Microstructural Evolution Dynamics in Rapid Joule Heating Densification of High-Nickel Cathodes.

High-energy density materials are essential for the advancement of next-generation lithium-ion batteries, which power a wide range of applications from portable electronics to electric vehicles. Among them, high-Nickel (Ni) layered oxide cathodes have emerged as promising candidates due to their high capacity and cost-effectiveness. However, pores and excessive grain growth in high-Ni layered oxides compromise energy density and mechanical integrity, while oversized grains hinder lithium-ion diffusion kinetics, necessitating a sintering strategy that promotes densification without inducing abnormal grain growth.

A Differentiable Material Point Method Framework for Shape Morphing.

We present a novel, physically-based morphing technique for elastic shapes, leveraging the differentiable material point method (MPM) with space-time control through per-particle deformation gradients to accommodate complex topology changes. This approach, grounded in MPM's natural handling of dynamic topologies, is enhanced by a chained iterative optimization technique, allowing for the creation of both succinct and extended morphing sequences that maintain coherence over time. Demonstrated across various challenging scenarios, our method is able to produce detailed elastic deformation and topology transitions, all grounded within our physics-based simulation framework.

Time-resolved probing of laser-induced nanostructuring processes in liquids.

Laser synthesis and processing of colloids (LSPC) in liquids has gained widespread applications in producing nanomaterials of different classes of solids. While the technical processes in different cases of ablation, fragmentation or colloidal fusion may look macroscopically different in each application, the underlying fundamental mechanisms are always the same cascade of laser interaction with matter, non-thermal or thermal energy deposition, phase transitions, and the subsequent structure formation processes. Disentangling these mechanisms represents a veritable challenge, as ultrafast and structurally sensitive experimental methods are required.

Electronic Melting of Silicon in Nanostructures using X-ray Forbidden Bragg Reflections.

We carried out a short beamtime at the Pohang Accelerator Laboratory x-ray Free Electron Laser to perform a pump-probe (PP) laser excitation diffraction experiment on the silicon (222) forbidden Bragg peak. To limit the x-ray penetration, we used a "device layer" silicon film wafer bonded to a silicon substrate. The sample, specially fabricated by MEMC Electronic Materials, had a Si(100) substrate bonded to a 170 nm Si(100) film rotated at 45° for crystallographic isolation.

Frustrated phonon with charge density wave in vanadium Kagome metal.

The formation of a star-of-David charge density wave superstructure, resulting from the coordinated displacements of vanadium ions on a corner-sharing triangular lattice, has garnered significant attention to comprehend the influence of electron-phonon interaction within geometrically intricate lattice of Kagome metals, specifically AVSb (where A represents K, Rb, or Cs). However, understanding of the underlying mechanism behind charge density wave formation, coupled with symmetry-protected lattice vibrations, remains elusive. Here, from femtosecond time-resolved X-ray scattering experiments, we reveal that the phonon mode, associated with cesium ions' out-of-plane motion, becomes frustrated in the charge density wave phase.

Development of the Nanobeam X-ray Experiments instrument at PAL-XFEL.

A Nanobeam X-ray Experiments (NXE) instrument was developed and installed at the hard X-ray beamline of the Pohang Accelerator Laboratory X-ray Free Electron Laser. This instrument consists of a diagnostic system, focusing optics, an X-ray diffraction endstation and a femtosecond laser delivery system. The NXE instrument enables sophisticated X-ray experiments using nanofocused X-rays.

Halloysite nanotubes enhanced polyimide/oxidized-lignin nanofiber separators for long-cycling lithium metal batteries.

The high energy density and robust cycle properties of lithium-ion batteries contribute to their extensive range of applications. Polyolefin separators are often used for the purpose of storing electrolytes, hence ensuring the efficient internal ion transport. Nevertheless, the electrochemical performance of lithium-ion batteries is constrained by its limited interaction with electrolytes and poor capacity for cation transport.

Inverted nucleation for photoinduced nonequilibrium melting.

