Transpacific Transport of Asian Peroxyacetyl Nitrate (PAN) Observed from Satellite: Implications for Ozone.

Peroxyacetyl nitrate (PAN) is produced in the atmosphere by photochemical oxidation of non-methane volatile organic compounds in the presence of nitrogen oxides (NOx), and it can be transported over long distances at cold temperatures before decomposing thermally to release NOx in the remote troposphere. It is both a tracer and a precursor for transpacific ozone pollution transported from East Asia to North America. Here, we directly demonstrate this transport with PAN satellite observations from the infrared atmospheric sounding interferometer (IASI). We reprocess the IASI PAN retrievals by replacing the constant prior vertical profile with vertical shape factors from the GEOS-Chem model that capture the contrasting shapes observed from aircraft over South Korea (KORUS-AQ) and the North Pacific (ATom). The reprocessed IASI PAN observations show maximum transpacific transport of East Asian pollution in spring, with events over the Northeast Pacific offshore from the Western US associated in GEOS-Chem with elevated ozone in the lower free troposphere. However, these events increase surface ozone in the US by less than 1 ppbv because the East Asian pollution mainly remains offshore as it circulates the Pacific High.

Ethylene industrial emitters seen from space.

Volatile organic compounds are emitted abundantly from a variety of natural and anthropogenic sources. However, in excess, they can severely degrade air quality. Their fluxes are currently poorly represented in inventories due to a lack of constraints from global measurements. Here, we track from space over 300 worldwide hotspots of ethylene, the most abundant industrially produced organic compound. We identify specific emitters associated with petrochemical clusters, steel plants, coal-related industries, and megacities. Satellite-derived fluxes reveal that the ethylene emissions of the industrial sources are underestimated or missing in the state-of-the-art Emission Database for Global Atmospheric Research (EDGAR) inventory. This work exposes global emission point-sources of a short-lived carbonated gas, complementing the ongoing large-scale efforts on the monitoring of inorganic pollutants.

On the weekly cycle of atmospheric ammonia over European agricultural hotspots.

The presence of a weekly cycle in the abundance of an atmospheric constituent is a typical fingerprint for the anthropogenic nature of its emission sources. However, while ammonia is mainly emitted as a consequence of human activities, a weekly cycle has never been detected in its abundances at large scale. We expose here for the first time the presence of a weekend effect in the NH3 total columns measured by the IASI satellite sounder over the main agricultural source regions in Europe: northwestern Europe (Belgium-the Netherlands-northwest Germany), the Po Valley, Brittany, and, to a lesser extent, the Ebro Valley. A decrease of 15% relative to the weekly mean is seen on Sunday-Monday observations in northwestern Europe, as a result of reduced NH3 emissions over the weekend. This is confirmed by in situ NH3 concentration data from the National Air Quality Monitoring Network in the Netherlands, where an average reduction of 10% is found around midnight on Sunday. The identified weekend effect presents a strong seasonal variability, with two peaks, one in spring and one in summer, coinciding with the two main (manure) fertilization periods. In spring, a reduction on Sunday-Monday up to 53 and 26% is found in the NH3 satellite columns and in situ concentrations, respectively, as fertilization largely drives atmospheric NH3 abundances at this time of the year.

Rapid rise in premature mortality due to anthropogenic air pollution in fast-growing tropical cities from 2005 to 2018.

Tropical cities are experiencing rapid growth but lack routine air pollution monitoring to develop prescient air quality policies. Here, we conduct targeted sampling of recent (2000s to 2010s) observations of air pollutants from space-based instruments over 46 fast-growing tropical cities. We quantify significant annual increases in nitrogen dioxide (NO2) (1 to 14%), ammonia (2 to 12%), and reactive volatile organic compounds (1 to 11%) in most cities, driven almost exclusively by emerging anthropogenic sources rather than traditional biomass burning. We estimate annual increases in urban population exposure to air pollutants of 1 to 18% for fine particles (PM2.5) and 2 to 23% for NO2 from 2005 to 2018 and attribute 180,000 (95% confidence interval: -230,000 to 590,000) additional premature deaths in 2018 (62% increase relative to 2005) to this increase in exposure. These cities are predicted to reach populations of up to 80 million people by 2100, so regulatory action targeting emerging anthropogenic sources is urgently needed.

Monthly Patterns of Ammonia Over the Contiguous United States at 2-km Resolution.

