Reactive nitrogen distribution and partitioning in the North American troposphere and lowermost stratosphere

被引:68
作者
Singh, H. B. [1 ]
Salas, L.
Herlth, D.
Kolyer, R.
Czech, E.
Avery, M.
Crawford, J. H.
Pierce, R. B.
Sachse, G. W.
Blake, D. R.
Cohen, R. C.
Bertram, T. H.
Perring, A.
Wooldridge, P. J.
Dibb, J.
Huey, G.
Hudman, R. C.
Turquety, S.
Emmons, L. K.
Flocke, F.
Tang, Y.
Carmichael, G. R.
Horowitz, L. W.
机构
[1] NASA, Ames Res Ctr, Moffett Field, CA 94035 USA
[2] NASA, Langley Res Ctr, Hampton, VA 23665 USA
[3] Univ Calif Irvine, Dept Chem, Irvine, CA 92717 USA
[4] Univ Calif Berkeley, Dept Chem, Berkeley, CA 92717 USA
[5] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 92717 USA
[6] Univ New Hampshire, Inst Study Earth Oceans & Space, Durham, NH 03824 USA
[7] Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA
[8] Harvard Univ, Dept Earth & Planetary Sci, Cambridge, MA 02138 USA
[9] Natl Ctr Atmospher Res, Boulder, CO 80301 USA
[10] Univ Iowa, Dept Chem & Biochem Engn, Iowa City, IA 52242 USA
[11] NOAA, Geophys Fluid Dynam Lab, Princeton, NJ 08542 USA
关键词
D O I
10.1029/2006JD007664
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
[1] A comprehensive group of reactive nitrogen species (NO, NO2, HNO3, HO2NO2, PANs, alkyl nitrates, and aerosol-NO3-) were measured over North America during July/August 2004 from the NASA DC-8 platform (0.1-12 km). Nitrogen containing tracers of biomass combustion (HCN and CH3CN) were also measured along with a host of other gaseous (CO, VOC, OVOC, halocarbon) and aerosol tracers. Clean background air as well as air with influences from biogenic emissions, anthropogenic pollution, biomass combustion, convection, lightning, and the stratosphere was sampled over the continental United States, the Atlantic, and the Pacific. The North American upper troposphere (UT) was found to be greatly influenced by both lightning NOx and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NOx. Observational data suggest that lightning was a far greater contributor to NOx in the UT than previously believed. PAN provided a dominant reservoir of reactive nitrogen in the UT while nitric acid dominated in the lower troposphere (LT). Peroxynitric acid (HO2NO2) was present in sizable concentrations peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the LT. Plumes from Alaskan fires contained large amounts of PAN and aerosol nitrate but little enhancement in ozone. A comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. We investigate the partitioning and interplay of the reactive nitrogen species within characteristic air masses and further examine their role in ozone formation.
引用
收藏
页数:15
相关论文
共 50 条
[1]   Direct measurements of the convective recycling of the upper troposphere [J].
Bertram, Timothy H. ;
Perring, Anne E. ;
Wooldridge, Paul J. ;
Crounse, John D. ;
Kwan, Alan J. ;
Wennberg, Paul O. ;
Scheuer, Eric ;
Dibb, Jack ;
Avery, Melody ;
Sachse, Glen ;
Vay, Stephanie A. ;
Crawford, James H. ;
McNaughton, Cameron S. ;
Clarke, Antony ;
Pickering, Kenneth E. ;
Fuelberg, Henry ;
Huey, Greg ;
Blake, Donald R. ;
Singh, Hanwant B. ;
Hall, Samuel R. ;
Shetter, Richard E. ;
Fried, Alan ;
Heikes, Brian G. ;
Cohen, Ronald C. .
SCIENCE, 2007, 315 (5813) :816-820
[2]   Global modeling of tropospheric chemistry with assimilated meteorology: Model description and evaluation [J].
Bey, I ;
Jacob, DJ ;
Yantosca, RM ;
Logan, JA ;
Field, BD ;
Fiore, AM ;
Li, QB ;
Liu, HGY ;
Mickley, LJ ;
Schultz, MG .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2001, 106 (D19) :23073-23095
[3]   European scientific assessment of the atmospheric effects of aircraft emissions [J].
Brasseur, GP ;
Cox, RA ;
Hauglustaine, D ;
Isaksen, I ;
Lelieveld, J ;
Lister, DH ;
Sausen, R ;
Schumann, U ;
Wahner, A ;
Wiesen, P .
ATMOSPHERIC ENVIRONMENT, 1998, 32 (13) :2329-2418
[4]   Variability in nocturnal nitrogen oxide processing and its role in regional air quality [J].
Brown, SS ;
Ryerson, TB ;
Wollny, AG ;
Brock, CA ;
Peltier, R ;
Sullivan, AP ;
Weber, RJ ;
Dubé, WP ;
Trainer, M ;
Meagher, JF ;
Fehsenfeld, FC ;
Ravishankara, AR .
SCIENCE, 2006, 311 (5757) :67-70
[5]  
Brunner D., 2001, J GEOPHYS RES-ATMOS, V106, P27673
[6]  
CLEARY PA, 2005, ATMOS CHEM PHYS DISC, V5, P4801, DOI DOI 10.5194/ACPD-5-4801-2005
[7]   Photochemistry of NO2 in earth's stratosphere:: Constraints from observations [J].
Cohen, RC ;
Murphy, JG .
CHEMICAL REVIEWS, 2003, 103 (12) :4985-4998
[8]   Large upper tropospheric ozone enhancements above midlatitude North America during summer:: In situ evidence from the IONS and MOZAIC ozone measurement network [J].
Cooper, O. R. ;
Stohl, A. ;
Trainer, M. ;
Thompson, A. M. ;
Witte, J. C. ;
Oltmans, S. J. ;
Morris, G. ;
Pickering, K. E. ;
Crawford, J. H. ;
Chen, G. ;
Cohen, R. C. ;
Bertram, T. H. ;
Wooldridge, P. ;
Perring, A. ;
Brune, W. H. ;
Merrill, J. ;
Moody, J. L. ;
Tarasick, D. ;
Nedelec, P. ;
Forbes, G. ;
Newchurch, M. J. ;
Schmidlin, F. J. ;
Johnson, B. J. ;
Turquety, S. ;
Baughcum, S. L. ;
Ren, X. ;
Fehsenfeld, F. C. ;
Meagher, J. F. ;
Spichtinger, N. ;
Brown, C. C. ;
McKeen, S. A. ;
McDermid, I. S. ;
Leblanc, T. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2006, 111 (D24)
[9]   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