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Under present environmental conditions, hybrid larch F1 (Larix gmelinii var. japonica × Larix kaempferi) is a promising afforestation species as it has a high growth rate and tolerance against grazing damage, disease and cold. However, the input of nitrogen (N) to forests due to the increase of anthropogenic N is causing imbalances of N compared to other nutrients, especially phosphorus (P), thus affecting the root growth of healthy seedlings. However, knowledge on how different N and P conditions affect F1 root growth is still limited. In this study, various N (3 levels) and P (no addition and addition) conditions were imposed to investigate the effect of N loading on larch F1 seedlings under different P conditions. Needle N: P ratio, aboveground growth, belowground growth as well as fine root production were measured. The results showed that needle N: P ratio was higher under low P loading, and aboveground growth of seedlings increased with N loading at both low and high P conditions. Relative fine root production was decreased by N loading. On the other hand, fine root to total dry proportion was increased by N loading at no P addition, suggesting that limited P availability could increase fine root production. Total root proportion to total dry mass was decreased by N loading at both P conditions. We concluded that N loading has different effects on above- and below-ground growth of larch F1 and its effects may also differ according to P conditions, indicating that both N and P conditions should be carefully considered when planting hybrid larch F1.

Masashi Sekine,1,2 Kahori Kita,1 Wenwei Yu1 1Center for Frontier Medical Engineering, 2Graduate School of Engineering, Chiba University, Chiba, Japan Abstract: Unlike forearm amputees, transhumeral amputees have residual stumps that are too small to provide a sufficient range of operation for their prosthetic parts to perform usual activities of daily living. Furthermore, it is difficult for small residual stumps to provide sufficient impact absorption for safe manipulation in daily living, as intact arms do. Therefore, substitution of upper limb function in transhumeral amputees requires a sufficient range of motion and sufficient viscoelasticity for shoulder prostheses under critical weight and dimension constraints. We propose the use of two different types of actuators, ie, pneumatic elastic actuators (PEAs) and servo motors. PEAs offer high power-to-weight performance and have intrinsic viscoelasticity in comparison with motors or standard industrial pneumatic cylinder actuators. However, the usefulness of PEAs in large working spaces is limited because of their short strokes. Servo motors, in contrast, can be used to achieve large ranges of motion. In this study, the relationship between the force and stroke of PEAs was investigated. The impact absorption of both types of actuators was measured using a single degree-of-freedom prototype to evaluate actuator compliance for safety purposes. Based on the fundamental properties of the actuators identified, a four degree-of-freedom robotic arm is proposed for prosthetic use. The configuration of the actuators and functional parts was designed to achieve a specified range of motion and torque calculated from the results of a simulation of typical movements performed in usual activities of daily living. Our experimental results showed that the requirements for the shoulder prostheses could be satisfied. Keywords: shoulder prosthesis, hybrid actuation, pneumatic elastic actuator, antagonistic mechanism, compliance

Regional aerosol model calculations were made using the Weather Research and Forecasting (WRF)-Community Multiscale Air Quality (CMAQ) and WRF-chem models to study spatial and temporal variations of aerosols around Beijing, China, in the summer of 2006, when the Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing) intensive campaign was conducted. Model calculations captured temporal variations of primary (such as elemental carbon. (EC)) and secondary (such as sulfate) aerosols observed in and around Beijing. The spatial distributions of aerosol optical depth observed by the MODTS satellite sensors were also reproduced over northeast China. Model calculations showed distinct differences in spatial distributions between primary and secondary aerosols in association with synoptic-scale meteorology. Secondary aerosols increased in air around Beijing on a scale of about 1000 × 1000 km2 under an anticyclonic pressure system. This air mass was transported northward from the high anthropogenic emission area extending south of Beijing with continuous photochemical production. Subsequent cold front passage brought clean air from the north, and polluted air around Beijing was swept to the south of Beijing. This cycle was repeated about once a week and was found to be responsible for observed enhancements/reductions of aerosols at the intensive measurement sites. In contrast to secondary aerosols, the spatial distributions of primary aerosols (EC) reflected those of emissions, resulting in only slight variability despite the changes in synopticscale meteorology. In accordance with these results, source apportionment simulations revealed that primary aerosols around Beijing were controlled by emissions within 100 km around Beijing within the preceding 24 h, while emissions as far as 500 km and within the preceding 3 days were found to affect secondary aerosols. Copyright 2009 by the American Geophysical Union.

