Showing papers by "Prasad S. Kasibhatla published in 2000"

Global distribution of carbon monoxide

Abstract: This study explores the evolution and distribution of carbon monoxide (CO) using the National Oceanic and Atmospheric Administration (NOAA) Geophysical Fluid Dynamics Laboratory three-dimensional global chemical transport model (GFDL GCTM). The work aims to gain an improved understanding of the global carbon monoxide budget, specifically focusing on the contribution of each of the four source terms to the seasonal variability of CO. The sum of all CO sources in the model is 2.5 Pg CO/yr (1 Pg = 103 Tg), including fossil fuel use (300 Tg CO/yr), biomass burning (748 Tg CO/yr), oxidation of biogenic hydrocarbons (683 Tg CO/yr), and methane oxidation (760 Tg CO/yr). The main sink for CO is destruction by the hydroxyl radical, and we assume a hydroxyl distribution based on three-dimensional monthly varying fields given by Spivakovsky et al. [1990], but we increase this field by 15% uniformly to agree with a methyl chloroform lifetime of 4.8 years [Prinn et al, 1995]. Our simulation produces a carbon monoxide field that agrees well with available measurements from the NOAA/Climate Monitoring and Diagnostics Laboratory global cooperative flask sampling network and from the Jungfraujoch observing station of the Swiss Federal Laboratories for Materials Testing and Research (EMPA) (93% of seasonal-average data points agree within ±25%) and flight data from measurement campaigns of the NASA Global Tropospheric Experiment (79% of regional-average data points agree within ±25%). For all 34 ground-based measurement sites we have calculated the percentage contribution of each CO source term to the total model-simulated distribution and examined how these contributions vary seasonally due to transport, changes in OH concentration, and seasonality of emission sources. CO from all four sources contributes to the total magnitude of CO in all regions. Seasonality, however, is usually governed by the transport and destruction by OH of CO emitted by fossil fuel and/or biomass burning. The sensitivity to the hydroxyl field varies spatially, with a 30% increase in OH yielding decreases in CO ranging from 4–23%, with lower sensitivities near emission regions where advection acts as a strong local sink. The lifetime of CO varies from 10 days over summer continental regions to well over a year at the winter poles, where we define lifetime as the turnover time in the troposphere due to reaction with OH.

Emission inventory development and processing for the Seasonal Model for Regional Air Quality (SMRAQ) project

Abstract: This paper describes the experiences and insights gained from inventory preparation and emissions processing for the Seasonal Model for Regional Air Quality (SMRAQ) project. The emission inventory was derived from the 1990 and 1995 Ozone Transport Assessment Group (OTAG) inventories. Here we outline the emissions processing strategy used for the May-to-September simulation, summarize the inventory characteristics and corrections made on the OTAG inventories, and describe the quality assurance steps taken as part of the processing. We then provide spatial maps and daily total time series charts of the hourly, gridded emissions of nitrogen oxides (NOx), reactive organic gases (ROG), and carbon monoxide (CO). Large peaks from electric utility point sources and urban mobile sources characterize the NOx emissions, and the NOx emissions in nonpeak regions are primarily mobile-source emissions. ROG emissions are dominated by biogenic isoprene production in the southern United States, and they have a strong seasonal variability. CO emissions are characterized by less variability, with area and mobile sources dominating the inventory. We compare ratios of season-average nonmethane organic gases to NOx between the emission inventory and the Photochemical Assessment Monitoring Stations (PAMS) data, and these comparisons show poor correlation between the inventory and ambient ratios.

A comparison of scavenging and deposition processes in global models: results from the WCRP Cambridge Workshop of 1995

Abstract: We report on results from a World Climate Research Program workshop on representations of scavenging and deposition processes in global transport models of the atmosphere 15 models were evaluated by comparing simulations of radon, lead, sulfur dioxide, and sulfate against each other, and against observations of these constituents This paper provides a survey on the simulation diVerences between models It identifies circumstances where models are consistent with observations or with each other, and where they diVer from observations or with each other The comparison shows that most models are able to simulate seasonal species concentrations near the surface over continental sites to within a factor of 2 over many regions of the globe Models tend to agree more closely over source (continental) regions than for remote (polar and oceanic) regions Model simulations diVer most strongly in the upper troposphere for species undergoing wet scavenging processes There are not a suYcient number of observations to characterize the climatology (long-term average) of species undergoing wet scavenging in the upper troposphere This highlights the need for either a diVerent strategy for model evaluation (eg, comparisons on an event by event basis) or many more observations of a few carefully chosen constituents

