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Can Li

Publications and source records attributed to Can Li.

At least 19 records

Noise Reduction for Solar-Induced Fluorescence Retrievals Using Machine Learning and Principal Component Analysis: Simulations and Applications to GOME-2 Satellite Retrievals

We use a spectral-based approach that employs principal component analysis along with a relatively shallow artificial neural network (NN) to substantially reduce noise and other artifacts in terrestrial chlorophyll solar-induced fluorescence (SIF) retrievals. SIF is a very small emission at red and far-red wavelengths that is difficult to measure and is highly sensitive to random errors and systematic artifacts. Our approach relies upon an assumption that a trained NN can effectively reconstruct the total SIF signal from a relatively small number of leading principal components of the satellite-observed far-red radiance spectra without using information from the trailing modes that contain most of the random errors. We test the approach with simulated reflectance spectra produced with a full atmospheric and surface radiative transfer model using different observing and geophysical parameters and various noise levels. Resulting noisy and noise-reduced retrieved SIF values are compared with true values to assess performance. We then apply our noise reduction approach to SIF derived from two different satellite spectrometers. For evaluation, since the truth in this case is unknown, we compare SIF retrievals from two independent sensors with each other. We also compare the noise-reduced SIF temporal variations with those from an independent gross primary product (GPP) product that should display similar variations. Results show that our noise reduction approach improves capture of SIF seasonal and inter-annual variability. Our approach should be applicable to many noisy data products derived from spectral measurements. Our methodology does not replace the original retrieval algorithms; rather the original noisy retrievals are needed as the target for the NN training process.

noise reduction, solar-induced fluorescence, SIF, ↗

Inverse Modeling of the Initial Stage of the 1991 Pinatubo Volcanic Cloud Accounting for Radiative Feedback of Volcanic Ash

The way volcanic clouds evolve is very sensitive to the initial spatial 3D distributions of volcanic materials, which are often unknown. In this study, we conducted inverse modeling of the Mt. Pinatubo cloud using TOMS 2D mapping of Aerosol Index and SO 2 loading during the first three post-eruption days to estimate the time-dependent emissions profiles and initial 3D spatial distributions of volcanic ash and SO 2 . We account for aerosol radiative feedback and dynamic lofting of volcanic ash in the inversion calculations for the first time. This resulted in a lower ash injection height (by 1.5 km for ash) than without ash radiative feedback. The Pinatubo eruption ejected ≈77% of fine ash at 12 to 23 km, ≈65% of SO 2 at 18–25 km. In contrast with previous studies, which suggested that all volcanic materials were emitted above the tropopause, a significant fraction of SO 2 (5.1 of 15.5 Mt) and fine ash (37.2 of 66.5 Mt) were ejected in the troposphere, where SO 2 quickly oxidized into sulfate aerosol that is short-lived in the troposphere. This explains the early presence of sulfate aerosols in the plume and why the models can reproduce the observed volcanic aerosols' optical depth (AOD), assuming lower-than-observed SO 2 emission in the stratosphere. Despite the quicker than in observations build-up of sulfate AOD, in a month after the eruption, the evolution of the Pinatubo AOD simulated using the obtained ash and SO 2 initial distributions converges with the available stratospheric aerosol and gas experiment (SAGE) observations.

Pinatubo volcanic ash and SO2 emissions↗

A Convexification-Based Outer-Approximation Method for Convex and Nonconvex MINLP

The advancement of domain reduction techniques has significantly enhanced the performance of solvers in mathematical programming. This paper delves into the impact of integrating convexification and domain reduction techniques within the Outer-Approximation method. We propose a refined convexification-based Outer-Approximation method alongside a Branch-and-Bound method for both convex and nonconvex Mixed-Integer Nonlinear Programming problems. These methods have been developed and incorporated into the open-source Mixed-Integer Nonlinear Decomposition Toolbox for Pyomo-MindtPy. Comprehensive benchmark tests were conducted, validating the effectiveness and reliability of our proposed algorithms. These tests highlight the improvements achieved by incorporating convexification and domain reduction techniques into the Outer-Approximation and Branch-and-Bound methods.

