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SAFARI 2000 is an international regional science initiative being developed for Southern Africa to explore, study and address linkages between land-atmosphere processes and the relationship of biogenic, pyrogenic or anthropogenic emissions and the consequences of their deposition to the functioning of the biogeophysical and biogeochemical systems of southern Africa.
A comprehensive group of reactive nitrogen species (NO, NOz, HN03, HOzN02, PANs, alkyl nitrates, and aerosol-NO3) were measured over North America during July/August 2004 from the NASA DC-8 platform (0.1 - 12 km). Nitrogen containing tracers of biomass combustion (HCN and CH3CN) were also measured along with a host of other gaseous (CO, VOC, OVOC, halocarbon) and aerosol tracers. Clean background air as well as air with influences from biogenic emissions, anthropogenic pollution, biomass combustion, convection, lightning, and the stratosphere was sampled over the continental United States, the Atlantic, and the Pacific. The North American upper troposphere (UT) was found to be greatly influenced by both lightning NO, and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NO,. Observational data suggest that lightning was a far greater contributor to NO, in the UT than previously believed. PAN provided a dominant reservoir of reactive nitrogen in the UT while nitric acid dominated in the lower troposphere (LT). Peroxynitric acid (H02N02) was present in sizable concentrations peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the LT. Plumes from Alaskan fires contained large amounts of PAN and aerosol nitrate but little enhancement in ozone. A comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. We investigate the partitioning and interplay of the reactive nitrogen species within characteristic air masses and further examine their role in ozone formation.
A comprehensive group of reactive nitrogen species (NO, NO2, HNO3, HO2NO2, PANs, alkyl nitrates, and aerosol-NO3) were measured in the troposphere and lowermost stratosphere over North America and the Atlantic during July/August 2004 (INTEX-A) from the NASA DC-8 platform (0.1-12 km). Less reactive nitrogen species (HCN and CH3CN), that are also unique tracers of biomass combustion, were also measured along with a host of other gaseous (CO, VOC, OVOC, halocarbon) and aerosol tracers. Clean background air as well as air with influences from biogenic emissions, anthropogenic pollution, biomass combustion, and stratosphere was sampled both over continental U. S., Atlantic and Pacific. The North American upper troposphere was found to be greatly influenced by both lightning NO(x) and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NO(x). Under polluted conditions PAN was a dominant carrier of reactive nitrogen in the upper troposphere while nitric acid dominated in the lower troposphere. Peroxynitric acid (HO2NO2) was present in sizable concentrations always peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the lower troposphere. Plumes from Alaskan fires contained large amounts of PAN and very little enhancement in ozone. Observational data suggest that lightning was a far greater contributor to NO(x) in the upper troposphere than previously believed. NO(x) and NO(y) reservoir appeared to be in steady state only in the middle troposphere where NO(x)/NO(y) was independent of air mass age. A first comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. These uncertainties likely propagate themselves in satellites derived NOx data. Observed data are interpreted to suggest that soil sinks of HCN/CH3CN are at best very small. We investigate the partitioning and interplay of the reactive nitrogen species within characteristic air masses and further examine their role in ozone formation.
A unified tropospheric chemistry-aerosol model within the Goddard Institute for Space Studies general circulation model II is applied to simulate an equilibrium CO2-forced climate in the year 2100 to examine the effects of climate change on global distributions of tropospheric ozone and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols. The year 2100 CO2 concentration as well as the anthropogenic emissions of ozone precursors and aerosols/aerosol precursors are based on the Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios (SRES) A2. Year 2100 global O3 and aerosol burdens predicted with changes in both climate and emissions are generally 5-20% lower than those simulated with changes in emissions alone; as exceptions, the nitrate burden is 38% lower, and the secondary organic aerosol burden is 17% higher. Although the CO2-driven climate change alone is predicted to reduce the global O3 concentrations over or near populated and biomass burning areas because of slower transport, enhanced biogenic hydrocarbon emissions, decomposition of peroxyacetyl nitrate at higher temperatures, and the increase of O3 production by increased water vapor at high NOx levels. The warmer climate influences aerosol burdens by increasing aerosol wet deposition, altering climate-sensitive emissions, and shifting aerosol thermodynamic equilibrium. Climate change affects the estimates of the year 2100 direct radiative forcing as a result of the climate-induced changes in burdens and different climatological conditions; with full gas-aerosol coupling and accounting for ozone and direct radiative forcings by the O2, sulfate, nitrate, black carbon, and organic carbon are predicted to be +0.93, -0.72, -1.0, +1.26, and -0.56 W m(exp -2), respectively, using present-day climate and year 2100 emissions, while they are predicted to be +0.76, -0.72, 0.74, +0.97, and -0.58 W m(exp -2), respectively, with year 2100 climate and emissions.
