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Volume 15, issue 2
Atmos. Chem. Phys., 15, 883-897, 2015
https://doi.org/10.5194/acp-15-883-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 15, 883-897, 2015
https://doi.org/10.5194/acp-15-883-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 26 Jan 2015

Research article | 26 Jan 2015

Aging of secondary organic aerosol generated from the ozonolysis of α-pinene: effects of ozone, light and temperature

C. Denjean1,2, P. Formenti1, B. Picquet-Varrault1, M. Camredon1, E. Pangui1, P. Zapf1, Y. Katrib1, C. Giorio3,*, A. Tapparo3, B. Temime-Roussel4, A. Monod4, B. Aumont1, and J. F. Doussin1 C. Denjean et al.
  • 1Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA), UMR-CNRS 7583, Université Paris-Est-Créteil (UPEC) et Université Paris Diderot (UPD), Institut Pierre Simon Laplace (IPSL), Créteil, France
  • 2Leibniz Institute for Tropospheric Research (TROPOS), Permoserstr. 15, 04318 Leipzig, Germany
  • 3Dipartimento di Scienze Chimiche, Università degli Studi di Padova, Via Marzolo 1, 35131 Padova, Italy
  • 4Aix Marseille Université, CNRS, LCE FRE 3416, 13331 Marseille, France
  • *now at: Department of Chemistry, University of Cambridge, Lensfield Road, CB2 1EW Cambridge, UK

Abstract. A series of experiments was conducted in the CESAM (French acronym for Experimental Multiphasic Atmospheric Simulation Chamber) simulation chamber to investigate the evolution of the physical and chemical properties of secondary organic aerosols (SOAs) during different forcings. The present experiments represent a first attempt to comprehensively investigate the influence of oxidative processing, photochemistry, and diurnal temperature cycling upon SOA properties. SOAs generated from the ozonolysis of α-pinene were exposed under dry conditions (< 1% relative humidity) to (1) elevated ozone concentrations, (2) light (under controlled temperature conditions) or (3) light and heat (6 °C light-induced temperature increase), and the resultant changes in SOA optical properties (i.e. absorption and scattering), hygroscopicity and chemical composition were measured using a suite of instrumentation interfaced to the CESAM chamber. The complex refractive index (CRI) was derived from integrated nephelometer measurements of 525 nm wavelength, using Mie scattering calculations and measured number size distributions. The particle size growth factor (GF) was measured with a hygroscopic tandem differential mobility analyzer (H-TDMA). An aerosol mass spectrometer (AMS) was used for the determination of the f44 / f43 and O : C ratio of the particles bulk.

No change in SOA size or chemical composition was observed during O3 and light exposure at constant temperature; in addition, GF and CRI of the SOA remained constant with forcing. On the contrary, illumination of SOAs in the absence of temperature control led to an increase in the real part of the CRI from 1.35 (±0.03) to 1.49 (±0.03), an increase of the GF from 1.04 (±0.02) to 1.14 (±0.02) and an increase of the f44 / f43 ratio from 1.73 (±0.03) to 2.23 (±0.03). The simulation of the experiments using the master chemical mechanism (MCM) and the Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) shows that these changes resulted from the evaporation of semi-volatile and less oxidized SOA species induced by the relatively minor increases in temperature (~ 6 °C). These surprising results suggest that α-pinene–O3 SOA properties may be governed more by local temperature fluctuations than by oxidative processing and photochemistry.

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