The effect of temperature and relative humidity on secondary organic aerosol formation from ozonolysis of Δ3-carene

Ditte Thomsen; Emil Mark Iversen; Jane Tygesen Skønager; Yuanyuan Luo; Linjie Li; Pontus Roldin; Michael Priestley; Henrik B. Pedersen; Mattias Hallquist; Mikael Ehn; Merete Bilde; Marianne Glasius

doi:10.1039/D3EA00128H

The effect of temperature and relative humidity on secondary organic aerosol formation from ozonolysis of Δ³-carene

Ditte Thomsen, Emil Mark Iversen, Jane Tygesen Skønager, Yuanyuan Luo, Linjie Li, Pontus Roldin, Michael Priestley, Henrik B. Pedersen, Mattias Hallquist, Mikael Ehn, Merete Bilde^*, Marianne Glasius^*

^*Corresponding author for this work

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Abstract

This study investigates the effects of temperature and relative humidity (RH) on the formation of secondary organic aerosol (SOA) from Δ³-carene, a prevalent monoterpene in boreal forests. Dark ozonolysis experiments of 10 ppb Δ³-carene were conducted in the Aarhus University Research on Aerosol (AURA) atmospheric simulation chamber at temperatures of 0, 10, and 20 °C. Under dry conditions (RH < 2%), the SOA formation in terms of both particle number and mass concentration shows minimal temperature dependence. This is in contrast to previous findings at higher initial concentrations and suggests an effect of VOC loading for Δ³-carene. Interestingly, the mass fraction of key oxidation products (cis-3-caric acid, cis-3-caronic acid) exhibit a temperature dependence suggesting continuous condensation at lower temperatures, while evaporation and further reactions over time become more favourable at higher temperatures. The oxygen-to-carbon ratios in the particle phase and the occurrence of highly oxygenated organic molecules (HOM) in the gas phase show modest increases with higher temperatures. Predictions from the Aerosol Dynamics and Gas- and Particle-Phase Chemistry Kinetic Multilayer Model (ADCHAM) agrees with the experimental results regarding both physical particle properties and aerosol composition considering the experimental uncertainties. At high RH (∼80%, 10 °C), a considerable increase in the particle nucleation rate and particle number concentration is observed compared to experiments under dry conditions. This is likely due to enhanced particle nucleation resulting from more stable cluster formation of water and inorganics at increased RH. However, RH does not affect the particle mass concentration.

Original language	English
Journal	Environmental Science: Atmospheres
Volume	4
Issue	1
Pages (from-to)	88-103
Number of pages	16
DOIs	https://doi.org/10.1039/D3EA00128H
Publication status	Published - Jan 2024

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10.1039/D3EA00128HLicence: CC BY-NC

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@article{4ff5f5f0825048e995b154215ee27b13,

title = "The effect of temperature and relative humidity on secondary organic aerosol formation from ozonolysis of Δ3-carene",

abstract = "This study investigates the effects of temperature and relative humidity (RH) on the formation of secondary organic aerosol (SOA) from Δ3-carene, a prevalent monoterpene in boreal forests. Dark ozonolysis experiments of 10 ppb Δ3-carene were conducted in the Aarhus University Research on Aerosol (AURA) atmospheric simulation chamber at temperatures of 0, 10, and 20 °C. Under dry conditions (RH < 2%), the SOA formation in terms of both particle number and mass concentration shows minimal temperature dependence. This is in contrast to previous findings at higher initial concentrations and suggests an effect of VOC loading for Δ3-carene. Interestingly, the mass fraction of key oxidation products (cis-3-caric acid, cis-3-caronic acid) exhibit a temperature dependence suggesting continuous condensation at lower temperatures, while evaporation and further reactions over time become more favourable at higher temperatures. The oxygen-to-carbon ratios in the particle phase and the occurrence of highly oxygenated organic molecules (HOM) in the gas phase show modest increases with higher temperatures. Predictions from the Aerosol Dynamics and Gas- and Particle-Phase Chemistry Kinetic Multilayer Model (ADCHAM) agrees with the experimental results regarding both physical particle properties and aerosol composition considering the experimental uncertainties. At high RH (∼80%, 10 °C), a considerable increase in the particle nucleation rate and particle number concentration is observed compared to experiments under dry conditions. This is likely due to enhanced particle nucleation resulting from more stable cluster formation of water and inorganics at increased RH. However, RH does not affect the particle mass concentration.",

author = "Ditte Thomsen and Iversen, {Emil Mark} and Sk{\o}nager, {Jane Tygesen} and Yuanyuan Luo and Linjie Li and Pontus Roldin and Michael Priestley and Pedersen, {Henrik B.} and Mattias Hallquist and Mikael Ehn and Merete Bilde and Marianne Glasius",

year = "2024",

month = jan,

doi = "10.1039/D3EA00128H",

language = "English",

volume = "4",

pages = "88--103",

journal = "Environmental Science: Atmospheres",

issn = "2634-3606",

publisher = "Royal Society of Chemistry",

number = "1",

}

The effect of temperature and relative humidity on secondary organic aerosol formation from ozonolysis of Δ³-carene. / Thomsen, Ditte ; Iversen, Emil Mark ; Skønager, Jane Tygesen et al.
In: Environmental Science: Atmospheres, Vol. 4, No. 1, 01.2024, p. 88-103.

