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Abstract Cloud and convective parameterizations strongly influence uncertainties in equilibrium climate sensitivity. We provide a proof‐of‐concept study to constrain these parameterizations in a perturbed parameter ensemble of the atmosphere‐only version of the Goddard Institute for Space Studies Model E2.1 simulations by evaluating model biases in the present‐day runs using multiple satellite climatologies and by comparing simulated δ 18 O of precipitation (δ 18 O p ), known to be sensitive to parameterization schemes, with a global database of speleothem δ 18 O records covering the Last Glacial Maximum (LGM), mid‐Holocene (MH) and pre‐industrial (PI) periods. Relative to modern interannual variability, paleoclimate simulations show greater sensitivity to parameter changes, allowing for an evaluation of model uncertainties over a broader range of climate forcing and the identification of parts of the world that are parameter sensitive. Certain simulations reproduced absolute δ 18 O p values across all time periods, along with LGM and MH δ 18 O p anomalies relative to the PI, better than the default parameterization. No single set of parameterizations worked well in all climate states, likely due to the non‐stationarity of cloud feedbacks under varying boundary conditions. Future work that involves varying multiple parameter sets simultaneously with coupled ocean feedbacks will likely provide improved constraints on cloud and convective parameterizations. , Plain Language Summary Equilibrium climate sensitivity (ECS) is a key climate metric that quantifies the rise in global mean surface temperature in response to doubling of atmospheric CO 2 . Changes in hydroclimate, temperature extremes, and other aspects of future climate projections are closely tied to a model's ECS. For decades, ECS range has remained wide despite improvements from using multiple lines of evidence. One persistent source of this spread is related to cloud and convective processes, which occur at scales too small to be explicitly resolved, and thus require parameterizations to be represented in climate models. These parameterizations directly influence water isotopes by modulating simulated clouds and atmospheric circulation, and thus can be used to constrain model processes and identify model biases. In this work, we demonstrated that paleoclimate simulations are more parameter sensitive than the modern, highlighting the potential of past climates in discriminating cloud and convective parameterizations. Using satellite‐ and proxy‐model comparisons, we identified the top performing parameterizations which differ for each time period likely due to varying cloud feedbacks under diverse climatic forcing. Overall, our results provide a framework for fine‐tuning model representations using combined paleoclimate and satellite data, offering a unique opportunity to assess model uncertainties over a broader range of climate variability. , Key Points Paleoclimate relative to modern are more parameter sensitive, allowing for an assessment of uncertainties over a variety of climate forcing Certain simulations reproduced the δ 18 O of precipitation from paleoclimate proxies better than the default parameterization No single set of parameters works well in all climate states likely due to varying boundary conditions influencing cloud feedbacks