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Jacob, D. J.

Publications and source records attributed to Jacob, D. J..

At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

A large increase in U.S. methane emissions over the past decade inferred from satellite data and surface observations

Abstract The global burden of atmospheric methane has been increasing over the past decade, but the causes are not well understood. National inventory estimates from the U.S. Environmental Protection Agency indicate no significant trend in U.S. anthropogenic methane emissions from 2002 to present. Here we use satellite retrievals and surface observations of atmospheric methane to suggest that U.S. methane emissions have increased by more than 30% over the 2002–2014 period. The trend is largest in the central part of the country, but we cannot readily attribute it to any specific source type. This large increase in U.S. methane emissions could account for 30–60% of the global growth of atmospheric methane seen in the past decade.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2015

Quantifying Sources and Sinks of Reactive Gases in the Lower Atmosphere Using Airborne Flux Observations

Atmospheric composition is governed by the interplay of emissions, chemistry, deposition, and transport. Substantial questions surround each of these processes, especially in forested environments with strong biogenic emissions. Utilizing aircraft observations acquired over a forest in the southeast U.S., we calculate eddy covariance fluxes for a suite of reactive gases and apply the synergistic information derived from this analysis to quantify emission and deposition fluxes, oxidant concentrations, aerosol uptake coefficients, and other key parameters. Evaluation of results against state-of-the-science models and parameterizations provides insight into our current understanding of this system and frames future observational priorities. As a near-direct measurement of fundamental process rates, airborne fluxes offer a new tool to improve biogenic and anthropogenic emissions inventories, photochemical mechanisms, and deposition parameterizations.

emission↗
DOE OSTI2015

Balancing aggregation and smoothing errors in inverse models

Inverse models use observations of a system (observation vector) to quantify the variables driving that system (state vector) by statistical optimization. When the observation vector is large, such as with satellite data, selecting a suitable dimension for the state vector is a challenge. A state vector that is too large cannot be effectively constrained by the observations, leading to smoothing error. However, reducing the dimension of the state vector leads to aggregation error as prior relationships between state vector elements are imposed rather than optimized. Here we present a method for quantifying aggregation and smoothing errors as a function of state vector dimension, so that a suitable dimension can be selected by minimizing the combined error. Reducing the state vector within the aggregation error constraints can have the added advantage of enabling analytical solution to the inverse problem with full error characterization. We compare three methods for reducing the dimension of the state vector from its native resolution: (1) merging adjacent elements (grid coarsening), (2) clustering with principal component analysis (PCA), and (3) applying a Gaussian mixture model (GMM) with Gaussian pdfs as state vector elements on which the native-resolution state vector elements are projected using radial basis functions (RBFs). The GMM method leads to somewhat lower aggregation error than the other methods, but more importantly it retains resolution of major local features in the state vector while smoothing weak and broad features.

Turner, A. J.↗
DOE OSTI2015

Estimating global and North American methane emissions with high spatial resolution using GOSAT satellite data

We use 2009–2011 space-borne methane observations from the Greenhouse Gases Observing SATellite (GOSAT) to estimate global and North American methane emissions with 4° × 5° and up to 50 km × 50 km spatial resolution, respectively. GEOS-Chem and GOSAT data are first evaluated with atmospheric methane observations from surface and tower networks (NOAA/ESRL, TCCON) and aircraft (NOAA/ESRL, HIPPO), using the GEOS-Chem chemical transport model as a platform to facilitate comparison of GOSAT with in situ data. This identifies a high-latitude bias between the GOSAT data and GEOS-Chem that we correct via quadratic regression. Our global adjoint-based inversion yields a total methane source of 539 Tg a −1 with some important regional corrections to the EDGARv4.2 inventory used as a prior. Results serve as dynamic boundary conditions for an analytical inversion of North American methane emissions using radial basis functions to achieve high resolution of large sources and provide error characterization. We infer a US anthropogenic methane source of 40.2–42.7 Tg a −1 , as compared to 24.9–27.0 Tg a −1 in the EDGAR and EPA bottom-up inventories, and 30.0–44.5 Tg a −1 in recent inverse studies. Our estimate is supported by independent surface and aircraft data and by previous inverse studies for California. We find that the emissions are highest in the southern–central US, the Central Valley of California, and Florida wetlands; large isolated point sources such as the US Four Corners also contribute. Using prior information on source locations, we attribute 29–44 % of US anthropogenic methane emissions to livestock, 22–31 % to oil/gas, 20 % to landfills/wastewater, and 11–15 % to coal. Wetlands contribute an additional 9.0–10.1 Tg a −1 .