Monthly, high-resolution (∼2 km) ammonia (NH3) column maps from the Infrared Atmospheric Sounding Interferometer (IASI) were developed across the contiguous United States and adjacent areas. Ammonia hotspots (95th percentile of the column distribution) were highly localized with a characteristic length scale of 12 km and median area of 152 km2. Five seasonality clusters were identified with k-means++ clustering. The Midwest and eastern United States had a broad, spring maximum of NH3 (67% of hotspots in this cluster). The western United States, in contrast, showed a narrower midsummer peak (32% of hotspots). IASI spatiotemporal clustering was consistent with those from the Ammonia Monitoring Network. CMAQ and GFDL-AM3 modeled NH3 columns have some success replicating the seasonal patterns but did not capture the regional differences. The high spatial-resolution monthly NH3 maps serve as a constraint for model simulations and as a guide for the placement of future, ground-based network sites.

Industrial and agricultural ammonia point sources exposed.

Through its important role in the formation of particulate matter, atmospheric ammonia affects air quality and has implications for human health and life expectancy1,2. Excess ammonia in the environment also contributes to the acidification and eutrophication of ecosystems3-5 and to climate change6. Anthropogenic emissions dominate natural ones and mostly originate from agricultural, domestic and industrial activities7. However, the total ammonia budget and the attribution of emissions to specific sources remain highly uncertain across different spatial scales7-9. Here we identify, categorize and quantify the world's ammonia emission hotspots using a high-resolution map of atmospheric ammonia obtained from almost a decade of daily IASI satellite observations. We report 248 hotspots with diameters smaller than 50 kilometres, which we associate with either a single point source or a cluster of agricultural and industrial point sources-with the exception of one hotspot, which can be traced back to a natural source. The state-of-the-art EDGAR emission inventory10 mostly agrees with satellite-derived emission fluxes within a factor of three for larger regions. However, it does not adequately represent the majority of point sources that we identified and underestimates the emissions of two-thirds of them by at least one order of magnitude. Industrial emitters in particular are often found to be displaced or missing. Our results suggest that it is necessary to completely revisit the emission inventories of anthropogenic ammonia sources and to account for the rapid evolution of such sources over time. This will lead to better health and environmental impact assessments of atmospheric ammonia and the implementation of suitable nitrogen management strategies.

Monitoring emissions from the 2015 Indonesian fires using CO satellite data.

Southeast Asia, in particular Indonesia, has periodically struggled with intense fire events. These events convert substantial amounts of carbon stored as peat to atmospheric carbon dioxide (CO2) and significantly affect atmospheric composition on a regional to global scale. During the recent 2015 El Niño event, peat fires led to strong enhancements of carbon monoxide (CO), an air pollutant and well-known tracer for biomass burning. These enhancements were clearly observed from space by the Infrared Atmospheric Sounding Interferometer (IASI) and the Measurements of Pollution in the Troposphere (MOPITT) instruments. We use these satellite observations to estimate CO fire emissions within an inverse modelling framework. We find that the derived CO emissions for each sub-region of Indonesia and Papua are substantially different from emission inventories, highlighting uncertainties in bottom-up estimates. CO fire emissions based on either MOPITT or IASI have a similar spatial pattern and evolution in time, and a 10% uncertainty based on a set of sensitivity tests we performed. Thus, CO satellite data have a high potential to complement existing operational fire emission estimates based on satellite observations of fire counts, fire radiative power and burned area, in better constraining fire occurrence and the associated conversion of peat carbon to atmospheric CO2 A total carbon release to the atmosphere of 0.35-0.60 Pg C can be estimated based on our results.This article is part of a discussion meeting issue 'The impact of the 2015/2016 El Niño on the terrestrial tropical carbon cycle: patterns, mechanisms and implications'.

Ammonia Emissions May Be Substantially Underestimated in China.

China is a global hotspot of atmospheric ammonia (NH3) emissions and, as a consequence, very high nitrogen (N) deposition levels are documented. However, previous estimates of total NH3 emissions in China were much lower than inference from observed deposition values would suggest, highlighting the need for further investigation. Here, we reevaluated NH3 emissions based on a mass balance approach, validated by N deposition monitoring and satellite observations, for China for the period of 2000 to 2015. Total NH3 emissions in China increased from 12.1 ± 0.8 Tg N yr-1 in 2000 to 15.6 ± 0.9 Tg N yr-1 in 2015 at an annual rate of 1.9%, which is approximately 40% higher than existing studies suggested. This difference is mainly due to more emission sources now having been included and NH3 emission rates from mineral fertilizer application and livestock having been underestimated previously. Our estimated NH3 emission levels are consistent with the measured deposition of NHx (including NH4+ and NH3) on land (11-14 Tg N yr-1) and the substantial increases in NH3 concentrations observed by satellite measurements over China. These findings substantially improve our understanding on NH3 emissions, implying that future air pollution control strategies have to consider the potentials of reducing NH3 emission in China.

Remote sensing and in situ measurements of methane and ammonia emissions from a megacity dairy complex: Chino, CA.

