Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air–water interface using material extracted from urban, remote and wood smoke aerosol. / Shepherd, Rosalie; King, Martin; Rennie, Adrian R.; Ward, Andrew; Frey, M.M.; Brough, Neil; Eveson, Joshua; Del Vento, sabino; Milsom, Adam ; Pfrang, Christian; Skoda, Maxmilian; Welbourn, Rebecca.

In: Environmental Science: Atmospheres, 12.04.2022.

Research output: Contribution to journalArticlepeer-review

Published

Standard

Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air–water interface using material extracted from urban, remote and wood smoke aerosol. / Shepherd, Rosalie; King, Martin; Rennie, Adrian R.; Ward, Andrew; Frey, M.M.; Brough, Neil; Eveson, Joshua; Del Vento, sabino; Milsom, Adam ; Pfrang, Christian; Skoda, Maxmilian; Welbourn, Rebecca.

In: Environmental Science: Atmospheres, 12.04.2022.

Research output: Contribution to journalArticlepeer-review

Harvard

Shepherd, R, King, M, Rennie, AR, Ward, A, Frey, MM, Brough, N, Eveson, J, Del Vento, S, Milsom, A, Pfrang, C, Skoda, M & Welbourn, R 2022, 'Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air–water interface using material extracted from urban, remote and wood smoke aerosol', Environmental Science: Atmospheres. https://doi.org/10.1039/d2ea00013j

APA

Shepherd, R., King, M., Rennie, A. R., Ward, A., Frey, M. M., Brough, N., Eveson, J., Del Vento, S., Milsom, A., Pfrang, C., Skoda, M., & Welbourn, R. (2022). Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air–water interface using material extracted from urban, remote and wood smoke aerosol. Environmental Science: Atmospheres. https://doi.org/10.1039/d2ea00013j

Vancouver

Author

Shepherd, Rosalie ; King, Martin ; Rennie, Adrian R. ; Ward, Andrew ; Frey, M.M. ; Brough, Neil ; Eveson, Joshua ; Del Vento, sabino ; Milsom, Adam ; Pfrang, Christian ; Skoda, Maxmilian ; Welbourn, Rebecca. / Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air–water interface using material extracted from urban, remote and wood smoke aerosol. In: Environmental Science: Atmospheres. 2022.

BibTeX

@article{702e68cbb5a04d95beced15cd6a3dc77,
title = "Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air–water interface using material extracted from urban, remote and wood smoke aerosol",
abstract = "The presence of an organic film on a cloud droplet or aqueous aerosol particle has the potential to alter the chemical, optical and physical properties of the droplet or particle. In the study presented, water insoluble organic materials extracted from urban, remote (Antarctica) and wood burning atmospheric aerosol were found to have stable, compressible, films at the air–water interface that were typically $6–18 A ̊ thick. These films are reactive towards gas-phase OH radicals and decay exponentially, with bimolecular rate constants for reaction with gas-phase OH radicals of typically 0.08–1.5 1010 cm3 molecule1 s1. These bimolecular rate constants equate to initial OH radical uptake coefficients estimated to be $0.6–1 except woodsmoke ($0.05). The film thickness and the neutron scattering length density of the extracted atmosphere aerosol material (from urban, remote and wood burning) were measured by neutron reflection as they were exposed to OH radicals. For the first time neutron reflection has been demonstrated as an excellent technique for studying the thin films formed at air–water interfaces from materials extracted from atmospheric aerosol samples. Additionally, the kinetics of gas-phase OH radicals with a proxy compound, the lipid 1,2-distearoyl-sn-glycero-3-phosphocholine (DSPC) was studied displaying significantly different behaviour, thus demonstrating it is not a good proxy for atmospheric materials that may form films at the air–water interface. The atmospheric lifetimes, with respect to OH radical oxidation, of the insoluble organic materials extracted from atmospheric aerosol at the air–water interface were a few hours. Relative to a possible physical atmospheric lifetime of 4 days, the oxidation of these films is important and needs inclusion in atmospheric models. The optical properties of these films were previously reported [Shepherd et al., Atmos. Chem. Phys., 2018, 18, 5235–5252] and there is a significant change in top of the atmosphere albedo for these thin films on core–shell atmospheric aerosol using the film thickness data and confirmation of stable film formation at the air–water interface presented here.",
author = "Rosalie Shepherd and Martin King and Rennie, {Adrian R.} and Andrew Ward and M.M. Frey and Neil Brough and Joshua Eveson and {Del Vento}, sabino and Adam Milsom and Christian Pfrang and Maxmilian Skoda and Rebecca Welbourn",
year = "2022",
month = apr,
day = "12",
doi = "10.1039/d2ea00013j",
language = "English",
journal = "Environmental Science: Atmospheres",
publisher = "Royal Society of Chemistry",

}

RIS

TY - JOUR

T1 - Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air–water interface using material extracted from urban, remote and wood smoke aerosol

AU - Shepherd, Rosalie

AU - King, Martin

AU - Rennie, Adrian R.

