2023 New's Items

Predictive stochastic analysis of massive filter-based electrochemical reaction networks

Barter D
Redkar NS
Persson KA
2024

Chemical reaction networks (CRNs) are powerful tools for obtaining insight into complex reactive processes. However, they are difficult to employ in domains such as electrochemistry where reaction mechanisms and outcomes are not well understood. To overcome these limitations, we report new methods to assist in CRN construction and analysis. Beginning with a known set of potentially relevant species, we enumerate and then filter all stoichiometrically valid reactions, constructing CRNs without reaction templates. By applying efficient stochastic algorithms, we can then interrogate...

Continuum-level modeling of Li-ion battery SEI by upscaling atomistically informed reaction mechanisms

Weddle PJ
Colclasure AM
Persson KA
2023

Understanding and controlling solid-electrolyte interphase (SEI) formation to stabilize cell performance is a significant challenge for next-generation Li-ion battery technologies. In recent years, computational modeling has become an essential tool in providing fundamental insights into SEI properties and dynamics. However, neither atomistic nor continuum-level approaches alone can capture the complexities of SEI ...

Enabling automated high-throughput Density Functional Theory studies of amorphous material surface reactions

Siron M
Persson KA
2023

Amorphous materials are increasingly considered for electronic and energy applications. However, modeling site-specific processes on amorphous materials is prohibitively expensive due to the large...

Rational Design of Fluorinated Electrolytes for Low Temperature Lithium-Ion Batteries

Yoo DJ
Zhang Z
Persson KA
2023

Nonaqueous carbonate electrolytes are commonly used in commercial lithium-ion battery (LIB). However, the sluggish Li+ diffusivity and high interfacial charge transfer resistance at low temperature (LT) limit their wide adoption among geographical areas with high latitudes and altitudes. Herein, a rational design of new electrolytes is demonstrated, which can significantly improve the low temperature performance below −20 °C. This electrolyte is achieved by tailoring the chemical structure, i.e., altering the fluorination position and the degree of...

Tin Metal Improves the Lithiation Kinetics of High-Capacity Silicon Anodes

Yao K
Tong W
Persson KA
2023

Si-based anodes present a great promise for high energy density lithium-ion batteries. However, its commercialization is largely hindered by a grand challenge of a rapid capacity fade. Here, we demonstrate excellent cycling stability on a Si–Sn thin film electrode that outperforms pure Si or Sn counterpart under the similar conditions. Combined with the first-principles calculations, in situ transmission electron microscopy studies reveal a reduced volume expansion, increased conductivity, as well as dynamic rearrangement upon lithiation of the Si–Sn film. We attribute the improved...

Spatially resolved structural order in low-temperature liquid electrolyte

Xie Y
Zheng H
Persson KA
2023

Determining the degree and the spatial extent of structural order in liquids is a grand challenge. Here, we are able to resolve the structural order in a model organic electrolyte of 1 M lithium hexafluorophosphate (LiPF6) dissolved in 1:1 (v/v) ethylene carbonate:diethylcarbonate by developing an integrated method of liquid-phase transmission electron microscopy (TEM), cryo-TEM operated at −30°C, four-dimensional scanning TEM, and data analysis based on deep learning. This study reveals the presence of short-range order (SRO) in the high–salt concentration...

Designing transparent conductors using forbidden optical transitions

Woods-Robinson R
Persson KA
2023

Many semiconductors present weak or forbidden transitions at their fundamental band gaps, inducing a widened region of transparency. This occurs in high-performing n-type transparent conductors (TCs) such as Sn-doped In2O3In2O3 (ITO); however, thus far, the presence of forbidden transitions has been neglected in the search for...

Stability and synthesis across barium tin sulfide material space

Woods-Robinson R
Zakutayev A
Persson KA
2023

Barium tin sulfide (Ba–Sn–S) is a ternary phase space with interesting material candidates for optoelectronic and thermoelectric applications, yet its properties have not been explored in-depth experimentally, and no thin films have been synthesized. This study uses combinatorial sputtering and theoretical calculations to survey the phase space of Ba–Sn–S materials. We experimentally find that at deposition temperatures up to 600 °C, phases of rocksalt-derived BaS structures (Fm...

A method to computationally screen for tunable properties of crystalline alloys

Woods-Robinson R
Persson KA
2023

Conventionally, high-throughput computational materials searches start from an input set of bulk compounds extracted from material databases, but, in contrast, many real functional materials are heavily engineered mixtures of compounds rather than single bulk compounds. We present a framework and open-source code to automatically construct and analyze possible alloys and solid solutions from a set of existing experimental or calculated ordered compounds, without requiring additional metadata except crystal structure. As a demonstration, we apply this framework to all compounds in the...

Chemical reaction networks and opportunities for machine learning

Wen M
Persson KA
2023

Chemical reaction networks (CRNs), defined by sets of species and possible reactions between them, are widely used to interrogate chemical systems. To capture increasingly complex phenomena, CRNs can be leveraged alongside data-driven methods and machine learning (ML). In this Perspective, we assess the diverse strategies available for CRN construction and analysis in pursuit of a wide range of scientific goals, discuss ML techniques currently being applied to CRNs and outline future CRN-ML approaches, presenting scientific and technical challenges to overcome.