Internal conversion in benzene, benzene-d sub 6, and sulfur dioxide
Benzene, benzene-d sub 6 and sulfur dioxide radiative lifetime measurement comparison, investigating internal conversion behavior
Smith, W. H.↗
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Trends in sulfur dioxide over the Indian subcontinent during 2003–2019
Sulfur dioxide (SO2) and its oxidation products profoundly impact the air quality and climate. In recent decades, contrasting SO2 trends have been observed over different regions of the globe due to urbanization, energy generation and control measures. In this study, we have investigated the SO2 trends over the rapidly developing Indian subcontinent using model reanalysis, satellite data, and emission inventories during 2003–2019 period. Copernicus Atmosphere Monitoring Service (CAMS) reanalysis shows rapid SO2 growth up to 0.4 ppbv/yr during 2003–2009, particularly significant over the Indo-Gangetic Plain (IGP) and eastern India. However, the growth becomes slower after 2010 and is followed by a stabilization or slight reduction. The CAMS results agree with the satellite-based observations, however, the model underestimates enhancements over eastern India. The analysis of inventory datasets also suggests slower growths in SO2 emissions and coal-fired electricity generation in recent years. Besides the changes in regional emissions, the enhancements in water vapor and OH radical coinciding with SO2 stabilization indicate strengthening of the sink processes. Model simulation (Modern-Era Retrospective analysis for Research and Applications version 2―MERRA-2) with constant emissions shows reduction in SO2 which confirms the stronger chemical losses. Overall, the SO2 trends over the Indian subcontinent are found to be a manifestation of the combined effects of the regional emission change and chemistry. Our findings highlight the need for studies to assess the impacts of changing SO2 trends in India on the regional and global climate.
Lakhima Chutia↗
Airborne measurements of sulfur dioxide, dimethyl sulfide, carbon disulfide, and carbonyl sulfide by isotope dilution gas chromatography/mass spectrometry
A gas chromatograph/mass spectrometer is described for determining atmospheric sulfur dioxide, carbon disulfide, dimethyl sulfide, and carbonyl sulfide from aircraft and ship platforms. Isotopically labelled variants of each analyte were used as internal standards to achieve high precision. The lower limit of detection for each species for an integration time of 3 min was 1 pptv for sulfur dioxide and dimethyl sulfide and 0.2 pptv for carbon disulfide and carbonyl sulfide. All four species were simultaneously determined with a sample frequency of one sample per 6 min or greater. When only one or two species were determined, a frequency of one sample per 4 min was achieved. Because a calibration is included in each sample, no separate calibration sequence was needed. Instrument warmup was only a few minutes. The instrument was very robust in field deployments, requiring little maintenance.
Bandy, Alan R.↗
An intercomparison of aircraft instrumentation for tropospheric measurements of sulfur dioxide
As part of the NASA Tropospheric Chemistry Program, a series of field intercomparisons have been conducted to evaluate the state-of-the art for measuring key tropospheric species. One of the objectives of the third intercomparison campaign in this series, Chemical Instrumentation Test and Evaluation 3 (CITE 3), was to evaluate instrumentation for making reliable tropospheric aircraft measurements of sulfur dioxide, dimethyl sulfide, hydrogen sulfide, carbon disulfide, and carbonyl sulfide. This paper reports the results of the intercomparisons of five sulfur dioxide measurement methods ranging from filter techniques, in which samples collected in flight are returned to the laboratory for analyses (chemiluminescent or ion chromatographic), to near real-time, in-flight measurements via gas chromatographic, mass spectrometric, and chemiluminescent techniques. All techniques showed some tendency to track sizeable changes in ambient SO2 such as those associated with altitude changes. For SO2 mixing ratios in the range of 200 pptv to a few ppbv, agreement among the techniques varies from about 30% to several orders of magnitude, depending upon the pair of measurements intercompared. For SO2 mixing ratios less than 200 pptv, measurements from the techniques are uncorrelated. In general, observed differences in the measurement of standards do not account for the flight results. The CITE 3 results do not unambiguously identify one or more of the measurement techniques as providing valid or invalid SO2 measurements, but identify the range of 'potential' uncertainty in SO2 measurements reported by currently available instrumentation and as measured under realistic aircraft environments.
