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Prior to the SOLVE deployment, we modified and ran a chemical transport model (CTM) to set up a stratospheric climatology for 1 September 1999. During and immediately following the SOLVE deployments, we ran the model in near-real-time and used these results in conjunction with SOLVE observations to draw conclusions about stratospheric transport.
Mounting concern regarding the possibility that increasing carbon dioxide concentrations will initiate climate change has stimulated interest in the feasibility of measuring CO2 mixing ratios from satellites. Currently, the most comprehensive set of atmospheric CO2 data is from the NOAA CMDL cooperative air sampling network, consisting of more than 40 sites where flasks of air are collected approximately weekly. Sporadic observations in the troposphere and stratosphere from airborne in situ and flask samplers are also available. Although the surface network is extensive, there is a dearth of data in the Southern Hemisphere and most of the stations were intentionally placed in remote areas, far from major sources. Sufficiently precise satellite observations with adequate spatial and temporal resolution would substantially increase our knowledge of the atmospheric CO2 distribution and would undoubtedly lead to improved understanding of the global carbon budget. We use a 3-D chemical transport model to investigate the ability of potential satellite instruments with a variety of orbits, horizontal resolution and vertical weighting functions to capture the variation in the modeled CO2 fields. The model is driven by analyzed winds from the Goddard Data Assimilation Office. Simulated CO2 fields are compared with existing surface and aircraft data, and the effects of the model convection scheme and representation of the planetary boundary layer are considered.
We are in the process of developing a nadir-viewing, aircraft-based high spectral resolution lidar (HSRL) at NASA Langley Research Center. The system is designed to measure backscatter and extinction of aerosols and tenuous clouds. The primary uses of the instrument will be to validate spaceborne aerosol and cloud observations, carry out regional process studies, and assess the predictions of chemical transport models. In this paper, we provide an overview of the instrument design and present the results of simulations showing the instrument's capability to accurately measure extinction and extinction-to-backscatter ratio.
In recent years, data assimilation has become an indispensable tool for our understanding of the global features of meteorological variables. However, assessments of transport characteristics using trajectory related methods as well as chemical transport models (CTMs) show that results derived from assimilated (or analyzed) winds exhibit significantly larger mixing and entrainment rates compared to results derived from GCM winds, which are closer to results derived from observations (e.g., Douglass et al., 2002; Schoeberl et al., 2002). This discrepancy presents a serious challenge to our ability to understand and model global trace gas transport and distribution. We use the GEOS-DAS to explore this issue by examining how the process of data assimilation alters the dynamics of the underlying GCM and how this leads to the excess of lower stratospheric mixing and transport in the subtropics. In particular, we show that significant model biases in tropical winds necessitate large analysis increments. These increments directly force large subtropical regions of instability with negative PV gradient on the one hand, and generate excessive noise in the tropical wind fields on the other. The result is an excess of transport in the lower stratospheric subtropics.
Mounting concern regarding the possibility that increasing carbon dioxide concentrations will initiate climate change has stimulated interest in the feasibility of measuring CO2 mixing ratios from satellites. Currently, the most comprehensive set of atmospheric CO2 data is from the NOAA CMDL cooperative air sampling network, consisting of more than 40 sites where flasks of air are collected approximately weekly. Sporadic observations in the troposphere and stratosphere from airborne in situ and flask samplers are also available. Although the surface network is extensive, there is a dearth of data in the Southern Hemisphere and most of the stations were intentionally placed in remote areas, far from major sources. Sufficiently precise satellite observations with adequate spatial and temporal resolution would substantially increase our knowledge of the atmospheric CO2 distribution and would undoubtedly lead to improved understanding of the global carbon budget. We use a 3-D chemical transport model to investigate the ability of potential satellite instruments with a variety of orbits, horizontal resolution and vertical weighting functions to capture the variation in the modeled CO2 fields. The model is driven by analyzed winds from the Goddard Data Assimilation Office. Simulated CO2 fields are compared with existing surface and aircraft data, and the effects of the model convection scheme and representation of the planetary boundary layer are considered.
We present a methodology for estimating the seasonal and interannual variation of biomass burning designed for use in global chemical transport models. The average seasonal variation is estimated from 4 years of fire-count data from the Along Track Scanning Radiometer (ATSR) and 1-2 years of similar data from the Advanced Very High Resolution Radiometer (AVHRR) World Fire Atlases. We use the Total Ozone Mapping Spectrometer (TOMS) Aerosol Index (AI) data product as a surrogate to estimate interannual variability in biomass burning for six regions: Southeast Asia, Indonesia and Malaysia, Brazil, Central America and Mexico, Canada and Alaska, and Asiatic Russia. The AI data set is available from 1979 to the present with an interruption in satellite observations from mid-1993 to mid-1996; this data gap is filled where possible with estimates of area burned from the literature for different regions. Between August 1996 and July 2000, the ATSR fire-counts are used to provide specific locations of emissions and a record of interannual variability throughout the world. We use our methodology to estimate mean seasonal and interannual variations for emissions of carbon monoxide from biomass burning, and we find that no trend is apparent in these emissions over the last two decades, but that there is significant interannual variability.
