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Using Machine Learning to Estimate Surface-Level SO2 Concentrations from Satellite-Based Measurements

Sulfur dioxide (SO2) is a criteria air pollutant due to its contributions to aerosol formation, rainfall acidification, and harm to human health. The placement of air quality monitoring sites is typically biased towards urban areas, leaving large areas with very limited monitoring data. The Ozone Monitoring Instrument (OMI) has been used to provide estimates of SO2 vertical column densities (VCDs) globally at spatial resolution of 10s of kms once per day. OMI SO2 VCDs have been previously used to estimate surface SO2 concentrations using chemical transport model (CTM) simulations. The CTMs use estimated emissions and assimilated meteorological data, and simulate the chemical and physical processes that determine the vertical profile of SO2, which can be used to derive a ratio between the surface concentrations and VCDs. These models are complex, computationally expensive, and have large uncertainties in the simulated surface-to-VCD ratio due to biases in emissions and relatively coarse resolution. Machine learning techniques are comparatively easier to use, much less computationally expensive to use after training, and can produce more accurate estimations of surface concentrations than the CTM-based method. The interpretation of machine learning models often poses challenges, and in some cases, non-physical variables unrelated to SO2 are used as predictors. In this work, we create an artificial neural network (ANN) to relate OMI retrievals and archived GEOS-FP boundary layer heights to surface SO2 concentrations from the ChinaHighAirPollutants ChinaHighSO2 dataset (CHAP; Wei et al., 2023) on a seasonal average timescale from 2013-2018. Our model only utilizes five variables that are directly relevant to the satellite retrieval, lifetime, and spatial distribution of SO2. The model was trained on 16 seasons (four of each) with independent validation (one of each season) and testing datasets (one of each season) to avoid overfitting. Our ANN generates surface SO2 concentrations that are sensitive (slope = 0.51) and consistent (r = 0.74) with the CHAP data, but are underpredicted by an average of 1.2 ppbv with a mean absolute error of 2.2 ppbv. These results are better than recent studies utilizing the CTM method. To our knowledge, this is the best performing machine learning model that only uses physical variables to predict surface SO2. Our work demonstrates that a carefully constructed, simple ML model can accurately estimate surface-based SO2 concentrations from satellite VCD measurements, and this technique has future promise to expend to newer, higher resolution satellites and other air pollutants.

SO2, air quality, OMI, machine learning↗
NASA NTRS2019

Disentangling the Drivers of the Summertime Ozone‐Temperature Relationship Over the United States

Summertime surface-level ozone (O3 ) is known to vary with temperature, but the relative roles of different processes responsible for causing the O3 -temperature relationship are not well quantified. In this study we use simulations of NASA's Global Modeling Initiative (GMI) chemical transport model (CTM) to isolate and assess the relative impact of atmospheric transport, chemistry, and emissions on O3 variability, events, and its correlation with temperature. Using observations from CASTNet in the contiguous United States, we show that the GMI CTM reproduces the spatiotemporal variability of O3 and the O3 -temperature relationship during the summer. We primarily focus on the total change in O3 due to a change in temperature (d O3 /d T). In regions with strong positive correlations between temperature and O3 such as the Northeast, Great Lakes, and Great Plains, temperature's association with transport primarily drives d O3 /d T with smaller contributions from temperature-dependent chemistry and anthropogenic emissions. There are regions, however, with near-zero correlation between temperature and O3 , and our findings suggest that transport is still an important driver of O3 variability in these regions, albeit not correlated with temperature. Transport is not directly dependent on temperature but rather is linked through an indirect association, and it is therefore important to understand the exact mechanisms that link transport to O3 and how these mechanisms will change in a warming world.

ozone, temperature, CTM↗
DOE OSTI2024

A Vertically Resolved Canopy Improves Chemical Transport Model Predictions of Ozone Deposition to North Temperate Forests

