A Method for Obtaining High Time and Spatial Resolution Convective Cloud Top Data for the TTL

A method for obtaining high time and spatial resolution convective cloud top data for the TTL Leonhard Pfister, Eric Jensen, Rei Ueyama, Eliot Atlas, and Maria Navarro Convective systems in the tropics have a maximum in the cloud top altitude distribution of about 13.5 km. However, there is a significant tail to this distribution -- a few percent reach the cold point tropopause (CPT) at 16.5 km, and there has been clear evidence of convective mass deposited as high as 19 km in the tropics. The region between 13.5 km and the cold point tropopause is transitional, between the free tropical troposphere where convective mixing dominates, and the stratosphere where slow upward ascent dominates. In this region (the Tropical Tropopause Layer), convective injection, slow ascent, and mixing from midlatitudes all have similar time scales. So, even though only a few percent of convective systems reach the CPT, convection is important. Space Based Lidar and cloud radar measurements have yielded information about long term average statistical distributions of cloud altitude as a function of location. However, we also need time-dependent cloud top altitude and cloud top potential temperature information, primarily to understand the water vapor and TTL cloud distributions. This is because the effect of convection depends on the local temperature, and on the subsequent temperature history. Time dependent cloud top information is also needed to understand short-lived tracers because cross-isentropic flow is time and space dependent. This paper presents a method of obtaining time and space dependent convective cloud top theta (and altitude) information using 3-hourly geostationary brightness temperature data, coupled with global 3 -hourly rainfall estimates and temperature analyses. We explore different mixing algorithms to obtain the most reasonable agreement with near-simultaneous observations by cloudsat and calipso. Observations of short-lived tracers from ATTREX, coupled with short-term trajectories are used to test the method's accuracy. An important caveat is the ambiguity of evaluating convective cloud top altitudes under from combined cloudsat and calipso measurements

Controls on atmospheric chloroiodomethane (CH2ClI) in marine environments

Mixing ratios of chloroiodomethane (CH2ClI) in ambient air were quantified in the coastal North Atlantic region (Thompson Farm, Durham, New Hampshire, and Appledore Island, Maine) and two remote Pacific areas (Christmas Island, Kiribati, and Oahu, Hawaii). Average mixing ratios were 0.15 ± 0.18 and 0.68 ± 0.66 parts per trillion by volume (pptv) at Thompson Farm and Appledore Island, respectively, compared to 0.10 ± 0.05 pptv at Christmas Island and 0.04 ± 0.02 pptv in Hawaii. Photolysis constrained the daytime mixing ratios of CH2ClI at all locations with the minimum occurring at 1600 local time. Daily average fluxes to the atmosphere were estimated from mixing ratios and loss due to photolysis at Appledore Island, Christmas Island and Hawaii, and were 58 ± 9, 19 ± 3, and 5.8 ± 1.0 nmol CH2ClI m−2 d−1, respectively. The measured sea‐to‐air flux from seawater equilibrator samples obtained near Appledore Island was 6.4 ± 2.9 nmol CH2ClI m−2 d−1. Mixing ratios of CH2ClI at Appledore Island increased with increasing wind speed. The maximum mixing ratios observed at Thompson Farm (1.6 pptv) and Appledore Island (3.4 pptv) are the highest reported values to date, and coincided with high winds associated with the passage of Tropical Storm Bonnie. We estimate that high winds during the 2004 hurricane season increased the flux of CH2ClI from the North Atlantic Ocean by 8 ± 2%

Airborne sampling of aerosol particles: Comparison between surface sampling at Christmas Island and P-3 sampling during PEM-Tropics B