Methane (CH4) and ammonia (NH3) directly and indirectly affect the atmospheric radiative balance with the latter leading to aerosol generation. Both have important spectral features in the Thermal InfraRed (TIR) that can be studied by remote sensing, with NH3 allowing discrimination of husbandry from other CH4 sources. Airborne hyperspectral imagery was collected for the Chino Dairy Complex in the Los Angeles Basin as well as in situ CH4, carbon dioxide (CO2) and NH3 data. TIR data showed good spatial agreement with in situ measurements and showed significant emissions heterogeneity between dairies. Airborne remote sensing mapped plume transport for ∼20 km downwind, documenting topographic effects on plume advection. Repeated multiple gas in situ measurements showed that emissions were persistent on half-year timescales. Inversion of one dairy plume found annual emissions of 4.1 × 105 kg CH4, 2.2 × 105 kg NH3, and 2.3 × 107 kg CO2, suggesting 2300, 4000, and 2100 head of cattle, respectively, and Chino Dairy Complex emissions of 42 Gg CH4 and 8.4 Gg NH3 implying ∼200k cows, ∼30% more than Peischl et al. (2013) estimated for June 2010. Far-field data showed chemical conversion and/or deposition of Chino NH3 occurs within the confines of the Los Angeles Basin on a four to six h timescale, faster than most published rates, and likely from higher Los Angeles oxidant loads. Satellite observations from 2011 to 2014 confirmed that observed in situ transport patterns were representative and suggests much of the Chino Dairy Complex emissions are driven towards eastern Orange County, with a lesser amount transported to Palm Springs, CA. Given interest in mitigating husbandry health impacts from air pollution emissions, this study highlights how satellite observations can be leveraged to understand exposure and how multiple gas in situ emissions studies can inform on best practices given that emissions reduction of one gas could increase those of others.

Towards a climate-dependent paradigm of ammonia emission and deposition.

Existing descriptions of bi-directional ammonia (NH3) land-atmosphere exchange incorporate temperature and moisture controls, and are beginning to be used in regional chemical transport models. However, such models have typically applied simpler emission factors to upscale the main NH3 emission terms. While this approach has successfully simulated the main spatial patterns on local to global scales, it fails to address the environment- and climate-dependence of emissions. To handle these issues, we outline the basis for a new modelling paradigm where both NH3 emissions and deposition are calculated online according to diurnal, seasonal and spatial differences in meteorology. We show how measurements reveal a strong, but complex pattern of climatic dependence, which is increasingly being characterized using ground-based NH3 monitoring and satellite observations, while advances in process-based modelling are illustrated for agricultural and natural sources, including a global application for seabird colonies. A future architecture for NH3 emission-deposition modelling is proposed that integrates the spatio-temporal interactions, and provides the necessary foundation to assess the consequences of climate change. Based on available measurements, a first empirical estimate suggests that 5°C warming would increase emissions by 42 per cent (28-67%). Together with increased anthropogenic activity, global NH3 emissions may increase from 65 (45-85) Tg N in 2008 to reach 132 (89-179) Tg by 2100.

Retrieving radius, concentration, optical depth, and mass of different types of aerosols from high-resolution infrared nadir spectra.

We present a sophisticated radiative transfer code for modeling outgoing IR radiation from planetary atmospheres and, conversely, for retrieving atmospheric properties from high-resolution nadir-observed spectra. The forward model is built around a doubling-adding routine and calculates, in a spherical refractive geometry, the outgoing radiation emitted by the Earth and the atmosphere containing one layer of aerosol. The inverse model uses an optimal estimation approach and can simultaneously retrieve atmospheric trace gases, aerosol effective radius, and concentration. It is different from existing codes, as most forward codes dealing with multiple scattering assume a plane-parallel atmosphere, and as for the retrieval, it does not rely on precalculated spectra, the use of microwindows, or two-step retrievals. The simultaneous retrieval on a broad spectral range exploits the full potential of current state-of-the-art hyperspectral IR sounders, such as AIRS and IASI, and should be particularly useful in studying major pollution events. We present five example retrievals of IASI spectra observed in the range from 800 to 1200 cm(-1) above dust, volcanic ash, sulfuric acid, ice particles, and biomass burning aerosols.

A 3000 K laboratory emission spectrum of water.

An emission spectrum of hot water with a temperature of about 3000 K is obtained using an oxy-acetylene torch. This spectrum contains a very large number of transitions. The spectrum, along with previous cooler laboratory emission spectra and an absorption spectrum recorded from a sunspot, is analyzed in the 500-2000 cm(-1) region. Use of a calculated variational linelist for water allows significant progress to be made on assigning transitions involving highly excited vibrational and rotational states. In particular emission from rotationally excited states up to J=42 and vibrational levels with up to eight quanta of bending motion are assigned.