Abstract Dry deposition is the second largest tropospheric ozone (O 3 ) sink and occurs through stomatal and nonstomatal pathways. Current O 3 uptake predictions are limited by the simplistic big‐leaf schemes commonly used in chemical transport models (CTMs) to parameterize deposition. Such schemes fail to reproduce observed O 3 fluxes over terrestrial ecosystems, highlighting the need for more realistic treatment of surface‐atmosphere exchange in CTMs. We address this need by linking a resolved canopy model (1D Multi‐Layer Canopy CHemistry and Exchange Model, MLC‐CHEM) to the GEOS‐Chem CTM and use this new framework to simulate O 3 fluxes over three north temperate forests. We compare results with in situ measurements from four field studies and with standalone, observationally constrained MLC‐CHEM runs to test current knowledge of O 3 deposition and its drivers. We show that GEOS‐Chem overpredicts observed O 3 fluxes across all four studies by up to 2×, whereas the resolved‐canopy models capture observed diel profiles of O 3 deposition and in‐canopy concentrations to within 10%. Relative humidity and solar irradiance are strong O 3 flux drivers over these forests, and uncertainties in those fields provide the largest remaining source of model deposition biases. Flux partitioning analysis shows that: (a) nonstomatal loss accounts for 60% of O 3 deposition on average; (b) in‐canopy chemistry makes only a small contribution to total O 3 fluxes; and (c) the CTM big‐leaf treatment overestimates O 3 ‐driven stomatal loss and plant phytotoxicity in these temperate forests by up to 7×. Results motivate the application of fully online vertically explicit canopy schemes in CTMs for improved O 3 predictions.

Vermeuel, Michael P. [Department of Soil, Water, a↗
DOE OSTI2025

Implications of reduced-complexity aerosol thermodynamics on organic aerosol mass concentration and composition over North America

Atmospheric organic aerosol (OA) mass concentrations can be affected by water uptake through its impact on the gas–particle partitioning of semi-volatile compounds. Current chemical transport models (CTMs) neglect this process. We have implemented the Binary Activity Thermodynamics model coupled to a volatility basis set partitioning scheme in the GEOS-Chem CTM, providing an efficient reduced-complexity OA model that predicts relative-humidity-dependent mixing and partitioning thermodynamics, while limiting the impact on computational efficiency. We provide a quantitative assessment of this water-sensitive OA treatment, focusing on a subdomain over North America. The updated OA scheme predicts a spatiotemporal mean enhancement in surface-level OA mass concentration of 145 % for January 2019 and 76 % for July 2019 compared to GEOS-Chem's most advanced OA scheme. The temporal mean surface-level OA organic mass concentration can increase by up to ∼590 % for January 2019 and ∼280 % for July 2019, with the greatest enhancements occurring over the ocean. The updated OA scheme also quantifies the OA-associated water content. The simulations show how different OA precursors and related OA surrogates contribute and respond to water uptake, including that due to changes in temperature and relative humidity over the diurnal cycle in selected winter and summer months. These results are independent of future CTM improvements involving updates to chemical reaction schemes and emission inventories. Our water-sensitive OA scheme allows for a better representation of the seasonal and regional variations in OA mass concentration in CTMs.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1990

Global impact of the Antarctic ozone hole - Dynamical dilution with a three-dimensional chemical transport model

The hypothesis that, once the Antarctic ozone hole is photochemically generated in the spring, the ozone deficit remains in the stratosphere throughout the year was investigated using a three-dimensional chemical transport model (CTM) for the stratosphere with linearized ozone chemistry. An Antarctic ozone hole was imposed on the basis of observations, and the dynamical dilution of the ozone-depleted air was followed for the next 12 months. The CTM calculations show that the transport of ozone-poor air from the Antarctic vortex results in measurable decreases to column ozone, extending to 30 deg S during the austral summer. By the end of the year, about 70 percent of the initially prescribed ozone deficit is replenished through stratospheric chemistry.

