12 research outputs found

    Process-resolving Regional Arctic System Model for Advanced Modeling and Prediction of Arctic Climate System

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    15th Conference on Polar Meteorology and OceanographyThe Regional Arctic System Model (RASM) is a fully coupled limited-domain ice-ocean-atmosphere-land hydrology model. Its domain is pan-Arctic, with the atmosphere and land components configured on a 50-km or 25-km grid. The ocean and sea ice components are configured on rotated sphere meshes with four configuration options: 1/12o (~9.3km) or 1/48o (~2.4km) in the horizontal space and with 45 or 60 vertical layers. As a regional climate model, RASM requires boundary conditions along its lateral boundaries and in the upper atmosphere, which are derived either from global atmospheric reanalyses for simulations of the past to present or from Earth System models (ESMs) for climate projections. In the former case, this allow comparison of RASM results with observations in place and time, which is a unique capability not available in global ESMs. RASM has been developed and used to investigate critical processes controlling the evolution of the Arctic climate system under a diminishing sea ice cover. Several examples of key physical processes and coupling between different model components will be presented, that improve the representation of the past and present Arctic climate system. The impact of such processes and feedbacks will be discussed with regard to improving model physics and reducing biases in the representation of its initial state for prediction of Arctic climate at time scales from synoptic to intra-annual

    High-Resolution Modeling of Arctic Climate Using the Regional Arctic System Model for Dynamical Downscaling of Global Climate Model Reanalyses and Projections

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    The article of record as published may be found at https://agu.confex.com/agu/osm20/meetingapp.cgi/Paper/641925Ocean Sciences Meeting 2020The Arctic is one of the most challenging regions to model climate change due to its complexity, including the cryosphere, small scale processes and feedbacks controlling its amplified response to global climate change. The combination of these factors defines the need for high spatial and temporal model resolution, which is commonly not practical for most state-of-the-art global Earth system models (ESMs), including those participating in the Coupled Model Intercomparison Project Phase 6. We offer an alternative approach to improve model physics and reduce uncertainties in modeling Arctic climate using a high resolution regional climate system model for dynamical downscaling of output from ESMs. The Regional Arctic System Model (RASM) has been developed to better understand the past and present operation of the Arctic climate system and to predict its change at time scales up to decades. RASM is a coupled model, consisting of the atmosphere, ocean, sea ice, land hydrology and river routing scheme components. Its domain is pan-Arctic, with 50-km or 25-km grids for the atmosphere and land components. The ocean and sea ice components are configured at ~9.3-km or ~2.4-km grids horizontally and with 45 or 60 vertical layers. For hindcast simulations, RASM derives boundary conditions from global atmospheric reanalyses, allowing comparison with observations in place and time, which is a unique capability not available with ESMs. We will discuss improvements to RASM model physics offered by high resolution and in generation of internally consistent realistic initial conditions for Arctic climate prediction. We will also discuss the need for fine-tuning of scale aware parameterizations of sub-grid physical processes in varying model configurations. Finally, selected results will be presented to demonstrate gains of dynamical downscaling in comparison with observations and with the global reanalysis and predictions

    Cryo-annealing of Photoreduced CdS Quantum Dot–Nitrogenase MoFe Protein Complexes Reveals the Kinetic Stability of the E<sub>4</sub>(2N2H) Intermediate

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    A critical step in the mechanism of N2 reduction to 2NH3 catalyzed by the enzyme nitrogenase is the reaction of the four-electron/four-proton reduced intermediate state of the active-site FeMo-cofactor (E4(4H)). This state is a junction in the catalytic mechanism, either relaxing by the reaction of a metal bound Fe-hydride with a proton forming H2 or going forward with N2 binding coupled to the reductive elimination (re) of two Fe-hydrides as H2 to form the E4(2N2H) state. E4(2N2H) can relax to E4(4H) by the oxidative addition (oa) of H2 and release of N2 or can be further reduced in a series of catalytic steps to release 2NH3. If the H2 re/oa mechanism is correct, it requires that oa of H2 be associative with E4(2N2H). In this report, we have taken advantage of CdS quantum dots in complex with MoFe protein to achieve photodriven electron delivery in the frozen state, with cryo-annealing in the dark, to reveal details of the E-state species and to test the stability of E4(2N2H). Illumination of frozen CdS:MoFe protein complexes led to formation of a population of reduced intermediates. Electron paramagnetic resonance spectroscopy identified E-state signals including E2 and E4(2N2H), as well as signals suggesting the formation of E6 or E8. It is shown that in the frozen state when pN2 is much greater than pH2, the E4(2N2H) state is kinetically stable, with very limited forward or reverse reaction rates. These results establish that the oa of H2 to the E4(2N2H) state follows an associative reaction mechanism
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