We have constructed an atmospheric inversion framework based on TM5-4DVAR to jointly assimilate measurements of methane and δC-13 of methane in order to estimate source-specific methane emissions. ...Here we present global emission estimates from this framework for the period 1999–2016. We assimilate a newly constructed, multi-agency database of CH4 and δC-13 measurements. We find that traditional CH4-only atmospheric inversions are unlikely to estimate emissions consistent with atmospheric δC-13 data and assimilating δC-13 data is necessary to derive emissions consistent with both measurements. Our framework attributes ca. 85% of the post-2007 growth in atmospheric methane to microbial sources, with about half of that coming from the tropics between 23.5° N and 23.5° S. This contradicts the attribution of the recent growth in the methane budget of the Global Carbon Project (GCP). We find that the GCP attribution is only consistent with our top-down estimate in the absence of δC-13 data. We find that at global and continental scales, δC-13 data can separate microbial from fossil methane emissions much better than CH4 data alone, and at smaller scales this ability is limited by the current δC-13 measurement coverage. Finally, we find that the largest uncertainty in using δC-13 data to separate different methane source types comes from our knowledge of atmospheric chemistry, specifically the distribution of tropospheric chlorine and the isotopic discrimination of the methane sink.
High levels of fine particulate matter (PM2.5) pollution in East Asia often exceed local air quality standards. Observations from the Korea United States-Air Quality (KORUS-AQ) field campaign in May ...and June 2016 showed that development of extreme pollution (haze) occurred through a combination of long-range transport and favorable meteorological conditions that enhanced local production of PM2.5. Atmospheric models often have difficulty simulating PM2.5 chemical composition during haze, which is of concern for the development of successful control measures. We use observations from KORUS-AQ to examine the ability of the GEOS-Chem chemical transport model to simulate PM2.5 composition throughout the campaign and identify the mechanisms driving the pollution event. At the surface, the model underestimates sulfate by -64% but overestimates nitrate by +36%. The largest underestimate in sulfate occurs during the pollution event, where models typically struggle to generate elevated sulfate concentrations due to missing heterogeneous chemistry in aerosol liquid water in the polluted boundary layer. Hourly surface observations show that the model nitrate bias is driven by an overestimation of the nighttime peak. In the model, nitrate formation is limited by the supply of nitric acid, which is biased by +100% against aircraft observations. We hypothesize that this is due to a large missing sink, which we implement here as a factor of five increase in dry deposition. We show that the resulting increased deposition velocity is consistent with observations of total nitrate as a function of photochemical age. The model does not account for factors such as the urban heat island effect or the heterogeneity of the built-up urban landscape resulting in insufficient model turbulence and surface area over the study area that likely results in insufficient dry deposition. Other species such as NH3 could be similarly affected but were not measured during the campaign. Nighttime production of nitrate is driven by NO2 hydrolysis in the model, while observations show that unexpectedly elevated nighttime ozone (not present in the model) should result in N2O5 hydrolysis as the primary pathway. The model is unable to represent nighttime ozone due to an overly rapid collapse of the afternoon mixed layer and excessive titration by NO. We attribute this to missing nighttime heating driving deeper nocturnal mixing that would be expected to occur in a city like Seoul. This urban heating is not considered in air quality models run at large enough scales to treat both local chemistry and long-range transport. Key model failures in simulating nitrate, mainly overestimated daytime nitric acid, incorrect representation of nighttime chemistry, and an overly shallow and insufficiently turbulent nighttime mixed layer, exacerbate the model’s inability to simulate the buildup of PM2.5 during haze pollution. To address the underestimate in sulfate most evident during the haze event, heterogeneous aerosol uptake of SO2 is added to the model which previously only considered aqueous production of sulfate from SO2 in cloud water. Implementing a simple parameterization of this chemistry improves the model abundance of sulfate but degrades the SO2 simulation implying that emissions are underestimated. We find that improving model simulations of sulfate has direct relevance to determining local vs. transboundary contributions to PM2.5. During the haze pollution event, the inclusion of heterogeneous aerosol uptake of SO2 decreases the fraction of PM2.5 attributable to long-range transport from 66% to 54%. Locally-produced sulfate increased from 1% to 25% of locally-produced PM2.5, implying that local emissions controls would have a larger effect than previously thought. However, this additional uptake of SO2 is coupled to the model nitrate prediction which affects the aerosol liquid water abundance and chemistry driving sulfate-nitrate-ammonium partitioning. An additional simulation of the haze pollution with heterogeneous uptake of SO2 to aerosol and simple improvements to the model nitrate simulation results in 30% less sulfate due to 40% less nitrate and aerosol water, and results in an underestimate of sulfate during the haze event. Future studies need to better consider the impact of model physical processes such as dry deposition and nighttime boundary layer mixing on the simulation of nitrate and the effect of improved nitrate simulations on the overall simulation of secondary inorganic aerosol (sulfate+nitrate+ammonium) in East Asia. Foreign emissions are rapidly changing, increasing the need to understand the impact of local emissions on PM2.5 in South Korea to ensure continued air quality improvements.