Bulk aerosol sampling of soluble ionic compounds from the NASA Wallops Island P-3 aircraft and a tower on Christmas Island during PEM-Tropics B provides an opportunity to assess the magnitude of particle losses in the University of New Hampshire airborne bulk aerosol sampling system. We find that most aerosol-associated ions decrease strongly with height above the sea surface, making direct comparisons between mixing ratios at 30 m on the tower and the lowest flight level of the P-3 (150 m) open to interpretation. Theoretical considerations suggest that vertical gradients of sea-salt aerosol particles should show exponential decreases with height. Observed gradients of Na+ and Mg2+, combining the tower observations with P-3 samples collected below 1 km, are well described by exponential decreases (r values of 0.88 and 0.87, respectively), though the curve fit underestimates average mixing ratios at the surface by 25%. Cascade impactor samples collected on the tower show that \u3e99% of the Na+ and Mg2+mass is on supermicron particles, 65% is in the 1–6 micron range, and just 20% resides on particles with diameters larger than 9 microns. These results indicate that our airborne aerosol sampling probes must be passing particles up to at least 6 microns with high efficiency. We also observed that nss SO42− and NH4+, which are dominantly on accumulation mode particles, tended to decrease between 150 and 1000 m, but they were often considerably higher at the lowest P-3 sampling altitudes than at the tower. This finding is presently not well understood

Effect of sulfate aerosol on tropospheric NOx and ozone budgets: Model simulations and TOPSE evidence

The distributions of NOx and O3 are analyzed during TOPSE (Tropospheric Ozone Production about the Spring Equinox). In this study these data are compared with the calculations of a global chemical/transport model (Model for OZone And Related chemical Tracers (MOZART)). Specifically, the effect that hydrolysis of N2O5 on sulfate aerosols has on tropospheric NOx and O3 budgets is studied. The results show that without this heterogeneous reaction, the model significantly overestimates NOx concentrations at high latitudes of the Northern Hemisphere (NH) in winter and spring in comparison to the observations during TOPSE; with this reaction, modeled NOx concentrations are close to the measured values. This comparison provides evidence that the hydrolysis of N2O5 on sulfate aerosol plays an important role in controlling the tropospheric NOx and O3 budgets. The calculated reduction of NOx attributed to this reaction is 80 to 90% in winter at high latitudes over North America. Because of the reduction of NOx, O3 concentrations are also decreased. The maximum O3reduction occurs in spring although the maximum NOx reduction occurs in winter when photochemical O3 production is relatively low. The uncertainties related to uptake coefficient and aerosol loading in the model is analyzed. The analysis indicates that the changes in NOxdue to these uncertainties are much smaller than the impact of hydrolysis of N2O5 on sulfate aerosol. The effect that hydrolysis of N2O5 on global NOx and O3 budgets are also assessed by the model. The results suggest that in the Northern Hemisphere, the average NOx budget decreases 50% due to this reaction in winter and 5% in summer. The average O3 budget is reduced by 8% in winter and 6% in summer. In the Southern Hemisphere (SH), the sulfate aerosol loading is significantly smaller than in the Northern Hemisphere. As a result, sulfate aerosol has little impact on NOx and O3 budgets of the Southern Hemisphere

Intercontinental transport of pollution manifested in the variability and seasonal trend of springtime O3 at northern middle and high latitudes

