Probing the subtropical lowermost stratosphere and the tropical upper troposphere and tropopause layer for inorganic bromine

Bodo Werner, Jochen Stutz, Max Spolaor, Lisa Scalone, Rasmus Raecke, James Festa, Santo Fedele Colosimo, Ross Cheung, Catalina Tsai, Ryan Hossaini, Martyn P. Chipperfield, Giorgio S. Taverna, Wuhu Feng, James W. Elkins, David W. Fahey, Ru Shan Gao, Erik J. Hintsa, Troy D. Thornberry, Free Lee Moore, Maria A. NavarroElliot L Atlas, Bruce C. Daube, Jasna Pittman, Steve Wofsy, Klaus Pfeilsticker

Research output: Contribution to journalArticle

10 Citations (Scopus)

Abstract

We report measurements of CH4 (measured in situ by the Harvard University Picarro Cavity Ringdown Spectrometer (HUPCRS) and NOAA Unmanned Aircraft System Chromatograph for Atmospheric Trace Species (UCATS) instruments), O3 (measured in situ by the NOAA dual-beam ultraviolet (UV) photometer), NO2, BrO (remotely detected by spectroscopic UV-visible (UV-vis) limb observations; see the companion paper of Stutz et al., 2016), and of some key brominated source gases in whole-air samples of the Global Hawk Whole Air Sampler (GWAS) instrument within the subtropical lowermost stratosphere (LS) and the tropical upper troposphere (UT) and tropopause layer (TTL). The measurements were performed within the framework of the NASA-ATTREX (National Aeronautics and Space Administration-Airborne Tropical Tropopause Experiment) project from aboard the Global Hawk (GH) during six deployments over the eastern Pacific in early 2013. These measurements are compared with TOMCAT/SLIMCAT (Toulouse Off-line Model of Chemistry And Transport/Single Layer Isentropic Model of Chemistry And Transport) 3-D model simulations,aiming at improvements of our understanding of the bromine budget and photochemistry in the LS, UT, and TTL. Changes in local O3 (and NO2 and BrO) due to transport processes are separated from photochemical processes in intercomparisons of measured and modeled CH4 and O3. After excellent agreement is achieved among measured and simulated CH4 and O3, measured and modeled [NO2] are found to closely agree with 15 ppt in the TTL (which is the detection limit) and within a typical range of 70 to 170 ppt in the subtropical LS during the daytime. Measured [BrO] ranges between 3 and 9 ppt in the subtropical LS. In the TTL, [BrO] reaches 0.5±0.5 ppt at the bottom (150 hPa=355K=14 km) and up to about 5 ppt at the top (70 hPa=425K=18.5 km; see Fueglistaler et al., 2009 for the definition of the TTL used), in overall good agreement with the model simulations. Depending on the photochemical regime, the TOMCAT=SLIMCAT simulations tend to slightly underpredict measured BrO for large BrO concentrations, i.e., in the upper TTL and LS. The measured BrO and modeled BrO/Bry inorg ratio is further used to calculate inorganic bromine, Brinorg y. For the TTL (i.e., when [CH4]≥1790 ppb), [Brinorg y] is found to increase from a mean of 2.63±1.04 ppt for potential temperatures (θ) in the range of 350-360K to 5.11±1.57 ppt for θ 390-400K, whereas in the subtropical LS (i.e., when [CH4]≤1790ppb), it reaches 7.66±2.95 ppt for θ in the range of 390-400 K. Finally, for the eastern Pacific (170-90°W), the TOMCAT/SLIMCAT simulations indicate a net loss of ozone of-0.3 ppbv day-1 at the base of the TTL (θ355 K) and a net production of C1.8 ppbv day-1 in the upper part (θ383 K).

Original languageEnglish (US)
Pages (from-to)1161-1186
Number of pages26
JournalAtmospheric Chemistry and Physics
Volume17
Issue number2
DOIs
StatePublished - Jan 25 2017

Fingerprint

bromine
tropopause
stratosphere
troposphere
simulation
photochemistry
photometer
air
potential temperature
transport process
sampler
limb
aircraft
cavity
spectrometer
ozone

ASJC Scopus subject areas

  • Atmospheric Science

Cite this

Probing the subtropical lowermost stratosphere and the tropical upper troposphere and tropopause layer for inorganic bromine. / Werner, Bodo; Stutz, Jochen; Spolaor, Max; Scalone, Lisa; Raecke, Rasmus; Festa, James; Fedele Colosimo, Santo; Cheung, Ross; Tsai, Catalina; Hossaini, Ryan; Chipperfield, Martyn P.; Taverna, Giorgio S.; Feng, Wuhu; Elkins, James W.; Fahey, David W.; Gao, Ru Shan; Hintsa, Erik J.; Thornberry, Troy D.; Lee Moore, Free; Navarro, Maria A.; Atlas, Elliot L; Daube, Bruce C.; Pittman, Jasna; Wofsy, Steve; Pfeilsticker, Klaus.