Optimization↗

Use of Machine Learning and Principal Component Analysis to Retrieve Nitrogen Dioxide (NO 2 ) With Hyperspectral Imagers and Reduce Noise in Spectral Fitting

Nitrogen dioxide (NO 2 ) is an important trace-gas pollutant and climate agent whose presence also leads to spectral interference in ocean color retrievals. NO 2 column densities have been retrieved with satellite UV–Vis spectrometers such as the Ozone Monitoring Instrument (OMI) and the Tropospheric Monitoring Instrument (TROPOMI) that typically have spectral resolutions of the order of 0.5 nm or better and spatial footprints as small as 3.6 km × 5.6 km. These NO 2 observations are used to estimate emissions, monitor pollution trends, and study effects on human health. Here, we investigate whether it is possible to retrieve NO 2 amounts with lower-spectral-resolution hyperspectral imagers such as the Ocean Color Instrument (OCI) that will fly on the Plankton, Aerosol, Cloud, ocean Ecosystem (PACE) satellite set for launch in early 2024. OCI will have a spectral resolution of 5 nm and a spatial resolution of ∼ 1 km with global coverage in 1–2 d. At this spectral resolution, small-scale spectral structure from NO 2 absorption is still present. We use real spectra from the OMI to simulate OCI spectra that are in turn used to estimate NO 2 slant column densities (SCDs) with an artificial neural network (NN) trained on target OMI retrievals. While we obtain good results with no noise added to the OCI simulated spectra, we find that the expected instrumental noise substantially degrades the OCI NO 2 retrievals. Nevertheless, the NO 2 information from OCI may be of value for ocean color retrievals. OCI retrievals can also be temporally averaged over timescales of the order of months to reduce noise and provide higher-spatial-resolution maps that may be useful for downscaling lower-spatial-resolution data provided by instruments such as OMI and TROPOMI; this downscaling could potentially enable higher-resolution emissions estimates and be useful for other applications. In addition, we show that NNs that use coefficients of leading modes of a principal component analysis of radiance spectra as inputs appear to enable noise reduction in NO 2 retrievals. Once trained, NNs can also substantially speed up NO 2 spectral fitting algorithms as applied to OMI, TROPOMI, and similar instruments that are flying or will soon fly in geostationary orbit.

NO2↗

Version 2 of the global catalogue of large anthropogenic and volcanic SO 2 sources and emissions derived from satellite measurements

Sulfur dioxide (SO 2 ) measurements from the Ozone Monitoring Instrument (OMI), Ozone Mapping and Profiler Suite (OMPS), and TROPOspheric Monitoring Instrument (TROPOMI) satellite spectrometers were used to update and extend the previously developed global catalogue of large SO 2 emission sources. This version 2 of the global catalogue covers the period of 2005–2021 and includes a total of 759 continuously emitting point sources releasing from about 10 kt yr −1 to more than 4000 kt yr −1 of SO 2 , that have been identified and grouped by country and primary source origin: volcanoes (106 sources); power plants (477); smelters (74); and sources related to the oil and gas industry (102). There are several major improvements compared to the original catalogue: it combines emissions estimates from three satellite instruments instead of just OMI, uses a new version 2 of the OMI and OMPS SO 2 dataset, and updated consistent site-specific air mass factors (AMFs) are used to calculate SO 2 vertical column densities (VCDs). The newest TROPOMI SO 2 data processed with the Covariance-Based Retrieval Algorithm (COBRA), used in the catalogue, can detect sources with emissions as low as 8 kt yr −1 (in 2018–2021) compared to the 30 kt yr −1 limit for OMI. In general, there is an overall agreement within ±12 % in total emissions estimated from the three satellite instruments for large regions. For individual emission sources, the spread is larger: the annual emissions estimated from OMI and TROPOMI agree within ±13 % in 50 % of cases and within ±28 % in 90 % of cases. The version 2 catalogue emissions were calculated as a weighted average of emission estimates from the three satellite instruments using an inverse-variance weighting method. OMI, OMPS, and TROPOMI data contribute 7 %, 5 %, and 88 % to the average, respectively, for small (<30 kt yr −1 ) sources and 33 %, 20 %, and 47 %, respectively, for large (>300 kt yr −1 ) sources. The catalogue data show an approximate 50 % decline in global SO 2 emissions between 2005 and 2021, although emissions were relatively stable during the last 3 years. The version 2 of the global catalogue has been posted at the NASA global SO 2 monitoring website (https://doi.org/10.5067/MEASURES/SO2/DATA406, Fioletov et al., 2022).

