We present the organization, instrumentation, datasets, data interpretation, modeling, and accomplishments of the multinational global atmospheric measurement program AGAGE (Advanced Global Atmospheric Gases Experiment). AGAGE is distinguished by its capability to measure globally, at high frequency, and at multiple sites all the important species in the Montreal Protocol and all the important non-carbon-dioxide (non-CO₂) gases assessed by the Intergovernmental Panel on Climate Change (CO₂ is also measured at several sites). The scientific objectives of AGAGE are important in furthering our understanding of global chemical and climatic phenomena. They are the following: (1) to accurately measure the temporal and spatial distributions of anthropogenic gases that contribute the majority of reactive halogen to the stratosphere and/or are strong infrared absorbers (chlorocarbons, chlorofluorocarbons – CFCs, bromocarbons, hydrochlorofluorocarbons – HCFCs, hydrofluorocarbons – HFCs and polyfluorinated compounds (perfluorocarbons – PFCs), nitrogen trifluoride – NF₃, sulfuryl fluoride – SO₂F₂, and sulfur hexafluoride – SF₆) and use these measurements to determine the global rates of their emission and/or destruction (i.e., lifetimes); (2) to accurately measure the global distributions and temporal behaviors and determine the sources and sinks of non-CO₂ biogenic–anthropogenic gases important to climate change and/or ozone depletion (methane – CH₄, nitrous oxide – N₂O, carbon monoxide – CO, molecular hydrogen – H₂, methyl chloride – CH₃Cl, and methyl bromide – CH₃Br); (3) to identify new long-lived greenhouse and ozone-depleting gases (e.g., SO₂F₂, NF₃, heavy PFCs (C₄F₁₀, C₅F₁₂, C₆F₁₄, C₇F₁₆, and C₈F₁₈) and hydrofluoroolefins (HFOs; e.g., CH₂ = CFCF₃) have been identified in AGAGE), initiate the real-time monitoring of these new gases, and reconstruct their past histories from AGAGE, air archive, and firn air measurements; (4) to determine the average concentrations and trends of tropospheric hydroxyl radicals (OH) from the rates of destruction of atmospheric trichloroethane (CH₃CCl₃), HFCs, and HCFCs and estimates of their emissions; (5) to determine from atmospheric observations and estimates of their destruction rates the magnitudes and distributions by region of surface sources and sinks of all measured gases; (6) to provide accurate data on the global accumulation of many of these trace gases that are used to test the synoptic-, regional-, and global-scale circulations predicted by three-dimensional models; and (7) to provide global and regional measurements of methane, carbon monoxide, and molecular hydrogen and estimates of hydroxyl levels to test primary atmospheric oxidation pathways at midlatitudes and the tropics. Network Information and Data Repository: http://agage.mit.edu/data or http://cdiac.ess-dive.lbl.gov/ndps/alegage.html (https://doi.org/10.3334/CDIAC/atg.db1001).

The hydroxyl free radical (OH) is the major oxidizing chemical in the atmosphere, destroying about 3.7 petagrams (Pg) of trace gases each year, including many gases involved in ozone depletion, the greenhouse effect and urban air pollution. Measurements of 1,1,1‐trichloroethane (methyl chloroform, CH₃CCl₃), which reacts with OH, provide the most accurate method currently utilized for determining the global behavior of OH. We report that CH₃CCl₃ levels rose steadily from 1978 to reach a maximum in 1992 and have since decreased rapidly to levels in 2004 about 30% of the levels when measurements began in 1978. Analysis of these observations shows that global average OH levels had a small maximum around 1989 and a larger minimum around 1998, with OH concentrations in 2003 being comparable to those in 1979. This post‐1998 recovery of OH reported here contrasts with the situation 4 years ago when reported OH was decreasing. The 1997–1999 OH minimum coincides with, and is likely caused by, major global wildfires and an intense El Nino event at this time.

Trends and variability in tropospheric hydroxyl (OH) radicals influence budgets of many greenhouse gases, air pollutant species, and ozone depleting substances. Estimations of tropospheric OH trends and variability based on budget analysis of methyl chloroform (CH₃CCl₃) and process‐based chemistry transport models often produce conflicting results. Here we use a previously tested transport model to simulate atmospheric CH₃CCl₃ for the period 1985–2018. Based on mismatches between model output and observations, we derive consistent anomalies in the inverse lifetime of CH₃CCl₃ (K_G) using measurements from two independent observational networks (National Oceanic and Atmospheric Administration and Advanced Global Atmospheric Gases Experiment). Our method allows a separation between “physical” (transport, temperature) and “chemical” (i.e., abundance) influences on OH + CH₃CCl₃ reaction rate in the atmosphere. Small increases in K_G due to “physical” influences are mostly driven by increases in the temperature‐dependent reaction between OH and CH₃CCl₃ and resulted in a smoothly varying increase of 0.80% decade⁻¹. Chemical effects on K_G, linked to global changes in OH sources and sinks, show larger year‐to‐year variations (∼2%–3%), and have a negative correlation with the El Niño Southern Oscillation. A significant positive trend in K_G can be derived after 2001, but it persists only through 2015 and only if we assume that CH₃CCl₃ emissions decayed more slowly over time than our best estimate suggests. If global CH₃CCl₃ emissions dropped below 3 Gg year⁻¹ after 2015, recent CH₃CCl₃ measurements indicate that the 2015–2018 loss rate of CH₃CCl₃ due to reaction with OH is comparable to its value 2 decades ago.