Robert B. Chatfield

Bio: Robert B. Chatfield is an academic researcher from Ames Research Center. The author has contributed to research in topics: Troposphere & Tropospheric ozone. The author has an hindex of 39, co-authored 85 publications receiving 5248 citations. Previous affiliations of Robert B. Chatfield include University at Albany, SUNY & Washington State University.

Estimates on the production of CO and H2 from the oxidation of hydrocarbon emissions from vegetation

Abstract: Extrapolating from extensive field measurements on foliar emissions in the U.S. approximate global inputs of isoprene and terpenes of 3.5 times 10 to the 14th power and 4.8 times 10 to the 14th power g(C)/yr, respectively, are obtained. The oxidation of these hydrocarbons could contribute in an important way to the atmospheric sources of CO (4.2-13.3 times 10 to the 14th power g/yr) and H2 (10-35 times 10 to the 12th power g/yr), and to organic species soluble in rainwater

Sulfur dioxide in remote oceanic air: Cloud transport of reactive precursors

Abstract: Reactive surface emissions of reduced sulfur gases can produce SO2 in the middle and upper troposphere at the levels of 80±30 pptv measured high over the remote oceans. We present simulations with a two-dimensional “Staubsauger” or “vacuum cleaner” model that combines a photochemical model with a description of vertical transport of trace species by convective clouds within larger synoptic circulations. Emissions of 20–60 Tg (S)/yr of (CH3)2S, H2S, or CS2, may produce the observed SO2. Roughly equal production rates of SO2 and methane sulfonic acid may be expected. The amount and exact vertical distribution of the SO2 produced remain uncertain: the greatest chemical uncertainties are the reaction yield of SO2 expectable under clean tropospheric conditions and also the liquid-phase removal of SO2, and the oxidation rate. The amount of upper tropospheric SO2 produced depends substantially on the proximity of strong reduced S sources to regions of active convection. However, the character of the solutions we present is invariably distinctly different from those obtained with one- or two-dimensional models employing the eddy-diffusion hypothesis. The results of the model point beyond its original conception, and stress the likely importance of the rainy tropical jungles and mid-latitude industrial regions, since both regions have large sulfur emissions arid frequently active cumulonimbus convection. This process, however, should contribute mainly to upper-tropospheric SO2. Other chemical implications are that tropospheric OH may depend critically on HOOH levels as well as the hydrocarbon and nitrogen oxide cycles. Cloud transport may play an important role in these cycles. The hydroxyl radical concentration depends as much on assumptions regarding HOOH reaction and transport as it does on NO levels.

Including the sub-grid scale plume rise of vegetation fires in low resolution atmospheric transport models

Abstract: We describe and begin to evaluate a parameterization to include the vertical transport of hot gases and particles emitted from biomass burning in low resolution atmospheric-chemistry transport models. This sub-grid transport mechanism is simulated by embedding a 1-D cloud-resolving model with appropriate lower boundary conditions in each column of the 3-D host model. Through assimilation of remote sensing fire products, we recognize which columns have fires. Using a land use dataset appropriate fire properties are selected. The host model provides the environmental conditions, allowing the plume rise to be simulated explicitly. The derived height of the plume is then used in the source emission field of the host model to determine the effective injection height, releasing the material emitted during the flaming phase at this height. Model results are compared with CO aircraft profiles from an Amazon basin field campaign and with satellite data, showing the huge impact that this mechanism has on model performance. We also show the relative role of each main vertical transport mechanisms, shallow and deep moist convection and the pyro-convection (dry or moist) induced by vegetation fires, on the distribution of biomass burning CO emissions in the troposphere.

Dimethyl sulfide in the marine atmosphere

Abstract: We have performed over 900 measurements of atmospheric dimethyl sulfide (DMS) in five different marine locations: the equatorial Pacific; Cape Grim, Tasmania; the Bahamas; the North Atlantic; and the Sargasso Sea At all locations, DMS concentrations were usually in the range of 100–400 ng S m−3, with similar average concentrations of approximately 150 ng S m−3 (107 parts per thousand by volume) Highest concentrations occurred during, but were not limited to, periods of sustained high winds and overcast skies, presumably owing to faster exchange from surface seawater and less photochemical activity in the atmosphere Lowest values occurred during airflow from continental regions, which provides higher levels of oxidants and free radicals to react with DMS Averaged over time, the concentrations in clean marine air reached a maximum at night and a minimum in the afternoon, when concentrations were about one third lower than during the nighttime maximum The observed concentrations of DMS in the marine atmosphere and their diurnal variability agree well with model simulations involving OH and NO3 oxidation of DMS and are consistent with a global sea-to-air DMS flux of about 40±20 Tg S yr−1 DMS may represent a major sink for NO3 in the marine troposphere

Analysis of the atmospheric distribution, sources, and sinks of oxygenated volatile organic chemicals based on measurements over the Pacific during TRACE‐P

Abstract: Airborne measurements of a large number of oxygenated volatile organic chemicals (OVOC) were carried out in the Pacific troposphere (0.1-12 km) in winter/spring of 2001 (24 February to 10 April). Specifically, these measurements included acetone (CH3COCH3), methylethyl ketone (CH3COC2H5, MEK), methanol (CH3OH), ethanol (C2H5OH), acetaldehyde (CH3CHO), propionaldehyde (C2H5CHO), peroxyacylnitrates (PANs) (C(sub n)H(sub 2n+1)COO2NO2), and organic nitrates (C(sub n)H(sub 2n+1)ONO2). Complementary measurements of formaldehyde (HCHO), methyl hydroperoxide (CH3OOH), and selected tracers were also available. OVOC were abundant in the clean troposphere and were greatly enhanced in the outflow regions from Asia. Background mixing ratios were typically highest in the lower troposphere and declined toward the upper troposphere and the lowermost stratosphere. Their total abundance (Summation of OVOC) was nearly twice that of nonmethane hydrocarbons (Summation of C2-C8 NMHC). Throughout the troposphere, the OH reactivity of OVOC is comparable to that of methane and far exceeds that of NMHC. A comparison of these data with western Pacific observations collected some 7 years earlier (February-March 1994) did not reveal significant differences. Mixing ratios of OVOC were strongly correlated with each other as well as with tracers of fossil and biomass/biofuel combustion. Analysis of the relative enhancement of selected OVOC with respect to CH3Cl and CO in 12 plumes originating from fires and sampled in the free troposphere (3-11 km) is used to assess their primary and secondary emissions from biomass combustion. The composition of these plumes also indicates a large shift of reactive nitrogen into the PAN reservoir thereby limiting ozone formation. A three-dimensional global model that uses state of the art chemistry and source information is used to compare measured and simulated mixing ratios of selected OVOC. While there is reasonable agreement in many cases, measured aldehyde concentrations are significantly larger than predicted. At their observed levels, acetaldehyde mixing ratios are shown to be an important source of HCHO (and HO x ) and PAN in the troposphere. On the basis of presently known chemistry, measured mixing ratios of aldehydes and PANs are mutually incompatible. We provide rough estimates of the global sources of several OVOC and conclude that collectively these are extremely large (150-500 Tg C / yr) but remain poorly quantified.

Bounding the role of black carbon in the climate system: A scientific assessment

Abstract: Black carbon aerosol plays a unique and important role in Earth's climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. This assessment provides an evaluation of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice. These effects are calculated with climate models, but when possible, they are evaluated with both microphysical measurements and field observations. Predominant sources are combustion related, namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom-up inventory methods are 7500 Gg yr−1 in the year 2000 with an uncertainty range of 2000 to 29000. However, global atmospheric absorption attributable to black carbon is too low in many models and should be increased by a factor of almost 3. After this scaling, the best estimate for the industrial-era (1750 to 2005) direct radiative forcing of atmospheric black carbon is +0.71 W m−2 with 90% uncertainty bounds of (+0.08, +1.27) W m−2. Total direct forcing by all black carbon sources, without subtracting the preindustrial background, is estimated as +0.88 (+0.17, +1.48) W m−2. Direct radiative forcing alone does not capture important rapid adjustment mechanisms. A framework is described and used for quantifying climate forcings, including rapid adjustments. The best estimate of industrial-era climate forcing of black carbon through all forcing mechanisms, including clouds and cryosphere forcing, is +1.1 W m−2 with 90% uncertainty bounds of +0.17 to +2.1 W m−2. Thus, there is a very high probability that black carbon emissions, independent of co-emitted species, have a positive forcing and warm the climate. We estimate that black carbon, with a total climate forcing of +1.1 W m−2, is the second most important human emission in terms of its climate forcing in the present-day atmosphere; only carbon dioxide is estimated to have a greater forcing. Sources that emit black carbon also emit other short-lived species that may either cool or warm climate. Climate forcings from co-emitted species are estimated and used in the framework described herein. When the principal effects of short-lived co-emissions, including cooling agents such as sulfur dioxide, are included in net forcing, energy-related sources (fossil fuel and biofuel) have an industrial-era climate forcing of +0.22 (−0.50 to +1.08) W m−2 during the first year after emission. For a few of these sources, such as diesel engines and possibly residential biofuels, warming is strong enough that eliminating all short-lived emissions from these sources would reduce net climate forcing (i.e., produce cooling). When open burning emissions, which emit high levels of organic matter, are included in the total, the best estimate of net industrial-era climate forcing by all short-lived species from black-carbon-rich sources becomes slightly negative (−0.06 W m−2 with 90% uncertainty bounds of −1.45 to +1.29 W m−2). The uncertainties in net climate forcing from black-carbon-rich sources are substantial, largely due to lack of knowledge about cloud interactions with both black carbon and co-emitted organic carbon. In prioritizing potential black-carbon mitigation actions, non-science factors, such as technical feasibility, costs, policy design, and implementation feasibility play important roles. The major sources of black carbon are presently in different stages with regard to the feasibility for near-term mitigation. This assessment, by evaluating the large number and complexity of the associated physical and radiative processes in black-carbon climate forcing, sets a baseline from which to improve future climate forcing estimates.

Climate Change 2007: Impacts, Adaptation and Vulnerability.

Abstract: Impatti, adattamento e vulnerabilita Le cause e le responsabilita dei cambiamenti climatici sono state trattate sul numero di ottobre della rivista Cda. Approfondiamo l’argomento presentando il documento: “Cambiamenti climatici 2007: impatti, adattamento e vulnerabilita” votato ad aprile 2007 dal secondo gruppo di lavoro del Comitato Intergovernativo sui Cambiamenti Climatici (Intergovernmental Panel on Climate Change). Si tratta del secondo di tre documenti che compongono il quarto rapporto sui cambiamenti climatici.

Oceanic phytoplankton, atmospheric sulphur, cloud albedo and climate

Abstract: The major source of cloud-condensation nuclei (CCN) over the oceans appears to be dimethylsulphide, which is produced by planktonic algae in sea water and oxidizes in the atmosphere to form a sulphate aerosol Because the reflectance (albedo) of clouds (and thus the Earth's radiation budget) is sensitive to CCN density, biological regulation of the climate is possible through the effects of temperature and sunlight on phytoplankton population and dimethylsulphide production. To counteract the warming due to doubling of atmospheric CO2, an approximate doubling of CCN would be needed.

Organic geochemistry of natural waters

Abstract: This book is written as a reference on organic substances in natural waters and as a supplementary text for graduate students in water chemistry. The chapters address five topics: amount, origin, nature, geochemistry, and characterization of organic carbon. Of these topics, the main themes are the amount and nature of dissolved organic carbon in natural waters (mainly fresh water, although seawater is briefly discussed). It is hoped that the reader is familiar with organic chemistry, but it is not necessary. The first part of the book is a general overview of the amount and general nature of dissolved organic carbon. Over the past 10 years there has been an exponential increase in knowledge on organic substances in water, which is the result of money directed toward the research of organic compounds, of new methods of analysis (such as gas chromatography and mass spectrometry), and most importantly, the result of more people working in this field. Because of this exponential increase in knowledge, there is a need to pull together and summarize the data that has accumulated from many disciplines over the last decade.

Biomass Burning in the Tropics: Impact on Atmospheric Chemistry and Biogeochemical Cycles

Abstract: The use of fire as a tool to manipulate the environment has been instrumental in the human conquest of Earth, the first evidence of the use of fires by early hominids dating back to 1–1.5 million years ago [1]. Even today, most human-ignited vegetation fires take place on the African continent, and its widespread, frequently burned savannas bear ample witness to this. Although natural fires can occur even in tropical forest regions [2, 3], the extent of fires has greatly expanded on all continents with the arrival of Homo sapiens. Measurements of charcoal in dated sediment cores have shown clear correlations between the rate of burning and human settlement [4]. Pollen records show a shift with human settlement from pyrophobic vegetation to pyrotolerant and pyrophilic species, testimony to the large ecological impact of human-induced fires.