Recent lbnl_es_mf items

Electrode-omics reveals epochs in silicon anode evolution underpinning electrochemomechanical resilience

Tue, 4 Aug 2026 00:00:00 +0000

Here, we advance electrode-omics to identify evolutionary bursts by which ethereal locally superconcentrated electrolytes (LSCEs) mitigate silicon anode degradation through its epochs of electrochemical and chemical reactions. Anode composites form initially at high potential from ethereal solvent and anion [bis(fluorosulfonyl)imide (FSI^-)] redox. A first evolutionary burst at lower potential enriches composites with lithium alkoxides (LiO-R) and lithium oxide (Li₂O) and depletes sulfur oxides (SO_x) species. As the cells are cycled, a second evolutionary burst takes place, where previously extinct SO_x species reemerge concurrently with a loss of LiO-R and Li₂O. This identifies reactions rooted in "SuFEx" chemistry, where oxoanionic LiO-R and Li₂O species, electrochemically generated in the solid-electrolyte interphase, chemically react with FSI^- in the electrolyte to form emergent species....

High-throughput analysis of total electron yield and outgassing under EUV exposure for accelerated photoresist materials discovery

Thu, 30 Jul 2026 00:00:00 +0000

As technology nodes shrink, extreme ultraviolet (EUV) photoresists are essential for high-resolution nanopatterning. Incident photons, as well as electrons generated during EUV exposure can cause both intended and unintended chemical reactions. Understanding these processes is critical for improving resist performance. This study investigates how resist components, particularly photoacid generators (PAGs) and photo decomposable quenchers (PDQ), influence photon- and electron-induced chemistry. It also aims to develop a high-throughput characterization method for efficient screening of novel materials. A high-throughput system combining total electron yield (TEY) and residual gas analysis (RGA) was developed. TEY measures electron generation and capture, while RGA monitors chemical transformations via outgassing. The method is applied to model resists. TEY and outgassing analysis revealed that PAGs and PDQs strongly influence electron behavior and outgassing characteristics. The...

Toward Hydrogen Isotope Separations through Strong Hydrogen Adsorption at Open Copper(I) Sites in an Ultramicroporous Metal–Organic Framework

Wed, 29 Jul 2026 00:00:00 +0000

Metal-organic frameworks with coordinatively unsaturated metal sites (open metal sites) capable of engaging in orbital interactions with π-acidic gases are of interest for enabling ambient-temperature gas separations, such as hydrogen isotope separations. In view of the weakly π-acidic nature of H₂, we sought to strengthen π-backbonding-mediated H₂ adsorption through pore confinement effects. Toward that end, we synthesized and characterized the ultramicroporous metal-organic framework Cu_xZn_5-xCl_4-yH_z(bbta)₃ (Cu^IZn-MFU-4; H₂bbta = 1H,5H-benzo(1,2-d:4,5-d')bistriazole), featuring π-basic trigonal pyramidal Cu^I sites that reside within 7 Å of one another at their closest. Gas adsorption measurements reveal an H₂ adsorption enthalpy of -38 kJ/mol, exceeding that of the larger-pore analog (Cu^IZn-MFU-4l;...

Identifying Strain Stacking Boundaries between Multiphase Domains in Atomically Thin Two-Dimensional Magnets

Wed, 29 Jul 2026 00:00:00 +0000

Stacking engineering of van der Waals materials is an important strategy to control the materials' properties, such as electronic correlations, ferroelectricity, and layer-dependent two-dimensional magnetism. A timely testbed for the study of the latter is atomically thin chromium trihalides (CrX₃, X = Cl, Br, I). Notably, by understanding the sliding mechanism between different stacking sequences, control of the stacking arrangement, and thus magnetic properties in CrX₃, can be achieved. Such insight, however, is currently lacking. Here, advanced electron microscopy methods are used to identify multiple stacking sequences corresponding to different bulk phases in atomically thin CrX₃ (X = Cl and Br) down to bilayer thickness and with lateral domain sizes as small as tens of nanometers. Indications of nanometer scale transitions and interactions at the stacking boundaries are found, including a universally preferred sliding direction that is consistent...

