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Cohen, Ronald C.

Publications and source records attributed to Cohen, Ronald C..

A double peak in the seasonality of California's photosynthesis as observed from space

Solar-induced chlorophyll fluorescence (SIF) has been shown to be a powerful proxy for photosynthesis and gross primary productivity (GPP). The recently launched TROPOspheric Monitoring Instrument (TROPOMI) features the required spectral resolution and signal-to-noise ratio to retrieve SIF from space. Here, we present a downscaling method to obtain 500 m spatial resolution SIF over California. We report daily values based on a 14 d window. TROPOMI SIF data show a strong correspondence with daily GPP estimates at AmeriFlux sites across multiple ecosystems in California. We find a linear relationship between SIF and GPP that is largely invariant across ecosystems with an intercept that is not significantly different from zero. Measurements of SIF from TROPOMI agree with MODerate Resolution Imaging Spectroradiometer (MODIS) vegetation indices – the normalized difference vegetation index (NDVI), enhanced vegetation index (EVI), and near-infrared reflectance of vegetation index (NIR$_v$) – at annual timescales but indicate different temporal dynamics at monthly and daily timescales. TROPOMI SIF data show a double peak in the seasonality of photosynthesis, a feature that is not present in the MODIS vegetation indices. The different seasonality in the vegetation indices may be due to a clear-sky bias in the vegetation indices, whereas previous work has shown SIF to have a low sensitivity to clouds and to detect the downregulation of photosynthesis even when plants appear green. We further decompose the spatiotemporal patterns in the SIF data based on land cover. The double peak in the seasonality of California's photosynthesis is due to two processes that are out of phase: grasses, chaparral, and oak savanna ecosystems show an April maximum, while evergreen forests peak in June. An empirical orthogonal function (EOF) analysis corroborates the phase offset and spatial patterns driving the double peak. The EOF analysis further indicates that two spatiotemporal patterns explain 84 % of the variability in the SIF data. Results shown here are promising for obtaining global GPP at sub-kilometer spatial scales and identifying the processes driving carbon uptake.

54 ENVIRONMENTAL SCIENCES↗

Estimating CO2 Emissions Using Real and Simulated Total Column Observations

Total column measurements of CO2 (XCO2) have been proposed as a possible way to estimate emissions from large urban regions. Using calculations from the Weather Research and Forecasting (WRF) model with a 1km emissions field, we investigate the viability of both real and proposed observing systems consisting of surface and/or column measurements for constraining emission sources of various types and sizes in the San Francisco Bay Area. We find that column observations are best suited for assessing enhancements downwind of very large emissions sources. For smaller sources (such as highways), in situ surface monitors are required to provide sufficient sensitivity. We explore methods for estimating emissions from the real and simulated observations.

Raheja, Garima↗

Estimating CO2 Emissions Using Real and Simulated Total Column XCO2 Observations

Rising atmospheric CO2 concentrations necessitate deeper understanding of urban sources and sinks. Various sensor technologies and data assimilation strategies can be used to determine short- and long-term atmospheric trends. We seek to find the optimal synthesis of various measurement types in order to characterizing different types of sources in an urban environment.

Raheja, Garima↗

Nitrogen Oxides in the Global Upper Troposphere: Interpreting Cloud-Sliced NO2 Observations from the OMI Satellite Instrument

Nitrogen oxides (NOx≡NO+NO2) in the upper troposphere (UT) have a large impact on global tropospheric ozone and OH (the main atmospheric oxidant). New cloud-sliced observations of UT NO2 at 450–280 hPa (∼6–9 km) from the Ozone Monitoring Instrument (OMI) produced by NASA and the Royal Netherlands Meteorological Institute (KNMI) provide global coverage to test our understanding of the factors controlling UT NOx. We find that these products offer useful information when averaged over coarse scales (20°×32°, seasonal), and that the NASA product is more consistent with aircraft observations of UT NO2. Correlation with Lightning Imaging Sensor (LIS) and Optical Transient Detector (OTD) satellite observations of lightning flash frequencies suggests that lightning is the dominant source of NOx to the upper troposphere except for extratropical latitudes in winter. The NO2 background in the absence of lightning is 10–20 pptv. We infer a global mean NOx yield of 280±80 moles per lightning flash, with no significant difference between the tropics and midlatitudes, and a global lightning NOx source of 5.9±1.7 Tg N a(exp −1). There is indication that the NOx yield per flash increases with lightning flash footprint and with flash energy.