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2015

Development of a Grid-Independent Geos-Chem Chemical Transport Model (v9-02) as an Atmospheric Chemistry Module for Earth System Models

The GEOS-Chem global chemical transport model (CTM), used by a large atmospheric chemistry research community, has been re-engineered to also serve as an atmospheric chemistry module for Earth system models (ESMs). This was done using an Earth System Modeling Framework (ESMF) interface that operates independently of the GEOSChem scientific code, permitting the exact same GEOSChem code to be used as an ESM module or as a standalone CTM. In this manner, the continual stream of updates contributed by the CTM user community is automatically passed on to the ESM module, which remains state of science and referenced to the latest version of the standard GEOS-Chem CTM. A major step in this re-engineering was to make GEOS-Chem grid independent, i.e., capable of using any geophysical grid specified at run time. GEOS-Chem data sockets were also created for communication between modules and with external ESM code. The grid-independent, ESMF-compatible GEOS-Chem is now the standard version of the GEOS-Chem CTM. It has been implemented as an atmospheric chemistry module into the NASA GEOS- 5 ESM. The coupled GEOS-5-GEOS-Chem system was tested for scalability and performance with a tropospheric oxidant-aerosol simulation (120 coupled species, 66 transported tracers) using 48-240 cores and message-passing interface (MPI) distributed-memory parallelization. Numerical experiments demonstrate that the GEOS-Chem chemistry module scales efficiently for the number of cores tested, with no degradation as the number of cores increases. Although inclusion of atmospheric chemistry in ESMs is computationally expensive, the excellent scalability of the chemistry module means that the relative cost goes down with increasing number of cores in a massively parallel environment.

CTM↗
NASA NTRS2014

HEMCO v1.0: A Versatile, ESMF-Compliant Component for Calculating Emissions in Atmospheric Models

We describe the Harvard-NASA Emission Component version 1.0 (HEMCO), a stand-alone software component for computing emissions in global atmospheric models. HEMCO determines emissions from different sources, regions, and species on a user-defined grid and can combine, overlay, and update a set of data inventories and scale factors, as specified by the user through the HEMCO configuration file. New emission inventories at any spatial and temporal resolution are readily added to HEMCO and can be accessed by the user without any preprocessing of the data files or modification of the source code. Emissions that depend on dynamic source types and local environmental variables such as wind speed or surface temperature are calculated in separate HEMCO extensions. HEMCO is fully compliant with the Earth System Modeling Framework (ESMF) environment. It is highly portable and can be deployed in a new model environment with only few adjustments at the top-level interface. So far, we have implemented HEMCO in the NASA Goddard Earth Observing System (GEOS-5) Earth system model (ESM) and in the GEOS-Chem chemical transport model (CTM). By providing a widely applicable framework for specifying constituent emissions, HEMCO is designed to ease sensitivity studies and model comparisons, as well as inverse modeling in which emissions are adjusted iteratively. The HEMCO code, extensions, and the full set of emissions data files used in GEOS-Chem are available at http: //wiki.geos-chem.org/HEMCO.