The sources contributing to tropospheric ozone over the Asian Pacific Rim in different seasons are quantified by analysis of Hong Kong and Japanese ozonesonde observations with a global three-dimensional (3-D) chemical transport model (GEOS-CHEM) driven by assimilated meteorological observations. Particular focus is placed on the extensive observations available from Hong Kong in 1996. In the middle-upper troposphere (MT- UT), maximum Asian pollution influence along the Pacific Rim occurs in summer, reflecting rapid convective transport of surface pollution. In the lower troposphere (LT) the season of maximum Asian pollution influence shifts to summer at midlatitudes from fall at low latitudes due to monsoonal influence. The UT ozone minimum and high variability observed over Hong Kong in winter reflects frequent tropical intrusions alternating with stratospheric intrusions. Asian biomass burning makes a major contribution to ozone at less than 32 deg.N in spring. Maximum European pollution influence (less than 5 ppbv) occurs in spring in the LT. North American pollution influence exceeds European influence in the UT-MT, reflecting the uplift from convection and the warm conveyor belts over the eastern seaboard of North America. African outflow makes a major contribution to ozone in the low-latitude MT-UT over the Pacific Rim during November- April. Lightning influence over the Pacific Rim is minimum in summer due to westward UT transport at low latitudes associated with the Tibetan anticyclone. The Asian outflow flux of ozone to the Pacific is maximum in spring and fall and includes a major contribution from Asian anthropogenic sources year-round.
The UNH investigation during TRACE-P provided measurements of selected acidic gases and aerosol species aboard the NASA DC-8 research aircraft. Our investigation focused on measuring HNO3, SO2, and fine (less than 2 microns) aerosol SO4(sup 2-) with two minute time resolution in near-real-time. We also quantified mixing ratios of aerosol ionic species, and aerosol (210)Pb and (7)Be collected onto bulk filters at better than 10 minute resolution. This suite of measurements contributed extensively to achieving the principal objectives of TRACE-P. In the context of the full data set collected by experimental teams on the DC-8, our observations provide a solid basis for assessing decadal changes in the chemical composition and source strength of Asian continental outflow. This region of the Pacific should be impacted profoundly by Asian emissions at this time with significant degradation of air quality over the next few decades. Atmospheric measurements in the western Pacific region will provide a valuable time series to help quantify the impact of Asian anthropogenic activities. Our data also provide important insight into the chemical and physical processes transforming Asian outflow during transport over the Pacific, particularly uptake and reactions of soluble gases on aerosol particles. In addition, the TRACE-P data set provide strong constraints for assessing and improving the chemical fields simulated by chemical transport models.
During the period 12 July - 8 August 2004, the NASA Ames 14-channel Airborne Tracking Sunphotometer (MTS-14) and Solar Spectral Flux Radiometer (SSFR) were operated aboard a Jetstream 31 (J31) aircraft and acquired measurements during nineteen science flights (approx. 53 flight hours) over the Gulf of Maine in support of the INTEX-NA (INtercontinental chemical Transport Experiment-North America) and ITCT (Intercontinental Transport and Chemical Transformation of anthropogenic pollution) field studies. In this paper, we will present results from analyses of those data sets. AATS-14 measures the direct solar beam transmission at fourteen discrete wavelengths (354-2138 nm), and provides instantaneous measurements of aerosol optical depth (AOD) spectra and water vapor column content, in addition to vertical profiles of aerosol extinction and water vapor density during suitable aircraft ascents and descents. SSFR consists of separate nadir and zenith viewing hemispheric FOV sensors that yield measurements of up- and downwelling solar irradiance at a spectral resolution of approx. 8-12 nm over the wavelength range 300-1700 nm. The objectives of the J31-based measurements during INTEX/ITCT were to provide AOD data for the evaluation of MODIS (MODerate-resolution Imaging Spectroradiometer) and MISR (Multi-angle Imaging Spectro-Radiometer) AOD retrievals, quantify sea surface spectral albedo (which can contribute the largest uncertainty to satellite aerosol retrievals for low aerosol loading), test closure (consistency) among suborbital results, test chemical-transport models using AOD profiles, and assess regional radiative forcing by combining satellite and suborbital results. Specific J31 flight patterns were designed to achieve these objectives, and they included a mixture of vertical profiles (spiral and ramped ascents and descents) and constant altitude horizontal transects at a variety of altitudes. Additional information is included in the original extended abstract.