Ultrafast photoinduced melting provides an essential platform for studying nonequilibrium phase transitions by linking the kinetics of electron dynamics to ionic motions. Knowledge of dynamic balance in their energetics is essential to understanding how the ionic reaction is influenced by femtosecond photoexcited electrons with notable time lag depending on reaction mechanisms. Here, by directly imaging fluctuating density distributions and evaluating the ionic pressure and Gibbs free energy from two-temperature molecular dynamics that verified experimental results, we uncovered that transient ionic pressure, triggered by photoexcited electrons, controls the overall melting kinetics.

Development of the multiplex imaging chamber at PAL-XFEL.

Various X-ray techniques are employed to investigate specimens in diverse fields. Generally, scattering and absorption/emission processes occur due to the interaction of X-rays with matter. The output signals from these processes contain structural information and the electronic structure of specimens, respectively.

Emergence of liquid following laser melting of gold thin films.

X-ray structural science is undergoing a revolution driven by the emergence of X-ray Free-electron Laser (XFEL) facilities. The structures of crystalline solids can now be studied on the picosecond time scale relevant to phonons, atomic vibrations which travel at acoustic velocities. In the work presented here, X-ray diffuse scattering is employed to characterize the time dependence of the liquid phase emerging from femtosecond laser-induced melting of polycrystalline gold thin films using an XFEL.

Nanoscale Three-Dimensional Network Structure of a Mesoporous Particle Unveiled via Adaptive Multidistance Coherent X-ray Tomography.

Mesoporous nanoparticles provide rich platforms to devise functional materials by customizing the three-dimensional (3D) structures of nanopores. With the pore network as a key tuning parameter, the noninvasive and quantitative characterization of these 3D structures is crucial for the rational design of functional materials. This has prompted researchers to develop versatile nanoprobes with a high penetration power to inspect various specimens sized a few micrometers at nanoscale 3D resolutions.

Observing femtosecond orbital dynamics in ultrafast Ge melting with time-resolved resonant X-ray scattering.

Photoinduced nonequilibrium phase transitions have stimulated interest in the dynamic interactions between electrons and crystalline ions, which have long been overlooked within the Born-Oppenheimer approximation. Ultrafast melting before lattice thermalization prompted researchers to revisit this issue to understand ultrafast photoinduced weakening of the crystal bonding. However, the absence of direct evidence demonstrating the role of orbital dynamics in lattice disorder leaves it elusive.

A novel high-performance electrospun of polyimide/lignin nanofibers with unique electrochemical properties and its application as lithium-ion batteries separators.

Polypropylene is currently one of the most widely used separators in lithium batteries because of its low cost and chemical stability. However, it also has some intrinsic flaws that hamper the battery performance, such as poor wettability, low ionic conductivity, and some safety issues. This work introduces a novel electrospun nanofibrous consisting of polyimide (PI) blended with lignin (L) to serve as a new class of bio-based separators for lithium-ion batteries.

Influence of structure and functional group of modified kraft lignin on adsorption behavior of dye.

Utilization of kraft lignin to produce bio-based adsorptive material for effective dye adsorption from industrial wastewater is essential to fulfilling the significant environmental protection needs. Lignin is the most abundant byproduct material with a chemical structure containing various functional groups. However, the complicated chemical structure makes it somewhat hydrophobic and incompatible, which limits its direct application as an adsorption material.

Ultrafast Energy Transfer Process in Confined Gold Nanospheres Revealed by Femtosecond X-ray Imaging and Diffraction.

Femtosecond laser pulses drive nonequilibrium phase transitions via reaction paths hidden in thermal equilibrium. This stimulates interest to understand photoinduced ultrafast melting processes, which remains incomplete due to challenges in resolving accompanied kinetics at the relevant space-time resolution. Here, by newly establishing a multiplexing femtosecond X-ray probe, we have successfully revealed ultrafast energy transfer processes in confined Au nanospheres.

Three-Dimensional Quantitative Coherent Diffraction Imaging of Treated with Peptide-Mineralized Au-Cluster Probes.