In the lowermost layer of the atmosphere - the troposphere - ozone is an important source of the hydroxyl radical, an oxidant that breaks down most pollutants and some greenhouse gases. High concentrations of tropospheric ozone are toxic, however, and have a detrimental effect on human health and ecosystem productivity1. Moreover, tropospheric ozone itself acts as an effective greenhouse gas. Much of the present tropospheric ozone burden is a consequence of anthropogenic emissions of ozone precursors resulting in widespread increases in ozone concentrations since the late 1800s. At present, east Asia has the fastest-growing ozone precursor emissions. Much of the springtime east Asian pollution is exported eastwards towards western North America. Despite evidence that the exported Asian pollution produces ozone, no previous study has found a significant increase in free tropospheric ozone concentrations above the western USA since measurements began in the late 1970s. Here we compile springtime ozone measurements from many different platforms across western North America. We show a strong increase in springtime ozone mixing ratios during 1995-2008 and we have some additional evidence that a similar rate of increase in ozone mixing ratio has occurred since 1984. We find that the rate of increase in ozone mixing ratio is greatest when measurements are more heavily influenced by direct transport from Asia. Our result agrees with previous modelling studies, which indicate that global ozone concentrations should be increasing during the early part of the twenty-first century as a result of increasing precursor emissions, especially at northern mid-latitudes, with western North America being particularly sensitive to rising Asian emissions. We suggest that the observed increase in springtime background ozone mixing ratio may hinder the USA s compliance with its ozone air quality standard.
The Geostationary Fourier Transform Spectrometer (GeoFTS) is an imaging spectrometer designed for an earth science mission to measure key atmospheric trace gases and process tracers related to climate change and human activity. The GeoFTS instrument is a half meter cube size instrument designed to operate in geostationary orbit as a secondary "hosted" payload on a commercial geostationary satellite mission. The advantage of GEO is the ability to continuously stare at a region of the earth, enabling frequent sampling to capture the diurnal variability of biogenic fluxes and anthropogenic emissions from city to continental scales. The science goal is to obtain a process-based understanding of the carbon cycle from simultaneous high spatial resolution measurements of carbon dioxide (CO2), methane (CH4), carbon monoxide (CO), and chlorophyll fluorescence (CF) many times per day in the near infrared spectral region to capture their spatial and temporal variations on diurnal, synoptic, seasonal and interannual time scales. The GeoFTS instrument is based on a Michelson interferometer design with a number of advanced features incorporated. Two of the most important advanced features are the focal plane arrays and the optical path difference mechanism. A breadboard GeoFTS instrument has demonstrated functionality for simultaneous measurements in the visible and IR in the laboratory and subsequently in the field at the California Laboratory for Atmospheric Remote Sensing (CLARS) observatory on Mt. Wilson overlooking the Los Angeles basin. A GeoFTS engineering model instrument is being developed which will make simultaneous visible and IR measurements under space flight like environmental conditions (thermal-vacuum at 180 K). This will demonstrate critical instrument capabilities such as optical alignment stability, interferometer modulation efficiency, and high throughput FPA signal processing. This will reduce flight instrument development risk and show that the GeoFTS design is mature and flight ready.
