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During the 2020 austral summer, the pristine atmosphere of the southwest Indian Ocean (SWIO) basin experienced significant perturbations. This study examines the variability of aerosols and carbon monoxide (CO) over this remote oceanic region and investigates the underlying processes in the upper troposphere–lower stratosphere (UT-LS). Aerosol profiles in January and February 2020 revealed a multi-layer structure in the tropical UT-LS. Numerical models – the FLEXible PARTicle dispersion model (FLEXPART) and the Modèle Isentropique de transport Mésoéchelle de l'Ozone Stratosphérique par Advection (MIMOSA) – indicated that the lower-stratospheric aerosol content was influenced by the intense and persistent stratospheric aerosol layer generated during the 2019–2020 extreme Australian bushfire events. A portion of this layer was transported eastward by prevailing easterly winds, leading to increased aerosol extinction profiles over Réunion on 27 and 28 January. Analysis of advected potential vorticity revealed isentropic transport of air masses containing Australian biomass burning aerosols from extratropical latitudes to Réunion at the 400 K isentropic level on 28 January. Interestingly, we found that biomass burning (BB) activity in eastern Africa, though weak during this season, significantly influenced (contributed up to 90 % of) the vertical distribution of CO and aerosols in the upper troposphere over the SWIO basin. Ground-based observations at Réunion confirmed the simultaneous presence of African and Australian aerosol layers. This study provides the first evidence of African BB emissions impacting the CO and aerosol distribution in the upper troposphere over the SWIO basin during the convective season. [ABSTRACT FROM AUTHOR]

Nitrous acid (HONO) is a key atmospheric component, acting as a major source of the hydroxyl radical (OH), the primary oxidant in the Earth's atmosphere. However, understanding its spatial and temporal variability remains a significant challenge. Recent TROPOspheric Monitoring Instrument (TROPOMI)/Sentinel-5 Precursor (S5P) ultraviolet–visible (UV–Vis) measurements of fresh fire plumes shed light on the impact of global pyrogenic HONO emissions. Here, we leverage Infrared Atmospheric Sounding Interferometer (IASI)/MetOp's global infrared satellite measurements, complementing midday TROPOMI observations with morning and evening overpasses, to detect and retrieve pyrogenic HONO in 2007–2023. Employing a sensitive detection method, we identify HONO enhancements within concentrated fire plumes worldwide. Most detections are in the Northern Hemisphere (NH) mid- and high latitudes, where intense wildfires and high injection heights favour HONO detection. IASI's nighttime measurements yield 10-fold more HONO detections than daytime measurements, emphasizing HONO 's extended lifetime in the absence of photolysis during the night. The annual detection count increases by at least 3–4 times throughout the IASI time series, mirroring the recent surge in intense wildfires at these latitudes. Additionally, we employ a neural-network-based algorithm for retrieving pyrogenic HONO total columns from IASI and compare them with TROPOMI in the same fire plumes. The results demonstrate TROPOMI's efficacy in capturing HONO enhancements in smaller fire plumes and in proximity to fire sources, while IASI's morning and evening overpasses enable HONO measurements further downwind, highlighting the survival of HONO or its secondary formation along long-range transport in smoke plumes. [ABSTRACT FROM AUTHOR]

© 2015. American Geophysical Union. All Rights Reserved. We show the results and evaluation with independent measurements from assimilating both MOPITT (Measurements Of Pollution In The Troposphere) and IASI (Infrared Atmospheric Sounding Interferometer) retrieved profiles into the Community Earth System Model (CESM). We used the Data Assimilation Research Testbed ensemble Kalman filter technique, with the full atmospheric chemistry CESM component Community Atmospheric Model with Chemistry. We first discuss the methodology and evaluation of the current data assimilation system with coupled meteorology and chemistry data assimilation. The different capabilities of MOPITT and IASI retrievals are highlighted, with particular attention to instrument vertical sensitivity and coverage and how these impact the analyses. MOPITT and IASI CO retrievals mostly constrain the CO fields close to the main anthropogenic, biogenic, and biomass burning CO sources. In the case of IASI CO assimilation, we also observe constraints on CO far from the sources. During the simulation time period (June and July 2008), CO assimilation of both instruments strongly improves the atmospheric CO state as compared to independent observations, with the higher spatial coverage of IASI providing better results on the global scale. However, the enhanced sensitivity of multispectral MOPITT observations to near surface CO over the main source regions provides synergistic effects at regional scales.

Nitrous acid (HONO) is a key atmospheric component, acting as a major source of the hydroxyl radical (OH), the primary oxidant in the Earth's atmosphere. However, understanding its spatial and temporal variability remains a significant challenge. Recent TROPOMI/S5P UV-Vis measurements of fresh fire plumes shed light on the impact of global pyrogenic HONO emissions. Here, we leverage IASI/Metop's global infrared satellite measurements, complementing midday TROPOMI observations with morning and evening overpasses, to detect and retrieve pyrogenic HONO in 2007–2023. Employing a sensitive detection method, we identify HONO enhancements within concentrated fire plumes worldwide. Most detections are in the North Hemisphere mid and high latitudes, where intense wildfires and high injection heights favour HONO detection. IASI's nighttime measurements yield tenfold more HONO detections than daytime, emphasizing HONO's extended lifetime in the absence of photolysis during the night. The annual detection count increases by at least 3–4 times throughout the IASI time series, mirroring the recent surge in intense wildfires at these latitudes. Additionally, we employ a neural network-based algorithm for retrieving pyrogenic HONO total columns from IASI and compare them with TROPOMI in the same fire plumes. The results demonstrate TROPOMI's efficacy in capturing HONO enhancements in smaller fire plumes and in proximity to fire sources, while IASI's morning and evening overpasses enable HONO measurements further downwind, highlighting the survival of HONO or its secondary formation along long-range transport in smoke plumes. [ABSTRACT FROM AUTHOR]

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 × 10 15 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. [ABSTRACT FROM AUTHOR]

The pristine atmosphere of the southwest Indian Ocean (SWIO) basin underwent significant perturbations during the 2020 austral summer. This study documents the complex variability of aerosols and carbon monoxide (CO) over this remote oceanic region and identifies the processes governing it in the upper troposphere – lower stratosphere (UT-LS). Aerosol profiles exhibit a multi-layer structure in the tropical UT-LS in January and February 2020. The numerical models (FLEXPART and MIMOSA) showed that the modulation of the aerosol content in the lower stratosphere is due to the intense and persistent stratospheric aerosol smoke layer generated during the 2019–20 extreme Australian bushfire events. One part of this stratospheric aerosol smoke layer was advected zonally by the prevailing easterly winds and its passage over Reunion was recorded by increased aerosol extinction profiles on 27th and 28th January. The analysis of the advected potential vorticity highlights an isentropic transport of air masses containing Australian biomass burning aerosol from extra-tropical latitudes to Reunion at the 400 K isentropic level, on 28th January. Interestingly, our results show that the biomass burning activity in eastern Africa, weak during this season, contributed to modulate (up to 90 %) the vertical distribution of CO and aerosols in the upper troposphere over the SWIO basin. The simultaneous presence of African and Australian aerosols smoke layers has been recorded by ground-based observations at Reunion. This study highlights for the first time the influence of the African emissions from biomass burning to the CO and aerosols distribution in the upper troposphere over the SWIO basin during the convective season. The results show that besides PyroCb -driven injection of biomass burning products to the stratosphere, an alternative pathway may exist during the regular deep-convection season in the tropics. [ABSTRACT FROM AUTHOR]