the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Chemistry-climate feedback of atmospheric methane in a methane emission flux driven chemistry-climate model
Abstract. The chemical sink of atmospheric methane (CH4) depends on the temperature and on the chemical composition. Here, we assess the feedback of atmospheric CH4 induced by changes of the chemical sink in a warming climate using a CH4 emission flux driven setup of the chemistry-climate model EMAC, in which the chemical feedback of CH4 mixing ratios can evolve explicitly. We perform idealized perturbation simulations driven either by increased carbon dioxide (CO2) mixing ratios, or by increased CH4 emission fluxes. The CH4 emission flux perturbation leads to a large increase of CH4 mixing ratios. Remarkably, the factor by which the CH4 mixing ratio increases is larger than the increase factor of the emission flux, because the atmospheric lifetime of CH4 is extended.
In contrast, the individual effect of the global surface air temperature (GSAT) increase is to shorten the CH4 lifetime, which results in a significant reduction of CH4 mixing ratios in our setup. The corresponding radiative feedback is estimated at -0.041 W/m2/K and -0.089 W/m2/K for the CO2 and CH4 perturbation, respectively. The explicit adaption of CH4 mixing ratios leads to secondary feedbacks of the hydroxyl radical (OH) and ozone (O3). Firstly, the OH response includes the CH4-OH feedback, which enhances the CH4 lifetime change, and, secondly, the formation of tropospheric O3 is reduced. Our CH4 perturbation induces the same response of GSAT per effective radiative forcing (ERF) as the CO2 perturbation, which supports the applicability of the ERF framework for CH4.
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CC1: 'Comment on egusphere-2024-2938', Zosia Staniaszek, 02 Oct 2024
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Thanks for a really interesting read and an important step in developing more models with methane emissions. The section on tagging the ozone response is particularly novel in a methane emissions driven system and really illustrates the wide ranging impact of changes in methane (that are often excluded by using a lower boundary condition).
The increase in mixing ratio above the level of increase in emissions is as expected due to the chemical feedbacks in the system and the lengthening of methane lifetime, albeit here the feedback factor is higher than most models (1.73 as a crude estimate using delta conc/delta emissions (Holmes et al 2018)). I would be interested in whether you could calculate a feedback factor for EMAC using these simulations. Also, a note that more recent feedback factors than those quoted here can be found in Sand et al 2023 Supplementary Table 2 (https://www.nature.com/articles/s43247-023-00857-8).
I would also be interested in the timescale of the change in methane mixing ratio, and the perturbation lifetime. In the methods section you mention a long spin up time. In UKESM-ems we found that with a large methane emissions decrease you get a much faster than expected change in mixing ratio due to the rapid increase in OH and decrease in methane lifetime, and I would expect the opposite effect in an increase such as done here.
Best wishes,
Zosia StaniaszekCitation: https://doi.org/10.5194/egusphere-2024-2938-CC1 -
RC1: 'Comment on egusphere-2024-2938', Anonymous Referee #1, 05 Nov 2024
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Stecher et al. (2024) assess the methane feedback on chemistry and climate by conducting chemistry-climate model simulations driven by the methane emissions. As the second most important greenhouse gas after CO2, it is critical to understand the methane cycle from the climate impact and mitigation perspectives. Several sets of model simulations are performed to assess the radiative and chemistry feedback in this work. The results show larger sensitivity of the methane lifetime towards climate change compared to previous studies. The impacts on O3 chemistry are also discussed thoroughly in a tagging approach. The manuscript is well written and organized. I recommend accepting the manuscript after minor revision.
General comments:
Ocean model coupling
A mixed layer ocean model is coupled in the REF-SSTvar simulations. How representative are the SSTs in these runs compared to the prescribed SSTs? This would have impacts on air-sea interactions and thus affecting atmospheric chemistry and composition in addition to the GSAT. The biases in reference cases may propagate into the perturbed cases, which would affect your assessment in the climate response. Do you think the biases could be canceled out between the reference run and perturbed run?Methane radiative feedback
The simulations between reference cases and perturbed cases suggest larger sensitivity of the methane lifetime towards climate change compared to previous studies and the authors attribute such difference to the different methane representations in the models, e.g., emission driven vs prescribed lower boundaries. But the authors also point out in the manuscript, the model-specific parameterizations, mechanisms, etc would lead to the model-dependent results. For example, using different radiative transfer models give very different radiative feedback as shown in the manuscript. How to better quantify the sensitivity to different model setup or model schemes? How to improve the model confidence in assessing methane radiative feedback?
Ozone
There are a lot of discussions in the manuscript on the impacts on tropospheric and stratospheric ozone. What about impacts on surface O3, which is more relevant to the health effects.Specific comments:
Page 9, Section 3.1, line 265-267, How sensitive of OH levels to lightning NOx? Do changes in lightning NOx play a role here?
Page 13, line 375-380: How do you treat N2O in the model? Does your model read N2O emissions or prescribe N2O at lower boundaries?
Figure S2 shows the difference in the specific humidity. Is specific humidity in your model also affected by chemistry? In other words, is water vapor a prognostic chemical tracer explicitly involved in the chemical reactions?
Citation: https://doi.org/10.5194/egusphere-2024-2938-RC1
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