Understanding isoprene photooxidation using observations and modeling over a subtropical forest in the southeastern US

Luping Su, Edward G. Patton, Jordi Vilà Guerau De Arellano, Alex B. Guenther, Lisa Kaser, Bin Yuan, Fulizi Xiong, Paul B. Shepson, Li Zhang, David O. Miller, William H. Brune, Karsten Baumann, Eric Edgerton, Andrew Weinheimer, Pawel K. Misztal, Jeong Hoo Park, Allen H. Goldstein, Kate M. Skog, Frank N. Keutsch, John E. Mak

Research output: Contribution to journalArticle

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Abstract

The emission, dispersion, and photochemistry of isoprene (C5H8) and related chemical species in the convective boundary layer (CBL) during sunlit daytime were studied over a mixed forest in the southeastern United States by combining ground-based and aircraft observations. Fluxes of isoprene and monoterpenes were quantified at the top of the forest canopy using a high-resolution proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS). Snapshot (2 min sampling duration) vertical profiles of isoprene, methyl vinyl ketone (MVK)Cmethacrolein (MACR), and monoterpenes were collected from aircraft every hour in the CBL (100-1000 m). Both ground-based and airborne collected volatile organic compound (VOC) data are used to constrain the initial conditions of a mixed-layer chemistry model (MXLCH), which is applied to examine the chemical evolution of the O3-NOx-HOx-VOC system and how it is affected by boundary layer dynamics in the CBL. The chemical loss rate of isoprene (1 h) is similar to the turbulent mixing timescale (0.1-0.5 h), which indicates that isoprene concentrations are equally dependent on both photooxidation and boundary layer dynamics. Analysis of a modelderived concentration budget suggests that diurnal evolution of isoprene inside the CBL is mainly controlled by surface emissions and chemical loss; the diurnal evolution of O3 is dominated by entrainment. The NO to HO2 ratio (NO :HO2) is used as an indicator of anthropogenic impact on the CBL chemical composition and spans a wide range (1-163). The fate of hydroxyl-substituted isoprene peroxyl radical (HOC5H8OO q; ISOPOO) is strongly affected by NO:HO2, shifting from NO-dominant to NO-HO2-balanced conditions from early morning to noontime. This chemical regime change is reflected in the diurnal evolution of isoprene hydroxynitrates (ISOPN) and isoprene hydroxy hydroperoxides (ISOPOOH).

Original languageEnglish (US)
Pages (from-to)7725-7741
Number of pages17
JournalAtmospheric Chemistry and Physics
Volume16
Issue number12
DOIs
StatePublished - Jun 24 2016

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isoprene
photooxidation
convective boundary layer
modeling
monoterpene
volatile organic compound
aircraft
boundary layer
turbulent mixing
photochemistry
ketone
forest canopy
mixed forest
entrainment
vertical profile
mixed layer
spectrometer
chemical composition
chemical
timescale

