1. Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Jülich plant atmosphere chamber
- Author
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Mikael Ehn, Jürgen Wildt, Einhard Kleist, Markku Kulmala, Veli-Matti Kerminen, Li Liao, Ralf Tillmann, Anton Rusanen, Astrid Kiendler-Scharr, Thomas F. Mentel, Pontus Roldin, M. Dal Maso, Michael Boy, Ditte Mogensen, Department of Physics, Ecosystem processes (INAR Forest Sciences), and Aerosol-Cloud-Climate -Interactions (ACCI)
- Subjects
Activity coefficient ,Atmospheric Science ,Particle number ,Nucleation ,114 Physical sciences ,Atmosphere ,lcsh:Chemistry ,THERMODYNAMIC MODEL ,Phase (matter) ,SULFURIC-ACID CONCENTRATION ,ddc:550 ,ACTIVITY-COEFFICIENTS ,Surface layer ,AEROSOL WALL LOSSES ,EMISSIONS ,Chemistry ,lcsh:QC1-999 ,OXIDATION-PRODUCTS ,Aerosol ,TROPOSPHERIC DEGRADATION ,Chemical engineering ,lcsh:QD1-999 ,13. Climate action ,GAS ,Environmental chemistry ,Particle ,GROWTH ,lcsh:Physics ,NUCLEATION - Abstract
We used the Aerosol Dynamics gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM) to simulate the contribution of BVOC plant emissions to the observed new particle formation during photooxidation experiments performed in the Jülich Plant-Atmosphere Chamber and to evaluate how well smog chamber experiments can mimic the atmospheric conditions during new particle formation events. ADCHAM couples the detailed gas-phase chemistry from Master Chemical Mechanism with a novel aerosol dynamics and particle phase chemistry module. Our model simulations reveal that the observed particle growth may have either been controlled by the formation rate of semi- and low-volatility organic compounds in the gas phase or by acid catalysed heterogeneous reactions between semi-volatility organic compounds in the particle surface layer (e.g. peroxyhemiacetal dimer formation). The contribution of extremely low-volatility organic gas-phase compounds to the particle formation and growth was suppressed because of their rapid and irreversible wall losses, which decreased their contribution to the nano-CN formation and growth compared to the atmospheric situation. The best agreement between the modelled and measured total particle number concentration (R2 > 0.95) was achieved if the nano-CN was formed by kinetic nucleation involving both sulphuric acid and organic compounds formed from OH oxidation of BVOCs.
- Published
- 2015
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