We describe a new algorithm to retrieve SO2 from satellite-measured hyperspectral radiances. We employ the principal component analysis technique in regions with no significant SO2 to capture radiance variability caused by both physical processes (e.g., Rayleigh and Raman scattering and ozone absorption) and measurement artifacts. We use the resulting principal components and SO2 Jacobians calculated with a radiative transfer model to directly estimate SO2 vertical column density in one step. Application to the Ozone Monitoring Instrument (OMI) radiance spectra in 310.5-340 nm demonstrates that this approach can greatly reduce biases in the operational OMI product and decrease the noise by a factor of 2, providing greater sensitivity to anthropogenic emissions. The new algorithm is fast, eliminates the need for instrument-specific radiance correction schemes, and can be easily adapted to other sensors. These attributes make it a promising technique for producing longterm, consistent SO2 records for air quality and climate research.
Aerosol variations and trends over different land and ocean regions during 1980-2009 are analyzed with the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model and observations from multiple satellite sensors and ground-based networks. Excluding time periods with large volcanic influences, the tendency of aerosol optical depth (AOD) and surface concentration over polluted land regions is consistent with the anthropogenic emission changes.The largest reduction occurs over Europe, and regions in North America and Russia also exhibit reductions. On the other hand, East Asia and South Asia show AOD increases, although relatively large amount of natural aerosols in Asia makes the total changes less directly connected to the pollutant emission trends. Over major dust source regions, model analysis indicates that the dust emissions over the Sahara and Sahel respond mainly to the near-surface wind speed, but over Central Asia they are largely influenced by ground wetness. The decreasing dust trend in the tropical North Atlantic is most closely associated with the decrease of Sahel dust emission and increase of precipitation over the tropical North Atlantic, likely driven by the sea surface temperature increase. Despite significant regional trends, the model-calculated global annual average AOD shows little changes over land and ocean in the past three decades, because opposite trends in different regions cancel each other in the global average. This highlights the need for regional-scale aerosol assessment, as the global average value conceals regional changes, and thus is not sufficient for assessing changes in aerosol loading.
We introduce our next generation algorithm to retrieve SO2 using radiance measurements from the Aura Ozone Monitoring Instrument (OMI). We employ a principal component analysis technique to analyze OMI radiance spectral in 310.5-340 nm acquired over regions with no significant SO2. The resulting principal components (PCs) capture radiance variability caused by both physical processes (e.g., Rayleigh and Raman scattering, and ozone absorption) and measurement artifacts, enabling us to account for these various interferences in SO2 retrievals. By fitting these PCs along with SO2 Jacobians calculated with a radiative transfer model to OMI-measured radiance spectra, we directly estimate SO2 vertical column density in one step. As compared with the previous generation operational OMSO2 PBL (Planetary Boundary Layer) SO2 product, our new algorithm greatly reduces unphysical biases and decreases the noise by a factor of two, providing greater sensitivity to anthropogenic emissions. The new algorithm is fast, eliminates the need for instrument-specific radiance correction schemes, and can be easily adapted to other sensors. These attributes make it a promising technique for producing long-term, consistent SO2 records for air quality and climate research. We have operationally implemented this new algorithm on OMI SIPS for producing the new generation standard OMI SO2 products.
Two recent papers have quantified long-term ozone (O3) changes observed at northernmidlatitude sites that are believed to represent baseline (here understood as representative of continental to hemispheric scales) conditions. Three chemistry-climate models (NCAR CAM-chem, GFDL-CM3, and GISS-E2-R) have calculated retrospective tropospheric O3 concentrations as part of the Atmospheric Chemistry and Climate Model Intercomparison Project and Coupled Model Intercomparison Project Phase 5 model intercomparisons. We present an approach for quantitative comparisons of model results with measurements for seasonally averaged O3 concentrations. There is considerable qualitative agreement between the measurements and the models, but there are also substantial and consistent quantitative disagreements. Most notably, models (1) overestimate absolute O3 mixing ratios, on average by approximately 5 to 17 ppbv in the year 2000, (2) capture only approximately 50% of O3 changes observed over the past five to six decades, and little of observed seasonal differences, and (3) capture approximately 25 to 45% of the rate of change of the long-term changes. These disagreements are significant enough to indicate that only limited confidence can be placed on estimates of present-day radiative forcing of tropospheric O3 derived from modeled historic concentration changes and on predicted future O3 concentrations. Evidently our understanding of tropospheric O3, or the incorporation of chemistry and transport processes into current chemical climate models, is incomplete. Modeled O3 trends approximately parallel estimated trends in anthropogenic emissions of NO(sub x), an important O3 precursor, while measured O3 changes increase more rapidly than these emission estimates.
