scholarly journals Chemical modeling of the reactivity of short-lived greenhouse gases: a model inter-comparison prescribing a well-measured, remote troposphere

2018 ◽  
Author(s):  
Michael J. Prather ◽  
Clare M. Flynn ◽  
Xin Zhu ◽  
Stephen D. Steenrod ◽  
Sarah A. Strode ◽  
...  
Keyword(s):  
Water Vapor ◽  
Greenhouse Gases ◽  
Atmospheric Chemistry ◽  
Synthetic Data ◽  
Chemical Mechanism ◽  
Ozone Production ◽  
Atmospheric Composition ◽  
Tracer Transport ◽  
Chemical Modeling ◽  
Model Simulations

Abstract. We develop a new protocol for merging in situ measurements with 3-D model simulations of atmospheric chemistry with the goal of integrating over the data to identify the most reactive air parcels in terms of tropospheric production and loss of the greenhouse gases ozone and methane. Presupposing that we can accurately measure atmospheric composition, we examine whether models constrained by such measurements agree on the chemical budgets for ozone and methane. In applying our technique to a synthetic data stream of 14,880 parcels along 180 W, we are able to isolate the performance of the photochemical modules operating within their global chemistry-climate and chemistry-transport models, removing the effects of modules controlling tracer transport, emissions, and scavenging. Differences in reactivity across models are driven only by the chemical mechanism and the diurnal cycle of photolysis rates, which are driven in turn by temperature, water vapor, solar zenith angle, clouds, and possibly aerosols and overhead ozone, which are calculated in each model. We evaluate six global models and identify their differences and similarities in simulating the chemistry through a range of innovative diagnostics. All models agree that the more highly reactive parcels dominate the chemistry (e.g., the hottest 10 % of parcels control 25–30 % of the total reactivities), but do not fully agree on which parcels comprise the top 10 %. Distinct differences in specific features occur, including the regions of maximum ozone production and methane loss, as well as in the relationship between photolysis and these reactivities. Unique, possibly aberrant, features are identified for each model, providing a benchmark for photochemical module development. Among the 6 models tested here, 3 are almost indistinguishable based on the inherent variability caused by clouds, and thus we identify 4, effectively distinct, chemical models. Based on this work, we suggest that water vapor differences in model simulations of past and future atmospheres may be a cause of the different evolution of tropospheric O3 and CH4, and lead to different chemistry-climate feedbacks across the models.

scholarly journals How well can global chemistry models calculate the reactivity of short-lived greenhouse gases in the remote troposphere, knowing the chemical composition

2018 ◽  
Vol 11 (5) ◽  
pp. 2653-2668 ◽  
Author(s):  
Michael J. Prather ◽  
Clare M. Flynn ◽  
Xin Zhu ◽  
Stephen D. Steenrod ◽  
Sarah A. Strode ◽  
...  
Keyword(s):  
Water Vapor ◽  
Greenhouse Gases ◽  
Atmospheric Chemistry ◽  
Synthetic Data ◽  
Chemical Mechanism ◽  
Ozone Production ◽  
Atmospheric Composition ◽  
Tracer Transport ◽  
Model Simulations ◽  
Photolysis Rates

Abstract. We develop a new protocol for merging in situ measurements with 3-D model simulations of atmospheric chemistry with the goal of integrating these data to identify the most reactive air parcels in terms of tropospheric production and loss of the greenhouse gases ozone and methane. Presupposing that we can accurately measure atmospheric composition, we examine whether models constrained by such measurements agree on the chemical budgets for ozone and methane. In applying our technique to a synthetic data stream of 14 880 parcels along 180∘ W, we are able to isolate the performance of the photochemical modules operating within their global chemistry-climate and chemistry-transport models, removing the effects of modules controlling tracer transport, emissions, and scavenging. Differences in reactivity across models are driven only by the chemical mechanism and the diurnal cycle of photolysis rates, which are driven in turn by temperature, water vapor, solar zenith angle, clouds, and possibly aerosols and overhead ozone, which are calculated in each model. We evaluate six global models and identify their differences and similarities in simulating the chemistry through a range of innovative diagnostics. All models agree that the more highly reactive parcels dominate the chemistry (e.g., the hottest 10 % of parcels control 25–30 % of the total reactivities), but do not fully agree on which parcels comprise the top 10 %. Distinct differences in specific features occur, including the spatial regions of maximum ozone production and methane loss, as well as in the relationship between photolysis and these reactivities. Unique, possibly aberrant, features are identified for each model, providing a benchmark for photochemical module development. Among the six models tested here, three are almost indistinguishable based on the inherent variability caused by clouds, and thus we identify four, effectively distinct, chemical models. Based on this work, we suggest that water vapor differences in model simulations of past and future atmospheres may be a cause of the different evolution of tropospheric O3 and CH4, and lead to different chemistry-climate feedbacks across the models.

