Observed OH and HO2 in the upper troposphere suggest a major source from convective injection of peroxides

L. Jaeglé, D. J. Jacob, P. O. Wennberg, C. M. Spivakovsky, T. F. Hanisco, E. J. Lanzendorf, E. J. Hintsa, D. W. Fahey, E. R. Keim, M. H. Proffitt, Elliot L Atlas, F. Flocke, S. Schauffler, C. T. McElroy, C. Midwinter, L. Pfister, J. C. Wilson

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Abstract

ER-2 aircraft observations of OH and HO2 concentrations in the upper troposphere during the NASA/STRAT campaign are interpreted using a photochemical model constrained by local observations of O3, H2O, NO, CO, hydrocarbons, albedo and overhead ozone column. We find that the reaction O(1D) + H2O is minor compared to acetone photolysis as a primary source of HOx (= OH + peroxy radicals) in the upper troposphere. Calculations using a diel steady state model agree with observed HOx concentrations in the lower stratosphere and, for some flights, in the upper troposphere. However, for other flights in the upper troposphere, the steady state model underestimates observations by a factor of 2 or more. These model underestimates are found to be related to a recent (< 1 week) convective origin of the air. By conducting time-dependent model calculations along air trajectories determined for the STRAT flights, we show that convective injection of CH3OOH and H2O2 from the boundary layer to the upper troposphere could resolve the discrepancy. These injections of HOx reservoirs cause large HOx increases in the tropical upper troposphere for over a week downwind of the convective activity. We propose that this mechanism provides a major source of HOx in the upper troposphere. Simultaneous measurements of peroxides, formaldehyde and acetone along with OH and HO2 are needed to test our hypothesis.

Original languageEnglish (US)
Pages (from-to)3181-3184
Number of pages4
JournalGeophysical Research Letters
Volume24
Issue number24
StatePublished - 1997
Externally publishedYes

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peroxides
troposphere
injection
flight
acetone
U-2 aircraft
peroxy radical
air
stratosphere
photolysis
albedo
formaldehyde
ozone
boundary layers
aircraft
hydrocarbons
boundary layer
trajectory
trajectories
hydrocarbon

ASJC Scopus subject areas

  • Earth and Planetary Sciences (miscellaneous)

Cite this

Jaeglé, L., Jacob, D. J., Wennberg, P. O., Spivakovsky, C. M., Hanisco, T. F., Lanzendorf, E. J., ... Wilson, J. C. (1997). Observed OH and HO2 in the upper troposphere suggest a major source from convective injection of peroxides. Geophysical Research Letters, 24(24), 3181-3184.

Observed OH and HO2 in the upper troposphere suggest a major source from convective injection of peroxides. / Jaeglé, L.; Jacob, D. J.; Wennberg, P. O.; Spivakovsky, C. M.; Hanisco, T. F.; Lanzendorf, E. J.; Hintsa, E. J.; Fahey, D. W.; Keim, E. R.; Proffitt, M. H.; Atlas, Elliot L; Flocke, F.; Schauffler, S.; McElroy, C. T.; Midwinter, C.; Pfister, L.; Wilson, J. C.

In: Geophysical Research Letters, Vol. 24, No. 24, 1997, p. 3181-3184.