Atmospheric mixing ratios of carbon dioxide (CO2) are largely controlled by anthropogenic emission sources and biospheric sources/sinks. Global biospheric fluxes of CO2 are controlled by complex processes facilitating the exchange of carbon between terrestrial ecosystems and the atmosphere. These processes which play a key role in these terrestrial ecosystem-atmosphere carbon exchanges are currently not fully understood, resulting in large uncertainties in the quantification of biospheric CO2 fluxes. Current models with these inherent deficiencies have difficulties simulating the global carbon cycle with high accuracy. We are developing a new modeling platform, GEOS-Chem-CASA by integrating the year-specific NASA-CASA (National Aeronautics and Space Administration - Carnegie Ames Stanford Approach) biosphere model with the GEOS-Chem (Goddard Earth Observation System-Chemistry) chemical transport model to improve the simulation of atmosphere-terrestrial ecosystem carbon exchange. We use NASA-CASA to explicitly represent the exchange of CO2 between terrestrial ecosystem and atmosphere by replacing the baseline GEOS-Chem land net CO2 flux and forest biomass burning CO2 emissions. We will present the estimation and evaluation of these "bottom-up" land CO2 fluxes, simulated atmospheric mixing ratios, and forest disturbance changes over the last decade. In addition, we will present our initial comparison of atmospheric column-mean dry air mole fraction of CO2 predicted by the model and those retrieved from NASA's OCO-2 (Orbiting Carbon Observatory-2) satellite instrument and model-predicted surface CO2 mixing ratios with global in situ observations. This evaluation is the first step necessary for our future work planned to constrain the estimates of biospheric carbon fluxes through "top-down" inverse modeling, which will improve our understanding of the processes controlling atmosphere-terrestrial ecosystem greenhouse gas exchanges, especially over regions which lack in situ observations.
In the past decades, significant efforts have been made to increase tropospheric ozone long-term monitoring. A large number of ground-based, airborne and space-borne instruments are currently providing valuable data to contribute to better understand tropospheric ozone budget and variability. Nonetheless, most of these instruments provide in-situ surface and column-integrated data, whereas vertically resolved measurements are still scarce. Besides ozonesondes and aircraft, lidar measurements have proven to be valuable tropospheric ozone profilers. Using the measurements from the tropospheric ozone differential absorption lidar (DIAL) located at the JPL Table Mountain Facility, California, and the GEOS-Chem and GEOS-5 model outputs, the impact of the North American monsoon on tropospheric ozone during summer 2014 is investigated. The influence of the Monsoon lightning-induced NOx will be evaluated against other sources (e.g. local anthropogenic emissions and the stratosphere) using also complementary data such as backward-trajectories analysis, coincident water vapor lidar measurements, and surface ozone in-situ measurements.
In 1959 the U.S. Army Corps of Engineers built Camp Century beneath the surface of the northwestern Greenland Ice Sheet. There they studied the feasibility of deploying ballistic missiles within the ice sheet. The base and its wastes were abandoned with minimal decommissioning in 1967, under the assumption they would be preserved for eternity by perpetually accumulating snowfall. Here we show that a transition in ice sheet surface mass balance at Camp Century from net accumulation to net ablation is plausible within the next 75years, under a business-as-usual anthropogenic emissions scenario (Representative Concentration Pathway 8.5). Net ablation would guarantee the eventual remobilization of physical, chemical, biological, and radiological wastes abandoned at the site. While Camp Century and four other contemporaneous ice sheet bases were legally established under a Danish-U.S. treaty, the potential remobilization of their abandoned wastes, previously regarded as sequestered, represents an entirely new pathway of political dispute resulting from climate change.
