Detection of iodine monoxide in the tropical free troposphere

被引:72
作者
Dix, Barbara [1 ]
Baidara, Sunil [1 ,2 ]
Bresch, James F. [3 ]
Hall, Samuel R. [3 ]
Schmidt, K. Sebastian [4 ]
Wang, Siyuan [1 ,2 ]
Volkamer, Rainer [1 ,2 ]
机构
[1] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA
[2] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA
[3] Natl Ctr Atmospher Res, Earth Syst Lab, Boulder, CO 80307 USA
[4] Univ Colorado, Atmospher & Space Phys Lab, Boulder, CO 80303 USA
基金
美国国家科学基金会;
关键词
atmospheric chemistry; oxidative capacity; halogens; heterogeneous chemistry; air-sea exchange; MARINE BOUNDARY-LAYER; ATLANTIC-OCEAN; BRO COLUMNS; OZONE; IO; SATELLITE; CHEMISTRY; OXIDE; STRATOSPHERE; ENTRAINMENT;
D O I
10.1073/pnas.1212386110
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Atmospheric iodine monoxide (IO) is a radical that catalytically destroys heat trapping ozone and reacts further to form aerosols. Here, we report the detection of IO in the tropical free troposphere (FT). We present vertical profiles from airborne measurements over the Pacific Ocean that show significant IO up to 9.5 km altitude and locate, on average, two-thirds of the total column above the marine boundary layer. IO was observed in both recent deep convective outflow and aged free tropospheric air, suggesting a widespread abundance in the FT over tropical oceans. Our vertical profile measurements imply that most of the IO signal detected by satellites over tropical oceans could originate in the FT, which has implications for our understanding of iodine sources. Surprisingly, the IO concentration remains elevated in a transition layer that is decoupled from the ocean surface. This elevated concentration aloft is difficult to reconcile with our current understanding of iodine life-times and may indicate heterogeneous recycling of iodine from aerosols back to the gas phase. Chemical model simulations reveal that the iodine-induced ozone loss occurs mostly above the marine boundary layer (34%), in the transition layer (40%) and FT (26%) and accounts for up to 20% of the overall tropospheric ozone loss rate in the upper FT. Our results suggest that the halogen-driven ozone loss in the FT is currently underestimated. More research is needed to quantify the widespread impact that iodine species of marine origin have on free tropospheric composition, chemistry, and climate.
引用
收藏
页码:2035 / 2040
页数:6
相关论文
共 46 条
[1]   Iodine oxide in the marine boundary layer [J].
Alicke, B ;
Hebestreit, K ;
Stutz, J ;
Platt, U .
NATURE, 1999, 397 (6720) :572-573
[2]   Constraints on inorganic gaseous iodine in the tropical upper troposphere and stratosphere inferred from balloon-borne solar occultation observations [J].
Butz, A. ;
Boesch, H. ;
Camy-Peyret, C. ;
Chipperfield, M. P. ;
Dorf, M. ;
Kreycy, S. ;
Kritten, L. ;
Prados-Roman, C. ;
Schwaerzle, J. ;
Pfeilsticker, K. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (18) :7229-7242
[3]   Short-lived alkyl iodides and bromides at Mace Head, Ireland: Links to biogenic sources and halogen oxide production [J].
Carpenter, LJ ;
Sturges, WT ;
Penkett, SA ;
Liss, PS ;
Alicke, B ;
Hebestreit, K ;
Platt, U .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1999, 104 (D1) :1679-1689
[4]  
Change C, 2007, 4 INT PAN CLIM CHANG
[5]   The CU ground MAX-DOAS instrument: characterization of RMS noise limitations and first measurements near Pensacola, FL of BrO, IO, and CHOCHO [J].
Coburn, S. ;
Dix, B. ;
Sinreich, R. ;
Volkamer, R. .
ATMOSPHERIC MEASUREMENT TECHNIQUES, 2011, 4 (11) :2421-2439
[6]   Assessment of upper tropospheric HOx sources over the tropical Pacific based on NASA GTE/PEM data:: Net effect on HOx and other photochemical parameters [J].
Crawford, J ;
Davis, D ;
Olson, J ;
Chen, G ;
Liu, S ;
Gregory, G ;
Barrick, J ;
Sachse, G ;
Sandholm, S ;
Heikes, B ;
Singh, H ;
Blake, D .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1999, 104 (D13) :16255-16273
[7]   The ERA-Interim reanalysis: configuration and performance of the data assimilation system [J].
Dee, D. P. ;
Uppala, S. M. ;
Simmons, A. J. ;
Berrisford, P. ;
Poli, P. ;
Kobayashi, S. ;
Andrae, U. ;
Balmaseda, M. A. ;
Balsamo, G. ;
Bauer, P. ;
Bechtold, P. ;
Beljaars, A. C. M. ;
van de Berg, L. ;
Bidlot, J. ;
Bormann, N. ;
Delsol, C. ;
Dragani, R. ;
Fuentes, M. ;
Geer, A. J. ;
Haimberger, L. ;
Healy, S. B. ;
Hersbach, H. ;
Holm, E. V. ;
Isaksen, L. ;
Kallberg, P. ;
Koehler, M. ;
Matricardi, M. ;
McNally, A. P. ;
Monge-Sanz, B. M. ;
Morcrette, J. -J. ;
Park, B. -K. ;
Peubey, C. ;
de Rosnay, P. ;
Tavolato, C. ;
Thepaut, J. -N. ;
Vitart, F. .
QUARTERLY JOURNAL OF THE ROYAL METEOROLOGICAL SOCIETY, 2011, 137 (656) :553-597
[8]   The Monte Carlo atmospheric radiative transfer model McArtim: Introduction and validation of Jacobians and 3D features [J].
Deutschmann, Tim ;
Beirle, Steffen ;
Friess, Udo ;
Grzegorski, Michael ;
Kern, Christoph ;
Kritten, Lena ;
Platt, Ulrich ;
Prados-Roman, Cristina ;
Pukite, Janis ;
Wagner, Thomas ;
Werner, Bodo ;
Pfeilsticker, Klaus .
JOURNAL OF QUANTITATIVE SPECTROSCOPY & RADIATIVE TRANSFER, 2011, 112 (06) :1119-1137
[9]   EMISSION OF IODINE FROM THE SEA-SURFACE IN THE PRESENCE OF OZONE [J].
GARLAND, JA ;
CURTIS, H .
JOURNAL OF GEOPHYSICAL RESEARCH-OCEANS, 1981, 86 (NC4) :3183-3186
[10]   A theoretical study of the oxidation of Hg0 to HgBr2 in the troposphere [J].
Goodsite, ME ;
Plane, JMC ;
Skov, H .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (06) :1772-1776