Here we use satellite observations of formaldehyde (HCHO)vertical column densities (VCD) from the TROPOspheric Monitoring Instrument (TROPOMI), aircraft measurements, combined with a nested regional ...chemical transport model (GEOS-Chem at 0.5°×0.625° resolution), to understand the variability and sources of summertime HCHO better in Alaska. We first evaluate GEOS-Chem with in-situ airborne measurements during Atmospheric Tomography Mission 1 (ATom-1) aircraft campaign. We show reasonable agreement between observed and modeled HCHO, isoprene, monoterpenes and the sum of methyl vinyl ketone and methacrolein (MVK+MACR) in continental boundary layer. In particular, HCHO profiles show spatial homogeneity in Alaska, suggesting a minor contribution of biogenic emissions to HCHO VCD. We further examine the TROPOMI HCHO product in Alaska summer, reprocessed by GEOS-Chem model output for a priori profiles and shape factors. For the year with low wildfire activity (e.g.,2018), we find that HCHO VCDs are largely dominated by background HCHO (58-71%), with minor contributions from wildfires (20-32%) and biogenic VOC emissions (8-10%). For the year with intense wildfires (e.g.,2019), summertime HCHO VCD is dominated by wildfire emissions (50-72%), with minor contributions from background (22-41%) and biogenic VOCs (6-10%). In particular, the model indicates a major contribution of wildfires from direct emissions of HCHO, instead of secondary production of HCHO from oxidation of larger VOCs. We find that the column contributed by biogenic VOC is often small and below the TROPOMI detection limit, in part due to the slow HCHO production from isoprene oxidation under low NOx conditions. This work highlights challenges for quantifying HCHO and its precursors in remote pristine regions.
Wildfires pose increasing risks to human health and properties in North America. Due to large uncertainties in fire emission, transport, and chemical transformation, it remains challenging to ...accurately predict air quality during wildfire events, hindering our collective capability to issue effective early warnings to protect public health and welfare. Here we present a new real-time Hazardous Air Quality Ensemble System (HAQES) by leveraging various wildfire smoke forecasts from three U.S. federal agencies (NOAA, NASA, and Navy). Compared to individual models, the HAQES ensemble forecast significantly enhances forecast accuracy. To further enhance forecasting performance, a weighted ensemble forecast approach was introduced and tested. Compared to the unweighted ensemble mean, the multilinear regression weighted ensemble reduced fractional bias by 34% in the major fire regions, false alarm rate by 72%, and increased hit rate by 17%. Finally, we improved the weighted ensemble using quantile regression and weighted regression methods to enhance the forecast of extreme air quality events. The advanced weighted ensemble increased the PM2.5 exceedance hit rate by 55% compared to the ensemble mean. Our findings provide insights into the development of advanced ensemble forecast methods for wildfire air quality, offering a practical way to enhance decision-making support to protect public health.
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DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Low-cost sensors for particulate matter mass (PM) enable spatially dense, high temporal resolution measurements of air quality that traditional reference monitoring cannot. Low-cost PM sensors are ...especially beneficial in low and middle-income countries where few, if any, reference grade measurements exist and in areas where the concentration fields of air pollutants have significant spatial gradients. Unfortunately, low-cost PM sensors also come with a number of challenges that must be addressed if their data products are to be used for anything more than a qualitative characterization of air quality. The various PM sensors used in low-cost monitors are all subject to biases and calibration dependencies, corrections for which range from relatively straightforward(e.g. meteorology, age of sensor) to complex (e.g. aerosol source, composition, refractive index). The methods for correcting and calibrating these biases and dependencies that have been used in the literature likewise range from simple linear and quadratic models to complex machine learning algorithms. Here we review the needs and challenges when trying to get high-quality data from low-cost sensors. We also present a set of best practices to follow to obtain high-quality data from these low-cost sensors.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Changing emissions of NOx and other ozone precursors drive trends in both production and loss of surface ozone, leading to surface ozone trends that differ according to the time of day. Consequently, ...the magnitude of the diurnal cycle in surface ozone is changing in several regions of the world. Changes in the diurnal cycle of ozone have implications for the metrics used to assess the impact of ozone on human health and vegetation, since different metrics are sensitive to different portions of the diurnal cycle. We use a high resolution model simulation to examine global changes in the magnitude of the diurnal cycle of O3 between 1980 and 2015. The simulation reproduces the negative trends in the tropospheric NO2 column over the eastern United States and Europe, and the positive trends over East Asia, seen by the Ozone Monitoring Instrument (OMI). It also gives a reasonable reproduction of the change in the diurnal cycle of surface ozone seen at rural sites in the eastern United States between the 1990s and 2000s. The simulation shows that the magnitude of the surface O3 diurnal cycle is increasing in regions with positive changes in NOx emissions, such as South and East Asia, and decreasing in regions with reductions in NOx emissions. It also shows changes in the diurnal cycle of the tropospheric ozone column, although these have fewer regions with statistically significant trends. These changes suggest that daily mean ozone is responding less than the mid-day ozone measured by the Total Ozone Mapping Spectrometer (TOMS) and OMI.