Characterizing interactions between microbial cells and their specific inhibitory drugs is essential for developing effective drugs and understanding the therapeutic mechanism. Functional metal nanoclusters can be effective inhibitory agents against microorganisms according to various characterization methods, but quantitative three-dimensional (3D) spatial structural analysis of intact cells is lacking. Herein, using coherent X-ray diffraction imaging, we performed in situ 3D visualization of unstained cells treated with peptide-mineralized Au-cluster probes at a resolution of ∼47 nm.

Quantitative analysis of the effect of radiation on mitochondria structure using coherent diffraction imaging with a clustering algorithm.

Radiation damage and a low signal-to-noise ratio are the primary factors that limit spatial resolution in coherent diffraction imaging (CDI) of biomaterials using X-ray sources. Introduced here is a clustering algorithm named based on deep learning, and it is applied to obtain accurate and consistent image reconstruction from noisy diffraction patterns of weakly scattering biomaterials. To investigate the impact of X-ray radiation on soft biomaterials, CDI experiments were performed on mitochondria from human embryonic kidney cells using synchrotron radiation.

Inducing thermodynamically blocked atomic ordering via strongly driven nonequilibrium kinetics.

Ultrafast light-matter interactions enable inducing exotic material phases by promoting access to kinetic processes blocked in equilibrium. Despite potential opportunities, actively using nonequilibrium kinetics for material discovery is limited by the poor understanding on intermediate states of driven systems. Here, using single-pulse time-resolved imaging with x-ray free-electron lasers, we found intermediate states of photoexcited bismuth nanoparticles that showed kinetically reversed surface ordering during ultrafast melting.

Stochastic chromatin packing of 3D mitotic chromosomes revealed by coherent X-rays.

DNA molecules are atomic-scale information storage molecules that promote reliable information transfer via fault-free repetitions of replications and transcriptions. Remarkable accuracy of compacting a few-meters-long DNA into a micrometer-scale object, and the reverse, makes the chromosome one of the most intriguing structures from both physical and biological viewpoints. However, its three-dimensional (3D) structure remains elusive with challenges in observing native structures of specimens at tens-of-nanometers resolution.

Oxidation-induced three-dimensional morphological changes in Ni nanoparticles observed by coherent X-ray diffraction imaging.

Three-dimensional structures of Ni nanoparticles undergoing significant morphological changes on oxidation were observed non-destructively using coherent X-ray diffraction imaging. The Ni particles were oxidized into NiO while forming pores of various sizes internally. For each Ni nanoparticle, one large void was identified at a lower corner near the interface with the substrate.

High-Throughput 3D Ensemble Characterization of Individual Core-Shell Nanoparticles with X-ray Free Electron Laser Single-Particle Imaging.

The structures as building blocks for designing functional nanomaterials have fueled the development of versatile nanoprobes to understand local structures of noncrystalline specimens. Progress in analyzing structures of individual specimens with atomic scale accuracy has been notable recently. In most cases, however, only a limited number of specimens are inspected lacking statistics to represent the systems with structural inhomogeneity.

Ultrafast x-ray diffraction study of melt-front dynamics in polycrystalline thin films.

Melting is a fundamental process of matter that is still not fully understood at the microscopic level. Here, we use time-resolved x-ray diffraction to examine the ultrafast melting of polycrystalline gold thin films using an optical laser pump followed by a delayed hard x-ray probe pulse. We observe the formation of an intermediate new diffraction peak, which we attribute to material trapped between the solid and melted states, that forms 50 ps after laser excitation and persists beyond 500 ps.

Characterizing the intrinsic properties of individual XFEL pulses via single-particle diffraction.

With each single X-ray pulse having its own characteristics, understanding the individual property of each X-ray free-electron laser (XFEL) pulse is essential for its applications in probing and manipulating specimens as well as in diagnosing the lasing performance. Intensive research using XFEL radiation over the last several years has introduced techniques to characterize the femtosecond XFEL pulses, but a simple characterization scheme, while not requiring ad hoc assumptions, to address multiple aspects of XFEL radiation via a single data collection process is scant. Here, it is shown that single-particle diffraction patterns collected using single XFEL pulses can provide information about the incident photon flux and coherence property simultaneously, and the X-ray beam profile is inferred.