GEOS-5↗
NASA NTRS2012

The United States' Next Generation of Atmospheric Composition and Coastal Ecosystem Measurements: NASA's Geostationary Coastal and Air Pollution Events (GEO-CAPE) Mission

The Geostationary Coastal and Air Pollution Events (GEO-CAPE) mission was recommended by the National Research Council's (NRC's) Earth Science Decadal Survey to measure tropospheric trace gases and aerosols and coastal ocean phytoplankton, water quality, and biogeochemistry from geostationary orbit, providing continuous observations within the field of view. To fulfill the mandate and address the challenge put forth by the NRC, two GEO-CAPE Science Working Groups (SWGs), representing the atmospheric composition and ocean color disciplines, have developed realistic science objectives using input drawn from several community workshops. The GEO-CAPE mission will take advantage of this revolutionary advance in temporal frequency for both of these disciplines. Multiple observations per day are required to explore the physical, chemical, and dynamical processes that determine tropospheric composition and air quality over spatial scales ranging from urban to continental, and over temporal scales ranging from diurnal to seasonal. Likewise, high-frequency satellite observations are critical to studying and quantifying biological, chemical, and physical processes within the coastal ocean. These observations are to be achieved from a vantage point near 95deg-100degW, providing a complete view of North America as well as the adjacent oceans. The SWGs have also endorsed the concept of phased implementation using commercial satellites to reduce mission risk and cost. GEO-CAPE will join the global constellation of geostationary atmospheric chemistry and coastal ocean color sensors planned to be in orbit in the 2020 time frame.

Atmospheric composition↗
NASA NTRS2012

Tropospheric Bromine Chemistry: Implications for Present and Pre-industrial Ozone and Mercury

We present a new model for the global tropospheric chemistry of inorganic bromine (Bry) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Bry include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone mixing ratios by <1-8 nmol/mol (6.5% globally), with the largest effects in the northern extratropics in spring. The global mean tropospheric OH concentration decreases by 4 %. Inclusion of bromine chemistry improves the ability of global models (GEOS-Chem and p-TOMCAT) to simulate observed 19th-century ozone and its seasonality. Bromine effects on tropospheric ozone are comparable in the present-day and pre-industrial atmospheres so that estimates of anthropogenic radiative forcing are minimally affected. Br atom concentrations are 40% higher in the pre-industrial atmosphere due to lower ozone, which would decrease by a factor of 2 the atmospheric lifetime of elemental mercury against oxidation by Br. This suggests that historical anthropogenic mercury emissions may have mostly deposited to northern mid-latitudes, enriching the corresponding surface reservoirs. The persistent rise in background surface ozone at northern mid-latitudes during the past decades could possibly contribute to the observations of elevated mercury in subsurface waters of the North Atlantic.

bromine↗
NASA NTRS2012

Climatic Effects of 1950-2050 Changes in US Anthropogenic Aerosols: Aerosol Trends and Radiative Forcing - Part 1

We calculate decadal aerosol direct and indirect (warm cloud) radiative forcings from US anthropogenic sources over the 1950-2050 period. Past and future aerosol distributions are constructed using GEOS-Chem and historical emission inventories and future projections from the IPCC A1B scenario. Aerosol simulations are evaluated with observed spatial distributions and 1980-2010 trends of aerosol concentrations and wet deposition in the contiguous US. Direct and indirect radiative forcing is calculated using the GISS general circulation model and monthly mean aerosol distributions from GEOS-Chem. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that its magnitude peaked in 1970-1990, with values over the eastern US (east of 100 deg W) of −2.0Wm(exp−2 for direct forcing including contributions from sulfate (−2.0Wm−2), nitrate (−0.2Wm(exp−2), organic carbon (−0.2Wm(exp−2), and black carbon (+0.4Wm(exp−2). The uncertainties in radiative forcing due to aerosol radiative properties are estimated to be about 50 %. The aerosol indirect effect is estimated to be of comparable magnitude to the direct forcing. We find that the magnitude of the forcing declined sharply from 1990 to 2010 (by 0.8Wm(exp−2) direct and 1.0Wm(exp−2 indirect), mainly reflecting decreases in SO2 emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO2 emissions have already declined by almost 60% from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources has already been realized. The small positive radiative forcing from US BC emissions (+0.3Wm(exp−2 over the eastern US in 2010; 5% of the global forcing from anthropogenic BC emissions worldwide) suggests that a US emission control strategy focused on BC would have only limited climate benefit.

