Gerbrand Ceder's research while affiliated with Lawrence Berkeley National Laboratory and other places

Publications (234)

Article
Li‐rich rocksalt oxides are promising cathode materials for lithium‐ion batteries due to their large capacity and energy density, and their ability to use earth‐abundant elements. The excess Li in the rocksalt, needed to achieve good Li transport, reduces the theoretical transition metal redox capacity and introduces a labile oxygen state, both of...
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The cluster expansion (CE) method has seen continuous and increasing use in the study of configuration-dependent properties of crystalline materials. The original development of the CE method along with the underlying mathematical formalism and assumptions was focused on the study of metallic alloys. Since then the methodology has been actively and...
Preprint
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Monte-Carlo sampling of lattice model Hamiltonians is a well-established technique in statistical mechanics for studying the configurational entropy of crystalline materials. When species to be distributed on the lattice model carry charge, the charge balance constraint on the overall system prohibits single-site Metropolis exchanges in MC. In this...
Article
Superionic conductors are key to the development of safe and high-energy-density, all-solid-state batteries. Using a combined theoretical and experimental approach, we explore the feasibility of increasing the ionic conductivity through pseudohalogen substitution in the Li argyrodite structure. Under the guidance of calculated thermodynamic stabili...
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There currently exist no quantitative methods to determine the appropriate conditions for solid-state synthesis. This not only hinders the experimental realization of novel materials but also complicates the interpretation and understanding of solid-state reaction mechanisms. Here, we demonstrate a machine-learning approach that predicts synthesis...
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Full-text available
Superionic lithium conductivity has only been discovered in a few classes of materials, mostly found in thiophosphates and rarely in oxides. Herein, we reveal that corner-sharing connectivity of the oxide crystal structure framework promotes superionic conductivity, which we rationalize from the distorted lithium environment and reduced interaction...
Article
We introduce ℓ0ℓ2-norm regularization and hierarchy constraints into linear regression for the construction of cluster expansions to describe configurational disorder in materials. The approach is implemented through mixed integer quadratic programming (MIQP). The ℓ2-norm regularization is used to suppress intrinsic data noise, while the ℓ0-norm is...
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The cycling of cathode materials for Li-ion batteries is often accompanied by a change in volume, posing a challenge to the integrity of cathode particles and electrolyte/cathode interface in solid-state batteries. To enhance capacity retention, it is thus crucial to design materials that remain structurally invariant during electrochemical cycling...
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Disordered multicomponent systems attract great interest due to their engineering design flexibility and subsequent rich space of properties. However, detailed characterization of the structure and atomic correlations remains challenging and hinders full navigation of these complex spaces. A lattice cluster expansion is one tool to obtain configura...
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Gold nanoparticles are highly desired for a range of technological applications due to their tunable properties, which are dictated by the size and shape of the constituent particles. Many heuristic methods for controlling the morphological characteristics of gold nanoparticles are well known. However, the underlying mechanisms controlling their si...
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Full-text available
The development of a materials synthesis route is usually based on heuristics and experience. A possible new approach would be to apply data-driven approaches to learn the patterns of synthesis from past experience and use them to predict the syntheses of novel materials. However, this route is impeded by the lack of a large-scale database of synth...
Preprint
Full-text available
We introduce the $\ell_0\ell_2$-norm regularization and hierarchy constraints into linear regression for the construction of cluster expansion to describe configurational disorder in materials. The approach is implemented through mixed integer quadratic programming (MIQP). The $\ell_2$-norm regularization is used to compress intrinsic data noise, w...
Preprint
Full-text available
Gold nanoparticles are highly desired for a range of technological applications due to their tunable properties, which are dictated by the size and shape of the constituent particles. Many heuristic methods for controlling the morphological characteristics of gold nanoparticles are well known. However, the underlying mechanisms controlling their si...