Prather, Michael↗
NASA NTRS1991

A comparison of three time-dependent wave packet methods for calculating electron-atom elastic scattering cross sections

Three time-dependent wave packet methods for performing elastic scattering calculations from screened Coulomb potentials are compared. The three methods are the time-dependent amplitude density method (TDADM), a Cayley-transform method (CTM), and the Chebyshev propagation method of Tal-Ezer and Kosloff. Both the TDADM and the CTM are based on a time-dependent integral equation for the wave function. In the first, the time-dependent amplitude density is propagated, while in the other two, the wave function is propagated. As a numerical example, phase shifts and cross sections are calculated using a screened Coulomb, Yukawa type potential over the range 200-1000 eV. It is found that, in most cases, all three methods yield comparable accuracy and are about equally efficient computationally. However for l = 0, where the Coulomb well is not screened by the centrifugal potential, the TDADM requires smaller grid spacings to maintain accuracy.

Judson, Richard S.↗
NASA NTRS1992

Rate 8/9 coded 8-PSK system for downlink applications

An advanced Coded Trellis Modulation (CTM) System which achieves a 2 bits/s/Hz bandwidth efficiency at an information rate of 200 Mbit/s while minimizing satellite power requirements, was developed for downlink earth station applications. The CTM system employs a high-speed rate 8/9 convolutional code with Viterbi decoding and an 8-Phase Shift Keying (PSK) modem. The minimum Euclidean distance between the modulated waveforms corresponding to the information sequences are maximized in order to maximize the noise immunity of the system. Nyquist filters with a square-root of 40 percent roll-off are used at the transmit and receive sides of the modem in order to minimize intersymbol interference, adjacent channel interference, and distortion at the nonlinear satellite power amplifier. The use of a coded system here also minimizes the effects of co-channel interference. The developed performance of the hardware system was measured to achieve within 1.5 dB from theory at a bit error rate of 5 x 10(exp -7) over an additive white Gaussian noise channel.

Fang, Russell↗
NASA NTRS1999

Ozone Budgets from a Global Chemistry/ Transport Model and Comparison to Observations from POLARIS

The objective of the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) field mission was to obtain data to better characterize the summertime seasonal decrease of ozone at mid to high latitudes. The decrease in ozone occurs mainly in the lower stratosphere and is expected to result from in situ chemical destruction. Instrumented balloons and aircraft were used in POLARIS, along with satellites, to measure ozone and chemical species which are involved with stratospheric ozone chemistry. In order to close the seasonal ozone budget, however, ozone transport must also be estimated. Comparison to a global chemistry and transport model (CTM) of the stratosphere indicates how well the summertime ozone loss processes are simulated and thus how well we can predict the ozone response to changing amounts of chemical source gases. Moreover, the model gives insight into the possible relative magnitude of transport contributions to the seasonal ozone decline. Initial comparison to the Goddard CTM, which uses transport winds and temperatures from meteorological data assimilation, shows a high ozone bias in the model and an attenuated summertime ozone loss cycle. Comparison of the model chemical partitioning, and ozone catalytic loss rates to those derived from measurements shows fairly close agreement both at ER-2 altitudes (20 km) and higher. This suggests that the model transport is too active in resupplying ozone to the high latitude region, although chemistry failings cannot be completely ruled out. Comparison of ozone and related species will be shown along with a full diagnosis of the model ozone budget and its possible sources of error.

Kawa, S. Randy↗
NASA NTRS1998

Model Simulations of Ozone in the Summer Lower Stratosphere

The Goddard 3D chemistry and transport model (CTM) uses winds and temperatures from the Goddard Earth Observing System Data Assimilation System (GEOS DAS); thus CTM simulations can be compared directly with observations from satellite, balloon and aircraft. In general, aspects of these comparisons show remarkable agreement between observation and model. One significant difference is that the model ozone is high biased below the ozone peak. The bias is apparently largest at high latitudes during the summer months. At the same time, comparisons with HALOE observations show that at mid to high latitudes, the ozone mixing ratio peak appears persistently at a lower altitude than observed by HALOE; the peak mixing ratio is also overestimated by the model. Both transport and photochemistry are possible contributors to the biased ozone in the lower stratosphere - excessive downward motion would increase lower stratospheric ozone, as would a too large vertical gradient in ozone. On the other hand, comparisons of model N2O and NOy with observations suggest transport deficiencies in the opposite sense, i.e., model N2O can be high relative to observations (particularly during winter), suggesting the need for stronger downward transport. Sensitivity studies have been carried out using parameterizations for ozone production and loss, NOy production and loss, and N2O loss. The goal of these studies is to clarify how problems in the photochemical scheme at and above the ozone peak influence the lower stratospheric ozone.

