Molecular understanding of new-particle formation from α-pinene between -50 and +25 °C

Simon, Mario; Dada, Lubna; Heinritzi, Martin; Scholz, Wiebke; Stolzenburg, Dominik; Fischer, Lukas; Wagner, Andrea C.; Kürten, Andreas; Rörup, Birte; He, Xu-Cheng; Almeida, João; Baalbaki, Rima; Baccarini, Andrea; Bauer, Paulus S.; Beck, Lisa; Bergen, Anton; Bianchi, Federico; Bräkling, Steffen; Brilke, Sophia; Caudillo, Lucia; Chen, Dexian; Chu, Biwu; Dias, António; Draper, Danielle C.; Duplissy, Jonathan; El-Haddad, Imad; Finkenzeller, Henning; Frege, Carla; Gonzalez-Carracedo, Loic; Gordon, Hamish; Granzin, Manuel; Hakala, Jani; Hofbauer, Victoria; Hoyle, Christopher R.; Kim, Changhyuk; Kong, Weimeng; Lamkaddam, Houssni; Lee, Chuan P.; Lehtipalo, Katrianne; Leiminger, Markus; Mai, Huajun; Manninen, Hanna E.; Marie, Guillaume; Marten, Ruby; Mentler, Bernhard; Molteni, Ugo; Nichman, Leonid; Nie, Wei; Ojdanic, Andrea; Onnela, Antti; Partoll, Eva; Petäjä, Tuukka; Pfeifer, Joschka; Philippov, Maxim; Quéléver, Lauriane L. J.; Ranjithkumar, Ananth; Rissanen, Matti P.; Schallhart, Simon; Schobesberger, Siegfried; Schuchmann, Simone; Shen, Jiali; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Tauber, Christian; Tham, Yee J.; Tomé, António R.; Vazquez-Pufleau, Miguel; Vogel, Alexander L.; Wagner, Robert; Wang, Mingyi; Wang, Dongyu S.; Wang, Yonghong; Weber, Stefan K.; Wu, Yusheng; Xiao, Mao; Yan, Chao; Ye, Penglin; Ye, Qing; Zauner-Wieczorek, Marcel; Zhou, Xueqin; Baltensperger, Urs; Dommen, Josef; Flagan, Richard C.; Hansel, Armin; Kulmala, Markku; Volkamer, Rainer; Winkler, Paul M.; Worsnop, Douglas R.; Donahue, Neil M.; Kirkby, Jasper; Curtius, Joachim

doi:10.5194/acp-20-9183-2020

Title: Molecular understanding of new-particle formation from α-pinene between -50 and +25 °C

Journal Article · Mon Aug 03 00:00:00 EDT 2020 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-20-9183-2020· OSTI ID:1644365

;

; Heinritzi, Martin;

;

; Kürten, Andreas; Rörup, Birte;

; Almeida, João;

;

; Bergen, Anton;

; Bräkling, Steffen;

; Caudillo, Lucia more »

Abstract. Highly oxygenated organic molecules (HOMs) contribute substantially to the formation and growth of atmospheric aerosol particles, which affect air quality, human health and Earth's climate. HOMs are formed by rapid, gas-phase autoxidation of volatile organic compounds (VOCs) such as α-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role in new-particle formation (NPF) and the early growth of atmospheric aerosols, even without any further assistance of other low-volatility compounds such as sulfuric acid. Both the autoxidation reaction forming HOMs and their NPF rates are expected to be strongly dependent on temperature. However, experimental data on both effects are limited. Dedicated experiments were performed at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN to address this question. In this study, we show that a decrease in temperature (from +25 to -50°C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the NPF rates (J1.7 nm) increase substantially. Measurements with two different chemical ionization mass spectrometers (using nitrate and protonated water as reagent ion, respectively) provide the molecular composition of the gaseous oxidation products, and a two-dimensional volatility basis set (2D VBS) model provides their volatility distribution. The HOM yield decreases with temperature from 6.2 % at 25°C to 0.7 % at -50°C. However, there is a strong reduction of the saturation vapor pressure of each oxidation state as the temperature is reduced. Overall, the reduction in volatility with temperature leads to an increase in the nucleation rates by up to 3 orders of magnitude at -50°C compared with 25°C. In addition, the enhancement of the nucleation rates by ions decreases with decreasing temperature, since the neutral molecular clusters have increased stability against evaporation. The resulting data quantify how the interplay between the temperature-dependent oxidation pathways and the associated vapor pressures affect biogenic NPF at the molecular level. Our measurements, therefore, improve our understanding of pure biogenic NPF for a wide range of tropospheric temperatures and precursor concentrations.

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Research Organization:: Univ. of California, Irvine, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: SC0014469

OSTI ID:: 1644365

Alternate ID(s):: OSTI ID: 1802673

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Vol. 20 Journal Issue: 15; ISSN 1680-7324

Publisher:: Copernicus Publications, EGUCopyright Statement

Country of Publication:: Germany

Language:: English

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Suppression of new particle formation from monoterpene oxidation by NO _x Wildt, J.; Mentel, T. F.; Kiendler-Scharr, A. Atmospheric Chemistry and Physics, Vol. 14, Issue 6 https://doi.org/10.5194/acp-14-2789-2014	journal	January 2014
Diffusion of H ₂ SO ₄ in Humidified Nitrogen: Hydrated H ₂ SO ₄ Hanson, D. R.; Eisele, F. The Journal of Physical Chemistry A, Vol. 104, Issue 8 https://doi.org/10.1021/jp993622j	journal	March 2000
The role of ions in new particle formation in the CLOUD chamber Wagner, Robert; Yan, Chao; Lehtipalo, Katrianne Atmospheric Chemistry and Physics, Vol. 17, Issue 24 https://doi.org/10.5194/acp-17-15181-2017	journal	January 2017
Calibration of a Chemical Ionization Mass Spectrometer for the Measurement of Gaseous Sulfuric Acid Kürten, Andreas; Rondo, Linda; Ehrhart, Sebastian The Journal of Physical Chemistry A, Vol. 116, Issue 24 https://doi.org/10.1021/jp212123n	journal	February 2012
Influence of temperature on the molecular composition of ions and charged clusters during pure biogenic nucleation Frege, Carla; Ortega, Ismael K.; Rissanen, Matti P. Atmospheric Chemistry and Physics, Vol. 18, Issue 1 https://doi.org/10.5194/acp-18-65-2018	journal	January 2018
Atmospheric sulphuric acid and neutral cluster measurements using CI-APi-TOF Jokinen, T.; Sipilä, M.; Junninen, H. Atmospheric Chemistry and Physics, Vol. 12, Issue 9 https://doi.org/10.5194/acp-12-4117-2012	journal	January 2012
Production of extremely low volatile organic compounds from biogenic emissions: Measured yields and atmospheric implications Jokinen, Tuija; Berndt, Torsten; Makkonen, Risto Proceedings of the National Academy of Sciences, Vol. 112, Issue 23 https://doi.org/10.1073/pnas.1423977112	journal	May 2015

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