2022 New's Items

Highly Tunable Magnetic Phases in Transition-Metal Dichalcogenide Fe 1 / 3 + δ NbS 2

Wu S
Xu Z
Haley SC
Weber SF
Settineri NS
Neaton JB
Analytis JG
Birgeneau RJ
2022

Layered transition-metal dichalcogenides (TMDCs) host a plethora of interesting physical phenomena ranging from charge order to superconductivity. By introducing magnetic ions into 2HTA2 (T=Nb...

Bidirectional phonon emission in two-dimensional heterostructures triggered by ultrafast charge transfer

Sood A
Haber JB
Carlström J
Peterson EA
Neaton JB
Heinz TF
Lindenberg AM
da Jornada FH
Raja A
2022

Photoinduced charge transfer in van der Waals heterostructures occurs on the 100 fs timescale despite weak interlayer coupling and momentum mismatch. However, little is understood about the microscopic mechanism behind this ultrafast process and the role of the lattice in mediating it. Here, using femtosecond electron diffraction, we directly visualize lattice dynamics in photoexcited heterostructures of WSe2/WS2 monolayers. Following the selective excitation of WSe2, we measure the concurrent heating of...

A room temperature polar magnetic metal

Zhang H
Shao YT
Chen R
Neaton JB
Fischer P
Muller D
Birgeneau R
Ramesh R
2022

The emergence of long-range magnetic order in noncentrosymmetric compounds has stimulated interest in the possibility of exotic spin transport phenomena and topologically protected spin textures for applications in next-generation spintronics. Polar magnets, with broken symmetries of spatial inversion and time reversal, usually host chiral spin textures. This work reports on a wurtzite-structure polar magnetic metal, identified as AA...

Room-temperature skyrmion lattice in a layered magnet (Fe0.5Co0.5)5GeTe2

Zhang H
Raftrey D
Chan YT
Wu W
Yao J
Fischer P
Neaton JB
Muller D
2022

Novel magnetic ground states have been stabilized in two-dimensional (2D) magnets such as skyrmions, with the potential next-generation information technology. Here, we report the experimental observation of a Néel-type skyrmion lattice at room temperature in a single-phase, layered 2D magnet, specifically a 50% Co–doped Fe5GeTe2 (FCGT) system. The thickness-dependent magnetic domain size follows Kittel’s law. The static spin textures and spin dynamics in FCGT nanoflakes were studied by Lorentz electron microscopy, variable-...

Accelerated Discovery of CH4 Uptake Capacity Metal–Organic Frameworks Using Bayesian Optimization

Taw E
Neaton JB
2022

High-throughput computational studies for discovery of metal–organic frameworks (MOFs) for separations and storage applications are often limited by the costs of computing thermodynamic quantities. Recent such studies at the time of writing may use ab initio results for a narrow selection of MOFs or empirical force-field methods for larger selections. Here, a proof-of-concept study is conducted using Bayesian optimization on CH4 uptake capacity of hypothetical MOFs for an existing dataset (Wilmer et al., Nature Chem. 2012, 4, 83)....

Metal–organic frameworks as O2-selective adsorbents for air separations

Jaramillo DE
Jaffe A
Snyder BER
Meihaus KR
Harris TD
Neaton JB
Long JR
2022

Oxygen is a critical gas in numerous industries and is produced globally on a gigatonne scale, primarily through energy-intensive cryogenic distillation of air. The realization of large-scale adsorption-based air separations could enable a significant reduction in associated worldwide energy consumption and would constitute an important component of broader efforts to combat climate change. Certain small-scale air separations are carried out using N2-selective adsorbents, although the low capacities, poor selectivities, and high regeneration...

Evaluation of the Stability of Diamine-Appended Mg2(dobpdc) Frameworks to Sulfur Dioxide

Parker ST
Smith A
Forse AC
Neaton JB
Reimer JA
Long JR
2022

Diamine-appended Mg2(dobpdc) (dobpdc4– = 4,4′-dioxidobiphenyl-3,3′-dicarboxylate) metal–organic frameworks are a promising class of CO2 adsorbents, although their stability to SO2─a trace component of industrially relevant exhaust streams─remains largely untested. Here, we investigate the impact of SO2 on the stability and CO2 capture performance of dmpn–Mg2(dobpdc) (dmpn = 2,2-dimethyl-1,3-propanediamine...

Band gaps of halide perovskites from a Wannier-localized optimally tuned screened range-separated hybrid functional

Ohad G
Wing D
Gant SE
Cohen AV
Haber JB
Sagredo F
Filip MR
Neaton JB
Kronik L
2022

The accurate prediction of the band gaps of halide perovskites within density functional theory is known to be challenging. The recently developed Wannier-localized optimally tuned screened range-separated hybrid functional was shown to be highly accurate for fundamental band gaps of standard semiconductors and insulators. This was achieved by selecting the parameters of the functional to satisfy an ansatz that generalizes the ionization potential theorem to the removal of charge from a state that corresponds to a Wannier function. Here, we present applications of the method to the...

Optimally tuned starting point for single-shot G W calculations of solids

Gant SE
Haber JB
Filip MR
Sagredo F
Wing D
Ohad G
Kronik L
Neaton JB
2022

The dependence of ab initio many-body perturbation theory within the GW approximation on the eigensystem used in calculating quasiparticle corrections limits this method's predictive power. Here, we investigate the accuracy of the recently developed Wannier-localized optimally tuned screened range-separated hybrid (WOT-SRSH) functional as a generalized Kohn-Sham starting point for single-shot G...

Zinc Titanium Nitride Semiconductor toward Durable Photoelectrochemical Applications

Greenaway AL
Ke S
Culman T
Gregoire JM
Neaton JB
Tamboli AC
Zakutayev A
2022

Photoelectrochemical fuel generation is a promising route to sustainable liquid fuels produced from water and captured carbon dioxide with sunlight as the energy input. Development of these technologies requires photoelectrode materials that are both photocatalytically active and operationally stable in harsh oxidative and/or reductive electrochemical environments. Such photocatalysts can be discovered based on co-design principles, wherein design for stability is based on the propensity for the photocatalyst to self-passivate under operating conditions and design for photoactivity...