volcanic↗

Change in Tropospheric Ozone in the Recent Decades and its Contribution to Global Total Ozone

Tropospheric ozone is a key chemically active trace gas and radiative forcer. Understanding its long-term changes is important to properly interpret observed changes in total column ozone and stratospheric ozone recovery. We investigate global and regional tropospheric ozone changes and their impact on total column ozone during 2005-2018 using satellite measurements and the NASA Goddard Earth Observing System Chemistry Climate Model (GEOSCCM). Global total ozone increased ~4 DU during 2005-2018 (+0.28±0.06 DU yr(exp -1)) as inferred from Ozone Monitoring Instrument (OMI). Consistent with previous studies, the OMI/MLS (Microwave Limb Sounder) derived global tropospheric ozone increased 2.2 DU during this period, 60% of the global total column ozone increase. While GEOSCCM reproduces reasonably well the total column increase, it overestimates the stratospheric ozone increase and underestimates the tropospheric ozone increase. We find that the tropospheric ozone increases are likely attributed to a growth of regional emissions of key ozone precursors, especially volatile organic compounds (VOCs) as reflected by the positive trends in formaldehyde (CH2O). Although carbon monoxide (CO) has been decreasing everywhere around the globe, it has relatively small impact on the tropospheric ozone trend. Trends in nitrogen dioxide (NO2) vary with regions, and these changes counteract or reinforce the positive effects of CH2O on the tropospheric ozone increases. The model underestimates the observed tropospheric ozone increase, especially over the US and Europe, because of underestimated NO2 emissions changes used in the model. The stratospheric ozone contribution increases during this period in the Northern Hemisphere and contributes to the tropospheric ozone increase.

Atmospheric chemistry↗

Perturbations in Stratospheric Aerosol Evolution Due to the Water-Rich Plume of the 2022 Hunga-Tonga Eruption

The January 2022 Hunga Tonga-Hunga Ha'apai (HTHH) volcanic eruption injected a relatively small amount of SO2, but significantly more water into the stratosphere than previously seen in the modern satellite record. Here we show that the large amount of water resulted in large perturbations to stratospheric aerosol evolution. Our Community Earth System Model simulation reproduces the enhanced water vapor observed by the Microwave Limb Sounder at pressure levels between 10 and 50 hPa for three months. Compared with a simulation without a water injection, this additional source of water vapor increases OH, which halves the SO2 lifetime. Subsequent coagulation creates larger sulfate particles that double the stratospheric aerosol optical depth. A seasonal forecast of volcanic plume transport in the southern hemisphere indicates this eruption will greatly enhance the aerosol surface area and water vapor near the polar vortex until at least October 2022, suggesting that there will continue to be an impact of the HTHH eruption on the climate system.

Atmospheric science↗

A New Machine Learning Based Analysis for Improving Satellite Retrieved Atmospheric Composition Data: OMI SO2 as an Example

