Abstract
Abstract Remarkable progress has occurred over the last 100 years in our understanding of atmospheric chemical composition, stratospheric and tropospheric chemistry, urban air pollution, acid rain, and the formation of airborne particles from gas-phase chemistry. Much of this progress was associated with the developing understanding of the formation and role of ozone and of the oxides of nitrogen, NO and NO2, in the stratosphere and troposphere. The chemistry of the stratosphere, emerging from the pioneering work of Chapman in 1931, was followed by the discovery of catalytic ozone cycles, ozone destruction by chlorofluorocarbons, and the polar ozone holes, work honored by the 1995 Nobel Prize in Chemistry awarded to Crutzen, Rowland, and Molina. Foundations for the modern understanding of tropospheric chemistry were laid in the 1950s and 1960s, stimulated by the eye-stinging smog in Los Angeles. The importance of the hydroxyl (OH) radical and its relationship to the oxides of nitrogen (NO and NO2) emerged. The chemical processes leading to acid rain were elucidated. The atmosphere contains an immense number of gas-phase organic compounds, a result of emissions from plants and animals, natural and anthropogenic combustion processes, emissions from oceans, and from the atmospheric oxidation of organics emitted into the atmosphere. Organic atmospheric particulate matter arises largely as gas-phase organic compounds undergo oxidation to yield low-volatility products that condense into the particle phase. A hundred years ago, quantitative theories of chemical reaction rates were nonexistent. Today, comprehensive computer codes are available for performing detailed calculations of chemical reaction rates and mechanisms for atmospheric reactions. Understanding the future role of atmospheric chemistry in climate change and, in turn, the impact of climate change on atmospheric chemistry, will be critical to developing effective policies to protect the planet.
Highlights
Any historical account of a field as broad and deep as atmospheric chemistry must, by necessity, be selective
Since more than 99% of the total available chlorine was stored in the reservoir species, and since most of the reservoir species react on the polar stratospheric clouds (PSCs) surfaces, the ClOx concentration in early spring increases to ;500 times greater than normal, and the ozone destruction rate increases depleting ozone and producing the polar stratospheric ozone holes in just a few weeks
Oxidation of volatile organic compound (VOC) mostly leads to volatile products, but, as noted above, a fraction of such reactions can produce species of sufficiently low vapor pressure such that their preferred state is to be in a condensed phase
Summary
Any historical account of a field as broad and deep as atmospheric chemistry must, by necessity, be selective. A selective account, such as this one gives the impression that progress was made by following a singular path. This impression could not be further from the truth! We progress through 100 years of stratospheric and tropospheric chemistry research highlighting progress made toward a chemical understanding of stratospheric ozone depletion, urban air quality, and atmospheric particle formation. We attempt to peer into the future and offer our subjective view of what the 100 years of gas-phase atmospheric chemistry might bring
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