The description and validation of the computationally Efficient CH4–CO–OH (ECCOHv1.01) chemistry module for 3-D model applications

We present the Efficient CH4–CO–OH (ECCOH) chemistry module that allows for the simulation of the methane, carbon monoxide, and hydroxyl radical (CH4–CO–OH) system, within a chemistry climate model, carbon cycle model, or Earth system model. The computational efficiency of the module allows many multi-decadal sensitivity simulations of the CH4–CO–OH system, which primarily determines the global atmospheric oxidizing capacity. This capability is important for capturing the nonlinear feedbacks of the CH4–CO–OH system and understanding the perturbations to methane, CO, and OH, and the concomitant impacts on climate. We implemented the ECCOH chemistry module in the NASA GEOS-5 atmospheric global circulation model (AGCM), performed multiple sensitivity simulations of the CH4–CO–OH system over 2 decades, and evaluated the model output with surface and satellite data sets of methane and CO. The favorable comparison of output from the ECCOH chemistry module (as configured in the GEOS-5 AGCM) with observations demonstrates the fidelity of the module for use in scientific research.

[1]  Toshihiko Masui,et al.  GLOBAL GHG EMISSION SCENARIOS UNDER GHG CONCENTRATION STABILIZATION TARGETS , 2008 .

[2]  Daniel J. Jacob,et al.  Interannual variability in tropical tropospheric ozone and OH: The role of lightning , 2013 .

[3]  J. B. Miller,et al.  Contribution of anthropogenic and natural sources to atmospheric methane variability , 2006, Nature.

[4]  Michael B. McElroy,et al.  A 3‐D model analysis of the slowdown and interannual variability in the methane growth rate from 1988 to 1997 , 2004 .

[5]  John C. Gille,et al.  A global comparison of carbon monoxide profiles and column amounts from Tropospheric Emission Spectrometer (TES) and Measurements of Pollution in the Troposphere (MOPITT) , 2009 .

[6]  J. Lamarque,et al.  Preindustrial to present-day changes in tropospheric hydroxyl radical and methane lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) , 2012 .

[7]  Ian Barnes,et al.  Sources and Cycling of Tropospheric Hydroxyl Radicals – An Overview , 2010 .

[8]  Mian Chin,et al.  Indonesian wildfires of 1997: Impact on tropospheric chemistry , 2003 .

[9]  Kevin B. Strawbridge,et al.  The effect of model spatial resolution on Secondary Organic Aerosol predictions: a case study at Whistler, BC, Canada , 2012 .

[10]  Bryan N. Duncan,et al.  Implications of carbon monoxide bias for methane lifetime and atmospheric composition in chemistry climate models , 2015 .

[11]  Steven Pawson,et al.  Goddard Earth Observing System chemistry‐climate model simulations of stratospheric ozone‐temperature coupling between 1950 and 2005 , 2008 .

[12]  Kostas Tsigaridis,et al.  Interannual variability of tropospheric trace gases and aerosols: The role of biomass burning emissions , 2015 .

[13]  P. M. Lang,et al.  Distributions and recent changes of carbon monoxide in the lower troposphere , 1998 .

[14]  J. Randerson,et al.  Assessing variability and long-term trends in burned area by merging multiple satellite fire products , 2009 .

[15]  Chih-Chung Chang,et al.  Maximum efficiency in the hydroxyl-radical-based self-cleansing of the troposphere , 2014 .

[16]  P. Jöckel,et al.  Small Interannual Variability of Global Atmospheric Hydroxyl , 2011, Science.

[17]  William J. Collins,et al.  Multimodel estimates of intercontinental source-receptor relationships for ozone pollution , 2008 .

[18]  Mark Lawrence,et al.  Interhemispheric di ff erences in the chemical characteristics of the Indian Ocean aerosol during INDOEX , 2002 .

[19]  Peter Bergamaschi,et al.  Global column-averaged methane mixing ratios from 2003 to 2009 as derived from SCIAMACHY: Trends and variability , 2011 .

[20]  Michael J. Prather,et al.  Future methane, hydroxyl, and their uncertainties: key climate and emission parameters for future predictions , 2012 .

[21]  Peter Bergamaschi,et al.  A multi-year methane inversion using SCIAMACHY, accounting for systematic errors using TCCON measurements , 2013 .

[22]  Luke D. Oman,et al.  The response of tropical tropospheric ozone to ENSO , 2011 .

[23]  Shian‐Jiann Lin A “Vertically Lagrangian” Finite-Volume Dynamical Core for Global Models , 2004 .

[24]  J. Lamarque,et al.  The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): overview and description of models, simulations and climate diagnostics , 2012 .

[25]  E. J. Dlugokencky,et al.  Atmospheric Methane Dry Air Mole Fractions (1983-2015) and Atmospheric Carbon Dioxide Dry Air Mole Fractions (1968-2015) from the NOAA ESRL Carbon Cycle Cooperative Global Air Sampling Network, original data files , 2016 .

[26]  Bryan N. Duncan,et al.  Parameterization of OH for efficient computation in chemical tracer models , 2000 .

[27]  Susan S. Kulawik,et al.  Carbon monoxide (CO) vertical profiles derived from joined TES and MLS measurements , 2013 .

[28]  Oliver Wild,et al.  How sensitive is tropospheric oxidation to anthropogenic emissions? , 2008 .