In: Atmospheric Chemistry and Physics, Vol. 17, No. 2, 25.01.2017, p. 1161-1186.

Research output: Contribution to journalArticle

Werner, B, Stutz, J, Spolaor, M, Scalone, L, Raecke, R, Festa, J, Fedele Colosimo, S, Cheung, R, Tsai, C, Hossaini, R, Chipperfield, MP, Taverna, GS, Feng, W, Elkins, JW, Fahey, DW, Gao, RS, Hintsa, EJ, Thornberry, TD, Lee Moore, F, Navarro, MA, Atlas, EL, Daube, BC, Pittman, J, Wofsy, S & Pfeilsticker, K 2017, 'Probing the subtropical lowermost stratosphere and the tropical upper troposphere and tropopause layer for inorganic bromine', Atmospheric Chemistry and Physics, vol. 17, no. 2, pp. 1161-1186. https://doi.org/10.5194/acp-17-1161-2017
Werner, Bodo ; Stutz, Jochen ; Spolaor, Max ; Scalone, Lisa ; Raecke, Rasmus ; Festa, James ; Fedele Colosimo, Santo ; Cheung, Ross ; Tsai, Catalina ; Hossaini, Ryan ; Chipperfield, Martyn P. ; Taverna, Giorgio S. ; Feng, Wuhu ; Elkins, James W. ; Fahey, David W. ; Gao, Ru Shan ; Hintsa, Erik J. ; Thornberry, Troy D. ; Lee Moore, Free ; Navarro, Maria A. ; Atlas, Elliot L ; Daube, Bruce C. ; Pittman, Jasna ; Wofsy, Steve ; Pfeilsticker, Klaus. / Probing the subtropical lowermost stratosphere and the tropical upper troposphere and tropopause layer for inorganic bromine. In: Atmospheric Chemistry and Physics. 2017 ; Vol. 17, No. 2. pp. 1161-1186.
@article{03330133dba64f799a860ca67b95111d,
title = "Probing the subtropical lowermost stratosphere and the tropical upper troposphere and tropopause layer for inorganic bromine",
abstract = "We report measurements of CH4 (measured in situ by the Harvard University Picarro Cavity Ringdown Spectrometer (HUPCRS) and NOAA Unmanned Aircraft System Chromatograph for Atmospheric Trace Species (UCATS) instruments), O3 (measured in situ by the NOAA dual-beam ultraviolet (UV) photometer), NO2, BrO (remotely detected by spectroscopic UV-visible (UV-vis) limb observations; see the companion paper of Stutz et al., 2016), and of some key brominated source gases in whole-air samples of the Global Hawk Whole Air Sampler (GWAS) instrument within the subtropical lowermost stratosphere (LS) and the tropical upper troposphere (UT) and tropopause layer (TTL). The measurements were performed within the framework of the NASA-ATTREX (National Aeronautics and Space Administration-Airborne Tropical Tropopause Experiment) project from aboard the Global Hawk (GH) during six deployments over the eastern Pacific in early 2013. These measurements are compared with TOMCAT/SLIMCAT (Toulouse Off-line Model of Chemistry And Transport/Single Layer Isentropic Model of Chemistry And Transport) 3-D model simulations,aiming at improvements of our understanding of the bromine budget and photochemistry in the LS, UT, and TTL. Changes in local O3 (and NO2 and BrO) due to transport processes are separated from photochemical processes in intercomparisons of measured and modeled CH4 and O3. After excellent agreement is achieved among measured and simulated CH4 and O3, measured and modeled [NO2] are found to closely agree with 15 ppt in the TTL (which is the detection limit) and within a typical range of 70 to 170 ppt in the subtropical LS during the daytime. Measured [BrO] ranges between 3 and 9 ppt in the subtropical LS. In the TTL, [BrO] reaches 0.5±0.5 ppt at the bottom (150 hPa=355K=14 km) and up to about 5 ppt at the top (70 hPa=425K=18.5 km; see Fueglistaler et al., 2009 for the definition of the TTL used), in overall good agreement with the model simulations. Depending on the photochemical regime, the TOMCAT=SLIMCAT simulations tend to slightly underpredict measured BrO for large BrO concentrations, i.e., in the upper TTL and LS. The measured BrO and modeled BrO/Bry inorg ratio is further used to calculate inorganic bromine, Brinorg y. For the TTL (i.e., when [CH4]≥1790 ppb), [Brinorg y] is found to increase from a mean of 2.63±1.04 ppt for potential temperatures (θ) in the range of 350-360K to 5.11±1.57 ppt for θ 390-400K, whereas in the subtropical LS (i.e., when [CH4]≤1790ppb), it reaches 7.66±2.95 ppt for θ in the range of 390-400 K. Finally, for the eastern Pacific (170-90°W), the TOMCAT/SLIMCAT simulations indicate a net loss of ozone of-0.3 ppbv day-1 at the base of the TTL (θ355 K) and a net production of C1.8 ppbv day-1 in the upper part (θ383 K).",
author = "Bodo Werner and Jochen Stutz and Max Spolaor and Lisa Scalone and Rasmus Raecke and James Festa and {Fedele Colosimo}, Santo and Ross Cheung and Catalina Tsai and Ryan Hossaini and Chipperfield, {Martyn P.} and Taverna, {Giorgio S.} and Wuhu Feng and Elkins, {James W.} and Fahey, {David W.} and Gao, {Ru Shan} and Hintsa, {Erik J.} and Thornberry, {Troy D.} and {Lee Moore}, Free and Navarro, {Maria A.} and Atlas, {Elliot L} and Daube, {Bruce C.} and Jasna Pittman and Steve Wofsy and Klaus Pfeilsticker",
year = "2017",
month = "1",
day = "25",
doi = "10.5194/acp-17-1161-2017",
language = "English (US)",
volume = "17",
pages = "1161--1186",
journal = "Atmospheric Chemistry and Physics",
issn = "1680-7316",
publisher = "European Geosciences Union",
number = "2",

