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  1. Liu, Zhiwen ; Psaltis, Demetri ; Shi, Kebin (Ed.)
  2. Liu, Zhiwen ; Psaltis, Demetri ; Shi, Kebin (Ed.)
  3. We present broadband full-stokes spectropolarimetry using a chiral metasurface, which can retrieve spatially distributed wavelength information and full-stokes polarization states in a single shot. 
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  4. Strong electron correlation plays an important role in transition-metal and heavy-metal chemistry, magnetic molecules, bond breaking, biradicals, excited states, and many functional materials, but it provides a significant challenge for modern electronic structure theory. The treatment of strongly correlated systems usually requires a multireference method to adequately describe spin densities and near-degeneracy correlation. However, quantitative computation of dynamic correlation with multireference wave functions is often difficult or impractical. Multiconfiguration pair-density functional theory (MC-PDFT) provides a way to blend multiconfiguration wave function theory and density functional theory to quantitatively treat both near-degeneracy correlation and dynamic correlation in strongly correlated systems; it is more affordable than multireference perturbation theory, multireference configuration interaction, or multireference coupled cluster theory and more accurate for many properties than Kohn–Sham density functional theory. This perspective article provides a brief introduction to strongly correlated systems and previously reviewed progress on MC-PDFT followed by a discussion of several recent developments and applications of MC-PDFT and related methods, including localized-active-space MC-PDFT, generalized active-space MC-PDFT, density-matrix-renormalization-group MC-PDFT, hybrid MC-PDFT, multistate MC-PDFT, spin–orbit coupling, analytic gradients, and dipole moments. We also review the more recently introduced multiconfiguration nonclassical-energy functional theory (MC-NEFT), which is like MC-PDFT but allows for other ingredients in the nonclassical-energy functional. We discuss two new kinds of MC-NEFT methods, namely multiconfiguration density coherence functional theory and machine-learned functionals. 
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  5. Abstract

    The atmospheric Green's function method is a technique for modeling the response of the atmosphere to changes in the spatial field of surface temperature. While early studies applied this method to changes in atmospheric circulation, it has also become an important tool to understand changes in radiative feedbacks due to evolving patterns of warming, a phenomenon called the “pattern effect.” To better study this method, this paper presents a protocol for creating atmospheric Green's functions to serve as the basis for a model intercomparison project, GFMIP. The protocol has been developed using a series of sensitivity tests performed with the HadAM3 atmosphere‐only general circulation model, along with existing and new simulations from other models. Our preliminary results have uncovered nonlinearities in the response of the atmosphere to surface temperature changes, including an asymmetrical response to warming versus cooling patch perturbations, and a change in the dependence of the response on the magnitude and size of the patches. These nonlinearities suggest that the pattern effect may depend on the heterogeneity of warming as well as its location. These experiments have also revealed tradeoffs in experimental design between patch size, perturbation strength, and the length of control and patch simulations. The protocol chosen on the basis of these experiments balances scientific utility with the simulation time and setup required by the Green's function approach. Running these simulations will further our understanding of many aspects of atmospheric response, from the pattern effect and radiative feedbacks to changes in circulation, cloudiness, and precipitation.

     
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    Abstract Radiative feedbacks depend on the spatial patterns of sea surface temperature (SST) and thus can change over time as SST patterns evolve—the so-called pattern effect. This study investigates intermodel differences in the magnitude of the pattern effect and how these differences contribute to the spread in effective equilibrium climate sensitivity (ECS) within CMIP5 and CMIP6 models. Effective ECS in CMIP5 estimated from 150-yr-long abrupt4×CO2 simulations is on average 10% higher than that estimated from the early portion (first 50 years) of those simulations, which serves as an analog for historical warming; this difference is reduced to 7% on average in CMIP6. The (negative) net radiative feedback weakens over the course of the abrupt4×CO2 simulations in the vast majority of CMIP5 and CMIP6 models, but this weakening is less dramatic on average in CMIP6. For both ensembles, the total variance in the effective ECS is found to be dominated by the spread in radiative response on fast time scales, rather than the spread in feedback changes. Using Green’s functions derived from two AGCMs shows that the spread in feedbacks on fast time scales may be primarily due to differences in atmospheric model physics, whereas the spread in feedback evolution is primarily governed by differences in SST patterns. Intermodel spread in feedback evolution is well explained by differences in the relative warming in the west Pacific warm-pool regions for the CMIP5 models, but this relation fails to explain differences across the CMIP6 models, suggesting that a stronger sensitivity of extratropical clouds to surface warming may also contribute to feedback changes in CMIP6. 
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  8. The strong couplings between electronic states in conical intersection regions are among the most challenging problems in quantum chemistry. XMS-CASPT2, a second-order multireference quasidegenerate perturbation theory, has been successful in describing potential energy surfaces near the conical intersections. We have recently proposed a less expensive method for this problem, namely state-interaction pair-density functional theory (SI-PDFT), which considers the coupling between electronic states described by multiconfiguration pair-density functional theory (MC-PDFT). Here we test the accuracy of SI-PDFT for closely coupled potential energy surfaces of methylamine along five different reaction paths for N–H bond fission. We choose paths that pass close to a conical intersection of the ground and first excited states. We find that SI-PDFT predicts potential energy curves and energy splittings near the locally avoided crossing in close proximity to those obtained by XMS-CASPT2. This validates the method for application to photochemical simulations. 
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