Dataset Information

Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range.

ABSTRACT: Nucleation and growth of aerosol particles from atmospheric vapors constitutes a major source of global cloud condensation nuclei (CCN). The fraction of newly formed particles that reaches CCN sizes is highly sensitive to particle growth rates, especially for particle sizes <10 nm, where coagulation losses to larger aerosol particles are greatest. Recent results show that some oxidation products from biogenic volatile organic compounds are major contributors to particle formation and initial growth. However, whether oxidized organics contribute to particle growth over the broad span of tropospheric temperatures remains an open question, and quantitative mass balance for organic growth has yet to be demonstrated at any temperature. Here, in experiments performed under atmospheric conditions in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN), we show that rapid growth of organic particles occurs over the range from [Formula: see text]C to [Formula: see text]C. The lower extent of autoxidation at reduced temperatures is compensated by the decreased volatility of all oxidized molecules. This is confirmed by particle-phase composition measurements, showing enhanced uptake of relatively less oxygenated products at cold temperatures. We can reproduce the measured growth rates using an aerosol growth model based entirely on the experimentally measured gas-phase spectra of oxidized organic molecules obtained from two complementary mass spectrometers. We show that the growth rates are sensitive to particle curvature, explaining widespread atmospheric observations that particle growth rates increase in the single-digit-nanometer size range. Our results demonstrate that organic vapors can contribute to particle growth over a wide range of tropospheric temperatures from molecular cluster sizes onward.

SUBMITTER: Stolzenburg D

PROVIDER: S-EPMC6140529 | biostudies-other | 2018 Sep

REPOSITORIES: biostudies-other

ACCESS DATA

Publications

Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range.

Stolzenburg Dominik D Fischer Lukas L Vogel Alexander L AL Heinritzi Martin M Schervish Meredith M Simon Mario M Wagner Andrea C AC Dada Lubna L Ahonen Lauri R LR Amorim Antonio A Baccarini Andrea A Bauer Paulus S PS Baumgartner Bernhard B Bergen Anton A Bianchi Federico F Bianchi Federico F Breitenlechner Martin M Brilke Sophia S Buenrostro Mazon Stephany S Chen Dexian D Dias António A Draper Danielle C DC Duplissy Jonathan J El Haddad Imad I Finkenzeller Henning H Frege Carla C Fuchs Claudia C Garmash Olga O Gordon Hamish H He Xucheng X Helm Johanna J Hofbauer Victoria V Hoyle Christopher R CR Kim Changhyuk C Kirkby Jasper J Kontkanen Jenni J Kürten Andreas A Lampilahti Janne J Lawler Michael M Lehtipalo Katrianne K Leiminger Markus M Mai Huajun H Mathot Serge S Mentler Bernhard B Molteni Ugo U Nie Wei W Nieminen Tuomo T Nowak John B JB Ojdanic Andrea A Onnela Antti A Passananti Monica M Petäjä Tuukka T Quéléver Lauriane L J LLJ Rissanen Matti P MP Sarnela Nina N Schallhart Simon S Tauber Christian C Tomé António A Wagner Robert R Wang Mingyi M Weitz Lena L Wimmer Daniela D Xiao Mao M Yan Chao C Ye Penglin P Zha Qiaozhi Q Baltensperger Urs U Curtius Joachim J Dommen Josef J Flagan Richard C RC Kulmala Markku M Smith James N JN Worsnop Douglas R DR Hansel Armin A Donahue Neil M NM Winkler Paul M PM

Proceedings of the National Academy of Sciences of the United States of America 20180828 37

Nucleation and growth of aerosol particles from atmospheric vapors constitutes a major source of global cloud condensation nuclei (CCN). The fraction of newly formed particles that reaches CCN sizes is highly sensitive to particle growth rates, especially for particle sizes <10 nm, where coagulation losses to larger aerosol particles are greatest. Recent results show that some oxidation products from biogenic volatile organic compounds are major contributors to particle formation and initial gro ...[more]

PMID: 30154167

Similar Datasets

Project description:Cyclohexene is an important intermediate during the combustion process of hydrocarbon and oxygenated fuels. In view of the lack of study on the combustion of cyclohexene in air, an experimental and modeling study is performed to investigate the chemistry of cyclohexene-air mixtures under a wide temperature range. The shock tube experiments are conducted at pressures of 2 and 10 atm with equivalence ratios of 0.5, 1.0 and 2.0 to determine the ignition delay times. The ignition data under 10 atm cover a wide temperature range varying from a low temperature of 770 K to a high temperature of 1222 K. No typical negative-temperature-coefficient is observed, but the ignition at low temperatures is shorter than the extrapolation at high temperatures. A detailed kinetic model of cyclohexene oxidation is proposed based on the low temperature mechanism of 1,3-cyclohexadiene and the existing high temperature mechanism of cyclohexene. The developed model reproduces the ignition delay times in air well, but it over predicts the ignition delays in argon conditions at higher temperatures. Sensitivity analyses under different temperatures and equivalence ratios are carried out to identify the key reactions affecting ignition. The reactions of H + O2 = O + OH and hydrogen abstraction reaction of cyclohexene with oxygen (CYHEXEN + O2 = CYHEXEN-3J + HO2) explain the change of ignition delay time of cyclohexene with equivalence ratios. Flux analysis gives the change of main reaction pathways under wide temperatures and different pressures. The retro-Diels-Alder reaction as the most important consumption channel of cyclohexene at the pressure of 2 atm and temperature of 1350 K is greatly suppressed when the pressure is increased to 10 atm, while the hydrogen abstraction reaction becomes the main consumption channel of cyclohexene at the high pressure. The proposed kinetic model for cyclohexene oxidation can be used to develop models of hydrocarbon and oxygenated fuels.

Dataset Information

Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range.

Publications

Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets