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Chatfield, Robert

Publications and source records attributed to Chatfield, Robert.

Seasonal and Diurnal Opportunities for XCH4, XCO2, and XCO for the Amazonian Rainforest Region Allowing Sampling and Validation

There is considerable interest in the aggregate methane emissions from the Amazon and similar moist tropical regions, and XCH4 measurements are well suited to constrain sources to the global atmosphere. Similarly, XCO2 measurements constrain CO2 in the region. XCO helps to partition CO2 patterns among burning and respiration processes. GeoCarb may allow these column measurements over the Western Hemisphere, but satellite retrieval require exacting calibration and validation by sun-focused Fourier transform spectrometers (FTS). The rarity of sufficiently large gaps in the cloud cover over the Amazon and similar rainforests restricts the validation opportunities for useful FTS observations and even more the opportunities for accurate retrievals. TropOMI observational statistics are extremely poor for the region. We have used two data sources to evaluate FTS opportunities at Manaus, Brazil, an FTS operated for 8 months near Manaus by Mavendra Dubey, and also sun-photometer measurements at several stations. The promise of using data from other satellites, e.g. GOES-16 ( (Geostationary Operational Environmental Satellite) and CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization gaps and aerosol layering will be described. We report initial results on five questions: (1) how frequent are observing opportunities of FTS?, (2) What evidence is there that gaps in clouds are wide enough for satellite retrievals at an appropriate accuracy, (3) What is the diurnal and seasonal variability of cloud gaps?, and (4) What limitations are currently suggested for unbiased FTS measurement of XCH4 due to diurnal effects, and (5) What evidence is there for incidence of problematic high aerosol extinction at higher layers of the troposphere (800 hPa to 120 hPa) which alter the XCH4 light-paths?

Chatfield, Robert↗

Tropospheric Ozone Profiling Using Simulated GEO-CAPE Measurement

Multi-spectral retrievals (UV+VIS, UV+TIR, UV+VIS+TIR) improve sensitivity to the variability in near-surface O3 by a factor of 2 - 2.7 over those from UV or TIR alone. Multi-spectral retrievals provide the largest benefit when there is enhanced O3 near the surface. Combining all 3 wavelengths (UV+VIS+TIR) provides the greatest sensitivity below 850 hPa, with a 36% improvement over UV+VIS and a 17% improvement over UV+TIR. The impacts of clouds and aerosols are being assessed.

human versus natural sources↗

Quantifying VOC-Reaction Tracers, Ozone Production, and Continuing Aerosol Production Rates in Urban and Far-Downwind Atmospheres

We have found a surprisingly informative decomposition of the complex question of smoggy ozone production (basically, [HO2] in a more locally determined field of [NO]) in the process of linked investigations of modestly smoggy Eastern North America (by NASA aircraft, July 2004) and rather polluted Flushing, NYC (Queens College, July, 2001). In both rural and very polluted situations, we find that a simple contour graph parameterization of the local principal ozone production rate can be estimated using only the variables [NO] and j(sub rads) [HCHO]: Po(O3) = c (j(sub rads) [HCHO])(sup a) [HCHO](sup b). Here j(sub rads) is the photolysis of HCHO to radicals, presumably capturing many harder-UV photolytic processes and the principle ozone production is that due to HO2; mechanisms suggest that ozone production due to RO2 is closely correlated, often suggesting a limited range of different proportionality factors. The method immediately suggests a local interpretation for concepts of VOC limitation and NOx limitation. We believe that the product j(sub rads) [HCHO] guages the oxidation rate of observed VOC mixtures in a way that also provides [HO2] useful for the principle ozone production rate k [HO2] [NO], and indeed, all ozone chemical production. The success of the method suggests that dominant urban primary-HCHO sources may transition to secondary plume-HCHO sources in a convenient way. Are there other, simple, near-terminal oxidized VOC's which help guage ozone production and aerosol particle formation? Regarding particles, we report on, to the extent NASA Research resources allow, on appealing relationships between far-downwind (Atlantic PBL) HCHO and very fine aerosol (including sulfate. Since j(sub rads) [HCHO] provides a time-scale, we may understand distant-plume particle production in a more quantitative manner. Additionally we report on a statistical search in the nearer field for relationships between glyoxals (important near-terminal aromatic and isoprene reaction products) and aerosol production, looking for VOC's that might be most implicated. All three variables j(sub rads), [HCHO], and [NO] are relatively easily measured in widespread air pollution monitoring networks, and all are deducible form space-borne observations, though estimation of [NO] from [NO2] (the species observable from space) may require care. We report also on airborne and surface observations of HCHO, suggesting that concentrated (urban) and more diffuse (forest) sources may be distinguishable from space. The use of the 3.58 micron microwindow for HCHO remote sensing should allow much sharper resolution of HCHO than the UV. UV sensing requires large and expensive instruments, but even these seem justified since formaldehyde is so informative.

