Role of convection in redistributing formaldehyde to the upper troposhere over Noth Atlantic during the summer 2004 INTEX campaign

Alan Fried, Jennifer R. Olson, James G. Walega, Jim H. Crawford, Gao Chen, Peter Weibring, Dirk Richter, Chad Roller, Frank Tittel, Michael Porter, Henry Fuelberg, Jeremy Halland, Timothy H. Bertram, Ronald C. Cohen, Kenneth Pickering, Brian G. Heikes, Julie A. Snow, Haiwei Shen, Daniel W. O'Sullivan, William Henry Brune & 18 others Xinrong Ren, Donald R. Blake, Nicola Blake, Glen Sachse, Glenn S. Diskin, James Podolske, Stephanie A. Vay, Richard E. Shetter, Samuel R. Hall, Bruce E. Anderson, Lee Thornhill, Antony D. Clarke, Cameron S. McNaughton, Hanwant B. Singh, Melody A. Avery, Gregory Huey, Saewung Kim, Dylan B. Millet

Research output: Contribution to journalArticle

25 Citations (Scopus)

Abstract

Measurements of formaldehyde (CH2O) from a tunable diode laser absorption spectrometer (TDLAS) were acquired onboard the NASA DC-8 aircraft during the summer 2004 INTEX-NA campaign to test our understanding of convection and CH2O production mechanisms in the upper troposphere (UT, 6-12 km) over continental North America and the North Atlantic Ocean. The present study utilizes these TDLAS measurements and results from a box model to (1) establish sets of conditions by which to distinguish "background" UT CH2O levels from those perturbed by convection and other causes; (2) quantify the CH2O precursor budgets for both air mass types; (3) quantify the fraction of time that the UT CH2O measurements over North America and North Atlantic are perturbed during the summer of 2004; (4) provide estimates for the fraction of time that such perturbed CH2O levels are caused by direct convection of boundary layer CH2O and/or convection of CH2O precursors; (5) assess the ability of box models to reproduce the CH2O measurements; and (6) examine CH2O and HO2 relationships in the presence of enhanced NO. Multiple tracers were used to arrive at a set of UT CH2O background and perturbed air mass periods, and 46% of the TDLAS measurements fell within the latter category. In general, production of CH2O from CH4 was found to be the dominant source term, even in perturbed air masses. This was followed by production from methyl hydroperoxide, methanol, PAN-type compounds, and ketones, in descending order of their contribution. At least 70% to 73% of the elevated UT observations were caused by enhanced production from CH2O precursors rather than direct transport of CH2O from the boundary layer. In the, presence of elevated NO, there was a definite trend in the CH2O measurement-model discrepancy, and this was highly correlated with HO2 measurement-model discrepancies in the UT.

Original languageEnglish (US)
Article numberD17306
JournalJournal of Geophysical Research Atmospheres
Volume113
Issue number17
DOIs
StatePublished - Sep 16 2008

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formaldehyde
Formaldehyde
summer
convection
air mass
spectrometer
laser
air masses
spectrometers
boundary layer
lasers
Semiconductor lasers
Spectrometers
semiconductor lasers
air
ketone
boxes
boundary layers
DC 8 aircraft
Boundary layers

All Science Journal Classification (ASJC) codes

  • Geophysics
  • Forestry
  • Oceanography
  • Aquatic Science
  • Ecology
  • Water Science and Technology
  • Soil Science
  • Geochemistry and Petrology
  • Earth-Surface Processes
  • Atmospheric Science
  • Earth and Planetary Sciences (miscellaneous)
  • Space and Planetary Science
  • Palaeontology

Cite this

Fried, Alan ; Olson, Jennifer R. ; Walega, James G. ; Crawford, Jim H. ; Chen, Gao ; Weibring, Peter ; Richter, Dirk ; Roller, Chad ; Tittel, Frank ; Porter, Michael ; Fuelberg, Henry ; Halland, Jeremy ; Bertram, Timothy H. ; Cohen, Ronald C. ; Pickering, Kenneth ; Heikes, Brian G. ; Snow, Julie A. ; Shen, Haiwei ; O'Sullivan, Daniel W. ; Brune, William Henry ; Ren, Xinrong ; Blake, Donald R. ; Blake, Nicola ; Sachse, Glen ; Diskin, Glenn S. ; Podolske, James ; Vay, Stephanie A. ; Shetter, Richard E. ; Hall, Samuel R. ; Anderson, Bruce E. ; Thornhill, Lee ; Clarke, Antony D. ; McNaughton, Cameron S. ; Singh, Hanwant B. ; Avery, Melody A. ; Huey, Gregory ; Kim, Saewung ; Millet, Dylan B. / Role of convection in redistributing formaldehyde to the upper troposhere over Noth Atlantic during the summer 2004 INTEX campaign. In: Journal of Geophysical Research Atmospheres. 2008 ; Vol. 113, No. 17.
@article{e0f74970354f49958ab51182575397a2,
title = "Role of convection in redistributing formaldehyde to the upper troposhere over Noth Atlantic during the summer 2004 INTEX campaign",
abstract = "Measurements of formaldehyde (CH2O) from a tunable diode laser absorption spectrometer (TDLAS) were acquired onboard the NASA DC-8 aircraft during the summer 2004 INTEX-NA campaign to test our understanding of convection and CH2O production mechanisms in the upper troposphere (UT, 6-12 km) over continental North America and the North Atlantic Ocean. The present study utilizes these TDLAS measurements and results from a box model to (1) establish sets of conditions by which to distinguish {"}background{"} UT CH2O levels from those perturbed by convection and other causes; (2) quantify the CH2O precursor budgets for both air mass types; (3) quantify the fraction of time that the UT CH2O measurements over North America and North Atlantic are perturbed during the summer of 2004; (4) provide estimates for the fraction of time that such perturbed CH2O levels are caused by direct convection of boundary layer CH2O and/or convection of CH2O precursors; (5) assess the ability of box models to reproduce the CH2O measurements; and (6) examine CH2O and HO2 relationships in the presence of enhanced NO. Multiple tracers were used to arrive at a set of UT CH2O background and perturbed air mass periods, and 46{\%} of the TDLAS measurements fell within the latter category. In general, production of CH2O from CH4 was found to be the dominant source term, even in perturbed air masses. This was followed by production from methyl hydroperoxide, methanol, PAN-type compounds, and ketones, in descending order of their contribution. At least 70{\%} to 73{\%} of the elevated UT observations were caused by enhanced production from CH2O precursors rather than direct transport of CH2O from the boundary layer. In the, presence of elevated NO, there was a definite trend in the CH2O measurement-model discrepancy, and this was highly correlated with HO2 measurement-model discrepancies in the UT.",
author = "Alan Fried and Olson, {Jennifer R.} and Walega, {James G.} and Crawford, {Jim H.} and Gao Chen and Peter Weibring and Dirk Richter and Chad Roller and Frank Tittel and Michael Porter and Henry Fuelberg and Jeremy Halland and Bertram, {Timothy H.} and Cohen, {Ronald C.} and Kenneth Pickering and Heikes, {Brian G.} and Snow, {Julie A.} and Haiwei Shen and O'Sullivan, {Daniel W.} and Brune, {William Henry} and Xinrong Ren and Blake, {Donald R.} and Nicola Blake and Glen Sachse and Diskin, {Glenn S.} and James Podolske and Vay, {Stephanie A.} and Shetter, {Richard E.} and Hall, {Samuel R.} and Anderson, {Bruce E.} and Lee Thornhill and Clarke, {Antony D.} and McNaughton, {Cameron S.} and Singh, {Hanwant B.} and Avery, {Melody A.} and Gregory Huey and Saewung Kim and Millet, {Dylan B.}",
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month = "9",
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doi = "10.1029/2007JD009760",
language = "English (US)",
volume = "113",
journal = "Journal of Geophysical Research: Atmospheres",
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number = "17",

}

Fried, A, Olson, JR, Walega, JG, Crawford, JH, Chen, G, Weibring, P, Richter, D, Roller, C, Tittel, F, Porter, M, Fuelberg, H, Halland, J, Bertram, TH, Cohen, RC, Pickering, K, Heikes, BG, Snow, JA, Shen, H, O'Sullivan, DW, Brune, WH, Ren, X, Blake, DR, Blake, N, Sachse, G, Diskin, GS, Podolske, J, Vay, SA, Shetter, RE, Hall, SR, Anderson, BE, Thornhill, L, Clarke, AD, McNaughton, CS, Singh, HB, Avery, MA, Huey, G, Kim, S & Millet, DB 2008, 'Role of convection in redistributing formaldehyde to the upper troposhere over Noth Atlantic during the summer 2004 INTEX campaign', Journal of Geophysical Research Atmospheres, vol. 113, no. 17, D17306. https://doi.org/10.1029/2007JD009760

Role of convection in redistributing formaldehyde to the upper troposhere over Noth Atlantic during the summer 2004 INTEX campaign. / Fried, Alan; Olson, Jennifer R.; Walega, James G.; Crawford, Jim H.; Chen, Gao; Weibring, Peter; Richter, Dirk; Roller, Chad; Tittel, Frank; Porter, Michael; Fuelberg, Henry; Halland, Jeremy; Bertram, Timothy H.; Cohen, Ronald C.; Pickering, Kenneth; Heikes, Brian G.; Snow, Julie A.; Shen, Haiwei; O'Sullivan, Daniel W.; Brune, William Henry; Ren, Xinrong; Blake, Donald R.; Blake, Nicola; Sachse, Glen; Diskin, Glenn S.; Podolske, James; Vay, Stephanie A.; Shetter, Richard E.; Hall, Samuel R.; Anderson, Bruce E.; Thornhill, Lee; Clarke, Antony D.; McNaughton, Cameron S.; Singh, Hanwant B.; Avery, Melody A.; Huey, Gregory; Kim, Saewung; Millet, Dylan B.

In: Journal of Geophysical Research Atmospheres, Vol. 113, No. 17, D17306, 16.09.2008.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Role of convection in redistributing formaldehyde to the upper troposhere over Noth Atlantic during the summer 2004 INTEX campaign

AU - Fried, Alan

AU - Olson, Jennifer R.

AU - Walega, James G.

AU - Crawford, Jim H.

AU - Chen, Gao

AU - Weibring, Peter

AU - Richter, Dirk

AU - Roller, Chad

AU - Tittel, Frank

AU - Porter, Michael

AU - Fuelberg, Henry

AU - Halland, Jeremy

AU - Bertram, Timothy H.

AU - Cohen, Ronald C.

AU - Pickering, Kenneth

AU - Heikes, Brian G.

AU - Snow, Julie A.

AU - Shen, Haiwei

AU - O'Sullivan, Daniel W.

AU - Brune, William Henry

AU - Ren, Xinrong

AU - Blake, Donald R.

AU - Blake, Nicola

AU - Sachse, Glen

AU - Diskin, Glenn S.

AU - Podolske, James

AU - Vay, Stephanie A.

AU - Shetter, Richard E.

AU - Hall, Samuel R.

AU - Anderson, Bruce E.

AU - Thornhill, Lee

AU - Clarke, Antony D.

AU - McNaughton, Cameron S.

AU - Singh, Hanwant B.

AU - Avery, Melody A.

AU - Huey, Gregory

AU - Kim, Saewung

AU - Millet, Dylan B.

PY - 2008/9/16

Y1 - 2008/9/16

N2 - Measurements of formaldehyde (CH2O) from a tunable diode laser absorption spectrometer (TDLAS) were acquired onboard the NASA DC-8 aircraft during the summer 2004 INTEX-NA campaign to test our understanding of convection and CH2O production mechanisms in the upper troposphere (UT, 6-12 km) over continental North America and the North Atlantic Ocean. The present study utilizes these TDLAS measurements and results from a box model to (1) establish sets of conditions by which to distinguish "background" UT CH2O levels from those perturbed by convection and other causes; (2) quantify the CH2O precursor budgets for both air mass types; (3) quantify the fraction of time that the UT CH2O measurements over North America and North Atlantic are perturbed during the summer of 2004; (4) provide estimates for the fraction of time that such perturbed CH2O levels are caused by direct convection of boundary layer CH2O and/or convection of CH2O precursors; (5) assess the ability of box models to reproduce the CH2O measurements; and (6) examine CH2O and HO2 relationships in the presence of enhanced NO. Multiple tracers were used to arrive at a set of UT CH2O background and perturbed air mass periods, and 46% of the TDLAS measurements fell within the latter category. In general, production of CH2O from CH4 was found to be the dominant source term, even in perturbed air masses. This was followed by production from methyl hydroperoxide, methanol, PAN-type compounds, and ketones, in descending order of their contribution. At least 70% to 73% of the elevated UT observations were caused by enhanced production from CH2O precursors rather than direct transport of CH2O from the boundary layer. In the, presence of elevated NO, there was a definite trend in the CH2O measurement-model discrepancy, and this was highly correlated with HO2 measurement-model discrepancies in the UT.

AB - Measurements of formaldehyde (CH2O) from a tunable diode laser absorption spectrometer (TDLAS) were acquired onboard the NASA DC-8 aircraft during the summer 2004 INTEX-NA campaign to test our understanding of convection and CH2O production mechanisms in the upper troposphere (UT, 6-12 km) over continental North America and the North Atlantic Ocean. The present study utilizes these TDLAS measurements and results from a box model to (1) establish sets of conditions by which to distinguish "background" UT CH2O levels from those perturbed by convection and other causes; (2) quantify the CH2O precursor budgets for both air mass types; (3) quantify the fraction of time that the UT CH2O measurements over North America and North Atlantic are perturbed during the summer of 2004; (4) provide estimates for the fraction of time that such perturbed CH2O levels are caused by direct convection of boundary layer CH2O and/or convection of CH2O precursors; (5) assess the ability of box models to reproduce the CH2O measurements; and (6) examine CH2O and HO2 relationships in the presence of enhanced NO. Multiple tracers were used to arrive at a set of UT CH2O background and perturbed air mass periods, and 46% of the TDLAS measurements fell within the latter category. In general, production of CH2O from CH4 was found to be the dominant source term, even in perturbed air masses. This was followed by production from methyl hydroperoxide, methanol, PAN-type compounds, and ketones, in descending order of their contribution. At least 70% to 73% of the elevated UT observations were caused by enhanced production from CH2O precursors rather than direct transport of CH2O from the boundary layer. In the, presence of elevated NO, there was a definite trend in the CH2O measurement-model discrepancy, and this was highly correlated with HO2 measurement-model discrepancies in the UT.

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UR - http://www.scopus.com/inward/citedby.url?scp=56349085641&partnerID=8YFLogxK

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DO - 10.1029/2007JD009760

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JO - Journal of Geophysical Research: Atmospheres

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SN - 2169-897X

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