SUMMERTIME PARTITIONING AND BUDGET OF NOY COMPOUNDS IN THE TROPOSPHERE OVER ALASKA AND CANADA - ABLE 3B

被引:61
作者
SANDHOLM, S
OLSON, J
BRADSHAW, J
TALBOT, R
SINGH, H
GREGORY, G
BLAKE, D
ANDERSON, B
SACHSE, G
BARRICK, J
COLLINS, J
KLEMM, K
LEFER, B
KLEMM, O
GORZELSKA, K
HERLTH, D
OHARA, D
机构
[1] NASA, LANGLEY RES CTR, HAMPTON, VA 23665 USA
[2] UNIV CALIF IRVINE, DEPT CHEM, IRVINE, CA 92717 USA
[3] UNIV NEW HAMPSHIRE, INST STUDY EARTH OCEANS & SPACE, DURHAM, NH 03824 USA
[4] NASA, AMES RES CTR, MOFFETT FIELD, CA 94035 USA
关键词
D O I
10.1029/93JD02458
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
As part of NASA's Arctic Boundary Layer Expedition 3A and 3B field measurement programs, measurements of NOx, HNO3, PAN, PPN, and NOy were made in the middle to lower troposphere over Alaska and Canada during the summers of 1988 and 1990. These measurements are used to assess the degree of closure within the reactive odd nitrogen (N-x O-y) budget through the comparison of the values of NOy measured with a catalytic convertor to the sum of individually measured NOy(i) compounds (i.e., Sigma NOy(i) = NOx + HNO3 + PAN + PPN). Significant differences were observed between the various study regions. In the lower 6 km of the troposphere over Alaska and the Hudson Bay lowlands of Canada a significant fraction of the NOy budget (30 to 60%) could not be accounted for by the measured Sigma NOy(i). This deficit in the NOy budget is about 100 to 200 parts per trillion by volume (pptv) in the lower troposphere (0.15 to 3 km) and about 200 to 400 pptv in the middle free troposphere (3 to 6.2 km). Conversely, the NOy budget in the northern Labrador and Quebec regions of Canada is almost totally accounted for within the combined measurement uncertainties of NOy and the various NOy(i) compounds. A substantial portion of the NOy budget's ''missing compounds'' appears to be coupled to the photochemical and/or dynamical parameters Influencing the tropospheric oxidative potential over these regions. A combination of factors are suggested as the causes for the variability observed in the NO budget. In addition, the apparent stability of compounds represented by the NOy budget deficit in the lower-altitude range questions the ability of these compounds to participate as reversible reservoirs for ''active'' odd nitrogen and suggest that some portion of the NOy budget may consist of relatively unreactive nitrogen-containing compounds.
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页码:1837 / 1861
页数:25
相关论文
共 56 条
[1]   SUMMERTIME TROPOSPHERIC OZONE DISTRIBUTIONS OVER CENTRAL AND EASTERN CANADA [J].
ANDERSON, BE ;
GREGORY, GL ;
BARRICK, JDW ;
COLLINS, JE ;
SACHSE, GW ;
SHIPHAM, MC ;
HUDGINS, CH .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1994, 99 (D1) :1781-1792
[2]   PARTITIONING AND BUDGET OF NOY SPECIES DURING THE MAUNA-LOA-OBSERVATORY PHOTOCHEMISTRY EXPERIMENT [J].
ATLAS, EL ;
RIDLEY, BA ;
HUBLER, G ;
WALEGA, JG ;
CARROLL, MA ;
MONTZKA, DD ;
HUEBERT, BJ ;
NORTON, RB ;
GRAHEK, FE ;
SCHAUFFLER, S .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1992, 97 (D10) :10449-10462
[3]   MEASUREMENTS OF NOX AND NOY CONCENTRATIONS AND FLUXES OVER ARCTIC TUNDRA [J].
BAKWIN, PS ;
WOFSY, SC ;
FAN, SM ;
FITZJARRALD, DR .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1992, 97 (D15) :16545-16557
[4]   SUMMERTIME MEASUREMENTS OF SELECTED NONMETHANE HYDROCARBONS IN THE ARCTIC AND SUB-ARCTIC DURING THE 1988 ARCTIC BOUNDARY-LAYER EXPEDITION (ABLE-3A) [J].
BLAKE, DR ;
HURST, DF ;
SMITH, TW ;
WHIPPLE, WJ ;
CHEN, TY ;
BLAKE, NJ ;
ROWLAND, FS .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1992, 97 (D15) :16559-16588
[5]   EFFECTS OF BIOMASS BURNING ON SUMMERTIME NONMETHANE HYDROCARBON CONCENTRATIONS IN THE CANADIAN WETLANDS [J].
BLAKE, DR ;
SMITH, TW ;
CHEN, TY ;
WHIPPLE, WJ ;
ROWLAND, FS .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1994, 99 (D1) :1699-1719
[6]   CONVERSION OF NITROGEN-DIOXIDE, NITRIC-ACID, AND NORMAL-PROPYL NITRATE TO NITRIC-OXIDE BY GOLD-CATALYZED REDUCTION WITH CARBON-MONOXIDE [J].
BOLLINGER, MJ ;
SIEVERS, RE ;
FAHEY, DW ;
FEHSENFELD, FC .
ANALYTICAL CHEMISTRY, 1983, 55 (12) :1980-1986
[7]   A 2-PHOTON LASER-INDUCED FLUORESCENCE FIELD INSTRUMENT FOR GROUND-BASED AND AIRBORNE MEASUREMENTS OF ATMOSPHERIC NO [J].
BRADSHAW, JD ;
RODGERS, MO ;
SANDHOLM, ST ;
KESHENG, S ;
DAVIS, DD .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1985, 90 (D7) :2861-2873
[8]   OZONE AND AEROSOL DISTRIBUTIONS IN THE SUMMERTIME TROPOSPHERE OVER CANADA [J].
BROWELL, EV ;
FENN, MA ;
BUTLER, CF ;
GRANT, WB ;
HARRISS, RC ;
SHIPHAM, MC .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1994, 99 (D1) :1739-1755
[9]   CONTRIBUTION OF ORGANIC NITRATES TO THE TOTAL REACTIVE NITROGEN BUDGET AT A RURAL EASTERN UNITED-STATES SITE [J].
BUHR, MP ;
PARRISH, DD ;
NORTON, RB ;
FEHSENFELD, FC ;
SIEVERS, RE ;
ROBERTS, JM .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1990, 95 (D7) :9809-9816
[10]   AIRCRAFT MEASUREMENTS OF NOX OVER THE EASTERN PACIFIC AND CONTINENTAL UNITED-STATES AND IMPLICATIONS FOR OZONE PRODUCTION [J].
CARROLL, MA ;
HASTIE, DR ;
RIDLEY, BA ;
RODGERS, MO ;
TORRES, AL ;
DAVIS, DD ;
BRADSHAW, JD ;
SANDHOLM, ST ;
SCHIFF, HI ;
KARECKI, DR ;
HARRIS, GW ;
MACKAY, GI ;
GREGORY, GL ;
CONDON, EP ;
TRAINER, M ;
HUBLER, G ;
MONTZKA, DD ;
MADRONICH, S ;
ALBRITTON, DL ;
SINGH, HB ;
BECK, SM ;
SHIPMAN, MC ;
BACHMEIER, AS .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1990, 95 (D7) :10205-10233