Online measurements of water-soluble organic carbon (WSOC) aerosols were made using a particle-into-liquid sampler (PILS) combined with a total organic carbon (TOC) analyzer at a rural site in the Pearl River Delta region, China, in July 2006. A macroporous nonionic (DAX-8) resin was used to quantify hydrophilic and hydrophobic WSOC, which are defined as the fractions of WSOC that penetrated through and retained on the DAX-8 column, respectively. Laboratory calibrations showed that hydrophilic WSOC (WSOCHPI) included low-molecular aliphatic dicarboxylic acids and carbonyls, saccharides, and amines, while hydrophobic WSOC (WSOCHPO) included longer-chain aliphatic dicarboxylic acids and carbonyls, aromatic acids, phenols, organic nitrates, cyclic acids, and fulvic acids. On average, total WSOC (TWSOC) accounted for 60% of OC, and WSOCHPO accounted for 60% of TWSOC. Both WSOC HIP and WSOCHPO increased with photochemical aging determined from the NOx/NOy ratio. In particular, the average WSOCHPO mass was found to increase by a factor of five within a timescale of ∼10 hours, which was substantially larger than that of WSOCHPI (by a factor of 2-3). The total increase in OC mass with photochemical aging was associated with the large increase in WSOCHPO mass. These results, combined with the laboratory calibrations, suggest that significant amounts of hydrophobic organic compounds (likely containing large carbon numbers) were produced by photochemical processing. By contrast, water-insoluble OC (WIOC) mass did not exhibit significant changes with photochemical aging, suggesting that chemical transformation of WIOC to WSOC was not a dominant process for the production of WSOC during the study period. Copyright 2009 by the American Geophysical Union.

Ground-based measurements of aerosol and trace gases were conducted at a rural site in Beijing in the summer of 2006 as a part of the Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing 2006). The size-resolved chemical composition of submicron aerosol was measured using an Aerodyne quadrupole aerosol mass spectrometer (AMS). The data obtained from 15 August to 10 September 2006 are presented. Meteorological analysis shows that the measurement period can be characterized as a cycle of low wind speed periods over the course of a few days (stagnant periods) followed by rapid advection of clean air from the north/northwest mostly due to passage of a midlatitude cyclone. Mass concentrations of total measured aerosol with diameters less than 1 μm. (total. PM1), which is defined as the sum of elemental carbon and nonrefractory components measured by the AMS, were highly variable, ranging from. ∼2 to ∼100 μm-3, Large variability of the PM1 composition and drastic changes in the sulfate (SO 2-4) size distribution were observed to be associated with the cycle of stagnant periods and advection of clean air, indicating that both chemical and physical properties of aerosols were significantly altered on a time scale of a few days. We have found the dominance of organic aerosol at lower total PM1 mass loadings and that of SO2-4 at higher mass loadings, which may have important implications for the PM control strategy in Beijing. Possible factors affecting the evolution of the mass concentration and size distribution of SO2-4 are discussed. Copyright 2009 by the American Geophysical Union.

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.