Despite recent progress, satellite retrievals of anthropogenic SO2 still suffer from relatively low signal-tonoise ratios. In this study, we demonstrate a new machine learning data analysis method to improve the quality of satellite SO2 products. In the absence of large ground-truth datasets for SO2, we start from SO2 slant column densities (SCDs) retrieved from the Ozone Monitoring Instrument (OMI) using a data-driven, physically based algorithm and calculate the ratio between the SCD and the root mean square (rms) of the fitting residuals for each pixel. To build the training data, we select presumably clean pixels with small SCD / rms ratios (SRRs) and set their target SCDs to zero. For polluted pixels with relatively large SRRs, we set the target to the original retrieved SCDs. We then train neural networks (NNs) to reproduce the target SCDs using predictors including SRRs for individual pixels, solar zenith, viewing zenith and phase angles, scene reflectivity, and O3 column amounts, as well as the monthly mean SRRs. For data analysis, we employ two NNs: (1) one trained daily to produce analyzed SO2 SCDs for polluted pixels each day and (2) the other trained once every month to produce analyzed SCDs for less polluted pixels for the entire month. Test results for 2005 show that our method can significantly reduce noise and artifacts over background regions. Over polluted areas, the monthly mean NN-analyzed and original SCDs generally agree to within ±15 %, indicating that our method can retain SO2 signals in the original retrievals except for large volcanic eruptions. This is further confirmed by running both the NN-analyzed and original SCDs through a topdown emission algorithm to estimate the annual SO2 emissions for ∼ 500 anthropogenic sources, with the two datasets yielding similar results. We also explore two alternative approaches to the NN-based analysis method. In one, we employ a simple linear interpolation model to analyze the original SCD retrievals. In the other, we develop a PCA–NN algorithm that uses OMI measured radiances, transformed and dimension-reduced with a principal component analysis (PCA) technique, as inputs to NNs for SO2 SCD retrievals. While the linear model and the PCA–NN algorithm can reduce retrieval noise, they both underestimate SO2 over polluted areas. Overall, the results presented here demonstrate that our new data analysis method can significantly improve the quality of existing OMI SO2 retrievals. The method can potentially be adapted for other sensors and/or species and enhance the value of satellite data in air quality research and applications.

Can Li↗

Evaluation of SO2, SO4(2−) and an Updated SO2 Dry Deposition Parameterization in the United Kingdom Earth System Model

In this study we evaluate simulated surface SO2 and sulphate (SO4(2-)) concentrations from the United Kingdom Earth System Model (UKESM1) against observations from ground based measurement networks in the USA and Europe for the period 1987 to 2014. We find that UKESM1 captures the historical trend for decreasing concentrations of atmospheric SO2 and SO4(2-) in both Europe and the USA over the period 1987 to 2014. However, in the polluted regions of the eastern USA and Europe, UKESM1 over-predicts surface SO2 concentrations by a factor of 3, while under-predicting surface SO4(2-) concentrations by 25-35%. In the cleaner western USA, the model over-predicts both surface SO2 and SO4(2-) concentrations by a factor of 12 and 1.5 respectively. We find that UKESM1’s bias in surface SO2 and SO4(2-) concentrations is variable according to region and season. We also evaluate UKESM1 against total column SO2 from the Ozone Monitoring Instrument (OMI) using an updated data product. This comparison provides information about the model’s global performance, finding that UKESM1 over predicts total column SO2 over much of the globe, including the large source regions of India, China, the USA and Europe as well as over outflow regions. Finally, we assess the impact of a more realistic treatment of the model’s SO2 dry deposition parameterization. This change increases SO2 dry deposition to the land and ocean surfaces, thus reducing the atmospheric loading of SO2 and SO(sup 2-)(sub 4). In comparison with the ground-based and satellite observations, we find that the modified parameterization reduces the models over prediction of surface SO2 concentrations and total column SO2. Relative to the ground-based observations the simulated surface SO4(2-) concentrations are also reduced, while the simulated SO2 dry deposition fluxes increase.