The Microwave Limb Sounder (MLS) on Aura is providing an extensive data set on stratospheric winter polar processing, including the first daily global observations of HCl, together with simultaneous measurements of ClO, HNO3, H2O, O3, N2O, and temperature (among others). We present first results charting the evolution of these quantities during the 2004 Antarctic late winter. MLS observations of chlorine deactivation and ozone loss during this period are shown to be consistent with results from the SLIMCAT chemical transport model.
We describe the operational algorithm for the retrieval of stratospheric, tropospheric, and total column densities of nitrogen dioxide NO2 from earthshine radiances measured by the Ozone Monitoring Instrument (OMI), aboard the EOS-Aura satellite. The algorithm uses the DOAS method for the retrieval of slant column NO densities. Air mass factors (AMFs) calculated from a stratospheric NO2 profile are used to make initial estimates of the vertical column density. Using data collected over a 24-h period, a smooth estimate of the global stratospheric field is constructed. Where the initial vertical column densities exceed the estimated stratospheric field, we infer the presence of tropospheric NO2, and recalculate the vertical column density (VCD) using an AMF calculated from an assumed tropospheric NO2 profile. The parameters that control the operational algorithm were selected with the aid of a set of data assembled from stratospheric and tropospheric chemical transport models. We apply the optimized algorithm to OMI data and present global maps of NO2 VCDs for the first time.
Satellite retrievals of the fine-mode fraction (FMF) of midvisible aerosol optical depth, tau, are potentially valuable for constraining chemical transport models and for assessing the global distribution of anthropogenic aerosols. Here we compare satellite retrievals of FMF from the Moderate Resolution Imaging Spectroradiometer (MODIS) to suborbital data on the submicrometer fraction (SMF) of tau. SMF is a closely related parameter that is directly measurable by in situ techniques. The primary suborbital method uses in situ profiling of SMF combined with airborne Sun photometry both to validate the in situ estimate of ambient extinction and to take into account the aerosol above the highest flight level. This method is independent of the satellite retrieval and has well-known accuracy but entails considerable logistical and technical difficulties. An alternate method uses Sun photometer measurements near the surface and an empirical relation between SMF and the Angstrom exponent, A, a measure of the wavelength dependence of optical depth or extinction. Eleven primary and fifteen alternate comparisons are examined involving varying mixtures of dust, sea salt, and pollution in the vicinity of Korea and Japan. MODIS ocean retrievals of FMF are shown to be systematically higher than suborbital estimates of SMF by about 0.2. The most significant cause of this discrepancy involves the relationship between 5 and fine-mode partitioning; in situ measurements indicate a systematically different relationship from what is assumed in the satellite retrievals. Based on these findings, we recommend: (1) satellite programs should concentrate on retrieving and validating since an excellent validation program is in place for doing this, and (2) suborbital measurements should be used to derive relationships between A and fine-mode partitioning to allow interpretation of the satellite data in terms of fine-mode aerosol optical depth.
We analyze aircraft observations obtained during INTEX-A (1 July 14 - August 2004) to examine the summertime influence of Asian pollution in the free troposphere over North America. By applying correlation analysis and Principal Component Analysis (PCA) to the observations between 6-12 km, we find dominant influences from recent convection and lightning (13 percent of observations), Asia (7 percent), the lower stratosphere (7 percent), and boreal forest fires (2 percent), with the remaining 71 percent assigned to background. Asian airmasses are marked by high levels of CO, O3, HCN, PAN, acetylene, benzene, methanol, and SO4(2-). The partitioning of reactive nitrogen species in the Asian plumes is dominated by peroxyacetyl nitrate (PAN) (approximately 600 pptv), with varying NO(x)/HNO3 ratios in individual plumes consistent with different plumes ages ranging from 3 to 9 days. Export of Asian pollution in warm conveyor belts of mid-latitude cyclones, deep convection, and lifting in typhoons all contributed to the five major Asian pollution plumes. Compared to past measurement campaigns of Asian outflow during spring, INTEX-A observations display unique characteristics: lower levels of anthropogenic pollutants (CO, propane, ethane, benzene) due to their shorter summer lifetimes; higher levels of biogenic tracers (methanol and acetone) because of a more active biosphere; as well as higher levels of PAN, NO(x), HNO3, and O3 (more active photochemistry possibly enhanced by injection of lightning NO(x)). The high delta O3/delta CO ratio (0.76 mol mol(exp -1)) of Asian plumes during INTEX-A is due to a combination of strong photochemical production and mixing with stratospheric air along isentropic surfaces. The GEOS-Chem global chemical transport model captures the timing and location of the Asian plumes remarkably well. However, it significantly underestimates the magnitude of the enhancements.
