scholarly journals A machine learning examination of hydroxyl radical differences among model simulations for CCMI-1

2020 ◽  
Vol 20 (3) ◽  
pp. 1341-1361 ◽  
Author(s):  
Julie M. Nicely ◽  
Bryan N. Duncan ◽  
Thomas F. Hanisco ◽  
Glenn M. Wolfe ◽  
Ross J. Salawitch ◽  
...  
Keyword(s):  
Hydroxyl Radical ◽  
Water Vapour ◽  
Climate Model ◽  
Uv Light ◽  
Temporal Trends ◽  
Historical Simulation ◽  
Sources And Sinks ◽  
Photolysis Frequency ◽  
Dynamics Simulations ◽  
Ozone Column

Abstract. The hydroxyl radical (OH) plays critical roles within the troposphere, such as determining the lifetime of methane (CH4), yet is challenging to model due to its fast cycling and dependence on a multitude of sources and sinks. As a result, the reasons for variations in OH and the resulting methane lifetime (τCH4), both between models and in time, are difficult to diagnose. We apply a neural network (NN) approach to address this issue within a group of models that participated in the Chemistry-Climate Model Initiative (CCMI). Analysis of the historical specified dynamics simulations performed for CCMI indicates that the primary drivers of τCH4 differences among 10 models are the flux of UV light to the troposphere (indicated by the photolysis frequency JO1D), the mixing ratio of tropospheric ozone (O3), the abundance of nitrogen oxides (NOx≡NO+NO2), and details of the various chemical mechanisms that drive OH. Water vapour, carbon monoxide (CO), the ratio of NO:NOx, and formaldehyde (HCHO) explain moderate differences in τCH4, while isoprene, methane, the photolysis frequency of NO2 by visible light (JNO2), overhead ozone column, and temperature account for little to no model variation in τCH4. We also apply the NNs to analysis of temporal trends in OH from 1980 to 2015. All models that participated in the specified dynamics historical simulation for CCMI demonstrate a decline in τCH4 during the analysed timeframe. The significant contributors to this trend, in order of importance, are tropospheric O3, JO1D, NOx, and H2O, with CO also causing substantial interannual variability in OH burden. Finally, the identified trends in τCH4 are compared to calculated trends in the tropospheric mean OH concentration from previous work, based on analysis of observations. The comparison reveals a robust result for the effect of rising water vapour on OH and τCH4, imparting an increasing and decreasing trend of about 0.5 % decade−1, respectively. The responses due to NOx, ozone column, and temperature are also in reasonably good agreement between the two studies.

scholarly journals A Machine Learning Examination of Hydroxyl Radical Differences Among Model Simulations for CCMI-1

2019 ◽  
Author(s):  
Julie M. Nicely ◽  
Bryan N. Duncan ◽  
Thomas F. Hanisco ◽  
Glenn M. Wolfe ◽  
Ross J. Salawitch ◽  
...  
Keyword(s):  
Water Vapor ◽  
Hydroxyl Radical ◽  
Climate Model ◽  
Uv Light ◽  
Temporal Trends ◽  
Historical Simulation ◽  
Sources And Sinks ◽  
Chemical Mechanisms ◽  
Photolysis Frequency ◽  
Dynamics Simulations

Abstract. Hydroxyl radical (OH) plays critical roles within the troposphere, such as determining the lifetime of methane (CH4), yet is challenging to model due to its fast cycling and dependence on a multitude of sources and sinks. As a result, the reasons for variations in OH and the resulting CH4 lifetime (τCH4), both between models and in time, are difficult to diagnose. We apply a neural network (NN) approach to address this issue within a group of models that participated in the Chemistry-Climate Model Initiative (CCMI). Analysis of the historical specified dynamics simulations performed for CCMI indicates that the primary drivers of τCH4 differences among ten models are the flux of UV light to the troposphere (indicated by the photolysis frequency JO1D) due mostly to clouds, mixing ratio of tropospheric ozone (O3), the abundance of nitrogen oxides (NOx≡NO+NO2), and details of the various chemical mechanisms that drive OH. Water vapor, carbon monoxide (CO), the ratio of NO:NOx, and formaldehyde (HCHO) explain moderate differences in τCH4, while isoprene, CH4, the photolysis frequency of NO2 by visible light (JNO2), overhead O3 column, and temperature account for little-to-no model variation in τCH4. We also apply the NNs to analysis of temporal trends in OH from 1980 to 2015. All models that participated in the specified dynamics historical simulation for CCMI demonstrate a decline in τCH4 during the analysed timeframe. The significant contributors to this trend, in order of importance, are tropospheric O3, JO1D, NOx, and H2O, with CO also causing substantial interannual variability in OH burden. Finally, the identified trends in τCH4 are compared to calculated trends in the tropospheric mean OH concentration from previous work, based on analysis of observations. The comparison reveals a robust result for the effect of rising water vapor on OH and τCH4, imparting an increasing and decreasing trend of about 0.5 % decade−1, respectively. The responses due to NOx, O3 column, and temperature are also in reasonably good agreement between the two studies, though a discrepancy in the CH4 response highlights a need for further examination of the CH4 feedback on the abundance of OH.