The Use of Synchrotron Radiation in the Medical Sciences

Tue, 28 Jul 2026 00:00:00 +0000

Synchrotron radiation (SR) sources provide unparalleled brilliance, collimation, coherence, and tunability, enabling specialized techniques that are crucial for advancing medical research across diverse fields from radiation oncology to rational drug design. Certain SR methods, such as macromolecular crystallography, are highly developed and automated, and have been used for decades for both fundamental understanding of biomolecules as well as pharmaceutical design, while other methods, such as microbeam radiation therapy, represent relatively recent developments. Scattering and diffraction methods using SR can provide atomic-level structural mapping of proteins, nucleic acids, and complexes. Imaging applications using SR continue to be developed and advanced for mapping of biological structures and potential use as diagnostics in disease detection. Spectroscopic methods are used to study elemental distributions relevant for detection of contamination in biological systems. Collectively,...

Recommendations and considerations for hydroxyl radical protein footprinting–mass spectrometry

Tue, 28 Jul 2026 00:00:00 +0000

Protein oxidative footprinting, using hydroxyl radical labeling detected by bottom-up proteomics, has progressed from an emerging method to a widely used approach in structural biology. Hydroxyl radicals generated from hydrogen peroxide (via photolysis, Fenton chemistry or electrochemistry) or directly from water (via X-rays, plasma or gamma rays) irreversibly encode structural information within protein side chains, which is read out using standard liquid chromatography–mass spectrometry workflows. Quantitative changes in labeling report on solvent accessibility and reveal effects of protein–protein interactions, ligand binding, protein folding, conformational changes or applied stress. Comparing labeling patterns between states provides detailed maps of structural changes and interaction sites. Over the past decade, oxidative footprinting has proven valuable as a solution-phase and in-cell method for protein structure analysis. This Perspective summarizes best practices for...

Unsupervised Segmentation and Clustering Workflow for Efficient Processing of 4D-STEM and 5D-STEM Data

Mon, 27 Jul 2026 00:00:00 +0000

Four-dimensional scanning transmission electron microscopy (4D-STEM) enables mapping of diffraction information with nanometer-scale spatial resolution, offering detailed insight into local structure, orientation, and strain. However, as data dimensionality and sampling density increase, particularly for in situ scanning diffraction experiments (5D-STEM), robust segmentation of structurally consistent behavior across sequential measurements becomes essential for efficient and physically meaningful analysis. Here, we introduce a clustering framework that identifies crystallographically distinct domains from 4D-STEM datasets. By using local diffraction-pattern similarity as a metric, the method extracts closed contours delineating spatially contiguous regions. This approach produces cluster-averaged diffraction patterns that improve signal quality while reducing data volume by orders of magnitude, enabling rapid and accurate orientation, phase, and strain mapping. We demonstrate...

Visualizing Millisecond Atomic Dynamics of Nanocrystals in Liquid

Wed, 22 Jul 2026 00:00:00 +0000

Atomic structures of nanomaterials are inherently dynamic and continuously reshaped through interactions with chemical species and external stimuli. Such dynamics are further amplified as the size and dimensionality of nanomaterials decrease. Despite advances in analytical methods, it remains challenging to capture the structural dynamics of nanomaterials in reactive environments with both atomic spatial resolution and commensurate temporal resolution. Here, we directly visualize atomic-scale dynamics of gold (Au) nanocrystals in reactive liquid environments with millisecond-speed liquid-cell electron microscopy (EM) and deep-learning denoising. We uncover reversible fluctuations in the local crystallinity of Au nanocrystals dependent on the surrounding chemical environment. These transient fluctuations, driven by interactions at nanocrystal-liquid interfaces, critically influence the dissolution kinetics and grain boundary relaxation. By overcoming the spatiotemporal limitations...

Visualizing Crystallization Dynamics and Transformation Pathways of Disordered Rocksalt Oxides During Thermally Activated Sol–Gel Synthesis

Wed, 22 Jul 2026 00:00:00 +0000

ABSTRACT Sol–gel synthesis is a wet‐chemical processing route for fabricating functional materials with control over composition and microstructure at relatively low temperatures compared to conventional solid‐state synthesis. While sol–gel process initiates with intermixed molecular precursors, the early‐stage nucleation pathways are insufficiently understood. Here, the chemical and structural transformation of disordered rocksalt (DRX) Li 1.2 Mn 0.4 Ti 0.4 O 2 (LMTO), a promising cathode material for lithium batteries, is studied by multiscale characterizations. In situ heating transmission electron microscopy (TEM) using a liquid cell visualizes and identifies crystallization pathways at the nanoscale. While some regions follow a classical multi‐step transition through thermodynamically stable intermediates, others exhibit a kinetic shortcut via a localized amorphous matrix to directly form the DRX structure. Macroscale Fourier transform infrared spectroscopy corroborates...

