[1] Bromoform (CHBr 3 ), dibromochloromethane (CHBr 2 Cl), and dibromomethane (CH 2 Br 2 ) in the atmosphere were measured at various sites, including tropical islands, the Arctic, and the open Pacific Ocean. Up to 40 ppt of bromoform was observed along the coasts of tropical islands under a sea breeze. Polybromomethane concentrations were highly correlated among the coastal samples, and the ratios CH 2 Br 2 /CHBr 3 and CHBr 2 Cl/ CHBr 3 showed a clear tendency to decrease with increasing CHBr 3 concentration. These findings are consistent with the observations that polybromomethanes are emitted mostly from macroalgae whose growth is highly localized to coastal areas and that CHBr 3 has the shortest lifetime among these three compounds. The relationship between the concentration ratios CHBr 3 /CH 2 Br 2 and CHBr 2 Cl/CH 2 Br 2 suggested a large mixing/ dilution effect on bromomethane ratios in coastal regions and yielded a rough estimate of 9 for the molar emission ratio of CHBr 3 /CH 2 Br 2 and of 0.7 for that of CHBr 2 Cl/CH 2 Br 2 . Using these ratios and an global emission estimate for CH 2 Br 2 (61 Gg/yr (Br)) calculated from its background concentration, the global emission rates of CHBr 3 and CHBr 2 Cl were calculated to be approximately 820(±310) Gg/yr (Br) and 43(±16) Gg/yr (Br), respectively, assuming that the bromomethanes ratios measured in this study are global representative. The estimated CHBr 3 emission is consistent with that estimated in a very recent study by integrating the sea-to-air flux database. Thus the contribution of CHBr 3 and CHBr 2 Cl to inorganic Br in the atmosphere is likely to be more important than previously thought. Citation: Yokouchi, Y., et al. (2005), Correlations and emission ratios among bromoform, dibromochloromethane, and dibromomethane in the atmosphere,

Balloon‐borne observations of frost‐point temperature and ozone in the equatorial western, central and eastern Pacific as well as over equatorial eastern Brazil provide a highly accurate data set of water vapor across the tropical tropopause. Data were obtained at San Cristóbal, Galapagos, Ecuador (0.9°S, 89.6°W), during the late northern winter and the late northern summer in 1998 and 1999 and at Juazeiro do Norte, Brazil (7.2°S, 39.3°W), in February and November 1997. Earlier data in the western Pacific region in March 1993 were reanalyzed to extend the scope of the observations. The data show three different circumstances in which saturation or supersaturation occurs and imply different mechanisms for dehydration at the tropical tropopause: (1) convective dehydration, (2) slow‐ascent dehydration, and (3) large‐scale wave‐driven dehydration. Furthermore, air that crosses the tropical tropopause in the late northern summer may be dehydrated further during late northern fall, as the average tropical tropopause rises and cools. Not all soundings show dehydration, and there are clear differences in the frequency and depth of saturation in different regions and seasons. The tropopause transition region can be identified in accurate measurements of relative humidity, even under conditions where ozone observations are ambiguous. Deep convection plays an important role in setting up this transition region, which is then subject to large‐scale wave activity and wave breaking at the tropopause or midlatitude intrusions. High relative humidities over regions of strong subsidence show that descending motion in the troposphere is limited to levels below the transition region.

[1] We investigated water vapor variations in the tropical lower stratosphere on seasonal, quasi-biennial oscillation (QBO), and decadal time scales using balloon-borne cryogenic frost point hygrometer data taken between 1993 and 2009 during various campaigns including the Central Equatorial Pacific Experiment (March 1993), campaigns once or twice annually during the Soundings of Ozone and Water in the Equatorial Region (SOWER) project in the eastern Pacific (1998Pacific ( -2003