scholarly journals Effects of Strongly Enhanced Atmospheric Methane Concentrations in a Fully Coupled Chemistry-Climate Model

2020 ◽  
Author(s):  
Laura Stecher ◽  
Franziska Winterstein ◽  
Martin Dameris ◽  
Patrick Jöckel ◽  
Michael Ponater ◽  
...  
Keyword(s):  
Hydroxyl Radical ◽  
Water Vapour ◽  
Climate Sensitivity ◽  
Radiative Forcing ◽  
Climate Model ◽  
Atmospheric Methane ◽  
Climate Feedbacks ◽  
Mixing Ratios ◽  
Radiative Impact ◽  
Stratospheric Water Vapour

Abstract. In a previous study the quasi-instantaneous chemical impacts (rapid adjustments) of strongly enhanced methane (CH4) mixing ratios have been analyzed. However, to quantify the influence of the respective slow climate feedbacks on the chemical composition it is necessary to include the radiation driven temperature feedback. Therefore, we perform sensitivity simulations with doubled and fivefold present-day (year 2010) CH4 mixing ratios with the chemistry-climate model EMAC and include in a novel set-up a mixed layer ocean model to account for tropospheric warming. We find that the slow climate feedbacks counteract the reduction of the hydroxyl radical in the troposphere, which is caused by the strongly enhanced CH4 mixing ratios. Thereby also the resulting prolongation of the tropospheric CH4 lifetime is weakened compared to the quasi-instantaneous response considered previously. Changes in the stratospheric circulation evolve clearly with the warming of the troposphere. The Brewer-Dobson circulation strengthens, affecting the response of trace gases, such as ozone, water vapour and CH4 in the stratosphere, and also causing stratospheric temperature changes. In the middle and upper stratosphere, the increase of stratospheric water vapour is reduced with respect to the quasi-instantaneous response. Weaker increases of the hydroxyl radical cause the chemical depletion of CH4 to be less strongly enhanced and thus the in situ source of stratospheric water vapour as well. However, in the lower stratosphere water vapour increases more strongly when tropospheric warming is accounted for enlarging its overall radiative impact. The response of the stratospheric adjusted temperatures driven by slow climate feedbacks is dominated by these increases of stratospheric water vapour, as well as strongly decreased ozone mixing ratios above the tropical tropopause, which result from enhanced tropical upwelling. While rapid radiative adjustments from ozone and stratospheric water vapour make an essential contribution to the effective CH4 radiative forcing, the radiative impact of the respective slow feedbacks is rather moderate. In line with this, the climate sensitivity from CH4 changes in this chemistry-climate model setup is not significantly different from the climate sensitivity in carbon dioxide-driven simulations, provided that the CH4 effective radiative forcing includes the rapid adjustments from ozone and stratospheric water vapour changes.

scholarly journals Computational Design of Radical Recognition Assay with the Possible Application of Cyclopropyl Vinyl Sulfides as Tunable Sensors

2021 ◽  
Vol 22 (14) ◽  
pp. 7637
Author(s):  
Liliya T. Sahharova ◽  
Evgeniy G. Gordeev ◽  
Dmitry B. Eremin ◽  
Valentine P. Ananikov
Keyword(s):  
Uv Light ◽  
Computational Design ◽  
Energy Profiles ◽  
Vinyl Sulfides ◽  
Tunable Sensors ◽  
Radical Generation ◽  
Metal Catalyzed ◽  
Dynamics Simulations ◽  
Simulations And Modeling ◽  
Insight Into