}

TY - JOUR

T1 - Probing the subtropical lowermost stratosphere and the tropical upper troposphere and tropopause layer for inorganic bromine

AU - Werner, Bodo

AU - Stutz, Jochen

AU - Spolaor, Max

AU - Scalone, Lisa

AU - Raecke, Rasmus

AU - Festa, James

AU - Fedele Colosimo, Santo

AU - Cheung, Ross

AU - Tsai, Catalina

AU - Hossaini, Ryan

AU - Chipperfield, Martyn P.

AU - Taverna, Giorgio S.

AU - Feng, Wuhu

AU - Elkins, James W.

AU - Fahey, David W.

AU - Gao, Ru Shan

AU - Hintsa, Erik J.

AU - Thornberry, Troy D.

AU - Lee Moore, Free

AU - Navarro, Maria A.

AU - Atlas, Elliot L

AU - Daube, Bruce C.

AU - Pittman, Jasna

AU - Wofsy, Steve

AU - Pfeilsticker, Klaus

PY - 2017/1/25

Y1 - 2017/1/25

N2 - We report measurements of CH4 (measured in situ by the Harvard University Picarro Cavity Ringdown Spectrometer (HUPCRS) and NOAA Unmanned Aircraft System Chromatograph for Atmospheric Trace Species (UCATS) instruments), O3 (measured in situ by the NOAA dual-beam ultraviolet (UV) photometer), NO2, BrO (remotely detected by spectroscopic UV-visible (UV-vis) limb observations; see the companion paper of Stutz et al., 2016), and of some key brominated source gases in whole-air samples of the Global Hawk Whole Air Sampler (GWAS) instrument within the subtropical lowermost stratosphere (LS) and the tropical upper troposphere (UT) and tropopause layer (TTL). The measurements were performed within the framework of the NASA-ATTREX (National Aeronautics and Space Administration-Airborne Tropical Tropopause Experiment) project from aboard the Global Hawk (GH) during six deployments over the eastern Pacific in early 2013. These measurements are compared with TOMCAT/SLIMCAT (Toulouse Off-line Model of Chemistry And Transport/Single Layer Isentropic Model of Chemistry And Transport) 3-D model simulations,aiming at improvements of our understanding of the bromine budget and photochemistry in the LS, UT, and TTL. Changes in local O3 (and NO2 and BrO) due to transport processes are separated from photochemical processes in intercomparisons of measured and modeled CH4 and O3. After excellent agreement is achieved among measured and simulated CH4 and O3, measured and modeled [NO2] are found to closely agree with 15 ppt in the TTL (which is the detection limit) and within a typical range of 70 to 170 ppt in the subtropical LS during the daytime. Measured [BrO] ranges between 3 and 9 ppt in the subtropical LS. In the TTL, [BrO] reaches 0.5±0.5 ppt at the bottom (150 hPa=355K=14 km) and up to about 5 ppt at the top (70 hPa=425K=18.5 km; see Fueglistaler et al., 2009 for the definition of the TTL used), in overall good agreement with the model simulations. Depending on the photochemical regime, the TOMCAT=SLIMCAT simulations tend to slightly underpredict measured BrO for large BrO concentrations, i.e., in the upper TTL and LS. The measured BrO and modeled BrO/Bry inorg ratio is further used to calculate inorganic bromine, Brinorg y. For the TTL (i.e., when [CH4]≥1790 ppb), [Brinorg y] is found to increase from a mean of 2.63±1.04 ppt for potential temperatures (θ) in the range of 350-360K to 5.11±1.57 ppt for θ 390-400K, whereas in the subtropical LS (i.e., when [CH4]≤1790ppb), it reaches 7.66±2.95 ppt for θ in the range of 390-400 K. Finally, for the eastern Pacific (170-90°W), the TOMCAT/SLIMCAT simulations indicate a net loss of ozone of-0.3 ppbv day-1 at the base of the TTL (θ355 K) and a net production of C1.8 ppbv day-1 in the upper part (θ383 K).