Observations (0–8 km) from the Tropospheric Ozone Production about the Spring Equinox (TOPSE) experiment are analyzed to examine air masses contributing to the observed variability of springtime O3 and its seasonal increase at 40°–85°N over North America. Factor analysis using the positive matrix factorization and principal component analysis methods is applied to the data set with 14 chemical tracers (O3, NOy, PAN, CO, CH4, C2H2, C3H8, CH3Cl, CH3Br, C2Cl4, CFC-11, HCFC-141B, Halon-1211, and 7Be) and one dynamic tracer (potential temperature). Our analysis results are biased by the measurements at 5–8 km (70% of the data) due to the availability of 7Be measurements. The identified tracer characteristics for seven factors are generally consistent with the geographical origins derived from their 10 day back trajectories. Stratospherically influenced air accounts for 14 ppbv (35–40%) of the observed O3 variability for data with O3concentrations \u3c100 ppbv at middle and high latitudes. It accounts for about 2.5 ppbv/month (40%) of the seasonal O3 trend at midlatitudes but for only 0.8 ppbv/month (\u3c20%) at high latitudes, likely reflecting more vigorous midlatitude dynamical systems in spring. At midlatitudes, reactive nitrogen-rich air masses transported through Asia are much more significant (11 ppbv in variability and 3.5 ppbv/month in trend) than other tropospheric contributors. At high latitudes the O3 variability is significantly influenced by air masses transported from lower latitudes (11 ppbv), which are poor in reactive nitrogen. The O3 trend, in contrast, is largely defined by air masses rich in reactive nitrogen transported through Asia and Europe across the Pacific or the Arctic (3 ppbv/month). The influence from the stratospheric source is more apparent at 6–8 km, while the effect of O3 production and transport within the troposphere is more apparent at lower altitudes. The overall effect of tropospheric photochemical production, through long-range transport, on the observed O3 variability and its seasonal trend is more important at high latitudes relative to more photochemically active midlatitudes

How Marine Emissions of Bromoform Impact the Remote Atmosphere

It is an open question how localized elevated emissions of bromoform (CHBr3) and other very short-lived halocarbons (VSLHs), found in coastal and upwelling regions, and low background emissions, typically found over the open ocean, impact the atmospheric VSLH distribution. In this study, we use the Lagrangian dispersion model FLEXPART to simulate atmospheric CHBr3 resulting from assumed uniform background emissions, and from elevated emissions consistent with those derived during three tropical cruise campaigns. The simulations demonstrate that the atmospheric CHBr3 distributions in the uniform background emissions scenario are highly variable with high mixing ratios appearing in regions of convergence or low wind speed. This relation holds on regional and global scales. The impact of localized elevated emissions on the atmospheric CHBr3 distribution varies significantly from campaign to campaign. The estimated impact depends on the strength of the emissions and the meteorological conditions. In the open waters of the western Pacific and Indian oceans, localized elevated emissions only slightly increase the background concentrations of atmospheric CHBr3, even when 1∘ wide source regions along the cruise tracks are assumed. Near the coast, elevated emissions, including hot spots up to 100 times larger than the uniform background emissions, can be strong enough to be distinguished from the atmospheric background. However, it is not necessarily the highest hot spot emission that produces the largest enhancement, since the tug-of-war between fast advective transport and local accumulation at the time of emission is also important. Our results demonstrate that transport variations in the atmosphere itself are sufficient to produce highly variable VSLH distributions, and elevated VSLHs in the atmosphere do not always reflect a strong localized source. Localized elevated emissions can be obliterated by the highly variable atmospheric background, even if they are orders of magnitude larger than the average open ocean emissions

Age spectra and other transport diagnostics in the North American monsoon UTLS from SEAC4^{4}RS in situ trace gas measurements

The upper troposphere and lower stratosphere (UTLS) region during the summer monsoon season over North America (NAM) is influenced by the transport of air from a variety of source regions over a wide range of timescales (hours to years). Age spectra are useful for characterizing the transport into such a region, and in this study we use and build on recently developed techniques to infer age spectra from trace gas measurements with photochemical lifetimes from days to centuries. We show that the measurements taken by the whole-air sampler instrument during the SEAC$^{4}$RS campaign can be used to derive not only age spectra, but also path-integrated lifetimes of each of the trace gases and partitioning between North American and tropical surface source origins. The method used here can also clearly identify and adjust for measurement outliers that were influenced by polluted surface source regions. The results are generally consistent with expected transport features of the NAM but also provide a range of transport diagnostics (age spectra, trace gas lifetimes and surface source regions) that have not previously been computed solely from in situ measurements. These methods may be applied to many other existing in situ datasets, and the transport diagnostics can be compared with chemistry–climate model transport in the UTLS