2023 New's Items

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...

Quasiparticle and Optical Properties of Carrier-Doped Monolayer MoTe2 from First Principles

Champagne A
Neaton JB
2023

The intrinsic weak and highly nonlocal dielectric screening of two-dimensional materials is well-known to lead to high sensitivity of their optoelectronic properties to environment. Less studied theoretically is the role of free carriers in those properties. Here, we use ab initio GW and Bethe-Salpeter equation calculations, with a rigorous treatment of dynamical screening and local-field effects, to study the doping dependence of the quasiparticle and optical properties of a monolayer transition-metal dichalcogenide, 2H MoTe2. We predict a quasiparticle...

Cooperative Carbon Dioxide Capture in Diamine-Appended Magnesium–Olsalazine Frameworks

Zhu Z
Long JR
Neaton JB
2023

Diamine-appended Mg2(dobpdc) (dobpdc4– = 4,4′-dioxidobiphenyl-3,3′-dicarboxylate) metal–organic frameworks have emerged as promising candidates for carbon capture owing to their exceptional CO2 selectivities, high separation capacities, and step-shaped adsorption profiles, which arise from a unique cooperative adsorption mechanism resulting in the formation of ammonium carbamate chains. Materials appended with primary,secondary-diamines featuring bulky substituents, in particular, exhibit excellent stabilities and CO2 adsorption...

Carbon Capture Phenomena in Metal-Organic Frameworks with Neural Network Potentials

Shaidu Y
Neaton JB
2023

Diamine-appended metal-organic frameworks are ultraporous materials exhibiting selective and cooperative CO2 adsorption mechanisms, leading to chemically tunable step-shaped isotherms and isobars that enable a large fraction of their full CO2 capacity to be captured or released with a modest change in...