248 research outputs found
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Evolution of mixing state of black carbon particles: Aircraft measurements over the western Pacific in March 2004
We report the evolution of the mixing state of black carbon (BC) particles in urban plumes measured by an airborne single particle soot photometer. The aircraft observations were conducted over the ocean near the coast of Japan in March 2004. The number fiaction of coated BC particles with a core diameter of 180 mn increased from 0.35 to 0.63 within 12 hours (h), namely 2.3% h-1, after being emitted from the Nagoya urban area in Japan. BC particles with a core diameter of 250 nm increased at the slower rate of 1.0% h-1. The increase in coated BC particles was associated with increases in non-sea salt sulfate and water-soluble organic carbon by a factor of approximately two, indicating that these compounds contributed to the coating on the BC particles. These results give direct evidence that BC particles become internally mixed on a time scale of 12 h in urban plumes. Copyright 2007 by the American Geophysical Union
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Asian chemical outflow to the Pacific in late spring observed during the PEACE-B aircraft mission
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Removal of NOx and NOy in Asian outflow plumes: Aircraft measurements over the western Pacific in Januray 2002
The Pacific Exploration of Asian Continental Emission Phase A (PEACE-A) aircraft measurement campaign was conducted over the western Pacific in January 2002. Correlations of carbon monoxide (CO) with carbon dioxide (CO2) and back trajectories are used to identify plumes strongly affected by Asian continental emissions. ΔCO/ΔCO2 ratios (i.e., linear regression slopes of CO-CO2) in the plumes generally fall within the variability range of the CO/CO2 emission ratios estimated from an emission inventory for east Asia, demonstrating the consistency between the aircraft measurements and the emission characterization. Removal rates of reactive nitrogen (NOx and NOy) for the study region (altitude <4 km, 124°-140°E, 25°-45°N) are estimated using the correlation with CO2, the photochemical age of the plumes, and the NOx/ CO2 emission ratio derived from the emission inventory. The plume age is estimated from the rates of hydrocarbon decay and hydroxyl radical (OH) concentration calculated using a constrained photochemical box model. The average lifetime of NOx is estimated to be 1.2 ± 0.4 days. Possible processes controlling the NOx lifetime are discussed in conjunction with results from earlier studies. The average lifetime of NOy is estimated to be 1.7 ± 0.5 days, which is comparable to the NOy lifetime of 1.7-1.8 days that has been previously reported for outflow from the United States. This similarity suggests the importance of chemical processing near the source regions in determining the NOy abundance. Copyright 2004 by the American Geophysical Union
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Emission estimates of selected volatile organic compounds from tropical savanna burning in northern Australia
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Measurements of reactive nitrogen produced by tropical thunderstorms during BIBLE-C
The Biomass Burning and Lightning Experiment phase C (BIBLE-C) aircraft mission was carried out near Darwin, Australia (12°S, 131°E) in December 2000. This was the first aircraft experiment designed to estimate lightning NO production rates in the tropics, where production is considered to be most intense. During the two flights (flights 10 and 13 made on December 9 and 11-12, respectively) enhancements of NOx (NO + NO2) up to 1000 and 1600 parts per trillion by volume (pptv, 10-s data) were observed at altitudes between 11.5 and 14 km. The Geostationary Meteorological Satellite (GMS) cloud (brightness temperature) data and ground-based lightning measurements by the Global Positioning and Tracking System (GPATS) indicate that there were intensive lightning events over the coast of the Gulf of Carpentaria, which took place upstream from our measurement area 10 to 14 h prior to the measurements. For these two flights, air in which NOx exceeded 100 pptv extended over 620 × 140 and 400 × 170 km2 (wind direction x perpendicular direction), respectively, suggesting a significant impact of lightning NO production on NOx levels in the tropics. We estimate the amount of NOx observed between 11.5 and 14 km produced by the thunderstorms to be 3.3 and 1.8 × 1025 NO molecules for flights 10 and 13, respectively. By using the GPATS lightning flash count data, column NO production rates are estimated to be 1.9-4.4 and 21-49 × 1025 NO molecules per single flash for these two flight data sets. In these estimations, it is assumed that the column NO production between 0 and 16 km is greater than the observed values between 11.5 and 14 km by a factor of 3.2, which is derived using results reported by Pickering et al. (1998). There are however large uncertainties in the GPATS lightning data in this study and care must be made when the production rates are referred. Uncertainties in these estimates are discussed. The impact on the ozone production rate is also described. Copyright 2007 by the American Geophysical Union
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Formation and transport of oxidized reactive nitrogen, ozone, and secondary organic aerosol in Tokyo
