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Thompson, Anne M.

Publications and source records attributed to Thompson, Anne M..

At least 127 records · Page 7

A trajectory modeling investigation of the biomass burning-tropical ozone relationship

The hypothesis that tropical total O3 maxima seen by the TOMS satellite derive from African biomass burning has been tested using isentropic trajectory analyses with global meteorological data fields. Two case studies from the 1989 biomass burning season demonstrate that a large fraction of the air arriving at the location of TOMS O3 maxima passed over regions of intense burning. Other trajectories initiated at a series of points over Africa and the Atlantic suggest flight strategies for field studies to be conducted in September 1992.

Pickering, Kenneth E.↗

Enhancement of free tropospheric ozone production by deep convection

It is found from model simulations of trace gas and meteorological data from aircraft campaigns that deep convection may enhance the potential for photochemical ozone production in the middle and upper troposphere by up to a factor of 60. Examination of half a dozen individual convective episodes show that the degree of enhancement is highly variable. Factors affecting enhancement include boundary layer NO(x) mixing ratios, differences in the strength and structure of convective cells, as well as variation in the amount of background pollution already in the free troposphere.

Pickering, Kenneth E.↗

The atmospheric CH4 increase since the Last Glacial Maximum. I - Source estimates

An estimate of the distribution of wetland area and associated CH4 emission is presented for the Last Glacial Maximum (LGM, 18 kyr BP, kiloyear Before Present) and the Pre-Industrial Holocene (PIH, 9000-200 years BP). The wetland source, combined with estimates of the other biogenic sources and sink, yields total source strengths of 120 and 180 Tg CH4/yr for LGM and PIH respectively. These source strengths are shown to be consistent with source estimates inferred from a photochemical model, and point to changes in wetland CH4 source as a major factor driving the atmospheric CH4 increase from LGM to PIH.

Chappellaz, Jerome A.↗

The atmospheric CH4 increase since the Last Glacial Maximum. II - Interactions with oxidants

Results of two studies of the effect of changing CH4 fluxes on global tropospheric oxidant levels, O3, OH, and H2O2, performed with a multibox photochemical model, are presented. A sensitivity study is conducted by scaling back CH4, CO, and NO emissions relative to the present-day budget. When the CH4 ice core record is compared to calculated CH4 abundances, corresponding CH4 fluxes for the preindustrial Holocene (PIH) and Last Glacial Maximum (LGM) are fairly well-constrained: 175-225 Tg CH/4/yr for PIH and 100-130 Tg CH4/yr for LGM. Specific scenarios for CH4/CO/NO are selected to represent sources for the PIH and LGM. The CH4 budget is taken from an evaluation of wetlands and other natural sources.

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.↗

Free tropospheric ozone production following entrainment of urban plumes into deep convection

It is shown that rapid vertical transport of air from urban plumes through deep convective clouds can cause substantial enhancement of the rate of O3 production in the free troposphere. Simulation of convective redistribution and subsequent photochemistry of an urban plume from Oklahoma City during the 1985 PRESTORM campaign shows enhancement of O3 production in the free tropospheric cloud outflow layer by a factor of almost 4. In contrast, simulation of convective transport of an urban plume from Manaus, Brazil, into a prestine free troposphere during GTE/ABLE 2B (1987), followed by a photochemical simulation, showed enhancement of O3 production by a factor of 35. The reasons for the different enhancements are (1) intensity of cloud vertical motion; (2) initial boundary layer O3 precursor concentrations; and (3) initial amount of background free tropospheric NO(x). Convective transport of ozone precursors to the middle and upper troposphere allows the resulting O3 to spread over large geographic regions, rather than being confined to the lower troposphere where loss processes are much more rapid. Conversely, as air with lower NO descends and replaces more polluted air, there is greater O3 production efficiency per molecule of NO in the boundary layer following convective transport. As a result, over 30 percent more ozone could be produced in the entire tropospheric column in the first 24 hours following convective transport of urban plumes.

Pickering, Kenneth E.↗

The oxidizing capacity of the earth's atmosphere - Probable past and future changes

A number of critical atmospheric chemical problems depend on the earth's oxidizing capacity, which is essentially the global burden of oxidants in the lower atmosphere. There is limited direct evidence for changes in the earth's oxidizing capacity since recent preindustrial times when, because of industrial and poulation growth, increasing amounts of O3 precursor trace gases (carbon monoxide, nitrogen oxides, and hydrocarbons) have been released into the atmosphere. The concentrations of O3 and possibly H2O2 have increased over large regions. Models predict that tropospheric O3 will increase about 0.3-1.0 percent per year over the next 50 years with both positive and negative trends possible for OH and H2O2. Models and the observational network for oxidants are improving, but validation of global models is still at an early stage.

