Using Satellite Remote Sensing and Modelling for Insights into N02 Air Pollution and NO2 Emissions

Nitrogen oxides (NO(x)) are key actors in air quality and climate change. Satellite remote sensing of tropospheric NO2 has developed rapidly with enhanced spatial and temporal resolution since initial observations in 1995. We have developed an improved algorithm and retrieved tropospheric NO2 columns from Ozone Monitoring Instrument. Column observations of tropospheric NO2 from the nadir-viewing satellite sensors contain large contributions from the boundary layer due to strong enhancement of NO2 in the boundary layer. We infer ground-level NO2 concentrations from the OMI satellite instrument which demonstrate significant agreement with in-situ surface measurements. We examine how NO2 columns measured by satellite, ground-level NO2 derived from satellite, and NO(x) emissions obtained from bottom-up inventories relate to world's urban population. We perform inverse modeling analysis of NO2 measurements from OMI to estimate "top-down" surface NO(x) emissions, which are used to evaluate and improve "bottom-up" emission inventories. We use NO2 column observations from OMI and the relationship between NO2 columns and NO(x) emissions from a GEOS-Chem model simulation to estimate the annual change in bottom-up NO(x) emissions. The emission updates offer an improved estimate of NO(x) that are critical to our understanding of air quality, acid deposition, and climate change

Effect of Particle Non-Sphericity on Satellite Monitoring of Drifting Volcanic Ash Clouds

Volcanic eruptions loft gases and ash particles into the atmosphere and produce effects that are both short term (aircraft hazards, interference with satellite measurements) and long term (atmospheric chemistry, climate). Large (greater than 0.5mm) ash particles fall out in minutes [Rose et al, 1995], but fine ash particles can remain in the atmosphere for many days. This fine volcanic ash is a hazard to modem jet aircraft because the operating temperatures of jet engines are above the solidus temperature of volcanic ash, and because ash causes abrasion of windows and airframe, and disruption of avionics. At large distances(10(exp 2)-10(exp 4) km or more) from their source, drifting ash clouds are increasingly difficult to distinguish from meteorological clouds, both visually and on radar [Rose et al., 1995]. Satellites above the atmosphere are unique platforms for viewing volcanic clouds on a global basis and measuring their constituents and total mass. Until recently, only polar AVHRR and geostationary GOES instruments could be used to determine characteristics of drifting volcanic ash clouds using the 10-12 micron window [Prata 1989; Wen and Rose 1994; Rose and Schneider 1996]. The NASA Total Ozone Mapping Spectrometer (TOMS) instruments aboard the Nimbus-7, Meteor3, ADEOS, and Earth Probe satellites have produced a unique data set of global SO2 volcanic emissions since 1978 (Krueger et al., 1995). Besides SO2, a new technique has been developed which uses the measured spectral contrast of the backscattered radiances in the 330-380nm spectral region (where gaseous absorption is negligible) in conjunction with radiative transfer models to retrieve properties of volcanic ash (Krotkov et al., 1997) and other types of absorbing aerosols (Torres et al., 1998)

Airborne MAX-DOAS Measurements Over California: Testing the NASA OMI Tropospheric NO2 Product

Airborne Multi-AXis Differential Optical Absorption Spectroscopy (AMAX-DOAS) measurements of NO2 tropospheric vertical columns were performed over California for two months in summer 2010. The observations are compared to the NASA Ozone Monitoring Instrument (OMI) tropospheric vertical columns (data product v2.1) in two ways: (1) Median data were compared for the whole time period for selected boxes, and the agreement was found to be fair (R = 0.97, slope = 1.4 +/- 0.1, N= 10). (2) A comparison was performed on the mean of coincident AMAX-DOAS measurements within the area of the corresponding OMI pixels with the tropospheric NASA OMI NO2 assigned to that pixel. The effects of different data filters were assessed. Excellent agreement and a strong correlation (R = 0.85, slope = 1.05 +/- 0.09, N= 56) was found for (2) when the data were filtered to eliminate large pixels near the edge of the OMI orbit, the cloud radiance fraction was2 km, and a representative sample of the footprint was taken by the AMAX-DOAS instrument. The AMAX-DOAS and OMI data sets both show a reduction of NO2 tropospheric columns on weekends by 38 +/- 24% and 33 +/- 11%, respectively. The assumptions in the tropospheric satellite air mass factor simulations were tested using independent measurements of surface albedo, aerosol extinction, and NO2 profiles for Los Angeles for July 2010 indicating an uncertainty of 12%

