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Missing OH reactivity in the global marine boundary layer

Thames, Alexander B. and Brune, William H. and Miller, David O. and Allen, Hannah M. and Apel, Eric C. and Blake, Donald R. and Bui, T. Paul and Commane, Roisin and Crounse, John D. and Daube, Bruce C. and Diskin, Glenn S. and DiGangi, Joshua P. and Elkins, James W. and Hall, Samuel R. and Hanisco, Thomas F. and Hannun, Reem A. and Hintsa, Eric and Hornbrook, Rebecca S. and Kim, Michelle J. and McKain, Kathryn and Moore, Fred L. and Nicely, Julie M. and Peischl, Jeffrey and Ryerson, Thomas B. and St. Clair, Jason M. and Sweeney, Colm and Teng, Alex and Thompson, Chelsea R. and Ullmann, Kirk and Wennberg, Paul O. and Wolfe, Glenn M. (2020) Missing OH reactivity in the global marine boundary layer. Atmospheric Chemistry and Physics, 20 (6). pp. 4013-4029. ISSN 1680-7324. doi:10.5194/acp-20-4013-2020.

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The hydroxyl radical (OH) reacts with thousands of chemical species in the atmosphere, initiating their removal and the chemical reaction sequences that produce ozone, secondary aerosols, and gas-phase acids. OH reactivity, which is the inverse of OH lifetime, influences the OH abundance and the ability of OH to cleanse the atmosphere. The NASA Atmospheric Tomography (ATom) campaign used instruments on the NASA DC-8 aircraft to measure OH reactivity and more than 100 trace chemical species. ATom presented a unique opportunity to test the completeness of the OH reactivity calculated from the chemical species measurements by comparing it to the measured OH reactivity over two oceans across four seasons. Although the calculated OH reactivity was below the limit of detection for the ATom instrument used to measure OH reactivity throughout much of the free troposphere, the instrument was able to measure the OH reactivity in and just above the marine boundary layer. The mean measured value of OH reactivity in the marine boundary layer across all latitudes and all ATom deployments was 1.9 s⁻¹, which is 0.5 s⁻¹ larger than the mean calculated OH reactivity. The missing OH reactivity, the difference between the measured and calculated OH reactivity, varied between 0 and 3.5 s⁻¹, with the highest values over the Northern Hemisphere Pacific Ocean. Correlations of missing OH reactivity with formaldehyde, dimethyl sulfide, butanal, and sea surface temperature suggest the presence of unmeasured or unknown volatile organic compounds or oxygenated volatile organic compounds associated with ocean emissions.

Item Type:Article
Related URLs:
URLURL TypeDescription
Brune, William H.0000-0002-1609-4051
Apel, Eric C.0000-0001-9421-818X
Blake, Donald R.0000-0002-8283-5014
Commane, Roisin0000-0003-1373-1550
Crounse, John D.0000-0001-5443-729X
Diskin, Glenn S.0000-0002-3617-0269
DiGangi, Joshua P.0000-0002-6764-8624
Elkins, James W.0000-0003-4701-3100
Hall, Samuel R.0000-0002-2060-7112
Hanisco, Thomas F.0000-0001-9434-8507
Hannun, Reem A.0000-0001-5195-5307
Hintsa, Eric0000-0002-5289-630X
Hornbrook, Rebecca S.0000-0002-6304-6554
Kim, Michelle J.0000-0002-4922-4334
McKain, Kathryn0000-0002-8323-5758
Moore, Fred L.0000-0002-8461-2535
Nicely, Julie M.0000-0003-4828-0032
Peischl, Jeffrey0000-0002-9320-7101
Ryerson, Thomas B.0000-0003-2800-7581
St. Clair, Jason M.0000-0002-9367-5749
Sweeney, Colm0000-0001-9568-0050
Thompson, Chelsea R.0000-0002-7332-9945
Ullmann, Kirk0000-0002-4724-9634
Wennberg, Paul O.0000-0002-6126-3854
Wolfe, Glenn M.0000-0001-6586-4043
Additional Information:© 2020 The Author(s). This work is distributed under the Creative Commons Attribution 4.0 License. Published by Copernicus Publications on behalf of the European Geosciences Union. Received: 24 Sep 2019 – Discussion started: 16 Oct 2019 – Revised: 30 Jan 2020 – Accepted: 02 Mar 2020 – Published: 02 Apr 2020. The authors thank the NASA ATom management team, pilots, logistical support team, aircraft operations team, and fellow scientists. We thank the reviewers for their helpful comments on the initial submission. Data availability. The data and model used in this paper are publicly available: data: (Wofsy et al., 2018); model framework: (last access: 12 July 2019); and MCMv331 chemical mechanism: (Rickard et al., 1997). Author contributions. ABT, DOM, and WHB made the OH, HO2, and OH reactivity measurements; performed the model runs; analyzed the data; and wrote the manuscript. GMW provided support of the use of the F0AM model framework used for the model runs. WHB, DOM, ABT, HMA, DRB, TPB, RC, JDC, BCD, GSD, JPD, JWE, SRH, TFH, RAH, EH, MJK, KM, FLM, JMN, JP, TBR, JMS, CS, APT, CT, KU, POW, and GMW provided ATom measurements used for the modeling and reviewed and edited the manuscript. The authors declare that they have no conflict of interest. This research has been supported by NASA (grant no. NNX15AG59A). This material is based upon work supported by the National Center for Atmospheric Research, which is a major facility sponsored by the National Science Foundation under cooperative agreement no. 1852977. Review statement. This paper was edited by Andreas Hofzumahaus and reviewed by two anonymous referees.
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Issue or Number:6
Record Number:CaltechAUTHORS:20200417-110627301
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Official Citation:Thames, A. B., Brune, W. H., Miller, D. O., Allen, H. M., Apel, E. C., Blake, D. R., Bui, T. P., Commane, R., Crounse, J. D., Daube, B. C., Diskin, G. S., DiGangi, J. P., Elkins, J. W., Hall, S. R., Hanisco, T. F., Hannun, R. A., Hintsa, E., Hornbrook, R. S., Kim, M. J., McKain, K., Moore, F. L., Nicely, J. M., Peischl, J., Ryerson, T. B., St. Clair, J. M., Sweeney, C., Teng, A., Thompson, C. R., Ullmann, K., Wennberg, P. O., and Wolfe, G. M.: Missing OH reactivity in the global marine boundary layer, Atmos. Chem. Phys., 20, 4013–4029,, 2020
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:102598
Deposited By: Tony Diaz
Deposited On:17 Apr 2020 18:35
Last Modified:16 Nov 2021 18:13

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