Mapping hydroxyl variability throughout the global remote troposphere via synthesis of airborne and satellite formaldehyde observations

Glenn M. Wolfe, Julie M. Nicely, Jason M.St Clair, Thomas F. Hanisco, Jin Liao, Luke D. Oman, William B. Brune, David Miller, Alexander Thames, Gonzalo González Abad, Thomas B. Ryerson, Chelsea R. Thompson, Jeff Peischl, Kathryn McCain, Colm Sweeney, Paul O. Wennberg, Michelle Kim, John D. Crounse, Samuel R. Hall, Kirk UllmannGlenn Diskin, Paul Bui, Cecilia Chang, Jonathan Dean-Day

Research output: Contribution to journalArticle

3 Citations (Scopus)

Abstract

The hydroxyl radical (OH) fuels tropospheric ozone production and governs the lifetime of methane and many other gases. Existing methods to quantify global OH are limited to annual and global-to-hemispheric averages. Finer resolution is essential for isolating model deficiencies and building process-level understanding. In situ observations from the Atmospheric Tomography (ATom) mission demonstrate that remote tropospheric OH is tightly coupled to the production and loss of formaldehyde (HCHO), a major hydrocarbon oxidation product. Synthesis of this relationship with satellite-based HCHO retrievals and model-derived HCHO loss frequencies yields a map of total-column OH abundance throughout the remote troposphere (up to 70% of tropospheric mass) over the first two ATom missions (August 2016 and February 2017). This dataset offers unique insights on near-global oxidizing capacity. OH exhibits significant seasonality within individual hemispheres, but the domain mean concentration is nearly identical for both seasons (1.03 ± 0.25 × 106 cm−3), and the biseasonal average North/South Hemisphere ratio is 0.89 ± 0.06, consistent with a balance of OH sources and sinks across the remote troposphere. Regional phenomena are also highlighted, such as a 10-fold OH depression in the Tropical West Pacific and enhancements in the East Pacific and South Atlantic. This method is complementary to budget-based global OH constraints and can help elucidate the spatial and temporal variability of OH production and methane loss.

Original languageEnglish (US)
Pages (from-to)11171-11180
Number of pages10
JournalProceedings of the National Academy of Sciences of the United States of America
Volume166
Issue number23
DOIs
StatePublished - Jun 4 2019

Fingerprint

Methane
Hydroxyl Radical
Formaldehyde
Tomography
Ozone
Budgets
Hydrocarbons
Gases
Datasets