Atomic Evolution of Hydrogen Intercalation Wave Dynamics in Palladium Nanocrystals Revealed by Liquid-Phase Transmission Electron Microscopy

Wed, 22 Jul 2026 00:00:00 +0000

Solute-intercalation-induced phase separation creates spatial heterogeneities in host materials, a phenomenon ubiquitous in batteries, hydrogen storage, and other energy devices. Despite many efforts, probing intercalation processes at the atomic scale has been a significant challenge. By utilizing liquid-phase transmission electron microscopy (TEM), we study hydrogen (de)intercalation in palladium nanocrystals as a model system and have achieved unprecedented atomic-resolution imaging of hydrogen intercalation wave dynamics. Our observations reveal that intercalation wave mechanisms, instead of shrinking-core mechanisms, prevail at ambient temperature for palladium nanocubes ranging from ∼60 nm down to ∼10 nm. Systematic image analysis uncovers the atomic evolution of the hydrogen intercalation wave, transitioning from nonplanar and inclined boundaries to those closely aligned with {100} planes. Our kinetic Monte Carlo simulations demonstrate that the observed intercalation wave...

The ABCs of phase retrieval: Connecting the acronyms of scanning transmission electron microscopy

Tue, 21 Jul 2026 00:00:00 +0000

High-resolution scanning transmission electron microscopy (S/TEM) is an indispensable tool for characterizing the structure and properties of materials down to the atomic scale. Conventional S/TEM imaging, however, is limited by the phase problem, whereby the phase of the electron exit wave is lost upon detection. Recent advances in diffractive imaging and 4D-STEM have enabled a range of phase-retrieval techniques that computationally reconstruct the missing information encoded in the phase of the transmission function. These approaches offer improved dose efficiency and enhanced sensitivity to weakly scattering signals, extending quantitative imaging to beam-sensitive materials composed of light elements. In this work, we introduce the phase problem in electron microscopy and survey the diverse landscape of phase-retrieval techniques used in the field. Despite their many acronyms and algorithmic variations, these techniques share a common physical and mathematical foundation....

Robust electron counting for direct electron detectors with the Back-propagation counting method

Wed, 15 Jul 2026 00:00:00 +0000

Electron microscopy (EM) is a foundational tool for directly assessing the structure of materials. Recent advances in direct electron detectors have improved signal-to noise ratios via single-electron counting. However, accurately counting electrons at high flux remains challenging. We developed a new method of electron counting for direct electron detectors, Back-Propagation Counting (BPC). BPC uses machine learning techniques designed for mathematical operations on large tensors but does not require large training datasets. In synthetic data, we show BPC is able to count multiple electron strikes per pixel and is robust to increasing occupancy. In experimental data, frames counted with BPC are shown to reconstruct diffraction peaks corresponding to individual nanoparticles with relatively higher intensity and produce images with improved contrast when compared to a standard counting method. Together, these results show that BPC excels in experiments where pixels see a high flux...

Photon Avalanching Nanoparticles

Wed, 15 Jul 2026 00:00:00 +0000

ConspectusAvalanches within nanoparticles seem like science fiction, but if they are avalanches of photons, they open up real-world innovations in imaging, sensing, optical computing, and other unexplored light-driven technologies. Avalanches are outsized events arising from the integration of many smaller inputs, and photon avalanching (PA) was first reported in bulk crystals in 1979 as an unexpectedly large jump in luminescence as excitation intensity was slowly increased. It would be 41 years before PA would be observed at the nanoscale in photon avalanching nanoparticles (ANPs), Tm³⁺-doped upconverting nanoparticles that show excited-to-ground state absorption inversion greater than 10,000:1 and emission that scales nonlinearly up to the 32nd power of the pump intensity. This extreme nonlinearity enables a real-time 5-fold improvement in the 150-year-old Abbe limit of spatial resolution, achieving 70 nm resolution using only simple scanning confocal microscopy....