Preprint
Full-text available
There currently exist no quantitative methods to determine the appropriate conditions for solid-state synthesis. This not only hinders the experimental realization of novel materials but also complicates the interpretation and understanding of solid-state reaction mechanisms. Here, we demonstrate a machine-learning approach that predicts synthesis...
Article
Relating the synthesis conditions of materials to their functional performance has long been an experience‐based trial‐and‐error process. However, this methodology is not always efficient in identifying an appropriate protocol and can lead to overlooked opportunities for the performance optimization of materials through simple modifications of the...
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Full-text available
A bottleneck in efficiently connecting new materials discoveries to established literature has arisen due to an increase in publications. This problem may be addressed by using named entity recognition (NER) to extract structured summary-level data from unstructured materials science text. We compare the performance of four NER models on three mate...
Preprint
Full-text available
Applying AI power to predict syntheses of novel materials requires high-quality, large-scale datasets. Extraction of synthesis information from scientific publications is still challenging, especially for extracting synthesis actions, because of the lack of a comprehensive labeled dataset using a solid, robust, and well-established ontology for des...
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A Unified Language of Synthesis Actions (ULSA) for describing inorganic synthesis is developed to help create a synthesis ontology and a solid foundation for autonomous robotic synthesis.
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Lead-Free halide double perovskites with enhanced stability have gained attention as a promising environmentally friendly alternative to lead-based halide perovskites. Amongst different halide double perovskites, Cs2AgBiBr6 has shown attractive optoelectronic...
Article
Compressed sensing has become a widely accepted paradigm to construct high dimensional cluster expansion models used for statistical mechanical studies of atomic configuration in complex multicomponent crystalline materials. However, strict sampling requirements necessary to obtain minimal coherence measurements for compressed sensing to guarantee...
Preprint
Full-text available
The factors controlling the size and morphology of nanoparticles have so far been poorly understood. Data-driven techniques are an exciting avenue to explore this field through the identification of trends and correlations in data. However, for these techniques to be utilized, large datasets annotated with the structural attributes of nanoparticles...
Preprint
Full-text available
The development of a materials synthesis route is usually based on heuristics and experience. A possible new approach would be to apply data-driven approaches to learn the patterns of synthesis from past experience and use them to predict the syntheses of novel materials. However, this route is impeded by the lack of a large-scale database of synth...
Article
Finding high‐voltage Ca cathode materials is a critical step to unleashing the full potential of high‐energy‐density Ca‐ion batteries. First‐principles calculations are used to demonstrate that P‐type layered calcium transition metal (TM) oxide materials (CaTM2O4) with a range of TM substitutions (TM = Ti, V, Cr, Mn, Fe, Co, and Ni) have excellent...
Article
Conventional Li-ion cathode materials are dominated by well-ordered structures, in which Li and transition metals occupy distinct crystallographic sites. We show in this paper that profoundly new degrees of freedom for the optimization of electrochemical properties may be accessed if controllable cation disorder is introduced. In a class of high-ca...
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Full-text available
In this paper we develop the stability rules for NASICON-structured materials, as an example of compounds with complex bond topology and composition. By first-principles high-throughput computation of 3881 potential NASICON phases, we have developed guiding stability rules of NASICON and validated the ab initio predictive capability through the syn...
Preprint
Full-text available
Compressed sensing has become a widely accepted paradigm to construct high dimensional cluster expansion models used for statistical mechanical studies of atomic configuration in complex multicomponent crystalline materials. However, strict sampling requirements necessary to obtain minimal coherence measurements for compressed sensing to guarantee...
Article
Full-text available
The key component in lithium solid‐state batteries (SSBs) is the solid electrolyte composed of lithium superionic conductors (SICs). Lithium oxide SICs offer improved electrochemical and chemical stability compared with sulfides, and their recent advancements have largely been achieved using materials in the garnet‐ and NASICON (sodium superionic c...
