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Kucsera, Tom L.

Publications and source records attributed to Kucsera, Tom L..

Investigation of Global Particulate Nitrate from the AeroCom Phase III Experiment

An assessment of global particulate nitrate and ammonium aerosol based on simulations from nine models participating in the Aerosol Comparisons between Observations and Models (AeroCom) phase III study is presented. A budget analysis was conducted to understand the typical magnitude, distribution, and diversity of the aerosols and their precursors among the models. To gain confidence regarding model performance, the model results were evaluated with various observations globally, including ground station measurements over North America, Europe, and east Asia for tracer concentrations and dry and wet depositions, as well as with aircraft measurements in the Northern Hemisphere mid-to-high latitudes for tracer vertical distributions. Given the unique chemical and physical features of the nitrate occurrence, we further investigated the similarity and differentiation among the models by examining (1) the pH-dependent NH3 wet deposition; (2) the nitrate formation via heterogeneous chemistry on the surface of dust and sea salt particles or thermodynamic equilibrium calculation including dust and sea salt ions; and (3) the nitrate coarse-mode fraction (i.e., coarse/total). It is found that HNO3, which is simulated explicitly based on full O3-HOx-NOx-aerosol chemistry by all models, differs by up to a factor of 9 among the models in its global tropospheric burden. This partially contributes to a large difference in NO3(-), whose atmospheric burden differs by up to a factor of 13. The atmospheric burdens of NH3 and NHC 4 differ by 17 and 4, respectively. Analyses at the process level show that the large diversity in atmospheric burdens of NO3(-), NH3, and NHC4(+) is also related to deposition processes. Wet deposition seems to be the dominant process in determining the diversity in NH3 and NHC 4 lifetimes. It is critical to correctly account for contributions of heterogeneous chemical production of nitrate on dust and sea salt, because this process overwhelmingly controls atmospheric nitrate production (typically greater than 80 %) and determines the coarse- and fine-mode distribution of nitrate aerosol.

Ammonium aerosol based on simulations↗

Estimated Accuracy of Three Common Trajectory Statistical Methods

Three well-known trajectory statistical methods (TSMs), namely concentration field (CF), concentration weighted trajectory (CWT), and potential source contribution function (PSCF) methods were tested using known sources and artificially generated data sets to determine the ability of TSMs to reproduce spatial distribution of the sources. In the works by other authors, the accuracy of the trajectory statistical methods was estimated for particular species and at specified receptor locations. We have obtained a more general statistical estimation of the accuracy of source reconstruction and have found optimum conditions to reconstruct source distributions of atmospheric trace substances. Only virtual pollutants of the primary type were considered. In real world experiments, TSMs are intended for application to a priori unknown sources. Therefore, the accuracy of TSMs has to be tested with all possible spatial distributions of sources. An ensemble of geographical distributions of virtual sources was generated. Spearman s rank order correlation coefficient between spatial distributions of the known virtual and the reconstructed sources was taken to be a quantitative measure of the accuracy. Statistical estimates of the mean correlation coefficient and a range of the most probable values of correlation coefficients were obtained. All the TSMs that were considered here showed similar close results. The maximum of the ratio of the mean correlation to the width of the correlation interval containing the most probable correlation values determines the optimum conditions for reconstruction. An optimal geographical domain roughly coincides with the area supplying most of the substance to the receptor. The optimal domain s size is dependent on the substance decay time. Under optimum reconstruction conditions, the mean correlation coefficients can reach 0.70 0.75. The boundaries of the interval with the most probable correlation values are 0.6 0.9 for the decay time of 240 h and 0.5 0.95 for the decay time of 12 h. The best results of source reconstruction can be expected for the trace substances with a decay time on the order of several days. Although the methods considered in this paper do not guarantee high accuracy they are computationally simple and fast. Using the TSMs in optimum conditions and taking into account the range of uncertainties, one can obtain a first hint on potential source areas.

Kabashnikov, Vitaliy P.↗

Convective and Wave Signatures in Ozone Profiles Over the Equatorial Americas: Views from TC4 (2007) and SHADOZ

During the months of July-August 2007 NASA conducted a research campaign called the Tropical Composition, Clouds and Climate Coupling (TC4) experiment. Vertical profiles of ozone were measured daily using an instrument known as an ozonesonde, which is attached to a weather balloon and launch to altitudes in excess of 30 km. These ozone profiles were measured over coastal Las Tablas, Panama (7.8N, 80W) and several times per week at Alajuela, Costa Rica (ION, 84W). Meteorological systems in the form of waves, detected most prominently in 100- 300 in thick ozone layer in the tropical tropopause layer, occurred in 50% (Las Tablas) and 40% (Alajuela) of the soundings. These layers, associated with vertical displacements and classified as gravity waves ("GW," possibly Kelvin waves), occur with similar stricture and frequency over the Paramaribo (5.8N, 55W) and San Cristobal (0.925, 90W) sites of the Southern Hemisphere Additional Ozonesondes (SHADOZ) network. The gravity wave labeled layers in individual soundings correspond to cloud outflow as indicated by the tracers measured from the NASA DC-8 and other aircraft data, confirming convective initiation of equatorial waves. Layers representing quasi-horizontal displacements, referred to as Rossby waves, are robust features in soundings from 23 July to 5 August. The features associated with Rossby waves correspond to extra-tropical influence, possibly stratospheric, and sometimes to pollution transport. Comparison of Las Tablas and Alajuela ozone budgets with 1999-2007 Paramaribo and San Cristobal soundings shows that TC4 is typical of climatology for the equatorial Americas. Overall during TC4, convection and associated meteorological waves appear to dominate ozone transport in the tropical tropopause layer.