[1] Here we present measurements of a range of carbon-based compounds: carbon dioxide (CO 2 ), carbon monoxide (CO), methane (CH 4 ), nonmethane hydrocarbons (NMHCs), methyl halides, and dimethyl sulfide (DMS) emitted by Australian savanna fires studied as part of the Biomass Burning and Lightning Experiment (BIBLE) phase B aircraft campaign, which took place during the local late dry season (28 August to 13 September 1999). Significant enhancements of short-lived NMHCs were observed in the boundary layer (BL) over the region of intensive fires and indicate recent emissions for which the mean transport time was estimated to be about 9 hours. Emission ratios relative to CO were determined for 20 NMHCs, 3 methyl halides, DMS, and CH 4 based on the BL enhancements in the source region. Tight correlations with CO were obtained for most of those compounds, indicating the homogeneity of the local savanna source. The emission ratios were in good agreement with some previous measurements of savanna fires for stable compounds but indicated the decay of emission ratios during transport for several reactive compounds. Based on the observed emission ratios, emission factors were derived and compared to previous studies. While emission factors (g species/kg dry mole) of CO 2 varied little according to the vegetation types, those of CO and NMHCs varied significantly. Higher combustion efficiency and a lower emission factor for methane in this study, compared to forest fires, agreed well with results for savanna fires in other tropical regions. The amount of biomass burned was estimated by modeling methods using available satellite data, and showed that 1999 was an above average year for savanna burning. The gross emissions of the trace gases from Australian savanna fires were estimated.

A polarization lidar was continuously operated aboard the research vessel Mirai in the tropical western Pacific over three northern winters: at 2.0°N, 138.0°E during November and December 2001; at 2.0°N, 138.5°E during November and December 2002; and at 7.5°N, 134.0°E during December 2004 and January 2005. Intensive radiosonde soundings were made from the vessel at 3‐h intervals during all three campaigns. The mechanisms that underlie the observed variations in cirrus in the tropical tropopause layer (TTL) are discussed from the viewpoint of large‐scale dynamics and transport. During the 2001 campaign, the tropopause region was cold, but the TTL was often clear, with only some subvisual cirrus. Potential vorticity data and trajectories show that the TTL during this period was strongly affected by dry air transport from the northern midlatitude lower stratosphere. During the 2002 campaign, a packet of large‐amplitude equatorial Kelvin waves was the primary control on the generation and disappearance of cirrus in the TTL. During the 2004–2005 campaign, a cold phase of large‐scale waves resulted in cirrus generation in the TTL in late December of 2004, similar to that observed during the 2002 campaign. Outflow from the South Pacific Convergence Zone (SPCZ) caused optically thick cirrus in the TTL, particularly during early January 2005, when we also observed regular diurnal variations in cirrus development within the TTL, that is, apparent sedimentation during the nighttime. We investigated two possible controlling processes, namely, horizontal advection together with diurnal variations in convective activity within the SPCZ and diurnal variations in local temperature due to tides and gravity waves. In the equatorial western Pacific, equatorial Kelvin waves are the important dynamical process that controls cirrus variations in the TTL. Dry‐air horizontal transport from the midlatitude lower stratosphere and wet‐air vertical transport near the tropical convergence regions should also be considered in fully explaining the cirrus observations in the TTL.

Abstract. Soundings of frost-point hygrometers, ozonesondes, and radiosondes at San Cristdbal Island (0.9øS, 89.6øW) in September 1998 provide an observational evidence that equatorial Kelvin waves around the tropopause act as a dehydration pump for the stratosphere. During the downwarddisplacement phase of a Kelvin wave, dry and ozone-rich stratospheric air is transported into the upper troposphere. During the upward-displacement phase, on the other hand, higher specific-humidity air moves up in the tropopause region, but at the same time, this upward motion causes cooling of the air that limits the water vapor amount entering the stratosphere. Also, wave breaking contributes to the irreversible transport of ozone across the tropopause. Considering their omnipresence at the equatorial tropopause, we suggest that Kelvin waves may be one of the important agents for maintaining the dryness of the tropical lower stratosphere.

[1] 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 (C 2 H 4 ) 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 CH 3 Cl 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. Citation: Kita, K., et al., Photochemical production of ozone in the upper troposphere in association with cumulus c...

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