Comparison of UV irradiances from Aura/Ozone Monitoring Instrument (OMI) with Brewer measurements at El Arenosillo (Spain) – Part 2: Analysis of site aerosol influence

Several validation studies have shown a notable overestimation of the clear sky ultraviolet (UV) irradiance at the Earth's surface derived from satellite sensors such as the Total Ozone Mapping Spectrometer (TOMS) and the Ozone Monitoring Instrument (OMI) with respect to ground-based UV data at many locations. Most of this positive bias is attributed to boundary layer aerosol absorption that is not accounted for in the TOMS/OMI operational UV algorithm. Therefore, the main objective of this study is to analyse the aerosol effect on the bias between OMI erythemal UV irradiance (UVER) and spectral UV (305 nm, 310 nm and 324 nm) surface irradiances and ground-based Brewer spectroradiometer measurements from October 2004 to December 2008 at El Arenosillo station (37.1° N, 6.7° W, 20 m a.s.l.), with meteorological conditions representative of the South-West of Spain. <br><br> The effects of other factors as clouds, ozone and the solar elevation over this intercomparison were analysed in detail in a companion paper (Antón et al., 2010). In that paper the aerosol effects were studied making only a rough evaluation based on aerosol optical depth (AOD) information at 440 nm wavelength (visible range) without applying any correction. We have used the precise information given by single scattering albedo (SSA) from AERONET for the determination of absorbing aerosols which has allowed the correction of the OMI UV data. <br><br> An aerosol correction expression was applied to the OMI operational UV data using two approaches to estimate the UV absorption aerosol optical depth, AAOD. The first approach was based on an assumption of constant SSA value of 0.91. This approach reduces the OMI UVER bias against the reference Brewer data from 13.4% to 8.4%. Second approach uses daily AERONET SSA values reducing the bias only to 11.6%. Therefore we have obtained a 37% and 12% of improvement respectively. For the spectral irradiance at 324 nm, the OMI bias is reduced from 10.5% to 6.98% for constant SSA and to 9.03% for variable SSA. Similar results were obtained for spectral irradiances at 305 nm, and 310 nm. <br><br> Contrary to what was expected, the constant SSA approach has a greater bias reduction than variable SSA, but this is a reasonable result according to the discussion about the reliability of SSA values. Our results reflect the level of accuracy that may be reached at the present time in this type of comparison, which may be considered as satisfactory taking into account the remaining dependence on other factors. Nevertheless, improvements must be accomplished to determine reliable absorbing aerosol properties, which appear as a limiting factor for improving OMI retrievals

In situ measurements of tropospheric volcanic plumes in Ecuador and Colombia during TC^4

A NASA DC-8 research aircraft penetrated tropospheric gas and aerosol plumes sourced from active volcanoes in Ecuador and Colombia during the Tropical Composition, Cloud and Climate Coupling (TC^4) mission in July–August 2007. The likely source volcanoes were Tungurahua (Ecuador) and Nevado del Huila (Colombia). The TC^4 data provide rare insight into the chemistry of volcanic plumes in the tropical troposphere and permit a comparison of SO_2 column amounts measured by the Ozone Monitoring Instrument (OMI) on the Aura satellite with in situ SO_2 measurements. Elevated concentrations of SO_2, sulfate aerosol, and particles were measured by DC-8 instrumentation in volcanic outflow at altitudes of 3–6 km. Estimated plume ages range from ~2 h at Huila to ~22–48 h downwind of Ecuador. The plumes contained sulfate-rich accumulation mode particles that were variably neutralized and often highly acidic. A significant fraction of supermicron volcanic ash was evident in one plume. In-plume O_3 concentrations were ~70%–80% of ambient levels downwind of Ecuador, but data are insufficient to ascribe this to O_3 depletion via reactive halogen chemistry. The TC^4 data record rapid cloud processing of the Huila volcanic plume involving aqueous-phase oxidation of SO_2 by H_2O_2, but overall the data suggest average in-plume SO_2 to sulfate conversion rates of ~1%–2% h^(−1). SO_2 column amounts measured in the Tungurahua plume (~0.1–0.2 Dobson units) are commensurate with average SO_2 columns retrieved from OMI measurements in the volcanic outflow region in July 2007. The TC^4 data set provides further evidence of the impact of volcanic emissions on tropospheric acidity and oxidizing capacity

