Constraining uncertainties in particle-wall deposition correction during SOA formation in chamber experiments
- 1School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, USA
- 2Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA, USA
- 3Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA
- 4Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA, USA
- 5School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
Abstract. 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 µm2 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 µm2 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 µm2 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.