SO2↗

Tracking aerosols and SO2 clouds from the Raikoke eruption: 3D view from satellite observations

The 21 June 2019 eruption of the Raikoke volcano (Kuril Islands, Russia; 48° N, 153° E) produced significant amounts of volcanic aerosols (sulfate and ash) and sulfur dioxide (SO2) gas that penetrated into the lower stratosphere. The dispersed SO2 and sulfate aerosols in the stratosphere were still detectable by multiple satellite sensors for many months after the eruption. For this study of SO2 and aerosol clouds we use data obtained from two of the Ozone Mapping and Profiler Suite sensors on the Suomi National Polar-orbiting Partnership satellite: total column SO2 from the Nadir Mapper and aerosol extinction profiles from the Limb Profiler as well as other satellite data sets. We evaluated the limb viewing geometry effect (the “arch effect”) in the retrieval of the LP standard aerosol extinction product at 674 nm. It was shown that the amount of SO2 decreases with a characteristic period of 8–18 d and the peak of stratospheric aerosol optical depth recorded at a wavelength of 674 nm lags the initial peak of SO2 mass by 1.5 months. Using satellite observations and a trajectory model, we examined the dynamics of an unusual atmospheric feature that was observed, a stratospheric coherent circular cloud of SO2 and aerosol from 18 July to 22 September 2019.

Eruption of the Raikoke volcano↗

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↗

Inconsistencies in Sulphur Dioxide Emissions from the Canadian Oil Sands and Potential Implications

Satellite-derived and reported sulfur dioxide (SO2) emissions from the Canadian oil sands are shown to have been consistent up to 2013. Post-2013, these sources of emissions data diverged, with reported emissions dropping by a factor of two, while satellite-derived emissions for the region remained relatively constant, with the discrepancy (satellite-derived emissions minus reported emissions) peaking at 50 kt(SO2) yr−1 around 2016. The 2013–2014 period corresponds to when new flue-gas desulfurization units came on-line. Previous work has established a high level of consistency between at-stack SO2 emissions observations and satellite estimates, and surface monitoring network SO2 concentrations over the same multi-year period show similar trends as the satellite data, with a slight increase in concentrations post-2013. No clear explanation for this discrepancy currently exists. The implications of the discrepancy towards estimated total sulfur deposition to downwind ecosystems were estimated relative to 2013 emissions levels, with the satellite-derived values leaving the area of regional critical load exceedances of aquatic ecosystems largely unchanged from 2013 values, 335 000 km2, and reported values potentially decreasing this area to 185,000 km2.

Sulphur dioxide (SO2) emissions↗

Version 2 Ozone Monitoring Instrument SO2 Product (OMSO2 V2): New Anthropogenic SO2 Vertical Column Density Dataset

The Ozone Monitoring Instrument (OMI) has been providing global observations of SO2 pollution since 2004. Here we introduce the new anthropogenic SO2 vertical column density (VCD) dataset in the version 2 OMI SO2 product (OMSO2 V2). As with the previous version (OMSO2 V1.3), the new dataset is generated with an algorithm based on principal component analysis of OMI radiances, but features several updates. The most important among those is the use of expanded lookup tables and model a priori profiles to estimate SO2 Jacobians for individual OMI pixels, in order to better characterize pixel-to-pixel variations in SO2 sensitivity, including over snow and ice. Additionally, new data screening and spectral fitting schemes have been implemented to improve the quality of the spectral fit. As compared with the planetary boundary layer SO2 dataset in OMSO2 V1.3, the new dataset has substantially better data quality, especially over areas that are relatively clean or affected by the south Atlantic anomaly. The updated retrievals over snow/ice yield more realistic seasonal changes in SO2 at high latitudes and offer enhanced sensitivity to sources during wintertime. An error analysis has been conducted to assess uncertainties in SO2 VCDs from both the spectral fit and Jacobian calculations. The uncertainties from spectral fitting are reflected in SO2 slant column densities (SCDs) and largely depend on the signal-to-noise ratio of the measured radiances, as implied by the generally smaller SCD uncertainties over clouds or for smaller solar zenith angles. The SCD uncertainties for individual pixels are estimated to be~0.15-0.3 DU (Dobson Units) between ~40°S and ~40°N and to be~0.2-0.5 DU at higher latitudes. The uncertainties from the Jacobians are approximately ~50-100% over polluted areas, and primarily attributed to errors in SO2 a priori profiles and cloud pressures, as well as the lack of explicit treatment for aerosols. Finally, the daily mean and median SCDs over the presumably SO2-free equatorial East Pacific have increased by only~0.0035 DU and ~0.003 DU respectively over the entire 15-year OMI record; while the standard deviation of SCDs has grown by only~0.02 DU or ~10%. Such remarkable long-term stability makes the new dataset particularly suitable for detecting regional changes in SO2 pollution.