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Air pollution in many of India's cities exceeds national and international standards, and effective pollution control strategies require knowledge of the sources that contribute to air pollution and ...their spatiotemporal variability. In this study, we examine the influence of a single pollution source, outdoor biomass burning, on particulate matter (PM) concentrations, surface visibility, and aerosol optical depth (AOD) from 2007 to 2013 in three of the most populous Indian cities. We define the upwind regions, or "airsheds," for the cities by using atmospheric back trajectories from the HYSPLIT model. Using satellite fire radiative power (FRP) observations as a measure of fire activity, we target pre-monsoon and post-monsoon fires upwind of the Delhi National Capital Region and pre-monsoon fires surrounding Bengaluru and Pune. We find varying contributions of outdoor fires to different air quality metrics. For the post-monsoon burning season, we find that a subset of local meteorological variables (air temperature, humidity, sea level pressure, wind speed and direction) and FRP as the only pollution source explained 39% of variance in Delhi station PM(sub 10) anomalies, 77% in visibility, and 30% in satellite AOD; additionally, per unit increase in FRP within the daily airshed (1000 MW), PM(sub 10) increases by 16.34 micrograms per cubic meter, visibility decreases by 0.097 km, and satellite AOD increases by 0.07. In contrast, for the pre-monsoon burning season, we find less significant contributions from FRP to air quality in all three cities. Further, we attribute 99% of FRP from post-monsoon outdoor fires within Delhi's average airshed to agricultural burning. Our work suggests that although outdoor fires are not the dominant air pollution source in India throughout the year, post-monsoon fires contribute substantially to regional air pollution and high levels of population exposure around Delhi. During 3-day blocks of extreme PM(sub 2.5) in the 2013 post-monsoon burning season, which coincided with statistically significant high fire activity, concentrations in Delhi averaged 304 micrograms per cubic meter, or more than 1000% above the 24-h PM(sub 2.5) guideline (25 micrograms per cubic meter) of the World Health Organization. These results suggest that providing viable alternatives to agricultural residue burning could help improve post-monsoon air quality for a growing population of 63 million (39% in urban areas) within Delhi's airshed.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
Atmospheric methane (CH4) concentrations have shown a puzzling resumption of growth since 2007 following a period of stabilization from 2000 to 2006. Multiple hypotheses have been proposed to explain ...the temporal variations in CH4 growth, which attributes the rise of atmospheric CH4 either to increases in emissions from fossil fuel activities, agriculture, and natural wetlands or to a decrease in the atmospheric chemical sink. Here, we use a comprehensive ensemble of CH4 source estimates and isotopic δ13C-CH4 source signature data to show that the resumption of CH4 growth is most likely due to increased anthropogenic emissions. Our emission scenarios that have the fewest biases with respect to isotopic composition suggest that the agriculture, landfill, and waste sectors were responsible for 53 ± 13% of the renewed growth over the period 2007–2017 compared to 2000–2006; industrial fossil fuel sources explained an additional 34 ± 24%, and wetland sources contributed the least at 13 ± 9%. The hypothesis that a large increase in emissions from natural wetlands drove the decrease in atmospheric δ13C-CH4 values cannot be reconciled with current process-based wetland CH4 models. This finding suggests the need for increased wetland measurements to better constrain the contemporary and future role of wetlands in the rise of atmospheric methane and climate feedbacks. Our findings highlight the predominant role of anthropogenic activities in driving the growth of atmospheric CH4 concentrations.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
Air pollution is a leading cause of global premature mortality and is especially prevalent in many low- and middle-income countries (LMICs). In sub-Saharan Africa, preliminary monitoring networks, ...satellite retrievals of air-quality-relevant species, and air quality models show ambient fine particulate matter (PM2.5) concentrations that far exceed the World Health Organization guidelines, yet many areas remain largely unmonitored and understudied. Deploying a network of five low-cost PurpleAir PM2.5 monitors over 2 years (2019–2021), we present the first multiyear ambient air pollution monitoring data results from Lomé, Togo, a major West African coastal city with a population of about 1.4 million people. The full-study time period network-wide mean measured daily PM2.5 concentration is 23.5 μg m–3 m–3. The strong regional influence of the dry and dusty Harmattan wind increases the local average PM2.5 concentration by up to 58% during December through February, but the diurnal and weekly trends in PM2.5 are largely controlled by local influences. At all sites, more than 87% of measured days exceeded the new WHO Daily PM2.5 guidelines; these first measurements highlight the need for air quality improvement in a rapidly growing urban metropolis.
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IJS, KILJ, NUK, PNG, UL, UM
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.
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IJS, KILJ, NUK, PNG, UL, UM
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