Toward High-Voltage Cathodes for Zinc-Ion Batteries: Discovery Pipeline and Material Design Rules.

Efficient energy storage systems are crucial to address the intermittency of renewable energy sources. As multivalent batteries, Zn-ion batteries (ZIBs), while inherently low voltage, offer a promising low-cost alternative to Li-ion batteries due to the viable use of zinc as the anode. However, to maximize the potential impact of ZIBs, rechargeable cathodes with improved Zn diffusion are needed.

Correction: Atomate2: modular workflows for materials science.

[This corrects the article DOI: 10.1039/D5DD00019J.].

Atomate2: modular workflows for materials science.

High-throughput density functional theory (DFT) calculations have become a vital element of computational materials science, enabling materials screening, property database generation, and training of "universal" machine learning models. While several software frameworks have emerged to support these computational efforts, new developments such as machine learned force fields have increased demands for more flexible and programmable workflow solutions. This manuscript introduces atomate2, a comprehensive evolution of our original atomate framework, designed to address existing limitations in computational materials research infrastructure.

Accelerated data-driven materials science with the Materials Project.

The Materials Project was launched formally in 2011 to drive materials discovery forwards through high-throughput computation and open data. More than a decade later, the Materials Project has become an indispensable tool used by more than 600,000 materials researchers around the world. This Perspective describes how the Materials Project, as a data platform and a software ecosystem, has helped to shape research in data-driven materials science.

Constitutive deletion of the obscurin-Ig58/59 domains induces atrial remodeling and Ca2+-based arrhythmogenesis.

Obscurin is a giant protein that coordinates diverse aspects of striated muscle physiology. Obscurin immunoglobulin domains 58/59 (Ig58/59) associate with essential sarcomeric and Ca2+ cycling proteins. To explore the pathophysiological significance of Ig58/59, we generated the Obscn-ΔIg58/59 mouse model, expressing obscurin constitutively lacking Ig58/59.

Ryanodine receptor stabilization therapy suppresses Ca- based arrhythmias in a novel model of metabolic HFpEF.

Heart Failure with preserved ejection fraction (HFpEF) has a high rate of sudden cardiac death (SCD) and empirical treatment is ineffective. We developed a novel preclinical model of metabolic HFpEF that presents with stress-induced ventricular tachycardia (VT). Mechanistically, we discovered arrhythmogenic changes in intracellular Ca handling distinct from the changes pathognomonic for heart failure with reduced ejection fraction.

How Does HF-DFT Achieve Chemical Accuracy for Water Clusters?

Bolstered by recent calculations of exact functional-driven errors (FEs) and density-driven errors (DEs) of semilocal density functionals in the water dimer binding energy [Kanungo, B. 2024, 15, 323-328], we investigate approximate FEs and DEs in neutral water clusters containing up to 20 monomers, charged water clusters, and alkali- and halide-water clusters. Our proxy for the exact density is rSCAN 50, a 50% global hybrid of exact exchange with rSCAN, which may be less correct than rSCAN for the compact water monomer but importantly more correct for long-range electron transfers in the noncompact water clusters.

Symmetry breaking and self-interaction correction in the chromium atom and dimer.

Density functional approximations to the exchange-correlation energy can often identify strongly correlated systems and estimate their energetics through energy-minimizing symmetry-breaking. In particular, the binding energy curve of the strongly correlated chromium dimer is described qualitatively by the local spin density approximation (LSDA) and almost quantitatively by the Perdew-Burke-Ernzerhof generalized gradient approximation (PBE-GGA), where the symmetry breaking is antiferromagnetic for both. Here, we show that a full Perdew-Zunger self-interaction-correction (SIC) to LSDA seems to go too far by creating an unphysical symmetry-broken state, with effectively zero magnetic moment but non-zero spin density on each atom, which lies ∼4 eV below the antiferromagnetic solution.

: predicting activation barriers through a chemically-interpretable, equivariant and physically constrained graph neural network.