[29]  Michael J. Prather,et al.  Time scales in atmospheric chemistry: Theory, GWPs for CH4 and CO, and runaway growth , 1996 .

[30]  Bryan N. Duncan,et al.  Observationally derived transport diagnostics for the lowermost stratosphere and their application to the GMI chemistry and transport model , 2007 .

[31]  Ralph J. Cicerone,et al.  Stellar occultation measurements of atmospheric ozone and chlorine from OAO 3 , 1976 .

[32]  H. Worden,et al.  Observations of near-surface carbon monoxide from space using MOPITT multispectral retrievals , 2010 .

[33]  R. Martin,et al.  Interannual and seasonal variability of biomass burning emissions constrained by satellite observations , 2003 .

[34]  Michael B. McElroy,et al.  A quantitative assessment of uncertainties affecting estimates of global mean OH derived from methyl chloroform observations , 2008 .

[35]  Michael J. Prather,et al.  Reactive greenhouse gas scenarios: Systematic exploration of uncertainties and the role of atmospheric chemistry , 2012 .

[36]  Andrea Molod,et al.  The GEOS-5 Atmospheric General Circulation Model: Mean Climate and Development from MERRA to Fortuna , 2012 .

[37]  O. Hasekamp,et al.  Error analysis for CO and CH 4 total column retrievals from SCIAMACHY 2.3 μm spectra , 2008 .

[38]  Derek M. Cunnold,et al.  Evidence for variability of atmospheric hydroxyl radicals over the past quarter century , 2005 .

[39]  Wouter Peters,et al.  Stability of tropospheric hydroxyl chemistry , 2002 .

[40]  Pieter P. Tans,et al.  Mixing ratios of carbon monoxide in the troposphere , 1992 .

[41]  Toshihiko Masui,et al.  Multi-gas Mitigation Analysis on Stabilization Scenarios Using Aim Global Model , 2006 .

[42]  Ralph J. Cicerone,et al.  Possible variations in atmospheric methane , 1977 .

[43]  Bryan N. Duncan,et al.  Model analysis of the factors regulating the trends and variability of carbon monoxide between 1988 and 1997 , 2008 .

[44]  Daniel Stone,et al.  Tropospheric OH and HO2 radicals: field measurements and model comparisons. , 2012, Chemical Society reviews.

[45]  G. Carmichael,et al.  Effect of different emission inventories on modeled ozone and carbon monoxide in Southeast Asia , 2014 .

[46]  Franz Rohrer,et al.  Strong correlation between levels of tropospheric hydroxyl radicals and solar ultraviolet radiation , 2006, Nature.

[47]  Maximilian Reuter,et al.  Long-term analysis of carbon dioxide and methane column-averaged mole fractions retrieved from SCIAMACHY , 2010 .

[48]  Nathaniel J. Livesey,et al.  Model study of the cross-tropopause transport of biomass burning pollution , 2007 .

[49]  David G. Streets,et al.  Linking ozone pollution and climate change: The case for controlling methane , 2002 .

[50]  Michael B. McElroy,et al.  Three-dimensional climatological distribution of tropospheric OH: Update and evaluation , 2000 .

[51]  Veronika Eyring,et al.  Analysis of Present Day and Future OH and Methane Lifetime in the ACCMIP Simulations , 2012 .

[52]  Merritt N. Deeter,et al.  Evaluation of MOPITT retrievals of lower‐tropospheric carbon monoxide over the United States , 2012 .

[53]  Jos Lelieveld,et al.  Impact of HONO on global atmospheric chemistry calculated with an empirical parameterization in the EMAC model , 2012 .

[54]  Richard G. Derwent,et al.  Multimodel simulations of carbon monoxide: Comparison with observations and projected near‐future changes , 2006 .

[55]  Michael B. McElroy,et al.  Tropospheric OH in a three-dimensional chemical tracer model: An assessment based on observations of CH3CCl3 , 1990 .

[56]  Paul J. Crutzen,et al.  Global and regional impacts of HONO on the chemical composition of clouds and aerosols , 2013 .

[57]  Peter Bergamaschi,et al.  Three years of greenhouse gas column-averaged dry air mole fractions retrieved from satellite - Part 2: Methane , 2008 .

[58]  Shamil Maksyutov,et al.  TransCom model simulations of CH4 and related species: linking transport, surface flux and chemical loss with CH4 variability in the troposphere and lower stratosphere , 2011 .

[59]  K. Wolter,et al.  El Niño/Southern Oscillation behaviour since 1871 as diagnosed in an extended multivariate ENSO index (MEI.ext) , 2011 .

[60]  Arlene M. Fiore,et al.  Impact of meteorology and emissions on methane trends, 1990–2004 , 2006 .

[61]  Mian Chin,et al.  Influence of the 2006 Indonesian biomass burning aerosols on tropical dynamics studied with the GEOS-5 AGCM , 2010 .

[62]  Bryan N. Duncan,et al.  Implications of model bias in carbon monoxide for methane lifetime , 2015 .

[63]  Bryan N. Duncan,et al.  Global budget of CO, 1988–1997: Source estimates and validation with a global model , 2007 .

[64]  Glenn S. Diskin,et al.  Multi-model study of chemical and physical controls on transport of anthropogenic and biomass burning pollution to the Arctic , 2014 .

[65]  Michael J. Prather,et al.  Lifetimes and eigenstates in atmospheric chemistry , 1994 .