modelling the contribution of biogenic volatile organic compounds to new particle formation in the jülich plant atmosphere chamber
;P. Roldin;L. Liao;D. Mogensen;M. Dal Maso;A. Rusanen;V.-M. Kerminen;T. F. Mentel;J. Wildt;E. Kleist;A. Kiendler-Scharr;R. Tillmann;M. Ehn;M. Kulmala;M. Boy
Journal of agricultural and food chemistry2015Vol. 15pp. 10777-10798
157
roldin2015atmosphericmodelling
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.