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Bridging the spatial gaps of the Ammonia Monitoring Network using satellite ammonia measurements

par Wang, Rui;Pan, Da;Guo, Xuehui;Sun, Kang;Clarisse, Lieven ;Van Damme, Martin ;Coheur, Pierre ;Clerbaux, Cathy ;Puchalski, Melissa;Zondlo, Mark A.
Référence Atmospheric chemistry and physics, 23, 20, page (13217-13234)
Publication Publié, 2023-10-01

Article révisé par les pairs

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Résumé :

Abstract. Ammonia (NH3) is a key precursor to fine particulate matter (PM2.5) and a primary form of reactive nitrogen. The limited number of NH3 observations hinders the further understanding of its impacts on air quality, climate, and biodiversity. Currently, NH3 ground monitoring networks are few and sparse across most of the globe, and even in the most established networks, large spatial gaps exist between sites and only a few sites have records that span longer than a decade. Satellite NH3 observations can be used to discern trends and fill spatial gaps in networks, but many factors influence the syntheses of the vastly different spatiotemporal scales between surface network and satellite measurements. To this end, we intercompared surface NH3 data from the Ammonia Monitoring Network (AMoN) and satellite NH3 total columns from the Infrared Atmospheric Sounding Interferometer (IASI) in the contiguous United States (CONUS) and then performed trend analyses using both datasets. We explored the sensitivity of correlations between the two datasets to factors such as satellite data availability and distribution over the surface measurement period, as well as agreement within selected spatial and temporal windows. Given the short lifetime of atmospheric ammonia and consequently sharp gradients, smaller spatial windows show better agreement than larger ones except in areas of relatively uniform, low concentrations where large windows and more satellite measurements improve the signal-to-noise ratio. A critical factor in the comparison is having satellite measurements across most of the measurement period of the monitoring site. When IASI data are available for at least 80 % of the days of AMoN's 2-week sampling period within a 25 km spatial window of a given site, IASI NH3 column concentrations and the AMoN NH3 surface concentrations have a correlation of 0.74, demonstrating the feasibility of using satellite NH3 columns to bridge the spatial gaps existing in the surface network NH3 concentrations. Both IASI and AMoN show increasing NH3 concentrations across the CONUS (median: 6.8 % yr−1 versus 6.7 % yr−1) in the last decade (2008–2018), suggesting the NH3 will become a greater contributor to nitrogen deposition. NH3 trends at AMoN sites are correlated with IASI NH3 trends (r = 0.66) and show similar spatial patterns, with the highest increases in the Midwest and eastern US. In spring and summer, increases in NH3 were larger than 10 % yr−1 in the eastern US and Midwest (cropland dominated) and the western US (pastureland dominated), respectively. NH3 hotspots are defined as regions where the IASI NH3 column is larger than the 95th percentile of the 11-year CONUS map (6.7 × 1015 molec.cm-2), they also experience increasing concentrations over time, with a median of NH3 trend of 4.7 % yr−1. IASI data show large NH3 increases in urban areas (8.1 % yr−1), including 8 of the top 10 most populous regions in the CONUS, where AMoN sites are sparse. A comparison between IASI NH3 concentration trends and state-level NH3 emission trends is then performed to reveal that positive correlations exist in states with strong agricultural NH3 emissions, while there are negative correlations in states with low NH3 emissions and large NOx emissions, suggesting the different roles of emission and partitioning in NH3 increases. The increases in NH3 could have detrimental effects on nearby eco-sensitive regions through nitrogen deposition and on aerosol chemistry in the densely populated urban areas, and therefore they should be carefully monitored and studied.