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At least 73 records · Page 4

The 'Weekend Effect' in Tropospheric NO2 Seen from the Ozone Monitoring Instrument

The Ozone Monitoring Instrument has gathered daily global data on NO2 and other atmospheric trace gases since its launch on the EOS Aura satellite in 2004. The large accumulated data set makes it possible to monitor changes of both meteorological and anthropogenic origin in tropospheric NOz amounts. In particular, averages on time scales on the order of a year show a distinct 'weekend effect' in NO2 variation, with smaller NO2 amounts seen on Saturday and/or Sunday than on the remaining weekdays. Using the OMI NO2 Standard Product (SP), we examine this effect in relation to geopolitical boundaries and investigate implications for identifying sources. We also use the SP data to find evidence for other short-term anthropogenic changes in NO2 emissions over heavily polluted regions including the United States, Europe and China.

Bucsela, E.↗

The Utility of the OMI HCHO and NO2 Data Products in Air Quality Decision- Making Activities

We will present three related air quality applications of the OMI HCHO (formaldehyde) and NO2 (nitrogen dioxide) data products, which we us to support mission planning of an OMI-like instrument for the proposed GEO-CAPE satellite that has as one of its objectives to study air quality from space. First, we will discuss a novel and practical application of the data products to the "weight of evidence" in the air quality decision-making process (e.g., State Implementation Plan (SIP)) for a city, region, or state to demonstrate that it is making progress toward attainment of the National Ambient Air Quality Standard (NAAQS) for ozone. Any trend, or lack thereof, in the observed OMI HCHO/NO2, which we use as an air quality indicator, may support that an emission control strategy implemented to reduce ozone is or is not occurring for a metropolitan area. Second, we will discuss how we use variations in the OMI HCHO product as a proxy for variability in the biogenic hydrocarbon, isoprene, which is an important player for the formation of high levels of ozone and the dominant source of HCHO in the eastern U.S. Third, we will discuss the variability of NO2 in the U.S. as indicated by the OMI NO2 product. In addition, we will show the impact of the 2005 hurricanes on pollutant emissions, including those associated with the intensive oil extraction and refining activities, in the Gulf of Mexico region using the OMI NO2 product. The variability of HCHO and NO2 as indicated by OMI helps us to understand changes in the OMI HCHO/NO2 and the implications for ozone formation.

Duncan, Bryan N.↗

Improved Satellite Retrievals of NO2 and SO2 over the Canadian Oil Sands and Comparisons with Surface Measurements

Satellite remote sensing is increasingly being used to monitor air quality over localized sources such as the Canadian oil sands. Following an initial study, significantly low biases have been identified in current NO2 and SO2 retrieval products from the Ozone Monitoring Instrument (OMI) satellite sensor over this location resulting from a combination of its rapid development and small spatial scale. Air mass factors (AMFs) used to convert line-of-sight "slant" columns to vertical columns were re-calculated for this region based on updated and higher resolution input information including absorber profiles from a regional-scale (15 km × 15 km resolution) air quality model, higher spatial and temporal resolution surface reflectivity, and an improved treatment of snow. The overall impact of these new Environment Canada (EC) AMFs led to substantial increases in the peak NO2 and SO2 average vertical column density (VCD), occurring over an area of intensive surface mining, by factors of 2 and 1.4, respectively, relative to estimates made with previous AMFs. Comparisons are made with long-term averages of NO2 and SO2 (2005-2011) from in situ surface monitors by using the air quality model to map the OMI VCDs to surface concentrations. This new OMI-EC product is able to capture the spatial distribution of the in situ instruments (slopes of 0.65 to 1.0, correlation coefficients of greater than 0.9). The concentration absolute values from surface network observations were in reasonable agreement, with OMI-EC NO2 and SO2 biased low by roughly 30%. Several complications were addressed including correction for the interference effect in the surface NO2 instruments and smoothing and clear-sky biases in the OMI measurements. Overall these results highlight the importance of using input information that accounts for the spatial and temporal variability of the location of interest when performing retrievals.

surface concentration↗

Impact of COVID-19 Restrictions on Atmospheric Concentrations of O3 and NO2 Across the Globe