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Metal penetration into a solid electrolyte (SE) is one of the critical problems impeding the practical application of solid-state batteries. In this study, we investigate the conditions under which electronic conductivity of the SE can lead to metal deposition and fracture within the SE. Three different stages for void filling (metal plating initia...
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CaFe2O4-type sodium postspinels (Na-CFs), with Na⁺ occupying tunnel sites, are of interest as prospective battery electrodes. While many compounds of this structure type require high-pressure synthesis, several compounds are known to form at ambient pressure. Here we report a large expansion of the known Na-CF phase space at ambient pressure, havin...
Article
Autonomous experimentation driven by artificial intelligence (AI) provides an exciting opportunity to revolutionize inorganic materials discovery and development. Herein, we review recent progress in the design of self-driving laboratories, including robotics to automate materials synthesis and characterization, in conjunction with AI to interpret...
Article
A promising high-voltage spinel oxide cathode material MgCrMnO4 with 18% Mg/Mn inversion was synthesized successfully. A new custom operando battery device was designed to study the cation migration mechanisms of the MgCrMnO4 cathode using 0.1 M Mg(TPFA)2 electrolyte dissolved in triglyme and activated carbon as the anode. For the first time in mul...
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Full-text available
High-rate cathode materials for Li-ion batteries require fast Li transport kinetics, which typically rely on topotactic Li intercalation/de-intercalation because it minimally disrupts Li transport pathways. In contrast to this conventional view, here we demonstrate that the rate capability in a Li-rich cation-disordered rocksalt cathode can be sign...
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Full-text available
Cation‐disordered rocksalt (DRX) materials have emerged as a class of novel high‐capacity cathodes for Li‐ion batteries. However, the commercialization of DRX cathodes will require reducing their capacity decay, which has been associated with oxygen loss during cycling. Recent studies show that fluorination of DRX cathodes can effectively reduce ox...
Article
An ion exchange reaction that can stabilize potassium transition metal oxides was proposed as a new approach to develop cathode materials for K-ion batteries (KIBs). ¹⁻⁴ Such ion exchange method indeed has frequently used for the development of novel Li-layered oxides to attain structural features of Na layered oxides. ⁵⁻⁷ Although the ion exchange...
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Layered intercalation compounds are the dominant cathode materials for rechargeable Li-ion batteries. In this article we summarize in a pedagogical way our work in understanding how the structure’s topology, electronic structure, and chemistry interact to determine its electrochemical performance. We discuss how alkali–alkali interactions within th...
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Autonomous synthesis and characterization of inorganic materials require the automatic and accurate analysis of X-ray diffraction spectra. For this task, we designed a probabilistic deep learning algorithm to identify complex multi-phase mixtures. At the core of this algorithm lies an ensemble convolutional neural network trained on simulated diffr...
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In this work, we report the presence of surface-densified phases (β-Ni5O8, γ-Ni3O4, and δ-Ni7O8) in LiNiO2 (LNO)- and LiNi0.8Al0.2O2 (LNA)-layered compounds by combined atomic level scanning transmission electron microscopy (STEM) and electron energy loss spectroscopy (EELS). These surface phases form upon electrochemical aging at high state of cha...
Article
Inspired by the fascinating class of hybrid organic-inorganic halide perovskite materials, halide double perovskites have emerged as non-toxic Pb-free contenders for application as active layers in optoelectronic devices. Heterovalent substitution of Pb²⁺ by non-toxic metal cations yields the double-perovskite structure, which allows for compositio...
Preprint
Full-text available
Autonomous synthesis and characterization of inorganic materials requires the automatic and accurate analysis of X-ray diffraction spectra. For this task, we designed a probabilistic deep learning algorithm to identify complex multi-phase mixtures. At the core of this algorithm lies an ensemble convolutional neural network trained on simulated diff...
Article
Pourbaix diagrams show solid-aqueous phase stability as a function of pH and redox potential and can be a valuable tool to guide the hydrothermal synthesis of transition metal oxides. However, the Pourbaix diagram is based on thermodynamics, and nucleation kinetics are not readily apparent in this framework. Here, we conduct a combined experimental...