Marais, Eloise A.↗

Southeast Atmosphere Studies: Learning from Model-Observation Syntheses

Concentrations of atmospheric trace species in the United States have changed dramatically over the past several decades in response to pollution control strategies, shifts in domestic energy policy and economics, and economic development (and resulting emission changes) elsewhere in the world. Reliable projections of the future atmosphere require models to not only accurately describe current atmospheric concentrations, but to do so by representing chemical, physical and biological processes with conceptual and quantitative fidelity. Only through incorporation of the processes controlling emissions and chemical mechanisms that represent the key transformations among reactive molecules can models reliably project the impacts of future policy, energy and climate scenarios. Efforts to properly identify and implement the fundamental and controlling mechanisms in atmospheric models benefit from intensive observation periods, during which collocated measurements of diverse, speciated chemicals in both the gas and condensed phases are obtained. The Southeast Atmosphere Studies (SAS, including SENEX, SOAS, NOMADSS and SEAC4RS) conducted during the summer of 2013 provided an unprecedented opportunity for the atmospheric modeling community to come together to evaluate, diagnose and improve the representation of fundamental climate and air quality processes in models of varying temporal and spatial scales. This paper is aimed at discussing progress in evaluating, diagnosing and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models. The effort focused primarily on model representation of fundamental atmospheric processes that are essential to the formation of ozone, secondary organic aerosol (SOA) and other trace species in the troposphere, with the ultimate goal of understanding the radiative impacts of these species in the southeast and elsewhere. Here we address questions surrounding four key themes: gas-phase chemistry, aerosol chemistry, regional climate and chemistry interactions, and natural and anthropogenic emissions. We expect this review to serve as a guidance for future modeling efforts.

atmospheric chemistry↗

Decadal Changes in Summertime Reactive Oxidized Nitrogen and Surface Ozone over the Southeast United States

Widespread efforts to abate ozone (O3) smog have significantly reduced emissions of nitrogen oxides (NOx) over the past 2 decades in the Southeast US, a place heavily influenced by both anthropogenic and biogenic emissions. How reactive nitrogen speciation responds to the reduction in NOx emissions in this region remains to be elucidated. Here we exploit aircraft measurements from ICARTT (International Consortium for Atmospheric Research on Transport and Transformation - July-August 2004), SENEX (Southeast Nexus - June-July 2013), and SEAC4RS (Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys - August-September 2013) and long-term ground measurement networks alongside a global chemistry-climate model to examine decadal changes in summertime reactive oxidized nitrogen (RON) and ozone over the Southeast US. We show that our model can reproduce the mean vertical profiles of major RON species and the total (NO (sub y)) in both 2004 and 2013. Among the major RON species, nitric acid (HNO3) is dominant (approximately 42-45 percent), followed by NOx (31 percent), total peroxy nitrates (Sigma PNs; 14 percent), and total alkyl nitrates (Sigma ANs; 9-12 percent) on a regional scale. We find that most RON species, including NOx, Sigma PNs, and HNO3, decline proportionally with decreasing NOx emissions in this region, leading to a similar decline in NO (sub y). This linear response might be in part due to the nearly constant summertime supply of biogenic VOC (Volatile Organic Compounds) emissions in this region. Our model captures the observed relative change in RON and surface ozone from 2004 to 2013. Model sensitivity tests indicate that further reductions of NOx emissions will lead to a continued decline in surface ozone and less frequent high-ozone events.

Li, Jingyi↗

Wintertime Overnight NOx Removal in a Southeastern United States Coal-Fired Power Plant Plume: A Model for Understanding Winter NOx Processing and Its Implications

Nitric oxide (NO) is emitted in large quantities from coal-burning power plants. During the day, the plumes from these sources are efficiently mixed into the boundary layer, while at night, they may remain concentrated due to limited vertical mixing during which they undergo horizontal fanning. At night, the degree to which NO is converted to HNO3 and therefore unable to participate in next-day ozone (O3) formation depends on the mixing rate of the plume, the composition of power plant emissions, and the composition of the background atmosphere. In this study, we use observed plume intercepts from the Wintertime INvestigation of Transport, Emissions and Reactivity (WINTER) campaign to test sensitivity of overnight NOx removal to the N2O5 loss rate constant, plume mixing rate, background O3, and background levels of volatile organic compounds using a 2-D box model of power plant plume transport and chemistry. The factor that exerted the greatest control over NOx removal was the loss rate constant of N2O5. At the lowest observed N2O5 loss rate constant, no other combination of conditions converts more than 10 percent of the initial NOx to HNO3. The other factors did not influence NOx removal to the same degree.

air quality↗

Why Do Models Overestimate Surface Ozone in the Southeast United States?