In situ measurements of tropospheric volcanic plumes in Ecuador and Colombia during TC

A NASA DC‐8 research aircraft penetrated tropospheric gas and aerosol plumes sourced from active volcanoes in Ecuador and Colombia during the Tropical Composition, Cloud and Climate Coupling (TC4 ) mission in July–August 2007. The likely source volcanoes were Tungurahua (Ecuador) and Nevado del Huila (Colombia). The TC4 data provide rare insight into the chemistry of volcanic plumes in the tropical troposphere and permit a comparison of SO2 column amounts measured by the Ozone Monitoring Instrument (OMI) on the Aura satellite with in situ SO2 measurements. Elevated concentrations of SO2, sulfate aerosol, and particles were measured by DC‐8 instrumentation in volcanic outflow at altitudes of 3–6 km. Estimated plume ages range from ∼2 h at Huila to ∼22–48 h downwind of Ecuador. The plumes contained sulfate‐rich accumulation mode particles that were variably neutralized and often highly acidic. A significant fraction of supermicron volcanic ash was evident in one plume. In‐plume O3 concentrations were ∼70%–80% of ambient levels downwind of Ecuador, but data are insufficient to ascribe this to O3 depletion via reactive halogen chemistry. The TC4 data record rapid cloud processing of the Huila volcanic plume involving aqueous‐phase oxidation of SO2 by H2O2, but overall the data suggest average in‐plume SO2 to sulfate conversion rates of ∼1%–2% h−1 . SO2 column amounts measured in the Tungurahua plume (∼0.1–0.2 Dobson units) are commensurate with average SO2 columns retrieved from OMI measurements in the volcanic outflow region in July 2007. The TC4 data set provides further evidence of the impact of volcanic emissions on tropospheric acidity and oxidizing capacit

Modeling of 2008 Kasatochi volcanic sulfate direct radiative forcing: Assimilation of OMI SO \u3c inf\u3e 2 plume height data and comparison with MODIS and CALIOP observations

Volcanic SO2 column amount and injection height retrieved from the Ozone Monitoring Instrument (OMI) with the Extended Iterative Spectral Fitting (EISF) technique are used to initialize a global chemistry transport model (GEOS-Chem) to simulate the atmospheric transport and lifecycle of volcanic SO2 and sulfate aerosol from the 2008 Kasatochi eruption, and to subsequently estimate the direct shortwave, top-of-the-atmosphere radiative forcing of the volcanic sulfate aerosol. Analysis shows that the integrated use of OMI SO2 plume height in GEOS-Chem yields: (a) good agreement of the temporal evolution of 3-D volcanic sulfate distributions between model simulations and satellite observations from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar with Orthogonal Polarisation (CALIOP), and (b) an e-folding time for volcanic SO 2 that is consistent with OMI measurements, reflecting SO2 oxidation in the upper troposphere and stratosphere is reliably represented in the model. However, a consistent (∼25%) low bias is found in the GEOS-Chem simulated SO2 burden, and is likely due to a high (∼20%) bias of cloud liquid water amount (as compared to the MODIS cloud product) and the resultant stronger SO2 oxidation in the GEOS meteorological data during the first week after eruption when part of SO2 underwent aqueous-phase oxidation in clouds. Radiative transfer calculations show that the forcing by Kasatochi volcanic sulfate aerosol becomes negligible 6 months after the eruption, but its global average over the first month is -1.3 Wm -2, with the majority of the forcing-influenced region located north of 20 N, and with daily peak values up to -2 Wm-2 on days 16-17. Sensitivity experiments show that every 2 km decrease of SO2 injection height in the GEOS-Chem simulations will result in a ∼25 % decrease in volcanic sulfate forcing; similar sensitivity but opposite sign also holds for a 0.03 μm increase of geometric radius of the volcanic aerosol particles. Both sensitivities highlight the need to characterize the SO 2 plume height and aerosol particle size from space. While more research efforts are warranted, this study is among the first to assimilate both satellite-based SO2 plume height and amount into a chemical transport model for an improved simulation of volcanic SO2 and sulfate transport