Tiny Bubbles: Measuring Strain Fields and Missing Atoms in Nanoscale He Bubbles via High-Resolution STEM Techniques

Tue, 7 Jul 2026 00:00:00 +0000

Tiny Bubbles: Measuring Strain Fields and Missing Atoms in Nanoscale He Bubbles via High-Resolution STEM Techniques

Enabling simultaneous time-resolved spectroscopy and X-ray footprinting mass spectrometry to study conformational dynamics in protein

Fri, 3 Jul 2026 00:00:00 +0000

Enabling simultaneous time-resolved spectroscopy and X-ray footprinting mass spectrometry to study conformational dynamics in protein

Understanding the Cathode Electrochemistry of Humidified Solid‐State Lithium‐Oxygen Batteries

Wed, 1 Jul 2026 00:00:00 +0000

Abstract Lithium‐oxygen batteries (LOBs) possess a high theoretical energy density, making them potential candidates for next‐generation energy storage. However, challenges such as reactive oxygen species‐induced component degradation hinder their practical use. Inorganic solid‐state electrolytes offer an alternative to degradation‐prone aprotic electrolytes, while also protecting lithium anodes from potential atmospheric reactants. This study explores the cathode electrochemistry of solid‐state LOBs using humidified oxygen, which forms an aqueous catholyte during initial cycling, thereby improving cathode‐electrolyte contact. To quantitatively analyze the cathode electrochemistry, a ‘Humidity‐Incorporated’ Differential Electrochemical Gas Monitoring System (HiDEMS) is developed to control humidity and monitor gas consumption and evolution in real time. When studying a Li‐O 2 cell that employs a NASICON‐type Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) solid electrolyte and a porous...

Optical and spin properties of nitrogen vacancy centers in diamond formed along high-energy heavy ion tracks

Tue, 30 Jun 2026 00:00:00 +0000

Exposure of matter to high-energy heavy ions induces defects along the ion trajectories through electronic and nuclear energy loss processes. Defects, including color centers, can recombine or form along latent damage tracks in semiconductors. Latent tracks in diamond were only recently observed. Here we report on color center formation in nitrogen-doped diamond along the latent tracks of 1 GeV gold and uranium ions. We optically observe direct formation of single vacancy related color centers (GR1-centers) along the tracks. Mobile vacancies can form NV-centers with native nitrogen atoms during thermal annealing. Molecular dynamics simulations show that isolated vacancies and vacancy clusters form through electronic stopping processes along ion trajectories. Moreover, by using 1 GeV Au ions with a dilute fluence, we create individually isolated quasi-1D chains of NV-centers, which appear as isolated bright luminescence strings and present competitive electron spin properties compared...

Measurements of Electronic Band Structure in CeCoGe3 by Angle-Resolved Photoemission Spectroscopy

Tue, 30 Jun 2026 00:00:00 +0000

In this paper, we present a comprehensive study of the electronic structure of CeCoGe3 throughout the entire Brillouin zone in the non-magnetic regime using angle-resolved photoemission spectroscopy (ARPES). The electronic structure agrees in large part with first principles calculations, including predicted topological nodal lines. Two new features in the band structure are also observed, namely a surface state and folded bands, the latter of which is argued to originate from a unit cell reconstruction.

Patterned, Low-Temperature Growth of Transition Metal Dichalcogenides for Low Resistance Raised Contacts

Mon, 29 Jun 2026 00:00:00 +0000

Transition metal dichalcogenide (TMD) monolayers are promising channel materials for next-generation electronic devices. A challenge is the high contact resistance between monolayer TMDs and metal contacts, especially for holes. In this regard, raised source/drain contacts are promising. However, the direct, patterned growth of raised contacts at CMOS-compatible temperatures remains largely unresolved. We present plasma-free selenization and sulfurization of metal oxides at substrate temperatures down to 400 °C, compatible with back-end-of-line thermal budgets. To achieve growth at such temperatures, gas-phase chalcogen precursors are first thermally activated at 950 °C. Films grown on single-crystal monolayer TMDs exhibit high crystal quality, as confirmed by transmission electron microscopy. Raised contacts on WSe₂ monolayers fabricated using this approach yield a low hole contact resistance of 0.3 kΩ·μm after chemical doping. This process is shown to be applicable...