Thompson, Anne M.↗

Ozone production potential following convective redistribution of biomass burning emissions

The effects of deep convection on the potential for forming ozone in the free troposphere have been simulated for regions where the trace gas composition is influenced by biomass burning. Cloud photochemical and dynamic simulations based on observations in the 1980 and 1985 Brazilian campaigns form the basis of a sensitivity study of the ozone production potential under differing conditions. It is seen that there is considerably more ozone formed in the middle and upper troposphere when convection has redistributed hydrocarbons, NO(x), and CO compared to the example of no convection.

Pickering, Kenneth E.↗

A regional estimate of convective transport of CO from biomass burning

A regional-scale estimate of the fraction of biomass burning emissions that are transported to the free troposphere by deep convection is presented. The focus is on CO and the study region is a part of Brazil that underwent intensive deforestation in the 1980s. The method of calculation is stepwise, scaling up from a prototype convective event, the dynamics of which are well-characterized, to the vertical mass flux of carbon monoxide over the region. Given uncertainties in CO emissions from biomass burning and the representativeness of the prototype event, it is estimated that 10-40 percent of CO emissions from the burning region may be rapidly transported to the free troposphere over the burning region. These relatively fresh emissions will produce O3 efficiently in the free troposphere where O3 has a longer lifetime than in the boundary layer.

Pickering, Kenneth E.↗

Methane on the greenhouse agenda

Options for reducing methane emissions, which could have a significant effect on global warming, are addressed. Emissions from landfills, coal mining, oil and natural gas systems, ruminants, animal wastes and wastewater, rice cultivation, and biomass burning are considered. Methods for implementing these emission reductions are discussed.

Hogan, Kathleen B.↗

Effect of chemical kinetics uncertainties on calculated constituents in a tropospheric photochemical model

Random photochemical reaction rates are employed in a 1D photochemical model to examine uncertainties in tropospheric concentrations and thereby determine critical kinetic processes and significant correlations. Monte Carlo computations are used to simulate different chemical environments and their related imprecisions. The most critical processes are the primary photodissociation of O3 (which initiates ozone destruction) and NO2 (which initiates ozone formation), and the OH/methane reaction is significant. Several correlations and anticorrelations between species are discussed, and the ozone/transient OH correlation is examined in detail. One important result of the modeling is that estimates of global OH are generally about 25 percent uncertain, limiting the precision of photochemical models. Techniques for reducing the imprecision are discussed which emphasize the use of species and radical species measurements.

Thompson, Anne M.↗

Photochemical ozone production in tropical squall line convection during NASA Global Tropospheric Experiment/Amazon Boundary Layer Experiment 2A

The role of convection was examined in trace gas transport and ozone production in a tropical dry season squall line sampled on August 3, 1985, during NASA Global Tropospheric Experiment/Amazon Boundary Layer Experiment 2A (NASA GTE/ABLE 2A) in Amazonia, Brazil. Two types of analyses were performed. Transient effects within the cloud are examined with a combination of two-dimensional cloud and one-dimensional photochemical modeling. Tracer analyses using the cloud model wind fields yield a series of cross sections of NO(x), CO, and O3 distribution during the lifetime of the cloud; these fields are used in the photochemical model to compute the net rate of O3 production. At noon, when the cloud was mature, the instantaneous ozone production potential in the cloud is between 50 and 60 percent less than in no-cloud conditions due to reduced photolysis and cloud scavenging of radicals. Analysis of cloud inflows and outflows is used to differentiate between air that is undisturbed and air that has been modified by the storm. These profiles are used in the photochemical model to examine the aftereffects of convective redistribution in the 24-hour period following the storm. Total tropospheric column O3 production changed little due to convection because so little NO(x) was available in the lower troposphere. However, the integrated O3 production potential in the 5- to 13-km layer changed from net destruction to net production as a result of the convection. The conditions of the August 3, 1985, event may be typical of the early part of the dry season in Amazonia, when only minimal amounts of pollution from biomass burning have been transported into the region.