Gregory, Gerald L.↗
Linking Improvements in Sulfur Dioxide Emissions to Decreasing Sulfate Wet Deposition By Combining Satellite and Surface Observations With Trajectory Analysis
Sulfur dioxide (SO2), a criteria pollutant, and sulfate (SO42−) deposition are major environmental concerns in the eastern U.S. and both have been on the decline for two decades. In this study, we use satellite column SO2 data from the Ozone Monitoring Instrument (OMI), and SO42− wet deposition data from the NADP (National Atmospheric Deposition Program) to investigate the temporal and spatial relationship between trends in SO2 emissions and the downward sulfate wet deposition over the eastern U.S. from 2005 to 2015. To establish the relationship between SO2 emission sources and receptor sites, we conducted a Potential Source Contribution Function (PSCF) analysis using HYSPLIT back trajectories for five selected Air Quality System (AQS) sites - (Hackney, OH, Akron, OH, South Fayette, PA, Wilmington, DE, and Beltsville, MD) - in close proximity to NADP sites with large downward SO42− trends since 2005. Back trajectories were run for three summers (JJA) and three winters (DJF) and used to generate seasonal climatology PSCFs for each site. The OMI SO2 and interpolated NADP sulfate deposition trends were normalized and overlapped with the PSCF, to identify the areas that had the highest contribution to the observed drop. The results suggest that emission reductions along the Ohio River Valley have led to decreases in sulfate deposition in eastern OH and western PA (Hackney, Akron and South Fayette). Farther to the east, emission reductions in southeast PA resulted in improvements in sulfate deposition at Wilmington, DE, while for Beltsville, reductions in both the Ohio River Valley and nearby favorably impacted sulfate deposition. For Beltsville, sources closer than 300 km from the site contribute roughly 56% observed deposition trends in winter, and 82% in summer, reflecting seasonal changes in transport pattern as well as faster oxidation and washout of sulfur in summer. This suggests that emissions and wet deposition are linked through not only the location of sources relative to the observing sites, but also to photochemistry and the weather patterns characteristic to the region, as evidenced by a west to east shift in the contribution between winter and summer. The method developed here is applicable to other regions with significant trends such as China and India, and can be used to estimate the potential benefits of emission reduction in those areas.
sulfur dioxide emissions↗
Impact of Regional Northern Hemisphere Mid-latitude Anthropogenic Sulfur Dioxide Emissions on Local and Remote Tropospheric Oxidants
The unintended consequences of reductions in regional anthropogenic sulfur dioxide (SO2) emissions implemented to protect human health are poorly understood. SO2 decreases began in the 1970s in the US and Europe and are expected to continue into the future, while recent emissions decreases in China are also projected to continue. In addition to the well-documented climate effects (warming) from reducing aerosols, tropospheric oxidation is impacted via aerosol modification of photolysis rates and radical sinks. Impacts on the hydroxyl radical and other trace constituents directly affect climate and air quality metrics such as surface ozone levels. We use the Geophysical Fluid Dynamics Laboratory Atmospheric Model version 3 nudged towards National Centers for Environmental Prediction (NCEP) reanalysis wind velocities to estimate the impact of SO2 emissions from the US, Europe, and China by differencing a control simulation with an otherwise identical simulation in which 2015 anthropogenic SO2 emissions are set to zero over one of the regions. Springtime sulfate aerosol changes occur both locally to the emission region and also throughout the Northern Hemispheric troposphere, including remote oceanic regions and the Arctic. Hydroperoxy (HO2) radicals are directly removed via heterogeneous chemistry on aerosol surfaces, including sulfate, in the model, and we find that sulfate aerosol produced by SO2 emissions from the three individual northern mid-latitude regions strongly reduces both HO2 and hydroxyl (OH) by up to 10 % year-round throughout most of the troposphere north of 30∘ N latitude. Regional SO2 emissions significantly increase nitrogen oxides (NOx) by about 5 %–8 % throughout most of the free troposphere in the Northern Hemisphere by increasing the NOx lifetime as the heterogeneous sink of HO2 on sulfate aerosol declines. Despite the NOx increases, tropospheric ozone decreases at northern mid-latitudes by 1 %–4 % zonally averaged and by up to 5 ppbv in summertime surface air over China, where the decreases in HO2 and OH suppress O3 production. Since 2015 anthropogenic SO2 emissions in China exceed those in the US or Europe, the oxidative response is greatest for the China perturbation simulation. Chemical effects of aerosols on oxidation (reactive uptake) dominate over radiative effects (photolysis rates), the latter of which are only statistically significant locally for the large perturbation over China. We find that the SO2 emissions decrease in China, which has yet to be fully realized, will have the largest impact on oxidants and related species in the Northern Hemisphere free troposphere compared to future decreases in Europe or the US. Our results bolster previous calls for a multipollutant strategy for air pollution mitigation to avoid the unintended consequence of aerosol removal leading to surface ozone increases that offset or mask surface ozone gains achieved by regulation of other pollutants, especially in countries where current usage of high-sulfur emitting fuels may be phased out in the future.