Chatfield, Robert↗

Workshop Report on Managing Solar Radiation

The basic concept of managing Earth's radiation budget is to reduce the amount of incoming solar radiation absorbed by the Earth so as to counterbalance the heating of the Earth that would otherwise result from the accumulation of greenhouse gases. The workshop did not seek to decide whether or under what circumstances solar radiation management should be deployed or which strategies or technologies might be best, if it were deployed. Rather, the workshop focused on defining what kinds of information might be most valuable in allowing policy makers more knowledgeably to address the various options for solar radiation management.

Lane, Lee↗

Analysis of North Atlantic Aircraft Data on Oxygenated Intermediate Species Using an Adapted Regional Chemistry-Transport Model

Our study is on the interaction of nitrogen oxides with organics as they are exported from their complex sources in Eastern North America. Both urban and specific industrial emissions contribute the nitrogen of the C-H-O-N compounds that affect the global atmosphere, helping determine both ozone and the self-cleaning radical chemistry of the troposphere mediated by the OH radical. Different industrial sources, urban, and natural emissions contribute the organic C. Peroxyacetyl nitrate, CH3C(double bonds O)OONO2 is the most interesting compound for which we can measure the outflow to the full depth of the Atlantic troposphere. As we adapt the 3-d chemical model to describe outflow for specific periods with sufficient accuracy, we are analyzing some valuable information in the NARE-97 complete airborne dataset. (NARE: North Atlantic Regional Experiment). Ames researchers find that there are substantial puzzles in the ratios of PAN/NO2. Peroxy acetyl nitrate provides one of the major long-distance export pathways for active nitrogen from Eastern North America. It should be closely linked with NO, (defined as the sum NO + NO2) by simple thermal association and decomposition reactions, at least when the ambient temperature is substantially above 5 C.

Chatfield, Robert↗

Making Intercontinental Burning Influences Quantitative: Lessons on Transport and Geochemistry From the 3-D Simulation of CO in PEM-T A and TRACE-A

We report on two aspects of the simulation of global transport of plumes originating from subtropical biomass fires. We use of meteorological assimilation (MM5) at 2-degree resolution with a Grail cloud parameterization and a Blackadar-based planetary boundary layer parameterization. Ames's GRACES model provides emissions, transport, and an appropriate level of simulated chemical transformation. We have worked with passive-tracer CO or linear chemistry. This is appropriate since we find major work to be done in evaluating CO source strengths and transport mechanisms before chemical integrations could be meaningful. First, we present mechanisms by which CO and other pollutants are introduced into the free troposphere, and are then transported with hate dilution from approx. 0 to approx. 180 degrees longitude. One principal conduit for these plumes is the vernal subtropical jet; however the plumes appear at various altitudes and latitudes as they influenced by frontal motions and (most likely) radiative processes. A common, repeated pattern of transport has pollutant plumes arriving in the distant Pacific Ocean from Africa and South America at 25 degrees south and 14 km altitude. Following this, there is then a general appearance of pollution at extending down to 5 kin at more equatorial (10 S) and polar latitudes (to 45 S). Second, we evaluate the quantitative success of our simulation. (Such success requires efforts considerably beyond trajectory analyses, and is necessary for our community to claim an understanding of the effects of biomass burning on global atmospheric chemistry and the planet's trend in oxidizing capacity.) We find that we simulate most pollution episodes sampled by Glenn Sachse's CO instrument and the Blake hydrocarbon analyses during PENT A. We will present our current ideas on why our general levels appear satisfactory when the observations are within 20 ppb of background levels, but substantially miss the variability associated with the most intense biomass burning plumes. As time allows, we will speculate on the origins of a class of plumes that appear in the mid-troposphere, but are missing from our simulations.

Chatfield, Robert↗