Eighteen C2-C7 NMHCs (nonmethane hydrocarbons) were measured hourly during the Integrated Measurement Program for Aerosol and Oxidant Chemistry in Tokyo (IMPACT) measurement campaigns conducted in central Tokyo during four different periods (summer/autumn of 2003 and winter/summer of 2004). The ambient atmospheric concentrations of NMHCs showed an inverse correlation with wind speed and mixing height and were significantly affected by mesoscale weather conditions. The mixing ratio of isoprene tightly correlated with solar flux and temperature in summer, as it was dominantly emitted by the local vegetation. All the observed NMHCs except isoprene showed high correlation with each other in winter (r2 > 0.5), suggesting concurrent accumulation under stagnant condition and common sources. Emission ratios were calculated on the basis of the correlation with carbon monoxide and ethyne. Compared to the typical winter NMEC composition, during summer there was a significant increase (up to 7 times higher than wintertime) of C4-C5 alkanes from ftiel evaporation; of C2-C3 alkenes, n-hexane and benzene from chemical industry; and of toluene from local manufacturers, reflecting the temperature dependence of these evaporative emissions. In addition to the online measurements in Tokyo, canister sampling at a suburban site (Kisai) followed by multidimensional GC analyses was conducted during the summer campaign in 2004. The atmospheric concentrations of longer-lived compounds (≥ several days) at Kisai showed the buildup under sea breeze circulation. The average ambient, concentration of toluene was 2 times higher than that in central Tokyo, likely because of substantial emissions from local industries as reported in the prefectural statistics. Copyright 2007 by the American Geophysical Union.

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.

Simultaneous measurements of speciated, total reactive nitrogen (NOy) and particulate NO3 (particle diameter

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.

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

The Pacific Exploration of Asian Continental Emission phase B (PEACE-B) aircraft mission was conducted over the western Pacific during April-May 2002. During several flights large enhancements of CO greater than 200 parts per billion by volume (ppbv) were served at altitudes between 5 and 10 km. In this paper, we describe vertical transport mechanisms over east Asia that were responsible for these enhancements, using the European Centre for Medium-Range Weather Forecasts (ECMWF) meteorological data and infrared cloud data obtained by the Geostationary Meteorological Satellite (GMS)-5. A case study for the highest CO event shows that it was likely due to vertical transport of pollutants caused by deep cumulus convection along a quasi-stationary frontal zone, which was formed over central China (around the Yangtze River at 30°N). In the mean meteorological field during the PEACE-B period, the warm, moist low-level southerlies converged into the frontal zone, sustaining cross-frontal temperature and moisture contrasts. Along the frontal zone, the mean vertical motion was distinctively upward, and a subtropical jet aloft was found to transport uplifted air parcels efficiently into the western Pacific. In this study, criteria to identify deep convection are defined using both the ECMWF and GMS data. The results show that convective activity, which was generally high below the subtropical jet, played an important role in producing updrafts over central China. The convective transport resulted mainly from a limited number of episodes, each of which followed the development of a weak cyclonic disturbance. Back trajectories of air parcels sampled at altitudes between 4 and 13 km on board the aircraft during PEACE-B show that among the air parcels originating from the 800-hPa level or below, 69% were likely to have undergone convective uplifting. In addition to convection, sloping isentropes often observed along the quasi-stationary jet axis yielded persistent slow quasi-adiabatic uplifting of air over the Far East, which was occasionally intensified with a classical warm conveyor belt (WCB) airstream on the passage of migratory cyclonic disturbances. Meteorological conditions during PEACE-B were thus favorable for the upliffing of boundary layer air influenced by anthropogenic emissions over central China. These results are consistent with the relatively high levels of Halon 1211 (CF2ClBr), a good tracer of Chinese anthropogenic emissions, observed in the air parcels that were likely uplifted in the frontal zone. Coyright 2004 by the American Geophysical Union.