anthropogenic sulfur dioxide emissions↗
IUE detection of sulfur dioxide in the atmosphere of Venus
Ultraviolet absorption bands of sulfur dioxide have been detected in the reflectance spectrum of Venus using the high resolution spectrometer of the International Ultraviolet Explorer (IUE). The identification of these bands in the 2080 to 2180 A range has been verified by comparison with laboratory absorption spectra. An estimate of the SO2 vertical column density using a reflecting layer model is 4 x 10 to the 16th sq cm.
Conway, R. R.↗
The Distribution of Sulfur Dioxide and Other Infrared Absorbers on the Surface of Io
The Galileo Near Infrared Mapping Spectrometer was used to investigate the distribution and properties of sulfur dioxide over the surface of Io, and qualitative results for the anti-jove hemisphere are presented here.
Sulfur↗
Interaction of sulfur dioxide and carbon dioxide with clean silver in ultrahigh vacuum.
It is shown that when a clean polycrystalline silver surface is subjected to sulfur dioxide at a pressure of 1 nanotorr, sulfur is chemisorbed to the silver. Heating the contaminated silver leads to an estimation of the minimum heat of desorption of 59 kcal/mol. Sulfur Auger peak height and relative function measurements of the surface during exposure show that adsorption occurs during 6 microtorr/sec exposure at 1 nanotorr.
Lassiter, W. S.↗
Constraining the Sulfur Dioxide Degassing Flux from Turrialba Volcano, Costa Rica Using Unmanned Aerial System Measurements
Observed sulfur dioxide (SO2)mixing ratios onboard unmanned aerial systems (UAS) duringMarch 11-13, 2013 are used to constrain the three-day averaged SO2 degassing flux fromTurrialba volcanowithin a Bayesian inverse modeling framework. A mesoscale model coupled with Lagrangian stochastic particle backward trajectories is used to quantify the source-receptor relationships at very high spatial resolutions (i.e., b1 km). The model shows better performance in reproducing the near-surface meteorological properties and observed SO2 variations when using a first-order closure non-local planetary boundary layer (PBL) scheme. The optimized SO2 degassing fluxes vary from 0.59 +/- 0.37 to 0.83 +/- 0.33 kt d−1 depending on the PBL scheme used. These fluxes are in good agreement with ground-based gas flux measurements, and correspond to corrective scale factors of 8-12 to the posteruptive SO2 degassing rate in the AeroCom emission inventory. The maximum a posteriori solution for the SO2 flux is highly sensitive to the specification of prior and observational errors, and relatively insensitive to the SO2 loss term and temporal averaging of observations. Our results indicate relatively low degassing activity but sustained sulfur emissions from Turrialba volcano to the troposphere during March 2013. This study demonstrates the utility of low-cost small UAS platforms for volcanic gas composition and flux analysis.