Douglass, Anne R.↗
NASA NTRS1998

Ozone Budgets from a Global Chemistry/Transport Model and Comparison to Observations from POLARIS

The objective of the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) field mission was to obtain data to better characterize the summertime seasonal decrease of ozone at mid to high latitudes. The decrease in ozone occurs mainly in the lower stratosphere and is expected to result from in situ chemical destruction. Instrumented balloons and aircraft were used in POLARIS, along with satellites, to measure ozone and chemical species which are involved with stratospheric ozone chemistry. In order to close the seasonal ozone budget, however, ozone transport must also be estimated. Comparison to a global chemistry and transport model (CTM) of the stratosphere indicates how well the summertime ozone loss processes are simulated and thus how well we can predict the ozone response to changing amounts of chemical source gases. Moreover, the model gives insight into the possible relative magnitude of transport contributions to the seasonal ozone decline. Initial comparison to the Goddard CTM, which uses transport winds and temperatures from meteorological data assimilation, shows a high ozone bias in the model and an attenuated summertime ozone loss cycle. Comparison of the model chemical partitioning and ozone catalytic loss rates to those derived from measurements shows fairly close agreement both at ER-2 altitudes (20 km) and higher. This suggests that the model transport is too active in resupplying ozone to the high latitude region, although chemistry failings cannot be completely ruled out. Comparison of ozone and related species will be shown along with a full diagnosis of the model ozone budget and its possible sources of error.

Kawa, S. Randolph↗
NASA NTRS1999

The Goddard Three Dimensional Chemistry and Transport Model-A Waystation on the Road to Predicting the Future of Stratospheric Ozone

The Goddard 3D Chemistry and Transport Model (CTM) is an off-line model which includes a full description of stratospheric photochemistry and calculates constituent transport using winds and temperatures from the Goddard Earth Observing System Data Assimilation System. The model can be used to understand and quantify the photochemical and transport processes which produce observed constituent evolution and variability. Data from any platform - ground based, aircraft, balloon, satellite - can play a role. Since any measurement systems has its own set of advantages and disadvantages (e.g., good temporal sampling but poor spatial sampling; good spatial and temporal sampling but poor vertical resolution; high vertical resolution and spatial sampling but poor temporal sampling), using data from disparate sources and a CTM can provide a more complete picture of atmospheric processes.

Douglass, Anne↗
NASA NTRS1997

A Three-Wave Model of the Stratosphere with Coupled Dynamics, Radiation and Photochemistry

A zonal mean chemistry transport model (2-D CTM) coupled with a semi-spectral dynamical model is used to simulate the distributions of trace gases in the present day atmosphere. The zonal-mean and eddy equations for the velocity and the geopotential height are solved in the semi-spectral dynamical model. The residual mean circulation is derived from these dynamical variables and used to advect the chemical species in the 2- D CTM. Based on a linearized wave transport equation, the eddy diffusion coefficients for chemical tracers are expressed in terms of the amplitude, frequency and growth rate of dynamical waves; local chemical loss rates; and a time constant parameterizing small scale mixing. The contributions to eddy flux are from the time varying wave amplitude (transient eddy), chemical reactions (chemical eddy) and small scale mixing. In spite of the high truncation in the dynamical module (only three longest waves are resolved), the model has simulated many observed characteristics of stratospheric dynamics and distribution of chemical species including ozone. Compared with the values commonly used in 2-D CTMs, the eddy diffusion coefficients for chemical species calculated in this model are smaller, especially in the subtropics. It is also found that the chemical eddy diffusion has only a small effects in determining the distribution of most slow species, including ozone in the stratosphere.

