Interannual Variability and Trends of CH4, CO and OH Using the Computationally-Efficient CH4-CO-OH (ECCOH) Module

Methane (CH4) is the second most important anthropogenic greenhouse gas (GHG). Its 100-year global warming potential (GWP) is 34 times larger than that for carbon dioxide. The 100-year integrated GWPof CH4 is sensitive to changes in hydroxyl radical (OH) levels.Oxidation of CH4 and carbon monoxide (CO) by OH is the main loss process, thus affecting the oxidizing capacity of the atmosphere and contributing to the global ozone background. Limitations of using archived, monthly OH fields for studies of methane's and COs evolution are that feedbacks of the CH4-CO-OH system on methane, CO and OH are not captured. In this study, we employ the computationally Efficient CH4-CO-OH (ECCOH) module (Elshorbany et al., 2015) to investigate the nonlinear feedbacks of the CH4-CO-OH system on the interannual variability and trends of the CH4, CO, OH system

Climate policy implications of nonlinear decline of Arctic land permafrost and other cryosphere elements

Arctic feedbacks accelerate climate change through carbon releases from thawing permafrost and higher solar absorption from reductions in the surface albedo, following loss of sea ice and land snow. Here, we include dynamic emulators of complex physical models in the integrated assessment model PAGE-ICE to explore nonlinear transitions in the Arctic feedbacks and their subsequent impacts on the global climate and economy under the Paris Agreement scenarios. The permafrost feedback is increasingly positive in warmer climates, while the albedo feedback weakens as the ice and snow melt. Combined, these two factors lead to significant increases in the mean discounted economic effect of climate change: +4.0% ($24.8 trillion) under the 1.5 °C scenario, +5.5$33.8 trillion) under the 2 °C scenario, and +4.8% ($66.9 trillion) under mitigation levels consistent with the current national pledges. Considering the nonlinear Arctic feedbacks makes the 1.5 °C target marginally more economically attractive than the 2 °C target, although both are statistically equivalent.This work is part of the ICE-ARC project funded by the European Union’s 7th Framework Programme, (grant 603887, contribution 006). D.Y. received additional funding from ERIM, Erasmus University Rotterdam, and Paul Ekins at the ISR, University College London. K.S. was funded by NSF (grant 1503559) and NASA (grants NNX14A154G, NNX17AC59A). E.J. was funded by the NGEE Arctic project supported by the BER Office of Science at the U.S. DOE. Y.E. was funded by the NSF (grant 1900795). E.B. was supported by the UK Met Office Hadley Centre Climate Programme funded by BEIS and DEFRA

Assessing chemistry schemes and constraints in air quality models used to predict ozone in London against the detailed Master Chemical Mechanism