AB - We report measurements of CH4 (measured in situ by the Harvard University Picarro Cavity Ringdown Spectrometer (HUPCRS) and NOAA Unmanned Aircraft System Chromatograph for Atmospheric Trace Species (UCATS) instruments), O3 (measured in situ by the NOAA dual-beam ultraviolet (UV) photometer), NO2, BrO (remotely detected by spectroscopic UV-visible (UV-vis) limb observations; see the companion paper of Stutz et al., 2016), and of some key brominated source gases in whole-air samples of the Global Hawk Whole Air Sampler (GWAS) instrument within the subtropical lowermost stratosphere (LS) and the tropical upper troposphere (UT) and tropopause layer (TTL). The measurements were performed within the framework of the NASA-ATTREX (National Aeronautics and Space Administration-Airborne Tropical Tropopause Experiment) project from aboard the Global Hawk (GH) during six deployments over the eastern Pacific in early 2013. These measurements are compared with TOMCAT/SLIMCAT (Toulouse Off-line Model of Chemistry And Transport/Single Layer Isentropic Model of Chemistry And Transport) 3-D model simulations,aiming at improvements of our understanding of the bromine budget and photochemistry in the LS, UT, and TTL. Changes in local O3 (and NO2 and BrO) due to transport processes are separated from photochemical processes in intercomparisons of measured and modeled CH4 and O3. After excellent agreement is achieved among measured and simulated CH4 and O3, measured and modeled [NO2] are found to closely agree with 15 ppt in the TTL (which is the detection limit) and within a typical range of 70 to 170 ppt in the subtropical LS during the daytime. Measured [BrO] ranges between 3 and 9 ppt in the subtropical LS. In the TTL, [BrO] reaches 0.5±0.5 ppt at the bottom (150 hPa=355K=14 km) and up to about 5 ppt at the top (70 hPa=425K=18.5 km; see Fueglistaler et al., 2009 for the definition of the TTL used), in overall good agreement with the model simulations. Depending on the photochemical regime, the TOMCAT=SLIMCAT simulations tend to slightly underpredict measured BrO for large BrO concentrations, i.e., in the upper TTL and LS. The measured BrO and modeled BrO/Bry inorg ratio is further used to calculate inorganic bromine, Brinorg y. For the TTL (i.e., when [CH4]≥1790 ppb), [Brinorg y] is found to increase from a mean of 2.63±1.04 ppt for potential temperatures (θ) in the range of 350-360K to 5.11±1.57 ppt for θ 390-400K, whereas in the subtropical LS (i.e., when [CH4]≤1790ppb), it reaches 7.66±2.95 ppt for θ in the range of 390-400 K. Finally, for the eastern Pacific (170-90°W), the TOMCAT/SLIMCAT simulations indicate a net loss of ozone of-0.3 ppbv day-1 at the base of the TTL (θ355 K) and a net production of C1.8 ppbv day-1 in the upper part (θ383 K).

UR - http://www.scopus.com/inward/record.url?scp=85010285088&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85010285088&partnerID=8YFLogxK

U2 - 10.5194/acp-17-1161-2017

DO - 10.5194/acp-17-1161-2017

M3 - Article

AN - SCOPUS:85010285088

VL - 17

SP - 1161

EP - 1186

JO - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

SN - 1680-7316

IS - 2

ER -