The processes involving the capture of free radicals were explored by performing DFT molecular dynamics simulations and modeling of reaction energy profiles. We describe the idea of a radical recognition assay, where not only the presence of a radical but also the nature/reactivity of a radical may be assessed. The idea is to utilize a set of radical-sensitive molecules as tunable sensors, followed by insight into the studied radical species based on the observed reactivity/selectivity. We utilize this approach for selective recognition of common radicals—alkyl, phenyl, and iodine. By matching quantum chemical calculations with experimental data, we show that components of a system react differently with the studied radicals. Possible radical generation processes were studied involving model reactions under UV light and metal-catalyzed conditions.

scholarly journals Pressure effects on water vapour lines: beyond the Voigt profile

2012 ◽  
Vol 370 (1968) ◽  
pp. 2495-2508 ◽  
Author(s):  
N. H. Ngo ◽  
H. Tran ◽  
R. R. Gamache ◽  
J. M. Hartmann
Keyword(s):  
Water Vapour ◽  
Line Shape ◽  
Pressure Effects ◽  
Shape Model ◽  
Line Shapes ◽  
Voigt Profile ◽  
Voigt Model ◽  
Velocity Changes ◽  
Dynamics Simulations ◽  
Induced Velocity

A short overview of recent results on the effects of pressure (collisions) regarding the shape of isolated infrared lines of water vapour is presented. The first part of this study considers the basic collisional quantities, which are the pressure-broadening and -shifting coefficients, central parameters of the Lorentzian (and Voigt) profile and thus of any sophisticated line-shape model. Through comparisons of measured values with semi-classical calculations, the influences of the molecular states (both rotational and vibrational) involved and of the temperature are analysed. This shows the relatively unusual behaviour of H 2 O broadening, with evidence of a significant vibrational dependence and the fact that the broadening coefficient (in cm −1 atm −1 ) of some lines increases with temperature. In the second part of this study, line shapes beyond the Voigt model are considered, thus now taking ‘velocity effects’ into account. These include both the influence of collisionally induced velocity changes that lead to the so-called Dicke narrowing and the influence of the dependence of collisional parameters on the speed of the radiating molecule. Experimental evidence of deviations from the Voigt shape is presented and analysed. The interest of classical molecular dynamics simulations, to model velocity changes, together with semi-classical calculations of the speed-dependent collisional parameters for line-shape predictions from ‘first principles’, are discussed.

scholarly journals Simulation of the isotopic composition of stratospheric water vapour – Part 1: Description and evaluation of the EMAC model

2015 ◽  
Vol 15 (10) ◽  
pp. 5537-5555 ◽  
Author(s):  
R. Eichinger ◽  
P. Jöckel ◽  
S. Brinkop ◽  
M. Werner ◽  
S. Lossow
Keyword(s):  
Isotopic Composition ◽  
Water Vapour ◽  
General Circulation ◽  
Climate Model ◽  
Hydrological Cycle ◽  
Circulation Model ◽  
Isotope Ratios ◽  
Physical Fractionation ◽  
Water Isotopologues ◽  
Stratospheric Water Vapour

Abstract. This modelling study aims at an improved understanding of the processes that determine the water vapour budget in the stratosphere by means of the investigation of water isotope ratios. An additional (and separate from the actual) hydrological cycle has been introduced into the chemistry–climate model EMAC, including the water isotopologues HDO and H218O and their physical fractionation processes. Additionally an explicit computation of the contribution of methane oxidation to H2O and HDO has been incorporated. The model expansions allow detailed analyses of water vapour and its isotope ratio with respect to deuterium throughout the stratosphere and in the transition region to the troposphere. In order to assure the correct representation of the water isotopologues in the model's hydrological cycle, the expanded system has been evaluated in several steps. The physical fractionation effects have been evaluated by comparison of the simulated isotopic composition of precipitation with measurements from a ground-based network (GNIP) and with the results from the isotopologue-enabled general circulation model ECHAM5-wiso. The model's representation of the chemical HDO precursor CH3D in the stratosphere has been confirmed by a comparison with chemical transport models (1-D, CHEM2D) and measurements from radiosonde flights. Finally, the simulated stratospheric HDO and the isotopic composition of water vapour have been evaluated, with respect to retrievals from three different satellite instruments (MIPAS, ACE-FTS, SMR). Discrepancies in stratospheric water vapour isotope ratios between two of the three satellite retrievals can now partly be explained.