scholarly journals Comparisons of observed and modeled OH and HO2concentrations during the ambient measurement period of the HOxComp field campaign

2012 ◽  
Vol 12 (5) ◽  
pp. 2567-2585 ◽  
Author(s):  
Y. Kanaya ◽  
A. Hofzumahaus ◽  
H.-P. Dorn ◽  
T. Brauers ◽  
H. Fuchs ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Chemical Mechanism ◽  
Ozone Production ◽  
High Yield ◽  
Base Case ◽  
Peroxy Radicals ◽  
Field Campaign ◽  
Mixing Ratios ◽  
Measurement Mode ◽  
Single Instrument

Abstract. A photochemical box model constrained by ancillary observations was used to simulate OH and HO2 concentrations for three days of ambient observations during the HOxComp field campaign held in Jülich, Germany in July 2005. Daytime OH levels observed by four instruments were fairly well reproduced to within 33% by a base model run (Regional Atmospheric Chemistry Mechanism with updated isoprene chemistry adapted from Master Chemical Mechanism ver. 3.1) with high R2 values (0.72–0.97) over a range of isoprene (0.3–2 ppb) and NO (0.1–10 ppb) mixing ratios. Daytime HO2(*) levels, reconstructed from the base model results taking into account the sensitivity toward speciated RO2 (organic peroxy) radicals, as recently reported from one of the participating instruments in the HO2 measurement mode, were 93% higher than the observations made by the single instrument. This also indicates an overprediction of the HO2 to OH recycling. Together with the good model-measurement agreement for OH, it implies a missing OH source in the model. Modeled OH and HO2(*) could only be matched to the observations by addition of a strong unknown loss process for HO2(*) that recycles OH at a high yield. Adding to the base model, instead, the recently proposed isomerization mechanism of isoprene peroxy radicals (Peeters and Müller, 2010) increased OH and HO2(*) by 28% and 13% on average. Although these were still only 4% higher than the OH observations made by one of the instruments, larger overestimations (42–70%) occurred with respect to the OH observations made by the other three instruments. The overestimation in OH could be diminished only when reactive alkanes (HC8) were solely introduced to the model to explain the missing fraction of observed OH reactivity. Moreover, the overprediction of HO2(*) became even larger than in the base case. These analyses imply that the rates of the isomerization are not readily supported by the ensemble of radical observations. One of the measurement days was characterized by low isoprene concentrations (∼0.5 ppb) and OH reactivity that was well explained by the observed species, especially before noon. For this selected period, as opposed to the general behavior, the model tended to underestimate HO2(*). We found that this tendency is associated with high NOx concentrations, suggesting that some HO2 production or regeneration processes under high NOx conditions were being overlooked; this might require revision of ozone production regimes.

scholarly journals The influence of temperature on ozone production under varying NO<sub><i>x</i></sub> conditions – a modelling study

2016 ◽  
Vol 16 (18) ◽  
pp. 11601-11615 ◽  
Author(s):  
Jane Coates ◽  
Kathleen A. Mar ◽  
Narendra Ojha ◽  
Tim M. Butler
Keyword(s):  
Central Europe ◽  
Surface Ozone ◽  
Reaction Rates ◽  
Air Pollutant ◽  
Box Model ◽  
Chemical Mechanism ◽  
Ozone Production ◽  
Nox Emissions ◽  
Model Simulations ◽  
Rate Of Increase

