22 Feb 2021

22 Feb 2021

Review status: this preprint is currently under review for the journal ACP.

Secondary organic aerosol phase behaviour in chamber photo-oxidation of mixed precursors

Yu Wang1, Aristeidis Voliotis1, Yunqi Shao1, Taomou Zong2, Xiangxinyue Meng2, Mao Du1, Dawei Hu1, Ying Chen3,a, Zhijun Wu2,4,5, M. Rami Alfarra1,6, and Gordon McFiggans1 Yu Wang et al.
  • 1Centre for Atmospheric Science, Department of Earth and Environmental Sciences, The University of Manchester, Manchester M13 9PL, UK
  • 2State Key Joint Laboratory of Environmental Simulation and Pollution Control, International Joint Laboratory for Regional Pollution Control, Ministry of Education (IJRC), College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
  • 3Lancaster Environment Centre, Lancaster University, LA1 4YQ, UK
  • 4International Joint Laboratory for Regional Pollution Control, 52425 Jülich, Germany, and Beijing 100871, China
  • 5Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Nanjing University of Information Science and Technology, Nanjing 210044, China
  • 6National Centre for Atmospheric Science, School of Earth and Environmental Sciences, The University of Manchester, Manchester, M13 9PL, UK
  • acurrently at: Exeter Climate Systems, University of Exeter, Exeter, EX4 4QE, UK

Abstract. The phase behaviour of aerosol particles plays a profound role in atmospheric physicochemical processes, influencing their physical and optical properties and further impacting climate and air quality. However, understanding of aerosol phase behaviour is still incomplete, especially that of multicomponent particles which contain inorganic compounds and secondary organic aerosol (SOA) from mixed volatile organic compound (VOC) precursors. We report measurements conducted in the Manchester Aerosol Chamber (MAC) to investigate the aerosol rebounding tendency, measured as bounce fraction, as a surrogate of particle phase behaviour during SOA formation from photo-oxidation of biogenic (α-pinene, isoprene) and anthropogenic (o-cresol) VOCs and their binary mixtures on deliquescent ammonium sulphate seed. Aerosol phase behaviour is RH and chemical composition dependent. Liquid (bounce fraction, BF < 0.2) at RH > 80 % and non-liquid behaviour (BF > 0.8) at RH < 30 % were observed, with a liquid-to-nonliquid transition with decreasing RH between 30 %~80 %. This RH-dependent phase behaviour (RHBF = 0.2, 0.5, 0.8) increased towards a maximum with increasing organic-inorganic-mass ratio (MRorg/inorg) during SOA formation evolution in all investigated VOC systems. With the use of comparable initial ammonium sulphate seed concentration, the SOA production rate of the VOC systems determines the MRorg/inorg, and consequently the change of the phase behaviour. Although less important than RH and MRorg/inorg, the SOA composition plays a second-order role, with differences in liquid-to-nonliquid transition at moderate MRorg/inorg of ~1 observed between biogenic and anthropogenic-containing VOC systems. The real atmospheric consequences of our results are that any processes changing ambient RH or MRorg/inorg will influence their particle phase behaviour. Where abundant anthropogenic VOCs contribute to SOA, compositional changes of SOA may influence phase behaviour at moderate organic mass fraction (~50 %) compared with purely biogenic SOA. Further studies are needed on more complex and realistic atmospheric mixtures.

Yu Wang et al.

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-105', Anonymous Referee #1, 20 Mar 2021
  • RC2: 'Comment on acp-2021-105', Anonymous Referee #2, 04 May 2021

Yu Wang et al.


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Short summary
Aerosol phase behaviour plays a profound role in atmospheric physicochemical processes. We designed dedicated chamber experiments to study phase state of secondary organic aerosol from biogenic and anthropogenic mixed precursors. Our results highlight the key role of organic-inorganic-ratio and relative humidity in phase state, but the sources and organic composition is less important. This result provides a solid laboratory evidence for understanding aerosol phase in complex atmosphere.