Comparison of UV irradiances from Aura/Ozone Monitoring Instrument (OMI) with Brewer measurements at El Arenosillo (Spain) – Part 1: Analysis of parameter influence

The main objective of this study is to compare the erythemal UV irradiance (UVER) and spectral UV irradiances (at 305, 310 and 324 nm) from the Ozone Monitoring Instrument (OMI) onboard NASA EOS/Aura polar sun-synchronous satellite (launched in July 2004, local equator crossing time 01:45 p.m.) with ground-based measurements from the Brewer spectrophotometer #150 located at El Arenosillo (South of Spain). The analyzed period comprises more than four years, from October 2004 to December 2008. The effects of several factors (clouds, aerosols and the solar elevation) on OMI-Brewer comparisons were analyzed. The proxies used for each factor were: OMI Lambertian Equivalent Reflectivity (LER) at 360 nm (clouds), the aerosol optical depth (AOD) at 440 nm measured from the ground-based Cimel sun-photometer (&lt;a href="http://aeronet.gsfc.nasa.gov"target="_blank"&gt;http://aeronet.gsfc.nasa.gov&lt;/a&gt;), and solar zenith angle (SZA) at OMI overpass time. The comparison for all sky conditions reveals positive biases (OMI higher than Brewer) 12.3% for UVER, 14.2% for UV irradiance at 305 nm, 10.6% for 310 nm and 8.7% for 324 nm. The OMI-Brewer root mean square error (RMSE) is reduced when cloudy cases are removed from the analysis, (e.g., RMSE~20% for all sky conditions and RMSE smaller than 10% for cloud-free conditions). However, the biases remain and even become more significant for the cloud-free cases with respect to all sky conditions. The mentioned overestimation is partially due to aerosol extinction influence. In addition, the differences OMI-Brewer typically decrease with SZA except days with high aerosol loading, when the bias is near constant. The seasonal dependence of the OMI-Brewer difference for cloud-free conditions is driven by aerosol climatology. &lt;br&gt;&lt;br&gt; To account for the aerosol effect, a first evaluation in order to compare with previous TOMS results (Antón et al., 2007) was performed. This comparison shows that the OMI bias is between +14% and +19% for UVER and spectral UV irradiances for moderately-high aerosol load (AOD&gt;0.25). The OMI bias is decreased by a factor of 2 (the typical bias varies from +8% to +12%) under cloud-free and low aerosol load conditions (AOD&lt;0.1). More detailed analysis of absorbing aerosols influence on OMI bias at our station is presented in a companion paper (Cachorro et al., 2010)

The Observed Response of Ozone Monitoring Instrument (OMI) NO2 Columns to NOx Emission Controls on Power Plants in the United States: 2005-2011

We show that Aura Ozone Monitoring Instrument (OMI) nitrogen dioxide (NO2) tropospheric column data may be used to assess changes of the emissions of nitrogen oxides (NOx) from power plants in the United States, though careful interpretation of the data is necessary. There is a clear response for OMI NO2 data to NOx emission reductions from power plants associated with the implementation of mandated emission control devices (ECDs) over the OMI record (2005e2011). This response is scalar for all intents and purposes, whether the reduction is rapid or incremental over several years. However, it is variable among the power plants, even for those with the greatest absolute decrease in emissions. We document the primary causes of this variability, presenting case examples for specific power plants

Comparison of TOMS and AVHRR volcanic ash retrievals from the August 1992 eruption of Mt. Spurr

On August 19, 1992, the Advanced Very High Resolution Radiometer (AVHRR) onboard NOAA-12 and NASA\u27s Total Ozone Mapping Spectrometer (TOMS) onboard the Nimbus-7 satellite simultaneously detected and mapped the ash cloud from the eruption of Mt. Spurr, Alaska. The spatial extent and geometry of the cloud derived from the two datasets are in good agreement and both AVHRR split window IR (11–12µm brightness temperature difference) and the TOMS UV Aerosol Index (0.34–0.38µm ultraviolet backscattering and absorption) methods give the same range of total cloud ash mass. Redundant methods for determination of ash masses in drifting volcanic clouds offer many advantages for potential application to the mitigation of aircraft hazards