The Lulin Atmospheric Background Station (LABS, 23.47 deg. N 120.87 deg. E, 2862 m ASL) in Central Taiwan was constructed in 2006 and is the only high-altitude background station in the western Pacific region for studying the influence of continental outflow. In this study, extensive optical properties of aerosols, including the aerosol light scattering coefficient [Sigma(sub s)] and light absorption coefficient [Sigma(sub a)], were collected from 2013 to 2014. The intensive optical properties, including mass scattering efficiency [Sigma(sub s)], mass absorption efficiency [Sigma(sub a)] single scattering albedo (Omega), scattering Angstrom exponent (A), and backscattering fraction (b), were determined and investigated, and the distinct seasonal cycle was observed. The value of [Alpha(sub a)] began to increase in January and reached a maximum in April; the mean in spring was 5.89 m(exp. 2) g(exp. -1) with a standard deviation (SD) of 4.54 m(exp. 2) g(exp. -1) and a 4.48 m(exp. 2) g(exp. -1) interquartile range (IQR: 2.95-7.43 m(exp. 2) g(exp. -1). The trend was similar in [Sigma(sub a)], with a maximum in March and a monthly mean of 0.84 m(exp. 2) g(exp. -1). The peak values of Omega (Mean = 0.92, SD = 0.03, IQR: 0.90 - 0.93) and A (Mean = 2.22, SD = 0.61, IQR: 2.12 = 2.47) occurred in autumn. These annual patterns of optical properties were associated with different long-range transport patterns of air pollutants such as biomass burning (BB) aerosol in spring and potential anthropogenic emissions in autumn. The optical measurements performed at LABS during spring in 2013 were compared with those simultaneously performed at the Doi Ang Kang Meteorology Station, Chiang Mai Province, Thailand (DAK, 19.93 deg. N, 99.05 deg. E, 1536 m a.s.l.), which is located in the Southeast Asia BB source region. Furthermore, the relationships among [Sigma(sub s)], [Sigma(sub a)], and (b) were used to characterize the potential aerosol types transported to LABS during different seasons, and the data were inspected according to the HYSPLIT 5-day backward trajectories, which differentiate between different regions of air mass origin.
The extreme rate of evaporation of the Dead Sea (DS) has serious implications for the surrounding area, including atmospheric conditions. This study analyzes the aerosol properties over the western and eastern parts of the DS during the year 2013, using MAIAC (Multi-Angle Implementation of Atmospheric Correction) for MODIS, which retrieves aerosol optical depth (AOD) data at a resolution of 1km. The main goal of the study is to evaluate MAIAC over the study area and determine, for the first time, theprevailing aerosol spatial patterns. First, the MAIAC-derived AOD data was compared with data from three nearby AERONET sites (Nes Ziona - an urban site, and Sede Boker and Masada - two arid sites), and with the conventional Dark Target (DT) and Deep Blue (DB) retrievals for the same days and locations, on a monthly basis throughout 2013. For the urban site, the correlation coefficient (r) for DTDB products showed better performance than MAIAC (r = 0.80, 0.75, and 0.64 respectively) year-round. However, in the arid zones, MAIAC showed better correspondence to AERONET sites than the conventional retrievals (r = 0.58 - 0.60 and 0.48 - 0.50 respectively). We investigated the difference in AOD levels, and its variability, between the Dead Sea coasts on a seasonal basis and calculated monthlyseasonal AOD averages for presenting AOD patterns over arid zones. Thus, we demonstrated that aerosol concentrations show a strong preference for the western coast, particularly during the summer season. This preference, is most likely a result of local anthropogenic emissions combined with the typical seasonal synoptic conditions, the Mediterranean Sea breeze, and the region complex topography. Our results also indicate that a large industrial zone showed higher AOD levels compared to an adjacent reference-site, i.e., 13 percent during the winter season.