Ion transport through reconfigurable nanoparticle-surfactant stabilized droplet interface bilayers

Mon, 29 Jun 2026 00:00:00 +0000

Despite their adaptability and mechanical stability, Pickering emulsions based on the interfacial assembly of colloidal particles have not found use in iontronics, since the dense interfacial packing of micron-sized particles precludes functional connectivity between two droplets. Here, we introduce a chemically reconfigurable droplet interface bilayer (DIB) platform based on the interfacial assembly of nanoparticle-surfactants (NPSs) that enables spontaneous or field-induced formation of ion-conducting nanochannels, eliminating the need of ionophores or nanochannel-forming proteins. These nanoscopic channels emerge from packing defects in the jammed interfacial assemblies of the charged NPSs and support size and charge selective, hysteretic ion transport governed by interfacial electrostatics and dimensional constraints. The NPS-DIBs show short-term and long-term plasticity, hallmarks of neuromorphic behavior, that are mediated by the structural and chemical design of the bilayer....

CRAGE-RB-PI-seq reveals transcriptional dynamics of plant-associated bacteria during root colonization

Mon, 29 Jun 2026 00:00:00 +0000

Plant roots release a wide array of metabolites into the rhizosphere, shaping microbial communities and their functions. While metagenomics has expanded our understanding of these communities, little is known about the physiology of their members in host environments. Transcriptome analysis via RNA sequencing is a common approach to learning more, but its use has been challenging because of low bacterial biomass and interference from plant RNA. To overcome this, we developed a randomly-barcoded promoter-library insertion sequencing (RB-PI-seq) combined with chassis-independent recombinase-assisted genome engineering (CRAGE). Using Pseudomonas simiae WCS417 as a model rhizobacterium, this method enabled targeted amplification of barcoded transcripts, bypassing plant RNA interference and allowing measurement of thousands of promoter activities during Arabidopsis root colonization. Our analysis revealed temporally resolved transcriptional regulation, including those associated with...

Pattern-enhanced Resonant Soft X-ray Scattering for Operando monitoring of electrochemical solid-liquid interfaces

Mon, 29 Jun 2026 00:00:00 +0000

Unveiling interfaces at sub-nanometer scales is essential for advancing the understanding of complex chemical transformations. However, characterizing solid-liquid interfaces with high dimensional sensitivity and temporal resolution remains challenging, due to their dynamic nature and inaccessibility by conventional probes. Here we present an approach, Pattern-enhanced Resonant Soft X-ray Scattering, to overcome the challenges. Rooted in a “sample-as-optics” philosophy, this technique utilizes precisely engineered line-grating nanopatterns to modulate near-field X-ray illumination, coherently enhancing scattering signals from the line-gratings. We implement the method using Ni line-grating nanopatterns in electrochemical water oxidation. The periodic nanostructures serve as diffractive optical elements to reveal the Ni oxidation gradients and structural dynamics at the electrode-electrolyte interfaces. Finite-element simulations corroborate the observed trends by modeling variations...

Supramolecular assembly of molecular wires alternating crown ethers and metal–halide complexes

Thu, 25 Jun 2026 00:00:00 +0000

Metal–halide complexes serve as key emissive centres in halide perovskites; however, precise control over their spatial organization through bottom-up assembly is challenging. Here we show that a crown-ether-assisted supramolecular assembly strategy can alternatingly connect metal–halide complexes and (crown ether@A)2+ (where ‘A’ is an alkaline earth metal cation) complexes into a one-dimensional molecular wire, which can then be packed into a hexagonal crystal structure. This process resulted in the creation of an (18C6@Ba)MnBr4 single crystal with green emission, achieving over 80% photoluminescence quantum yield and a narrow full width at half maximum. In addition, the non-centrosymmetric crystal structure gave rise to strong nonlinear optical responses, including second-harmonic generation. This versatile supramolecular assembly approach could be generalized to create various [M(I)X2]−, [M(I)X3]2−, [M(II)X4]2− and [M(III)X5]2− molecular wires, broadening the potential for...

