A mass-balance/photochemical assessment of DMS sea-to-air flux as inferred from NASA GTE PEM-West a and B observations

This study reports dimethyl sulfide (DMS) sea-to-air fluxes derived from a mass-balance/photochemical-modeling approach. The region investigated was the western North Pacific covering the latitude range of 0°-30°N. Two NASA airborne databases were used in this study: PEM-West A in September-October 1991 and PEM-West B in February-March 1994. A total of 35 boundary layer (BL) sampling runs were recorded between the two programs. However, after filtering these data for pollution impacts and DMS lifetime considerations, this total was reduced to 13. Input for each analysis consisted of atmospheric DMS measurements, the equivalent mixing depth (EMD) for DMS, and model estimated values for OH and NO3. The evaluation of the EMD took into account both DMS within the BL as well as that transported into the overlying atmospheric buffer layer (BuL). DMS fluxes ranged from 0.6 to 3.0 μmol m-2d-1 for PEM-West A (10 sample runs) and 1.4 to 1.9 μmol m-2d-1 for PEM-West B (3 sample runs). Sensitivity analyses showed that the photochemically evaluated DMS flux was most influenced by the DMS vertical profile and the diel profile for OH. A propagation of error analysis revealed that the uncertainty associated with individual flux determinations ranged from a factor of 1.3 to 1.5. Also assessed were potential systematic errors. The first of these relates to our noninclusion of large-scale mean vertical motion as it might appear in the form of atmospheric subsidence or as a convergence. Our estimates here would place this error in the range of O to 30%. By far the largest systematic error is that associated with stochastic events (e.g., those involving major changes in cloud coverage). In the latter case, sensitivity tests suggested that the error could be as high as a factor of 2. With improvements in such areas as BL sampling time, direct observations of OH, improved DMS vertical profiling, direct assessment of vertical velocity in the field, and preflight (24 hours) detailed meteorological data, it appears that the uncertainty in this approach could be reduced to ±25%. Copyright 1999 by the American Geophysical Union

Interdisciplinary study of atmospheric processes and constituents of the mid-Atlantic coastal region.

Past research projects for the year 1974-1975 are listed along with future research programs in the area of air pollution control, remote sensor analysis of smoke plumes, the biosphere component, and field experiments. A detailed budget analysis is presented. Attachments are included on the following topics: mapping forest vegetation with ERTS-1 MSS data and automatic data processing techniques, and use of LARS system for the quantitative determination of smoke plume lateral diffusion coefficients from ERTS images of Virginia

Ambient Atmospheric Hydrocarbon Content as Determined by Gas Chromatographic Techniques from Rural Tidewater Virginia in Late Spring 1974

In an attempt to ascertain the naturally generated hydrocarbon contribution to the air quality of the Hampton Roads region of Tidewater Virginia, a series of 27 air samples was obtained in two rural locations during late spring of 1974. These samples were analyzed for their hydrocarbon content (carbon number range C5 to C10) using gas chromatographic techniques. The thirty different hydrocarbon species were identified and monitored in the experiment. Preliminary analysis of the data indicates an average concentration of 397 parts per billion by weight (carbon) for the total non-methane hydrocarbon loading for C5 to C10 during the experiment. This value exceeds the National Primary Air Quality Standards as set by the Environmental Protection Agency

Highlights of OH, H2SO4, and methane sulfonic acid measurements made aboard the NASA P-3B during Transport and Chemical Evolution over the Pacific

Measurements of hydroxyl radical (OH), sulfuric acid (H2SO4), and methane sulfonic acid (MSA) were performed aboard the NASA P-3B using the selected ion chemical ionization mass spectrometry technique during the Transport and Chemical Evolution over the Pacific (TRACE-P) study. Photochemical box model calculations of OH concentrations yielded generally good agreement with an overall tendency to overestimate the measured OH by ∼20%. Further analysis reveals that this overestimation is present only at altitudes greater than ∼1.5 km, with the model underestimating OH measurements at lower altitudes. Boundary layer H2SO4 measurements, performed in a volcanic plume off the southern coast of Japan, revealed some of the largest marine boundary layer H2SO4 concentrations ever observed and were accompanied by new particle formation. Nighttime measurements of OH, H2SO4, and MSA in the remote pacific off Midway Island revealed significant boundary layer concentrations of H2SO4 and MSA, indicating evidence of nighttime boundary layer oxidation processes but in the absence of OH. A cursory exploration of the sources of production of the H2SO4 and MSA observed at night is presented

Carbonyl sulfide and carbon disulfide: Large-scale distributions over the western Pacific and emissions from Asia during TRACE-P

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

Evaluating regional emission estimates using the TRACE-P observations

Measurements obtained during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) experiment are used in conjunction with regional modeling analysis to evaluate emission estimates for Asia. A comparison between the modeled values and the observations is one method to evaluate emissions. Based on such analysis it is concluded that the inventory performs well for the light alkanes, CO, ethyne, SO2, and NOₓ. Furthermore, based on model skill in predicting important photochemical species such as O₃, HCHO, OH, HO₂, and HNO₃, it is found that the emissions inventories are of sufficient quality to support preliminary studies of ozone production. These are important finding in light of the fact that emission estimates for many species (such as speciated NMHCs and BC) for this region have only recently been estimated and are highly uncertain. Using a classification of the measurements built upon trajectory analysis, we compare observed species distributions and ratios of species to those modeled and to ratios estimated from the emissions inventory. It is shown that this technique can reconstruct a spatial distribution of propane/benzene that looks remarkably similar to that calculated from the emissions inventory. A major discrepancy between modeled and observed behavior is found in the Yellow Sea, where modeled values are systematically underpredicted. The integrated analysis suggests that this may be related to an underestimation of emissions from the domestic sector. The emission is further tested by comparing observed and measured species ratios in identified megacity plumes. Many of the model derived ratios (e.g., BC/CO, SOₓ/C₂H₂) fall within ∼25% of those observed and all fall outside of a factor of 2.5. (See Article file for details of the abstract.)Department of Civil and Environmental EngineeringAuthor name used in this publication: Wang, T

Carbonyl sulfide and carbon disulfide: Large-scale distributions over the western Pacific and emissions from Asia during TRACE-P

An extensive set of carbonyl sulfide (OCS) and carbon disulfide (CS2) 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 CS2levels (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 CS2 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