Aircraft measurements of ozone (O3) and its precursors (reactive nitrogen, CO, nonmethane hydrocarbons) were made over the western Pacific during the Transport and Chemical Evolution Over the Pacific (TRACE-P) campaign, which was conducted during February-April 2001. Biomass burning activity was high over Southeast Asia (SEA) during this period (dry season), and convective activity over SEA frequently transported air from the boundary layer to the free troposphere, followed by eastward transport to the sampling region over the western Pacific south of 30°N. This data set allows for systematic investigations of the chemical and physical processes in the outflow from SEA. Methyl chloride (CH3Cl) and CO are chosen as primary and secondary tracers, respectively, to gauge the degree of the impact of emissions of trace species from biomass burning. Biomass burning is found to be a major source of reactive nitrogen (NO x, PAN, HNO3, and nitrate) and O3 in this region from correlations of these species with the tracers. Changes in the abundance of reactive nitrogen during upward transport are quantified from the altitude change of the slopes of the correlations of these species with CO. NOx decreased with altitude due to its oxidation to HNO3. On the other hand, PAN was conserved during transport from the lower to the middle troposphere, consistent with its low water solubility and chemical stability at low temperatures. Large losses of HNO3 and nitrate, which are highly water soluble, occurred in the free troposphere, most likely due to wet removal by precipitation. This has been shown to be the major pathway of NOy loss in the middle troposphere. Increases in the mixing ratios of O3 and its precursors due to biomass burning in SEA are estimated using the tracers. Enhancements of CO and total reactive nitrogen (NOy), which are directly emitted from biomass burning, were largest at 2-4 km. At this altitude the increases in NOy and O3 were 810 parts per trillion by volume (pptv) and 26 parts per billion by volume (ppbv) above their background values of 240 pptv and 31 ppbv, respectively. The slope of the O3-CO correlation in biomass burning plumes was similar to those observed in fire plumes in northern Australia, Africa, and Canada. The O3 production efficiency (OPE) derived from the O3-CO slope and NOx/CO emission ratio (ER) is shown to be positively correlated with the C2H4 /NOx ER, indicating that the C2H4/NO x ER is a critical parameter in determining the OPE. Comparison of the net O3 flux across the western Pacific region and total O3 production due to biomass burning in SEA suggests that about 70% of O3 produced was transported to the western Pacific. Copyright 2004 by the American Geophysical Union.

An extensive set of carbonyl sulfide (OCS) and carbon disulfide (CS 2) observations were made as part of the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) project, which took place in the early spring 2001. TRACE-P sampling focused on the western Pacific region but in total included the geographic region 110°E to 290°E longitude, 5°N to 50°N latitude, and 0-12 km altitude. Substantial OCS and CS2 enhancements were observed for a great many air masses of Chinese and Japanese origin during TRACE-P. Over the western Pacific, mean mixing ratios of long-lived OCS and shorter-lived CS2 showed a gradual decrease by about 10% and a factor of 5-10, respectively, from the surface to 8-10 km altitude, presumably because land-based sources dominated their distribution during February through April 2001. The highest mean OCS and CS 2 levels (580 and 20 pptv, respectively, based on 2.5° × 2.5° latitude bins) were observed below 2 km near the coast of Asia, at latitudes between 25°N and 35°N, where urban Asian outflow was strongest. Ratios of OCS versus CO for continental SE Asia were much lower compared to Chinese and Japanese signatures and were strongly associated with biomass burning/biofuel emissions. We present a new inventory of anthropogenic Asian emissions (including biomass burning) for OCS and CS2 and compare it to emission estimates based on regional relationships of OCS and CS 2 to CO and CO2. The OCS and CS2 results for the two methods compare well for continental SE Asia and Japan plus Korea and also for Chinese CS2 emissions. However, it appears that the inventory underestimates Chinese emissions of OCS by about 30-100%. This difference may be related to the fact that we did not include natural sources such as wetland emissions in our inventory, although the contributions from such sources are believed to be at a seasonal low during the study period. Uncertainties in OCS emissions from Chinese coal burning, which are poorly characterized, likely contribute to the discrepancy. Copyright 2004 by the American Geophysical Union.

In situ aircraft measurements of ozone (O3) and its precursors were made over northern Australia in August-September 1999 during the Biomass Burning and Lightning Experiment Phase B (BIBLE-B). A clear positive correlation of O3 with carbon monoxide (CO) was found in biomass burning plumes in the boundary layer (

