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Published February 14, 2017 | Supplemental Material + Published
Journal Article Open

Constraining uncertainties in particle-wall deposition correction during SOA formation in chamber experiments


The effect of vapor-wall deposition on secondary organic aerosol (SOA) formation has gained significant attention; however, uncertainties in experimentally derived SOA mass yields due to uncertainties in particle-wall deposition remain. Different approaches have been used to correct for particle-wall deposition in SOA formation studies, each having its own set of assumptions in determining the particle-wall loss rate. In volatile and intermediate-volatility organic compound (VOC and IVOC) systems in which SOA formation is governed by kinetically limited growth, the effect of vapor-wall deposition on SOA mass yields can be constrained by using high surface area concentrations of seed aerosol to promote the condensation of SOA-forming vapors onto seed aerosol instead of the chamber walls. However, under such high seed aerosol levels, the presence of significant coagulation may complicate the particle-wall deposition correction. Here, we present a model framework that accounts for coagulation in chamber studies in which high seed aerosol surface area concentrations are used. For the α-pinene ozonolysis system, we find that after accounting for coagulation, SOA mass yields remain approximately constant when high seed aerosol surface area concentrations ( ≥  8000 µm^2 cm^(−3)) are used, consistent with our prior study (Nah et al., 2016) showing that α-pinene ozonolysis SOA formation is governed by quasi-equilibrium growth. In addition, we systematically assess the uncertainties in the calculated SOA mass concentrations and yields between four different particle-wall loss correction methods over the series of α-pinene ozonolysis experiments. At low seed aerosol surface area concentrations (< 3000 µm^2 cm^(−3)), the SOA mass yields at peak SOA growth obtained from the particle-wall loss correction methods agree within 14 %. However, at high seed aerosol surface area concentrations ( ≥  8000 µm^2 cm^(−3)), the SOA mass yields at peak SOA growth obtained from different particle-wall loss correction methods can differ by as much as 58 %. These differences arise from assumptions made in the particle-wall loss correction regarding the first-order particle-wall loss rate. This study highlights the importance of accounting for particle-wall deposition accurately during SOA formation chamber experiments and assessing the uncertainties associated with the application of the particle-wall deposition correction method when comparing and using SOA mass yields measured in different studies.

Additional Information

© Author(s) 2017. This work is distributed under the Creative Commons Attribution 3.0 License. Received: 14 Sep 2016 – Discussion started: 19 Sep 2016. Revised: 06 Jan 2017 – Accepted: 16 Jan 2017 – Published: 14 Feb 2017. This research was funded by NSF grants 1455588 and AGS-1523500 and the US Environmental Protection Agency STAR grant (Early Career) RD-83540301. Renee C. McVay was supported by a National Science Foundation Graduate Research Fellowship under grant No. DGE-1144469. Data availability: The experimental data can be accessed by request (ng@chbe.gatech.edu). The Supplement related to this article is available online at doi:10.5194/acp-17-2297-2017-supplement. Edited by: M. C. Facchini. Reviewed by: two anonymous referees. The authors declare that they have no conflict of interest. This publication's contents are solely the responsibility of the grantee and do not necessarily represent the official views of the US EPA. Furthermore, the US EPA does not endorse the purchase of any commercial products or services mentioned in the publication.

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