Abstract. Surface ozone is a secondary air pollutant produced during the atmospheric photochemical degradation of emitted volatile organic compounds (VOCs) in the presence of sunlight and nitrogen oxides (NOx). Temperature directly influences ozone production through speeding up the rates of chemical reactions and increasing the emissions of VOCs, such as isoprene, from vegetation. In this study, we used an idealised box model with different chemical mechanisms (Master Chemical Mechanism, MCMv3.2; Common Representative Intermediates, CRIv2; Model for OZone and Related Chemical Tracers, MOZART-4; Regional Acid Deposition Model, RADM2; Carbon Bond Mechanism, CB05) to examine the non-linear relationship between ozone, NOx and temperature, and we compared this to previous observational studies. Under high-NOx conditions, an increase in ozone from 20 to 40 °C of up to 20 ppbv was due to faster reaction rates, while increased isoprene emissions added up to a further 11 ppbv of ozone. The largest inter-mechanism differences were obtained at high temperatures and high-NOx emissions. CB05 and RADM2 simulated more NOx-sensitive chemistry than MCMv3.2, CRIv2 and MOZART-4, which could lead to different mitigation strategies being proposed depending on the chemical mechanism. The increased oxidation rate of emitted VOC with temperature controlled the rate of Ox production; the net influence of peroxy nitrates increased net Ox production per molecule of emitted VOC oxidised. The rate of increase in ozone mixing ratios with temperature from our box model simulations was about half the rate of increase in ozone with temperature observed over central Europe or simulated by a regional chemistry transport model. Modifying the box model set-up to approximate stagnant meteorological conditions increased the rate of increase of ozone with temperature as the accumulation of oxidants enhanced ozone production through the increased production of peroxy radicals from the secondary degradation of emitted VOCs. The box model simulations approximating stagnant conditions and the maximal ozone production chemical regime reproduced the 2 ppbv increase in ozone per degree Celsius from the observational and regional model data over central Europe. The simulated ozone–temperature relationship was more sensitive to mixing than the choice of chemical mechanism. Our analysis suggests that reductions in NOx emissions would be required to offset the additional ozone production due to an increase in temperature in the future.

scholarly journals A comparison of atmospheric composition using the Carbon Bond and Regional Atmospheric Chemistry Mechanisms

2013 ◽  
Vol 13 (3) ◽  
pp. 6923-6969 ◽  
Author(s):  
G. Sarwar ◽  
J. Godowitch ◽  
B. Henderson ◽  
K. Fahey ◽  
G. Pouliot ◽  
...  
Keyword(s):  
Hydrogen Peroxide ◽  
Atmospheric Chemistry ◽  
Production Efficiency ◽  
Fine Particles ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Ozone Production ◽  
Atmospheric Composition ◽  
Organic Nitrate ◽  
Carbon Bond

Abstract. We incorporate the recently developed Regional Atmospheric Chemistry Mechanism (version 2, RACM2) into the Community Multiscale Air Quality modeling system for comparison with the existing 2005 Carbon Bond mechanism with updated toluene chemistry (CB05TU). Compared to CB05TU, RACM2 enhances the domain-wide monthly mean hydroxyl radical concentrations by 46% and nitric acid by 26%. However, it reduces hydrogen peroxide by 2%, peroxyacetic acid by 94%, methyl hydrogen peroxide by 19%, peroxyacetyl nitrate by 40%, and organic nitrate by 41%. RACM2 predictions generally agree better with the observed data than the CB05TU predictions. RACM2 enhances ozone for all ambient levels leading to higher bias at low (< 60 ppbv) concentrations but improved performance at high (>70 ppbv) concentrations. The RACM2 ozone predictions are also supported by increased ozone production efficiency that agrees better with observations. Compared to CB05TU, RACM2 enhances the domain-wide monthly mean sulfate by 10%, nitrate by 6%, ammonium by 10%, anthropogenic secondary organic aerosols by 42%, biogenic secondary organic aerosols by 5%, and in-cloud secondary organic aerosols by 7%. Increased inorganic and organic aerosols with RACM2 agree better with observed data. While RACM2 enhances ozone and secondary aerosols by relatively large margins, control strategies developed for ozone or fine particles using the two mechanisms do not differ appreciably.

Complexities of communicating atmospheric composition and its impacts during the COVID-19 public health crisis in 2020

2021 ◽  
Author(s):  
Claudia Volosciuk
Keyword(s):  
Public Health ◽  
Carbon Dioxide ◽  
Greenhouse Gases ◽  
Atmospheric Chemistry ◽  
Stratospheric Ozone ◽  
Scientific Information ◽  
Atmospheric Composition ◽  
Physical Parameters ◽  
Health Crisis ◽  
Public Health Crisis

