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Tropospheric ozone (O3) is an important greenhouse gas that is also hazardous to human health. The formation of O3 is sensitive to the levels of its precursors NOx (≡NO + NO2) and peroxy radicals, for example, generated by the oxidation of volatile organic compounds (VOCs). A better understanding of this sensitivity will show how changes in the levels of these trace gases could affect O3 levels today and in the future, and thus air quality and climate. In this study, we investigate O3 sensitivity in the tropical troposphere based on in situ observations of NO, HO2 and O3 from four research aircraft campaigns between 2015 and 2023. These are OMO (Oxidation Mechanism Observations), ATom (Atmospheric Tomography Mission), CAFE Africa (Chemistry of the Atmosphere Field Experiment in Africa) and CAFE Brazil, in combination with simulations using the EMAC atmospheric chemistry—climate model. We use the metric α(CH3O2) together with NO to investigate the O3 formation sensitivity. We show that O3 formation is generally NOx‐sensitive in the lower and middle tropical troposphere and is in a transition regime in the upper troposphere. By distinguishing observations impacted by lightning or not we show that NO from lightning is the most important driver of O3 sensitivity in the tropics. NOx‐sensitive chemistry predominates in regions without lightning impact, with α(CH3O2) ranging between 0.56 and 0.82 and observed average O3 levels between 35 and 55 ppbv. Areas affected by lightning exhibit strongly VOC‐sensitive O3 chemistry with α(CH3O2) of about 1 and average O3 levels between 55 and 80 ppbv. Plain Language Summary: Ozone (O3) in the troposphere is both an air pollutant and a greenhouse gas. It is formed from nitrogen oxides (NOx) and volatile organic compounds (VOCs). The formation can be sensitive to either of these precursors depending on their abundance. Considering the high relevance of O3 in regard to human health and global warming, it is important to understand this sensitivity of O3 formation, which allows to predict future changes in O3. Here, we investigate O3 formation sensitivity toward NOx and VOCs in the tropical troposphere based on aircraft measurements during four research campaigns between 2015 and 2023, and a global model. We include observations of NO, HO2 (hydroperoxyl radicals) and O3 over South America, the Middle East and the Pacific, Atlantic and Indian Ocean. We find that O3 formation is sensitive to NOx in the lower tropical troposphere. In the upper tropical troposphere, lightning events control O3 chemistry and promote strong VOC‐sensitive O3 formation. Key Points: α(CH3O2) correlated with NO is a powerful metric for indicating O3 sensitivity and is valid throughout the troposphereO3 chemistry in the remote tropical lower troposphere is found to be NOx‐sensitiveNO emissions from lightning drive O3 sensitivity in the tropical upper troposphere and induce highly VOC‐sensitive chemistry [ABSTRACT FROM AUTHOR]

Even though anthropogenic mercury (Hg) emissions to the atmosphere are ∼2.5 times higher in the Northern Hemisphere (NH) than in the Southern Hemisphere (SH), atmospheric Hg concentrations in the NH are only ∼1.5 times higher than in the SH. Global Hg models attribute this apparent discrepancy to large SH oceanic Hg emissions or to interhemispheric exchange of Hg through the atmosphere. However, no observational data set exists to serve as a benchmark to validate whether these coarse‐resolution models adequately represent the complex dynamics of interhemispheric Hg exchange. During the 2015–2016 El Niño, we observed at mount Chacaltaya in the tropical Andes a ∼50% increase in ambient Hg compared to the year before, coinciding with a shift in synoptic transport pathways. Using this event as a case study, we investigate the impact of interhemispheric exchange on atmospheric Hg in tropical South America. We use HYSPLIT to link Hg observations to long‐range transport and find that the observed Hg increase relates strongly to air masses from the tropical Pacific upper troposphere (UT), a region directly impacted by interhemispheric exchange. Inclusion of the modeled seasonality of interhemispheric air mass exchange strengthens this relationship significantly. We estimate that interhemispheric exchange drives Hg seasonality in the SH tropical Pacific UT, with strongly enhanced Hg between July and October. We validate this seasonality with previously published aircraft Hg observations. Our results suggest that the transport of NH‐influenced air masses to tropical South America via the Pacific UT occurs regularly but became more detectable at Chacaltaya in 2015–2016 because of a westward shift in air mass origin. Plain Language Summary: Human activities have released much more mercury, a toxic pollutant, into the Northern Hemisphere (NH) atmosphere than into the Southern Hemisphere (SH) atmosphere. Yet, the difference in mercury concentrations between the two hemispheres is not very large. Model studies attribute this unexpectedly low interhemispheric mercury difference to large emissions from SH oceans or to the exchange of airborne mercury between hemispheres. This interhemispheric mercury exchange is complex, however, and direct observational evidence is lacking. Here, we examine the strong increase in atmospheric mercury during the 2015–2016 El Niño at mount Chacaltaya in tropical South America. We examine and exclude potential SH sources for this increase, such as mercury emissions from wildfires or marine mercury emissions. Instead, we find that this mercury increase was likely caused by interhemispheric mercury exchange at high altitudes over the tropical Pacific Ocean, and the subsequent transport of mercury‐rich NH‐influenced air to tropical South America. We propose that Chacaltaya mercury observations could be used as a reference to test if current mathematical models can correctly predict interhemispheric mercury exchange. Key Points: We use the strong increase in atmospheric Hg at Chacaltaya mountain in tropical South America during the 2015–2016 El Niño for a case studyIn 2015–2016, air mass origin for Chacaltaya shifted westward, with greatly enhanced influence of the tropical Pacific upper troposphere (UT)Our results suggest that interhemispheric exchange in the tropical Pacific UT can bring Northern Hemisphere Hg to Chacaltaya [ABSTRACT FROM AUTHOR]