Journal
ATMOSPHERIC CHEMISTRY AND PHYSICS
Volume 15, Issue 18, Pages 10777-10798Publisher
COPERNICUS GESELLSCHAFT MBH
DOI: 10.5194/acp-15-10777-2015
Keywords
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Funding
- Cryosphere-Atmosphere Interactions in a Changing Arctic Climate (CRAICC)
- Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning FORMAS [214-2014-1445]
- Maj and Tor Nessling foundation [2009362]
- Academy of Finland [128731]
- program in Atmospheric Sciences (ATM-DP) at the University of Helsinki
- PEGASOS (Pan-European Gas-Aerosolsclimate interaction Study) project [FP7-ENV-2010-265148]
- Academy of Finland (AKA) [128731, 128731] Funding Source: Academy of Finland (AKA)
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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 Julich 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 (R-2 > 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.
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