We use a machine learning algorithm combining information from the NASA GEOS composition forecast (GEOS-CF) model and surface observations of nitrogen dioxide (NO2) and ozone (O3) at more than 5,000 observation sites to assess the impact of COVID-19 restrictions on surface air quality in 46 countries. Our methodology removes the compounding impacts of meteorology, seasonality and atmospheric chemistry on air pollution, thus allowing for a quantitative estimate of the change in surface air quality following COVID-19 containment measures. Compared to GEOS-CF model predictions that do not include emission reductions related to COVID-19 restrictions, surface observations show a drop in surface NO2 of up to 60% after the implementation of lockdowns. Average NO2 concentrations between February 2020 to June 2020 were 18% lower than business as usual. The earliest and strongest declines are observed over China, followed by Europe and the US. While NO2 concentrations over China recovered within 2 months, the recovery has been slower over Europe and the US. The impact of COVID-19 restrictions on O3 is complicated by non-linear atmospheric chemistry. Locally, O3 can show a short-term increase of up to 50% as a result of the decrease in NO2, which leads to a reduction in night time titration. However, this effect is offset by a decrease in photochemical production during the day. Our results indicate that these two competing processes resulted in a net zero change in average surface ozone during the first 5 months of the pandemic. The results also indicate that the reduced photochemical production becomes increasingly important over time. Our analysis is based on surface observations and model simulations available in near real-time, and we will present an up-to-date view of the short and medium-term impacts of COVID-19 restrictions on air quality around the world.

COVID-19↗

Updated assessment of TROPOMI NO2 and HCHO columns using airborne spectrometers during the MOOSE and TRACER-AQ field campaigns

Airborne spectrometer data offers the opportunity to evaluate satellite product performance without the impact of subpixel heterogeneity between the different satellite and ground-based measurement footprints. Previous measurements during the Long Island Sound Tropospheric Ozone Study were used to evaluate TROPOMI’s v1.3 NO2 product and found very strong relationships (r2=0.96) between the airborne spectrometer and TROPOMI with a systematic low bias mostly attributed to the coarse a priori profile assumption within the standard TROPOMI retrieval. This presentation will update that analysis using the most up-to-date version 2 TROPOMI NO2 product as well as expand analysis to the HCHO product. In summer 2021, NASA GeoCAPE Airborne Simulator (GCAS) collected measurements over southeast Michigan/western Ontario for the Michigan-Ontario Ozone Source Experiment (MOOSE) and Houston, Texas during the TRacking Aerosol Convection ExpeRiment – Air Quality (TRACER-AQ). Flight strategies for both deployments included repeated systematic sampling over common areas of interest coinciding with TROPOMI. During these flights, GCAS NO2 tropospheric columns are available at 250 m x 560 m resolution. Preliminary evaluation of GCAS NO2 retrievals with Pandora spectrometer data in Houston, Texas (3 sites) shows a median percent difference of 1.4% with an interquartile range of -15.5-14.9% (r2=0.72). Column HCHO was also retrieved at a slightly coarser resolution in Houston, Texas (750 m x 1680 m) showing distinct spatial patterns associated with secondary production through the oxidation of VOCs downwind of industrial facilities. Comparison to Pandora HCHO showed a low bias of ~25% (r2=0.29) with further investigation needed to identify the cause for this bias. This presentation will share how the GCAS/Pandora/TROPOMI NO2 and HCHO intercompare and will also extend analysis toward thinking about how these assets will contribute to the validation of future geostationary observations.

Laura Judd↗

Illustrating the Spatiotemporal Complexity of No2 Columns Using A Multi-Perspective Observing System: Moving Toward Geostationary Product Validation and Applications

As a precursor to secondary pollutants like ozone and PM2.5, nitrogen dioxide (NO2) is crucial to understand when addressing air quality issues. However, due to NO2’s short lifetime during the daytime and complexity of emission sources in urbanized regions, interpreting datasets from ground or satellite perspectives alone are challenged by variance in spatial and temporal resolutions. High resolution airborne mapping (< 1 km) of NO2 column densities across morning, midday, and afternoon add a unique perspective toward interpreting satellite data with respect to ground-measurements. This presentation focuses on the interpretation of spatiotemporal complexity of NO2 columns from the Synergistic TEMPO Air Quality Science Study (STAQS). The mission’s goal is to integrate geostationary observations from Tropospheric Emissions: Monitoring of Pollution (TEMPO) with traditional and enhanced air quality monitoring to improve the understanding of air quality science for increased societal benefit. We will demonstrate the interweaved perspective of NO2 columns from ground-based Pandora spectrometers and satellite-based observations (e.g., TROPOMI) as compared to high spatial resolution airborne observations from the GEOstationary Coastal and Air Pollution Events (GEO-CAPE) Airborne Simulator (GCAS). This includes the evaluation of each dataset through comparison to each other to identify potential biases in data products and the impact of heterogeneity on these comparisons. Airborne data will also be used as a proxy for geostationary observations with morning, midday, and afternoon raster maps collected over four cities (Los Angeles, Chicago, Toronto, and New York City). Finally, recent research outcomes will be presented to demonstrate how airborne and geostationary observations can be used to evaluate emission inventories and air quality models.