All Science Journal Classification (ASJC) codes

  • Atmospheric Science

Cite this

Su, L., Patton, E. G., De Arellano, J. V. G., Guenther, A. B., Kaser, L., Yuan, B., ... Mak, J. E. (2016). Understanding isoprene photooxidation using observations and modeling over a subtropical forest in the southeastern US. Atmospheric Chemistry and Physics, 16(12), 7725-7741. https://doi.org/10.5194/acp-16-7725-2016
Su, Luping ; Patton, Edward G. ; De Arellano, Jordi Vilà Guerau ; Guenther, Alex B. ; Kaser, Lisa ; Yuan, Bin ; Xiong, Fulizi ; Shepson, Paul B. ; Zhang, Li ; Miller, David O. ; Brune, William H. ; Baumann, Karsten ; Edgerton, Eric ; Weinheimer, Andrew ; Misztal, Pawel K. ; Park, Jeong Hoo ; Goldstein, Allen H. ; Skog, Kate M. ; Keutsch, Frank N. ; Mak, John E. / Understanding isoprene photooxidation using observations and modeling over a subtropical forest in the southeastern US. In: Atmospheric Chemistry and Physics. 2016 ; Vol. 16, No. 12. pp. 7725-7741.
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abstract = "The emission, dispersion, and photochemistry of isoprene (C5H8) and related chemical species in the convective boundary layer (CBL) during sunlit daytime were studied over a mixed forest in the southeastern United States by combining ground-based and aircraft observations. Fluxes of isoprene and monoterpenes were quantified at the top of the forest canopy using a high-resolution proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS). Snapshot (2 min sampling duration) vertical profiles of isoprene, methyl vinyl ketone (MVK)Cmethacrolein (MACR), and monoterpenes were collected from aircraft every hour in the CBL (100-1000 m). Both ground-based and airborne collected volatile organic compound (VOC) data are used to constrain the initial conditions of a mixed-layer chemistry model (MXLCH), which is applied to examine the chemical evolution of the O3-NOx-HOx-VOC system and how it is affected by boundary layer dynamics in the CBL. The chemical loss rate of isoprene (1 h) is similar to the turbulent mixing timescale (0.1-0.5 h), which indicates that isoprene concentrations are equally dependent on both photooxidation and boundary layer dynamics. Analysis of a modelderived concentration budget suggests that diurnal evolution of isoprene inside the CBL is mainly controlled by surface emissions and chemical loss; the diurnal evolution of O3 is dominated by entrainment. The NO to HO2 ratio (NO :HO2) is used as an indicator of anthropogenic impact on the CBL chemical composition and spans a wide range (1-163). The fate of hydroxyl-substituted isoprene peroxyl radical (HOC5H8OO q; ISOPOO) is strongly affected by NO:HO2, shifting from NO-dominant to NO-HO2-balanced conditions from early morning to noontime. This chemical regime change is reflected in the diurnal evolution of isoprene hydroxynitrates (ISOPN) and isoprene hydroxy hydroperoxides (ISOPOOH).",
author = "Luping Su and Patton, {Edward G.} and {De Arellano}, {Jordi Vil{\`a} Guerau} and Guenther, {Alex B.} and Lisa Kaser and Bin Yuan and Fulizi Xiong and Shepson, {Paul B.} and Li Zhang and Miller, {David O.} and Brune, {William H.} and Karsten Baumann and Eric Edgerton and Andrew Weinheimer and Misztal, {Pawel K.} and Park, {Jeong Hoo} and Goldstein, {Allen H.} and Skog, {Kate M.} and Keutsch, {Frank N.} and Mak, {John E.}",
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Su, L, Patton, EG, De Arellano, JVG, Guenther, AB, Kaser, L, Yuan, B, Xiong, F, Shepson, PB, Zhang, L, Miller, DO, Brune, WH, Baumann, K, Edgerton, E, Weinheimer, A, Misztal, PK, Park, JH, Goldstein, AH, Skog, KM, Keutsch, FN & Mak, JE 2016, 'Understanding isoprene photooxidation using observations and modeling over a subtropical forest in the southeastern US', Atmospheric Chemistry and Physics, vol. 16, no. 12, pp. 7725-7741. https://doi.org/10.5194/acp-16-7725-2016

Understanding isoprene photooxidation using observations and modeling over a subtropical forest in the southeastern US. / Su, Luping; Patton, Edward G.; De Arellano, Jordi Vilà Guerau; Guenther, Alex B.; Kaser, Lisa; Yuan, Bin; Xiong, Fulizi; Shepson, Paul B.; Zhang, Li; Miller, David O.; Brune, William H.; Baumann, Karsten; Edgerton, Eric; Weinheimer, Andrew; Misztal, Pawel K.; Park, Jeong Hoo; Goldstein, Allen H.; Skog, Kate M.; Keutsch, Frank N.; Mak, John E.

In: Atmospheric Chemistry and Physics, Vol. 16, No. 12, 24.06.2016, p. 7725-7741.

Research output: Contribution to journalArticle

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T1 - Understanding isoprene photooxidation using observations and modeling over a subtropical forest in the southeastern US

AU - Su, Luping

AU - Patton, Edward G.

AU - De Arellano, Jordi Vilà Guerau

AU - Guenther, Alex B.

