Abstract
We use a real-time temperature-programmed desorption chemical-ionization mass spectrometer (FIGAERO-CIMS) to measure particle-phase composition and volatility of nucleated particles, studying pure α-pinene oxidation over a wide temperature range (-50 °C to +25 °C) in the CLOUD chamber at CERN. Highly oxygenated organic molecules are much more abundant in particles formed at higher temperatures, shifting the compounds toward higher O/C and lower intrinsic (300 K) volatility. We find that pure biogenic nucleation and growth depends only weakly on temperature. This is because the positive temperature dependence of degree of oxidation (and polarity) and the negative temperature dependence of volatility counteract each other. Unlike prior work that relied on estimated volatility, we directly measure volatility via calibrated temperature-programmed desorption. Our particle-phase measurements are consistent with gas-phase results and indicate that during new-particle formation from α-pinene oxidation, gas-phase chemistry directly determines the properties of materials in the condensed phase. We now have consistency between measured gas-phase product concentrations, product volatility, measured and modeled growth rates, and the particle composition over most temperatures found in the troposphere.
Original language | English |
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Pages (from-to) | 12357-12365 |
Number of pages | 9 |
Journal | Environmental Science and Technology |
Volume | 53 |
Issue number | 21 |
DOIs | |
Publication status | Published - 5 Nov 2019 |
Externally published | Yes |
Publication type | A1 Journal article-refereed |
Funding
We thank the European Organization for Nuclear Research (CERN) for supporting CLOUD with important technical and financial resources. This research has received funding from the U.S. National Science Foundation under grants AGS-1801574, AGS-1801897, AGS-1649147, and AGS-1602086; the EC Horizon 2020 Programme (Marie-Sklodowska-Curie Innovative Training Network “CLOUD-MOTION” No. 764991); European Union Horizon 2020 programme MC–COFUND Grant 665779; German Federal Ministry of Education and Research (No. 01LK1601A); ERC-Consolidator Grant NANODYNAMITE 616075; Horizon 2020 Marie Sklodowska-Curie Grant 656994 (Nano-CAVa); ERC Advanced “ATM-GP” grant No. 227463; and the Swiss National Science Foundation Project 20FI20_159851, 200021_169090, 200020_172602 and 20FI20_172622. The FIGAERO–CIMS was supported by an MRI grant for the U.S. NSF AGS-1531284 as well as the Wallace Research Foundation. Q.Y. was supported by a Faculty for the Future Fellowship from the Schlumberger Foundation.
Publication forum classification
- Publication forum level 2
ASJC Scopus subject areas
- General Chemistry
- Environmental Chemistry