Skip to content

Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations

Research output: Contribution to journalArticle

Standard

Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations. / Evoy, Erin; Maclean, Adrian M.; Rovelli, Grazia; Li, Ying; Tsimpidi, Alexandra P.; Karydis, Vlassis A.; Kamal, Saeid; Lelieveld, Jos; Shiraiwa, Manabu; Reid, Jonathan P.; Bertram, Allan K.

In: Atmospheric Chemistry and Physics, Vol. 19, 09.08.2019, p. 10073-10085.

Research output: Contribution to journalArticle

Harvard

Evoy, E, Maclean, AM, Rovelli, G, Li, Y, Tsimpidi, AP, Karydis, VA, Kamal, S, Lelieveld, J, Shiraiwa, M, Reid, JP & Bertram, AK 2019, 'Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations', Atmospheric Chemistry and Physics, vol. 19, pp. 10073-10085. https://doi.org/10.5194/acp-19-10073-2019

APA

Evoy, E., Maclean, A. M., Rovelli, G., Li, Y., Tsimpidi, A. P., Karydis, V. A., ... Bertram, A. K. (2019). Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations. Atmospheric Chemistry and Physics, 19, 10073-10085. https://doi.org/10.5194/acp-19-10073-2019

Vancouver

Evoy E, Maclean AM, Rovelli G, Li Y, Tsimpidi AP, Karydis VA et al. Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations. Atmospheric Chemistry and Physics. 2019 Aug 9;19:10073-10085. https://doi.org/10.5194/acp-19-10073-2019

Author

Evoy, Erin ; Maclean, Adrian M. ; Rovelli, Grazia ; Li, Ying ; Tsimpidi, Alexandra P. ; Karydis, Vlassis A. ; Kamal, Saeid ; Lelieveld, Jos ; Shiraiwa, Manabu ; Reid, Jonathan P. ; Bertram, Allan K. / Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations. In: Atmospheric Chemistry and Physics. 2019 ; Vol. 19. pp. 10073-10085.

Bibtex

@article{3c74816964f54545b368a5d9dcecb9d7,
title = "Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations",
abstract = "Information on the rate of diffusion of organic molecules within secondary organic aerosol (SOA) is needed to accurately predict the effects of SOA on climate and air quality. Diffusion can be important for predicting the growth, evaporation, and reaction rates of SOA under certain atmospheric conditions. Often, researchers have predicted diffusion rates of organic molecules within SOA using measurements of viscosity and the Stokes-Einstein relation (D ∝ 1/η, where D is the diffusion coefficient and η is viscosity). However, the accuracy of this relation for predicting diffusion in SOA remains uncertain. Using rectangular area fluorescence recovery after photobleaching (rFRAP), we determined diffusion coefficients of fluorescent organic molecules over 8 orders in magnitude in proxies of SOA including citric acid, sorbitol, and a sucrose-citric acid mixture. These results were combined with literature data to evaluate the Stokes-Einstein relation for predicting the diffusion of organic molecules in SOA. Although almost all the data agree with the Stokes-Einstein relation within a factor of 10, a fractional Stokes-Einstein relation (D ∝ 1/ηξ) with ξ = 0:93 is a better model for predicting the diffusion of organic molecules in the SOA proxies studied. In addition, based on the output from a chemical transport model, the Stokes-Einstein relation can overpredict mixing times of organic molecules within SOA by as much as 1 order of magnitude at an altitude of ∼ 3 km compared to the fractional Stokes-Einstein relation with ξ = 0.93. These results also have implications for other areas such as in food sciences and the preservation of biomolecules.",
author = "Erin Evoy and Maclean, {Adrian M.} and Grazia Rovelli and Ying Li and Tsimpidi, {Alexandra P.} and Karydis, {Vlassis A.} and Saeid Kamal and Jos Lelieveld and Manabu Shiraiwa and Reid, {Jonathan P.} and Bertram, {Allan K.}",
year = "2019",
month = "8",
day = "9",
doi = "10.5194/acp-19-10073-2019",
language = "English",
volume = "19",
pages = "10073--10085",
journal = "Atmospheric Chemistry and Physics",
issn = "1680-7316",
publisher = "Copernicus GmbH",

}

RIS - suitable for import to EndNote

TY - JOUR

T1 - Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations

AU - Evoy, Erin

AU - Maclean, Adrian M.