The atmospheric CO2 mixing ratio was measured using a continuous measurement system onboard a Gulfstream-II aircraft between the northern midlatitudes and the southern subtropics during the Biomass Burning and Lightning Experiment Phase A (BIBLE A) campaign in September-October 1998. The vertical distribution Of CO2 over tropical regions was almost constant from the surface to an altitude of 13 km. CO2 enhancements from biomass burning and oceanic release were observed in the tropical boundary layer. Measurements in the upper troposphere indicate interhemispheric exchange was effectively suppressed between 2°N-7°N. Interhemispheric transport of air in the upper troposphere was suppressed effectively in this region. The CO2 mixing ratios in the Northern and Southern Hemispheres were almost constant, with an average value of about 365 parts per million (ppm) and 366 ppm, respectively. The correlation between the CO2 and NOy mixing ratios observed north of 7°N was apparently different from that obtained south of 2°N. This fact strongly supports the result that the north-south boundary in the upper troposphere during BIBLE A was located around 2°N-7°N as the boundary is not necessary a permanent feature.

The Biomass Burning and Lightning Experiment phase A (BIBLE-A) aircraft observation campaign was conducted from 24 September to 10 October 1998, during a La Niña period. During this campaign, distributions of ozone and its precursors (NO, CO, and nonmethane hydrocarbons (NMHCs)) were observed over the tropical Pacific Ocean, Indonesia, and northern Australia. Mixing ratios of ozone and its precursors were very low at altitudes between 0 and 13.5 km over the tropical Pacific Ocean. The mixing ratios of ozone precursors above 8 km over Indonesia were often significantly higher than those over the tropical Pacific Ocean, even though the prevailing easterlies carried the air from the tropical Pacific Ocean to over Indonesia within several days. For example, median NO and CO mixing ratios in the upper troposphere were 12 parts per trillion (pptv) and 72 parts per billion (ppbv) over the tropical Pacific Ocean and were 83 pptv and 85 ppbv over western Indonesia, respectively. Meteorological analyses and high ethene (C2H4) mixing ratios indicate that the increase of the ozone precursors was caused by active convection over Indonesia through upward transport of polluted air, mixing, and lightning all within the few days prior to observation. Sources of ozone precursors are discussed by comparing correlations of some NMHCs and CH3Cl concentrations with CO between the lower and upper troposphere. Biomass burning in Indonesia was nearly inactive during BIBLE-A and was not a dominant source of the ozone precursors, but urban pollution and lightning contributed importantly to their increases. The increase in ozone precursors raised net ozone production rates over western Indonesia in the upper troposphere, as shown by a photochemical model calculation. However, the ozone mixing ratio (∼20 ppbv) did not increase significantly over Indonesia because photochemical production of ozone did not have sufficient time since the augmentation of ozone precursors. Backward trajectories show that many air masses sampled over the ocean south of Indonesia and over northern Australia passed over western Indonesia 4-9 days prior to being measured. In these air masses the mixing ratios of ozone precursors, except for short-lived species, were similar to those over western Indonesia. In contrast, the ozone mixing ratio was higher by about 10 ppbv than that over Indonesia, indicating that photochemical production of ozone occurred during transport from Indonesia. The average rate of ozone increase (1.8 ppbv/d during this transport is similar to the net ozone formation rate calculated by the photochemical model. This study shows that active convection over Indonesia carried polluted air upward from the surface and had a discernable influence on the distribution of ozone in the upper troposphere over the Indian Ocean, northern Australia, and the south subtropical Pacific Ocean, combined with NO production by lightning.

Aircraft observations of ozone and its precursors (NO, NOy, CO, and nonmethane hydrocarbons) were made near Japan (26°-44°N) between 21 and 24 April 1998 to investigate the effect of transport and chemistry on the tropospheric ozone over east Asia in spring. The average mixing ratios of ozone and its precursors in the upper troposphere were higher than those observed during February-March 1994. Significantly higher values of CO indicate that the influence of surface sources mediated by convection was large throughout the troposphere during the period. Highly polluted air masses were observed in the upper troposphere at 8-11 km over the Japan Sea on 24 April. These air masses were influenced by cumulus convection associated with a cold front over northeast China about 1 day prior to the observation. However, the majority of observed air masses in the upper troposphere were not directly affected by the recent emissions of the ozone precursors from east Asia. Instead, convection over other regions in the northern midlatitude, followed by long-range transport, affected the abundances of ozone precursors in the upper troposphere. In these air masses, ozone was positively correlated with NOx and C3H8, indicating the effect of photochemical ozone production. The diurnal-average column-integrated rate of ozone production, estimated by a photochemical box model, was larger than the NH average and local stratospheric flux at NH midlatitudes in spring by a factor of 3-20. The net production rates in the majority of the air masses were estimated to be 0.5-4.4 ppbv d-1 in the upper troposphere. These results indicate the important role photochemistry plays in controlling the upper tropospheric ozone abundance in spring.