Measurements of the major reactive nitrogen species (NOy)i (NOx, peroxyacyl nitrates, HNO3, and particulate nitrate (NO3-), total reactive nitrogen (NOy), volatile organic compounds, OH and HO2, and organic aerosol were made near the urban center of Tokyo in different seasons of 2003-2004 to study the processes involving oxidized forms of reactive nitrogen and O3. Generally, NOx constituted the dominant fraction of NOy throughout the seasons. The NOx/NOy and HNO3/NOy ratios were lowest and highest, respectively, in summer, owing to the seasonally high OH concentration. The fraction of NOy that remained in the atmosphere after emission (RNOy) decreased with the decrease in the NOx/NOy ratio in summer and fall. It is likely that the median seasonal-diurnal variations Of Ox = O3 + NO2 were controlled by those of the background O3 levels, photochemical O3 formation, and vertical transport. Ox showed large increases during midday under stagnant conditions in mid-August 2004. Their in situ production rates calculated by a box model were too slow to explain the observed increases. The high Ox was likely due to the accumulation of Ox from previous days in the upper part of the boundary layer (BL) followed by transport down to near the surface by mixing after sunrise. Considering the tight correlation between Ox and secondary organic aerosol (SOA), it is likely that SOA also accumulated during the course of sea-land breeze circulation in the BL. Copyright 2008 by the American Geophysical Union
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Reactive nitrogen over the tropical western Pacific: Influence from lightning and biomass burning during BIBLE A
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Photochemistry of ozone over the western Pacific from winter to spring
Aircraft measurements of ozone (O3) and its precursors, including NO, CO, H2O, and nonmethane hydrocarbons (NMHCs), were made over the western Pacific in the 20° - 45°N latitude range in January and April-May 2002 during the Pacific Exploration of Asian Continental Emission (PEACE)-A and B campaigns. These measurements have provided data sets that, in combination with Transport and Chemical Evolution over the Pacific (TRACE-P) data taken in March 2001, enable studies of O3 photochemistry from winter to late spring. A photochemical box model is used to calculate ozone formation (F(O3)) and destruction (D(O3)) rates constrained by the observed species concentrations. The values of F(O3) and D(O3) are controlled directly by NO, J(O1D) (O3 photolysis frequency), H2O, OH, and HO2. Changes in HO2 concentration cause corresponding changes in both F(O3) and D(O3) leading to their coupling. Concentrations of these species, which are strongly influenced by photochemistry and transport from the Asian continent, underwent large seasonal variations. In the boundary layer (0-3 km), NO was much higher in January than in April-May, because of stronger winds, lower convective activities, and lower oxidation rates by OH in winter. The net O3 formation rate, given by P(O3) = F(O3) - D(O3), was largely positive in the boundary layer at 30°-45°N (1.5-4 ppbv d-1) in January, mainly because of high NO and low H2O values. Net O3 formation continued from January to the end of March, demonstrating that the western Pacific is an important O3 source region during this season. Net O3 formation nearly ceased by late April/May because of the decrease in NO and the increase in H2O. In the latitude range of 20°-30°N, P(O3) in the boundary layer was positive in January and turned negative by March. The earlier transition was mainly due to lower NO and higher H2O concentrations, combined with weaker transport and higher temperatures than those at 30°-45°N. The upper troposphere (6-12 km) has been shown to be a region of net O3 formation throughout most of the year because of high NO and low H2O. The present study illustrates that a decrease in the net O3 formation rate at 20°-45°N latitude from winter to late spring is explained systematically by the increases in J(O1D), H2O, OH, and HO2 (primarily due to increases in temperature and solar radiation) and the decrease in NO (primarily due to decrease in transport from the Asian continent). Differences in the seasonal variation of O3 photochemistry observed over the North American continent are interpreted in terms of the differences in factors controlling O3 formation and destruction. Copyright 2004 by the American Geophysical Union
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Mechanisms that influence the formation of high-ozone regions in the boundary layer downwind of the Asian continent in winter and spring
The seasonal variation of ozone (O3) in the boundary layer (BL) over the western Pacific is investigated using a chemistry-transport model. The model results for January and April-May 2002 were evaluated by comparison with PEACE aircraft observations. In January, strong northwesterlies efficiently transported NOx from the continent, leading to an O3 increase of approximately 5-10 ppbv over a distance of about 3000 km. In April, southwesterlies dominated due to anticyclone development over the western Pacific. Along this flow, O3 continued to be produced by NO x emitted from East Asia. This resulted in the formation of a high-O3 (> 50 ppbv) region extending along the coastal areas of East Asia. This seasonal change in O3 was driven in part by a change in the net O3 production rate due to increases in solar UV and H 2O. Its exact response depended on the NOx values in the BL. The net O3 production rate increased between winter and spring over the Asian continent and decreased over the remote western Pacific. Model simulations show that about 25% of the total O3 (of 10-20 ppbv) increase over the coastal region of Northeast Asia was due to local production from NOx emissions from China, and the rest was due to changes in background levels as well as emissions from Korea, Japan, and east Siberia. Uplift of BL air over Asia, horizontal transport in the free troposphere, and subsidence were the principal mechanisms of transporting Asian O3 to the central and eastern North Pacific Copyright 2008 by the American Geophysical Union
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