AU - Rovelli, Grazia

AU - Li, Ying

AU - Tsimpidi, Alexandra P.

AU - Karydis, Vlassis A.

AU - Kamal, Saeid

AU - Lelieveld, Jos

AU - Shiraiwa, Manabu

AU - Reid, Jonathan P.

AU - Bertram, Allan K.

PY - 2019/8/9

Y1 - 2019/8/9

N2 - Information on the rate of diffusion of organic molecules within secondary organic aerosol (SOA) is needed to accurately predict the effects of SOA on climate and air quality. Diffusion can be important for predicting the growth, evaporation, and reaction rates of SOA under certain atmospheric conditions. Often, researchers have predicted diffusion rates of organic molecules within SOA using measurements of viscosity and the Stokes-Einstein relation (D ∝ 1/η, where D is the diffusion coefficient and η is viscosity). However, the accuracy of this relation for predicting diffusion in SOA remains uncertain. Using rectangular area fluorescence recovery after photobleaching (rFRAP), we determined diffusion coefficients of fluorescent organic molecules over 8 orders in magnitude in proxies of SOA including citric acid, sorbitol, and a sucrose-citric acid mixture. These results were combined with literature data to evaluate the Stokes-Einstein relation for predicting the diffusion of organic molecules in SOA. Although almost all the data agree with the Stokes-Einstein relation within a factor of 10, a fractional Stokes-Einstein relation (D ∝ 1/ηξ) with ξ = 0:93 is a better model for predicting the diffusion of organic molecules in the SOA proxies studied. In addition, based on the output from a chemical transport model, the Stokes-Einstein relation can overpredict mixing times of organic molecules within SOA by as much as 1 order of magnitude at an altitude of ∼ 3 km compared to the fractional Stokes-Einstein relation with ξ = 0.93. These results also have implications for other areas such as in food sciences and the preservation of biomolecules.

AB - Information on the rate of diffusion of organic molecules within secondary organic aerosol (SOA) is needed to accurately predict the effects of SOA on climate and air quality. Diffusion can be important for predicting the growth, evaporation, and reaction rates of SOA under certain atmospheric conditions. Often, researchers have predicted diffusion rates of organic molecules within SOA using measurements of viscosity and the Stokes-Einstein relation (D ∝ 1/η, where D is the diffusion coefficient and η is viscosity). However, the accuracy of this relation for predicting diffusion in SOA remains uncertain. Using rectangular area fluorescence recovery after photobleaching (rFRAP), we determined diffusion coefficients of fluorescent organic molecules over 8 orders in magnitude in proxies of SOA including citric acid, sorbitol, and a sucrose-citric acid mixture. These results were combined with literature data to evaluate the Stokes-Einstein relation for predicting the diffusion of organic molecules in SOA. Although almost all the data agree with the Stokes-Einstein relation within a factor of 10, a fractional Stokes-Einstein relation (D ∝ 1/ηξ) with ξ = 0:93 is a better model for predicting the diffusion of organic molecules in the SOA proxies studied. In addition, based on the output from a chemical transport model, the Stokes-Einstein relation can overpredict mixing times of organic molecules within SOA by as much as 1 order of magnitude at an altitude of ∼ 3 km compared to the fractional Stokes-Einstein relation with ξ = 0.93. These results also have implications for other areas such as in food sciences and the preservation of biomolecules.

UR - http://www.scopus.com/inward/record.url?scp=85070455381&partnerID=8YFLogxK

U2 - 10.5194/acp-19-10073-2019

DO - 10.5194/acp-19-10073-2019

M3 - Article

AN - SCOPUS:85070455381

VL - 19

SP - 10073

EP - 10085

JO - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

SN - 1680-7316

ER -