In situ aircraft measurements of trace gases and aerosols were made in the boundary layer (BL) and free troposphere (FT) over Indonesia and Australia during the Biomass Burning and Lightning Experiment (BIBLE)-A and B conducted in August-October 1998 and 1999. Concentrations of ozone (O3) and its precursors [CO, reactive nitrogen (NOx), non-methane hydrocarbons (NMHCs)] were measured in these campaigns to identify the sources of NOx and to estimate the effects of biomass burning and lightning on photochemical production of O3. Over Indonesia, in-situ production of NOx by lightning was found to be a major source of reactive nitrogen in the upper troposphere during BIBLE-A. In some circumstances, increases in reactive nitrogen were often associated with enhancements in CO and NMHCs, suggesting that the sources were biomass burning and fossil fuel combustion, followed by upward transport by cumulus convection. Over Australia the levels of O3, CO, reactive nitrogen, and NMHCs were elevated throughout the troposphere compared to those observed in the tropical Pacific. However, the mechanisms responsible for the enhanced concentrations in the BL and FT are distinctly different. The emissions from biomass burning that occurred in northern Australia were restricted to the BL because of strong subsidence in the period. In the FT over Australia, elevated concentrations of O3 and its precursors result from injections of emissions as the air masses travel over Africa, South America, the Indian Ocean, and Indonesia en route to Australia. In all cases, O3 levels in the biomass burning plumes were enhanced due to photochemical production.

The impact of aircraft emissions on reactive nitrogen in the upper troposphere (UT) and lowermost stratosphere (LS) was estimated using the NOy-O3 correlation obtained during the Subsonic Assessment (SASS) Ozone and Nitrogen Oxide Experiment (SONEX) carried out over the U.S. continent and North Atlantic Flight Corridor (NAFC) region in October and November 1997. To evaluate the large-scale impact, we made a reference NOy-O3 relationship in air masses, upon which aircraft emissions were considered to have little impact. For this purpose, the integrated input of NOx from aircraft into an air mass along a 10-day back trajectory (ΔNOy) was calculated based on the Abatement of Nuisance Caused by Air Traffic/European Commission (ANCAT/EC2) emission inventory. The excess NOy (dNOy) was calculated from the observed NOy and the reference NOy-O3 relationship. As a result, a weak positive correlation was found between the dNOy and ΔNOy, and dNOy and NOx/NOy values, while no positive correlation between the dNOy and CO values was found, suggesting that dNOy values can be used as a measure of the NOx input from aircraft emissions. The excess NOy values calculated from another NOy-O3 reference relationship made using in situ condensation nuclei data also agreed with these dNOy values, within the uncertainties. At the NAFC region (45° N-60° N) the median value of dNOy in the troposphere increased with altitude above 9 km and reached 70 parts per trillion by volume (pptv) (20% of NOy) at 11 km. The excess NOx was estimated to be about half of the dNOy values, corresponding to 30% of the observed NOx level. Higher dNOy values were generally found in air masses where O3 = 75-125 ppbv, suggesting a more pronounced effect around the tropopause. The median value of dNOy in the stratosphere at the NAFC region at 8.5-11.5 km was about 120 pptv. The higher dNOy values in the LS were probably due to the accumulated effect of aircraft emissions, given the long residence time of affected air in the LS. Similar dNOy values were also obtained in air masses sampled over the U.S. continent. Copyright 2000 by the American Geophysical Union.