&lt;p&gt;The Global Atmosphere Watch (GAW) Programme of the World Meteorological Organization (WMO) is driven by the need to understand the variability and trends in atmospheric composition and the related physical parameters, and to assess the consequences thereof. GAW provides reliable scientific information for a broad spectrum of users, including policymakers, on topics related to atmospheric chemical composition. The programme supports international environmental and climate agreements and improves our understanding of climate change and long-range transboundary air pollution through its work on greenhouse gases, aerosols, reactive gases, atmospheric deposition, stratospheric ozone, and ultraviolet radiation. GAW provides information based on combinations of observations, data analysis and modelling activities, and supports a number of applications at the global, regional and urban scale. This implies a variety of target groups and communication vectors. Due to the complexity and interrelations of the different constituents in atmospheric chemistry and the diversity of the target audience, communication of the related issues represents a substantial challenge. Some examples are questions like &amp;#8220;If greenhouse gas emissions are falling, why do concentrations not decrease?&amp;#8221;, &amp;#8220;if satellite data show pollution reductions, why can&amp;#8217;t we say that it is due to emission reductions?&amp;#8221; etc. &amp;#160;&lt;/p&gt;&lt;p&gt;To sustain the credibility and increase the visibility of GAW within the WMO community and other national/international bodies, the broader scientific and policy communities, as well as the general public, increasing efforts towards &amp;#8220;communicating GAW&amp;#8221; are taken. The global pandemic related to COVID-19 was the dominating topic around the globe in 2020. This required adjustments to communication efforts. Due to in-person meetings being impossible, all communication efforts required delivery and engagement through virtual formats.&lt;/p&gt;&lt;p&gt;While emissions of carbon dioxide (among others) have decreased temporarily in 2020 due to COVID-19 restrictions, concentrations have continued to increase. This has led to confusion among many non-scientists who were surprised that the restrictions they were experiencing did not even have the effect of decreasing atmospheric concentrations of carbon dioxide. Thereby, the crisis has provided an opportunity to explain the difference between emissions and concentrations, emphasizing that carbon dioxide (and other greenhouse gases) are long-lived and remain in the atmosphere for a long time, and highlighting the importance to reach net-zero emissions. Similar confusion was related to the interpretation of the pollution levels and also required additional communication efforts.&lt;/p&gt;&lt;p&gt;Reflections on communication of atmospheric composition in the framework of WMO/GAW, including challenges and opportunities during the public health crisis will be presented.&lt;/p&gt;

scholarly journals OH and HO<sub>2</sub> radical chemistry in a midlatitude forest: Measurements and model comparisons

2019 ◽  
Author(s):  
Michelle L. Lew ◽  
Pamela S. Rickly ◽  
Brandon P. Bottorff ◽  
Sofia Sklaveniti ◽  
Thierry Léonardis ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Global Climate ◽  
Oxidation Products ◽  
Chemical Mechanism ◽  
Ozone Production ◽  
Peroxy Radicals ◽  
Mixing Ratios ◽  
Photolysis Rates ◽  
Model Predictions ◽  
Ho2 Radical

Abstract. Reactions of the hydroxyl (OH) and peroxy radicals (HO2 and RO2) play a central role in the chemistry of the atmosphere. In addition to controlling the lifetimes of many trace gases important to issues of global climate change, OH radical reactions initiate the oxidation of volatile organic compounds (VOCs) which can lead to the production of ozone and secondary organic aerosols in the atmosphere. Previous measurements of these radicals in forest environments characterized by high mixing ratios of isoprene and low mixing ratios of nitrogen oxides (NOx) have shown serious discrepancies with modeled concentrations. These results bring into question our understanding of the atmospheric chemistry of isoprene and other biogenic VOCs under low NOx conditions. During the summer of 2015, OH and HO2 radical concentrations as well as total OH reactivity were measured using Laser-Induced Fluorescence - Fluorescence Assay by Gas Expansion (LIF-FAGE) techniques as part of the Indiana Radical, Reactivity and Ozone Production Intercomparison (IRRONIC). This campaign took place in a forested area near the Indiana University, Bloomington campus characterized by high mixing ratios of isoprene and low mixing ratios of NOx. Supporting measurements of photolysis rates, VOCs, NOx, and other species were used to constrain a zero-dimensional box model based on the Regional Atmospheric Chemistry Mechanism (RACM2) and the Master Chemical Mechanism (MCM). Using an OH chemical scavenger technique, the study revealed the presence of an interference with the LIF-FAGE measurements of OH that increased with both ambient concentrations of ozone and temperature. Subtraction of the interference resulted in measured OH concentrations that were in better agreement with model predictions, although the model still underestimated the measured concentrations, likely due to an underestimation of the concentration of NO at this site. Measurements of HO2 radical concentrations during the campaign included a fraction of isoprene-based peroxy radicals (HO2* = HO2 + αRO2) and were found to agree with model predictions. On average, the measured reactivity was consistent with that calculated from measured OH sinks to within 20 %, with modeled oxidation products accounting for the missing reactivity, although significant missing reactivity (approximately 40 % of the total measured reactivity) was observed on some days.