Beyond Contrast Transfer: Spectral SNR as a Finite-Dose Metric for STEM Phase Retrieval

Wed, 24 Jun 2026 00:00:00 +0000

The contrast transfer function (CTF) is widely used to evaluate phase retrieval methods in scanning transmission electron microscopy (STEM), including center-of-mass imaging, parallax imaging, direct ptychography, and iterative ptychography. However, the CTF reflects only the maximum usable signal, neglecting the effects of finite electron fluence and the Poisson-limited nature of detection. As a result, it can significantly overestimate practical performance, especially in low-dose regimes. Here, we employ the spectral signal-to-noise ratio (SSNR), as a finite-dose statistical framework to evaluate the recoverable signal as a function of spatial frequency. Using numerical reconstructions of white-noise objects, we show that center-of-mass, parallax, and direct ptychography exhibit dose-independent SSNRs, with close-form analytic expressions. In contrast, iterative ptychography exhibits a surprising dose dependence: at low fluence, its SSNR converges to that of direct ptychography;...

Relaxing Direct Ptychography Sampling Requirements via Parallax Imaging Insights

Wed, 24 Jun 2026 00:00:00 +0000

Direct ptychography enables the retrieval of information encoded in the phase of an electron wave passing through a thin sample by deconvolving the interference effects of a converged probe with known aberrations. Under the weak phase object approximation, this permits the optimal transfer of information using noniterative techniques. However, the achievable resolution of the technique is traditionally limited by the probe step size-setting stringent Nyquist sampling requirements. At the same time, parallax imaging has emerged as a dose-efficient phase technique which relaxes sampling requirements and enables scan-upsampling. Here, we formulate parallax imaging as a quadratic approximation to part of the direct ptychography kernel and use this insight to enable upsampling in direct ptychography. We validate our analytical results numerically using simulated and experimental reconstructions.

X-ray footprinting/mass spectrometry provides a new, detailed view of intrinsically disordered protein structural ensembles

Tue, 23 Jun 2026 00:00:00 +0000

X-ray footprinting/mass spectrometry provides a new, detailed view of intrinsically disordered protein structural ensembles

Mesoporous peptide frameworks engineered from crystallizable collagen-mimetic peptide amphiphiles

Tue, 16 Jun 2026 00:00:00 +0000

The rational design of porous frameworks with tunable pore dimensions and chemical functionalities is a critical step toward their implementation in diverse applications. While traditional porous materials are typically constructed from abiotic components, there is increasing interest in employing biologically derived building blocks (e.g., peptides and proteins) that offer unmatched structural and functional diversity. Here, we report the construction of crystalline mesoporous frameworks that are self-assembled from amphiphilic collagen-mimetic peptides. Comprehensive structural characterization via microscopy, spectroscopy, and computational techniques provides insights into the assembly packing model, in which hexagonally packed channels are interconnected by antiparallel-aligned collagen triple helices via hydrophobic and electrostatic interactions. Lastly, we demonstrate the functional potential of aCMP frameworks through the encapsulation of various molecular guests,...

A Prodrug Strategy to Conditionally Trap Therapeutic Payloads for Improved Tumor Retention

Mon, 15 Jun 2026 00:00:00 +0000

Altered extracellular proteolysis has been exploited to selectively activate therapeutics in diseases such as cancer; however, once activated, extracellular drugs can diffuse away, limiting efficacy. We address this challenge by coupling proteolytic activation with membrane tethering to retain drugs within diseased tissue. To accomplish this, we developed "restricted interaction peptides" (RIPs), a delivery platform that leverages elevated proteolytic activity to activate membrane-interacting peptides, localizing cargos near the site of proteolysis. We demonstrate that RIPs can deliver diverse therapeutic cargos, including cytotoxins and radioisotopes. As proof of concept, we engineered "FRIP," a RIP designed for cleavage by fibroblast activation protein (FAP), an endoprotease upregulated in solid tumors and fibrosis. Efficient P4-P4' substrate sequences were identified and incorporated into FRIPs. Cell-based studies showed that, upon activation, the peptide adhered to membranes...

A dual membrane-adsorption evaporator for solar-powered lithium extraction from complex brines