scholarly journals On the role of trend and variability in the hydroxyl radical (OH) in the global methane budget

2020 ◽  
Vol 20 (21) ◽  
pp. 13011-13022
Author(s):  
Yuanhong Zhao ◽  
Marielle Saunois ◽  
Philippe Bousquet ◽  
Xin Lin ◽  
Antoine Berchet ◽  
...  
Keyword(s):  
Hydroxyl Radical ◽  
El Niño ◽  
Climate Model ◽  
El Nino ◽  
Interannual Variations ◽  
Atmospheric Methane ◽  
Tropical Regions ◽  
Ch4 Emissions ◽  
Methane Budget

Abstract. Decadal trends and interannual variations in the hydroxyl radical (OH), while poorly constrained at present, are critical for understanding the observed evolution of atmospheric methane (CH4). Through analyzing the OH fields simulated by the model ensemble of the Chemistry–Climate Model Initiative (CCMI), we find (1) the negative OH anomalies during the El Niño years mainly corresponding to the enhanced carbon monoxide (CO) emissions from biomass burning and (2) a positive OH trend during 1980–2010 dominated by the elevated primary production and the reduced loss of OH due to decreasing CO after 2000. Both two-box model inversions and variational 4D inversions suggest that ignoring the negative anomaly of OH during the El Niño years leads to a large overestimation of the increase in global CH4 emissions by up to 10 ± 3 Tg yr−1 to match the observed CH4 increase over these years. Not accounting for the increasing OH trends given by the CCMI models leads to an underestimation of the CH4 emission increase by 23 ± 9 Tg yr−1 from 1986 to 2010. The variational-inversion-estimated CH4 emissions show that the tropical regions contribute most to the uncertainties related to OH. This study highlights the significant impact of climate and chemical feedbacks related to OH on the top-down estimates of the global CH4 budget.

scholarly journals How sensitive is the recovery of stratospheric ozone to changes in concentrations of very short-lived bromocarbons?

2014 ◽  
Vol 14 (19) ◽  
pp. 10431-10438 ◽  
Author(s):  
X. Yang ◽  
N. L. Abraham ◽  
A. T. Archibald ◽  
P. Braesicke ◽  
J. Keeble ◽  
...  
Keyword(s):  
Climate Model ◽  
Stratospheric Ozone ◽  
Montreal Protocol ◽  
Background Concentrations ◽  
Future Situation ◽  
Antarctic Ozone ◽  
The Antarctic ◽  
The Impact ◽  
Ozone Column ◽  
Policy Question

Abstract. Naturally produced very short-lived substances (VSLS) account for almost a quarter of the current stratospheric inorganic bromine, Bry. Following VSLS oxidation, bromine radicals (Br and BrO) can catalytically destroy ozone. The extent to which possible increases in surface emissions or transport of these VSLS bromocarbons to the stratosphere could counteract the effect of halogen reductions under the Montreal Protocol is an important policy question. Here, by using a chemistry–climate model, UM-UKCA, we investigate the impact of a hypothetical doubling (an increase of 5 ppt Bry) of VSLS bromocarbons on ozone and how the resulting ozone changes depend on the background concentrations of chlorine and bromine. Our model experiments indicate that for the 5 ppt increase in Bry from VSLS, the ozone decrease in the lowermost stratosphere of the Southern Hemisphere (SH) may reach up to 10% in the annual mean; the ozone decrease in the Northern Hemisphere (NH) is smaller (4–6%). The largest impact on the ozone column is found in the Antarctic spring. There is a significantly larger ozone decrease following the doubling of the VSLS burden under a high stratospheric chlorine background than under a low chlorine background, indicating the importance of the inter-halogen reactions. For example, the decline in the high-latitude, lower-stratospheric ozone concentration as a function of Bry is higher by about 30–40% when stratospheric Cly is ~ 3 ppb (present day), compared with Cly of ~ 0.8 ppb (a pre-industrial or projected future situation). Bromine will play an important role in the future ozone layer. However, even if bromine levels from natural VSLS were to increase significantly later this century, changes in the concentration of ozone will likely be dominated by the decrease in anthropogenic chlorine. Our calculation suggests that for a 5 ppt increase in Bry from VSLS, the Antarctic ozone hole recovery date could be delayed by approximately 6–8 years, depending on Cly levels.