A comparison of scavenging and deposition processes in global models: Results from the WCRP Cambridge workshop of 1995

Abstract: We report on results from a World Climate Research Program workshop on representations of scavenging and deposition processes in global transport models of the atmosphere. 15 models were evaluated by comparing simulations of radon, lead, sulfur dioxide, and sulfate against each other, and against observations of these constituents. This paper provides a survey on the simulation diVerences between models. It identifies circumstances where models are consistent with observations or with each other, and where they diVer from observations or with each other. The comparison shows that most models are able to simulate seasonal species concentrations near the surface over continental sites to within a factor of 2 over many regions of the globe. Models tend to agree more closely over source (continental) regions than for remote (polar and oceanic) regions. Model simulations diVer most strongly in the upper troposphere for species undergoing wet scavenging processes. There are not a suYcient number of observations to characterize the climatology (long-term average) of species undergoing wet scavenging in the upper troposphere. This highlights the need for either a diVerent strategy for model evaluation (e.g., comparisons on an event by event basis) or many more observations of a few carefully chosen constituents.

Do emissions from ships have a significant impact on concentrations of nitrogen oxides in the marine boundary layer

Abstract: The potential impact of ship emissions on concentrations of nitrogen oxides and reactive nitrogen compounds in the marine boundary layer is assessed using a global chemical transport model. The model predicts significant enhancements of these compounds over large regions, especially over the northern midlatitude oceans. This result is consistent with a recently published study, though the impacts predicted here are more widespread and the peak enhancements are not as large. However, comparisons of model results with recent measurements over the central North Atlantic Ocean do not provide support for these model predictions. While one cannot completely overlook the possibility that emissions of nitrogen oxides from ships may be overestimated, our analysis suggests that there may be a gap in our understanding of the chemical evolution of ship plumes as they mix into the background atmosphere in the marine boundary layer. On a related note, it is also possible that the overestimate of the impacts of ships on nitrogen oxides in the marine boundary layer by global models is due to the lack of parameterized representations of plume dynamics and chemistry in these models.

A study of DMS oxidation in the tropics : Comparison of Christmas Island field observations of DMS, SO2, and DMSO with model simulations

Abstract: This study reports comparisonsbetween model simulations, based on current sulfurmechanisms, with the DMS, SO2 and DMSOobservational data reported by Bandy et al.(1996) in their 1994 Christmas Island field study. For both DMS and SO2, the model results werefound to be in excellent agreement with theobservations when the observations were filtered so asto establish a common meteorological environment. Thisfiltered DMS and SO2 data encompassedapproximately half of the total sampled days. Basedon these composite profiles, it was shown thatoxidation of DMS via OH was the dominant pathway withno more than 5 to 15% proceeding through Cl atoms andless than 3% through NO3. This analysis wasbased on an estimated DMS sea-to-air flux of 3.4 ×109 molecs cm-2 s-1. The dominant sourceof BL SO2 was oxidation of DMS, the overallconversion efficiency being evaluated at 0.65 ± 0.15. The major loss of SO2 was deposition to theocean's surface and scavenging by aerosol. Theresulting combined first order k value was estimated at 1.6 × 10-5 s-1. In contrast to the DMSand SO2 simulations, the model under-predictedthe observed DMSO levels by nearly a factor of 50. Although DMSO instrument measurement problems can notbe totally ruled out, the possibility of DMSO sourcesother than gas phase oxidation of DMS must beseriously considered and should be explored in futurestudies.

Seasonal modeling of regional ozone pollution in the eastern United States

Abstract: In this study, we report on the results from a comprehensive model simulation of regional ozone (O3) throughout a season in the eastern United States. The model is shown to perform better in terms of simulating seasonal, rather than episodic, characteristics of the regional surface O3 distribution. This finding suggests that it may be more appropriate to use models of this type to assess seasonal O3 patterns rather than following the current paradigm of developing regional control strategies based on event-specific simulations.