Preprint
In this paper we develop the stability rules for NASICON structured materials, as an example of compounds with complex bond topology and composition. By applying machine learning to the ab-initio computed phase stability of 3881 potential NASICONs we can extract a simple two-dimensional descriptor that is extremely good at separating stable from un...
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Full-text available
High-entropy (HE) ceramics, by analogy with HE metallic alloys, are an emerging class of solid solutions composed of a large number of species. These materials offer the benefit of large compositional flexibility and can be used in a wide variety of applications, including thermoelectrics, catalysts, superionic conductors and battery electrodes. We...
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Full-text available
Research publications are the major repository of scientific knowledge. However, their unstructured and highly heterogenuous format creates a significant obstacle to large-scale analysis of the information contained within. Recent progress in natural language processing (NLP) has provided a variety of tools for high-quality information extraction f...
Preprint
BACKGROUND The rate of publication of COVID-19 literature is astonishing and the research is extremely varied. Innovative tools are needed to aid researchers to find patterns in this vast amount of literature to identify subsets of interest in an automated fashion. OBJECTIVE We present a new online software resource with a friendly user interface...
Article
The pursuit of scalable and manufacturable all-solid-state batteries continues to intensify, motivated by the rapidly increasing demand for safe, dense electrical energy storage. In this perspective, we describe the numerous, often conflicting implications of materials choices that have been made in the search for effective mitigations to the inter...
Article
Background: Papers on COVID-19 are being published at a high rate and concern many different topics. Innovative tools are needed to aid researchers to find patterns in this vast amount of literature to identify subsets of interest in an automated fashion. Objective: We present a new online software resource with a friendly user interface that al...
Article
Discovering high-energy cathode materials is critical to construct K-ion batteries for practical applications. Owing to the great success of layered oxides in Li- and Na-ion system, K layered cathodes have...
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Full-text available
The tremendous improvement in performance and cost of lithium-ion batteries (LIBs) have made them the technology of choice for electrical energy storage. While established battery chemistries and cell architectures for Li-ion batteries achieve good power and energy density, LIBs are unlikely to meet all the performance, cost, and scaling targets re...
Preprint
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The ongoing COVID-19 pandemic has had far-reaching effects throughout society, and science is no exception. The scale, speed, and breadth of the scientific community's COVID-19 response has lead to the emergence of new research literature on a remarkable scale -- as of October 2020, over 81,000 COVID-19 related scientific papers have been released,...
Article
Using both computations and experiments, we demonstrate that the performance of Li-excess cation-disordered rocksalt cathodes can be improved by Mg substitution. Mg reduces the amount of Li in the compound that is strongly bound to F and thereby increases the capacity. This enables the use of fluorination as a tool to improve stability of the compo...
Article
Given the emergence of data science and machine learning throughout all aspects of society, but particularly in the scientific domain, there is increased importance placed on obtaining data. Data in materials science are particularly heterogeneous, based on the significant range in materials classes that are explored and the variety of materials pr...
Article
To design a synthesis route for energy storage materials, the phase diagram is a useful starting point. However, non-equilibrium intermediates often appear during synthesis—which are difficult to anticipate and often persist as impurities in the final reaction product. In addition, intermediate phases may template the morphology of particles. Thus,...
Article
Fast-charging batteries typically employ electrodes capable of accommodating lithium continuously via solid-solution transformation because they have few kinetic barriers apart from Li ⁺ diffusion.[1, 2] One exception is lithium titanate, an anode that can cycle without the Li plating observed in graphite [3] and exhibits extraordinary rate capabil...
Article
The effect of ionic and electronic conductivity in the solid electrolytes (SE) on metal (such as Li, Na) deposition and dendrite propagation in the SE are investigated. A new framework for metal formation inside defects (such as voids, grain boundaries) in the SE due to the electronic conductivity of the SE is established. We find that for typical...