Microphysical explanation of the RH‐dependent water affinity of biogenic organic aerosol and its importance for climate

N. Rastak; Aki Pajunoja; Juan C. Acosta Navarro; Jin Ma; M. Song; D. G. Partridge; A. Kirkevåg; Yu Jun Leong; HU WEIWEI; N. F. Taylor; A. Lambe; K. Cerully; Aikaterini Bougiatioti; P. Liu; Radovan Krejci; T. Petäjä; Carl J. Percival; P. Davidovits; D. R. Worsnop; Annica Ekman; Athanasios Nenes; S. Martin; Jose L Jimenez; Don Collins; David Topping; A. K. Bertram; Zuend Andreas; Annele Virtanen; Ilona Riipinen

doi:10.1002/2017gl073056

Microphysical explanation of the RH‐dependent water affinity of biogenic organic aerosol and its importance for climate

N. Rastak, Aki Pajunoja, Juan C. Acosta Navarro, Jin Ma, M. Song, D. G. Partridge, A. Kirkevåg, Yu Jun Leong, HU WEIWEI, N. F. Taylor, A. Lambe, K. Cerully, Aikaterini Bougiatioti, P. Liu, Radovan Krejci, T. Petäjä, Carl J. Percival, P. Davidovits, D. R. Worsnop, Annica EkmanAthanasios Nenes, S. Martin, Jose L Jimenez, Don Collins, David Topping, A. K. Bertram, Zuend Andreas, Annele Virtanen, Ilona Riipinen

Marine and Atmospheric Research

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Abstract

A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.

Original language	English
Pages (from-to)	5167-5177
Journal	Geophysical Research Letters
Volume	44
Issue number	10
DOIs	https://doi.org/10.1002/2017gl073056
Publication status	Published - 28 May 2017

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Rastak, N., Pajunoja, A., Navarro, J. C. A., Ma, J., Song, M., Partridge, D. G., Kirkevåg, A., Leong, Y. J., WEIWEI, HU., Taylor, N. F., Lambe, A., Cerully, K., Bougiatioti, A., Liu, P., Krejci, R., Petäjä, T., Percival, C. J., Davidovits, P., Worsnop, D. R., ... Riipinen, I. (2017). Microphysical explanation of the RH‐dependent water affinity of biogenic organic aerosol and its importance for climate. Geophysical Research Letters, 44(10), 5167-5177. https://doi.org/10.1002/2017gl073056

@article{e738c0e041364d859b61a21c8cdfbb12,

title = "Microphysical explanation of the RH‐dependent water affinity of biogenic organic aerosol and its importance for climate",

abstract = "A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.",

author = "N. Rastak and Aki Pajunoja and Navarro, {Juan C. Acosta} and Jin Ma and M. Song and Partridge, {D. G.} and A. Kirkev{\aa}g and Leong, {Yu Jun} and HU WEIWEI and Taylor, {N. F.} and A. Lambe and K. Cerully and Aikaterini Bougiatioti and P. Liu and Radovan Krejci and T. Pet{\"a}j{\"a} and Percival, {Carl J.} and P. Davidovits and Worsnop, {D. R.} and Annica Ekman and Athanasios Nenes and S. Martin and Jimenez, {Jose L} and Don Collins and David Topping and Bertram, {A. K.} and Zuend Andreas and Annele Virtanen and Ilona Riipinen",

year = "2017",

month = may,

day = "28",

doi = "10.1002/2017gl073056",

language = "English",

volume = "44",

pages = "5167--5177",

journal = "Geophysical Research Letters",

issn = "0094-8276",

publisher = "John Wiley and Sons Inc.",

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Rastak, N, Pajunoja, A, Navarro, JCA, Ma, J, Song, M, Partridge, DG, Kirkevåg, A, Leong, YJ, WEIWEI, HU, Taylor, NF, Lambe, A, Cerully, K, Bougiatioti, A, Liu, P, Krejci, R, Petäjä, T, Percival, CJ, Davidovits, P, Worsnop, DR, Ekman, A, Nenes, A, Martin, S, Jimenez, JL, Collins, D, Topping, D, Bertram, AK, Andreas, Z, Virtanen, A & Riipinen, I 2017, 'Microphysical explanation of the RH‐dependent water affinity of biogenic organic aerosol and its importance for climate', Geophysical Research Letters, vol. 44, no. 10, pp. 5167-5177. https://doi.org/10.1002/2017gl073056

TY - JOUR

T1 - Microphysical explanation of the RH‐dependent water affinity of biogenic organic aerosol and its importance for climate

AU - Rastak, N.

AU - Pajunoja, Aki

AU - Navarro, Juan C. Acosta

AU - Ma, Jin

AU - Song, M.

AU - Partridge, D. G.

AU - Kirkevåg, A.

AU - Leong, Yu Jun

AU - WEIWEI, HU

AU - Taylor, N. F.

AU - Lambe, A.

AU - Cerully, K.

AU - Bougiatioti, Aikaterini

AU - Liu, P.

AU - Krejci, Radovan

AU - Petäjä, T.

AU - Percival, Carl J.

AU - Davidovits, P.

AU - Worsnop, D. R.

AU - Ekman, Annica

AU - Nenes, Athanasios

AU - Martin, S.

AU - Jimenez, Jose L

AU - Collins, Don

AU - Topping, David

AU - Bertram, A. K.

AU - Andreas, Zuend

AU - Virtanen, Annele

AU - Riipinen, Ilona

PY - 2017/5/28

Y1 - 2017/5/28

N2 - A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.

AB - A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.

UR - http://dx.doi.org/10.1002/2017gl073056

U2 - 10.1002/2017gl073056

DO - 10.1002/2017gl073056

M3 - Article

SN - 0094-8276

VL - 44

SP - 5167

EP - 5177

JO - Geophysical Research Letters

JF - Geophysical Research Letters

IS - 10

ER -

Microphysical explanation of the RH‐dependent water affinity of biogenic organic aerosol and its importance for climate

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