2009),

ANR-10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010),

European Project: 212520,EC:FP7:ENV,FP7-ENV-2007-1,MEGAPOLI(2008),

European Project: 228335,EC:FP7:INFRA,FP7-INFRASTRUCTURES-2008-1,EUROCHAMP-2(2009)

+ 14

Publisher

HAL CCSD,

European Geosciences Union

Abstract

International audience Nitrous acid measurements were carried out during the MEGAPOLI summer and winter field campaigns at SIRTA observatory in Paris surroundings. Highly variable HONO levels were observed during the campaigns, ranging from 10 ppt to 500 ppt in summer and from 10 ppt to 1.7 ppb in winter. Significant HONO mixing ratios have also been measured during daytime hours, comprised between some tenth of ppt and 200 ppt for the summer campaign and between few ppt and 1 ppb for the winter campaign. Ancillary measurements, such as NOx , O3 , photolysis frequencies, meteorological parameters (pressure, temperature, relative humidity , wind speed and wind direction), black carbon concentration , total aerosol surface area, boundary layer height and soil moisture, were conducted during both campaigns. In addition, for the summer period, OH radical measurements were made with a CIMS (Chemical Ionisation Mass Spectrometer). This large dataset has been used to investigate the HONO budget in a suburban environment. To do so, calculations of HONO concentrations using PhotoStationary State (PSS) approach have been performed, for daytime hours. The comparison of these calculations with measured HONO concentrations revealed an underestimation of the calculations making evident a missing source term for both campaigns. This unknown HONO source exhibits a bell-shaped like average diurnal profile with a maximum around noon of approximately 0.7 ppb h−1 and 0.25 ppb h−1 , during summer and winter respectively. This source is the main HONO source during daytime hours for both campaigns. In both cases, this source shows a slight positive correlation with J (NO2) and the product between J (NO2) and soil moisture. This original approach had, thus, indicated that this missing source is photolytic and might be heterogeneous occurring at ground surface and involving water content available on the ground. Published by Copernicus Publications on behalf of the European Geosciences Union. 2806 V. Michoud et al.: Study of the unknown HONO daytime source