Pickering, Kenneth E.↗

Two approaches to determining the sea-to-air flux of dimethyl sulfide - Satellite ocean color and a photochemical model with atmospheric measurements

The feasibility of using remotely sensed data to map the marine sources of a photoreactive trace gas was investigated by comparing satellite ocean color data with result of a photochemical model with atmospheric measurements of dimethyl sulfide (DMS). A mean DMS flux for a region in the tropical North Atlantic for October 1980 was derived, using an empirical relationship between DMS and chlorophyll a data obtained by the CZCS instrument, and was compared with the sea-to-air flux derived from a one-dimensional photochemical model that reproduces boundary layer concentrations of ozone, CO, NO, and hydrocarbons measured by an experimental vessel cruising at the same location and time. Results suggest that surface sensing of DMS sources is feasible but only in regions and seasons where phytoplankton pigment is a meaningful marker for biogenic emissions.

Thompson, Anne M.↗

Cloud draft structure and trace gas transport

During the second Amazon Boundary Layer Experiment (ABLE 2B), meteorological observations, chemical measurements, and model simulations are utilized in order to interpret convective cloud draft structure and to analyze its role in transport and vertical distribution of trace gases. One-dimensional photochemical model results suggest that the observed poststorm changes in ozone concentration can be attributed to convective transports rather than photochemical production and the results of a two-dimensional time-dependent cloud model simulation are presented for the May 6, 1987 squall system. The mesoscale convective system exhibited evidence of significant midlevel detrainment in addition to transports to anvil heights. Chemical measurements of O3 and CO obtained in the convective environment are used to predict photochemical production within the troposphere and to corroborate the cloud model results.

Scala, John R.↗

Model calculations of tropospheric ozone production potential following observed convective events

The profiles of CO, NO, O3, water vapor, and temperature, observed in 1985 during and after a series of convective events over rural areas of the south-central United States, were used to model the nonurban ozone production rates and to evaluate the effects of convective clouds on the tropospheric trace-gas chemistry. A comparison of trace-gas profiles measured in and around a large cumulonimbus during its dissipation showed that ozone production in the upper troposphere may be increased fourfold by convection relative to undisturbed air. The convective enhancement of O3 production for the entire tropospheric comlumn was found to be about 50 percent.

Pickering, Kenneth E.↗

Perturbations to tropospheric oxidants, 1985-2035. I - Calculations of ozone and OH in chemically coherent regions

A one-dimensional model based on the sensitivity coefficients of Thompson (1990) is used to calculate regional changes in tropospheric O3 and OH due to specified global or regional changes in CH4 and CO emissions over the period 1985-2035. The methods applied are explained, and the results are presented in extensive tables and graphs and characterized in detail. A 10-15-percent increase in global tropospheric O3 and a 10-15-percent decrease in OH are predicted for both (1) global scenarios with continuing increases in CH4 and CO and (2) regional scenarios where emissions are limited in some regions but not in others; significant regional variation in O3 is predicted for (2). If depletion of O3 in the stratosphere and global warming are introduced into (1) or (2), however, they nearly cancel out the tropospheric O3 increases and OH decreases.

Thompson, Anne M.↗

Comparison of parameterized nitric acid rainout rates using a coupled stochastic-photochemical tropospheric model

A major tropospheric loss of soluble species such as nitric acid results from scavenging by water droplets. Several theoretical formulations have been advanced which relate an effective time-independent loss rate for soluble species to statistical properties of precipitation such as the wet fraction and length of a precipitation cycle. In this paper, various 'effective' loss rates that have been proposed are compared with the results of detailed time-dependent model calculations carried out over a seasonal time scale. The model is a stochastic precipitation model coupled to a tropospheric photochemical model. The results of numerous time-dependent seasonal model runs are used to derive numerical values for the nitric acid residence time for several assumed sets of preciptation statistics. These values are then compared with the results obtained by utilizing theoretical 'effective' loss rates in time-independent models.

Stewart, Richard W.↗

Sensitivity of tropospheric hydrogen peroxide to global chemical and climate change

The sensitivities of tropospheric HO2 and hydrogen peroxide (H2O2) levels to increases in CH4, CO, and NO emissions and to changes in stratospheric O3 and tropospheric O3 and H2O have been evaluated with a one-dimensional photochemical model. Specific scenarios of CH4-CO-NO(x) emissions and global climate changes are used to predict HO2 and H2O2 changes between 1980 and 2030. Calculations are made for urban and nonurban continental conditions and for low latitudes. Generally, CO and CH4 emissions will enhance H2O2; NO emissions will suppress H2O2 except in very low NO(x) regions. A global warming or stratospheric O3 depletion will add to H2O2. Hydrogen peroxide increases from 1980 to 2030 could be 100 percent or more in the urban boundary layer.

Thompson, Anne M.↗