Ozone pollution in the Southeast US involves complex chemistry driven by emissions of anthropogenic nitrogen oxide radicals (NO(x) triple bond NO + NO2) and biogenic isoprene. Model estimates of surface ozone concentrations tend to be biased high in the region and this is of concern for designing effective emission control strategies to meet air quality standards. We use detailed chemical observations from the SEAC(exp 4)RS aircraft campaign in August and September 2013, interpreted with the GEOS-Chem chemical transport model at 0.25 deg x 0.3125 deg horizontal resolution, to better understand the factors controlling surface ozone in the Southeast US. We find that the National Emission Inventory (NEI) for NO(x) from the US Environmental Protection Agency (EPA) is too high. This finding is based on SEAC(exp 4)RS observations of NO(x) and its oxidation products, surface network observations of nitrate wet deposition fluxes, and OMI satellite observations of tropospheric NO2 columns. Our results indicate that NEI NO(x) emissions from mobile and industrial sources must be reduced by 30-60%, dependent on the assumption of the contribution by soil NO(x) emissions. Upper-tropospheric NO2 from lightning makes a large contribution to satellite observations of tropospheric NO2 that must be accounted for when using these data to estimate surface NO(x) emissions. We find that only half of isoprene oxidation proceeds by the high-NO(x) pathway to produce ozone; this fraction is only moderately sensitive to changes in NO(x) emissions because isoprene and NO(x) emissions are spatially segregated. GEOS-Chem with reduced NO(x) emissions provides an unbiased simulation of ozone observations from the aircraft and reproduces the observed ozone production efficiency in the boundary layer as derived from a regression of ozone and NO(x) oxidation products. However, the model is still biased high by 6 plus or minus 14 ppb relative to observed surface ozone in the Southeast US. Ozonesondes launched during midday hours show a 7 ppb ozone decrease from 1.5 km to the surface that GEOS-Chem does not capture. This bias may reflect a combination of excessive vertical mixing and net ozone production in the model boundary layer.

Oxidation↗

HOx Observation and Model Comparison During INTEX-A 2004

OH and HO2 were measured with the Airborne Tropospheric Hydrogen Oxides Sensor (ATHOS) as part of a large measurement suite from the NASA DC-8 aircraft during the Intercontinental Chemical Transport Experiment - A (INTEX-A). This mission, which was conducted mainly over North America and the western Atlantic Ocean in summer 2004, was an excellent test of atmospheric oxidation chemistry. Throughout the troposphere, observed OH was generally 0.60 of the modeled OH; below 8 km, observed HO2 was generally 0.78 of modeled HO2. If the over-prediction of tropospheric OH is not due to an instrument calibration error, then it implied less global tropospheric oxidation capacity and longer lifetimes for gases like methane and methyl chloroform than currently thought. This discrepancy falls well outside uncertainties in both the OH measurement and rate coefficients for known reactions and points to a large unknown OH loss. If the modeled OH is forced to agree with observed values by introducing of an undefined OH loss that removed HOx (HOx=OH+HO2), the observed and modeled HO2 and HO2/OH ratios are largely reconciled within the measurement uncertainty. HO2 behavior above 8 km was markedly different. The observed-to-modeled ratio correlating with NO. The observed-to-modeled HO2 ratio increased from approximately 1 at 8 km to more than approximately 2.5 at 11 km with the observed-to-modeled ratio correlating with NO. The observed-to-modeled HO2 and NO were both considerably greater than observations from previous campaigns. In addition, the observed-to-modeled HO2/OH, which is sensitive to cycling reactions between OH and HO2, increased from approximately 1.2 at 8 km to almost 4 above 11 km. In contrast to the lower atmosphere, these discrepancies above 8 km suggest a large unknown HOx source and additional reactants that cycle HOx from OH to HO2. In the continental planetary boundary layer, the OH observed-to-modeled ratio increased from 0.6 when isoprene was less than 0.1 ppbv to over 3 when isoprene was greater than 2 ppbv, suggesting that forests throughout the United States are emitting unknown HOx sources. Progress in resolving these discrepancies requires further examinations of possible unknown OH sinks and HOx sources and a focused research activity devoted to ascertaining the accuracy of the OH and HO2 measurements.

