Nanoparticle (NP) high pressure behavior has been extensively studied over the years. In this review, we summarize recent progress on the studies of pressure induced NP phase behavior, property, and ...applications. This review starts with a brief overview of high pressure characterization techniques, coupled with synchrotron X-ray scattering, Raman, fluorescence, and absorption. Then, we survey the pressure induced phase transition of NP atomic crystal structure including size dependent phase transition, amorphization, and threshold pressures using several typical NP material systems as examples. Next, we discuss the pressure induced phase transition of NP mesoscale structures including topics on pressure induced interparticle separation distance, NP coupling, and NP coalescence. Pressure induced new properties and applications in different NP systems are highlighted. Finally, outlooks with future directions are discussed.
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IJS, KILJ, NUK, PNG, UL, UM
This article reviews the fundamentals of variational transition state theory (VTST), its recent theoretical development, and some modern applications. The theoretical methods reviewed here include ...multidimensional quantum mechanical tunneling, multistructural VTST (MS-VTST), multi-path VTST (MP-VTST), both reaction-path VTST (RP-VTST) and variable reaction coordinate VTST (VRC-VTST), system-specific quantum Rice-Ramsperger-Kassel theory (SS-QRRK) for predicting pressure-dependent rate constants, and VTST in the solid phase, liquid phase, and enzymes. We also provide some perspectives regarding the general applicability of VTST.
This article reviews the fundamentals of variational transition state theory (VTST), its recent theoretical development, and some modern applications.
Recent advances in polymer synthesis have allowed remarkable control over chain microstructure and conformation. Capitalizing on such developments, here we create well-controlled chain folding in ...sulfonated polyethylene, leading to highly uniform hydrated acid layers of subnanometre thickness with high proton conductivity. The linear polyethylene contains sulfonic acid groups pendant to precisely every twenty-first carbon atom that induce tight chain folds to form the hydrated layers, while the methylene segments crystallize. The proton conductivity is on par with Nafion 117, the benchmark for fuel cell membranes. We demonstrate that well-controlled hairpin chain folding can be utilized for proton conductivity within a crystalline polymer structure, and we project that this structure could be adapted for ion transport. This layered polyethylene-based structure is an innovative and versatile design paradigm for functional polymer membranes, opening doors to efficient and selective transport of other ions and small molecules on appropriate selection of functional groups.
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IJS, KISLJ, NUK, SBMB, UL, UM, UPUK
We extend a phase-field/gradient damage formulation for cohesive fracture to the dynamic case. The model is characterized by a regularized fracture energy that is linear in the damage field, as well ...as non-polynomial degradation functions. Two categories of degradation functions are examined, and a process to derive a given degradation function based on a local stress–strain response in the cohesive zone is presented. The resulting model is characterized by a linear elastic regime prior to the onset of damage, and controlled strain-softening thereafter. The governing equations are derived according to macro- and microforce balance theories, naturally accounting for the irreversible nature of the fracture process by introducing suitable constraints for the kinetics of the underlying microstructural changes. The model is complemented by an efficient staggered solution scheme based on an augmented Lagrangian method. Numerical examples demonstrate that the proposed model is a robust and effective method for simulating cohesive crack propagation, with particular emphasis on dynamic fracture.
•We develop a regularized model of cohesive fracture with applications to quasi-static and dynamic problems.•A new degradation function is derived and tested.•Options for enforcing irreversibility constraints are examined.•The convergence of the model with decreasing regularization length is examined.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
We experimentally demonstrate a functional silicon metadevice at telecom wavelengths that can efficiently control the wavefront of optical beams by imprinting a spatially varying transmittance phase ...independent of the polarization of the incident beam. Near-unity transmittance efficiency and close to 0–2π phase coverage are enabled by utilizing the localized electric and magnetic Mie-type resonances of low-loss silicon nanoparticles tailored to behave as electromagnetically dual-symmetric scatterers. We apply this concept to realize a metadevice that converts a Gaussian beam into a vortex beam. The required spatial distribution of transmittance phases is achieved by a variation of the lattice spacing as a single geometric control parameter.
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IJS, KILJ, NUK, PNG, UL, UM
This work documents the first version of the U.S. Department of Energy (DOE) new Energy Exascale Earth System Model (E3SMv1). We focus on the standard resolution of the fully coupled physical model ...designed to address DOE mission‐relevant water cycle questions. Its components include atmosphere and land (110‐km grid spacing), ocean and sea ice (60 km in the midlatitudes and 30 km at the equator and poles), and river transport (55 km) models. This base configuration will also serve as a foundation for additional configurations exploring higher horizontal resolution as well as augmented capabilities in the form of biogeochemistry and cryosphere configurations. The performance of E3SMv1 is evaluated by means of a standard set of Coupled Model Intercomparison Project Phase 6 (CMIP6) Diagnosis, Evaluation, and Characterization of Klima simulations consisting of a long preindustrial control, historical simulations (ensembles of fully coupled and prescribed SSTs) as well as idealized CO2 forcing simulations. The model performs well overall with biases typical of other CMIP‐class models, although the simulated Atlantic Meridional Overturning Circulation is weaker than many CMIP‐class models. While the E3SMv1 historical ensemble captures the bulk of the observed warming between preindustrial (1850) and present day, the trajectory of the warming diverges from observations in the second half of the twentieth century with a period of delayed warming followed by an excessive warming trend. Using a two‐layer energy balance model, we attribute this divergence to the model's strong aerosol‐related effective radiative forcing (ERFari+aci = −1.65 W/m2) and high equilibrium climate sensitivity (ECS = 5.3 K).
Plain Language Summary
The U.S. Department of Energy funded the development of a new state‐of‐the‐art Earth system model for research and applications relevant to its mission. The Energy Exascale Earth System Model version 1 (E3SMv1) consists of five interacting components for the global atmosphere, land surface, ocean, sea ice, and rivers. Three of these components (ocean, sea ice, and river) are new and have not been coupled into an Earth system model previously. The atmosphere and land surface components were created by extending existing components part of the Community Earth System Model, Version 1. E3SMv1's capabilities are demonstrated by performing a set of standardized simulation experiments described by the Coupled Model Intercomparison Project Phase 6 (CMIP6) Diagnosis, Evaluation, and Characterization of Klima protocol at standard horizontal spatial resolution of approximately 1° latitude and longitude. The model reproduces global and regional climate features well compared to observations. Simulated warming between 1850 and 2015 matches observations, but the model is too cold by about 0.5 °C between 1960 and 1990 and later warms at a rate greater than observed. A thermodynamic analysis of the model's response to greenhouse gas and aerosol radiative affects may explain the reasons for the discrepancy.
Key Points
This work documents E3SMv1, the first version of the U.S. DOE Energy Exascale Earth System Model
The performance of E3SMv1 is documented with a set of standard CMIP6 DECK and historical simulations comprising nearly 3,000 years
E3SMv1 has a high equilibrium climate sensitivity (5.3 K) and strong aerosol‐related effective radiative forcing (‐1.65 W/m2)
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DOBA, FZAB, GIS, IJS, IZUM, KILJ, NLZOH, NUK, OILJ, PILJ, PNG, SAZU, SBCE, SBMB, SIK, UILJ, UKNU, UL, UM, UPUK
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