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Submicron aerosol composition measurements

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Submicron aerosol composition measurements during ACRIDICON-CHUVA: Indications for secondary organic aerosol formation in the upper tropical troposphere March 1, 2016 ACRIDICON-CHUVA Workshop Christiane
Submicron aerosol composition measurements during ACRIDICON-CHUVA: Indications for secondary organic aerosol formation in the upper tropical troposphere March 1, 2016 ACRIDICON-CHUVA Workshop Christiane Schulz, Johannes Schneider, Stephan Borrmann Stephan Mertes, Udo Kästner Francesco Canonaco MPI Chemistry Mainz, Gutenberg University Mainz, Germany TROPOS Leipzig, Germany PSI Villingen, Switzerland Instrument C-ToF-AMS Compact Time-of-Flight Aerosol Mass Spectrometer Sub-micron non-refractory particle composition (approx. PM1) Species: organics, sulfate, nitrate, ammonium, chloride Quantitative measurements Time resolution: 30 s Size range: nm Expected results: Particle composition Mass concentration Vertical profiles C-ToF-AMS in HALO J. Schneider, ACRIDICON-CHUVA campaign, Manaus, Brazil, Instrument C-ToF-AMS HASI CVI Pressure controlled inlet p p J. Schneider, ACRIDICON-CHUVA campaign, Manaus, Brazil, Instrument C-ToF-AMS HASI CVI Pressure controlled inlet p p J. Schneider, ACRIDICON-CHUVA campaign, Manaus, Brazil, Instrument C-ToF-AMS HASI CVI Pressure controlled inlet p p J. Schneider, ACRIDICON-CHUVA campaign, Manaus, Brazil, Instrument C-ToF-AMS HASI CVI Pressure controlled inlet p p J. Schneider, ACRIDICON-CHUVA campaign, Manaus, Brazil, Instrument C-ToF-AMS HASI CVI Pressure controlled inlet p p J. Schneider, ACRIDICON-CHUVA campaign, Manaus, Brazil, Instrument C-ToF-AMS HASI CVI Pressure controlled inlet p p J. Schneider, ACRIDICON-CHUVA campaign, Manaus, Brazil, Instrument C-ToF-AMS HASI CVI Pressure controlled inlet p p J. Schneider, ACRIDICON-CHUVA campaign, Manaus, Brazil, Vertical Profiles ACRIDICON-CHUVA Aerosol Measurements Organics Nitrate Sulfate Vertical Profiles ACRIDICON-CHUVA Aerosol Measurements Maximum at low altitudes Organics Nitrate Sulfate Vertical Profiles ACRIDICON-CHUVA Aerosol Measurements Decrease at middle altitudes Organics Nitrate Sulfate Vertical Profiles ACRIDICON-CHUVA Aerosol Measurements Increase at high altitudes for organics and nitrate But not for sulfate Organics Nitrate Sulfate Vertical Profiles ACRIDICON-CHUVA Aerosol Measurements Vertical or long range transport? Cloud processing? Formation? Condensation? Increase at high altitudes for organics and nitrate But not for sulfate Organics Nitrate Sulfate Vertical Profiles ACRIDICON-CHUVA Aerosol Measurements AC AC 11: Outflow flight with tracer sampling Organics Nitrate Sulfate Vertical Profile AC Flight Path AC Flight Path AC 11 colour coded with organic mass concentration Flight Path AC 11 colour coded with organic mass concentration Flight Path AC11 High altitude (11-12 km) Outflow Influence of Manaus Time Series AC 11 HASI only Time Series AC 11 Influence of Manaus HASI only Time Series AC 11 Influence of Manaus HASI only Time Series AC 11 Influence of Manaus: Similar aerosol composition at low altitudes HASI only Time Series AC 11 High altitude (11 12 km) HASI only Time Series AC 11 High altitude (11 12 km): Increase of organics and nitrate HASI only Time Series AC 11 Outflow HASI only Time Series AC 11 Increase of organics and nitrate at high altitudes Outflow HASI only Mass Spectra Low altitudes: Manaus plume Organics, NO 3, SO 4 Organic spectra: aged oxidized organic aerosol (OOA) High altitudes: km Outflow: Organics, NO 3 Organic spectra: OOA, isoprene epoxydiol secondary organic aerosol (IEPOX- SOA) Organics, NO 3 Organic spectra: OOA, IEPOX-SOA Aging of Organic Aerosol f43: fraction of signal at m/z 43 to organic signal f44: fraction of signal at m/z 44 to organic signal Aging of Organic Aerosol f43: fraction of signal at m/z 43 to organic signal f44: fraction of signal at m/z 44 to organic signal Ratio of f43 and f44: information of oxidation state aging of organic aerosol Ng et al. ACP Aging of Organic Aerosol Aging of Organic Aerosol Aged organic aerosol Low altitude Mass Spectra: aged OOA D p 200 nm Fresher organic aerosol High altitude Mass Spectra: OOA, IEPOX-SOA D p 100 nm Aging of Organic Aerosol CVI Residual particles: even younger organics High altitude Mass Spectra: Hydrocarbonlike organic aerosol (HOA) IEPOX-SOA Isoprene EPOXidiol Secondary Organic Aerosol Oxidation of isoprene Source of isoprene: vegetation Indications for IEPOX-SOA in mass spectra at high altitudes - Marker peak: m/z 82 - f82: fraction of signal at m/z 82 to organic signal Robinson et al. ACP 2011; Hu et al. ACP IEPOX-SOA Isoprene EPOXidiol Secondary Organic Aerosol Oxidation of isoprene Source of isoprene: vegetation Indications for IEPOX-SOA in mass spectra at high altitudes - Marker peak: m/z 82 - f82: fraction of signal at m/z 82 to organic signal Robinson et al. ACP 2011; Hu et al. ACP Summary AC 11 Increase of organic and nitrate mass concentration with altitude No such increase observed for sulfate Organic aerosol: younger aerosol at higher altitudes aerosol formation (by condensation and/or nucleation) at higher altitudes Indications for Isoprene EPOXidiol Secondary Organic Aerosol (IEPOX-SOA) Cloud residues: even younger organic aerosol, mass spectra similar to HOA Thank you for your attention! Christiane Schulz
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