A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics

By N. Donahue, S. Epstein, Spyros N. Pandis, A. Robinson. 2010

754 citations recorded by the source corpus.

We develop the thermodynamic underpinnings of a two-dimensional volatility basis set (2D-VBS) employ- ing saturation mass concentration (C o ) and the oxygen con- tent (O:C) to describe volatility, mixing thermodynamics, and chemical evolution of organic aerosol. The work ad- dresses a simple question: "Can we reasonably constrain organic-aerosol composition in the atmosphere based on only two measurable organic properties, volatility and the extent of oxygenation?" This is an extension of our earlier one- dimensional approach employing volatility only (C = C o , where is an activity coefficient). Using available con- straints on bulk organic-aerosol composition, we argue that one can reasonably predict the composition of organics (car- bon, oxygen and hydrogen numbers) given a location in the C o - O:C space. Further, we argue that we can constrain the activity coefficients at various locations in this space based on the O:C of the organic aerosol.

Subfields: Atmospheric Science, Global and Planetary Change

View Paper: https://www.semanticscholar.org/paper/f42a9e50c4e8958d7192542f8ed0fb4a1d485f81

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Citations in the corpus

Online coupled regional meteorology chemistry models in Europe: current status and prospects (2013, background): “The approach has been recently extended to account also for the degree of oxidation of SOA species (Donahue et al., 2011).”
Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition (2017, methodology): “1a in Shiraiwa et al. (2017)), we use an equation with a similar formulation to the 182 equation used to predict the saturation mass concentration or volatility (Donahue et al., 2011; Li 183 et al., 2016): 184 Tg = (𝑛!!”
Understanding atmospheric organic aerosols via factor analysis of aerosol mass spectrometry: a review (2011, background): “Because both of these axes can be experimentally obtained, this 2D model provides a useful framework for describing OA evolution that can be constrained by measurements [111].”
Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol (2019, methodology): “This assumption of extremely low vapor pressure was motivated in part by utilizing existing structure−activity relationships (SAR) (e.g., (Donahue et al., 2011) for the observed elemental compositions).28 Ehn et al. (2014) also showed that the behavior of the observed molecules when in contact with…”
Impact of organic molecular structure on the estimation of atmospherically relevant physicochemical parameters (2021, methodology): “…of compounds across∼ 15 orders of magnitude in vapor pressure (Jimenez et al., 2009), wide ranges of oxygenation, volatility and solubility (e.g., Donahue et al., 2011; Hodzic et al., 2014; Lannuque et al., 2018), and several orders of magnitude in reactivities (Lee et al., 2006), with many…”