Activation barriers of elementary reactions are essential to predict molecular reaction mechanisms and kinetics. However, computing these energy barriers by identifying transition states with electronic structure methods (, density functional theory) can be time-consuming and computationally expensive. In this work, we introduce , an equivariant graph neural network that predicts activation barriers using coefficients of any frontier molecular orbital (such as the highest occupied molecular orbital) of reactant and product complexes as graph node features.

Unconventional Error Cancellation Explains the Success of Hartree-Fock Density Functional Theory for Barrier Heights.

Energy barriers, which control the rates of chemical reactions, are seriously underestimated by computationally efficient semilocal approximations for the exchange-correlation energy. The accuracy of a semilocal density functional approximation is strongly boosted for reaction barrier heights by evaluating that approximation non-self-consistently on Hartree-Fock electron densities, which has been known for ∼30 years. The conventional explanation is that the Hartree-Fock theory yields the more accurate density.

Revealing quasi-excitations in the low-density homogeneous electron gas with model exchange-correlation kernels.

Time-dependent density functional theory within the linear response regime provides a solid mathematical framework to capture excitations. The accuracy of the theory, however, largely depends on the approximations for the exchange-correlation (xc) kernels. Away from the long-wavelength (or q = 0 short wave-vector) and zero-frequency (ω = 0) limit, the correlation contribution to the kernel becomes more relevant and dominant over exchange.

Ryanodine Receptor Stabilization Therapy Suppresses Ca -Based Arrhythmias in a Novel Model of Metabolic HFpEF.

Heart Failure with preserved ejection fraction (HFpEF) is the most prevalent form of heart failure worldwide and its significant mortality is associated with a high rate of sudden cardiac death (SCD; 30% - 40%). Chronic metabolic stress is an important driver of HFpEF, and clinical data show metabolic stress as a significant risk factor for ventricular arrhythmias in HFpEF patients. The mechanisms of SCD and ventricular arrhythmia in HFpEF remain critically understudied and empirical treatment is ineffective.

Calcium and bicarbonate signaling pathways have pivotal, resonating roles in matching ATP production to demand.

Mitochondrial ATP production in ventricular cardiomyocytes must be continually adjusted to rapidly replenish the ATP consumed by the working heart. Two systems are known to be critical in this regulation: mitochondrial matrix Ca ([Ca]) and blood flow that is tuned by local cardiomyocyte metabolic signaling. However, these two regulatory systems do not fully account for the physiological range of ATP consumption observed.

The Predictive Power of Exact Constraints and Appropriate Norms in Density Functional Theory.

Ground-state Kohn-Sham density functional theory provides, in principle, the exact ground-state energy and electronic spin densities of real interacting electrons in a static external potential. In practice, the exact density functional for the exchange-correlation (xc) energy must be approximated in a computationally efficient way. About 20 mathematical properties of the exact xc functional are known.

Understanding Density-Driven Errors for Reaction Barrier Heights.

Delocalization errors, such as charge-transfer and some self-interaction errors, plague computationally efficient and otherwise accurate density functional approximations (DFAs). Evaluating a semilocal DFA non-self-consistently on the Hartree-Fock (HF) density is often recommended as a computationally inexpensive remedy for delocalization errors. For sophisticated meta-GGAs like SCAN, this approach can achieve remarkable accuracy.

Symmetry Breaking with the SCAN Density Functional Describes Strong Correlation in the Singlet Carbon Dimer.

The SCAN (strongly constrained and appropriately normed) meta-generalized gradient approximation (meta-GGA), which satisfies all 17 exact constraints that a meta-GGA can satisfy, accurately describes equilibrium bonds that are normally correlated. With symmetry breaking, it also accurately describes some sd equilibrium bonds that are strongly correlated. While sp equilibrium bonds are nearly always normally correlated, the C singlet ground state is known from correlated wave function theory to be a rare case of strong correlation in an sp equilibrium bond.