Ren, Xinrong↗

The Role of Convection in Redistributing Formaldehyde to the Upper Troposphere Over North America and the North Atlantic during the Summer 2004 INTEX Campaign

Measurements of CH2O from a tunable diode laser absorption spectrometer (TDLAS) were acquired onboard the NASA DC-8 during the summer 2004 INTEX-NA (Intercontinental Chemical Transport Experiment - North America) campaign to test our understanding of convection and production mechanisms in the upper troposphere (UT, 6-12-km) over continental North America and the North Atlantic Ocean. Point-by-point comparisons with box model calculations, when MHP (CH3OOH) measurements were available for model constraint, resulted in a median CH2O measurement/model ratio of 0.91 in the UT. Multiple tracers were used to arrive at a set of UT CH2O background and perturbed air mass periods, and 46% of the TDLAS measurements fell within the latter category. At least 66% to 73% of these elevated UT observations were caused by enhanced production from CH2O precursors rather than direct transport of CH2O from the boundary layer. This distinction is important, since the effects from the former can last for over a week or more compared to one day or less in the case of convective transport of CH2O itself. In general, production of CH2O from CH4 was found to be the dominant source term, even in perturbed air masses. This was followed by production from MHP, methanol, PAN type compounds, and ketones, in descending order of their contribution. In the presence of elevated NO from lightning and potentially from the stratosphere, there was a definite trend in the CH2O discrepancy, which for the highest NO mixing ratios produced a median CH2O measurement/model ratio of 3.9 in the 10-12-km range. Discrepancies in CH2O and HO2 in the UT with NO were highly correlated and this provided further information as to the possible mechanism(s) responsible. These discrepancies with NO are consistent with additional production sources of both gases involving CH3O2 + NO reactions, most likely caused by unmeasured hydrocarbons.

Fried, Alan↗

Direct Measurements of the Convective Recycling of the Upper Troposphere

We present a statistical representation of the aggregate effects of deep convection on the chemistry and dynamics of the Upper Troposphere (UT) based on direct aircraft observations of the chemical composition of the UT over the Eastern United States and Canada during summer. These measurements provide new and unique observational constraints on the chemistry occurring downwind of convection and the rate at which air in the UT is recycled, previously only the province of model analyses. These results provide quantitative measures that can be used to evaluate global climate and chemistry models.

Bertram, Timothy H.↗

Surface and Lightning Sources of Nitrogen Oxides over the United States: Magnitudes, Chemical Evolution, and Outflow

We use observations from two aircraft during the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) campaign over the eastern United States and North Atlantic during summer 2004, interpreted with a global 3-D model of tropospheric chemistry (GEOS-Chem) to test current understanding of the regional sources, chemical evolution, and export of nitrogen oxides. The boundary layer NO(x) data provide top-down verification of a 50% decrease in power plant and industry NO(x) emissions over the eastern United States between 1999 and 2004. Observed 8-12 8 km NO(x) concentrations in ICARTT were 0.55 +/- 36 ppbv, much larger than in previous United States aircraft campaigns (ELCHEM, SUCCESS, SONEX). We show that regional lightning was the dominant source of this NO(x) and increased upper tropospheric ozone by 10 ppbv. Simulating the ICARTT upper tropospheric NO(x) observations with GEOS-Chem require a factor of 4 increase in the model NO(x) yield per flash (to 500 mol/flash). Observed OH concentrations were a factor of 2 lower than can be explained from current photochemical models, and if correct would imply a broader lightning influence in the upper troposphere than presently thought.An NO(y)-CO correlation analysis of the fraction f of North American NO(x) emissions vented to the free troposphere as NO(y) (sum of NO(x) and its oxidation products PAN and HNO3) s shows observed f=16+/-10 percent and modeled f=14 +/- 8 percent, consistent with previous studies. Export to the lower free troposphere is mostly HNO3 but at higher altitudes is mostly PAN. The model successfully simulates NO(y) export efficiency and speciation, supporting previous model estimates of a large U.S. contribution to tropospheric ozone through NO(x) and PAN export.