climate change↗
NASA NTRS2012

Regional Warming from Aerosol Removal over the United States: Results from a Transient 2010-2050 Climate Simulation

We use a general circulation model (NASA Goddard Institute for Space Studies GCM 3) to investigate the regional climate response to removal of aerosols over the United States. We perform a pair of transient 2010e2050 climate simulations following a scenario of increasing greenhouse gas concentrations, with and without aerosols over the United States and with present-day aerosols elsewhere. We find that removing U.S. aerosol significantly enhances the warming from greenhouse gases in a spatial pattern that strongly correlates with that of the aerosol. Warming is nearly negligible outside the United States, but annual mean surface temperatures increase by 0.4e0.6 K in the eastern United States. Temperatures during summer heat waves in the Northeast rise by as much as 1e2 K due to aerosol removal, driven in part by positive feedbacks involving soil moisture and low cloud cover. Reducing U.S. aerosol sources to achieve air quality objectives could thus have significant unintended regional warming consequences.

Mickley, L. J.↗
NASA NTRS2011

Magnitude and Seasonality of Wetland Methane Emissions from the Hudson Bay Lowlands (Canada)

The Hudson Bay Lowlands (HBL) is the second largest boreal wetland ecosystem in the world and an important natural source of global atmospheric methane. We quantify the HBL methane emissions by using the GEOS-Chem chemical transport model to simulate aircraft measurements over the HBL from the ARCTAS and pre-HIPPO campaigns in May-July 2008, together with continuous 2004-2008 surface observations at Fraserdale (southern edge of HBL) and Alert (Arctic background). The difference in methane concentrations between Fraserdale and Alert is shown to be a good indicator of HBL emissions, and implies a sharp seasonal onset of emissions in late May (consistent with the aircraft data), a peak in July-August, and a seasonal shut-off in September. The model, in which seasonal variation of emission is mainly driven by surface temperature, reproduces well the observations in summer but its seasonal shoulders are too broad. We suggest that this reflects the suppression of emissions by snow cover and greatly improve the model simulation by accounting for this effect. Our resulting best estimate for HBL methane emissions is 2.3 Tg/a, several-fold higher than previous estimates (Roulet et al., 1994; Worthy et al., 2000).

Pickett-Heaps, C. A.↗
NASA NTRS2009

Source Attribution and Interannual Variability of Arctic Pollution in Spring Constrained by Aircraft (ARCTAS, ARCPAC) and Satellite (AIRS) Observations of Carbon Monoxide

We use aircraft observations of carbon monoxide (CO) from the NASA ARCTAS and NOAA ARCPAC campaigns in April 2008 together with multiyear (2003-2008) CO satellite data from the AIRS instrument and a global chemical transport model (GEOS-Chem) to better understand the sources, transport, and interannual variability of pollution in the Arctic in spring. Model simulation of the aircraft data gives best estimates of CO emissions in April 2008 of 26 Tg month-1 for Asian anthropogenic, 9.1 for European anthropogenic, 4.2 for North American anthropogenic, 9.3 for Russian biomass burning (anomalously large that year), and 21 for Southeast Asian biomass burning. We find that Asian anthropogenic emissions are the dominant source of Arctic CO pollution everywhere except in surface air where European anthropogenic emissions are of similar importance. Synoptic pollution influences in the Arctic free troposphere include contributions of comparable magnitude from Russian biomass burning and from North American, European, and Asian anthropogenic sources. European pollution dominates synoptic variability near the surface. Analysis of two pollution events sampled by the aircraft demonstrates that AIRS is capable of observing pollution transport to the Arctic in the mid-troposphere. The 2003-2008 record of CO from AIRS shows that interannual variability averaged over the Arctic cap is very small. AIRS CO columns over Alaska are highly correlated with the Ocean Nino Index, suggesting a link between El Nino and northward pollution transport. AIRS shows lower-than-average CO columns over Alaska during April 2008, despite the Russian fires, due to a weakened Aleutian Low hindering transport from Asia and associated with the moderate 2007-2008 La Nina. This suggests that Asian pollution influence over the Arctic may be particularly large under strong El Nino conditions.