AU - Kaser, Lisa

AU - Yuan, Bin

AU - Xiong, Fulizi

AU - Shepson, Paul B.

AU - Zhang, Li

AU - Miller, David O.

AU - Brune, William H.

AU - Baumann, Karsten

AU - Edgerton, Eric

AU - Weinheimer, Andrew

AU - Misztal, Pawel K.

AU - Park, Jeong Hoo

AU - Goldstein, Allen H.

AU - Skog, Kate M.

AU - Keutsch, Frank N.

AU - Mak, John E.

PY - 2016/6/24

Y1 - 2016/6/24

N2 - The emission, dispersion, and photochemistry of isoprene (C5H8) and related chemical species in the convective boundary layer (CBL) during sunlit daytime were studied over a mixed forest in the southeastern United States by combining ground-based and aircraft observations. Fluxes of isoprene and monoterpenes were quantified at the top of the forest canopy using a high-resolution proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS). Snapshot (2 min sampling duration) vertical profiles of isoprene, methyl vinyl ketone (MVK)Cmethacrolein (MACR), and monoterpenes were collected from aircraft every hour in the CBL (100-1000 m). Both ground-based and airborne collected volatile organic compound (VOC) data are used to constrain the initial conditions of a mixed-layer chemistry model (MXLCH), which is applied to examine the chemical evolution of the O3-NOx-HOx-VOC system and how it is affected by boundary layer dynamics in the CBL. The chemical loss rate of isoprene (1 h) is similar to the turbulent mixing timescale (0.1-0.5 h), which indicates that isoprene concentrations are equally dependent on both photooxidation and boundary layer dynamics. Analysis of a modelderived concentration budget suggests that diurnal evolution of isoprene inside the CBL is mainly controlled by surface emissions and chemical loss; the diurnal evolution of O3 is dominated by entrainment. The NO to HO2 ratio (NO :HO2) is used as an indicator of anthropogenic impact on the CBL chemical composition and spans a wide range (1-163). The fate of hydroxyl-substituted isoprene peroxyl radical (HOC5H8OO q; ISOPOO) is strongly affected by NO:HO2, shifting from NO-dominant to NO-HO2-balanced conditions from early morning to noontime. This chemical regime change is reflected in the diurnal evolution of isoprene hydroxynitrates (ISOPN) and isoprene hydroxy hydroperoxides (ISOPOOH).

AB - The emission, dispersion, and photochemistry of isoprene (C5H8) and related chemical species in the convective boundary layer (CBL) during sunlit daytime were studied over a mixed forest in the southeastern United States by combining ground-based and aircraft observations. Fluxes of isoprene and monoterpenes were quantified at the top of the forest canopy using a high-resolution proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS). Snapshot (2 min sampling duration) vertical profiles of isoprene, methyl vinyl ketone (MVK)Cmethacrolein (MACR), and monoterpenes were collected from aircraft every hour in the CBL (100-1000 m). Both ground-based and airborne collected volatile organic compound (VOC) data are used to constrain the initial conditions of a mixed-layer chemistry model (MXLCH), which is applied to examine the chemical evolution of the O3-NOx-HOx-VOC system and how it is affected by boundary layer dynamics in the CBL. The chemical loss rate of isoprene (1 h) is similar to the turbulent mixing timescale (0.1-0.5 h), which indicates that isoprene concentrations are equally dependent on both photooxidation and boundary layer dynamics. Analysis of a modelderived concentration budget suggests that diurnal evolution of isoprene inside the CBL is mainly controlled by surface emissions and chemical loss; the diurnal evolution of O3 is dominated by entrainment. The NO to HO2 ratio (NO :HO2) is used as an indicator of anthropogenic impact on the CBL chemical composition and spans a wide range (1-163). The fate of hydroxyl-substituted isoprene peroxyl radical (HOC5H8OO q; ISOPOO) is strongly affected by NO:HO2, shifting from NO-dominant to NO-HO2-balanced conditions from early morning to noontime. This chemical regime change is reflected in the diurnal evolution of isoprene hydroxynitrates (ISOPN) and isoprene hydroxy hydroperoxides (ISOPOOH).

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