Xi, Xin↗
X-ray and infrared studies of several ruthenium-sulfur dioxide complexes
X-ray and infrared data on crystal and molecular structure of ruthenium-sulfur dioxide complexes
MOLECULAR STRUCTURE↗
A Sulfur Dioxide Covariance-Based Retrieval Algorithm (COBRA): Application to TROPOMI Reveals New Emission Sources
Sensitive and accurate detection of sulfur dioxide (SO 2 ) from space is important for monitoring and estimating global sulfur emissions. Inspired by detection methods applied in the thermal infrared, we present here a new scheme to retrieve SO 2 columns from satellite observations of ultraviolet back-scattered radiances. The retrieval is based on a measurement error covariance matrix to fully represent the SO 2 -free radiance variability, so that the SO 2 slant column density is the only retrieved parameter of the algorithm. We demonstrate this approach, named COBRA, on measurements from the TROPOspheric Monitoring Instrument (TROPOMI) aboard the Sentinel-5 Precursor (S-5P) satellite. We show that the method reduces significantly both the noise and biases present in the current TROPOMI operational DOAS SO 2 retrievals. The performance of this technique is also benchmarked against that of the Principal Component Algorithm (PCA) approach. We find that the quality of the data is similar and even slightly better with the proposed COBRA approach. The ability of the algorithm to retrieve SO 2 accurately is also further supported by comparison with ground-based observations. We illustrate the great sensitivity of the method with a high-resolution global SO 2 map, considering two and a half years of TROPOMI data. In addition to the known sources, we detect many new SO 2 emission hotspots worldwide. For the largest sources, we use the COBRA data to estimate SO 2 emission rates. Results are comparable to other recently published TROPOMI-based SO 2 emissions estimates, but the associated uncertainties are significantly lower than with the operational data. Next, for a limited number of weak sources, we demonstrate the potential of our data for quantifying SO 2 emissions with a detection limit of about 8 kt yr -1 , a factor of 4 better than the emissions derived from the Ozone Monitoring Instrument (OMI). We anticipate that the systematic use of our TROPOMI COBRA SO 2 column data set at a global scale will allow identifying and quantifying missing sources, and help improving SO 2 emission inventories.
SO2↗
Linking Improvements in Sulfur Dioxide Emissions to Decreasing Sulfate Wet Deposition by Combining Satellite and Surface Observations with Trajectory Analysis
Sulfur dioxide (SO2), a criteria pollutant, and sulfate (SO42) deposition are major environmental concerns in the eastern U.S. and both have been on the decline for two decades. In this study, we use satellite column SO2 data from the Ozone Monitoring Instrument (OMI), and SO42 wet deposition data from the NADP (National Atmospheric Deposition Program) to investigate the temporal and spatial relationship between trends in SO2 emissions and the downward sulfate wet deposition over the eastern U.S. from 2005 to 2015. To establish the relationship between SO2 emission sources and receptor sites, we conducted a Potential Source Contribution Function (PSCF) analysis using HYSPLIT back trajectories for five selected Air Quality System (AQS) sites - (Hackney, OH, Akron, OH, South Fayette, PA, Wilmington, DE, and Beltsville, MD) - in close proximity to NADP sites with large downward SO42 trends since 2005. Back trajectories were run for three summers (JJA) and three winters (DJF) and used to generate seasonal climatology PSCFs for each site. The OMI SO2 and interpolated NADP sulfate deposition trends were normalized and overlapped with the PSCF, to identify the areas that had the highest contribution to the observed drop. The results suggest that emission reductions along the Ohio River Valley have led to decreases in sulfate deposition in eastern OH and western PA (Hackney, Akron and South Fayette). Farther to the east, emission reductions in southeast PA resulted in improvements in sulfate deposition at Wilmington, DE, while for Beltsville, reductions in both the Ohio River Valley and nearby favorably impacted sulfate deposition. For Beltsville, sources closer than 300km from the site contribute roughly 56% observed deposition trends in winter, and 82% in summer, reflecting seasonal changes in transport pattern as well as faster oxidation and washout of sulfur in summer. This suggests that emissions and wet deposition are linked through not only the location of sources relative to the observing sites, but also to photochemistry and the weather patterns characteristic to the region, as evidenced by a west to east shift in the contribution between winter and summer. The method developed here is applicable to other regions with significant trends such as China and India, and can be used to estimate the potential benefits of emission reduction in those areas.
Acid depostion↗
The abundance of sulfur dioxide below the clouds of Venus
We present a new method for determining the abundance of sulfur dioxide below the clouds of Venus. Absorption by the 3nu3 band of SO2 near 2.45 microns has been detected in high-resolution spectra of the night side of Venus recorded at the Canada-France Hawaii telescope in 1989 and 1991. The inferred SO2 abundance is 130 +/- 40 ppm at all observed locations and pertains to the 35-45 km region. These values are comparable to those measured by the Pioneer Venus and Venera 11/12 entry probes in 1978. This stability stands in contrast to the apparent massive decrease in SO2 observed at the cloud tops since these space missions. These results are consistent with laboratory and modeling studies of the SO2 destruction rates in the lower atmosphere of Venus. The new spectroscopic technique presented here allows a remote monitoring of the SO2 abundance below the clouds, a likely tracer of Venusian volcanism.