Fisher, J. A.↗
NASA NTRS2004

Satellite Mapping of Rain-Induced Nitric Oxide Emissions from Soils

We use space-based observations of NO2 columns from the Global Ozone Monitoring Experiment (GOME) to map the spatial and seasonal variations of NOx emissions over Africa during 2000. The GOME observations show not only enhanced tropospheric NO2 columns from biomass burning during the dry season but also comparable enhancements from soil emissions during the rainy season over the Sahel. These soil emissions occur in strong pulses lasting 1-3 weeks following the onset of rain, and affect 3 million sq km of semiarid sub-Saharan savanna. Surface observations of NO2 from the International Global Atmospheric Chemistry (IGAC)/Deposition of Biochemically Important Trace Species (DEBITS)/Africa (IDAF) network over West Africa provide further evidence for a strong role for microbial soil sources. By combining inverse modeling of GOME NO2 columns with space-based observations of fires, we estimate that soils contribute 3.3+/-1.8 TgN/year, similar to the biomass burning source (3.8+/-2.1 TgN/year), and thus account for 40% of surface NO(x) emissions over Africa. Extrapolating to all the tropics, we estimate a 7.3 TgN/year biogenic soil source, which is a factor of 2 larger compared to model-based inventories but agrees with observation-based inventories. These large soil NO(x) emissions are likely to significantly contribute to the ozone enhancement originating from tropical Africa.

Jaegle, L.↗
NASA NTRS2004

Analysis of the Atmospheric Distribution, Sources, and Sinks of Oxygenated Volatile Organic Chemicals Based on Measurements over the Pacific during TRACE-P

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.

Singh, H. B.↗
NASA NTRS2004

Characterization of Transport Errors in Chemical Forecasts from a Global Tropospheric Chemical Transport Model

We propose a new methodology to characterize errors in the representation of transport processes in chemical transport models. We constrain the evaluation of a global three-dimensional chemical transport model (GEOS-CHEM) with an extended dataset of carbon monoxide (CO) concentrations obtained during the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft campaign. The TRACEP mission took place over the western Pacific, a region frequently impacted by continental outflow associated with different synoptic-scale weather systems (such as cold fronts) and deep convection, and thus provides a valuable dataset. for our analysis. Model simulations using both forecast and assimilated meteorology are examined. Background CO concentrations are computed as a function of latitude and altitude and subsequently subtracted from both the observed and the model datasets to focus on the ability of the model to simulate variability on a synoptic scale. Different sampling strategies (i.e., spatial displacement and smoothing) are applied along the flight tracks to search for systematic model biases. Statistical quantities such as correlation coefficient and centered root-mean-square difference are computed between the simulated and the observed fields and are further inter-compared using Taylor diagrams. We find no systematic bias in the model for the TRACE-P region when we consider the entire dataset (i.e., from the surface to 12 km ). This result indicates that the transport error in our model is globally unbiased, which has important implications for using the model to conduct inverse modeling studies. Using the First-Look assimilated meteorology only provides little improvement of the correlation, in comparison with the forecast meteorology. These general statements can be refined when the entire dataset is divided into different vertical domains, i.e., the lower troposphere (less than 2 km), the middle troposphere (2-6 km), and the upper troposphere (greater than 6 km). The best agreement between the observations and the model is found in the lower and middle troposphere. Downward displacements in the lower troposphere provide a better fit with the observed value, which could indicate a problem in the representation of boundary layer height in the model. Significant improvement is also found for downward and southward displacements in the upper troposphere. There are several potential sources of errors in our simulation of the continental outflow in the upper troposphere which could lead to such biases, including the location and/or the strength of deep convective cells as well as that of wildfires in Southeast Asia.

