2023 New's Items

Enabling selective zinc-ion intercalation by a eutectic electrolyte for practical anodeless zinc batteries

Li C
Nazar LF
Persson KA
2023

Two major challenges hinder the advance of aqueous zinc metal batteries for sustainable stationary storage: (1) achieving predominant Zn-ion (de)intercalation at the oxide cathode by suppressing adventitious proton co-intercalation and dissolution, and (2) simultaneously overcoming Zn dendrite growth at the anode that triggers parasitic electrolyte reactions. Here, we reveal the competition between Zn2+vs proton intercalation chemistry of a typical oxide cathode using ex-situ/operando techniques, and alleviate side reactions by developing a cost...

Assessing the Accuracy of Density Functional Approximations for Predicting Hydrolysis Reaction Kinetics

Epstein AR
Persson KA
2023

Hydrolysis reactions are ubiquitous in biological, environmental, and industrial chemistry. Density functional theory (DFT) is commonly employed to study the kinetics and reaction mechanisms of hydrolysis processes. Here, we present a new data set, Barrier Heights for HydrOlysis - 36 (BH2O-36), to enable the design of density functional approximations (DFAs) and the rational selection of DFAs for applications in aqueous chemistry. BH2O-36 consists of 36 diverse organic and inorganic forward and reverse hydrolysis reactions with reference energy barriers ΔE‡...

Variable Amine Spacing Determines Depolymerization Rate in Polydiketoenamines

Epstein AR
Persson KA
2023

The design of circular polymers has emerged as a necessity due to the lack of efficient recycling methods for many commodity plastics, particularly those used in durable products. Among the promising circular polymers, polydiketoenamines (PDKs) stand out for their ability to undergo highly selective depolymerization in strong acid, allowing monomers to be recovered from additives and fillers. Varying the triketone monomer in PDK variants is known to strongly affect the depolymerization rate; however, it remains unclear how the chemistry of the cross-linker, far from the reaction...

COVIDScholar: An automated COVID-19 research aggregation and analysis platform

Dagdelen J
Persson KA
2023

The ongoing COVID-19 pandemic produced far-reaching effects throughout society, and science is no exception. The scale, speed, and breadth of the scientific community’s COVID-19 response lead to the emergence of new research at the remarkable rate of more than 250 papers published per day. This posed a challenge for the scientific community as traditional methods of engagement with the literature were strained by the volume of new research being produced. Meanwhile, the urgency of response lead to an increasingly prominent role for preprint servers and a diffusion of relevant...

SolvationAnalysis: A Python toolkit for understanding liquid solvation structure in classical molecular dynamics simulations

Cohen OA
Persson KA
2023

The macroscopic behavior of matter is determined by the microscopic arrangement of atoms, but this arrangement is often difficult or impossible to observe experimentally. Instead, researchers use simulation techniques like molecular dynamics to probe the microscopic structure and dynamics of everything from proteins to battery electrolytes. SolvationAnalysis extracts solvation information from completed molecular dynamics simulations, letting researchers access key solvation structure statistics with minimal effort and accelerating scientific research.

Mitigating the High-Charge Detrimental Phase Transformation in LiNiO2 Using Doping Engineering

Cheng J
Persson KA
2023

Cobalt-free layered LiNiO2 has gained increased interest due to the scarcity and high cost of cobalt. However, LiNiO2 suffers from poor cycling stability, which is mainly due to oxygen loss and structural instability, especially when operating at high voltages. Herein, we present a doping strategy to mitigate the detrimental O3-to-O1 phase transformation in LiNiO2 from first-principles calculations. Temperature–composition phase diagrams of pristine and doped Li1–xNiO2...

Zircon Structure as a Prototype Host for Fast Monovalent and Divalent Ionic Conduction

Chen Q
Persson KA
2023

“Beyond Li-ion” energy storage solutions based on ions such as Na, Mg, Ca, and Zn have attracted increasing attention due to growing concerns about the cost, resource availability, and safety of the currently dominant Li-ion batteries. One of the greatest challenges for beyond-Li systems, especially multivalent ones, is the lack of materials with high ionic mobility. In this study, we find that zircon-type YPO4 presents a unique structural environment that enables superior conduction of multiple species including Na+, Ca...

High-throughput calculations of charged point defect properties with semi-local density functional theory—performance benchmarks for materials screening applications

Broberg D
Persson KA
2023

Calculations of point defect energetics with Density Functional Theory (DFT) can provide valuable insight into several optoelectronic, thermodynamic, and kinetic properties. These calculations commonly use methods ranging from semi-local functionals with a-posteriori corrections to more computationally intensive hybrid functional approaches. For applications of DFT-based high-throughput computation for data-driven materials discovery, point defect properties are of interest, yet are currently excluded from available materials databases. This work presents a benchmark...

Phonon-Induced Localization of Excitons in Molecular Crystals from First Principles

Alvertis AM
Neaton JB
2023

The spatial extent of excitons in molecular systems underpins their photophysics and utility for optoelectronic applications. Phonons are reported to lead to both exciton localization and delocalization. However, a microscopic understanding of phonon-induced (de)localization is lacking, in particular, how localized states form, the role of specific vibrations, and the relative importance of quantum and thermal nuclear fluctuations. Here, we present a first-principles study of these phenomena in solid pentacene, a prototypical molecular crystal, capturing the formation of bound...

Exciton Lifetime and Optical Line Width Profile via Exciton–Phonon Interactions: Theory and First-Principles Calculations for Monolayer MoS2

Chan YH
Louie SG
Neaton JB
2023

Exciton dynamics dictates the evolution of photoexcited carriers in photovoltaic and optoelectronic devices. However, interpreting their experimental signatures is a challenging theoretical problem due to the presence of both electron–phonon and many-electron interactions. We develop and apply here a first-principles approach to exciton dynamics resulting from exciton–phonon coupling in monolayer MoS2 and reveal the highly selective nature of exciton–phonon coupling due to the internal spin structure of excitons, which leads to a surprisingly long lifetime...