Laura Judd↗

A Decade of Change in NO2 and SO2 over the Canadian Oil Sands As Seen from Space

A decade (20052014) of observations from the Ozone Monitoring Instrument (OMI) were used to examine trends in nitrogen dioxide(NO2) and sulfur dioxide (SO2) over a large region of western Canada and the northern United States, with a focus on the Canadian oil sands. In the oil sands, primarily over an area of intensive surface mining, NO2 tropospheric vertical column densities (VCDs) are seen to be increasing by as much as 10year, with the location of the largest trends in a newly developing NO2 lobe well removed from surface monitoring stations. SO2 VCDs in the oil sands have remained approximately constant. The only other significant increase in the region was seen in NO2 over Bakken gas fields in North Dakota which showed increases of up to5yr. By contrast, other locations in the region show substantial declines in both pollutants, providing strong evidence to the efficacy of environmental pollution control measures implemented by both nations. The OMI-derived trends were found to be consistent with those from the Canadian surface monitoring network, although in the case of SO2, it was necessary to apply a correction in order to remove the residual signal from volcanic eruptions present in the OMI data.

NO2↗

Evaluation of Modeling NO2 Concentrations Driven by Satellite-Derived and Bottom-Up Emission Inventories Using In-Situ Measurements Over China

Chemical transport models together with emission inventories are widely used to simulate NO2 concentrations over China, but validation of the simulations with in situ measurements has been extremely limited. Here we use ground measurements obtained from the air quality monitoring network recently developed by the Ministry of Environmental Protection of China to validate modeling surface NO2 concentrations from the CHIMERE regional chemical transport model driven by the satellite-derived DECSO and the bottom-up MIX emission inventories. We applied a correction factor to the observations to account for the interferences of other oxidized nitrogen compounds (NOz), based on the modeled ratio of NO2 to NOz. The model accurately reproduces the spatial variability in NO2 from in situ measurements, with a spatial correlation coefficient of over 0.7 for simulations based on both inventories. A negative and positive bias is found for the simulation with the DECSO (slopeD0.74 and 0.64 for the daily mean and daytime only) and the MIX (slopeD1.3 and 1.1) inventories, respectively, suggesting an underestimation and overestimation of NOx emissions from corresponding inventories. The bias between observed and modeled concentrations is reduced, with the slope dropping from 1.3 to 1.0 when the spatial distribution of NOx emissions in the DECSO inventory is applied as the spatial proxy for the MIX inventory, which suggests an improvement of the distribution of emissions between urban and suburban or rural areas in the DECSO inventory compared to that used in the bottom-up inventory. A rough estimate indicates that the observed concentrations, from sites predominantly placed in the populated urban areas, may be 10-40% higher than the corresponding model grid cell mean. This reduces the estimate of the negative bias of the DECSO-based simulation to the range of -30 to 0% on average and more firmly establishes that the MIX inventory is biased high over major cities. The performance of the model is comparable over seasons, with a slightly worse spatial correlation in summer due to the difficulties in resolving the more active NOx photochemistry and larger concentration gradients in summer by the model. In addition, the model well captures the daytime diurnal cycle but shows more significant disagreement between simulations and measurements during nighttime, which likely produces a positive model bias of about 15% in the daily mean concentrations. This is most likely related to the uncertainty in vertical mixing in the model at night.