Shia, Run-Lie↗
NASA NTRS2000

The Sensitivity of Model Ozone to Advective and Photochemical Processes in the High Latitude Winter Lower Stratosphere

Three dimensional chemistry and transport models (CTMs) contain a set of coupled continuity equations which describe the evolution of constituents such as ozone and other minor species which affect ozone. Both advection and photochemical processes contribute to constituent evolution, and a CTM provides a means to evaluate these contributions separately. Such evaluation is particularly useful when both terms are important to the modeled tendency. An example is the ozone tendency in the high latitude winter lower stratosphere, where advection tends to increase ozone, and catalytic processes involving chlorine radicals tend to decrease ozone. The Goddard three dimensional chemistry and transport model uses meteorological fields from the Goddard Earth Observing System Data Assimilation System, thus the modeled ozone evolution may reproduce the observed evolution and provide a test of the model representation of photochemical processes if the transport is shown to be modeled appropriately. We have investigated the model advection further using diabatic trajectory calculations. For long lived constituents such as N2O, the model field for a particular time on a potential temperature surface is compared with a field produced by calculating 15 day back trajectories for a fixed latitude longitude grid, and mapping model N2O at the terminus of the back trajectories onto the initial grid. This provides a quantitative means to evaluate two aspects of the CTM transport: one, the model horizontal gradient between middle latitudes and the polar vortex is compared with the gradient produced using the non-diffusive trajectory calculation; two, the model vertical advection, which is produced by the divergence of the horizontal winds, is compared with the vertical transport expected from diabatic cooling.

Douglass, A.↗
NASA NTRS2001

The Interaction Between Dynamics and Chemistry of Ozone in the Set-up Phase of the Northern Hemisphere Polar Vortex

The morphology and evolution of the stratospheric ozone (O3) distribution at high latitudes in the Northern Hemisphere (NH) are examined for the late summer and fall seasons of 1999. This time period sets the O3 initial condition for the SOLVE/THESEO field mission performed during winter 1999-2000. In situ and satellite data are used along with a three-dimensional model of chemistry and transport (CTM) to determine the key processes that control the distribution of O3 in the lower-to-middle stratosphere. O3 in the vortex at the beginning of the winter season is found to be nearly constant from 500 to above 800 K with a value at 3 ppmv +/- approx. 10%. Values outside the vortex are up to a factor of 2 higher and increase significantly with potential temperature. The seasonal time series of data from POAM shows that relatively low O3 mixing ratios, which characterize the vortex in late fall, are already present at high latitudes at the end of summer before the vortex circulation sets up. Analysis of the CTM output shows that the minimum O3 and increase in variance in late summer are the result of: 1) stirring of polar concentric O3 gradients by nascent wave-driven transport, and 2) an acceleration of net photochemical loss with decreasing solar illumination. The segregation of low O3 mixing ratios into the vortex as the circulation strengthens through the fall suggests a possible feedback role between O3 chemistry and the vortex formation dynamics. Trajectory calculations from O3 sample points early in the fall, however, show only a weak correlation between initial O3 mixing ratio and potential vorticity later in the season consistent with order-of-magnitude calculations for the relative importance of O3 in the fall radiative balance at high latitudes. The possible connection between O3 chemistry and the dynamics of vortex formation does suggest that these feedbacks and sensitivities need to be better understood in order to make confident predictions of the recovery of NH O3.

Kawa, S. R.↗
NASA NTRS2003

The 2002 Antarctic Ozone Hole

Since 1979, the ozone hole has grown from near zero size to over 24 Million km2. This area is most strongly controlled by levels of inorganic chlorine and bromine oncentrations. In addition, dynamical variations modulate the size of the ozone hole by either cooling or warming the polar vortex collar region. We will review the size observations, the size trends, and the interannual variability of the size. Using a simple trajectory model, we will demonstrate the sensitivity of the ozone hole to dynamical forcing, and we will use these observations to discuss the size of the ozone hole during the 2002 Austral spring. We will further show how the Cly decreases in the stratosphere will cause the ozone hole to decrease by 1-1.5% per year. We will also show results from a 3-D chemical transport model (CTM) that has been continuously run since 1999. These CTM results directly show how strong dynamics acts to reduce the size of the ozone hole.