All Science Journal Classification (ASJC) codes

  • General

Cite this

Wolfe, Glenn M. ; Nicely, Julie M. ; Clair, Jason M.St ; Hanisco, Thomas F. ; Liao, Jin ; Oman, Luke D. ; Brune, William B. ; Miller, David ; Thames, Alexander ; Abad, Gonzalo González ; Ryerson, Thomas B. ; Thompson, Chelsea R. ; Peischl, Jeff ; McCain, Kathryn ; Sweeney, Colm ; Wennberg, Paul O. ; Kim, Michelle ; Crounse, John D. ; Hall, Samuel R. ; Ullmann, Kirk ; Diskin, Glenn ; Bui, Paul ; Chang, Cecilia ; Dean-Day, Jonathan. / Mapping hydroxyl variability throughout the global remote troposphere via synthesis of airborne and satellite formaldehyde observations. In: Proceedings of the National Academy of Sciences of the United States of America. 2019 ; Vol. 166, No. 23. pp. 11171-11180.
@article{3978992d7a0444cf850f8554e64f0255,
title = "Mapping hydroxyl variability throughout the global remote troposphere via synthesis of airborne and satellite formaldehyde observations",
abstract = "The hydroxyl radical (OH) fuels tropospheric ozone production and governs the lifetime of methane and many other gases. Existing methods to quantify global OH are limited to annual and global-to-hemispheric averages. Finer resolution is essential for isolating model deficiencies and building process-level understanding. In situ observations from the Atmospheric Tomography (ATom) mission demonstrate that remote tropospheric OH is tightly coupled to the production and loss of formaldehyde (HCHO), a major hydrocarbon oxidation product. Synthesis of this relationship with satellite-based HCHO retrievals and model-derived HCHO loss frequencies yields a map of total-column OH abundance throughout the remote troposphere (up to 70{\%} of tropospheric mass) over the first two ATom missions (August 2016 and February 2017). This dataset offers unique insights on near-global oxidizing capacity. OH exhibits significant seasonality within individual hemispheres, but the domain mean concentration is nearly identical for both seasons (1.03 ± 0.25 × 106 cm−3), and the biseasonal average North/South Hemisphere ratio is 0.89 ± 0.06, consistent with a balance of OH sources and sinks across the remote troposphere. Regional phenomena are also highlighted, such as a 10-fold OH depression in the Tropical West Pacific and enhancements in the East Pacific and South Atlantic. This method is complementary to budget-based global OH constraints and can help elucidate the spatial and temporal variability of OH production and methane loss.",
author = "Wolfe, {Glenn M.} and Nicely, {Julie M.} and Clair, {Jason M.St} and Hanisco, {Thomas F.} and Jin Liao and Oman, {Luke D.} and Brune, {William B.} and David Miller and Alexander Thames and Abad, {Gonzalo Gonz{\'a}lez} and Ryerson, {Thomas B.} and Thompson, {Chelsea R.} and Jeff Peischl and Kathryn McCain and Colm Sweeney and Wennberg, {Paul O.} and Michelle Kim and Crounse, {John D.} and Hall, {Samuel R.} and Kirk Ullmann and Glenn Diskin and Paul Bui and Cecilia Chang and Jonathan Dean-Day",
year = "2019",
month = "6",
day = "4",
doi = "10.1073/pnas.1821661116",
language = "English (US)",
volume = "166",
pages = "11171--11180",
journal = "Proceedings of the National Academy of Sciences of the United States of America",
issn = "0027-8424",
number = "23",

}

Wolfe, GM, Nicely, JM, Clair, JMS, Hanisco, TF, Liao, J, Oman, LD, Brune, WB, Miller, D, Thames, A, Abad, GG, Ryerson, TB, Thompson, CR, Peischl, J, McCain, K, Sweeney, C, Wennberg, PO, Kim, M, Crounse, JD, Hall, SR, Ullmann, K, Diskin, G, Bui, P, Chang, C & Dean-Day, J 2019, 'Mapping hydroxyl variability throughout the global remote troposphere via synthesis of airborne and satellite formaldehyde observations', Proceedings of the National Academy of Sciences of the United States of America, vol. 166, no. 23, pp. 11171-11180. https://doi.org/10.1073/pnas.1821661116

Mapping hydroxyl variability throughout the global remote troposphere via synthesis of airborne and satellite formaldehyde observations. / Wolfe, Glenn M.; Nicely, Julie M.; Clair, Jason M.St; Hanisco, Thomas F.; Liao, Jin; Oman, Luke D.; Brune, William B.; Miller, David; Thames, Alexander; Abad, Gonzalo González; Ryerson, Thomas B.; Thompson, Chelsea R.; Peischl, Jeff; McCain, Kathryn; Sweeney, Colm; Wennberg, Paul O.; Kim, Michelle; Crounse, John D.; Hall, Samuel R.; Ullmann, Kirk; Diskin, Glenn; Bui, Paul; Chang, Cecilia; Dean-Day, Jonathan.

In: Proceedings of the National Academy of Sciences of the United States of America, Vol. 166, No. 23, 04.06.2019, p. 11171-11180.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Mapping hydroxyl variability throughout the global remote troposphere via synthesis of airborne and satellite formaldehyde observations

AU - Wolfe, Glenn M.

AU - Nicely, Julie M.

AU - Clair, Jason M.St

AU - Hanisco, Thomas F.