Influence of Ocean and Atmosphere Components on Simulated Climate Sensitivities

2013 ◽  
Vol 26 (1) ◽  
pp. 231-245 ◽  
Author(s):  
Michael Winton ◽  
Alistair Adcroft ◽  
Stephen M. Griffies ◽  
Robert W. Hallberg ◽  
Larry W. Horowitz ◽  
...  
Keyword(s):  
Sea Ice ◽  
Climate Models ◽  
Climate Model ◽  
Model Simulation ◽  
Coupled Model ◽  
Ocean Model ◽  
Historical Simulation ◽  
Model Version ◽  
Salinity Response ◽  
The Impact

Abstract The influence of alternative ocean and atmosphere subcomponents on climate model simulation of transient sensitivities is examined by comparing three GFDL climate models used for phase 5 of the Coupled Model Intercomparison Project (CMIP5). The base model ESM2M is closely related to GFDL’s CMIP3 climate model version 2.1 (CM2.1), and makes use of a depth coordinate ocean component. The second model, ESM2G, is identical to ESM2M but makes use of an isopycnal coordinate ocean model. The authors compare the impact of this “ocean swap” with an “atmosphere swap” that produces the GFDL Climate Model version 3 (CM3) by replacing the AM2 atmospheric component with AM3 while retaining a depth coordinate ocean model. The atmosphere swap is found to have much larger influence on sensitivities of global surface temperature and Northern Hemisphere sea ice cover. The atmosphere swap also introduces a multidecadal response time scale through its indirect influence on heat uptake. Despite significant differences in their interior ocean mean states, the ESM2M and ESM2G simulations of these metrics of climate change are very similar, except for an enhanced high-latitude salinity response accompanied by temporarily advancing sea ice in ESM2G. In the ESM2G historical simulation this behavior results in the establishment of a strong halocline in the subpolar North Atlantic during the early twentieth century and an associated cooling, which are counter to observations in that region. The Atlantic meridional overturning declines comparably in all three models.

scholarly journals Preindustrial-to-present-day radiative forcing by tropospheric ozone from improved simulations with the GISS chemistry-climate GCM

2003 ◽  
Vol 3 (5) ◽  
pp. 1675-1702 ◽  
Author(s):  
D. T. Shindell ◽  
G. Faluvegi ◽  
N. Bell
Keyword(s):  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
General Circulation ◽  
Climate Model ◽  
Circulation Model ◽  
Tropospheric Chemistry ◽  
True Value ◽  
Tropopause Region ◽  
Dynamics Simulations ◽  
Goddard Institute

Abstract. Improved estimates of the radiative forcing from tropospheric ozone increases since the preindustrial have been calculated with the tropospheric chemistry model used at the Goddard Institute for Space Studies (GISS) within the GISS general circulation model (GCM). The chemistry in this model has been expanded to include simplified representations of peroxyacetylnitrates and non-methane hydrocarbons in addition to background NOx-HOx-Ox-CO-CH4 chemistry. The GCM has improved resolution and physics in the boundary layer, improved resolution near the tropopause, and now contains a full representation of stratospheric dynamics. Simulations of present-day conditions show that this coupled chemistry-climate model is better able to reproduce observed tropospheric ozone, especially in the tropopause region, which is critical to climate forcing. Comparison with preindustrial simulations gives a global annual average radiative forcing due to tropospheric ozone increases of 0.30 W/m2 with standard assumptions for preindustrial emissions. Locally, the forcing reaches more than 0.8 W/m2 in parts of the northern subtropics during spring and summer, and is more than 0.6 W/m2 through nearly all the Northern subtropics and mid-latitudes during summer. An alternative preindustrial simulation with soil NOx emissions reduced by two-thirds and emissions of isoprene, paraffins and alkenes from vegetation increased by 50% gives a forcing of 0.33 W/m2. Given the large uncertainties in preindustrial ozone amounts, the true value may lie well outside this range.

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