OMI, SO2, Remote Sensing↗

A New Discrete Wavelength BUV Algorithm for Consistent Volcanic SO2 Retrievals from Multiple Satellite Missions

This paper describes a new discrete wavelength algorithm developed for retrieving volcanic sulfur dioxide (SO2) vertical column density (VCD) from UV observing satellites. The Multi-Satellite SO2 algorithm (MS_SO2) simultaneously retrieves column densities of sulfur dioxide, ozone, and Lambertian effective reflectivity (LER) and its spectral dependence. It is used operationally to process measurements from the heritage Total Ozone Mapping Spectrometer (TOMS) onboard NASA's Nimbus-7 satellite (N7/TOMS: 1978-1993) and from the current Earth Polychromatic Imaging Camera (EPIC) onboard Deep Space Climate Observatory (DSCOVR: 2015-) from the Earth-Sun Lagrange (L1) orbit. Results from MS_SO2 algorithm for several volcanic cases were assessed using the more sensitive principal component analysis (PCA) algorithm. The PCA is an operational algorithm used by NASA to retrieve SO2 from hyperspectral UV spectrometers, such as the Ozone Monitoring Instrument (OMI) onboard NASA's Earth Observing System Aura satellite and Ozone Mapping and Profiling Suite (OMPS) onboard NASA-NOAA Suomi National Polar Partnership (SNPP) satellite. For this comparative study, the PCA algorithm was modified to use the discrete wavelengths of the Nimbus-7/TOMS instrument, described in Sect. S1 of the Supplement. Our results demonstrate good agreement between the two retrievals for the largest volcanic eruptions of the satellite era, such as the 1991 Pinatubo eruption. To estimate SO2 retrieval systematic uncertainties, we use radiative transfer simulations explicitly accounting for volcanic sulfate and ash aerosols. Our results suggest that the discrete-wavelength MS_SO2 algorithm, although less sensitive than hyperspectral PCA algorithm, can be adapted to retrieve volcanic SO2 VCDs from contemporary hyperspectral UV instruments, such as OMI and OMPS, to create consistent, multi-satellite, long-term volcanic SO2 climate data records.

Bradford L Fisher↗

Five Decades Observing Earth's Atmospheric Trace Gases Using Ultraviolet and Visible Backscatter Solar Radiation from Space

Over the last five decades, Earth’s atmosphere has been extensively monitored from space using different spectral ranges. Early efforts were directed at improving weather forecasts with the first meteorological satellites launched in the 1960s. Soon thereafter, the intersection between weather, climate and atmospheric chemistry led to the observation of atmospheric composition from space. During the 1970s the Nimbus satellite program started regular monitoring of ozone integrated columns and water vapor profiles using the Backscatter Ultraviolet Spectrometer, the Infrared Interferometer Spectrometer and the Satellite Infrared Spectrometer instruments. Five decades after these pioneer efforts, continuous progress in instrument design, and retrieval techniques allow researchers to monitor tropospheric concentrations of a wide range of species with implications for air quality, climate and weather. The time line of historic, present and future space-borne instruments measuring ultraviolet and visible backscattered solar radiation designed to quantify atmospheric trace gases is presented. We describe the instruments technological evolution and the basic concepts of retrieval theory. We include a review of algorithms developed for ozone, nitrogen dioxide, sulfur dioxide, formaldehyde, bromine monoxide, water vapor and glyoxal, a selection of studies using these algorithms, the challenges they face and how these challenges can be addressed. The paper ends by providing insights on the opportunities that new instruments will bring to the atmospheric chemistry, weather and air quality communities and how to address the pressing need for long-term, inter-calibrated data records necessary to monitor the response of the atmosphere to rapidly changing ecosystems.

Infrared Interferometer Spectrometer↗

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↗