Testing the rSCAN Density Functional for the Thermodynamic Stability of Solids with and without a van der Waals Correction.

A central aim of materials discovery is an accurate and numerically reliable description of thermodynamic properties, such as the enthalpies of formation and decomposition. The rSCAN revision of the strongly constrained and appropriately normed (SCAN) meta-generalized gradient approximation (meta-GGA) balances numerical stability with high general accuracy. To assess the rSCAN description of solid-state thermodynamics, we evaluate the formation and decomposition enthalpies, equilibrium volumes, and fundamental band gaps of more than 1000 solids using rSCAN, SCAN, and PBE, as well as two dispersion-corrected variants, SCAN+rVV10 and rSCAN+rVV10.

Construction of meta-GGA functionals through restoration of exact constraint adherence to regularized SCAN functionals.

The strongly constrained and appropriately normed (SCAN) meta-GGA exchange-correlation functional [Sun et al., Phys. Rev.

Calcium Signaling Silencing in Atrial Fibrillation: Implications for Atrial Sodium Homeostasis.

Atrial fibrillation (AF) is the most common type of cardiac arrhythmia, affecting more than 33 million people worldwide. Despite important advances in therapy, AF's incidence remains high, and treatment often results in recurrence of the arrhythmia. A better understanding of the cellular and molecular changes that (1) trigger AF and (2) occur after the onset of AF will help to identify novel therapeutic targets.

rSCAN-D4: Dispersion corrected meta-generalized gradient approximation for general chemical applications.

We combine a regularized variant of the strongly constrained and appropriately normed semilocal density functional [J. Sun, A. Ruzsinszky, and J.

Interpretations of ground-state symmetry breaking and strong correlation in wavefunction and density functional theories.

Strong correlations within a symmetry-unbroken ground-state wavefunction can show up in approximate density functional theory as symmetry-broken spin densities or total densities, which are sometimes observable. They can arise from soft modes of fluctuations (sometimes collective excitations) such as spin-density or charge-density waves at nonzero wavevector. In this sense, an approximate density functional for exchange and correlation that breaks symmetry can be more revealing (albeit less accurate) than an exact functional that does not.

Accurate and Numerically Efficient rSCAN Meta-Generalized Gradient Approximation.

The recently proposed rSCAN functional [ 2019 150, 161101] is a regularized form of the SCAN functional [ 2015 115, 036402] that improves SCAN's numerical performance at the expense of breaking constraints known from the exact exchange-correlation functional. We construct a new meta-generalized gradient approximation by restoring exact constraint adherence to rSCAN. The resulting functional maintains rSCAN's numerical performance while restoring the transferable accuracy of SCAN.

Simple hydrogenic estimates for the exchange and correlation energies of atoms and atomic ions, with implications for density functional theory.

Exact density functionals for the exchange and correlation energies are approximated in practical calculations for the ground-state electronic structure of a many-electron system. An important exact constraint for the construction of approximations is to recover the correct non-relativistic large-Z expansions for the corresponding energies of neutral atoms with atomic number Z and electron number N = Z, which are correct to the leading order (-0.221Z and -0.

Identification of an I-dependent and I-mediated proarrhythmic mechanism in cardiomyocytes derived from pluripotent stem cells of a Brugada syndrome patient.

Brugada syndrome (BrS) is an inherited cardiac arrhythmia commonly associated with SCN5A mutations, yet its ionic mechanisms remain unclear due to a lack of cellular models. Here, we used human induced pluripotent stem cell-derived cardiomyocytes (hiPSC-CMs) from a BrS patient (BrS1) to evaluate the roles of Na currents (I) and transient outward K currents (I) in BrS induced action potential (AP) changes. To understand the role of these current changes in repolarization we employed dynamic clamp to "electronically express" I and restore normal resting membrane potentials and allow normal recovery of the inactivating currents, I, I and I.