AU - Ward, Andrew

AU - Frey, M.M.

AU - Brough, Neil

AU - Eveson, Joshua

AU - Del Vento, sabino

AU - Milsom, Adam

AU - Pfrang, Christian

AU - Skoda, Maxmilian

AU - Welbourn, Rebecca

PY - 2022/4/12

Y1 - 2022/4/12

N2 - The presence of an organic film on a cloud droplet or aqueous aerosol particle has the potential to alter the chemical, optical and physical properties of the droplet or particle. In the study presented, water insoluble organic materials extracted from urban, remote (Antarctica) and wood burning atmospheric aerosol were found to have stable, compressible, films at the air–water interface that were typically $6–18 A ̊ thick. These films are reactive towards gas-phase OH radicals and decay exponentially, with bimolecular rate constants for reaction with gas-phase OH radicals of typically 0.08–1.5 1010 cm3 molecule1 s1. These bimolecular rate constants equate to initial OH radical uptake coefficients estimated to be $0.6–1 except woodsmoke ($0.05). The film thickness and the neutron scattering length density of the extracted atmosphere aerosol material (from urban, remote and wood burning) were measured by neutron reflection as they were exposed to OH radicals. For the first time neutron reflection has been demonstrated as an excellent technique for studying the thin films formed at air–water interfaces from materials extracted from atmospheric aerosol samples. Additionally, the kinetics of gas-phase OH radicals with a proxy compound, the lipid 1,2-distearoyl-sn-glycero-3-phosphocholine (DSPC) was studied displaying significantly different behaviour, thus demonstrating it is not a good proxy for atmospheric materials that may form films at the air–water interface. The atmospheric lifetimes, with respect to OH radical oxidation, of the insoluble organic materials extracted from atmospheric aerosol at the air–water interface were a few hours. Relative to a possible physical atmospheric lifetime of 4 days, the oxidation of these films is important and needs inclusion in atmospheric models. The optical properties of these films were previously reported [Shepherd et al., Atmos. Chem. Phys., 2018, 18, 5235–5252] and there is a significant change in top of the atmosphere albedo for these thin films on core–shell atmospheric aerosol using the film thickness data and confirmation of stable film formation at the air–water interface presented here.

AB - The presence of an organic film on a cloud droplet or aqueous aerosol particle has the potential to alter the chemical, optical and physical properties of the droplet or particle. In the study presented, water insoluble organic materials extracted from urban, remote (Antarctica) and wood burning atmospheric aerosol were found to have stable, compressible, films at the air–water interface that were typically $6–18 A ̊ thick. These films are reactive towards gas-phase OH radicals and decay exponentially, with bimolecular rate constants for reaction with gas-phase OH radicals of typically 0.08–1.5 1010 cm3 molecule1 s1. These bimolecular rate constants equate to initial OH radical uptake coefficients estimated to be $0.6–1 except woodsmoke ($0.05). The film thickness and the neutron scattering length density of the extracted atmosphere aerosol material (from urban, remote and wood burning) were measured by neutron reflection as they were exposed to OH radicals. For the first time neutron reflection has been demonstrated as an excellent technique for studying the thin films formed at air–water interfaces from materials extracted from atmospheric aerosol samples. Additionally, the kinetics of gas-phase OH radicals with a proxy compound, the lipid 1,2-distearoyl-sn-glycero-3-phosphocholine (DSPC) was studied displaying significantly different behaviour, thus demonstrating it is not a good proxy for atmospheric materials that may form films at the air–water interface. The atmospheric lifetimes, with respect to OH radical oxidation, of the insoluble organic materials extracted from atmospheric aerosol at the air–water interface were a few hours. Relative to a possible physical atmospheric lifetime of 4 days, the oxidation of these films is important and needs inclusion in atmospheric models. The optical properties of these films were previously reported [Shepherd et al., Atmos. Chem. Phys., 2018, 18, 5235–5252] and there is a significant change in top of the atmosphere albedo for these thin films on core–shell atmospheric aerosol using the film thickness data and confirmation of stable film formation at the air–water interface presented here.

U2 - 10.1039/d2ea00013j

DO - 10.1039/d2ea00013j

M3 - Article

JO - Environmental Science: Atmospheres

JF - Environmental Science: Atmospheres

ER -