Bezard, Bruno↗
Advection of sulfur dioxide over the western Atlantic Ocean during CITE 3
During the NASA Chemical Instrumentation Test and Evaluation 3 sulfur intercomparison over the western Atlantic Ocean, five techniques for the determination of sulfur dioxide were evaluated. The response times of the techniques varied from 3 to 30 min. Based on the ensemble of measurements reported, it was clear that advection of SO2 from the North American continent occurred in the boundary layer (altitude less than 1 km) with only one exception. The vertical distribution of SO2 above the boundary layer for the northern and southern Atlantic Ocean was remarkably similar duing this experiment.
Thornton, D. C.↗
Using CATS Near-Real-time Lidar Observations to Monitor and Constrain Volcanic Sulfur Dioxide (SO2) Forecasts
An eruption of Italian volcano Mount Etna on 3 December 2015 produced fast-moving sulfur dioxide (SO2) and sulfate aerosol clouds that traveled across Asia and the Pacific Ocean, reaching North America in just 5 days. The Ozone Profiler and Mapping Suite's Nadir Mapping UV spectrometer aboard the U.S. National Polar-orbiting Partnership satellite observed the horizontal transport of the SO2 cloud. Vertical profiles of the colocated volcanic sulfate aerosols were observed between 11.5 and 13.5 km by the new Cloud Aerosol Transport System (CATS) space-based lidar aboard the International Space Station. Backward trajectory analysis estimates the SO2 cloud altitude at 7-12 km. Eulerian model simulations of the SO2 cloud constrained by CATS measurements produced more accurate dispersion patterns compared to those initialized with the back trajectory height estimate. The near-real-time data processing capabilities of CATS are unique, and this work demonstrates the use of these observations to monitor and model volcanic clouds.
space↗
The importance of ozone in the oxidation of sulfur dioxide in nonurban tropospheric clouds
In studies of the various possible mechanisms which contribute to the conversion of atmospheric sulfur dioxide to sulfate aerosol in the atmosphere, oxidation within the aqueous, droplet phase of tropospheric clouds has been identified as a major contributor. It has appeared that possibly much of this oxidation is by hydrogen peroxide, with the contribution from ozone being only minimal. The present investigation is concerned with the relative importance of O3 and H2O2 oxidation as a function of pH. The results of a new experimental study of the O3-S(IV) reaction in aqueous solution are presented, and potential S(IV) oxidation rates by O3 in cloud water are compared with those predicted for H2O2. The investigation indicates the potential importance of O3 as a contributor to the overall oxidative conversion of SO2 within typical nonpolluted tropospheric clouds.
Maahs, H. G.↗
Airborne sulfur trace species intercomparison campaign: Sulfur dioxide, dimethylsulfide, hydrogen sulfide, carbon disulfide, and carbonyl sulfide
Results from an airborne intercomparison of techniques to measure tropospheric levels of sulfur trace gases are presented. The intercomparison was part of the NASA Global Tropospheric Experiment (GTE) and was conducted during the summer of 1989. The intercomparisons were conducted on the Wallops Electra aircraft during flights from Wallops Island, Virginia, and Natal, Brazil. Sulfur measurements intercompared included sulfur dioxide (SO2), dimethylsulfide (DMS), hydrogen sulfide (H2S), carbon disulfide (CS2), and carbonyl sulfide (OCS). Measurement techniques ranged from filter collection systems with post-flight analyses to mass spectrometer and gas chromatograph systems employing various methods for measuring and identifying the sulfur gases during flight. Sampling schedules for the techniques ranged from integrated collections over periods as long as 50 minutes to one- to three-minute samples every ten or fifteen minutes. Several of the techniques provided measurements of more than one sulfur gas. Instruments employing different detection principles were involved in each of the sulfur intercomparisons. Also included in the intercomparison measurement scenario were a host of supporting measurements (i.e., ozone, nitrogen oxides, carbon monoxide, total sulfur, aerosols, etc.) for purposes of: (1) interpreting results (i.e., correlation of any noted instrument disagreement with the chemical composition of the measurement environment); and (2) providing supporting chemical data to meet CITE-3 science objectives of studying ozone/sulfur photochemistry, diurnal cycles, etc. The results of the intercomparison study are briefly discussed.
Gregory, Gerald L.↗