The chemical and dynamical processes governing the zonal variability of tropical tropospheric ozone and carbon monoxide are investigated for November 2004 using satellite observations, in-situ measurements, and chemical transport models in conjunction with inverse-estimated surface emissions. Vertical ozone profile estimates from the Tropospheric Emission Spectrometer (TES) and ozone sonde measurements from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network show the so called zonal 'wave-one' pattern, which is characterized by peak ozone concentrations (70-80 ppb) centered over the Atlantic, as well as elevated concentrations of ozone over Indonesia and Australia (60-70 ppb) in the lower troposphere. Observational evidence from TES CO vertical profiles and Ozone Monitoring Instrument (OMI) NO2 columns point to regional surface emissions as an important contributor to the elevated ozone over Indonesia. This contribution is investigated with the GEOS-Chem chemistry and transport model using surface emission estimates derived from an optimal inverse model, which was constrained by TES and Measurements Of Pollution In The Troposphere (MOPITT) CO profiles (Jones et al., 2007). These a posteriori estimates, which were over a factor of 2 greater than climatological emissions, reduced differences between GEOS-Chem and TES ozone observations by 30-40% and led to changes in GEOS-Chem upper tropospheric ozone of up to 40% over Indonesia. The remaining residual differences can be explained in part by upper tropospheric ozone produced from lightning NOx in the South Atlantic. Furthermore, model simulations from GEOS-Chem indicate that ozone over Indonesian/Australian is more sensitive to changes in surface emissions of NOx than ozone over the tropical Atlantic.
Concurrent (August 2006) measurements of tropospheric NO2 columns from OMI aboard Aura (1330 local overpass time) and SCIAMACHY aboard Envisat (1000 local overpass time) offer an opportunity to examine the consistency between the two instruments under tropospheric background conditions and the effect of different observing times. For scenes with tropospheric NO 2 columns <5.0 x 10(exp 15) molecules cm 2, SCIAMACHY and OMI agree within 1.0-2.0 x 10(exp 15) molecules cm 2, consistent with the detection limits of both instruments. We find evidence for a low bias of 0.2 x 10(exp 15) molecules cm 2 in OMI observations over remote oceans. Over the fossil fuel source regions at northern midlatitudes, we find that SCIAMACHY observes up to 40% higher NO2 at 1000 local time (LT) than OMI at 1330 LT. Over biomass burning regions in the tropics, SCIAMACHY observes up to 40% lower NO 2 columns than OMI. These differences are present in the spectral fitting of the data (slant column) and are augmented in the fossil fuel regions and dampened in the tropical biomass burning regions by the expected increase in air mass factor as the mixing depth rises from 1000 to 1330 LT. Using a global 3-D chemical transport model (GEOS-Chem), we show that the 1000-1330 LT decrease in tropospheric NO2 column over fossil fuel source regions can be explained by photochemical loss, dampened by the diurnal cycle of anthropogenic emissions that has a broad daytime maximum. The observed 1000-1330 LT NO2 column increase over tropical biomass burning regions points to a sharp midday peak in emissions and is consistent with a diurnal cycle of emissions derived from geostationary satellite fire counts.
.We interpret observations of trace-gases from three satellite platforms to provide top-down constraints on the production of NO by lightning. The space-based observations are tropospheric NO2 columns from SCIAMACHY, tropospheric O3 columns from OMI and MLS, and upper tropospheric HNO3 from ACE-FTS. A global chemical transport model (GEOS-Chem) is used to identify locations and time periods in which lightning would be expected to dominate the trace gas observations. The satellite observations are sampled at those locations and time periods. All three observations exhibit a maximum in the tropical Atlantic region and a minimum in the tropical Pacific. This wave-1 pattern is driven by injection of lightning NO into the upper troposphere over the tropical continents, followed by photochemical production of NO2, HNO3, and O3 during transport. Lightning produces a broad enhancement over the tropical Atlantic and Africa of 2-6 x 10(exp 14) molecules NO2/sq cm, 4 x 10(exp 17) molecules O3/sq cm (15 Dobson Units), and 125 pptv of upper tropospheric HNO3. The lightning background is 25-50% weaker over the tropical Pacific. A global source of 6+/-2 Tg N/yr from lightning in the model best represents the satellite observations of tropospheric NO2, O3, and HNO3.
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.
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).