Air pollution is the environmental factor with the greatest impact on human health in Europe. Understanding the key processes driving air quality across the relevant spatial scales, especially during pollution exceedances and episodes, is essential to provide effective predictions for both policymakers and the public. It is particularly important for policy regulators to understand the drivers of local air quality that can be regulated by national policies versus the contribution from regional pollution transported from mainland Europe or elsewhere. One of the main objectives of the Coupled Urban and Regional processes: Effects on AIR quality (CUREAIR) project is to determine local and regional contributions to ozone events. A detailed zero-dimensional (0-D) box model run with the Master Chemical Mechanism (MCMv3.2) is used as the benchmark model against which the less explicit chemistry mechanisms of the Generic Reaction Set (GRS) and the Common Representative Intermediates (CRIv2-R5) schemes are evaluated. GRS and CRI are used by the Atmospheric Dispersion Modelling System (ADMS-Urban) and the regional chemistry transport model EMEP4UK, respectively. The MCM model uses a near-explicit chemical scheme for the oxidation of volatile organic compounds (VOCs) and is constrained to observations of VOCs, NOx, CO, HONO (nitrous acid), photolysis frequencies and meteorological parameters measured during the ClearfLo (Clean Air for London) campaign. The sensitivity of the less explicit chemistry schemes to different model inputs has been investigated: Constraining GRS to the total VOC observed during ClearfLo as opposed to VOC derived from ADMS-Urban dispersion calculations, including emissions and background concentrations, led to a significant increase (674% during winter) in modelled ozone. The inclusion of HONO chemistry in this mechanism, particularly during wintertime when other radical sources are limited, led to substantial increases in the ozone levels predicted (223%). When the GRS and CRIv2-R5 schemes are run with the equivalent model constraints to the MCM, they are able to reproduce the level of ozone predicted by the near-explicit MCM to within 40% and 20% respectively for the majority of the time. An exception to this trend was observed during pollution episodes experienced in the summer, when anticyclonic conditions favoured increased temperatures and elevated O3. The in situ O3 predicted by the MCM was heavily influenced by biogenic VOCs during these conditions and the low GRS [O3] : MCM [O3] ratio (and low CRIv2-R5 [O3] : MCM [O3] ratio) demonstrates that these less explicit schemes under-represent the full O3 creation potential of these VOCs. To fully assess the influence of the in situ O3 generated from local emissions versus O3 generated upwind of London and advected in, the time since emission (and, hence, how far the real atmosphere is from steady state) must be determined. From estimates of the mean transport time determined from the NOx : NOy ratio observed at North Kensington during the summer and comparison of the O3 predicted by the MCM model after this time, ∼60% of the median observed [O3] could be generated from local emissions. During the warmer conditions experienced during the easterly flows, however, the observed [O3] may be even more heavily influenced by London's emissions

On the interpretation of in situ HONO observations via photochemical steady state

A substantial body of recent literature has shown that boundary layer HONO levels are higher than can be explained by simple, established gas-phase chemistry, to an extent that implies that additional HONO sources represent a major, or the dominant, precursor to OH radicals in such environments. This conclusion may be reached by analysis of point observations of (for example) OH, NO and HONO, alongside photochemical parameters; however both NO and HONO have non-negligible atmospheric lifetimes, so these approaches may be problematic if substantial spatial heterogeneity exists. We report a new dataset of HONO, NOx and HOx observations recorded at an urban background location, which support the existence of additional HONO sources as determined elsewhere. We qualitatively evaluate the possible impacts of local heterogeneity using a series of idealised numerical model simulations, building upon the work of Lee et al. (J. Geophys. Res., 2013, DOI: 10.1002/2013JD020341). The simulations illustrate the time required for photostationary state approaches to yield accurate results following substantial perturbations in the HOx/NOx/NOy chemistry, and the scope for bias to an inferred HONO source from NOx and VOC emissions in either a positive or negative sense, depending upon the air mass age following emission. To assess the extent to which these impacts may be present in actual measurements, we present exploratory spatially resolved measurements of HONO and NOx abundance obtained using a mobile instrumented laboratory. Measurements of the spatial variability of HONO in urban, suburban and rural environments show pronounced changes in abundance are found in proximity to major roads within urban areas, indicating that photo-stationary steady state (PSS) analyses in such areas are likely to be problematic. The measurements also show areas of very homogeneous HONO and NOx abundance in rural, and some suburban, regions, where the PSS approach is likely to be valid. Implications for future exploration of HONO production mechanisms are discussed

Tropospheric Ozone Assessment Report : A critical review of changes in the tropospheric ozone burden and budget from 1850 to 2100