Research output: Contribution to journalArticle

Jaeglé, L, Jacob, DJ, Wennberg, PO, Spivakovsky, CM, Hanisco, TF, Lanzendorf, EJ, Hintsa, EJ, Fahey, DW, Keim, ER, Proffitt, MH, Atlas, EL, Flocke, F, Schauffler, S, McElroy, CT, Midwinter, C, Pfister, L & Wilson, JC 1997, 'Observed OH and HO2 in the upper troposphere suggest a major source from convective injection of peroxides', Geophysical Research Letters, vol. 24, no. 24, pp. 3181-3184.
Jaeglé L, Jacob DJ, Wennberg PO, Spivakovsky CM, Hanisco TF, Lanzendorf EJ et al. Observed OH and HO2 in the upper troposphere suggest a major source from convective injection of peroxides. Geophysical Research Letters. 1997;24(24):3181-3184.
Jaeglé, L. ; Jacob, D. J. ; Wennberg, P. O. ; Spivakovsky, C. M. ; Hanisco, T. F. ; Lanzendorf, E. J. ; Hintsa, E. J. ; Fahey, D. W. ; Keim, E. R. ; Proffitt, M. H. ; Atlas, Elliot L ; Flocke, F. ; Schauffler, S. ; McElroy, C. T. ; Midwinter, C. ; Pfister, L. ; Wilson, J. C. / Observed OH and HO2 in the upper troposphere suggest a major source from convective injection of peroxides. In: Geophysical Research Letters. 1997 ; Vol. 24, No. 24. pp. 3181-3184.
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abstract = "ER-2 aircraft observations of OH and HO2 concentrations in the upper troposphere during the NASA/STRAT campaign are interpreted using a photochemical model constrained by local observations of O3, H2O, NO, CO, hydrocarbons, albedo and overhead ozone column. We find that the reaction O(1D) + H2O is minor compared to acetone photolysis as a primary source of HOx (= OH + peroxy radicals) in the upper troposphere. Calculations using a diel steady state model agree with observed HOx concentrations in the lower stratosphere and, for some flights, in the upper troposphere. However, for other flights in the upper troposphere, the steady state model underestimates observations by a factor of 2 or more. These model underestimates are found to be related to a recent (< 1 week) convective origin of the air. By conducting time-dependent model calculations along air trajectories determined for the STRAT flights, we show that convective injection of CH3OOH and H2O2 from the boundary layer to the upper troposphere could resolve the discrepancy. These injections of HOx reservoirs cause large HOx increases in the tropical upper troposphere for over a week downwind of the convective activity. We propose that this mechanism provides a major source of HOx in the upper troposphere. Simultaneous measurements of peroxides, formaldehyde and acetone along with OH and HO2 are needed to test our hypothesis.",
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T1 - Observed OH and HO2 in the upper troposphere suggest a major source from convective injection of peroxides

AU - Jaeglé, L.

AU - Jacob, D. J.

AU - Wennberg, P. O.

AU - Spivakovsky, C. M.

AU - Hanisco, T. F.

AU - Lanzendorf, E. J.

AU - Hintsa, E. J.

AU - Fahey, D. W.

AU - Keim, E. R.

AU - Proffitt, M. H.

AU - Atlas, Elliot L

AU - Flocke, F.

AU - Schauffler, S.

AU - McElroy, C. T.

AU - Midwinter, C.

AU - Pfister, L.

AU - Wilson, J. C.

PY - 1997

Y1 - 1997

N2 - ER-2 aircraft observations of OH and HO2 concentrations in the upper troposphere during the NASA/STRAT campaign are interpreted using a photochemical model constrained by local observations of O3, H2O, NO, CO, hydrocarbons, albedo and overhead ozone column. We find that the reaction O(1D) + H2O is minor compared to acetone photolysis as a primary source of HOx (= OH + peroxy radicals) in the upper troposphere. Calculations using a diel steady state model agree with observed HOx concentrations in the lower stratosphere and, for some flights, in the upper troposphere. However, for other flights in the upper troposphere, the steady state model underestimates observations by a factor of 2 or more. These model underestimates are found to be related to a recent (< 1 week) convective origin of the air. By conducting time-dependent model calculations along air trajectories determined for the STRAT flights, we show that convective injection of CH3OOH and H2O2 from the boundary layer to the upper troposphere could resolve the discrepancy. These injections of HOx reservoirs cause large HOx increases in the tropical upper troposphere for over a week downwind of the convective activity. We propose that this mechanism provides a major source of HOx in the upper troposphere. Simultaneous measurements of peroxides, formaldehyde and acetone along with OH and HO2 are needed to test our hypothesis.

AB - ER-2 aircraft observations of OH and HO2 concentrations in the upper troposphere during the NASA/STRAT campaign are interpreted using a photochemical model constrained by local observations of O3, H2O, NO, CO, hydrocarbons, albedo and overhead ozone column. We find that the reaction O(1D) + H2O is minor compared to acetone photolysis as a primary source of HOx (= OH + peroxy radicals) in the upper troposphere. Calculations using a diel steady state model agree with observed HOx concentrations in the lower stratosphere and, for some flights, in the upper troposphere. However, for other flights in the upper troposphere, the steady state model underestimates observations by a factor of 2 or more. These model underestimates are found to be related to a recent (< 1 week) convective origin of the air. By conducting time-dependent model calculations along air trajectories determined for the STRAT flights, we show that convective injection of CH3OOH and H2O2 from the boundary layer to the upper troposphere could resolve the discrepancy. These injections of HOx reservoirs cause large HOx increases in the tropical upper troposphere for over a week downwind of the convective activity. We propose that this mechanism provides a major source of HOx in the upper troposphere. Simultaneous measurements of peroxides, formaldehyde and acetone along with OH and HO2 are needed to test our hypothesis.

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