Thompson, Anne M.↗

Tropical Tropospheric Ozone: A Multi-Satellite View From TOMS and Other Instruments

New tropospheric ozone and aerosol products from the TOMS (Total Ozone Mapping Spectrometer) satellite instrument can resolve episodic pollution events in the tropics and interannual and seasonal variability. Modified-residual (MR) Nimbus 7 tropical tropospheric ozone (TTO), two maps/month (1979-1992, 1-deg latitude by 2-deg longitude) within the region in which total ozone displays a tropical wave-one pattern (maximum 20S to 20N), are available in digital form at http://metosrv2.umd.edu/~tropo. Also available are preliminary 1996-1999 MR-TTO maps based on real-time Earth-Probe (EP)/TOMS observations. Examples of applications are given.

Thompson, Anne M.↗

Tropospheric Ozone Pollution from Space: New Views from the TOMS (Total Ozone Mapping Spectrometer) Instrument

New products from the TOMS (Total Ozone Mapping Spectrometer) >satellite instrument can resolve pollution events in tropical and mid-latitudes, Over the past several years, we have developed tropospheric ozone data sets by two methods. The modified-residual technique [Hudson and Thompson, 1998; Thompson and Hudson, 1999] uses v. 7 TOMS total ozone and is applicable to tropical regimes in which the wave-one pattern in total ozone is observed. The TOMSdirect method [Hudson et at., 2000] represents a new algorithm that uses TOMS radiances to extract tropospheric ozone in regions of constant stratospheric ozone and tropospheric ozone displaying high mixing ratios and variability characteristic of pollution, Absorbing aerosols (dust and smoke; Herman et at., 1997 Hsu et al., 1999), a standard TOMS product, provide transport and/or source marker information to interpret tropospheric ozone. For the Nimbus 7/TOMS observing period (1979-1992), modified-residual TTO (tropical tropospheric ozone) appears as two maps/month at I-degree latitude 2-degree longitude resolution at a homepage and digital data are available (20S to 20N) by ftp at http://metosrv2. umd.edu/~tropo/ 14y_data.d. Preliminary modified-residual TTO data from the operational Earth-Probe/TOMS (1996- present) are posted in near-real-time at the same website. Analyses with the new tropospheric ozone and aerosol data are illustrated by the following (I)Signals in tropical tropospheric ozone column and smoke amount during ENSO (El Nino-Southern Oscillation) events, e.g. 1982-1983 and the intense ENSO induced biomass fires of 1997-1998 over the Indonesian region [Thompson et a[, 2000a, Thompson and Hudson, 1999]. (2) Trends in tropospheric ozone and smoke aerosols in various tropical regions (Atlantic, Pacific, Africa, Brazil). No significant trends were found for ozone from1980-1990 [Thompson and Hudson, 19991 although smoke aerosols increased during the period [Hsu et al.,1999]. (3) Temporal and spatial offsets ("paradoxes") in tropical tropospheric ozone and smoke aerosol in regions of greatest tropical biomass burning [Thompson et at., 1996;2000b]. (4) Trans-boundary pollution tracking. With an air parcel (trajectory) model, smoke aerosol and ozone and dust plumes can be tracked across oceans (e.g., Asia to North America; North America to Europe) and national boundaries, e.g. Indonesia to Singapore and Malaysia during the 1997 ENSO fires.

Thompson, Anne M.↗

Upper tropospheric ozone production following mesoscale convection during STEP/EMEX

The chemistry and dynamics of a convective system observed on February 2, 1987 in the EMEX and STEP campaigns are analyzed. Chemical and thermodynamic profiles in undisturbed air near the EMEX 9 system indicate that the troposphere was well mixed by previous convection. As a consequence there was little direct transport from the boundary layer to the upper troposphere and air transported upward was detrained throughout the middle and upper troposphere. There was minimal effect on O3 production. Other convective complexes located 800-900 km upstream produced greater perturbations on trace gas profile immediately below the tropopause. Ozone production was reduced by about 0.25 ppbv/d at these altitudes, representing a reduction in P(O3) of 15-20 percent over the column from 14.5 to 17 km. P(O3) from 12 to 17 km in a region distant from active convection and subject to lightning was 2-3 times higher than it would have been without lightning.

Pickering, Kenneth E.↗

On the sensitivity of a residual circulation model to differences in input temperature data

The residual mean circulation (RMC) formulation of zonally averaged transport in the middle atmosphere produces a circulation which depends on the distributions of net diabatic heating and temperature. Such circulations are from two temperature data sets, using the same radiative transfer code (Rosenfield et al. 1987). These circulations are then used to transport N2O in a photochemical model. The circulations and the resulting N2O distributions are notably different during the Northern Hemisphere winter, with that based on the NMC temperatures producing too much upward transport in the tropical stratosphere, as judged by comparison with the stratospheric and mesoscale sounder data. The experiment demonstrates that model calculations, in general, and perturbation assessments, in particular, are likely to be quite sensitive to the choice of input temperature data (where this is not computed self-consistently). It also reveals what appears to be a seasonally dependent bias in NMC zonally averaged temperatures with respect to those obtained from the LIMS instrument during 1978/1979.

Guthrie, Paul D.↗