NO2 modelling↗

The distribution of NO2(plus) in the lower ionosphere

Data on the NO2(+)(46 AMU) were obtained with a rocket-borne quadrupole ion mass spectrometer. The ion 46(+) is most prevalent in the vicinity of 90 km and is always observed in the presence of 48(+), identified as NO(+)-H2O. The observed concentrations of O(+)(16), O2(+)(32), NO2(+)(46), NO(+)-H2O(48), electrons, and the ratio 48(+)/46(+) are tabulated for altitudes from 87.8 to 93.2 km. Reactions governing the distribution of NO2(+) are briefly discussed, and it is felt that photoionization and charge exchange reactions are insufficient to account for the NO2(+) concentration at 90 km.

Aikin, A. C.↗

Ruby laser induced emission from NO2

Two different types of emission from excited NO2 were observed using pulsed ruby laser light at 6943 A. The first type of fluorescence was seen in the near IR and results from the single photon excitation of NO2 from the ground 2-A1 state. By observing the emission as a function of time an unexpected behavior was observed in the near IR and could be explained by a consecutive deactivation mechanism, wherein a secondary species is preferentially detected. A second type of emission recently observed in the blue spectral region is weaker and is due to a multiphoton process. The intensity of the blue emission is a function of the cube of the laser intensity at low pressures and approaches the square at high pressures. This variation is attributed to simultaneous deactivation of the excited NO2 intermediate by collision (square) and by anti-Stokes Raman scattering off of the excited NO2 (cube).

Hakala, D. F.↗

Kinetics of hydrogen-oxygen and methane-oxygen ignition sensitized by NO or NO2

In a study of methane ignition sensitized by NO2, the induction period chemical kinetics were examined by monitoring reactants and intermediates (CH4, NO2, OH, NO, CO, CO2, and H2O) prior to ignition. Data were obtained at pressure of 2-4 atm, temperatures of 1300-1900 K, equivalence ratios of 0.5-1.0, and NO2 up to 3.4 mole %. A tentative NO2 sensitization mechanism was deduced from the analysis of photometric observations and the comparison of computer modeling with observations.

Slack, M. W.↗

The enhanced oxidation of SO2 by NO2 on carbon particulates

The oxidation of SO2 on carbon particles in dry air and in air at 65% relative humidity (RH) was found to be greatly enhanced by the presence of gaseous NO2. Exposures of 20-80ppm SO2 + 10ppm NO2 on 1-mg samples of commercial carbon black were found to produce both sorption and desorption coverages (weight retained after desorption into N2) of over one order of magnitude greater than for corresponding SO2 exposures. Significant agglomeration and wetting were observed to occur progressively during exposures at 65% RH, and samples, even after 150-h exposure, rarely reached steady-state weight gain. The wetting may have regenerated fresh reactive carbon surface. Sorptions conducted in nitrogen atmospheres, rather than in air, appeared to produce slightly higher sorptions and weight retentions for equivalent exposure concentrations and times, indicating that NO2 served as the oxidizer and that molecular oxygen, or some trace constitutents in air, may have weakly inhibited the oxidation by NO2. Wet chemical analysis of the desorbed phase indicated that sulfate, presumably H2SO4 accounted for over half of the retained weight. Measurements of pH from water-quenched samples indicated a highly acidic surface phase, and suggested the oxidation process could proceed in an acidic environment.

Cofer, W. R., III↗

Kinetics of the ClO + NO2 + M reaction

The ClO + NO2 + M reaction has been studied with two techniques: Fourier transform infrared spectroscopy of the products, and flash photolysis-ultraviolet absorption to monitor the decay of ClO in excess NO2. The measured third-order rate constant is 1.5 x 10 to the -31st cm to the 6th/molecule-squared per sec at 298 K with M = N2, in good agreement with previous literature values, but the rate constant appears to decrease by up to a factor of three in the presence of increasing amounts of OClO. For the infrared studies a stoichiometric mixture of ClO and NO2 was prepared in a flow system by mixing NO with OClO; at least as much NO2 as ClONO2 was produced under a variety of experimental conditions. These two sets of results are incompatible with the assumption made in previous kinetic studies that ClONO2 is the only recombination product; other isomers such as OClONO or ClOONO are likely to be formed three to four times faster. These results imply that potential stratospheric ozone depletion due to chlorofluoromethanes may be even larger than previously thought.