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

TY - JOUR

T1 - The effect of temperature and relative humidity on secondary organic aerosol formation from ozonolysis of Δ3-carene

AU - Thomsen, Ditte

AU - Iversen, Emil Mark

AU - Skønager, Jane Tygesen

AU - Luo, Yuanyuan

AU - Li, Linjie

AU - Roldin, Pontus

AU - Priestley, Michael

AU - Pedersen, Henrik B.

AU - Hallquist, Mattias

AU - Ehn, Mikael

AU - Bilde, Merete

AU - Glasius, Marianne

PY - 2024/1

Y1 - 2024/1

N2 - This study investigates the effects of temperature and relative humidity (RH) on the formation of secondary organic aerosol (SOA) from Δ3-carene, a prevalent monoterpene in boreal forests. Dark ozonolysis experiments of 10 ppb Δ3-carene were conducted in the Aarhus University Research on Aerosol (AURA) atmospheric simulation chamber at temperatures of 0, 10, and 20 °C. Under dry conditions (RH < 2%), the SOA formation in terms of both particle number and mass concentration shows minimal temperature dependence. This is in contrast to previous findings at higher initial concentrations and suggests an effect of VOC loading for Δ3-carene. Interestingly, the mass fraction of key oxidation products (cis-3-caric acid, cis-3-caronic acid) exhibit a temperature dependence suggesting continuous condensation at lower temperatures, while evaporation and further reactions over time become more favourable at higher temperatures. The oxygen-to-carbon ratios in the particle phase and the occurrence of highly oxygenated organic molecules (HOM) in the gas phase show modest increases with higher temperatures. Predictions from the Aerosol Dynamics and Gas- and Particle-Phase Chemistry Kinetic Multilayer Model (ADCHAM) agrees with the experimental results regarding both physical particle properties and aerosol composition considering the experimental uncertainties. At high RH (∼80%, 10 °C), a considerable increase in the particle nucleation rate and particle number concentration is observed compared to experiments under dry conditions. This is likely due to enhanced particle nucleation resulting from more stable cluster formation of water and inorganics at increased RH. However, RH does not affect the particle mass concentration.

AB - This study investigates the effects of temperature and relative humidity (RH) on the formation of secondary organic aerosol (SOA) from Δ3-carene, a prevalent monoterpene in boreal forests. Dark ozonolysis experiments of 10 ppb Δ3-carene were conducted in the Aarhus University Research on Aerosol (AURA) atmospheric simulation chamber at temperatures of 0, 10, and 20 °C. Under dry conditions (RH < 2%), the SOA formation in terms of both particle number and mass concentration shows minimal temperature dependence. This is in contrast to previous findings at higher initial concentrations and suggests an effect of VOC loading for Δ3-carene. Interestingly, the mass fraction of key oxidation products (cis-3-caric acid, cis-3-caronic acid) exhibit a temperature dependence suggesting continuous condensation at lower temperatures, while evaporation and further reactions over time become more favourable at higher temperatures. The oxygen-to-carbon ratios in the particle phase and the occurrence of highly oxygenated organic molecules (HOM) in the gas phase show modest increases with higher temperatures. Predictions from the Aerosol Dynamics and Gas- and Particle-Phase Chemistry Kinetic Multilayer Model (ADCHAM) agrees with the experimental results regarding both physical particle properties and aerosol composition considering the experimental uncertainties. At high RH (∼80%, 10 °C), a considerable increase in the particle nucleation rate and particle number concentration is observed compared to experiments under dry conditions. This is likely due to enhanced particle nucleation resulting from more stable cluster formation of water and inorganics at increased RH. However, RH does not affect the particle mass concentration.

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U2 - 10.1039/D3EA00128H

DO - 10.1039/D3EA00128H

M3 - Journal article

SN - 2634-3606

VL - 4

SP - 88

EP - 103

JO - Environmental Science: Atmospheres

JF - Environmental Science: Atmospheres

IS - 1

ER -

The effect of temperature and relative humidity on secondary organic aerosol formation from ozonolysis of Δ³-carene

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