Atmospheric mixing ratios of carbon dioxide (CO2) are largely controlled by anthropogenic emissions and biospheric fluxes. The processes controlling terrestrial biosphere-atmosphere carbon exchange are currently not fully understood, resulting in terrestrial biospheric models having significant differences in the quantification of biospheric CO2 fluxes. Atmospheric transport models assimilating measured (in situ or space-borne) CO2 concentrations to estimate "top-down" fluxes, generally use these biospheric CO2 fluxes as a priori information. Most of the flux inversion estimates result in substantially different spatio-temporal posteriori estimates of regional and global biospheric CO2 fluxes. The Orbiting Carbon Observatory 2 (OCO-2) satellite mission dedicated to accurately measure column CO2 (XCO2) allows for an improved understanding of global biospheric CO2 fluxes. OCO-2 provides much-needed CO2 observations in data-limited regions facilitating better global and regional estimates of "top-down" CO2 fluxes through inversion model simulations. The specific objectives of our research are to: 1) conduct GEOS-Chem 4D-Var assimilation of OCO-2 observations, using several state-of-the-science biospheric CO2 flux models as a priori information, to better constrain terrestrial CO2 fluxes, and 2) quantify the impact of different biospheric model prior fluxes on OCO-2-assimilated a posteriori CO2 flux estimates. Here we present our assessment of the importance of these a priori fluxes by conducting Observing System Simulation Experiments (OSSE) using simulated OCO-2 observations with known "true" fluxes.
Methane is an important greenhouse gas, responsible for about 20 of the warming induced by long-lived greenhouse gases since pre-industrial times. By reacting with hydroxyl radicals, methane reduces the oxidizing capacity of the atmosphere and generates ozone in the troposphere. Although most sources and sinks of methane have been identified, their relative contributions to atmospheric methane levels are highly uncertain. As such, the factors responsible for the observed stabilization of atmospheric methane levels in the early 2000s, and the renewed rise after 2006, remain unclear. Here, we construct decadal budgets for methane sources and sinks between 1980 and 2010, using a combination of atmospheric measurements and results from chemical transport models, ecosystem models, climate chemistry models and inventories of anthropogenic emissions. The resultant budgets suggest that data-driven approaches and ecosystem models overestimate total natural emissions. We build three contrasting emission scenarios which differ in fossil fuel and microbial emissions to explain the decadal variability in atmospheric methane levels detected, here and in previous studies, since 1985. Although uncertainties in emission trends do not allow definitive conclusions to be drawn, we show that the observed stabilization of methane levels between 1999 and 2006 can potentially be explained by decreasing-to-stable fossil fuel emissions, combined with stable-to-increasing microbial emissions. We show that a rise in natural wetland emissions and fossil fuel emissions probably accounts for the renewed increase in global methane levels after 2006, although the relative contribution of these two sources remains uncertain.
Past studies have suggested that ozone in the troposphere has increased globally throughout much of the 20th century due to increases in anthropogenic emissions and transport. We show, by combining satellite measurements with a chemical transport model, that during the last four decades tropospheric ozone does indeed indicate increases that are global in nature, yet still highly regional. Satellite ozone measurements from Nimbus-7 and Earth Probe Total Ozone Mapping Spectrometer (TOMS) are merged with ozone measurements from the Aura Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) to determine trends in tropospheric ozone for 1979–2016. Both TOMS (1979–2005) and OMI/MLS (2005–2016) depict large increases in tropospheric ozone from the Near East to India and East Asia and further eastward over the Pacific Ocean. The 38-year merged satellite record shows total net change over this region of about +6 to +7 Dobson units (DU) (i.e., ∼15 %–20 % of average background ozone), with the largest increase (∼4 DU) occurring during the 2005–2016 Aura period. The Global Modeling Initiative (GMI) chemical transport model with time-varying emissions is used to aid in the interpretation of tropospheric ozone trends for 1980–2016. The GMI simulation for the combined record also depicts the greatest increases of +6 to +7 DU over India and East Asia, very similar to the satellite measurements. In regions of significant increases in tropospheric column ozone (TCO) the trends are a factor of 2–2.5 larger for the Aura record when compared to the earlier TOMS record; for India and East Asia the trends in TCO for both GMI and satellite measurements are ∼+3 DU decade(exp −1) or greater during 2005–2016 compared to about +1.2 to +1.4 DU decade(exp −1) for 1979–2005. The GMI simulation and satellite data also reveal a tropospheric ozone increases in ∼+4 to +5 DU for the 38-year record over central Africa and the tropical Atlantic Ocean. Both the GMI simulation and satellite-measured tropospheric ozone during the latter Aura time period show increases of ∼+3 DU decade−1 over the N Atlantic and NE Pacific.