scholarly journals Description and evaluation of the UKCA stratosphere–troposphere chemistry scheme (StratTrop vn 1.0) implemented in UKESM1

2020 ◽  
Vol 13 (3) ◽  
pp. 1223-1266 ◽  
Author(s):  
Alexander T. Archibald ◽  
Fiona M. O'Connor ◽  
Nathan Luke Abraham ◽  
Scott Archer-Nicholls ◽  
Martyn P. Chipperfield ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
General Model ◽  
Current Model ◽  
Model Performance ◽  
Chemical Mechanism ◽  
System Model ◽  
Atmospheric Composition ◽  
Earth System ◽  
Model Simulations ◽  
Overall Performance

Abstract. Here we present a description of the UKCA StratTrop chemical mechanism, which is used in the UKESM1 Earth system model for CMIP6. The StratTrop chemical mechanism is a merger of previously well-evaluated tropospheric and stratospheric mechanisms, and we provide results from a series of bespoke integrations to assess the overall performance of the model. We find that the StratTrop scheme performs well when compared to a wide array of observations. The analysis we present here focuses on key components of atmospheric composition, namely the performance of the model to simulate ozone in the stratosphere and troposphere and constituents that are important for ozone in these regions. We find that the results obtained for tropospheric ozone and its budget terms from the use of the StratTrop mechanism are sensitive to the host model; simulations with the same chemical mechanism run in an earlier version of the MetUM host model show a range of sensitivity to emissions that the current model does not fall within. Whilst the general model performance is suitable for use in the UKESM1 CMIP6 integrations, we note some shortcomings in the scheme that future targeted studies will address.

scholarly journals The role of plume-scale processes in long-term impacts of aircraft emissions

2019 ◽  
Author(s):  
Thibaud M. Fritz ◽  
Sebastian D. Eastham ◽  
Raymond L. Speth ◽  
Steven R. H. Barrett
Keyword(s):  
Atmospheric Chemistry ◽  
Large Scale ◽  
Maximum Error ◽  
Chemical Mechanism ◽  
Ozone Production ◽  
Lagrangian Model ◽  
Small Scale ◽  
Plume Model ◽  
Soot Emissions

Abstract. Emissions from aircraft engines contribute to atmospheric NOx, driving changes in both the climate and in surface air quality. Existing atmospheric models typically assume instant dilution of emissions into large-scale grid cells, neglecting non-linear, small-scale processes occurring in aircraft wakes. They also do not explicitly simulate the formation of ice crystals, which could drive local chemical processing. This assumption may lead to errors in estimates of aircraft-attributable ozone production, and in turn to biased estimates of aviation’s current impacts on the atmosphere and the effect of future changes in emissions. This includes soot emissions, on which contrail ice forms. These emissions are expected to reduce as biofuel usage increases, but their chemical effects are not well captured by existing models. To address this problem, we develop a Lagrangian model which explicitly models the chemical and microphysical evolution of an aircraft plume. It includes a unified tropospheric-stratospheric chemical mechanism that incorporates heterogeneous chemistry on background and aircraft-induced aerosols. Microphysical processes are also simulated, including the formation, persistence, and chemical influence of contrails. The plume model is used to quantify how the long-term (24-hour) atmospheric chemical response to an aircraft plume varies in response to different environmental conditions, and engine characteristics, and fuel properties. We find that an instant dilution model consistently overestimates ozone production compared to the plume model, up to a maximum error of ~ 200 % at cruise altitudes. Instant dilution of emissions also underestimates the fraction of remaining NOx, although the magnitude and sign of the error vary with season, altitude, and latitude. We also quantify how changes in soot emissions affect plume behavior. Our results show that a 50 % reduction in black carbon emissions, as may be possible through blending with certain biofuels, leads to contrails which evaporate ~ 9 % faster and are 14 % optically thinner. The conversion of emitted NOx to HNO3 and N2O5 falls by 65 % and 69 % respectively, resulting in chemical feedbacks which are not resolved by instant-dilution approaches. The persistent discrepancies between results from the instant dilution approach and from the aircraft plume model demonstrate that a parametrization of effective emission indices should be incorporated into 3-D atmospheric chemistry transport models.