Bey, I.↗
NASA NTRS2004

Climate Response to the Increase in Tropospheric Ozone since Preindustrial Times: A Comparison between Ozone and Equivalent CO2 Forcings

We examine the characteristics of the climate response to anthropogenic changes in tropospheric ozone. Using a general circulation model, we have carried out a pair of equilibrium climate simulations with realistic present-day and preindustrial ozone distributions. We find that the instantaneous radiative forcing of 0.49 W m(sup -2) due to the increase in tropospheric ozone since preindustrial times results in an increase in global mean surface temperature of 0.28 C. The increase is nearly 0.4 C in the Northern Hemisphere and about 0.2 C in the Southern Hemisphere. The largest increases (greater than 0.8 C) are downwind of Europe and Asia and over the North American interior in summer. In the lower stratosphere, global mean temperatures decrease by about 0.2 C due to the diminished upward flux of radiation at 9.6 micrometers. The largest stratospheric cooling, up to 1.0 C, occurs over high northern latitudes in winter, with possibly important implications for the formation of polar stratospheric clouds. To identify the characteristics of climate forcing unique to tropospheric ozone, we have conducted two additional climate equilibrium simulations: one in which preindustrial tropospheric ozone concentrations were increased everywhere by 18 ppb, producing the same global radiative forcing as present-day ozone but without the heterogeneity; and one in which CO2 was decreased by 25 ppm relative to present day, with ozone at present-day values, to again produce the same global radiative forcing but with the spectral signature of CO2 rather than ozone. In the first simulation (uniform increase of ozone), the global mean surface temperature increases by 0.25 C, with an interhemispheric difference of only 0.03 C, as compared with nearly 0.2 C for the heterogeneous ozone increase. In the second simulation (equivalent CO2), the global mean surface temperature increases by 0.36 C, 30% higher than the increase from tropospheric ozone. The stronger surface warming from CO2 is in part because CO2 forcing (obscured by water vapor) is shifted relatively poleward where the positive ice-albedo feedback amplifies the climate response and in part because the magnitude of the CO2 forcing in the mid-troposphere is double that of ozone. However, we find that CO2 is far less effective than tropospheric ozone in driving lower stratospheric cooling at high northern latitudes in winter.

Mickley L. J.↗
NASA NTRS2003

Oxygenated Organic Chemicals in the Pacific Troposphere: Distribution, Sources and Chemistry

Airborne measurements of a large number of oxygenated organic chemicals (Oxorgs) were carried out in the Pacific troposphere (0.1-12 km) in the Spring of 2001 (Feb. 24-April 10). Specifically these measuremen ts included acetone, methylethyl ketone (MEK), methanol, ethanol, ace taldehyde, propionaldehyde, PANS, and organic nitrates. Complementary measurements of formaldehyde, organic peroxides, and tracers were al so available. Ox-orgs were abundant in the clean troposphere and were greatly enhanced in the outflow regions from Asia. Their mixing ratios were typically highest in the lower troposphere and declined toward s the upper troposphere and the lowermost stratosphere. Their total a bundance (Ox-orgs) significantly exceeded that of NMHC (C2-C8 NMHC). A comparison of these data with observations collected some seven yea rs earlier (Feb.-March, 1994), did not reveal any significant changes . Throughout the troposphere mixing ratios of Ox-orgs were strongly c orrelated with each other as well as with tracers of fossil and bioma sshiof'uel combustion. Analysis of the relative enhancement of selected Oxorgs with respect to CH3Cl and CO in twelve sampled plumes, origi nating from fires, is used to assess their primary and secondary sour ces from biomass combustion. The composition of these plumes also ind icates a large shift of reactive nitrogen into the PAN reservoir ther eby limiting ozone formation. The Harvard 3-D photochemical model, th at uses state of the art chemistry and source information, is used to compare simulated and observed mixing ratios of selected species. A 1 -D model is used to explore the chemistry of aldehydes. These results will be presented.

Singh, Hanwant B.↗