AU - Liao, Jin

AU - Oman, Luke D.

AU - Brune, William B.

AU - Miller, David

AU - Thames, Alexander

AU - Abad, Gonzalo González

AU - Ryerson, Thomas B.

AU - Thompson, Chelsea R.

AU - Peischl, Jeff

AU - McCain, Kathryn

AU - Sweeney, Colm

AU - Wennberg, Paul O.

AU - Kim, Michelle

AU - Crounse, John D.

AU - Hall, Samuel R.

AU - Ullmann, Kirk

AU - Diskin, Glenn

AU - Bui, Paul

AU - Chang, Cecilia

AU - Dean-Day, Jonathan

PY - 2019/6/4

Y1 - 2019/6/4

N2 - The hydroxyl radical (OH) fuels tropospheric ozone production and governs the lifetime of methane and many other gases. Existing methods to quantify global OH are limited to annual and global-to-hemispheric averages. Finer resolution is essential for isolating model deficiencies and building process-level understanding. In situ observations from the Atmospheric Tomography (ATom) mission demonstrate that remote tropospheric OH is tightly coupled to the production and loss of formaldehyde (HCHO), a major hydrocarbon oxidation product. Synthesis of this relationship with satellite-based HCHO retrievals and model-derived HCHO loss frequencies yields a map of total-column OH abundance throughout the remote troposphere (up to 70% of tropospheric mass) over the first two ATom missions (August 2016 and February 2017). This dataset offers unique insights on near-global oxidizing capacity. OH exhibits significant seasonality within individual hemispheres, but the domain mean concentration is nearly identical for both seasons (1.03 ± 0.25 × 106 cm−3), and the biseasonal average North/South Hemisphere ratio is 0.89 ± 0.06, consistent with a balance of OH sources and sinks across the remote troposphere. Regional phenomena are also highlighted, such as a 10-fold OH depression in the Tropical West Pacific and enhancements in the East Pacific and South Atlantic. This method is complementary to budget-based global OH constraints and can help elucidate the spatial and temporal variability of OH production and methane loss.

AB - The hydroxyl radical (OH) fuels tropospheric ozone production and governs the lifetime of methane and many other gases. Existing methods to quantify global OH are limited to annual and global-to-hemispheric averages. Finer resolution is essential for isolating model deficiencies and building process-level understanding. In situ observations from the Atmospheric Tomography (ATom) mission demonstrate that remote tropospheric OH is tightly coupled to the production and loss of formaldehyde (HCHO), a major hydrocarbon oxidation product. Synthesis of this relationship with satellite-based HCHO retrievals and model-derived HCHO loss frequencies yields a map of total-column OH abundance throughout the remote troposphere (up to 70% of tropospheric mass) over the first two ATom missions (August 2016 and February 2017). This dataset offers unique insights on near-global oxidizing capacity. OH exhibits significant seasonality within individual hemispheres, but the domain mean concentration is nearly identical for both seasons (1.03 ± 0.25 × 106 cm−3), and the biseasonal average North/South Hemisphere ratio is 0.89 ± 0.06, consistent with a balance of OH sources and sinks across the remote troposphere. Regional phenomena are also highlighted, such as a 10-fold OH depression in the Tropical West Pacific and enhancements in the East Pacific and South Atlantic. This method is complementary to budget-based global OH constraints and can help elucidate the spatial and temporal variability of OH production and methane loss.

UR - http://www.scopus.com/inward/record.url?scp=85066999177&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85066999177&partnerID=8YFLogxK

U2 - 10.1073/pnas.1821661116

DO - 10.1073/pnas.1821661116

M3 - Article

C2 - 31110019

AN - SCOPUS:85066999177

VL - 166

SP - 11171

EP - 11180

JO - Proceedings of the National Academy of Sciences of the United States of America

JF - Proceedings of the National Academy of Sciences of the United States of America

SN - 0027-8424

IS - 23

ER -