scholarly journals Synthesis of the Southeast Atmosphere Studies: Investigating Fundamental Atmospheric Chemistry Questions

2018 ◽  
Vol 99 (3) ◽  
pp. 547-567 ◽  
Author(s):  
Annmarie G. Carlton ◽  
Joost de Gouw ◽  
Jose L. Jimenez ◽  
Jesse L. Ambrose ◽  
Alexis R. Attwood ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Anthropogenic Pollution ◽  
Ozone Production ◽  
Atmospheric Composition ◽  
Eastern United States ◽  
Remotely Sensed Data ◽  
Sources And Sinks ◽  
Particle Properties ◽  
Pollutant Concentrations ◽  
Powerful Constraint

Abstract The Southeast Atmosphere Studies (SAS), which included the Southern Oxidant and Aerosol Study (SOAS); the Southeast Nexus (SENEX) study; and the Nitrogen, Oxidants, Mercury and Aerosols: Distributions, Sources and Sinks (NOMADSS) study, was deployed in the field from 1 June to 15 July 2013 in the central and eastern United States, and it overlapped with and was complemented by the Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. SAS investigated atmospheric chemistry and the associated air quality and climate-relevant particle properties. Coordinated measurements from six ground sites, four aircraft, tall towers, balloon-borne sondes, existing surface networks, and satellites provide in situ and remotely sensed data on trace-gas composition, aerosol physicochemical properties, and local and synoptic meteorology. Selected SAS findings indicate 1) dramatically reduced NOx concentrations have altered ozone production regimes; 2) indicators of “biogenic” secondary organic aerosol (SOA), once considered part of the natural background, were positively correlated with one or more indicators of anthropogenic pollution; and 3) liquid water dramatically impacted particle scattering while biogenic SOA did not. SAS findings suggest that atmosphere–biosphere interactions modulate ambient pollutant concentrations through complex mechanisms and feedbacks not yet adequately captured in atmospheric models. The SAS dataset, now publicly available, is a powerful constraint to develop predictive capability that enhances model representation of the response and subsequent impacts of changes in atmospheric composition to changes in emissions, chemistry, and meteorology.

The Nonlinear Nature of Atmospheric Chemistry

2021 ◽  
Author(s):  
Michael Prather
Keyword(s):  
Greenhouse Gases ◽  
Atmospheric Chemistry ◽  
Multiple Solutions ◽  
Taylor Expansion ◽  
Nonlinear Behavior ◽  
Nonlinear Problems ◽  
Tropospheric Chemistry ◽  
Tracer Transport ◽  
The Rich ◽  
Nonlinear Nature

&lt;p&gt;When scientific or policy-relevant questions involve atmospheric chemistry, one often hears &quot;nonlinear&quot; being invoked, but the precise nature of the nonlinearity is never delineated, and we are left with the fuzzy impression that nonlinear problems are difficult, with no simple answer.&amp;#160; I have even seen it used to avoid including indirect greenhouse gases in the Kyoto Protocol.&amp;#160; For differentiable systems, nonlinear behavior can be expressed through a Taylor expansion whereby any of the 2&lt;sup&gt;nd&lt;/sup&gt; order terms (x&lt;sup&gt;2&lt;/sup&gt;, y&lt;sup&gt;2&lt;/sup&gt; or xy) are the first nonlinear parts.&amp;#160; In this lecture I explore a range of scientific discoveries or developments in atmospheric chemistry where the nonlinear nature was critical to understanding the problem.&amp;#160; I select a set of problems worked on by many colleagues and myself over the last four decades.&amp;#160; These include: &amp;#160;multiple solutions in stratospheric chemistry; catastrophic depletion of ozone; numerical methods for tracer transport; our developing understanding of methane; chemical feedbacks and indirect greenhouse gases; and finally the rich heterogeneity of gases that drives tropospheric chemistry. I hope to convince you that by recognizing the nonlinear nature of atmospheric chemistry and understanding when it is important and when it is not, we can advance the field.&amp;#160; &amp;#160;&lt;/p&gt;

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