Newman, P. A.↗
NASA NTRS2004

Sensitivity of the FVGCM to Changes in Ozone

We have carried out an experiment with the finite volume general circulation model (FVGCM). This experiment consisted of two different imposed changes in the climatological ozone fields assumed in the radiation code. for conditions with no significant ozone hole. This distribution was obtained from a 50-year simulation of the full stratospheric ozone chemistry, with a time-dependent chlorine loading, done with our off-line chemical transport model (CTM). Three years (1978-1980) of this simulation were averaged to form a monthly, zonal-mean ozone distribution that was used in the 20-year integration of the FVGCM for "unperturbed" conditions. The second 20-year GCM integration included a fully-developed ozone hole. This ozone distribution was from three years, 1998-2000, from the same CTM simulation. The goal of this work is to determine the coupled response of the chemistry and dynamics of the stratosphere. These experiments are the first step in understanding the coupled response. An important initial question concerns the significance of the signals: if 20-year integrations turn out to be too short, the runs will be extended.

Stolarski↗
NASA NTRS2005

Trends from the Long-term Data Record and Models: What Do They Tell Us About our Ability to Predict Ozone Recovery?

Our industrial society has performed an experiment on the stratospheric ozone layer over the last several decades. The initial part of this experiment was the rapidly increasing release of halogen-containing compounds that carry chlorine and bromine to the stratosphere where they can cause a loss of ozone. The present part of this experiment is the implementation of the Montreal Protocol, which has led to a leveling off of these halogen compounds and the beginning of their slow removal from the atmosphere. The observation and attribution of ozone response to the halogens has been a particularly important and difficult task because of the impact of solar cycle uv variation, two major volcanic eruptions (El Chichon and Pinatubo), and interannual dynamic variability of the stratosphere. We have run 3 different simulations of the chemistry and transport of ozone and the minor constituents that affect ozone to help evaluate our understanding of the causes of ozone change and to assess our ability to predict ozone recovery with the removal of halogens from the stratosphere. One simulation, using the Goddard chemical transport model (CTM), had interannual variability in the dynamics for the entire 50 years of simulation, which included the past 3 decades (1974-2004) and the next 2 decades to 2022. The other two simulations used the Global Modeling Initiative (GMI) CTM with no dynamical variability: one used a the winds and temperatures from a repeating warm Arctic winter and the other used a repeating cold Arctic winter. All simulations included the effects of aerosol surfaces from volcanic eruptions on chemical reactions as well as the variation in UV over the 11-year solar cycle.

Strahan, Susan↗
NASA NTRS2009

The Impact of Tropical Recirculation on Polar Composition

We derive the tropical modal age of air from an analysis of the water vapor tape recorder. We combine the observationally derived modal age with mean age of air from CO2 and SF6 to create diagnostics for the independent evaluation of the vertical transport rate and horizontal recirculation into the tropics between 16-32 km. These diagnostics are applied to two Global Modeling Initiative (GMI) chemistry and transport model (CTM) age tracer simulations to give new insights into the tropical transport characteristics of the meteorological fields from the GEOS4-GCM and the GEOS4-DAS. Both simulations are found to have modal ages that are in reasonable agreement with the empirically derived age (i.e ., transit times) over the entire altitude range. Both simulations show too little horizontal recirculation into the tropics above 22 km, with the GEOS4-DAS fields having greater recirculation. Using CH4 as a proxy for mean age, comparisons between HALOE and model CH4 in the Antarctic demonstrate how the strength of tropical recirculation affects polar composition in both CTM experiments. Better tropical recirculation tends to improve the CH4 simulation in the Antarctic. However, mean age in the Antarctic lower stratosphere can be compromised by poor representation of tropical ascent, tropical recirculation, or vortex barrier strength. The connection between polar and tropical composition shown in this study demonstrates the importance of diagnosing each of these processes separately in order to verify the adequate representation of the processes contributing to polar composition in models.

Strahan, S. E.↗