Our understanding of the processes that control the burden and budget of tropospheric ozone has changed dramatically over the last 60 years. Models are the key tools used to understand these changes, and these underscore that there are many processes important in controlling the tropospheric ozone budget. In this critical review, we assess our evolving understanding of these processes, both physical and chemical. We review model simulations from the International Global Atmospheric Chemistry Atmospheric Chemistry and Climate Model Intercomparison Project and Chemistry Climate Modelling Initiative to assess the changes in the tropospheric ozone burden and its budget from 1850 to 2010. Analysis of these data indicates that there has been significant growth in the ozone burden from 1850 to 2000 (approximately 43 + 9%) but smaller growth between 1960 and 2000 (approximately 16 +/- 10%) and that the models simulate burdens of ozone well within recent satellite estimates. The Chemistry Climate Modelling Initiative model ozone budgets indicate that the net chemical production of ozone in the troposphere plateaued in the 1990s and has not changed since then inspite of increases in the burden. There has been a shift in net ozone production in the troposphere being greatest in the northern mid and high latitudes to the northern tropics, driven by the regional evolution of precursor emissions. An analysis of the evolution of tropospheric ozone through the 21st century, as simulated by Climate Model Intercomparison Project Phase 5 models, reveals a large source of uncertainty associated with models themselves (i.e., in the way that they simulate the chemical and physical processes that control tropospheric ozone). This structural uncertainty is greatest in the near term (two to three decades), but emissions scenarios dominate uncertainty in the longer term (2050- 2100) evolution of tropospheric ozone. This intrinsic model uncertainty prevents robust predictions of near-term changes in the tropospheric ozone burden, and we review how progress can be made to reduce this limitation

Tropospheric Oxidation Capacity and Ozone Photochemical Formation: Investigation of the current understanding of urban atmospheric chemistry: Field Measurements and Modeling Study in the city of Santiago de Chile

The present study provides a detailed analysis of the tropospheric photochemical oxidation processes and ozone photochemical formation under typical polluted urban conditions taking the city of Santiago de Chile as an example. Two field measurement campaigns were carried out in the city of Santiago de Chile during summer and winter. The oxidation capacity of the atmosphere over the urban area of Santiago, Chile and its seasonal dependency has been studied during the two measurement campaigns. The measurement data were used to constrain a simple photostationary-state (PSS) model and a zero dimensional photochemical box model based on the MCMv3.1. Summertime photochemical ozone formation in the urban area of Santiago, Chile has also been investigated using MCMv3.1. The results of the model simulations have been compared with a set of potential empirical indicator relationships. The ozone forming potential of each measured VOC has been determined using the MCM box model. The impacts of the above study on possible summertime ozone control strategies in Santiago are discussed. As a result of this explicit study, questions have been also raised and outlooks to the Future are presented.https://digitalcommons.usf.edu/books/1061/thumbnail.jp

Calling: Earth #045 - Yasin Elshorbany, Atmospheric Scientist

In this episode of Calling: Earth, we talk with Yasin Elshorbany, Assistant Professor in the USF School of Geosciences about his research of atmospheric chemistry and how that can relate to climate change, and economic change and impact. More about Yasin can be found here: Selected Works Google Scholar USF SGS Faculty Webpag

Impact of HONO on global atmospheric chemistry calculated with an empirical parameterization in the EMAC model

The photolysis of HONO is important for the atmospheric HOx (OH + HO2) radical budget and ozone formation, especially in polluted air. Nevertheless, owing to the incomplete knowledge of HONO sources, realistic HONO mechanisms have not yet been implemented in global models. We investigated measurement data sets from 15 field measurement campaigns conducted in different countries worldwide. It appears that the HONO/NOx ratio is a good proxy predictor for HONO mixing ratios under different atmospheric conditions. From the robust relationship between HONO and NOx, a representative mean HONO/NOx ratio of 0.02 has been derived. Using a global chemistry-climate model and employing this HONO/NOx ratio, realistic HONO levels are simulated, being about one order of magnitude higher than the reference calculations that only consider the reaction OH + NO -\u3e HONO. The resulting enhancement of HONO significantly impacts HOx levels and photo-oxidation products (e.g, O-3, PAN), mainly in polluted regions. Furthermore, the relative enhancements in OH and secondary products are higher in winter than in summer, thus enhancing the oxidation capacity in polluted regions, especially in winter when other photolytic OH sources are of minor importance. Our results underscore the need to improve the understanding of HONO chemistry and its representation in atmospheric models