Molina, M. J.↗

Production of NO2/-/ and N2O by nitrifying bacteria at reduced concentrations of oxygen

The influence of oxygen concentration on the production of NO2(-) and N2O by nitrifying marine bacteria of the genus Nitrosomonas is investigated. Pure cultures of the ammonium-oxiding bacteria isolated from the Western Tropical Atlantic Ocean were grown at oxygen partial pressures from 0.005 to 0.2 atm, and concentrations of N2O in the air above the growth medium and dissolved NO2(-) were determined. Decreasing oxygen concentrations are observed to induce a marked decrease in NO2(-) production rates and increase in N2O evolution, leading to an increase of the relative yield of N2O with respect to NO2(-) from 0.3% to nearly 10%. Similar yields of N2O at atmospheric oxygen levels are found for nitrifying bacteria of the genera Nitrosomonas, Nitrosolobus, Nitrosospira and Nitrosococcus, while nitrite-oxydizing bacteria and a dinoflagellate did not produce detectable quantities of N2O. Results support the view that nitrification is a major source of N2O in the environment.

Goreau, T. J.↗

Measurements of stratospheric NO2 from the Solar Mesosphere Explorer satellite. I - An overview of the results

The visible light spectrometer on board the Solar Mesosphere Explorer spacecraft measures stratospheric NO2 in the 20-40 km altitude region and provides accurate daytime NO2 density profiles with nearly complete latitudinal coverage over an extended period of time. The instrument and data analysis are discussed in detail, and NO2 results for winter/spring 1982 are presented and compared to current theoretical models. Agreement with other measurements is good, and comparison with NOx models indicates that although the overall agreement is acceptable, improvements in the models are required before good agreement is reached at all latitudes. The data indicate that NO2 has a strong memory of the physical conditions present in the stratosphere over a time period of several days.

Mount, G. H.↗

The variability of stratospheric and mesospheric NO2 in the polar winter night observed by LIMS

The LIMS experiment sounded the upper atmosphere from late October 1978 to late May 1979 and provided vertical profiles of atmospheric temperature, 03, H2O, HNO3, and NO2. Radiance averaging was used before retrieval to measure the altitude distribution of NO2 over the altitude range from the lower stratosphere into the mesosphere. Observations in the polar winter night region northward of about 70 deg N reveal NO2 levels near 175 ppbv at about 70 km, and they show a significant longitudinal variability (factor of 4 to 7). A definite temporal trend exists, showing a buildup of mesospheric and stratospheric NO2 during the polar night and a subsequent slowing of the increase of decline after sunlight returns, depending on altitude. The data represent the first experimental evidence that the thermosphere is an NO(x) source for the mesosphere and stratosphere.

Russell, M. J., III↗

Seasonal and diurnal variation of the atmospheric NO2 at Syowa Station, Antarctica

Extensive attention has been directed to nitrogen dioxide (NO2) since its important role in the atmospheric chemistry relating to the stratospheric ozone (e.g., WMO, 1982) has been pointed out. However, the behavior of NO2 in the atmosphere has still not been fully confirmed, although ground-based, balloon and satellite measurements of NO2 have been reported by many scientists. Especially, only a few measurements made at high latitude in the Southern Hemisphere have been reported. The total atmospheric NO2 by ground-based visible absorption spectroscopy at Syowa Station (69 deg S, 39.6 deg E), Antarctica. The observation continued from March 1983, to January 1984. The principles of measurement, instrumentation and the method of data analysis are described in detail.

Shibasaki, K.↗

Kinetic studies of the reaction of the SO radical with NO2 and ClO from 210 to 363 K

The rates of the reactions of the SO radical with NO2 and ClO (significant in the upper atmosphere of earth and Venus) were determined in a discharge flow system near 1 torr pressure with detection of radical and molecular species using collision-free sampling mass spectrometry. The rate constants were obtained from the decay of SO radicals in the presence of an excess of NO2 and ClO. The NO2 reaction was examined between 210 and 363 K and found to be temperature invariant: SO + NO2 yields SO2 + NO; k1 = (1.37 + or - 0.10) x 10 to the -11th cu cm/s. In addition, the ClO reaction was observed to be independent of temperature between 248 and 363 K: SO + ClO yields SO2 + Cl; k2 = (3.22 + or - 0.48) x 10 to the -11th cu cm/s. A comparison was made with previous investigations of these reactions at room temperature and with other radical-radical reactions involving SO or ClO.

Brunning, J.↗