Hudman, Rynda C.↗

Evaluation of Space-Based Constraints on Global Nitrogen Oxide Emissions with Regional Aircraft Measurements over and Downwind of Eastern North America

We retrieve tropospheric nitrogen dioxide (NO 2) columns for May 2004 to April 2005 from the SCIAMACHY satellite instrument to derive top-down emissions of nitrogen oxides (NO(x) = NO + NO2) via inverse modeling with a global chemical transport model (GEOS-Chem). Simulated NO 2 vertical profiles used in the retrieval are evaluated with airborne measurements over and downwind of North America (ICARTT); a northern midlatitude lightning source of 1.6 Tg N/yr minimizes bias in the retrieval. Retrieved NO2 columns are validated (r2 = 0.60, slope = 0.82) with coincident airborne in situ measurements. The top-down emissions are combined with a priori information from a bottom-up emission inventory with error weighting to achieve an improved a posteriori estimate of the global distribution of surface NOx emissions. Our a posteriori NOx emission inventory for land surface NOx emissions (46.1 Tg N/yr) is 22% larger than the GEIA-based a priori bottom-up inventory for 1998, a difference that reflects rising anthropogenic emissions, especially from East Asia A posteriori NOx emissions for East Asia (9.8 Tg N/yr) exceed those from other continents. The a posteriori inventory improves the GEOS-Chem simulation of NOx, peroxyacetylnitrate, and nitric acid with respect to airborne in situ measurements over and downwind of New York City. The a posteriori is 7% larger than the EDGAR 3.2FT2000 global inventory, 3% larger than the NEI99 inventory for the United States, and 68% larger than a regional inventory for 2000 for eastern Asia. SCIAMACHY NO2 columns over the North Atlantic show a weak plume from lightning NO(x).

Martin, Randall V.↗

Assessment of the Effects of High-Speed Aircraft in the Stratosphere: 1998

This report assesses the potential atmospheric impacts of a proposed fleet of high-speed civil transport (HSCT) aircraft. The purpose of the report is to assess the effects of HSCT's on atmospheric composition and climate in order to provide a scientific basis for making technical, commercial, and environmental policy decisions regarding the HSCT fleet. The work summarized here was carried out as part of NASA's Atmospheric Effects of Aviation Project (a component of the High-Speed Research Program) as well as other NASA, U.S., and international research programs. The principal focus is on change in stratospheric ozone concentrations. The impact on climate change is also a concern. The report describes progress in understanding atmospheric processes, the current state of understanding of HSCT emissions, numerical model predictions of HSCT impacts, the principal uncertainties in atmospheric predictions, and the associated sensitivities in predicted effects of HSCT'S.

Kawa, S. Randolph↗

Assessment of the Effects of High-Speed Aircraft in the Stratosphere: 1998

This report assesses the potential atmospheric impacts of a proposed fleet of high-speed civil transport (HSCT) aircraft. The purpose of the report is to assess the effects of HSCT's on atmospheric composition and climate in order to provide a scientific basis for making technical, commercial, and environmental policy decisions regarding the HSCT fleet. The work summarized here was carried out as part of NASA's Atmospheric Effects of Aviation Project (a component of the High-Speed Research Program) as well as other NASA, U.S., and international research programs. The principal focus is on change in stratospheric ozone concentrations. The impact on climate change is also a concern. The report describes progress in understanding atmospheric processes, the current state of understanding of HSCT emissions, numerical model predictions of HSCT impacts, the principal uncertainties in atmospheric predictions, and the associated sensitivities in predicted effects of HSCT's.

Kawa, S. Randolph↗

Airborne Instruments for the In Situ Detection of ClONO2, NO2, ClO, and BrO in the Stratosphere

Design and construction of an in situ sensor for the detection of stratospheric ClONO2, ClO, BrO, and NO2, was conceived as a two-year program. The experiment has two novel components: a resistive silicon thermal dissociation heater used to fragment ClONO2 into ClO and NO2 and a laser-induced fluorescence sensor for N02. These two new components are integrated into an experiment that uses technology developed in our labs for the ER-2 ClO and ER-2 HO(X) instruments. During the first year we reconstructed our laboratory prototypes for ClONO2 and NO2 detection and made substantial improvements in the calibration apparatus. Results from these laboratory experiments have been used to refine the design of the flight instrument. During this year we began the design of all of the long-lead items required to produce a flight instrument: including the design and fabrication of the air flow system used to direct stratospheric air to our halogen sensors, design and prototyping of an aircraft-compatible thermal dissociation heater, and development and test of a new high powered laser system. Finally, we have designed and released for fabrication several subsystems.

Anderson, James G.↗